Cold Fusion: Advances in Condensed Matter Nuclear Science 0128159448, 9780128159446

Table of contents :
Cover
Cold Fusion:
Advances in Condensed Matter
Nuclear Science
Copyright
Dedication
Contributors
Preface
Part 1: Electrochemistry
1
Production of helium in cold fusion experiments
Introduction
First set of heat and helium measurements (1990)
Analysis of the first set of helium measurements
Experimental measurement of He-4 diffusion into glass flasks
Second set of helium measurements (1991-92)
Analysis of the third set of helium measurements (1993-94)
Discussion of China Lake heat and He-4 results
Related research by other laboratories
The CalTech and MIT He-4 experiments in 1989
Acknowledgments
References
2
Review of Pd/D co-deposition
Introduction
Heat
Tritium
Energetic particles
γ-/X-Ray emissions
Transmutation
Conclusions
Acknowledgments
References
3
Electrochemical loading to produce the Fleischmann-Pons heat effect (FPHE)
Introduction
Variability
Electrochemistry
Surface structure
Bulk metallurgy
Progress
High reproducibility excess heat at SRI
Conclusions
References
4
Fundamentals of isoperibolic calorimetric for cold fusion experiments
Introduction: Choosing an isoperibolic calorimeter
Isoperibolic calorimetric equations and possible simplifications
Applications to cold fusion experiments
More about the lower bound heat transfer coefficient
The neglected PG and PW terms
The straight-line method
Radiative heat transfer coefficient
Cell cooling experiments
Additional calorimetric topics
Calorimetric results from CalTech, MIT, and Harwell
Appendix
Acknowledgments
References
5
Can clean and stable deuterium loading and well-tailored microstructure improve reproducibility?
Introduction
Morphology of deuterated thick Pd rod during long-term electrolysis in 0.1M LiOD
Experimental
Electrolyte and experimental cell
Electrode and electric leads
The working-electrode and counter-electrode configuration
Microstructure characterization using scanning electron microscope (SEM)
Results and discussion
Microstructure of thick Pd rod and dilation under long-term electrolysis-Exp. 1
Microstructure of thick Pd rod under long-term electrolysis-Exp. 2
SEM views of the electrode surface
SEM views of the electrode interior
Nuclear reaction cycle model
Microstructural change of a Pd rod during repeated cathodic and anodic electrolysis in glycerin-phosphoric acid: First abso ...
Experimental
Results and discussion
Microstructure of the α+β phase coexistence region characterized from in situ small punch test and the knowledge of hydroge ...
Coincidence of two hydrogen states with the characteristic hydrogen states: Defects induced by the interaction of hydrogen ...
Two types of H electrode characterized above Vmin
Summary and suggestion
Acknowledgments
References
Part 2: Gas Phase
6
Gas phase
Introduction
Diffusion of deuterium through palladium
Fralick
Biberian
Li
Iwamura
Piantelli
Brillouin
Loading of hydrogen and deuterium in nanoparticles
Aratas double cathode
NEDO
Leslie case catalyst
Mizuno
Conclusion
References
7
Electrically induced anomalous thermal phenomena in nanostructured wires
Historical background
Gas-phase experiments
Experiments with nickel alloys
Introducing iron
Observation of thermionic-like behavior
Effect of gas mixtures
Recent improvements in reactor design and AHE control
Conclusions
Acknowledgments
References
8
Experimental procedures for excess heat generation from cold fusion reactions
Air-flow calorimetry
Introduction
Insulated box
Blower
Measurement and data acquisition
Relationship between blower input and airflow velocity
Relationship between blower input and air outlet temperature
Method 1: Plasma deposition
Introduction
Reactor
Reactants
Activation
Plasma deposition process
Plasma discharge description
Excess heat generation
Details of excess heat generation tests with various gas pressure, input power, and output/input ratios
Control of reactor temperature and variation of the output/input ratio
Control of gas pressure
Change in temperature settings of reactor and internal heater
Input time indication of output/input ratio change
Excess heat example
Method 2: Direct deposition
Introduction
Material
Results
Temperature dependence for excesses heat generation
Summary
Acknowledgments
References
9
Heat generation experiments using nano-sized metal composite and hydrogen gas
Introduction
Experiment
Results and discussion
Concluding remarks
Acknowledgment
References
10
Screening energy for low energy nuclear reactions in condensed matter
Introduction
Screening energy and nuclear reaction cross section
Experimental procedure
Screening energy for d+d reaction in metals
Screening energy for Li+d reaction in solid and liquid metal Li
Temperature dependence of Us in liquid Li
CCM of d+d reaction induced by molecular beam
Summary
References
Part 3: Transmutations
11
Review of permeation-induced nuclear transmutation reactions
Introduction
Experimental method and results
Discussion
Concluding remarks
Acknowledgment
References
12
Effective LENR and transmutation of stable and radioactive isotopes in growing biological systems
Introduction
Biophysical aspects of transmutation process
Experiments on fusion and transmutation of stable isotopes in microbiological systems
Nuclear reactions with participation of light and middle mass isotopes in pure microbiological cultures
Transmutation of stable isotopes in microbe syntrophin associations
Experiments on transmutation of radioactive isotopes and reactor waste in microbiological systems
Experiments on utilization of the reactor Ba140 isotope by anaerobic syntrophic association
Experiments on accelerated deactivation and transmutation of long-lived reactor Cs137 isotope in growing anaerobic microbe ...
LENR experiments with radioactive Cs137 isotope and aerobic microbe syntrophic association
Physical foundation of biological transmutation
Conclusion
Acknowledgments
References
13
Transmutations and isotopic shifts in LENR experiments
Introduction and background
General remarks on experimental methodology
Patterson power cell and transmutation product measurements by Miley et al.
Lugano report and Parkhomov replications
Iwamuras deuterium gas permeation experiments
Glow discharge studies
Edward Eskos ``cool fusion´´
Carbon Arc experiments
Nano-dust fusion transmutation
Transmutation on an industrial scale
Biological transmutations
Alchemy: Myth or science?
Alchemical synthesis of silver from silicon (Peter Grandics)
Alchemical experiments at Texas A&M University
Activity patterns noted in European alchemical accounts
Indian alchemical texts
Concluding remarks
References
Part 4: Models and Theories
14
The basic nature of the cold fusion effect
Introduction
My involvement
Experimental studies
The nature of fusion
Hot fusion
Cold fusion
Model of the LENR process
Conclusion
Acknowledgments
References
15
Models based on phonon-nuclear coupling
Introduction
Phonon-nuclear coupling
Finite basis Hamiltonians
Phonon-mediated nuclear excitation transfer
Applications for phonon-mediated nuclear excitation transfer
Up-conversion and down-conversion
Applications for up-conversion and down-conversion
Subdivision and down-conversion
Other nuclear effects
Active sites
Conclusion
References
16
A study on electron deep orbits by quantum relativistic methods
Introduction
Interest of the electron deep orbits (EDOs) for the low-energy-nuclear reaction (LENR)
Starting point of our study
Arguments against the EDO states and possible solutions
The works of Maly and Vavra on ``DDLs´´
The anomalous solutions of the Dirac equation
The deep orbits, as solutions of the Dirac equation with a corrected potential for a nucleus of finite size
Ansatz used for finding the ``inside´´ solutions and continuity conditions
The question of orthogonality of the solutions, and the boundary conditions
Results obtained by computations of the DDL wave functions for modified potentials, further developments, and discussion
Computation process for orbital mean radii
Results obtained from parameters near those of Maly and Vavra
Varying the parameters
Some criticisms of the considered method of corrected potential, and attempts to correct discrepancies
The lack of dependence of the inside solutions on the nuclear charge potential, and the coherence of the values of energies
The discontinuity of the derivative of solutions
Question of the sign of the EDOs solutions
Involvement of special relativity in the EDOs
Comparing the relativistic and the nonrelativistic versions of the Schrödinger equation
Meaning of the term α2 appearing in the equation
Study of the magnetic interactions near the nucleus
Summary of the magnetic interactions near the nucleus
Interactions involving only the electron spin
Magnetic interactions involving the nuclear spin
Diamagnetic terms
The Vigier-Barut model
Works of Barut, as a source of the V-B model
Vigier-Barut model, and related works
Relativistic confinements and the question of the Heisenberg uncertainty relation (HUR)
Computation of the coefficient γ
The effective potential Veff is strong enough to confine electrons in deep orbits
Question about the stability of the EDOs
Potential energy terms for expecting a resonance. Seeking local energy minimum
Local energy minimum, with a relative weakening of near-nuclear interactions
Conclusions, question, and perspectives
Acknowledgment
References
17
Universal mechanism of LENR in physical and biological systems on the base of coherent correlated states of interacting pa ...
Introduction
Formalism and general regularities of CCS in LENR applications
Generation of ``giant´´ energy fluctuations and increase of barrier transparency
Anomalous features and the mechanism of LENR ``natural selection´´ based on CCS
Methods of CCS formation in realistic physical, biological, and geological systems
Formation of CCS for periodical modulation of harmonic oscillator parameters
Experiments on LENR stimulation at resonant action on the active medium
Features of CCS formation at a continuous change of parabolic potential well parameters
CCS formation at limited increase of parabolic potential well width
CCS formation at limited decrease of a width of parabolic potential well
Formation of CCS at pulse modulation of potential well parameters
The influence of damping and random force on CCS formation
Conclusions
References
Index
A
B
C
D
E
F
G
H
I
J
K
L
M
N
O
P
Q
R
S
T
V
W
X
Back Cover

Citation preview

Cold Fusion

Cold Fusion Advances in Condensed Matter Nuclear Science

Edited by

Jean-Paul Biberian Honorary Professor Department of Physics University of Aix-Marseille—Marseille France

Elsevier Radarweg 29, PO Box 211, 1000 AE Amsterdam, Netherlands The Boulevard, Langford Lane, Kidlington, Oxford OX5 1GB, United Kingdom 50 Hampshire Street, 5th Floor, Cambridge, MA 02139, United States © 2020 Elsevier Inc. All rights reserved. No part of this publication may be reproduced or transmitted in any form or by any means, electronic or mechanical, including photocopying, recording, or any information storage and retrieval system, without permission in writing from the publisher. Details on how to seek permission, further information about the Publisher’s permissions policies and our arrangements with organizations such as the Copyright Clearance Center and the Copyright Licensing Agency, can be found at our website: www.elsevier.com/permissions. This book and the individual contributions contained in it are protected under copyright by the Publisher (other than as may be noted herein). Notices Knowledge and best practice in this field are constantly changing. As new research and experience broaden our understanding, changes in research methods, professional practices, or medical treatment may become necessary. Practitioners and researchers must always rely on their own experience and knowledge in evaluating and using any information, methods, compounds, or experiments described herein. In using such information or methods they should be mindful of their own safety and the safety of others, including parties for whom they have a professional responsibility. To the fullest extent of the law, neither the Publisher nor the authors, contributors, or editors, assume any liability for any injury and/or damage to persons or property as a matter of products liability, negligence or otherwise, or from any use or operation of any methods, products, instructions, or ideas contained in the material herein. Library of Congress Cataloging-in-Publication Data A catalog record for this book is available from the Library of Congress British Library Cataloguing-in-Publication Data A catalogue record for this book is available from the British Library ISBN 978-0-12-815944-6

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This book is dedicated to Stanley Pons from the University of Utah, and the late Professor Martin Fleischmann from the University of Southampton. They are great scientists. They risked their careers and fame to announce their discovery of Cold Fusion, as it was known then. They are heroes who deserve our gratitude. They opened a new field in science, the Condensed Matter Nuclear Science, which changed the face of not only science, but in the future, it may change our entire technological civilization. This planet is in great danger because of climate change, the energy supply, and a lack of clean water; and this new science will be part of the solution. This book is also dedicated to the hundreds of scientists, engineers, self-made men and women from all over the world who have spent their time, effort, and money to replicate, study, improve, and commercialize this discovery.

Contributors Jean-Paul Biberian Honorary Professor, Department of Physics, University of Aix-Marseille—Marseille, France Francesco Celani ISCMNS_L1, Ferentino; INFN-LNF, Frascati, Italy K. Fang School of Nuclear Science and Technology, Lanzhou University, Lanzhou, PR China L.P. Forsley Global Energy Corporation, Annandale, VA, United States Peter L. Hagelstein Massachusetts Institute of Technology, Cambridge, MA, United States Y. Honda Research Center for Electron Photon Science, Tohoku University, Sendai, Japan Yasuhiro Iwamura Condensed Matter Nuclear Reaction Division, Research Center for Electron Photon Science, Tohoku University, Sendai, Japan J. Kasagi Research Center for Electron Photon Science, Tohoku University, Sendai, Japan Alla Kornilova Moscow State University, Moscow, Russia Cesare Lorenzetti ISCMNS_L1, Ferentino, Italy Michael C.H. McKubre Energy Research Center, SRI International, Menlo Park, CA, United States A. Meulenberg Science for Humanity Trust, Inc., Tucker, GA, United States Melvin H. Miles College of Science and Technology, Dixie State University, St. George, UT, United States Tadahiko Mizuno Hydrogen Engineering Application & Development Company, Sapporo, Japan P.A. Mosier-Boss Global Energy Corporation, Annandale, VA, United States Hiroo Numata Graduate School of Metallurgy and Ceramics Science, Tokyo Institute of Technology, Tokyo, Japan J.L. Paillet Aix-Marseille University, Marseille, PACA, France

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Contributors

K.P. Rajeev Department of Physics, IIT Kanpur, Kanpur, India Jed Rothwell LENR-CANR.org, Chamblee, GA, United States Mahadeva Srinivasan Bhabha Atomic Research Centre (BARC), Mumbai, India Edmund Storms Kiva Laboratory, Santa Fe, NM, United States Vladimir Vysotskii Kiev National Shevchenko University, Kiev, Ukraine M.V. Vysotskyy Kiev National Shevchenko University, Kiev, Ukraine

Preface On March 23, 1989, Professors Stanley Pons from the University of Utah and Martin Fleischmann from the University of Southampton announced during a press conference that they had achieved nuclear reactions in a test tube. Immediately, all around the world scientists tried to replicate this incredible discovery. Many failed, but a few succeeded. At the same time, unanimously almost all theoreticians declared that it was impossible to achieve nuclear fusion at room temperature. A few theoreticians such as Nobel laureate Julian Schwinger proposed models to try to explain the impossible reaction. Nevertheless, in spite of experimental successes, the field was very quickly almost banned from official science everywhere on earth, although many peer-reviewed papers were published initially. However, a number of scientists, both experimentalists and theoreticians, kept working under difficult conditions, either in their own institutions or in private laboratories, with limited funding. In spite of these very difficult circumstances they did not stop working and developing both the science and the technology. Thirty years after the announcement, even though hundreds of scientific papers were published in peer-reviewed journals in the 1990s, the field is still banned from official science. A community of enthusiast scientists managed to organize themselves. They put together international conferences (International Conferences on Cold Fusion) that attracted hundreds of people. They have also organized local meetings in Europe, Russia, Japan, and the United States. In order to have a scientific nexus, and to get together, they have also created a society, the International Society of Condensed Matter Nuclear Science. This society not only provides information about the subject, but has also a peer-reviewed journal, the “Journal of Condensed Matter Nuclear Science” where close to 400 papers have been published in the past 11 years. This book is a review of the work accomplished by some of these pioneers. There are experimental chapters, and also theoretical ones. It is our hope that the main scientific community will discover or rediscover this important field of science. Only a few of the large number of scientists currently working in this field have a chapter in this book. Those who have not been selected deserve our recognition for what they have accomplished. I thank all the authors who have contributed to this book. I also want to thank Jed Rothwell for checking the English of the authors whose mother tongue is not English. This includes me. Nuclear reactions in condensed matter will open amazing possibilities for a new source of energy. This breakthrough will have an impact on our lives and the lives of coming generations. Once the technology is developed, energy will be accessible everywhere on our planet. We hope that this discovery will help bring peace to the world by removing the need for wars to access energy resources. This book is divided into four sections. The first one is dedicated to electrochemistry. Fleischmann and Pons discovered the effect thanks to their ability to develop a simple and powerful calorimeter which was extremely sensitive and precise. Without that device they would not have been capable of making their discovery. The second section shows that the anomalous effect can also be observed in gas phase, that is, in hydrogen or deuterium atmospheres. This is very important because in order to transform heat into electricity the higher the heat source, the better the conversion efficiency. The third section relates to transmutations. This effect was not discovered at first, but chemical and isotopic analysis soon showed that new elements were formed, and that the isotopic distribution of others was anomalous. This discovery triggered interest in another discovery that two centuries of old science

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completely ignored: biological transmutations. New experiments have shown that biology is not only doing chemistry, but also nuclear reactions. The last section concerns models and theories. Our present theories on nuclear reactions are based on two body reactions. In the case of Condensed Matter Nuclear Science, we are in a multibody situation. In the past, no research in that direction was made. From day 1, some theoreticians, instead of saying that cold fusion was impossible, tried to find ways to resolve the impossible. There is still a lot to do, but ideas are on the table and when a valid theory is found, it will help improve the experimental work. Jean-Paul Biberian

CHAPTER

Production of helium in cold fusion experiments

1 Melvin H. Miles

College of Science and Technology, Dixie State University, St. George, UT, United States

Introduction Research on cold fusion at the China Lake Navy laboratory (Naval Air Warfare Center Weapons Division, NAWCWD) began on the first weekend following the announcement on March 23, 1989 by Martin Fleischman and Stanley Pons. It was 6 months later (September 1989) before our group detected any sign of excess heat production. By then, research reports from CalTech, MIT, and Harwell had given cold fusion a triple whammy of rejection. Scientists often resorted to ridicule to discredit cold fusion, and some were even saying that Fleischmann and Pons had committed scientific fraud. Most palladium (Pd) sources do not produce any cold fusion effects [1]. The Pd made by JohnsonMatthey (J-M) under special conditions specified by Fleischmann was not made available until later in 1989. I was likely one of the first recipients of this special Pd material when I received my purchase from Johnson-Matthey of a 6-mm-diameter Pd rod in September 1989. Our first reports of excess heat came from repeated use of the same two sections of this J-M palladium (J-M Pd) rod [1–3]. However, our final conclusions about our first excess heat results came late in 1989, thus China Lake was listed with CalTech, MIT, Harwell, and other groups reporting no excess heat effects in the November 1989 DOE-ERAB report [4]. These same two J-M Pd rods were later used in our first set of experiments (1990) showing helium-4 (He-4) production correlated with our excess heat (enthalpy) results [5–7]. Two later sets of experiments at China Lake using more accurate helium measurements, including the use of metal flasks for gas samples, confirmed our first set of measurements [8]. Following our initial research in 1990–91 on correlated heat and He-4 production, other cold fusion research groups reported evidence for He-4 production [9]. This report, however, will focus mainly on the research of the author at NAWCWD in China Lake, California, during the years 1990–95 [1, 8].

First set of heat and helium measurements (1990) The proponents of cold fusion were being largely drowned out by cold fusion critics by 1990. In fact, the first International Cold Fusion Conference (ICCF-1) was held from March 28 to 31, 1990 in Salt Lake City, Utah. I found this to be a very unusual scientific conference with a mix of cold fusion Cold Fusion. https://doi.org/10.1016/B978-0-12-815944-6.00001-4 # 2020 Elsevier Inc. All rights reserved.

3

4

Chapter 1 Production of helium in cold fusion experiments

proponents, many critics, and the press. Most presentations were followed by unscientific ridicule by critics in the question period with comments such as “All this sounds like something from Alice in Wonderland.” Two valid questions by critics, however, were: “Where are the neutrons?” and “Where is the Ash?” If the cold fusion reactions were the same as hot fusion reactions, as most critics erroneously thought, then the amounts of excess power being reported (0.1–5 W) would have produced a deadly number of neutrons (>1010 n/s). Furthermore, if there were a fusion reaction in the palladium-deuterium (Pd-D) system, then there should appear a fusion product—sometimes incorrectly referred to as ash. Some researchers, such as Bockris and Storms, were reporting tritium as a product, but the amounts were far too small to explain the excess enthalpy. The reported production of neutrons in cold fusion experiments was even smaller (about 10
7 of the tritium). Julian Schwinger, a Nobel laureate, suggested at ICCF-1 the possibility of a D + H fusion reaction that produces only helium-3 (He-3) as a product and no neutrons or radiation [10]. Because of this, I considered measurements for He-3 in my next experiments, but the mass spectrometer at China Lake was designed for only larger molecules made by organic chemists. However, later in 1990, Ben Bush called to discuss both a possible temporary position at China Lake and my cold fusion results. He held a temporary position at the University of Texas in Austin, and the instrument there could measure He-3 in small quantities. We worked out details in following telephone conversations about how to collect gas samples of the electrolysis gases and ship them to Texas for both He-3 and He-4 measurements by their mass spectrometry expert. My next two experiments, fortunately, produced unusually large excess power effects for our first set of correlated heat and helium measurements [5–7]. These helium results were first published as a preliminary note [5], then in the ICCF-2 Proceedings [6], and eventually as a detailed publication [7]. There was no detectable He-3, but there was evidence for He-4 correlated with the excess enthalpy. I had never met Ben Bush and decided to code the gas samples with the birthdays of my family members. My own measurements of excess power were recorded in permanent laboratory notebooks before the samples were sent to Texas for analysis. These were single-blind tests because Dr. Bush did not know how much, if any, excess power was being produced when an electrolysis gas sample was collected. I am glad, in retrospect, that this was done because I later learned that Dr. Bush was gung ho on proving cold fusion was correct. Scientists must always leave it completely up to experimental results to answer important scientific questions. It seemed to me, on the other hand, that scientists at MIT and CalTech in 1989 were focused only on proving that cold fusion was wrong. There was a “Wake for Cold Fusion” held at MIT at 4 p.m. on June 16, 1989a even before their cold fusion experiments were completed [11]. When all results for this first helium study were completed early in 1991, I thought about how this research could be published quickly as a preliminary note. All research, except for the helium measurements, was done at China Lake. However, critics of cold fusion were prominent in 1991, and any publication from China Lake had to be first cleared by several management levels. This publication could be held up or even rejected for publication by the Navy personnel at China Lake. As a solution, I had this manuscript submitted by Bush and Lagowski at the University of Texas at Austin, Texas where they were listed as the first authors. A few months later, Dr. Ronald L. Derr, Head of the Research Department at China Lake, admonished me for the publication of this work from China Lake in this

a

The flyer for this “Wake” at MIT ridiculed cold fusion with statements like “Black Armbands Optional” and “Sponsored by the Center for Contrived Fantasies.”

Analysis of the first set of helium measurements

5

manner. However, Dr. Derr, along with my Branch Head, Dr. Richard A. Hollins, were among the few supporters of my cold fusion research at NAWCWD in 1991. Many others thought that such work damaged the reputation of this Navy laboratory.

Analysis of the first set of helium measurements Neither Ben Bush nor I really knew how much helium should be produced in my experiments by a fusion reaction, but my quick calculations showed that it might be quite small because of its dilution by the D2 and O2 gases produced by the electrolysis gases. Recently, I have found an easier and accurate method to calculate the amount of He-4 theoretically expected from the experimental measurements of excess power. Theoretically, the fusion of deuterons to form He-4 produces 2.6173712  1011 He-4 atoms per second per watt of excess power. This is based on the fact that each D + D fusion event produces 23.846478 MeV of energy per helium atom from Einstein’s Eq. E ¼ Δmc2. Multiplying the number of atoms per second per watt by the experimental excess power in watts gives the theoretical rate of He-4 production in atoms per second. The rate of electrolysis gases generated (D2 + O2) per second is given by Molecules=s ¼ ð0:75 I=FÞ NA

(1)

where I is the cell current in Amps, F is the Faraday constant, and NA is Avogadro’s number. Note that the electrolysis reaction for one Faraday written as 0.5 D2O ! 0.5 D2 + 0.25 O2 produces 0.75 mol of D2 + O2 gases. The largest excess power in the first set of He-4 measurements was 0.52 W at a cell current of 0.660 A. Therefore, the theoretical rate of He-4 production divided by the rate of D2 + O2 molecules produced by electrolysis gives a ratio (R) for He-4 atoms to D2 + O2 molecules as shown by the following equation: R¼


2:617  1011 He-4 atoms=s W ð0:52 WÞ
½ð0:75Þ ð0:660AÞ=ð96, 485A s=molÞ 6:022  1023 D2 + O2 molecules=mol

(2)

This calculation yields R ¼ 44.1  10
9 or 44.1 parts per billion (ppb) of He-4 atoms. This is the theoretical concentration of He-4 present in electrolysis gases for this experiment if no He-4 remains trapped in Pd. and if no other significant fusion reactions occur. Normally, about half of this theoretical amounts of He-4 is experimentally measured in electrolysis gas. By combining the various constants in Eq. (2), a simpler expression (Eq. 3) is obtained that gives He-4 directly: He-4 ðppbÞ ¼ 55:91 ðPX =I Þ

(3)

where PX is the excess power in watts and I is the cell current in Amps. The first set (1990) of our China Lake results are shown in Table 1. The theoretical amount of He-4 expected (ppb) based on the measured excess power and the cell current is also listed. This is compared with the 1990 mass spectrometry results from the University of Texas in terms of large, medium, small, or no observed He-4 peaks. The dates for the gas sample collections are also listed. Two similar calorimeters (A,B) were run simultaneously, in series, in the same water bath controlled to 0.01 °C [1–3].

6

Chapter 1 Production of helium in cold fusion experiments

Table 1 Results for the 1990 China Lake experiments. Sample 12/14/90-A 10/21/90-B 12/17/90-A 11/25/90-B 11/20/90-A 11/27/90-A 10/30/90-B 10/30/90-A 10/17/90-A 12/17//90-B

PX (W) b

0.52 0.46 0.40 0.36 0.24 0.22 0.17 0.14 0.07 0.29c

Theoretical He-4 (ppb)a

Measured He-4

44.1 48.7 42.4 38.1 25.4 23.3 18.0 14.8 7.4 30.7c

Large peak Large peak Medium peak Large peak Medium peak Large peak Small peak Small peak No peak No peak

a

The University of Texas Detection Limit was about 5 ppb He-4 based on Table 1. I ¼ 0.660 A. For all others I ¼ 0.528 A. Calorimetric error due to low D2O solution level.

b c

The theoretical He-4 amounts generally follow the peak size reported experimentally for He-4 except for the one sample where there was an apparent calorimetric error. The simple exchange of the first medium peak with the last large peak would give perfect agreement. Perhaps a simple mix-up of two gas samples in 1990 for the He-4 measurements was all that prevented perfect agreement. Also, theoretical amounts of He-4 vary only by a factor of three between the large and small peaks. Previous estimates [6–8] of the number of He-4 atoms in these flasks were in error because the rate of helium production is directly proportional to the excess power. Finally, the detection limit for He-4 measured at the University of Texas was about 5 ppb based on Table 1. This is in line with the 1.1 ppb experimental error reported later by the US Bureau of Mines laboratory in Amarillo, Texas [8]. The rate for atmospheric helium diffusing into these glass flasks was later measured to be 0.18 ppb/day. Thus 28 days of flask storage would be needed to reach the 5 ppb detection limit. No correlation was found for the He-4 amounts and the flask storage times [6, 7]. Six control experiments using the same glass flasks and H2O + LiOH electrolysis produced no excess enthalpy at China Lake and no He-4 was measured at the University of Texas [5–8]. In less than 2 years from the Fleischmann and Pons 1989 cold fusion announcement, our research had shown that He-4 was the major cold fusion product. However, most of the scientific world no longer had interest in cold fusion and our 1990–1991 heat and He-4 correlations were mostly ignored. Secondary experiments were also conducted for these heat-production cells. Dental films within the calorimeter was used to test for any ionizing radiation, and gold and indium foils were used to test for any activation due to neutrons. These dental films were clearly exposed by radiation in both calorimetric cells A and B [6, 7]. A nearby Geiger counter also recorded unusually high activity during this time period. No activation of the gold or indium foils were observed; hence, the average neutron flux was estimated to be 10 MeV alpha particles by CR-39 [16, 31]. The source of these “long-range alpha” particles is ternary or quaternary fission [59].

Conclusions The Pd/D co-deposition technique has proven to be a very reproducible means of initiating nuclear events inside the palladium lattice. Furthermore, the structure of the Pd lattice created as a result of Pd/D co-deposition facilitates these nuclear reactions. The resultant deposit has a high surface

References

33

area. Potential reagents for these reactions are D, Pd, Li, T, and H as well as trace amounts of other metals that provide nucleation sites that give rise to defects as well as physical and electronic vacancies within the lattice [60]. The products observed indicate that several varieties of nuclear reactions are occurring. These include primary and secondary fusion reactions to produce neutrons, protons, tritium, and
10 MeV protons and neutrons. There is evidence of transmutation as shown by the production of Ag that can arise from either proton (
10 MeV) or neutron capture by Pd. The observation of long-range alpha particles indicates the occurrence of ternary and quaternary fission of Pd that is supported by the presence of such elements as Fe, Cr, Ni, and Al with a corresponding decrease in Pd. The nature of the reaction responsible for the loss of thermal tritium when highly tritiated D2O is used in these experiments is not understood. This loss of tritium is not observed when bulk Pd is used instead of Pd/D co-deposition. This suggests that the reaction involved with the consumption of thermal tritium is related to the high surface area of the Pd deposit and/or the vacancies present in the lattice. These vacancies allow more than two deuterons to occupy a site in the Pd lattice [61].

Acknowledgments The authors acknowledge the contributions of Stan Szpak for initially developing the Pd/D co-deposition technique. They are grateful for the support of Frank Gordon which allowed Stan Szpak and the authors to conduct their research at the Navy laboratory. They are thankful for the support of Dr. Jay Khim of JWK Corporation. Finally, the authors acknowledge all the researchers who have conducted Pd/D co-deposition experiments as their findings not only corroborated our results, but also provided additional data to elucidate the nature of the reactions occurring inside the Pd lattice.

References [1] S. Szpak, P.A. Mosier-Boss, S.R. Scharber, J.J. Smith, Charging of the Pd/nH system: role of the interphase, J. Electroanal. Chem. 337 (1992) 147–163. [2] S. Szpak, P.A. Mosier-Boss, S.R. Scharber, J.J. Smith, Cyclic voltammetry of Pd+ D codeposition, J. Electroanal. Chem. 380 (1995) 1–6. [3] S. Szpak, P.A. Mosier-Boss, J.J. Smith, Deuterium uptake during Pd-D codeposition, J. Electroanal. Chem. 379 (1994) 121–127. [4] S. Szpak, P.A. Mosier-Boss, J.J. Smith, On the behavior of the cathodically polarized Pd/D system: a response to Vigier’s comments, Phys. Lett. A 221 (1996) 141–143. [5] P.A. Mosier-Boss, S. Szpak, The Pd/nH system: transport processes and development of thermal instabilities, Nuovo Cimento Societa` Italiana di Fisica A 112 (1999) 577–586. [6] S. Szpak, P.A. Mosier-Boss, M.H. Miles, M. Fleischmann, Thermal behavior of polarized Pd/D electrodes prepared by co-deposition, Thermochim. Acta 410 (2004) 101–107. [7] S. Szpak, P.A. Mosier-Boss, R.D. Boss, On the behavior of the Pd/D system: evidence for tritium production, Fusion Sci. Technol. 33 (1998) 38–51. [8] S. Szpak, P.A. Mosier-Boss, J.J. Smith, On the behavior of the cathodically polarized Pd/D system: search for emanating radiation, Phys. Lett. A 210 (1996) 382–390. [9] S. Szpak, P.A. Mosier-Boss, C. Young, F.E. Gordon, Evidence of nuclear reactions in the Pd lattice, Naturwissenschaften 92 (2005) 394–397. [10] P.A. Mosier-Boss, It is not low energy – but it is nuclear, J. Condens. Matter Nucl. Sci. 13 (2014) 432–442.

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[11] S. Szpak, P.A. Mosier-Boss, F.E. Gordon, Further evidence of nuclear reactions in the Pd/D lattice: emission of charged particles, Naturwissenschaften 94 (2007) 511–514. [12] P.A. Mosier-Boss, S. Szpak, F.E. Gordon, L.P.G. Forsley, Use of CR-39 in Pd/D co-deposition experiments, Eur. Phys. J. Appl. Phys. 40 (2007) 293–303. [13] P.A. Mosier-Boss, S. Szpak, F.E. Gordon, L.P.G. Forsley, Characterization of tracks in CR-39 detectors obtained as a result of Pd/D co-deposition, Eur. Phys. J. Appl. Phys. 46 (2009) 30901. [14] P.A. Mosier-Boss, S. Szpak, F.E. Gordon, L.P.G. Forsley, Triple tracks in CR-39 as the result of Pd-D codeposition: evidence of energetic neutrons, Naturwissenschaften 96 (2009) 135–142. [15] P.A. Mosier-Boss, J.Y. Dea, L.P.G. Forsley, M.S. Morey, J.R. Tinsley, J.P. Hurley, F.E. Gordon, Comparison of Pd/D co-deposition and DT neutron generated triple tracks observed in CR-39 detectors, Eur. Phys. J. Appl. Phys. 51 (2010) 20901. [16] P.A. Mosier-Boss, F.E. Gordon, L.P.G. Forsley, D. Zhou, Detection of high energy particles using CR-39 detectors part 1: results of microscopic examination, scanning, and LET analysis, Int. J. Hydrogen Energy 42 (2017) 416–428. [17] S. Szpak, P.A. Mosier-Boss, M.H. Miles, Calorimetry of Pd + D co-deposition, Fusion Sci. Technol. 36 (1999) 234–241. [18] M.H. Miles, NEDO final report – Electrochemical calorimetric studies of palladium and palladium alloys in heavy water, University of La Verne, 2004. [19] M.H. Miles, B.F. Bush, K.B. Johnson, Anomalous effects in deuterated systems – final report, Naval Air Warfare Center Weapons Division, 1996. NAWCWPNS TP 8302. [20] D.J. Cravens, D.G. Letts, Practical techniques in CF research – triggering methods, in: Proceedings of the Tenth International Conference on Condensed Matter Nuclear Science, Cambridge, MA, 2003. [21] D. Letts, Codeposition methods: a search for enabling factors, J. Condens. Matter Nucl. Sci. 4 (2011) 81–92. [22] D. Letts, P.L. Hagelstein, Modified Szpak protocol for excess heat, J. Condens. Matter Nucl. Sci. 6 (2012) 44–54. [23] L.F. Dechario, L.P. Forsley, P.A. Mosier-Boss, K.J. Long, P. Rayms-Keller, S. Barker, M. Shea, B.M. Steinetz, T.L. Benyo, D.L. Ellis, I. Locci, W.D. Jennings, R.C. Hendricks, A Multi-Laboratory Study of Anomalous Elements and Magnetic Field Effects in LENR Codeposition Experiments, Naval Surface Warfare Center, Dahlgren, VA, 2019 (in review). [24] J. Dash, A. Ambadkar, Co-deposition of palladium with hydrogen isotopes, in: Proceedings of the Eleventh International Conference on Condensed Matter Nuclear Science, Marseille, France, 2004. [25] M. Swartz, G. Verner, Excess heat from low electrical conductivity heavy water spiral-wound Pd/D2O/Pt and Pd/D2O-PdCl2/Pt devices, in: Proceedings of the Tenth International Conference on Condensed Matter Nuclear Science, Cambridge, MA, 2003. [26] M. Swartz, Excess power gain using high impedance and codepositional LANR devices monitored by calorimetry, heat flow, and paired Stirling engines, in: Proceedings of the Fourteenth International Conference on Condensed Matter Nuclear Science, Washington, DC, 2008. [27] F.L. Tanzella, J. Bao, M.C.H. McKubre, Cryogenic calorimetry of “exploding” PdDx wires, J. Condens. Matter Nucl. Sci. 6 (2012) 90–100. [28] F. Tanzella, J. Bao, M. McKubre, P. Hagelstein, Stimulation of metal deuteride wires at cryogenic temperatures, J. Condens. Matter Nucl. Sci. 8 (2012) 176–186. [29] J.O.’.M. Bockris, C.-C. Chien, D. Hodko, Z. Minevski, Tritium and helium production in palladium electrodes and the fugacity of deuterium therein, in: Proceedings of the Third International Conference on Condensed Matter Nuclear Science, Nagoya, Japan, 1992. [30] K.-H. Lee, H. Jang, S.-J. Kim, A change of tritium content in D2O solutions during Pd/D co-deposition, J. Condens. Matter Nucl. Sci. 13 (2014) 294–298. [31] A.S. Roussetski, A.G. Lipson, E.I. Saunin, F. Tanzella, M. McKubre, Detection of high energy particles using CR-39 detectors part 2: results of in-depth destructive etching analysis, Int. J. Hydrogen Energy 42 (2017) 429–436.

References

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[32] P.J. Smith, R.C. Hendricks, B.M. Steinetz, Bubble Detector Neutron Dosimeter Measurements During Electrolytic Co-deposition, NASA John H. Glenn Research Center, Cleveland, OH, 2019 (in review). [33] N. Robertson, H. Saito, J. Yurkovic, S. Zakskorn, Field assisted electroplating, J. Sci. Expl. 23 (2009) 452–455. [34] P.A. Mosier-Boss, L.P. Forsley, Energetic particle emission in Pd/D co-deposition: an undergraduate research project to replicate a new scientific phenomenon, J. Lab. Chem. Educ. 6 (2018) 69–76. [35] M. Karahadian, H.M. Doss, Evidence of particles during electrochemical Pd-D co-deposition, in: American Physical Society Meeting, Boston, MA, 2019. [36] S. Szpak, P.A. Mosier-Boss, J.J. Smith, On the behavior of Pd deposited in the presence of evolving deuterium, J. Electroanal. Chem. 302 (1991) 255–260. [37] P.A. Mosier-Boss, J.Y. Dea, F.E. Gordon, L.P.G. Forsley, M.H. Miles, Review of twenty years of LENR research using Pd/D co-deposition, J. Condens. Matter Nucl. Sci. 4 (2011) 173–187. [38] G. Guisbiers, G. Abudukelimu, D. Hourlier, Size-dependent catalytic and melting properties of platinumpalladium nanoparticles, Nanoscale Res. Lett. 6 (2011) 396. [39] S. Szpak, P.A. Mosier-Boss, C. Young, F.E. Gordon, The effect of an external electric field on surface morphology of co-deposited Pd/D films, J. Electroanal. Chem. 580 (2005) 284–290. [40] M.E. Shaheen, J.E. Gagnon, B.J. Fryer, Laser ablation of iron: a comparison between femtosecond and picosecond laser pulses, J. Appl. Phys. 114 (2013) 083110. [41] D.J. Nagel, Characteristics and energetics of craters in LENR experimental materials, J. Condens. Matter Nucl. Sci. 10 (2013) 1–14. [42] Y.E. Kim, Conventional nuclear theory of low-energy nuclear reactions in metals: alternative approach to clean fusion energy generation, J. Condens. Matter Nucl. Sci. 13 (2014) 264–276. [43] M.H. Miles, M. Fleischmann, Measurements of excess power effects in Pd/D2O systems using a new isoperibolic calorimeter, J. Condens. Matter Nucl. Sci. 4 (2011) 45–55. [44] M.H. Miles, Investigations of possible shuttle reactions in co-deposition systems, J. Condens. Matter Nucl. Sci. 8 (2012) 12–22. [45] M.R. Swartz, Impact of an applied magnetic field on a high impedance dual anode LANR device, J. Condens. Matter Nucl. Sci. 4 (2011) 93–105. [46] P.A. Mosier-Boss, L.P. Forsley, F.E. Gordon, D. Letts, D. Cravens, M.H. Miles, M. Swartz, J. Dash, F. Tanzella, P. Hagelstein, M. McKubre, J. Bao, Condensed matter nuclear reaction products observed in Pd/D co-deposition experiments, Curr. Sci. 108 (2015) 656–659. [47] B.G. Cartwright, E.K. Shirk, P.B. Price, A nuclear-track recording polymer of unique sensitivity and resolution, Nucl. Instrum. Meth. Phys. 153 (1978) 457–460. [48] R.A. Oriani, J.C. Fisher, Generation of nuclear tracks during electrolysis, Jpn. J. Appl. Phys. 41 (2002) 6180–6183. [49] A.G. Lipson, A.S. Roussetski, G.H. Miley, E.I. Saunin, Phenomenon of an energetic charged particle emission from hydrogen/deuterium loaded metals, in: Proceedings of the Tenth International Conference on Condensed Matter Nuclear Science, Cambridge, MA, 2003. [50] A.G. Lipson, A.S. Roussetski, G.H. Miley, C.H. Castano, In-situ charged particles and x-ray detection in Pd thin film-cathodes during electrolysis in Li2SO4/H2O, in: The Proceedings of the Ninth International Conference on Condensed Matter Nuclear Science, Beijing, China, 2002. n )3α reaction at 14.4 MeV in a kinematically com[51] B. Antolkovic, Z. Dolenec, The neutron-induced 12C(n,  plete experiment, Nucl. Phys. A 237 (1975) 235–252. [52] S.K. Murali, B.B. Cipiti, J.F. Santarius, G.L. Kulcinski, Study of fusion regimes in an inertial electrostatic confinement device using the new eclipse disk diagnostic, Phys. Plasmas 13 (2006) 053111. [53] P.A. Mosier-Boss, L.P. Forsley, P.J. McDaniel, Investigation of nano-nuclear reactions in condensed matter – final report, Defense Threat Reduction Agency, 2016. [54] Ş. Turhan, A. Zararsiz, H. Y€ucel, Sample geometry and efficiency determination of bremsstrahlung radiation of 90Sr on gamma detection systems, J. Radioanal. Nucl. Chem. 269 (2006) 141–145.

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[55] F. Ditro´i, F. Ta´rka´nyi, S. Taka´cs, I. Mahunka, J. Csikai, A. Hermanne, M.S. Uddin, M. Hagiwara, M. Baba, T. Ido, Y. Shubin, A.I. Dityuk, Measurement of activation cross sections of the proton induced nuclear reactions on palladium, J. Radioanal. Nucl. Chem. 272 (2007) 231–235. [56] H. Bi-Tao, P.P. Zarubin, U.U. Juravlev, 106,110Pd(p,nγ)106,110Ag reactions at Ep ¼ 6.0–7.7 MeV, Chin. Phys. 16 (2007) 989–993. [57] Introduction to Energy Dispersive X-Ray Spectrometry (EDS), https://cfamm.ucr.edu/documents/eds-intro. pdf. Accessed 19 February 2019. [58] G. Miley, P.J. Shrestha, Review of transmutation reactions in solids, in: Proceedings of the Tenth International Conference on Condensed Matter Nuclear Science, Cambridge, MA, 2003. [59] H. Semat, Introduction to Atomic and Nuclear Physics, fifth ed., Springer, 1972. [60] L.F. DeChiaro, L.P. Forsley, P. Mosier-Boss, Strained layer ferromagnetism in transition metals and its impact upon low energy nuclear reactions, J. Condens. Matter Nucl. Sci. 17 (2015) 1–26. [61] P.L. Hagelstein, I. Chaudhary, Arguments for dideuterium near monovacancies in PdD, in: Proceedings of the Fifteenth International Conference on Condensed Matter Nuclear Science, Rome, Italy, 2009.

CHAPTER

Electrochemical loading to produce the Fleischmann-Pons heat effect (FPHE)

3

Michael C.H. McKubrea Energy Research Center, SRI International, Menlo Park, CA, United States

Introduction My experience with PdH and PdD began when I joined SRI in 1978 to work on (amongst other things) developing an in situ (potentially in-core) hydrogen sensor for conventional fission reactor pressurized water systems (including CANDU, a heavy water reactor, hence studying PdD). I worked on this steadily for 11 years under funding from the Electric Power Research Institute (EPRI) managed by Tom Passell. By 1989, I considered myself as “an expert” on palladium hydrides (vainly as Martin Fleischmann began to study this system in 1947—before I was born!). I never found Martin’s intuition on this faulty although he freely admitted that the system was “very complex” (i.e., he did not know everything).

Variability Up until the time I began to set up “cold fusion” experiments, I had designed and run many hundreds of palladium-hydrogen and palladium-deuterium electrochemical experiments, although rarely were these identical. In 1989, I had no anticipation of the range of variability of result we would obtain from “nominally identical,” “well-performed” experiments using bulk Pd, D2O or H2O, and Li, “only” systems. At the outset of our investigation into the “new world” suggested by the Fleischmann-Pons announcement [1], we (the group at SRI) had extensive experience precisely with the Pd/D electrochemical system, had already developed a resistive technique and instrument to measure the uptake of H and D into Pd [2], and had achieved expert status in the field of electrochemical impedance spectroscopy [3], the tool probably best adapted to understanding (and thus controlling) the kinetics upof deposition and loading of H and D into Pd. At this point, a reasonable question might be: if you know what you need to do, why can’t you always do it? Why is there any degree of irreproducibility? a

Retired 2016.

Cold Fusion. https://doi.org/10.1016/B978-0-12-815944-6.00003-8 # 2020 Elsevier Inc. All rights reserved.

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Chapter 3 Electrochemical loading

The answer is straightforward: the material conditions of our experiments are not completely under our control. Electrochemistry takes place at an electrified interface between two “difficult” materials: a solid phase, bulk Pd; and a liquid phase, the electrolyte. Neither of these phases are fully under our control. The degree of this “lack of control” was certainly not obvious to us in 1989, and remains opaque to many in our field. Once this problem became apparent to us in the early days of studying the Fleischmann-Pons heat effect (FPHE) at SRI, experiments were designed to probe the parameters of reproducibility. Sets of 12 cells were prepared, intentionally identically, and operated simultaneously to monitor the time evolution of electrochemical and physicochemical parameters having the potential to be, pertinent to the FPHE. Single lengths of palladium wires were selected from known, well-characterized sources. These were sectioned into 13 identical lengths (12 active electrodes plus a reserved blank). These wire sections (typically 3 or 5 cm in length and 1 or 3 mm in diameter) were machined to remove surface damage and inclusions, spot welded with five contacts (one cathode current contact and four wires for axial resistance measurement). The prepared sections were then annealed, surface etched to remove surface contaminants and mounted in 12 identical cells of the type shown in Fig. 1. These processes all were performed in the same batch and by the same person. The 12 cells were filled with the electrolyte from a single source and then operated electrically in series, in a 3
4 matrix in the same constant temperature chamber. The variables measured continuously were current (one measurement), cell voltage, pseudoreference cathode potential, temperature, and axial electrical resistance to determine D/Pd loading, all measurements being monitored in a multiplexed manner with the same instruments. Intermittent measurements were made of the cathode interfacial impedance. With 12 intentionally identical experiments, every one behaved differently. Not only in terms of their heat production, significant and marked differences were observed in: the current-voltage-time profile for both the cell voltage and reference potential; the ability and willingness of each electrode to absorb deuterium measured by the resistance ratio-time curve; the maximum loading achievable; and the interfacial kinetic and mass transport processes reflected in the interfacial impedance. Every one of these parameters was importantly different for each of the 12 electrodes in every group tested. This set of experiments was repeated several times in an attempt to understand the origins of the irreproducibility, and therefore seek to control it. Trace impurity differences were observed to be contributory and these divided into two sets: deleterious impurities (poisons) that we learned to avoid; impurities that were beneficial to high loading in controlled amounts. This was a highly useful (and somewhat surprising) exercise. Although we were able to make progress and reduce the dispersion, we were not able to control the irreproducibility simply by electrochemical (and trace chemical) means in the electrolyte phase. This variability was found to have three principle sources: electrochemistry; surface structure; and bulk metallurgy.

Electrochemistry To obtain “useful” FPHE results from “the electrochemical insertion of D into Pd,” I continue to believe the evidence of my eyes that one must attain and maintain (for a time) high loading or more accurately high chemical potentials of D—at least in the near-surface region. In order to have high chemical potential of D in the near-surface region, one must have equal or greater chemical potential of D at the surface, the two-dimensional, electrified interface between the bulk electrolyte and bulk metal. The chemical potential of adsorbed D atoms in the interlayer (interface) is controlled in water

Variability

Hermetic 10pin connector Gasket

39

Gas tube containing catheter Screws Catalyst RTD

PTFE top plate Quartz liner

Recombination catalyst in Pt wire basket PTFE spray separator cone PTFE cap

Electrolyte PTFE liner Pd cathode

Stainless steel outer casing

Pt wire anode

Quartz anode cage PTFE base

FIG. 1 Electrochemical cell for loading and calorimetric studies.

by the rates of three well-studied electrochemical reactions and several parasitic reactions especially if CO2 is present in the (basic) electrolyte—as it always is. As Bockris showed so long ago these reactions are strongly influenced by even parts per trillion (ppt) concentrations of some impurities. At SRI, we spent several person-years studying beneficial and deleterious impurity effects down to ppm levels. As Martin would say this too is “complex” and very few if any of us have ever had impurity effects under control (except by swamping them with “more dirt”).

Surface structure The “curse” of Pd—and perhaps the reason for its success—is that D atoms on the surface (adsorbed) exchange freely and fast with D atoms in the bulk (absorbed). In this way, Pd as an element and in its alloys is truly unique—at least at low and intermediate temperatures. I continue to believe also that this

40

Chapter 3 Electrochemical loading

facility (or facileness) to allow a D flux to flow at very high rates across the interface (equivalent to 1–10 mA cm2 of D atom flow, or more) is crucial to the FPHE. There is no equilibrium in electrochemical loading of hydrogen isotopes into palladium. Instead, D atoms are being lost from surface to bulk, and returned to the surface from the bulk in what I have called an “exchange flux.” Attempting to “fill” Pd with D (or H and both isotopes are always present) is like filling a leaky bucket—or a leaky transmission line as sites on the surface, for example, emergent defects, grain boundaries, etc., bleed laboriously loaded D out, greatly affecting the interfacial state and thus electrochemical kinetics (there are also thermodynamic factors). This is a problem as the surface continuously transforms by deposition and selective dissolution thus changing the electrochemical interface with time. We have means of knowing a fair bit about interfacial kinetics, even in an active FPHE experiment, although few have ever used the available tools with good purpose. I did (this was my electrochemical background), and so has Vittorio Violante, and Martin Fleischmann was fascinated by the evidence gathered and their implications when I first presented him with results [4]. The interfacial electrochemical impedance is interestingly characteristic for active and preactive successful heat-producing FPHE experiments. This is a story for another day (after a lot more work) but structures that form adventitiously on Pd surfaces during electrolysis are, I believe, implicated (necessary but not sufficient) in promoting the effect itself.

Bulk metallurgy The same is true for the Pd(D) bulk. I do not believe that the FPHE is a property of PdDx, as we normally understand the phases of this material, for any value of the stoichiometry factor x. I believe that a new phase or structure of matter, or void or structure of voids in matter, must form to host the conditions needed for the FPHE. Subsurface changes must occur, possibly up to and including the surface, to create what Ed Storms [5] has designated as the nuclear-active environment (NAE). Without adequate and further studies, specifically experimental, we are left to conjecture rather loosely what the NAE is, how it forms, and how it works to create the FPHE. Ed Storms has one hypothesis that he explores and elucidates in his second book on this topic [6] but freely acknowledges that a lot more study and discussion is required. I explore another potential idea briefly in what follows here. However, whichever and whatever the NAE may be, if we are going to, or are forced to, rely on Pd as our host for NAE, and loading by electrochemistry as our means to create it, then we are going to need to know a lot more about PdD (PdH and possibly PdT) than we presently do. An alternative is that we avoid bulk Pd and electrochemistry entirely, or use these judiciously to create the NAE, and then employ other means to produce the FPHE. No suggested alternate procedures are offered here.

Progress Someone new to the field wanting to recreate the FPHE, or to maximize their chances of doing so, while pursuing the hypothesis that the effect can originate from “the electrochemical insertion of D into Pd” should pay close (I would argue closer) attention to the past (and to the present). Notable contributors worth closer attention include: Fleischmann and Pons themselves; Bockris in his LENR work and in his fundamental teachings (see Ref. [7]); Storms [5, 6] and Rothwell (via his online library and understanding of its contents); Cravens and Letts; the “Italians” Violante, La Gatta and Celani (and others); Miles and Szpak (et al.); the “theorists”: Preparata, Hagelstein, Takahashi et al.; Dardik & Energetics.

High reproducibility excess heat at SRI

41

Obviously, there are many others who have also contributed but the teachings of this set have in many cases been understudied and underappreciated. This criticism includes my group at SRI who needed painstakingly to relearn many of the lessons about loading deuterium into palladium. It was with some chagrin that we watched others re-relearn some of our learnings and teachings, sometimes repeatedly. Our meander forwards in understanding has been something of a random walk. For the moment, we will postpone discussion of three critical questions: 1. What is the purpose or role of deuterium loading in palladium? 2. How much loading is needed to produce the FPHE? 3. What else is needed to produce the effect? We will return to these questions later but for now let us examine the further questions: 4. What factors must be controlled to load deuterium electrochemically into palladium cathodes in aqueous electrolytic system? 5. What physical processes limit our ability to load D atoms; what is the limit on loading? Looking from the inside of the cathode out the physical parameters that first draw our attention are: •

•

• • •

The bulk-phase Pd metallurgy: grain size and orientation; impurities and impurity distribution; grain boundaries (width, composition, and permeability); and the presence of cracks, voids, and inclusions. The electrified metal-electrolyte interface: surface preparation, machining, acid dissolution, ion, or atom implantation; surface morphology and degree of polish; width and spacing of grain boundaries projected on the surface and depth of etching; and the presence of surface adsorbed impurities: catalysts, poisons, blocking species, etc. The electrolyte: the nature of the anion, cation; concentration, ionic strength; the effect of pH (pD); and minor dissolved additives. The anode: material; geometry; anode-cathode spacing; and anode-cathode separators. The electrochemical current: current density and current density distribution; current-time profile: dc, ramps, pulse, non-dc effects; and anodic reversal.

All of these factors are important as probably are several others unlisted. In the space available, we will not be able to cover more than a few and I will focus below on what has worked in the past in the group of our immediate collaboration: SRI, ENEA, Energetics, MIT.

High reproducibility excess heat at SRI In our work at SRI, we experienced three episodes of highly reproducible excess heat production. All very different experiments, all with better than 50% reproducibility of excess heat production, and all with very different protocols. For all three, the degree of loading was critical. These three sets were: 1. Fleischmann-Pons replication SRI cells P 12–22 [8]: thermodynamically closed, pressurized; 1 M LiOD (with additives); 3-mm diameter Engelhard Lot #1 Pd (with surface treatment); dc loading at “low” current density and stimulated at high (up to 0.9 A cm2); SRI mass-flow calorimetry; >3σ excess heat observation 93% (one blank and one aborted cell in the set of 16); >5σ excess heat observation 79%.

42

Chapter 3 Electrochemical loading

2. Energetics/ENEA replication cells ETI 35–61 [9] thermodynamically open but physically closed, unpressurized; 0.1 M LiOD (with additives); 50 μm ENEA Pd with surface treatment (one cathode in this set from ETI Omer, Israel); superwave current stimulation loading at “low” current density and stimulated at high (up to several A cm2 transiently); energetics heat flow calorimetry; >3σ excess heat observation 84% (one blank and three failed cells in the set of 23); >5σ excess heat observation 63%. 3. SRI “exploding wire” [10]: loading and sealing in thermodynamically open, unpressurized cells; 5
105 M SrSO4 (with Hg additive for hydrogen sealing); 50–250 μm diameter Pd wires; dc step current stimulation (to wire failure); SRI latent heat calorimetry; >3σ excess heat observation 70% (one failed test in the set of 46, blanks run previously); >5σ excess heat observation 50%. In the SRI work (and that of many others), D/Pd loading was inferred from measurements of the resistance ratio R/R°, where R° is the resistance of Pd absent D (or H). Much effort and many years were spent in the calibration of the functional relationship between D/Pd and R/R°. Our final publication on this topic describes our most recent thinking and calibration [11], but it should be recognized that R/R° is our proxy for loading. Fig. 2 shows various attempts to measure the resistance ratio vs loading functionality directly (blue curves), calibrate using laboratory and literature data (individual points) [11], and apply a polynomial fit [12]. Resistance measurement of loading contains interpretation ambiguities

1.9 1.8

H

D

SC-B.MM,FLT Table1

D/Pd

R/R° up

R/R° low

TCR(H)

TCR(D)

Resistance ratio (R/R°)

1.7 10 1.6 1.5 1.4 5 1.3 1.2

Temperature coefficient of resistance [K–1] 10–3

15

2

1.1 1

0 0

0.1

0.2

0.3

0.4

0.5

0.6

0.7

0.8

0.9

1

Atomic ratio (loading)

FIG. 2 Resistance ratio (R/R°) and temperature coefficient of resistance versus atomic ratio (H/Pd and D/Pd).

High reproducibility excess heat at SRI

43

associated with temperature and geometry effects (cathode shape change and loading heterogeneity, etc.) as well as the choice of calibration function. To compare loading at high values between experiments and laboratories, and while recognizing that the R itself has no (or little) fundamental significance in whatever process gives rise to excess heat, it is in many ways less ambiguous to discuss and compare the measured value of resistance ratio, R/R° on the right-hand side of the resistance maximum, rather than the derived variable D/Pd. For this reason when summarizing the SRI and ENEA results for protocols 1 and 2 above, we have chosen to reflect both variables, D/Pd and R/R° and the calibration function, as shown in Fig. 3. This graph plots the minimum measured value of R/R° (on the right side of the resistance maximum) vs inferred maximum loading (D/Pd) for 67 experiments carried out at SRI in various calorimeters and with various outcomes. Data points in green and yellow are those for which no excess heat was measured and fall exclusively in the upper left quadrant. Data points in red and orange (predominantly in the lower right quadrant) are those in which statistically significant (>3σ) excess heat was measured.

FIG. 3 Resistance ratio and derived loading values for 67 experiments of Pd cathodes in LiOD electrolytes; data points in the upper left quadrant displayed no excess heat; data points in the bottom right quadrant exhibited statistically significant (>3σ) excess heat or tritium production.

44

Chapter 3 Electrochemical loading

1200

All results—excess energy 1000

Excess energy (kJ)

800 y = 1660.7x – 1332.4 R² = 0.0837 600

400

200

0 0.88

0.90

0.92

0.94

0.96 0.98 Loading (D/Pd)

1.00

1.02

1.04

1.06

FIG. 4 Excess energy (kJ) vs maximum loading obtained (D/Pd).

The double meaning and color coding of excess heat caused one of our community considerable confusion at ICCF18 [13] but seems an efficient way to present the fact that cathodes that have at some point attained (and maintained for some period of time) R/R° 0.927, exhibit a high propensity for excess heat production. So much so that only one experiment, ETI 035-9, with R/R° of 1.385 and D/Pd of 0.972 “defies” the rule and produced no excess heat (although it did generate a significant amount of tritium [8]). This, however, is not a complete story. Fig. 4 plots the integral of excess power, that is, excess energy, vs D/Pd for all 67 experiments. The linear regression fit is unconvincing with the regression coefficient R2 ¼ 0.0837. Attention is drawn to two points: the green filled diamond (no excess heat) is ETI 035-9 discussed above; the red filled diamond (exhibiting large loading and large excess heat) is ETI 035-8, the “sister” experiment run simultaneously in an identical calorimeter using Violante (ENEA, Frascati) prepared foils. Such foils have relatively large surface area but small volume. If we normalize the excess energy by surface area, a slightly clearer picture emerges as shown in Fig. 5. The linear regression fit is worse (R2 ¼ 0.0351) and the data appear to have a roughly Gaussian distribution as suggested by the blue curve drawn using the statistical mean (D/Pd ¼ 0.944) and standard deviation (σ ¼ 0.020) of all results exhibiting positive energy excess.

High reproducibility excess heat at SRI

45

8

All results—excess energy/area 7

Excess energy density (MJ/cm2)

6

5

4

3

2

y = 4018.5x – 3215 R² = 0.0351

1

0 0.88

0.90

0.92

0.94

0.96

0.98

1.00

1.02

1.04

1.06

Loading (D/Pd)

FIG. 5 Excess energy density (MJ cm2) vs maximum loading obtained (D/Pd).

At the eighth International Workshop on Anomalies in Hydrogen/Deuterium Loaded Metals, October 2007 in Catania, Sicily, Paolo Tripodi presented reasoning and conclusions that few of us then accepted [14]. Representing HERA (Hydrogen Energy Research Agency based in Rome), Tripodi argued in support of a γ-phase in the PdD system that played a role in both the FPHE and in hightemperature superconductivity. Indirect experimental evidence for existence of a γ-phase was first reported by Tripodi, McKubre et al. [15] in 2000. In the related research, both SRI/Tripodi [16] and Lipson/Miley [17] pursued the notion and evidence that suitably prepared PdD (and PdH) were capable of facilitating an internal structure or “superstoichiometry” able to support an extreme level of high-temperature superconductivity; the γ-phase. From Tripodi [8], PdH and PdD systems exhibit the following phase structures using the hitherto unexpected rapid rise in the temperature coefficient of thermal conductivity shown in Fig. 2 to define the onset of the existence of the β- + γ-phase: α-phase in the stoichiometry range 0 < x < 0.05. α + β phases in the stoichiometry range 0.05 < x < 0.70. β-phase in the stoichiometry range 0.70 < x < 0.95. β + γ phases in the stoichiometry range x > 0.95.

46

Chapter 3 Electrochemical loading

Tripodi argued speculatively that high-temperature superconductivity was a characteristic of the γ-phase but that the excess enthalpy observed in the FPHE occurred only in the region of stoichiometry in which the β- and γ-phases coexist. Quoting Tripodi [14] (my emphasis): “To obtain excess heat in Cold Fusion we suggest to consider a stoichiometry window and not a stoichiometry threshold” and presented the following graphic. This was the first (and only) time I have heard this suggestion, which most of us dismissed as unreasonable, unconvincing, or uncomfortable at that time. Reviewing our results in the form presented in Fig. 5, I am not currently as sure that Tripodi was wrong and certainly he should be commended for opening this line of inquiry. Whether threshold or window the central question still remains: “How do we enter the region of stoichiometry in which condensed matter nuclear reactions—or at least the phenomenon of excess heat, the Fleischmann Pons Heat Effect, might be observed?” Let us examine the assertion that the ability of palladium cathodes to attain and maintain high loading levels, at high current density and for long times, is controlled by two principal factors: 1. The condition of the electrochemical interface which allows the attainment of high deuterium surface activity (high chemical potential). 2. The defect density and mechanical condition of the bulk material which permits the Pd lattice to withstand and contains high bulk deuterium activities when D atoms equilibrate to produce extreme pressures of D2 gas inside closed incipient voids within the metal. Why do some attempts to produce the FPHE succeed with a particular current-time protocol while similar cathodes (in some cases the same cathode) fail under similar or near-identical electrochemical conditions and identical current ramps? Let us focus first on failure. What went wrong in even our best cells? The conditions of our most successful procedures to demonstrate excess heat in SRI Fleischmann-Pons replication cells (i.e., those not employing superwave electrochemical loading or Hg treatment on very fine wires) are tabulated below. A set of 12 experiments with broad similarity were examined to illuminate the role of these two factors (surface and bulk) in facilitating or inhibiting excess heat production. The experimental conditions are summarized in Table 1. Developing the discussion of results first presented at ICCF7 [18], a total of 26 current ramps were performed in the 12 experiments in Table 1 with SRI mass-flow calorimetric interrogation. To achieve a suitable normalization from such a diverse data set what is plotted in Figs. 6–8 is the value of the resistance divided by the resistance value (R°°) at the chosen reference current density (i° ¼ 33 mA cm2) at the beginning of the current ramp. This normalized resistance ratio value (R/R°°) is plotted vs the normalized current density (i/i°). The data are presented in semilogarithmic form for reasons discussed subsequently. All current ramps shown in Figs. 7–9 were conducted at the same linear sweep rate (∂ i/∂ t). Despite the similar treatment and identical current sweep rate, the normalized data reveal three distinct modes of loading performance that we refer to as Modes A, B, and C. The suffix on experiments named in Figs. 7–9 (e.g., P15 4) indicates the chronological number of the ramp data plotted (preceding ramps normally being identical). Of the 26 ramps plotted in Figs. 7–9, 8 (31%) exhibit Mode A behavior, 8 (31%) exhibit Mode B behavior, and 10 (38%) exhibit Mode C behavior as described below. Mode A is characterized by a linear decrease of Pd resistance beyond the resistance maximum, with logarithmic increase in electrochemical current. This mode is most frequently associated with the

Table 1 Summary of experiments using Pd cathodes electrolyzed in 1 M base. Bath Temp (°C)

Electrolyte 1.0 M

Additive

P12 P13 P14 P15 P16 P17 Ml M2 M4 LL5 LL18 LL28

30 30 30 30 30 30 30 30 30 30 20 22

LiOD LiOH LiOD LiOD LiOD LiOD LiOD LiOD LiOD LiOD LiOD LiOD

Al Al Al Al Al Si Al Al Cu,Al Al None None

Conc. (ppm)

Electrode Source

Len. (cm) Dia. (cm)

Anneal Temp. (°C)

Time (h)

200 200 200 200 200 200 200 200 200 200

E#l E#l E#l E#l E#l E#l JM “Z” E#l JM “Z” E#3 IMRA IMRAa

3.0
0.30 3.0
0.30 3.0
0.30 3.0
0.30 3.0
0.30 3.0
0.30 3.0
0.20 3.0
0.28 10.0
0.10 3.0
0.28 3.0
0.10 3.0
0.20

800 800 800 800 800 800 800 800 800 800 As rcvd. As rcvd.

3 3 3 3 3 3 3 3 3 3

Treatment 1,2,4 1,2 1,2,3 1,2 1,2,3 1,2 2 1,2 1,1,2 1,2 None 2

a Material supplied by M. Fleischmann. Surface treatment: 1 ¼ surface machined; 2 ¼ aqua regia rinse; 3 ¼ 3He implant; 4 ¼ 4He implant. Bulk: E#1 ¼ Engelhard Lot #1; JM “Z” is a special lot of high purity palladium obtained from Johnson Matthey intended to replicate the metallurgy of the original Fleischmann Pons supply; E#3 ¼ Engelhard Lot #3; IMRA ¼ Institut Minoru de Recherche Avanc e Pd supplied by Fleischmann.

High reproducibility excess heat at SRI

Experiment #

47

48

Chapter 3 Electrochemical loading

2 T = 300K

Excess of enthalpy region 1.8

R/Ro

1.6

1.4

b+g

b

g

1.2

Deuterium 1

0.8

0.9

1

1.2

1.1

1.3

x

FIG. 6 The Tripodi conjecture [14].

1.00

Log-linear decrease 0.98 0.96 P13 1 0.94 0.92 0.90 0.88 0.86

P15 3 P15 4 P16 4 P17 3* Ml 1 M4 1 LL29* Lower Upper

* Axial Current

Typical 0.84

R/R°° 1

Relative current density (i/i°)

FIG. 7 Mode A: linear decrease of R/R°° (loading) with Log[i/i°].

10

100

High reproducibility excess heat at SRI

P12 4

1.00

MPa 101

0.98

140 0.96

P14 1 P15 1

186

P15 2

238

P15 3

298

P17 1*

366

P17 2*

441

LL5

0.94

0.92

523

Abrupt deload 0.90

R/R°° 1

Relative current density (i/i°)

Lower Upper

10

100

FIG. 8 Mode B: initial linear decrease of R/R°° with Log[i/i°] followed by abrupt and irreversible increase in R/R°° (deloading).

1.00 P12 1 P12 2

0.99

P12 3 P14 2 P15 5

0.98

M2 3 M4 2 M4 3

0.97

M4 4 LL18 Lower

0.96

Upper

Shallow

Typical

0.95

R/R°° 1

Relative current density (i/i°)

10

FIG. 9 Mode C: initial shallow decrease of R/R°° with Log[i/i°] followed by a flatter response or deloading.

100

49

50

Chapter 3 Electrochemical loading

appearance of calorimetrically determined excess heat consistent with the empirical expression developed to describe SRI results [19]: Pxs ∝ ðx  x∗Þ2 ði  i∗Þ |∂x=∂t|,where x ¼ D=Pd, x∗  0:875, i∗ ¼ 50  400mAcm2

This expression teaches us that, to produce significant excess heat, we need to achieve simultaneously both high loading (low R/R°°) and high current (large i/i°), thus Mode A behavior. How do we achieve Mode A? What prevents or handicaps this achievement? We know from other studies that the interfacial electrochemical kinetics of hydrogen discharge onto and thus absorption into a Pd cathode is complicated to a degree and in detail not well understood. Nevertheless, the simplest law governing electrochemical deposition is that expounded by Tafel [7] from which one would expect a log-linear dependence of loading on current density. Whether our observation of this dependence in Mode A is a happy coincidence or of fundamental significance I don’t know but we can be reassured somewhat that if the electrochemistry is working well then so must the interface be. Mode A is consistent with good electrochemistry that is consistent with good surface condition. Mode B follows the initial log-linear decrease of the Mode A trajectory but departs from this behavior with a rapid increase in resistance when the R/R°° falls below a critical value. We interpret this apparently rapid deloading as resulting from mechanical failure of the Pd lattice when closed voids within the metal open a pathway to the surface to release molecular D2. We conjecture that this occurs in materials for which the defect density and mechanical condition of the bulk Pd lattice can no longer withstand and contain the extreme pressures produced by D2 gas inside closed incipient voids. These are regions in which Pd atoms are not held together by metal-metal bonds as may occur in voids or at sites of metal oxide (or other) inclusions. The yield strength of the metal in such regions is conjectured [14] to be less than the pressure imposed by released molecular D2 gas in equilibrium with high bulk metal-phase D atom activities. The vertical scale superimposed in Fig. 8 shows the equilibrium D2 pressure calculated from the data of Baranowski [20] by assuming that the reference current condition (i° ¼ 33 mA cm2) produces the resistance ratio maximum (R/R°° ¼ 1.96). The units of pressure are megapascals. The break toward higher resistance in Fig. 8 occurs within a relatively narrow range of equilibrium pressures; 300 < Pmax < 500 MPa. This range conforms plausibly with that expected for the yield strength of palladium deuteride (although this number is undetermined experimentally). We conclude tentatively, therefore, that the failure in Mode B is of mechanical lattice disruption. [It is worth noting parenthetically in this context that the palladium bulk metal source that was most successful at producing the FPHE was Engelhard Lot #1, designated as E#1 in Table 1. This material was also the least pure Pd ever employed in the FPHE studies at SRI, with a nominal (manufacturer listed) purity of 99.7% and a tested purity more like 99.2%. In the context of preventing metal yield with cracks propagating to the surface to cause D2 release, high atomically distributed impurity levels would be considered favorable, the alloys normally having much higher yield strengths than pure Pd.] Mode C behavior displays a shallow decrease in resistance with approximately symmetric increase as the [log] current density is increased beyond a threshold value. We interpret this as evidence of “poor” electrochemistry or at least poor surface condition that becomes worse with time, current density, or some combination of these two, as species or structures antagonistic to loading (via blocking or poisoning) transport to and deposit at the electrified interface.

High reproducibility excess heat at SRI

51

We should note that the normalized current density at which the cathodes begin to deload (characterized by increasing R/R°°) is similar in Mode C to that for Mode B, albeit more widely scattered and at much higher values if R/R°° in Mode C. Nevertheless, we are imputing different physical reasons for the failure to load in the two modes. Let’s look more closely at Mode B. If we ignore the surface free energy considerations important only for very small voids, the pressure achieved under equilibrium conditions in such voids is that required to attain the measured value of resistivity ratio in gas loading experiments. When this internal pressure exceeds the yield strength of the palladium host material for an electrochemically loaded specimen that is not supported by high external gas pressure, cracks will form, ultimately connecting to the surface and providing a conduit for molecular deuterium to leave the cathode. The dimensions of these cracks are such that electrochemical processes cannot proceed effectively within them, and molecular D2 thus leaves the cathode with no effective means of replacement, resulting in rapid cathode deloading and increase in R/R°°. As noted, the resistance minimum occurs at approximately the same current density in Modes B and C. However, Mode C behavior is characterized by a much diminished deuterium absorption (much greater R/ R°°) with a much shallower rate of response to increasing Log[i/i°] for both loading and unloading. The argument for mechanical failure in Mode B seems at least self-consistent but this cannot be the reason for failure in Mode C because the maximum estimated internal gas pressure in voids would be much too low to cause mechanical disruption. The failure here appears to be of and at the interface, either due to blockage and restricted diffusion, or to electrochemical conditions which are not conducive to the attainment of high surface activity. This conclusion is consistent with the shallow initial response of loading (R/R°°) with current density and the very much shallower rate of deloading. The analysis above, while potentially helpful particularly for understanding our failures, is substantially oversimplified and must be appended with the following qualifying statements: (A) Not all ramps that were performed are included in this database. For some, the reason was technical (e.g., poor resistance measurement or varying experiment condition). In some cases, the 33 mA cm2 rest was not observed, or not well observed, so the normalization used to plot the data in Figs. 7–9 was not possible. In some case, the ramp rate was changed thus preventing good data comparison. (B) Ramp P15-3 is plotted as both Modes A and B. (C) Because of the normalization, adequate loading and excess heat was observed for some cathodes exhibiting Mode C behavior. This is because these cathodes had already obtained high loading at the normalizing current density (33 mA cm2), and one of the reasons for Mode C behavior is prior good loading. (D) Some cathodes (notably P14) improved from Mode C to Mode A behavior presumably as the surface restructured favorably for good electrochemistry. (E) A more puzzling behavior was observed for P14, P15, and P17 in which cathodes “recovered” from Mode B to Mode A on following ramps (P14 in fact from Mode B to Mode C to Mode A on subsequent ramps). If the cause of Mode B is mechanical lattice disruption, how can we explain healing the bulk metal? Four effects might be taken into consideration: (a) Essentially every experiment shown in Table 1 contained minor elemental electrolyte additions (in most cases 200 ppm of Al). This concentration of Al in the electrolyte, and selected other elements, had previously been determined empirically [8] to be highly conducive to the attainment or maintenance of the high loading condition. Although the physical mechanism is not well understood, Al was observed to attach preferentially to the

52

Chapter 3 Electrochemical loading

surface sites of emergent grain boundaries. It is conceivable that grain boundaries are principle pathways for molecule deloading facilitated by mechanical disruption, and that this pathway can be “healed” by Al, in time. (b) The surface of a heavily electrolyzed palladium cathode is not Pd. In addition to the deposition of deliberate and adventitious cations, our electrolytes contained high levels (1 M concentration) of Li which deposits only semireversibly onto the Pd cathode and incorporates into it. Li atoms substitute in place for Pd, forming one or more of the LixPd phases. Cathodes electrolyzed at high current density for periods as long as 1000 h incorporate Li up to 3 μm below the (new) surface. The mechanical (and other) effects of this incorporation are not known but may well place the surface in compression and tend to counter forces giving rise to Mode B behavior (mechanical weakness), and/or prevent internally initiated cracks from propagating to the surface. (c) The rapid release of D2 (H2) from a well-loaded Pd cathode can sometimes be observed with a “naked” eye (well protected). Occasionally when examining optically a cathode at loading PdD0.9 or above one will observe jets of bubbles emerging from the surface, accompanied by a rapid increase in electrode axial resistance (decrease in D/Pd loading). The rate of gas emergence and resistance change is far greater than can be accounted by metal-phase atomic diffusion, as if a crack had opened to a bulk void or the surface cap of a grain boundary had been removed (i.e., Mode B). Even more remarkably, however, these “vents” appear to selfheal and these electrodes often reload spontaneously, sometimes to even higher levels without recurrence of the phenomenon. (d) It has been speculated [21, 22] that the NAE is one or other of the super abundant vacancies (SAV) phases first identified by Fukai [23]. Fukai argues that these are the thermodynamically stable phases of PdH and PdD (and many other fcc metals) at high hydrogen chemical potentials. These phases, he claims, are normally prevented from forming by kinetic inhibition as self-diffusion to the free surface of a bulk specimen is a very slow process. It is possible that the fine cracks that cause rapid loading loss are a source of vacancy gain thus facilitating the formation of a high vacancy phase. In this conjecture, short-range diffusion to the crack wall would tend both to annihilate the crack (preventing further hydrogen isotope loss) and create a population or density of SAV-phase material as putative NAE. It seems likely that at least two factors must be controlled in order to obtain Mode A behavior which leads to high loading at high current densities and, potentially, access to the region of composition in which excess heat may be observed: (i) the condition of the electrochemical interface which allows the attainment of high deuterium surface activity and (ii) the defect density and mechanical condition of the bulk material which permits the Pd lattice to withstand and contain high bulk deuterium activities. Because of the high permeability of D in Pd, in order to obtain the desired Mode A behavior, the surface must be everywhere in the desired electrochemical condition and the bulk metal must be homogeneously sound. Only cathodes which are uniformly sound in both surface and bulk dimensions may be capable of sustaining high loading at high current densities thought to be necessary for excess heat production.

References

53

Conclusions 1. Empirical evidence from the experimental groups with which I am most familiar, SRI Menlo Park (the United States) and ENEA Frascati (Italy), strongly supports the hypothesis that attainment of the FPHE depends critically on at least preestablishment of a high deuterium:palladium stoichiometric ratio. 2. Following Tripodi we pose the question: does the onset or initiating condition of the FPHE occur above a threshold as previously asserted [24, 25], or in a window of stoichiometry as conjectured by Tripodi [14]? Evidence is presented here consistent with the latter and defining a range in which both the well-known β-phase and Fukai’s γ-phase coexist. 3. Whether threshold or window, attainment of suitable loading in bulk palladium requires careful control of a number of parameters and has proved challenging. From an analysis of historic SRI data, it appears that two factors above all others control the attainment and maintenance of high D/ Pd stoichiometry: the electrochemical susceptibility of the cathode surface; the mechanical strength of the bulk metal and the absence of voids or nonmetallic bulk-phase inclusions. 4. These conclusions taken together with apparent (albeit circumstantial) evidence for “self-healing cracks” followed by excess heat production lend support to the conjecture that the introduction of space in the lattice to facilitate SAV formation (in this case cracks) may allow electrodes to enter the coexistent state of β + γ phases more easily or rapidly and allow excess heat production. This last enumerated conclusion requires several assumptions and should be regarded as highly speculative. If correct, however, it might allow ready understanding and easier attainment of the environment or regions within PdD in which nuclear reactions can occur. We shall explore this further.

References [1] M. Fleischmann, S. Pons, Electrochemically induced nuclear fusion of deuterium, J. Electroanal. Chem. 261 (1989) 301. Errata in 263, p. 187. [2] D.D. Macdonald, M.C.H. McKubre, A.C. Scott, P. Wentrcek, Continuous in-situ method for the measurement of dissolved hydrogen, Ind. Eng. Chem. Fundam. 20 (1981) 280. [3] N. Bonanos, B. Steele, E. Butler, W. Johnson, W. Worrell, D.D. Macdonald, M.C.H. McKubre, Applications of impedance spectroscopy, Chapter 4, in: J.R. Macdonald (Ed.), Electrochemical Impedance Methods, Wiley-Interscience, New York, 1987. [4] M.C.H. McKubre, R.C. Rocha-Filho, S.I. Smedley, F.L. Tanzella, Calorimetry and electrochemistry in the D/ Pd system, in: Proc. ICCF1, 1990. [5] E. Storms, The Science of Low Energy Nuclear Reaction, World Scientific Publishing Company, 2007. [6] E. Storms, The Explanation for Low Energy Nuclear Reaction, Infinite Energy Press, Concord, MA, 2014. [7] J.O.’.M. Bockris, A.K.N. Reddy, Modern Electrochemistry, Plenum Press, New York, 1970. [8] M.C.H. McKubre, et al., Development of Advanced Concepts for Nuclear Processes in Deuterated Metals, TR-104195, Electric Power Research Institute, Palo Alto, 1994. [9] M.C.H. McKubre, F.L. Tanzella, I. Dardik, A. El Boher, T. Zilov, E. Greenspan, C. Sibilia, V. Violante, Replication of condensed matter heat production, in: J. Marwan (Ed.), Low-Energy Nuclear Reactions Sourcebook, ACS Symposium Series 998, Oxford University Press, 2008, p. 219. [10] M.C.H. McKubre, J. Bao, F.L. Tanzella, P.L. Hagelstein, Calorimetric studies of the destructive stimulation of palladium and nickel fine wires, in: Proc. ICCF17, 2012.

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Chapter 3 Electrochemical loading

[11] S. Crouch-Baker, M.C.H. McKubre, F.L. Tanzella, Variation of resistance with composition in the β-phase of the H-Pd system at 298 K, Z. Phys. Chem. 204 (1998) 247–254. [12] W.-S. Zhang, Z.-F. Zhang, Z.-L. Zhang, Some problems on the resistance method in the in situ measurement of hydrogen content in palladium electrode, J. Electroanal. Chem. 528 (2002) 1–17. [13] D. Kidwell, Low energy nuclear reaction research at the Naval Research Laboratory, in: Keynote Lecture ICCF18, 2013. [14] P. Tripodi, D. Di Gioacchino, J.D. Vinko, PdH(D,T)x system: are excess of enthalpy and superconductivity two concurrent phenomena affected by stoichiometry x? in: 8th International Workshop on Anomalies in Hydrogen/Deuterium Loaded Metals, Catania, Sicily, 2007. [15] P. Tripodi, M.C.H. McKubre, F.L. Tanzella, P.A. Honnor, D. Di Gioacchino, F. Celani, V. Violante, Temperature coefficient of resistivity at compositions approaching PdH, Phys. Lett. A 276 (2000) 122. [16] P. Tripodi, U.S. Patent No. 7,033,568, High TC Palladium Hydride Superconductor, 2006. [17] A. Lipson, C. Castano, G. Miley, B. Lyakhov, A. Mitin, Emergence of high-temperature superconductivity in hydrogen cycled Pd compounds as evidence for super-stoichiometric H/D sites, in: Proc. ICCF12, J. Condensed Matter Nuclear Science, 2006, pp. 128–146. [18] M.C.H. McKubre, F.L. Tanzella, Materials issues of loading deuterium into palladium and the association with excess heat, in: Proc. ICCF7, Vancouver, 1998. [19] M.C.H. McKubre, S. Crouch-Baker, A.K. Hauser, S.I. Smedley, F.L. Tanzella, M.S. Williams, S. S. Wing, Concerning reproducibility of excess power production, in: Proc. ICCF5, Monte Carlo, 1995. [20] B. Baranowski, S.M. Filipek, M. Szustakowski, J. Farny, W. Woryna, Search for cold fusion in some Me-D systems at high pressures of gaseous deuterium, J. Less Common Met. 158 (1990) 347. [21] M.R. Staker, Coupled calorimetry and resistivity measurements, in conjunction with an emended and more complete phase diagram of the palladium—isotopic hydrogen system, in: Proc. ICCF21, Ft. Collins, Submitted to JCMNS. 2019. [22] M.C.H. McKubre, M.R. Staker, On the role of Super Abundant Vacancies (SAV) in hydrogen loading and production of the Fleischmann Pons heat effect (FPHE), in: Presented at the 13th International Workshop on Anomalies in Hydrogen Loaded Metals, Oasi di Greccio, Italy, 5–9 October, 2018. [23] Y. Fukai, The Metal–Hydrogen System: Basic Bulk Properties, second ed., Springer, Berlin, Germany, 2005. [24] M.C.H. McKubre, S. Crouch-Baker, A.M. Riley, S.I. Smedley, F.L. Tanzella, Excess power observations in electrochemical studies of the D/Pd system, the influence of loading, in: Proc. ICCF5, “Frontiers of Cold Fusion”, Nagoya, Japan, vol. 1992, Universal Academy Press, Tokyo, Japan, 1992. [25] K. Kunimatsu, N. Hasegawa, A. Kubota, N. Imai, M. Ishikawa, M. Akita, Y. Tsuchida, Deuterium loading ratio and excess heat generation during electrolysis of heavy water by a palladium cathode in a closed cell using a partially immersed fuel cell anode, in: Proc. ICCF5, “Frontiers of Cold Fusion”, Nagoya Japan, Universal Academy Press, Tokyo, Japan, 1992.

CHAPTER

Fundamentals of isoperibolic calorimetric for cold fusion experiments

4 Melvin H. Miles

College of Science and Technology, Dixie State University, St. George, UT, United States

Introduction: Choosing an isoperibolic calorimeter Both the size and shape of the isoperibolic calorimeter are very important. The calorimetric cell should contain between 20 and 100 mL of electrolyte. The shape of the cell should be cylindrical with a small diameter and a length considerably greater than the cell diameter. For example, the three F-P Dewar calorimeters used by the author had inner diameters of 2.5 cm, heights of 25.0 cm (with the top 8.0 cm silvered) and contained 90 cm3 of electrolyte [1]. The size and shape of the calorimeter must provide adequate stirring by the electrolysis gases, give a sensitive response by the cell temperature to the generation of any excess power, and minimize the rate of change in the electrolyte level with time due to electrolysis. Trade-offs are necessary among these factors. For example, a larger cell diameter would reduce the rate of change of the electrolyte level but adequate stirring by the electrolysis gases would be compromised. A smaller cell diameter for a given cell height would make the cell temperature readings more sensitive to any excess power, but the rate of change of the electrolyte level would be increased. A small calorimetric cell with an electrolyte volume of only 18 mL was used for several years by the author, but a larger volume of H2O around the cell acted as a heat integrator and helped to minimize the electrolyte level effect [2]. The Dewar-type cells provide an important advantage for directly observing processes inside the cell. For most heat conduction cells, visible light is blocked by the insulation and other cell components. However, heat conduction cells are simpler to construct [2, 3]. It requires an expert glassblower to construct a Dewar cell with the desired vacuum to minimize heat transport by conduction. The main heat transfer for Dewar cells is via electromagnetic radiation (mostly infrared) with no memory effect. The heat transfer by conduction is a much slower process where heat can linger in the insulation. Additional advantages of Dewar cells have been discussed elsewhere [4]. The cell constant for a Dewar cell will gradually increase with time (years) due to the diffusion of atmospheric helium into the Dewar vacuum [1]. In contrast, heat conduction cells have shown no measurable changes over several years of use [2]. The author has used both types of isoperibolic calorimeters, and an F-P Dewar cell would be preferred if it could be properly constructed [1, 5, 6]. Both the kC and kR cell constants can be estimated from the cell dimensions. The thermal conductivities of most cell materials are available for estimating the conductive heat transfer coefficient, kC. Cold Fusion. https://doi.org/10.1016/B978-0-12-815944-6.00004-X # 2020 Elsevier Inc. All rights reserved.

55

56

Chapter 4 Fundamentals of isoperibolic calorimetric

The Stefan-Boltzmann constant, kB ¼ 5.670373  108 Wm2 K4, is useful for the estimation of the radiative heat transfer coefficient, kR [1].

Isoperibolic calorimetric equations and possible simplifications The isoperibolic calorimeter is an open thermodynamic system where both matter and energy can be exchanged with its surroundings. The exchange of energy can be in the form of both heat and work as well as matter. The correct mathematical modeling of the isoperibolic calorimeter must include all power sources that flow into and out of the calorimeter. These power sources are the electrochemical power (PEI), the power applied by any internal heater (PH), any anomalous power sources (PX), the power carried away by the electrolysis gases (PG), power exchanged by conduction (PC) or radiation (PR), and power due to rate of pressure-volume (P-V) work done by the generated gases (PW). The resulting equation can be expressed simply as PCALOR ¼ PEI + PH + PX + PG + PC + PR + PW

(1)

where PCALOR is the net power of the calorimetric system. A long and unwieldy equation results when all equations for the various terms are included in Eq. (1) [1, 5, 6]. As usual in thermodynamics, heat or power added to the system (calorimeter) is positive while power that flows out of the calorimeter to the surroundings is negative. Several assumptions can greatly simplify Eq. (1). First PG and PW are small except at high cell currents (I > 0.5 A) and high cell temperatures (T > 60°C). Furthermore, an in-cell heater is seldom used except in the F-P calorimetry. Therefore, Eq. (1) simplifies to Cp MdT=dt ¼ ðE  EH Þ I + PX  kC ðT  Tb Þ  kR f ðT Þ

(2)

where f(T) ¼ T4  T4b for heat transfer by radiation. The calorimeter is usually modeled by using only the heat conduction or the heat radiation term depending on the type of calorimeter used [1, 2].

Applications to cold fusion experiments The simplest starting point for any cold fusion experiment is to assume the excess power is zero (PX ¼ 0) and calculate a lower bound heat transfer coefficient at various times throughout the experiment. For a heat conduction calorimeter where PR ¼ 0, the lower bound coefficient (kC0 ) is given by   kC0 ¼ ðE  EH ÞI  Cp MdT=dt =ðT  Tb Þ

(3)

where EH is the thermoneutral potential and CpM is the heat capacity of the system. All these terms have been defined elsewhere [1–7]. Initially, CpM can be calculated from the heat capacities of all cell components inside the main thermal barrier [1]. The total cell heat capacity (J/K) is expressed in terms of the molar heat capacity of D2O (CP) and an equivalent number of moles (M) that yields the correct total heat capacity. The accurate evaluation of dT/dt (K/s) often requires a graph of the cell temperature versus time. At the beginning of an experiment, the rate of the cell temperature increases with time

More about the lower bound heat transfer coefficient

57

will be large and positive in Eq. (3). Theoretically, the cell temperature should increase linearly with time for the first 10–15 min [8, 9]. This is true for both types of isoperibolic cells. After several hours of electrolysis, dT/dt will be small, but this term seldom remains exactly zero under normal cell operations and should not be neglected [9]. The cell temperature may sometimes decrease with time due to various factors such as a decrease in the cell current or a decreasing cell voltage with time. The first test of a new calorimeter should be running a control such as a platinum cathode in a D2O + LiOD electrolyte. Because the excess power should be zero, the use of Eq. (3) will yield the true cell constant when the PG and PW terms are small. The use of a platinum cathode in H2O is inferior because H2O and D2O differ in heat capacities. The use of a palladium cathode in H2O as a control adds another problem in giving an early excess heat effect due to the exothermic loading of hydrogen into the palladium. The use of controls is important because no calorimetric system can be accurately calibrated in the presence of an unknown excess power effect [1]. If any exothermic chemical effects are present in the Pt/D2O control, such as recombination, the cell temperature will be larger than expected, and the lower-bound heat transfer coefficient, kC0 , will be smaller than normal. For experiments using palladium cathodes in D2O electrolytes, kC0 defined in Eq. (3) will be useful in showing time periods of possible excess power resulting in lower than normal kC0 values. A convenient and accurate method for calculating any excess power (PX) is the equation
PX ¼ kC  kC0 ðT  Tb Þ

(4)

where kC is the true heat transfer coefficient [9]. A related equation for Dewar calorimeters is
PX ¼ kR  kR0 f ðT Þ

(5)

where kR0 is defined by Eq. (3) when f(T) replaces T  Tb [1, 10]. It has been assumed here that the bath temperature is constant where d(T  Tb)/dt ¼ dT/dt. There will likely be calorimetric errors if there are significant changes in the bath temperature because the temperature inside the calorimetric cell will be slow to adjust to changes in the bath temperature. This is due to large time constants (30–60 min) for most isoperibolic calorimeters. Bath temperatures may change somewhat due to room temperature changes, convection changes, or even to changes in the room lighting or sunlight exposure. Ideally, room temperature changes should be less than about 1°C and the bath temperature changes less than 0.01°C [1]. Another factor often overlooked is the level of the water bath. Only a small portion of the calorimetric cell should be exposed to the room temperature air and this portion must be constant. Air is a much better insulator for heat flow than water. Fiberglass insulation around the cell top helps to minimize the effect of room air.

More about the lower bound heat transfer coefficient The lower bound heat transfer coefficient, kC0 as defined in Eq. (3), is very useful for showing if any excess power is initially present in an experiment. A rearrangement of Eq. (4) yields kC0 ¼ kC  PX =ΔT

(6)

58

Chapter 4 Fundamentals of isoperibolic calorimetric

where ΔT ¼ T  Tb. Note that ΔT is quite small initially in an experiment which may result in negative kC0 values when excess power is present. If PX ¼ 0, then kC0 ¼ kC. However, if any excess power is present, then kC0 can initially be negative when ΔT is small and kC < PX/ΔT and then become zero when kC ¼ PX/ΔT and eventually approaches the value of kC when ΔT becomes large and kC ≫ PX/ΔT. This behavior for kC0 has been observed experimentally when excess power is initially present [9]. This excess power can simply result from the initial exothermic loading of hydrogen or deuterium into palladium. This initial behavior of kC0 is another reason not to use a Pd/H2O control. Similar initial effects for the radiative lower bound heat transfer coefficient, kR0 , have been previously reported by Fleischmann and Pons [10]. For radiative heat transfer, Eq. (6) simply becomes kR0 ¼ kR  PX =f ðT Þ

(7)

where f(T) involves temperatures to the fourth power. The initial behavior of kC0 or kR0 can be useful in predicting if an experiment is likely to show significant excess power [10]. Therefore, the data from the beginning of an experiment should not be ignored.

The neglected PG and PW terms The PG term is complicated and requires the measurement of the laboratory atmospheric pressure during the experiments and the calculation of the equilibrium vapor pressure of D2O in the cell for each measured cell temperature. This term accounts for the heat transferred from the cell by the D2, O2, and D2O gases that exit the cell during electrolysis. A useful guide for the magnitude of the PG term versus the cell temperature is given in Fig. 3 of Ref. [2]. Very few, if any, cold fusion groups have reported the atmospheric pressure measurements required for the PG calculations except for the F-P and China Lake publications [11]. Although the PG term is usually small and may be ignored at lower cell temperatures, this term becomes the dominant term as the cell temperature approaches the D2O boiling point (101.42° C). In fact, the excess power during the cell boiling can be estimated by the rate of boiling [1, 10]. Further discussion of the PG term is found in the Appendix. The small PW term due to the work done by the generated electrolysis gases can be easily calculated as needed from the equation PW ¼  RT ð0:75 I=FÞ

(8)

where I is the cell current in amperes and T is the cell temperature in Kelvin. Unlike the PG term, the PW term increases only slowly with the cell temperature at a constant cell current. At I ¼ 0.500 A, for example, PW is 10.1 mW at 40°C (313.15 K) and 11.4 mW at 80°C (353.15 K), while the PG term increases from 12.8 to 114.9 mW at these same two temperatures [2]. The PW term was never used in any of the F-P publications, and some believe that this term was included in the thermoneutral potential (EH) based on ΔH for the D2O electrolysis reaction. However, at constant pressure ΔH ¼ q (heat) and does not involve any P-V work. This PW term was needed to explain the small negative excess power on Day 61 of the Pd-B study due to the large cell current (I ¼ 1.000 A) [1]. The addition of PW changed the mean excess power from  5.0 to 17.3 mW.

The straight-line method

59

The effect of neglecting the PG and PW terms leads simply to an underestimation of the excess power. Including the PG and PW terms would give a smaller kC0 (or kR0 ) in Eq. (3), hence a larger value for PX from Eq. (4) (or Eq. 5). The F-P methods were always designed such that any errors or approximations would result in an underestimation of the excess power [1, 5, 6, 10].

The straight-line method The F-P data analysis often involved the rearrangement of the calorimetric equation to a straight-line form [1, 12, 13]. For a heat conduction calorimeter where PC ≫ PR, Eq. (1) becomes ðPNET + PX Þ=ΔT ¼ Cp MðdT=dtÞ=ΔT + kC

(9)

where PNET ¼ PEI + PH + PG + PW and ΔT ¼ T  Tb. Simplifying by using PNET  PEI when PH, PG, and PW are small yields ½ðE  EH ÞI + PX =ΔT ¼ Cp MðdT=dtÞ=ΔT + kC

(10)

where Eq. (10) is in the desired straight-line form, y ¼ mx + b, with y ¼ [(E  EH)I + PX]/ΔT, m ¼ CpM, x ¼ (dT/dt)/ΔT, and b ¼ kC. Note that both y and kC have units of W/K, CpM has units of J/K, and x has units of s1 in Eq. (10). The y-intercept at x ¼ 0 gives kC. A useful substitution is x ¼ x0 /CpM0 where CpM0 is an estimation of CpM. Therefore,
y ¼ Cp M=Cp M0 x0 + kC

(11)

where now y, x0 , and kC each have units of W/K and the slope of the line will be nearly unity when CpM0 is a good estimation for CpM. The application of Eq. (11) to the first 125 min of a recent Pd-B experiment with the assumptions of PX ¼ 0, EH ¼ 1.527 V, and CpM0 ¼ 450 J/K is shown in Fig. 1. The straight-line fit is good (R2 ¼ 0.9986) and the y-intercept yields the lower-bound heat transfer coefficient, kC0 ¼ 0.1258 W/K. This value for kC0 , however, is not correct because it is even larger than the true kC. Furthermore, the line slope (m ¼ 0.7733) is too small and gives the cell heat capacity as CpM ¼ 0.7733 (450 J/K) ¼ 348 J/K. This value for CpM is much too small, thus excess power must be present in this experiment during this initial 125 min time period. When the calculated PX values are included in the determination of y, then Fig. 1 gives a perfect straight-line fit with R2 ¼ 1.000, CpM ¼ 450 J/K, and kC ¼ 0.1205 W/K as expected. An important application of the straight-line method expressed by Eq. (10) or Eq. (11) is for the calibration of a new calorimetric system using a control, such as Pt/D2O. When there is no excess power, the y-intercept gives the true cell constant (kC) and the line slope gives the correct heat capacity of the system (CpM). Time periods of significant cell temperature changes are desired, such as the beginning of an experiment, time periods following D2O additions, time periods where the cell current is changed, or time periods where an internal heater is applied. Fleischmann has reported similar straightline methods for the Dewar calorimetric data [1, 11, 12].

60

Chapter 4 Fundamentals of isoperibolic calorimetric

Pd-0.5B data (first 125 min) results when PX set to zero 1.4 1.2

y(W/k)

1.0 0.8

y = 0.773302x + 0.125816 R 2 = 0.998637

0.6 0.4 0.2 0.0 0.0

0.2

0.4

0.6

0.8

1.0

1.2

1.4

1.6

X′(W/k)

FIG. 1 Straight-line for Pd-B calorimetric data (y ¼ 0.7733 x0 + 0.1258, R2 ¼ 0.9986).

Radiative heat transfer coefficient Eqs. (1), (9), and (10) are all differential equations because of the PCALOR ¼ CpMdT/dt term in each. Furthermore, all terms in these equations may vary with time. It is well known from the differential equations of chemical kinetics that more accurate results can be obtained from the integration over time of the differential rate equations. The same is true for the differential equations used in cold fusion. However, numerical integration methods must be used for these complex equations. It seems that only Fleischmann has accomplished this task for the F-P Dewar calorimetry. Fleischmann has explored various numerical integration methods, including Simpson’s rule, the trapezoidal rule, and the mid-point rule and has favored the trapezoidal rule in a later publication [1]. Various radiative heat transfer coefficients have been used by Fleischmann due to his investigation of backward or forward numerical integration methods over various periods of time. These coefficients, including the direct use of the differential equation, are defined by (kR)i,j,l where i ¼ 1 denotes “differential,” i ¼ 2 for “backward integration,” i ¼ 3 for “forward integration,” l ¼ 1 denotes “lower bound,” and l ¼ 2 denotes “true.” Different time periods in the use of 2-day cycles are defined by values for j (if used) [1]. For example, (kR)262 was often favored by Fleischmann, which defines backward integration (i ¼ 2) starting at the mid-point of the 2-day cycle (j ¼ 6) for the “true” (l ¼ 2) value for kR. Fleischmann has shown that the backward integration of the calorimetric data provides more accurate results than the forward integration methods [1]. Using Fleischmann’s notation, kC ¼ k102 and kC0 ¼ k101 where j ¼ 0 denotes the entire measurement period. Detailed discussions of (kR)i,j,l can be rather complicated and are not really necessary unless one uses integration methods and wants to reduce the calorimetric error to about 0.1 mW [11]. This early concern for calorimetric accuracy by F-P may be related to the

Cell cooling experiments

61

fact that even 0.1 mW of excess power could produce a deadly rate of neutrons (about 107 n/s) if the cold fusion reactions were the same as hot fusion reactions. However, the major cold fusion product is helium-4 [13–15], and the very low rate of neutron production in cold fusion experiments is generally not even measurable, especially when no significant excess heat is present [5, 16], despite the opportunistic claims made by Steven Jones in 1989 [17]. The strange electrolyte used by Jones in his electrochemical cells consisted of an unusual mixture of 11 different chemicals [17], and his reported neutron results have never been verified.

Cell cooling experiments Experimental cell cooling can be investigated at any time by simply turning off the cell current. This should preferably be done with a Pt/D2O control where PX ¼ 0. The calorimetric terms PEI, PG, and PW will also be zero when I ¼ 0. The calorimetric differential equation then simplifies to Cp MdT=dt ¼ kC ðT  Tb Þ

(12)


dT=ðT  Tb Þ ¼  kC =Cp M dt

(13)

and can be rearranged to give

This equation can be readily integrated to yield
ln ðTo  Tb Þ=ðT  Tb Þ ¼ kC =Cp M t

(14)

where To is the initial cell temperature at the selected time for t ¼ 0, and T is the measured cell temperature as the cell cools. Thus Eq. (14) can also be expressed as
T  Tb ¼ ΔTo exp kC =Cp M t

(15)

where ΔTo ¼ To  Tb. This shows the exponential cooling of the cell. The time constant (thermal relaxation time) for the calorimeter is given by τ ¼ CpM/kC. Eq. (14) gives another straight-line fit, y ¼ mx, where y ¼ ln (To  Tb)/(T  Tb), m ¼ kC/CpM and x ¼ t in seconds. The experimental cell cooling data provides for an accurate determination for the ratio, kC/CpM, for the calibration of a new calorimetric system. These equations also illustrate the advantage of integrated equations (Eq. 14) compared to the differential equations (Eq. 12) in the determination of experimental values (kC/CpM). A less accurate value is obtained from Eq. (12) rearranged as kC/CpM ¼ (dT/dt)/(T  Tb). For cell cooling experiments, the electrolyte should be at the proper level such that CpM ¼ CpM°. Cell cooling studies can also be done for Pd/D2O experiments where excess power (PX) may be present. This excess power may linger past the time of shutting off the cell (heat-after-death) and slow the cell cooling rate. This was used by F-P to detect effects of excess power on the cell cooling for their Dewar cells [18]. For heat conduction when the excess power is known, the initial cell cooling rate is given by dT=dt ¼ ½kC ðTo  Tb Þ=Cp M + PX =Cp M

(16)

62

Chapter 4 Fundamentals of isoperibolic calorimetric

This equation cannot be integrated because the variation of PX with time is not known. However, this excess power due to “heat-after-death” generally gradually decreases with time. For Dewar cells with radiative heat transfer, the equations are considerably more complicated. Assuming the excess power is zero, the differential equation is Cp MdT=dt ¼ kR T 4  Tb4




(17)

The integrated result for this differential equation is given in the Appendix. The cell cooling for a Dewar cell and a heat conduction cell are very similar. In fact, the integrated equations for Dewar and heat conduction cells will have the same slope if their heat capacities are equal and if their cell constants have the relationship given by kC ¼ 4 T3b kR. For example, a bath temperature of 300 K and a kR value of 0.800  109 W/K would require that kC ¼ 0.0864 W/K.

Additional calorimetric topics The electrolysis of D2O produces changes with the time of both the cell constant, kC, and the heat capacity, CpM, of the calorimetric cell. These effects are linear at a constant cell current such that kC ¼ k°C (l  at) and CpM ¼ CpM° (l  bt). The change in the moles of D2O with time is given by M ¼ M°  ðl + βÞðIt=2FÞ

(18)

where β is a dimensionless term allowing for D2O losses by evaporation or other means besides electrolysis [1, 5]. These changes in kC and CpM with time can also be conveniently expressed in terms of the electrolyte volume for a given calorimetric cell. There is a loss of 0.812 mL of D2O per day due to electrolysis when I ¼ 0.100 A. The volume effect on kC must be determined by experimental measurements. For example, the volume effect is 0.0002 W/K per mL for the present calorimeter used by the author. The volume effect on CpM can be calculated as 4.65 J/K per mL of D2O. The fraction of D2O loss by evaporation depends on the experimental condition, but typically β ¼ 0.05 when the glass exit tube for the electrolysis gases is near room temperature. Considerable refluxing of D2O vapor occurs in the upper regions of the cell as well as in the glass exit tube. The exact expression for PCALOR allows for changes in both the cell temperature and the moles of D2O (M) with time [2, 7]. Using ΔT ¼ T  Tb yields PCALOR ¼ Cp d=dtðΔTMÞ ¼ Cp MdΔT=dt + Cp ΔTdM=dt ¼ Cp MdΔT=dt  Cp ΔT ðl + βÞI=2F

(19)

where M is expressed by Eq. (18). The second term is usually small and can often be neglected to give PCALOR ¼ CpMdT/dt when the bath temperature is constant. However, the F-P earlier publications often cited Eq. (19) [5]. The accurate determination of the rate of the cell temperature change with time (dT/dt in K/s units) can often be challenging. The tangent to the cell temperature versus time curve is needed. This can often be approximated by using two adjacent points, preferably equally spaced, and using the chord

Calorimetric results from calTech, MIT, and harwell

63

joining these two points: dT/dt  (T2  To)/(t2  to) for point t1. This result should be checked with the experimental T vs t graph. This was also the method used by Fleischmann [1].

Calorimetric results from CalTech, MIT, and Harwell The unusually quick scientific rejection of cold fusion in 1989 was mainly due to the reports of no calorimetric excess heat effects from CalTech, MIT, and Harwell [19–21]. Therefore, these 1989–90 publications need to be critically examined. This has been done by several groups with the conclusion that the calorimetric measurements by these three major institutions were all seriously flawed [4, 7, 22, 23]. Most of the calorimetric terms in Eq. (1) are not found in the CalTech, MIT, or Harwell publications. For example, none of these three institutions discuss the important CpMdT/dt differential equation term, and there is no mention of the PG and PW terms. In addition, the calorimetric studies were all of the short duration rather than the weeks or months of electrolysis often required for the cold fusion excess heat effects [5]. Finally, none of these institutions reported the attainment of the high D/Pd loading required for excess heat effects [12]. Furthermore, these institutions were not open-minded about the possibility of cold fusion, and this attitude may have affected their research results [24]. Problems with the CalTech calorimetry were their apparent use of short, fat cells where additional vigorous mechanical stirring was required. This stirring added an estimated 0.3°C to the cell temperature reading [19], and this reduced their cell temperature accuracy. Further analyses of the CalTech calorimetric methods shows that they generally measured changes in excess power and not the actual excess power [4, 7]. The excess power will often remain steady over long time periods where ΔPX  0. The CalTech publication reports unusual adjustments of the cell constant for the Pd-D2O experiment but not for the Pd-H2O studies [19]. Changing the cell constant can always be a method to zero out any excess power effects. A small excess power effect for Pd-D2O experiments was actually present in the CalTech report if the cell constant was not changed [7]. The major problem of the MIT calorimetry was their unexplained shifting of the raw experimental data showing a small excess power effect to give a published figure with near-zero excess power [4]. The poor sensitivity of the MIT calorimetry (40 mW) and their use of a small volume cathode (0.1  9.0 cm, V ¼ 0.07 cm3) would make it difficult for the detection of any excess power. This poor calorimetric sensitivity was likely due to their use of too much glass wool insulation which forced the main heat transport pathway to be out of the cell top into the room temperature air rather than to the constant bath temperature [23]. The Harwell calorimetry [21] showed initial periods of large endothermic cell behavior which may be explained by their neglect of the CpMdT/dt term. Most of the initial power goes into heating the cell contents, and endothermic behavior always results in experiments when this is ignored. Harwell also used several large-volume calorimeters (500 and 1000 mL) which would be much less sensitive for any excess heat effects. Another problem was that Harwell often used palladium cathodes of unfavorable geometry such as palladium beads, ribbons, and bars where there would be poor symmetry between the anode and palladium cathode. This unfavorable geometry would make it difficult to obtain high deuterium loadings. To their credit, Harwell is the only institution that made their raw experimental data available to others for independent analysis [22]. Both CalTech and MIT refused to make their experimental cold fusion data available for outside examinations.

64

Chapter 4 Fundamentals of isoperibolic calorimetric

The most serious problem with the 1989 reports of no cold fusion effects by CalTech, MIT, and Harwell is the fact that most sources of palladium materials show no cold fusion effects [2]. These three influential institutions simply gave up on their cold fusion research much too soon. My China Lake group also failed to detect any cold fusion effects during the first 6 months of research [25]. Almost all of my excess heat effects came from two sources for palladium: the special Johnson-Matthey palladium first made commercially available late in 1989 and the US Navy’s palladium-boron materials produced in 1994 [1, 2]. It remains unknown why these two sources of palladium gave excess heat effects in nearly every experiment while most other palladium sources failed to produce any cold fusion effects. A research program has been recently formed to further investigate the promising palladiumboron materials [26].

Appendix At higher cell temperatures where it is necessary to calculate the power carried out of the cell in the form of the heated D2, O2, and D2O gases generated in the cell, the PG term shown in Eq. (A.1) should be used.   PG ¼ ðI=FÞ 0:5 Cp, D2 + 0:25 CP, O2 + 0:75 P0 Cp, D2 O ΔT  0:75ðI=FÞP0 L

(A.1)

where P0 ¼ P/(P*  P) and P* ¼ PD2 + PO2 + PD2O ¼ Patm. This PG term is referenced to the bath temperature with ΔT ¼ T  Tb. The D2O vapor pressure at any cell temperature is represented by P while P* is the atmospheric pressure in the laboratory. The Cp terms are the heat capacities (J mol1 K1) for each of the three gases. The D2O electrolysis reaction for one Faraday (F) is 0.5 D2O ! 0.5 D2 + 0.25 O2, thus the coefficients of 0.5 for D2 and 0.25 for O2 to give 0.75 mol of these two gases generated per Faraday. The fraction P0 of D2O vapor in the electrolysis gases is given by Dalton’s law of partial pressures as P0 ¼ P/(PD2 + PO2) ¼ P/(P*–P). The largest term in Eq. (A.1) is the second term involving the enthalpy of vaporization of D2O (L). This heat of vaporization of D2O varies somewhat with the cell temperature with L ¼ 45.401 kJ/mol at 25°C and L ¼ 41.673 kJ/mol at the boiling point of D2O (101.42°C). The vapor pressure of D2O (P) at various temperatures is available in tables (see CRC handbooks), but it is more convenient to calculate the values from the Clausius-Clapeyron equations expressed as ln P ðD2 OÞ ¼ ΔHvap =RT + C

(A.2)

where L ¼ ΔHvap in Eq. (A.1). Assuming ΔHvap is independent of temperature, then a graph of ln P vs l/ T should be linear with a slope of  ΔHvap/R. The vapor pressure data for D2O from 20°C to 100°C (293.15–373.15 K) gives Fig. A.1. The vapor pressure was expressed in units of Torr where 1 atm ¼ 760 Torr ¼ 101.325 kPa. The resulting equation for P in Torr units is expressed by ln P ¼ 5:296830x103 =T + 20:799716

A similar equation for the vapor pressure of H2O is

(A.3)

Appendix

65

lnPD2O(g) vs 1000/T 7.0 6.5

y = –5.296830x + 20.799716

6.0

R 2 = 0.999866

lnP

5.5 5.0 4.5 4.0 3.5 3.0 2.5 2.6

2.8

3.0

3.2

3.4

(1000/T)

FIG. A.1 The vapor pressure of D2O shown as ln P versus 1000/T (R2 ¼ 0.999866).

ln PðH2 OÞ ¼ 5:152051x103 =T + 20:457211

(A.4)

These two equations can be used to calculate the vapor pressure of D2O or H2O in units of Torr (mmHg) at any cell temperature. The slope of the line gives a mean ΔHvap ¼ 44.040 kJ/mol for D2O and ΔHvap ¼ 42.837 kJ/mol for H2O. Fleischmann preferred using the Clausius-Clapeyron equation with the boiling point of D2O as 374.57 K and the enthalpy of vaporization at the boiling point as L ¼ 41,672.60 J/mol [1]. This yields the equation ln P ðD2 OÞ ¼ 6:6333184  x

(A.5)

where x ¼ 13.380846 (374.57  T)/T. The use of Eq. (A.5) yields more accurate vapor pressures for D2O at higher cell temperatures near the boiling point where PG becomes large. A third equation for the vapor pressure of D2O is given on p. 88 of Ref. [2] where the vapor pressure is expressed in atmospheres. As an example, the vapor pressure of D2O at 90°C is 495.72 Torr. Eq. (A.5) yields 498.96 Torr, Eq. (A.3) gives 499.66 Torr and the China Lake equation [2] provides 503.29 Torr. All three equations are within 1.5% of the experimental value. The integration of Eq. (17) for the cooling of Dewar cell yields [9]   lnðTo  Tb Þ=ðT  Tb Þ  lnðTo + Tb Þ=ðT + Tb Þ + 2 tan 1 ðT=Tb Þ  tan 1 ðTo =Tb Þ ¼ 4Tb 3 kR t=Cp M

(A.6)

The major term in Eq. (A.6) is the first term which is the same as the left-hand side (LHS) of Eq. (14). The additional LHS terms in Eq. (A.6) serve as a small correction term for heat transferred by radiation. Note that 4 T3b kR ¼ kC0 where kC0 is the corresponding cell constant for heat conduction. A similar relationship is found for PR ¼ kR (T4  T4b) using T ¼ Tb + ΔT which yields PR ¼ kR [4T3b ΔT + 6 T2b ΔT2 + 4 Tb ΔT3 + ΔT4] where ΔT ¼ T  Tb. The largest term is 4 T3b ΔT, thus PR   4 T3b kR ΔT ¼ kC0 ΔT where kC0 ¼ 4 T3b kR. This 4 T3b kR ΔT term was often used in the F-P publications for the small effect

66

Chapter 4 Fundamentals of isoperibolic calorimetric

of heat conduction in the Dewar calorimeter [1, 5]. This same term shows up mathematically in Eq. (A.6). Further information about the various calorimetric terms is found in the Appendix of previous publications [4, 9].

Acknowledgments My cold fusion research and writing efforts for more than 10 years have been supported by an anonymous fund at the Denver Foundation through the Dixie Foundation at Dixie State University. An adjunct faculty position at the University of LaVerne and a Visiting Professor affiliation at Dixie State University are also acknowledged. The author especially thanks Martin Fleischmann and Stanley Pons for the development of the various modeling equations required for accurate electrochemical isoperibolic calorimetry.

References [1] M.H. Miles, M. Fleischmann, M.A. Imam, Calorimetric analysis of a heavy water electrolysis experiment using a Pd-B alloy cathode, Naval Research Laboratory Report, NRL/MR/6320-01-8526, March 26, 2001, 155 p. https://lenr-canr.org/acrobat/MilesMcalorimetrd.pdf. [2] M.H. Miles, B.F. Bush, K.B. Johnson, Anomalous effects in deuterated systems, Naval Air Warfare Center Weapons Division Report, NAWCWPNS TP8302, September, 1996, 98 p. https://lenr-canr.org/acrobat/ MilesManomalousea.pdf. [3] M.H. Miles, M. Fleischmann, Measurements of excess power effects in Pd/D2O systems using a new isoperibolic calorimeter, J. Condensed Matter Nucl. Sci. 4 (2011) 45–55 (See also ICCF-15 Proceedings, Rome, Italy, October 5–9, 2009, pp. 22–26). https://lenr-canr.org/acrobat/BiberianJPjcondensedc.pdf#page¼53. [4] M.H. Miles, M. Fleischmann, Twenty year review of isoperibolic calorimetric measurements of the Fleischmann-Pons effect, in: D.J. Nagel, M.E. Melich (Eds.), Proceedings of 14th International Conference on Cold Fusion (ICCFf-14), vol. 1, University of Utah, Salt Lake City, 2008, pp. 6–10. https://lenr-canr.org/ acrobat/MilesMisoperibol.pdf. [5] M. Fleischmann, S. Pons, M.W. Anderson, L.J. Li, M. Hawkins, Calorimetry of the palladium-deuteriumheavy water system, J. Electroanal. Chem. 287 (1990) 293–348. https://lenr-canr.org/acrobat/ Fleischmancalorimetr.pdf. [6] S. Pons, M. Fleischmann, The calorimetry of electrode reactions and measurements of excess enthalpy generation in the electrolysis of D2O using Pd-based cathodes, in: T. Bressani, E. Del Guidice, G. Preparata (Eds.), The Science of Cold Fusion: Proceedings of the II Annual Conference on Cold Fusion, Italian Physical Society, Bologna, Italy, 1991, pp. 349–362. ISBN 88-7794-045-X, https://lenr-canr.org/acrobat/ PonsSthecalorim.pdf. [7] M.H. Miles, B.F. Bush, D. Stilwell, Calorimetric principles and problems in measurements of excess power during Pd-D2O electrolysis, J. Phys. Chem. 98 (1994) 1948–1952. [8] M.H. Miles, Excerpts from Martin Fleischmann letters, J. Condensed Matter Nucl. Sci. 19 (2016) 210–218. https://lenr-canr.org/acrobat/BiberianJPjcondensedr.pdf#page¼218. [9] M.H. Miles, The Fleischmann-Pons calorimetric methods, equations and new applications, J. Condensed Matter Nucl. Sci. 24 (2017) 1–14. https://lenr-canr.org/acrobat/BiberianJPjcondensedw.pdf#page¼13. [10] M. Fleischmann, S. Pons, Calorimetry of the Pd-D2O system: from simplicity via complications to simplicity, Phys. Lett. A 176 (1993) 118–129. https://lenr-canr.org/acrobat/Fleischmancalorimetra.pdf. [11] M. Fleischmann, M.H. Miles, The instrument function of isoperibolic calorimeters: excess enthalpy generation due to parasitic reduction of oxygen, in: P.L. Hagelstein, S.R. Chubb (Eds.), Condensed Matter Nuclear Science: Proceedings of the 10th International Conferences on Cold Fusion, Cambridge, MA, 24–29 August

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[13]

[14]

[15]

[16] [17] [18] [19]

[20]

[21]

[22]

[23] [24] [25]

[26]

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2003, World Scientific Publishing Co., Singapore, 2006, pp. 247–268. https://lenr-canr.org/acrobat/ Fleischmantheinstrum.pdf. M.H. Miles, M.C. McKubre, Cold fusion after a quarter-century: the Pd/D system, in: D. Fletcher, Z.-Q. Tian, D.E. Williams (Eds.), Developments in Electrochemistry: Science Inspired by Martin Fleischmann, John Wiley and Sons, United Kingdom, 2014, pp. 245–260. ISBN 9781118694435. M.H. Miles, Correlation of excess enthalpy and helium-4 production: a review, in: P.L. Hagelstein, S. R. Chubb (Eds.), Condensed Matter Nuclear Science, ICCF-10 Proceedings 24–29 August 2003, World Scientific, Singapore, 2006, pp. 123–131. ISBN 981-256l-564-7, https://www.lenr-canr.org/acrobat/ MilesMcorrelatioa.pdf. M.H. Miles, R.A. Hollins, B.F. Bush, J.J. Lagowski, Correlation of excess power and helium production during H2O and D2O electrolysis using palladium cathodes, J. Electroanal. Chem. 346 (1993) 99–117. https:// lenr-canr.org/acrobat/MilesMcorrelatioa.pdf. M. McKubre, F. Tanzella, P. Tripodi, P. Hagelstein, The emergence of a coherent explanation for anomalies observed in D/Pd and H/Pd systems: evidence for 4He and 3H production, in: F. Scaramuzzi (Ed.), Proceedings of the 8th International Conference on Cold Fusion, Italian Physical Society, Bologna, Italy, 2000, pp. 3–10. ISBN l88-7794-256-8, https://lenr-canr.org/acrobat/McKubreMCHtheemergen.pdf. S. Pons, M. Fleischmann, Concerning the detection of neutrons and X-rays from cells containing palladium cathodes polarized in heavy water, IL Nuovo Cimento 105 (1992) 763–772. S.E. Jones, E.P. Palmer, J.B. Czirr, D.L. Decker, G.L. Jensen, J.M. Thorne, S.F. Taylor, J. Rafelski, Observation of cold nuclear fusion in condensed matter, Nature 338 (1989) 737–740. S. Pons, M. Fleischmann, Heat after death, Trans. Fusion Technol. 26 (4T) (1994) 87–95. https://lenr-canr. org/acrobat/PonsSheatafterd.pdf. N.S. Lewis, C.A. Barnes, M.J. Heben, A. Kumar, S.R. Lunt, G.E. McManis, G.M. Miskelly, R.M. Penner, M. J. Sailor, P.G. Santangelo, G.A. Shreve, B.J. Tufts, M.G. Youngquist, R.N. Kavanagh, S.E. Kellogg, R. B. Vogelaar, T.R. Wang, R. Kondrat, R. New, Searches for low-temperature nuclear fusion of deuterium in palladium, Nature 340 (1989) 525–530. D. Albagli, R. Ballinger, V. Cammarata, X. Chen, R.M. Crooks, C. Fiore, M.P.S. Gaudreau, I. Hwang, C.K. Li, P. Lindsay, S.C. Luckhardt, R.R. Parker, R.D. Petrasso, M.O. Schloh, K.W. Wenzel, M. S. Wrighton, Measurements and analysis of neutron and gamma-ray emission rates, other fusion products, and power in electrochemical cells having Pd cathodes, J. Fusion Energy 9 (1990) 133–148. D.E. Williams, D.J.S. Findlay, D.H. Craston, M.R. Sene, M. Bailey, S. Croft, B.W. Hooten, C.P. Jones, A.R. J. Kucernak, J.A. Mason, R.I. Taylor, Upper bounds on ‘cold fusion’ in electrolytic cells, Nature 342 (1989) 375–384. M.E. Melich, W.N. Hansen, Some lessons from 3 years of electrochemical calorimetry, in: H. Ikegami (Ed.), Frontiers of Cold Fusion, Universal Academy Press, Tokyo, Japan, 1993, pp. 397–400. ISBN 4-946443-12-6, https://lenr-canr.org/acrobat/MelichMEsomelesson.pdf. M.H. Miles, P.L. Hagelstein, New analysis of MIT calorimetric errors, J. Condensed Matter Nucl. Sci. 8 (2012) 132–138. https://lenr-canr.org/acrobat/BiberianJPjcondensedg.pdf#page¼138. E.F. Mallove, Fire From Ice: Searching for the Truth Behind the Cold Fusion Furor, John Wiley and Sons, New York, 1991. pp. 136–147, 172. ISBN 0-471-53139-1. Cold fusion research – a review of the Energy Research Advisory Board to the United States Department of Energy, DOE/S-0073 DE90 005611, November 1989, p. 24. https://lenr-canr.org/acrobat/ERABreportofth. pdf. S.B. Katinsky, D.J. Nagel, M.H. Miles, M.A. Imam, LEAP: The LENRIA Experiment and Analysis Program, in: Program and Abstracts, 21st International Conference on Condensed Matter Nuclear Science (ICCF-21), Colorado State University, Fort Collins, Colorado, 3–8 June 2018.

CHAPTER

Can clean and stable deuterium loading and well-tailored microstructure improve reproducibility?

5 Hiroo Numata

Graduate School of Metallurgy and Ceramics Science, Tokyo Institute of Technology, Tokyo, Japan

Introduction The poor reproducibility of cold fusion experiments has been attributed to localization of the reactive region and insufficient understanding of both optimal sample pretreatment methods and deuterium loading behavior. Here, we observe the morphologies of the surface and interior of postelectrolysis Pd rod, conduct in situ measurements of their physicochemical properties, and finally propose a new and reproducible experimental method for cold fusion experiments. Since the 1990s, new measurement methods for hydrogen-metal systems have been developed in the field of material science. New information regarding the microscopic hydrogen distribution within metals, particularly the strong interaction between hydrogen and lattice defects and vacancies, is also gradually coming to light. Considering these circumstances, we have incorporated views from studies that used these new experimental methods to clarify our experimental results. First, in Section “Morphology of deuterated thick Pd rod during long-term electrolysis in 0.1 M LiOD” we describe the results of deuterium absorption on a well-annealed, thick Pd rod during long-term electrolysis in 0.1 M LiOD, accompanied with neutron measurements and observation of postelectrolysis Pd electrodes. In this section, we describe the important aspects of the sample pretreatment method and experimental apparatus that enable a stable and clean long-term experiment. Later in the section, we compare the surface and internal morphologies of postelectrolysis Pd sample with those of natural phenomenon of the earth, and discuss peculiar morphologies observed in a deuterated Pd electrode. In addition, it is inferred that the improved reproducibility of cold fusion experiments could be attainable by elucidating the Pd loading behavior in the field of material science.

Cold Fusion. https://doi.org/10.1016/B978-0-12-815944-6.00005-1 # 2020 Elsevier Inc. All rights reserved.

69

70

Chapter 5 Clean loading and microstructure in Pd-D

Morphology of deuterated thick Pd rod during long-term electrolysis in 0.1 M LiOD Experimental

Cold fusion experiments at ambient temperatures have been conducted by electrolysis of heavy water on a Pd electrode and on other stable metals, e.g., Ni and Ti. Fig. 1A shows the electrolysis cell, in particular: the dimensions and arrangement of the electrode, the counter electrode, and the electrolyte. The constituent components of the measurement systems for excess heat generation and neutron emission are not shown, nor is an isothermal water bath used to control the cell temperature. The experimental apparatus and detailed procedures are described below. The basic goals of the cell design are: • •

long-term maintenance of pure electrolyte and clean electrolytic cell conditions and ensuring stable current supply lead for the Pd rod and stable reference electrode.

Moreover, a simpler system without recombiner catalysts was devised, reducing contamination. The remaining sources of contamination were corrosion products from the surface of the cell components, i.e., transparent quartz, the bottom surface of a silicon rubber stopper, plated Au and dimensional stable like anode, which might be exposed to caustic alkali liquid and its film. As it turned out, contamination was minimal, and thus the contaminants were mostly due to periodic D2O replenishing.

Electrolyte and experimental cell A 0.1 M LiOD solution was prepared by addition of Li2O (Wako pure chemicals: 95%) into D2O (Isotech: 99.9%). The concentration of LiOD solution was substantially increased during the course of electrolysis because a small amount of 0.1 M LiOD was poured into the cell every day to replenish

11 7 6

5 8

7

10 2 53

1

4

3 20

9 32

9

1 Pd rod cathode 2 Anode 3 0.1M LiOD electrolyte 4 Double jacketed transparent quartz cell 5 Addition tube 6 Thermocouple 7 Guide for deuterium gas 8 Guide for oxygen gas 9 Circulating water inlet 10 Circulating water outlet 11 Current supply unit: mm

(B)

(A) FIG. 1 Schematic diagram of electrolytic cell for deuterium absorption on a Pd electrode in 0.1 M LiOD (A), and Pd electrode’s optical micrograph of cross-sectional surface area of electrode (B).

Morphology of deuterated thick pd rod during long-term electrolysis in 0.1 M LiOD

71

it. During long-term electrolysis, incremental fills were made with pure heavy water to minimize the effect of electrolyte concentration on the electrochemical systems. The experimental cell (about 130 mL volume) was made out of transparent quartz, which has a water jacket. The temperature in the jacket was controlled at 40 and 50
0.5°C. The material of the cell container has to be corrosion resistant with a caustic hot aqueous solution, so Teflon could be satisfactory. In this case, transparent quartz was prepared as the container, because it exhibited more corrosion resistance than conventional Pyrex glass and nontransparent quartz. In addition, transparent quartz is superior to Teflon for the visual observation of the H evolution reaction. The electrode potential was referred to the potential of dynamic type (α + β) PdD reference electrode. The counter electrode lead orifice served as the gas outlet port.

Electrode and electric leads A Ti rod (3 mm ϕ) Au plated served as an electric lead. The Ti rod was prepared with abrasion and Ni strike plating. It was screwed into the upper end of the Pd electrode. The Pd electrodes, which were thick Pd rods, were made by casting, and thus high purity Pd ingots were cast into a high purity alumina tube in a flow of Ar (2 L/min). Subsequently, Pd cast electrodes exhibited highly grown grains, confirmed by optical microscopic observation.

The working-electrode and counter-electrode configuration The working electrode was set approximately in the center of the cylindrical space circumscribed by the counter electrode. This configuration ensures that the local current density on the surface of the working electrode is homogenous. Such idealized cylindrical geometry allows the conditions for D absorption, i.e., the α and β phases appearance concentric and, therefore, the stress state of the electrode is a function of radial distance. We successfully performed nonintermittent electrolysis for 2 and ca. 6 months in two experimental runs, referred to as Exp. 1 (electrode geometry: 9 mm ϕ, 5.3 cm long) and Exp. 2 (21 mm ϕ, 3.2 cm long), respectively. The electrolysis details are shown in Table 1. The characteristics of both the experimental procedures are [1, 2]: (1) Cast and thick rod Pd electrode (emery paper abrasion or acid treatment) (2) Preelectrolysis using disposable Pd plate for electrolytic cell cleaning Table 1 Experimental conditions of Exp. 1 and Exp. 2: Pretreatment and current density. Run No.

Current density (mAcm22)

Pretreatments (Acid treatment: A, Polishing: P, Evacuation: E)

Exp. 1: Dimension of electrode 9.0φ, 53 mm long First Second Third Fourth

0.05–40, 40–500 40 40 40

Cast, 800°C anneal (106 Torr), A P, A, E E, P, A E, P, A

Exp. 2: Dimension of electrode 21φ, 32 mm long First

0.05–102.4

Cast, 800°C anneal (106 Torr), D2 gas charge, A

72

(3) (4) (5) (6)

Chapter 5 Clean loading and microstructure in Pd-D

Annealing (a very low dislocation density) Preparatory gas phase absorption of D2 (D/Pd ¼ 0.36) Increase in electrolysis current in a form of stepwise; and Temperature cycling

The results of neutron measurement are described elsewhere [1, 2].

Microstructure characterization using scanning electron microscope (SEM) A cross-sectioned sample was prepared by sectioning an electrode in the traverse and radial directions. Then the sample was polished using 6 μm diamond paste and lightly etched by dilute hydrochloric acid.

Results and discussion

Microstructure of thick Pd rod and dilation under long-term electrolysis—Exp. 1 To measure the diameter at three positions, as shown in Fig. 2, a sample was dismounted from the cell after interrupting electrolysis and carefully re-installed. This procedure was repeated four times (see Table 1), at intervals of two months or less. In Fig. 2, the dilation of the Pd electrode was plotted against the run number. For the first run, the dilation at the bottom end showed a maximum of 7%, while those in the upper regions exhibited a lesser extent than that at the bottom. During the second, third and fourth runs, the values at these positions asymptotically approached 7.8%–8.3%. It is noted that a high count rate of neutron (CRN) and energy spectrum of 2.45 MeV appeared in the first run, during which the largest dilatation occurred. Although we have found no explanation for the relation between a neutron

A B C

e (%)

10

5

7.8 ~8.3%

0

1st

2nd

3rd

4th

Pd D(0.36 + d )

FIG. 2 Radial dilation: ε% of postelectrolysis Pd electrode at three positions (A–C) during first to fourth runs. Reproduced with permission from H. Numata, R. Takagi, I. Ohno, K. Kawamura, S. Haruyama, Neutron Emission and Surface Observation During A Long-Term Evolution of Deuterium on Pd in 0.1 M LiOD, Conf. Proc. vol. 33, ACCF2. The Science of Cold Fusion. 1991, p. 71.

Results and discussion

73

emission and the largest expansion of a material, it is helpful in understanding the anomaly to inspect the inside of the specimen with metallographic observations [1, 2]. The microstructure of the cross-sectional surface area of the apex is shown in Fig. 1B. As shown in Fig. 1B, the sample as a whole consisted of four columnar grains (the cross-sectioned circle divided into four quadrants), each of which looked like it had grown inside from a crucible wall during cooling, based on a metallographic examination. Since such a peculiar grain structure could not be obtained by conventional metal formation, another mechanism for grain boundary change is considered. Based on the optical micrograph of four columnar grains, we infer that long prisms have grown longitudinally along the electrode center. However, this explanation was unexpected, since the temperatures of the electrode and the outside of the counter electrode showed no significant change corresponding to a heat burst. Hence, this is only likely to happen when low heat evolution in the interior lasts a long time; long enough to promote abnormal grain growth. Coupland et al. [3] found the recrystallized grain near the area of the electrical connection. The recrystallization temperature of hydrated Pd was determined where the sample was subjected to high pressure distortion [4]. The grain growth of V nanocrystalline in a H atmosphere was accelerated, where H could assist grain growth by reducing the formation energy of vacancies [5]. Comparing the result of high CRN observed the heat evolution in the interior occurred moderately, resulting in the symmetrical grain structure.

Microstructure of thick Pd rod under long-term electrolysis—Exp. 2 Visual observations of the electrode surface show that it is characterized by three different morphologies, which are schematically drawn in Fig. 3A–C. We found no surface crack but two faults (see Fig. 3C), marked blisters (A) and blisters with a feather-like pattern arranged in two arrays (B) [1]. These morphologies were located at 120 and 150 degrees right turns from the reference position: (C). Thus, there appeared to be two line imperfections: a long fault and a center line of the feather pattern all over the surface. From the above observation, in the view of the cross-sectional area (see Fig. 5) the line imperfections, which traverse the rod interior, thrust out to one side at the fault and the other side at the center of the feather.

SEM views of the electrode surface Fig. 4A–D shows the typical SEM (JOEL model T-330 20 kV) images of the electrode surface where they exhibit a plain terrace appearing slip bands, and the long fault partly covered by gray overlayer, before the chemical etching pretreatment [7] (A), holes that are gathered to long fault (B), double slip (C), and vortex (D). These morphologies of the surface or interior can be understood as the result of long-term or repeated deuterium absorption in a Pd electrode. During the absorption, deuterium diffuses into interstitial sites accompanied with stress field, and thereby occasionally could generate a dislocation. The continued absorption might promote the dislocation motion, resulting in a slip band on the surface. Note that the appeared morphologies are accomplished by long-term and clean electrolysis using a well-annealed sample. It was found that these holes (Fig. 4B) were concentrated near the long fault line (Fig. 4A), which was substantiated by measuring the hole distribution profiles (hole density plot vs distance from fault line) at three positions along the long fault [1]. Thus, it is considered that morphology, faults, and holes are all relevant. Combining the optical microscopic observation and the SEM images of the fault gathering holes, the cross-sectional microstructure of deuterated Pd shows inhomogeneous structure, a core,

74

Chapter 5 Clean loading and microstructure in Pd-D

ℰ 3.27 %

120 degrees

150 degrees

150 degrees ℰ 1.66 %

(A)

(B)

(C)

FIG. 3 Surface appearance of postelectrolysis Pd electrode showing blister (A), feather pattern, and center line indicates reference position (B), and two long and short faults (C). Reproduced with permission from H. Numata, R. Takagi, I. Ohno, K. Kawamura, S. Haruyama, Neutron Emission and Surface Observation During A Long-Term Evolution of Deuterium on Pd in 0.1 M LiOD, Conf. Proc. vol. 33, ACCF2. The Science of Cold Fusion. 1991, p. 71.

and blanket, as is schematically illustrated in the right of Fig. 5. It consists of two big columnar grains (core) in the interior, columnar ones with random orientations near the surface (blanket), and fault and holes on the surface. It seems that the latter grain structure (blanket) remained unchanged throughout the long-term electrolysis, while the core was recrystallized, resulting in grain growth. During the longterm deuterization, the lattice of the two big crystals expands in a different direction aligned in the center, which causes a fault and/or regularly arranged holes on the surface. Then the holes were formed around the fault, whereupon the deuterium gas, including the reaction products of the inside, gushed out. It is interesting to compare the formation process of the long fault and blisters (holes) on the Pd surface with those of a crater and faults: the natural phenomena and mantle movement inside the Earth (see the left of Fig. 5). It is known that the Earth evolves heat constantly in the interior. The mantle movement thereby induces cleavage in the crust, accompanied with craters and faults, as shown in the left of Fig. 5. This phenomenon seems like that of the misoriented Pd grains, which causes a fault on the blanket, as shown in the right of Fig. 5. That is, both movements of the mantle and the deuterated Pd grains are consistent, and hence the hole-formation around the long fault on the Pd surface is attributable to gas evolution, like volcano gas from a volcanic eruption. Hence, we can explain the microstructure of the Pd electrode: two large grains in the interior surrounded by random columnar grains can be attributable to the occurrence of heat evolution and plastic deformation in the interior.

Results and discussion

75

e

ac

rr Te

Fault

(A)

(B)

(C)

(D)

FIG. 4 SEM of Pd electrode surface showing exposed terrace along the long fault (A), holes on Pd electrode surface (B), double slip (C), and vortex, which appeared on Pd electrode surface (D). Reproduced with permission from Ref. H. Numata, I. Ohno, In Situ Potentiometric, Resistance and Dilatometric Measurements of Palladium Electrodes During Repeated Electrochemical Hydrogen Absorption, Fusion Technol. 38 (2000) 206. Copyright 2000, Taylor & Francis.

Another similarity of the two phenomena might be in an earthquake caused by mantle movement and the enormous emission of energetic particles, where the latter has been frequently recognized as evidence of a cold fusion reaction. Recently, the Kobe earthquake was categorized as an active-fault type, which appeared as a trace of faults on the ground. The anomalous emission of charged-particles was reported before the earthquake and was confirmed by the analysis of a jet-like cloud, which was formed vertically from the ground [8]. It is quite reasonable to suppose that the charged-particle emission observed was a precursor to giant ground slippage that generated faults on the Earth’s surface. According to that earthquake mechanism, the traces of fault and holes on the deuterated Pd surface could be a precursor to the enormous emission of charged particles involving neutrons as a result of a cold fusion reaction. Thus, several similarities are found between the behavior of a deuterated Pd electrode and geological phenomena on the Earth.

76

Chapter 5 Clean loading and microstructure in Pd-D

Deuterated Palladium Gas, particle gush

Earth’s mantle Energy release

Hole

Fault

Crater, fault

Movement Plate (crust) Mantle Core

Heat Grain boundary

Single X’al

FIG. 5 Mechanism of surface holes formed along the fault of a Pd rod during long-term electrolysis in 0.1 M LiOD. Reproduced with permission from H. Numata, R. Takagi, I. Ohno, K. Kawamura, S. Haruyama, Neutron Emission and Surface Observation During A Long-Term Evolution of Deuterium on Pd in 0.1 M LiOD, Conf. Proc. vol. 33, ACCF2. The Science of Cold Fusion. 1991, p. 71. Copyright 1991, Italian Physical Society.

Fig. 4C shows the other morphology of double slip of the surface. It is elucidated that two morphologies, including blister and its surrounding slip bands, are identified as the same as those linked to the third stage in the FCC single crystal stress-strain curve [9]. Comparing the stress–strain curve of similar metal and the dilations of the deuterated Pd electrode’s diameter during first to fourth runs (shown above), it is concluded that the area showing double slip is subjected to high stress/strain, which is characterized as a “local” phenomenon. Fig. 4D shows a significant morphology termed as a “vortex” on a thick rod Pd electrode surface after long-term electrolysis in 0.1 M LiOD [10]. This is not substance that adhered on the surface. It is material on which the pattern was deeply impressed in the shape of a ditch. The formation mechanism of this morphology has been investigated using PC simulation. Although a precise description is not shown here, a rudimentary pattern of rotating particles’ locus as the trace of vortex has been obtained based on the scavenger process 1 and 2 of N-cycle model (see Fig. 7) [11].

SEM views of the electrode interior Fig. 6A–C shows SEM images of the cross-sectional surface of the deuterated Pd electrode (Exp. 2). In Fig. 6C, the enlarged image of a void is characterized by a sharp wall and surrounded by a nonporous structure. In Fig. 6B the whole matrix is composed of voids and a circumference-like blanket, and nanopores distributed over the rest of the void’s areas. For morphology evolution, the characteristic feature of porous structure (Fig. 6A) closely resembles the morphology of nanoporous metal by dealloying; therefore, the feature might reflect some phase transformation. It is seen that the overall image of voids (see Fig. 6B) is similar to the matrix of the Ni-H system where H absorption is performed under high H pressure [12].

Nuclear reaction cycle model Since the results of the microscopic observations are not real-time information from electrolysis in progress (unlike measurements of the instantaneous electrode potential, CRN, or the bath temperature), it is impossible to know when such microscopic structures appeared, or the time correlation with CRN.

Results and discussion

77

Porous structure Void

15kv

5 μm

5k

20kv

(A)

3.5k

5 μm

(B)

20kv

20k

1 μm

(C) FIG. 6 SEM of cross-sectional surface of a deuterated Pd electrode showing porous structure (A), porous structure and voids (B), and void and circumference (C).

However, it is possible to solve such problems with an analogy with a natural phenomenon, as presented later. We assume the cold fusion reaction is a complicated phenomenon. Thus, our experiments have been focused on understanding the individual phenomena that make up the cold fusion phenomenon. Given that purpose, by considering the phenomenon as an energy engine, N-cycle model [6, 13, 14] it was proposed from a point of view of its continuous operation (4 reciprocating cycle). It consists of four sequential processes: intaking/compression-triggering-reaction-scavenging, taking into account of the correspondence to long-term electrolysis of a thick rod Pd (as shown in the right of Fig. 5). The following two key benefits result: (1) enhanced reproducibility of the experiments is achieved by continuing the cycle (2) after systematic consideration the hidden process could be explored Let us examine the correspondence of the N-cycle model to the phenomena of the experiment (see Fig. 7). In the absorption/compression process of the reactants, a barrier layer of deuterium migration by compression stress (which also corresponds to the B side of the single-side electrolysis referred to in the report [6, 14]) is formed as absorption is in progress, resulting in formation of a

78

Chapter 5 Clean loading and microstructure in Pd-D

Outside trigger

Heat and/ or products emission

Inside trigger

Compressed region

Reaction

1

Deuterium over potential to surface of specimen brittle part Intake of reactant follwed by compression

2

Scavenger

to neighboring reaction vessels

Deuterium and products Reaction vessel: Many regions surrounded by strained tough zone

FIG. 7 Nuclear reaction cycle model.

vessel composed of the interior and blanket (corresponding to the barrier layer for D outgas). In the compression process, the interior appears to make expansion owing to the continued absorption, i.e., a part of the generated deuterium is contributed to further slow absorption. However, the compression pressure of the blanket brings a kind of enhanced pinch effect, resulting in an increase of the internal pressure (in what is otherwise an increase in stress). In the reaction process a reaction should be caused by an external trigger that is applied to the inside (i.e., injection of energetic particles from the outside) or by an internal trigger. As an actual internal trigger, case I and II (also shown in the report [1, 10, 15]) depends on whether the role of the fault formation is the final step of the reaction process, i.e., simultaneously with the reaction, or whether it is a reaction induced by allowing the fault formation to provide the blanket with a path to expedite further absorption [15]. In case I, emission of the neutrons and charged particles at first occurs as a precursor phenomenon of the cold fusion reaction similar to an earthquake as listed in [1, 6]. In case II, in the compression process, the D/Pd of a vessel could be insufficient to the reaction. Hence, the occurrence of further absorption allows an increase of the D/Pd ratio, resulting in triggering of the cold fusion reaction. In the process of scavenging, very many holes, concentrated on both sides of the fault, found in the experiment [1] were identified as discharge ports of the reaction products (including unreacted deuterium) [15, 16].

Microstructural change of a Pd rod during repeated cathodic and anodic electrolysis in glycerin-phosphoric acid: First absorption of H in Pd (x < 0.8) in the C mode Storms suggested that irreproducible data could be attributed to D2 out-diffusion through surface cracks from the deloading behavior of β-PdD [17]. As discussed in N-cycle model, the importance of the microstructure of deuterated Pd is emphasized in reproducibility of cold fusion experiments. Thus, it is

Results and discussion

79

interesting to know how the microstructural changes; evolution of lattice defects and vacancy-clusters with an increase in the H/Pd ratio could have an influence on reaction sites of a cold fusion reaction. Although the cold fusion mechanism, which might be closely related with reaction sites, has been conjecture, we will study the relationships between H-induced lattice defects and the known cold fusion phenomena. In the former section, the morphologies of postelectrolysis Pd exhibited the heavily deformed features involving slip bands, holes, and long faults. They basically occurred by deuterium penetration from the surface to substrate, during which defects, i.e., dislocation and vacancy, were formed, concurrently. In the case of long-term H evolution, accumulation, and redistribution of such defects could lead to the microstructural changes shown above. However, there is a lack of research data on how such microstructural changes with composition occur during loading. Hence, for a precise understanding of phase-change and microstructural change of a Pd electrode during H (D) absorption (i.e., loading), in situ measurements of the electrode potential, dilation, and resistance are of interest under well-controlled H absorption. In Section “Microstructural change of a Pd rod during repeated cathodic and anodic electrolysis in glycerin-phosphoric acid: First absorption of H in Pd (x < 0.8) in the C mode” the experimental data from the Pd-H system is considered identical to the Pd-D data.

Experimental The absorption and desorption of H in Pd rod electrodes (0.8 and 2 mm ϕ, 50 mm length, 99.95%) were performed by applying galvanostatic cathodic pulse currents in glycerin and phosphoric acid (abbreviated as first or repeated C mode), as shown in Fig. 3 of Ref. [6]. In the repeated C mode, H absorption by cathodic currents was first conducted until x of 1.0, followed by potentiostatically controlled anodic current to recover the initial desorbed x. A set of absorption and desorption discharges was repeated until the repetition number was attained. After each galvanostatic discharge for a fixed number of hours, the potential, dilation, and resistance of Pd were measured after they reached a steady state. To ensure the loading level, hydrogen concentration (the H/Pd ratio: x) is given by the summation of each increment of the concentration converted by the charges (current multiplied by time of electrolysis), in accordance with Faraday’s law. In situ measurements are the best method of assuring exact coincidence among those measured variables.

Results and discussion Fig. 8 shows the in situ measured potential (E), dilation (Δl/l0), and resistance (R/R0) changes as a function of x (H/Pd ratio) under the first C mode. The latter two variables are expressed as ratios; measured values divided by initial ones, where Δl, l0, and R0 denote incremental dilation, initial length, and initial resistance, respectively. The term “first” means that the sample is characterized as free from bearing deformation due to H absorption/desorption reaction. In Fig. 8 the concentration αmax is the limit of the α phase, βmin is the limit of the α + β phase coexistence, βtr is the transition from the β phase to β + PdH2 x, Vmin is the onset of the β + void coexistence region, and Rtr is the transition from increasing resistance to a damped one. In Fig. 8 the lower inset shows α single, α + β phase coexistence, β single, and β + void coexistence regions, where the corresponding microstructures are schematically illustrated. Fig. 8 also shows the percentage (%) of different phases. As for the potential (E) in Fig. 8, when x reaches αmax, a phase change from the α phase to the β phase begins. In the H/Pd ratio: αmax  βmin, the potential exhibits constant value at 0.18 to 0.20 V,

Chapter 5 Clean loading and microstructure in Pd-D

Coulommetrically obtained H/Pd ratio 0.20 0.40 0.60 0.80

–0.16 (a) –0.18 –0.20 –0.22 Ca max –0.24 –0.26 –0.28 –0.30 100

Phase

E (a + b)

1.6 Cb min

DI/Io

R/Ro

1.4

(b) Cb tr

C Vmin (b + void)

1.2 1.0

b

a

0.020

0.010

0

PdH2-X Void

0%

a

1.0 1.8

C Rtr

Dilation, DI/Io

Potential, E/V vs SCE

0

Resistance ratio, R/Ro

80

b

PdH2-X

Void

Tunnel

FIG. 8 Schematic of the evolution of phases and voids of Pd-H system as a function of H/Pd ratio during the first C mode. Reproduced from H. Numata, I. Ohno, In Situ Potentiometric, Resistance and Dilatometric Measurements of Palladium Electrodes During Repeated Electrochemical Hydrogen Absorption, Fusion Technol. 38 (2000) 206.

where the (α + β) two phases coexist; it then transitions to another constant value at βmin. The (β + void) coexisting region above Vmin has constant value at 0.28 V that is due to the coexistence of the β phase and voids. Above βmin, the lattice constant of the β phase was considerably smaller than that obtained from gas equilibrium experiment [6]. This suggests that the electrochemically formed shrunken β phase possessing strained regions might be one cause of void formation, accompanied with the potential less noble shift at C(βtr). Shown below is the description focusing on the coincidence among the potential, resistance, dilation, and apparent molar volume during the first C mode. As shown in Fig. 9A, the potential decreases with increasing x within the single α phase and reaches a constant value corresponding to the (α + β) coexistence (two-phase coexistence region). Meanwhile, the resistance monotonically increases at a steady slope with respect to x, and the dilation similarly rises. The corresponding apparent molar volume is the slope of the plot of dilation vs x and, therefore, has a constant value. In the (α + β) two-phase coexistence region, where the potential is constant and dilation and resistance vary, the latter two increase at a constant slope with respect to x. Consequently, the apparent molar volume has a constant value in this region, as seen in Fig. 9B. Thus, the potential exhibits the single α phase and the (α + β) phase coexistence at x < βmin, where the apparent molar volume follows two constant values (1.64 (α phase) and 0.40 (α + β coexistence) cm3/mol). On the other hand, where x is at least βmin, the potential begins to transition to a decline; the slope of the dilation increases at first and then begins to decrease. Here, the apparent molar volume changes to form a single peak, as shown in the figure. The slope of the resistance begins to decrease at the starting point of the potential transition at x βtr and approaches 1.8 at C(Rtr). Tripodi et al. investigated the effect of H insertion on the resistance and strain of a Pd electrode

0.024

1.9

−0.18

0.020

1.8

(a + b)

(a)

C(btr)

−0.20

0.016

−0.22

C(amax)

C(bmin)

0.012

−0.24

(b)

−0.26

(b +void)

0.004

−0.28 −0.30

(A)

0.008

Dilation, Δl/l0 Resistance ratio, R/R0

Potential , E/V vs SCE

−0.16

C(Vmin)

0.20

0.40

0.60

1.0

0.80

Coulometrically obtained H/Pd ratio

1.0

1.7 (a)

1.6 1.5

0.8 C(Rtr)

C(amax)

1.4

(b+void)

(b)

1.3 (a + b)

1.2

C(bmin)

1.0

(B)

0.6 0.4

C(Vmin)

0.2

1.1

0 0

1.2

C(btr)

0.20 0.40 0.60 0.80 Coulometrically obtained H/Pd ratio

0

1.0

0

Apparent molar volume, VH/cm3(g atom H)−1

81

Results and discussion

FIG. 9 The C mode potential, dilation, resistance, and apparent molar volume as a function x of the first C mode absorption at 40°C. (A) Potential (□) and dilation (n) as a function of x; (B) resistance (△) and apparent molar volume (◊) as a function of x.

Micro voids Slip band

(A)

Macro voids

Tangled dislocation

(B)

(C)

FIG. 10 Schematics of slip bands in crystal (A); tangled dislocation cell (B) and macro void formation; micro voids and macro voids (C).

under the constant mechanical stress applied [18]. They showed that the strains due to mechanical stress and lattice expansion was separated from the total strain measured. The resistivity differences between annealed and as-drawn samples are attributed to the resultant mechanical strains. Here, the coincidence of the changes in potential and apparent molar volume with respect to x (Fig. 9A and B) is discussed. There is a concentration at which both variables coincidently begin to change dramatically from the β single phase to the (β + void) coexistence phase (in the figure, βmin and Vmin). The negative potential transition (0.20 to 0.28 V) and the peak in apparent molar volume indicate that there are two ways in which changes occur in Pd at absorptions above βmin. When this concentration is reached, as noted above, a high-concentration vacancy-cluster structure is formed with high strain, and the change in potential, or, in other words, the increase in hydrostatic pressure (stress) causes the transformation from micro to macro voids. At that time, the peak in apparent molar volume and changes in resistance are, qualitatively speaking, consistent with macro void formation (voids are noted in Fig. 8) [6]. It is possible to surmise the following, based on a study of the interaction between hydrogen and lattice defects and voids. Although there have been few systematic studies of the microstructure of Pd due to H absorption, Fig. 10 is a schematic of the morphology of slip bands, tangled dislocation cell, micro voids, and macro voids. Qualitatively, even for metals other than Pd, dislocations and

82

Chapter 5 Clean loading and microstructure in Pd-D

vacancy-clusters occur within the material as H absorption progresses. As plastic deformation becomes large, slip bands first appear within a crystal, lines of dislocation form a tangle, and within that tangled structure, dislocation cells with fewer internal dislocations are formed, as shown in Fig. 10A and B. Vacancy clusters increase in concentration as H absorption increases. In the case of iron, it has been reported that even with a low concentration of vacancy clusters, macro voids form through nanoscale micro voids (see Fig. 10C). When that occurs, increased void size is caused by hydrostatic pressure (stress) [19]. We have discussed the evolution of the characteristic dislocations and macro void formation as a result of the electrochemical H absorption, which occurs within crystal grains and at grain boundaries, the latter occurs as a new phase (see Section “Coincidence of two hydrogen states with the characteristic hydrogen states: Defects induced by the interaction of hydrogen and applied stress”).

Microstructure of the α + β phase coexistence region characterized from in situ small punch test and the knowledge of hydrogen embrittlement Apart from the void formation above βmin, it is known that the dilation, resistance, and potential approximately recover their initial values after desorption, provided the absorption is slow and limited to within the α single phase [20]. While x is in the (α + β) two-phase coexistence region, the β phase possessing different lattice constant precipitates in the α phase, despite both being FCC. Therefore, there is a reaction due to a strain field formation. It has been shown that strain occurs during H absorption, which is confirmed by in situ neutron diffraction measurement [21]. Below is a summary of established information based on observations of defects in the microstructure related to structural degradation noted in the (α + β) two-phase coexistence region in the framework for hydrogen embrittlement (HE) in a conventional metal. Note that the microstructure discussed here does not refer to voids but rather to the phenomena arising through the propagation of the dislocations. Ductile-to-brittle transition hydrogen concentration (DBTC) is a measure of hydrogen embrittlement of material, which is usually determined using in situ small punch (SP) testing. DBTC refers to H concentration below which a material exhibits ductile fracture and above which it exhibits surface brittle fracture. On the basis of the results of fundamental studies of HE in materials, Nagumo inferred that brittle fracture is the result of crystal instability. Here, instability is a property that specifically occurs due to heating to the melting point or reducing the elastic modulus. In addition, it is explained thermodynamically that brittleness begins suddenly at a certain critical concentration if there is a progressive increase in the concentration of lattice defects [22]. Matsumoto showed that in most materials, the value of the DBTC concentration coincides with the inflection point of the two-phase coexistence region in a hydrogen pressure-composition diagram given for that material, where the value is shown in the schematic in Fig. 11A [23]. Fig. 11B shows the apparent molar volume and potential of the repetitions 2 and 3-H/Pd ratio diagram in the repeated C mode; the hatched arrow indicates the DBTC value obtained based on the above results. The primary conclusion obtained from this Pd-H system is that if absorption proceeds to the (α + β) two-phase coexistence, lattice defects accumulate in the material and brittleness occurs. According to the Matsumoto paper noted above, and Nagumo’s suggestion [22], between a H/Pd ratio of C(αmax) and C(βmin) where the transition from the α phase to the β phase begins, the increase in defect concentration or the accumulation of defects occurs continuously (see Fig. 10A and B). Note that if stress continues to increase and slip bands transfer to the surface, there occurs the release of the stress in a localized area. The above is also supported by the TDA research clarified below.

83

Results and discussion

0.15

0.2

0.3

0.4

C = K p1/2

0.10 Inflection point:

0.05 0

(A)

C(DBinf)

1.2

C(amax)

C(bmin2)

−0.18

0.5 Potential, E/V vs SCE

Pressure, p1/2/ MPa1/2

0.20

0.1

Δ(bmin)

C(bmin3)

1.0

−0.20

0.8

−0.22

C(btr) Inflection point: C(DBinf)

−0.24 −0.26

(B)

(b + void)

C(bmin3)

0

0.22

0.6 0.4

(a + b)

−0.28 −0.30

C(Vmin)

0.44

0.65

0.87

0.2

Apparent molar volume, VH/cm3(g atom H)−1

−0.16

Hydrogen content, H/M ratio

0

0 1.09

Coulometrically obtained H/Pd ratio

FIG. 11 Schematics of a typical PCT diagram indicating inflection point: C(DBinf) (A); the in situ measurements of potential of second (double dotted line) and third (dotted line) repetitions, and third apparent molar volume (solid line) during the C mode (B) as a function of x. △(βmin) denotes (βmin) incremental charge between second and third repetition.

Coincidence of two hydrogen states with the characteristic hydrogen states: Defects induced by the interaction of hydrogen and applied stress Next, a Pd electrode experiences an increase in lattice defects in the (α + β) two-phase coexistence region and void formation as the H absorption progresses. Here, both processes are discussed in reference to the reports on Thermal Desorption Analysis (TDA) that were developed using a new experimental protocol. The study of hydrogen states by TDA combined with SIMS elucidated two desorption peaks of hydrogen were at one peak (termed peak 1) at low temperature (100°C or 500 experiments on the growth of microbiological cultures on a nutrient medium, including both stable and radioactive cesium, were carried out. The results of many experiments have shown that the effectiveness of individual types of microorganisms (e.g., E. coli etc.) for nuclear fusion is about 50–100 times lower than the effect of syntrophic associations—communities in which there are more than three thousand different types of microorganisms. During the last 15 years, we have conducted several successively optimizing studies aimed at finding the most optimal method for such utilization. The first experiments on the stimulated utilization of Cs137 were conducted in 2002–04, based on radioactive isotopes extracted from the reactor at the Chernobyl nuclear power plant. These experiments were conducted with the participation of our colleagues Prof. V.N. Pavlovich and A. Odintsov from the Institute for Nuclear Research and the Institute for Nuclear Safety Problems in Kiev [18]. The microbiological MCT granules were prepared by our colleague Dr. A.B. Tashirev from the Institute of Microbiology in Kiev. After testing the initial technology, experiments with Cs137 isotope were performed. In these experiments, we used the same closed glass cuvettes, each containing 10 mL of distilled water, in which the salt containing Cs137 was dissolved. The total activity of each of the cuvettes was about 2*104 bq. The scheme of investigations is shown in Fig. 10 (top). Equal amounts of the concentrated biomass of the anaerobic syntrophic association (MCT granules) were placed in 7 cuvettes. In 6 cuvettes, purified salts of K, Ca, Na, Fe, Mg, and P were added to the active water. These chemical elements are among the most vital for any living system. The main purpose of using such additives was to find ways to block possible channels of transmutation, because if a specific chemical element is present in the system, and it is one of the vital elements needed to sustain life, then the assimilation of its biochemical analogue during transmutation becomes unlikely. In addition, such substitutions were carried out with the goal of creating the optimal composition of micro-nutrients for rapid growth of microorganisms. The results obtained below confirm the importance of such substitutions. Two additional cuvettes were used for monitoring: one contained the same radioactive water and MCT (but did not contain additional salts), and the other contained only radioactive water. All of the cuvettes were closed and kept at a temperature of 20°C. The amplitude of the gamma-ray spectrum of the cuvette was measured every 7 days with the same detector, in which a Ge crystal was used. Particular attention was paid to reducing the influence of errors associated with the measurement process. For this purpose, we used cuvettes with a low height, and the detector with a large Ge crystal. The cuvettes were set at the same position in the center of the crystal of the detector for each measurement. The results of the changes in the relative activity of the Cs137 isotope are shown in Fig. 10 (bottom) and in Table 3. In these experiments we observed increased rates of gamma-activity (more precisely—accelerated rate of utilization) of Cs137 isotope in all experiments with MCT and with the presence of different additional salts during 100 days. In the control experiment (cuvette with radioactive water but without MCT), the “usual” law of nuclear decay applies, and the life-time was about 30 years. The most rapidly increasing decay rate, which occurred with effective lifetime τ*  310 days (involving an increase in rate, and decrease in lifetime by a factor of 35 times) was observed in the presence of Ca salt. In the presence of an abnormal (redundant) quantity of potassium in the nutritious media, the process of

222

Chapter 12 Effective LENR and transmutation of stable and radioactive isotopes

Anaerobic syntrophic association "Microbial catalyst-transmutator" (MCT granules)

MCT MCT MCT MCT MCT MCT H20 H20 H20 H20 H20 H20 137 Cs137 Cs137 Cs137 Cs Cs137 Cs137 KCl CaCO3 NaCl FeSO4 MgSO4 P

Control 1. Control 2. MCT H20 H20 Cs137 Cs137

Periodic measurement of Cs137 isotope activity.

Cs137 without MCT (control), τ ≈ 30 years

Activity, Q(t)/Q(0) 1.00 0.98

Cs137 + MCT+KCl τ* ≈ 10 years

0.96 0.94

Cs137 + MCT+NaCl τ* ≈ 480 days

0.92

Cs137+ MCT τ* ≈ 380 days

0.90 0.88 0

5

10

15

Cs137+MCT +CaCO 3 τ* ≈ 310 days 20

25

30

t (days)

35

40

45

FIG. 10 Scheme of studies of the utilization of Cs137 isotopes under different conditions (top) and the kinetic of the accelerated utilization (deactivation) of the Cs137 isotope in “biological cells” in the presence of anaerobic microbe syntrophic association and various chemical elements.

Table 3 Deactivation of Cs137 water solution in optimal experiment (MCT + active water with presence of Cs137 + CaCO3 salt). Start

Finish of experiments (in 100 days)

Isotope, energy of gamma-radiation

N1, registered events per 103 s

N2, registered events per 103 s

Cs137, 661.7 keV

266,900

216,800

Error (absolute/ relative)

Natural decay per 100 d

Change (N2 2 N1)/ N2

478 (0.2%)

0.6%

24%

Experiments on transmutation of radioactive isotopes

223

Cesium transmutation becomes very weak and the life-time of the decay was about 10 years. A possible reaction of Cs137 isotope utilization in these experiments is: Cs137 + p ¼ Ba138 + ΔE

The result of this reaction is the creation of a stable Ba138 isotope. This reaction is energetically favorable (ΔE ¼ 5.58 MeV is positive). The fastest decrease in activity was observed in a cuvette containing a calcium salt. This was equivalent to a decrease in the lifetime of Cs137 by a factor of 35 to τ*  310 days. It is very important to note that this decrease in activity was not related to the accelerated decay, but was the result of nuclear transmutation of radioactive Cs137 isotope to the stable Ba138 during Cs137 + p reaction with participation of water protons. If we consider this process from the standpoint of biochemistry, then this reaction coincides with the previously studied reaction of transmutation of a stable Cs133 isotope into an Ba134 isotope. Concerning the “biological expediency” of such a hypothesis, it should be noted that Ba2+ and K+ ions are biochem˚, ical analogs: they have approximately the same ionic radii in the divalent state (RBa  1.4 A ˚ RK  1.33 A). Since the replaceable element (potassium) is one of the vitally important trace elements, the probability of such a substitution is quite large and the ions of the synthesized barium can replace potassium ions in metabolic processes with the growth of cultures. Such a substitution appears to be more effective than the “direct” replacement of potassium by cesium in the case of potassium defi˚ ciency. This can be seen from the large difference in the ionic radii of cesium RCs  1.65–1.69 A ˚ and potassium RK  1.33 A. Another interesting question relates to the cause of the increased efficiency of utilization when using an additional calcium salt. These phenomena are probably connected with general problems of metabolic processes involving microbiological cultures: optimal growth of microcultures takes place when a balanced relation of micro elements occurs. The phenomenon of low energy transmutation of chemical elements and isotopes in biological systems and creating conditions for sustaining it is based upon the heuristic proposition that if some of the required elements or microelements are not present in the living environment (or nutrient media), then, given that certain prerequisites are met, it will be synthesized as a result of the transmutation. In fact such an approach unambiguously suggests that the ratio of all the necessary elements in each type of living organism is fixed.

LENR experiments with radioactive Cs137 isotope and aerobic microbe syntrophic association Further improvement of bio- and nuclear technologies has led to significant progress in the processes under consideration, using more optimal biological substances and their growth regimes. The experiments completed in 2016 [32] showed that the utilization process can be accelerated many times using specially prepared aerobic microbe syntrophic associations and an optimized set of macro- and microelements. These new types of syntrophic associations were initially tested at the transmutation of stable isotopes as described above. These successes and a deeper understanding of the physical and biological processes accompanying nuclear phenomena in dynamic systems have led to significant progress and optimizing the process of transmutation. This is clearly demonstrated by the high transmutation efficiency of the stable Cs133 isotope considered above by help of much more effective types of aerobic microbe syntrophic associations. Aeration was carried out using microcompressors and evaporation

224

Chapter 12 Effective LENR and transmutation of stable and radioactive isotopes

was compensated by the addition of distilled water. Glucose was used as a substrate for aerobic syntrophic association. At certain time intervals, gamma-spectroscopic measurements of gamma-radiation with energy of 661.65 keV were performed. To suppress measurement errors associated with the possible redistribution of radioactive waste to the volume of experimental samples, high-sensitivity detectors located at a great distance from the investigated samples were used. In these experiments, a NaI detector with a diameter of 50 mm was used. The results of our last experiments are presented in Fig. 11. These experiments were conducted with active participation of our colleagues Dr. S. Gaidamaka and Dr. V. Kashcheev. The mean decrease in Cs137 concentration over 14 days was 23%, based on parallel experiments, which corresponds to an acceleration of deactivation >200 times in relation to the spontaneous decay and acceleration of the transmutation process by 6 times in relation to the most optimal action of the MCT synrotrophic association (Fig. 10). In some cases, a decrease in the concentration of Cs137 in these experiments reached 70% in 14 days (Fig. 11B) [32]. These results correspond to an increase in the efficiency of transmutation (as compared to anaerobic associations) by a factor of 20 to 30. It should be noted that, with appropriate controlled correction of

Cs-137 activity (%)

100

Control without microcultures

95 90 85 80 75

Time (days)

70

Cs-137 activity (concentration) (%)

(A)

(B)

5

0

10

15

100 90 80 70 60 50 40 30 20 10 0

20

Time (days) 0

5

10

15

20

FIG. 11 Reduction of gamma-activity of Cs137 aqueous solution in the optimized syntrophic association: (A) the average data for the series of experiments (upper horizontal line - control experiment without presence of microcultures); (B) the similar reduction at the most optimal conditions from the same series.

Physical foundation of biological transmutation

225

the composition of the medium, a further decrease in activity (and hence the concentration of Cs137) is possible at the same pace. We also developed a technology for even deeper deactivation (up to 100%) of the radioactive medium in 30 to 50 days. For further stages (up to 100%) of Cs137 isotope transmutation, it is necessary to make the operational changes to the composition of the nutrient medium during transmutation.

Physical foundation of biological transmutation To explain the physical basis of such a transmutation, it is necessary to take into account three important circumstances inherent in any reaction involving charged particles with low energy: •

• •

abnormally high (compared with the “standard” on the basis of estimates of commonly used equations of quantum mechanics and nuclear physics) probability of a tunneling effect at low particle energies; complete absence of radioactive daughter isotopes; extremely strong suppression of concomitant gamma radiation.

After a detailed analysis of all the experiments (both on biological transmutation and related to lowenergy nuclear reactions (LENR) in “ordinary” physical systems) we came to the following conclusion: the most effective method for producing transmutations and for a very significant increase in the transparency of a potential barrier at low particle energies is associated with the use of coherent correlated states (CCS) of particles interacting with the atoms (nuclei) forming this barrier [50–66]. The most characteristic property of CCS is the possibility of forming controlled giant energy fluctuations of a particle whose amplitude can be thousands or even millions of times greater than the average (thermal) energy of a particle and reach values δE  10…50 keV and more. In a concentrated form, this is reflected in the modified uncertainty relations, called the Schr€odinger-Robertson uncertainty relations: qffiffiffiffiffiffiffiffiffiffiffiffiffi qffiffiffiffiffiffiffiffiffiffiffiffiffi 2 ; δEδt  G ħ=2, G  1= 1  r 2 , δpδq  Gpq ħ=2, Gpq  1= 1  rpq Et Et Et __

rAB ¼

__

_

_

< A B + B A > =2 < A >< B > qffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi _ _ < A 2 >< B 2 >

in which the product of the fluctuations of the corresponding dynamic variables A and B (coordinate, momentum, energy, time, etc.) is determined by the corresponding correlation coefficients rpq and rEt (and coefficients of correlation efficiency Gpq and GEt, the magnitudes of which are limited by the intervals 0 | rpq | , | rEt | 1, 1 Gpq, GEt < ∞ [51–66]. Direct calculations have shown that in a stationary state in any system r2pq, r2Et ! 0 and Gpq, GEt  1. In this result, the Schr€ odinger-Robertson uncertainty relations take the form of well-known Heisenberg uncertainty relations. Another situation takes place in dynamic systems, including living objects. It is well known that the growth front of any biological object is never ideally homogeneous—local heterogeneities (potential nano-wells with size L  2...4 A˚ ) are always formed, which are leveled and eliminated during the growth process. Each of these nano-wells is a nonstationary oscillator for particles (iones) that are localized in it. In the process of the dynamically (nonstationary) changing of the

226

Chapter 12 Effective LENR and transmutation of stable and radioactive isotopes

parameters of these wells, CCS can be formed for these particles with a large value of the coefficients of correlation efficiency (up to Gpq, GEt  103...104 and more [52]) and, accordingly, with unlimitedly increasing fluctuations of kinetic energy: δT ¼ ðδpÞ2 =2M  G2pq ħ2 =8MðδqÞ2  G2pq ħ2 =2ML2  5:::50 keV

which can exist for a relatively long time, δt  GEtħ/2δT  1017...1018 s and which is enough both to pass through the potential barrier and stimulation of nuclear reaction. It is easy to verify that in the absence of CCS process (i.e., for uncorrelated states with Gpq, GEt ¼ 1), the duration δt ¼ ħ/2δT  6 ∗ 1020...3 ∗ 1021 s of the existence of the same energy fluctuation δT  5...100 keV becomes extremely small and does not allow for the tunnel transition process and subsequent nuclear reaction. In works [50–66], different modes of CCS formation under different methods of weak external action on particles are discussed and investigated—squeezing or expanding potential well [50, 51, 55, 58], periodic action of resonant [56, 58] and nonresonant [61, 62] frequencies, pulse modulation of potential well [62, 64] and action of a pulsed magnetic field [64], CCS formation under influence of random defusing fluctuations [59], and many other factors. An exact calculation, carried out using quantum mechanics, shows that during the formation of the CCS there is a very significant increase in the transparency coefficient of the potential barrier from that which is typical of slow particles (at room temperature) and “usual” uncorrelated states very small values D  10800...10500, up to large values D  101...105 for correlated states. These are in good agreement with experiments. From this point of view, the growth of the nonstationary zone of any biological object represents a system of potential disposable nanoreactors, in which a reaction involving these particles is possible. Similar processes can occur in the space between two cells during cell division, in mitochondria, at the entrance to biological membranes, in the process of DNA replication, etc. A more detailed description and analysis of fundamental nuclear processes that occur at low energy is contained in the chapter on coherent correlated states of interacting particles.

Conclusion The experimental results presented here, and a very short theoretical analysis substantiating these data, show that the method of transmutation of stable and radioactive isotopes in the presence of growing microbiological cultures and their associations may be an effective way of solving many fundamental problems of ecology and industry. This method can be used to deactivate a large amount of radioactive liquid [31, 67], to produce rare isotopes [30], and to dispose of chemical toxic materials in the treatment of many medical diseases, replacing ineffective drugs and so on. The efficiency of using this technology for the production of rare (and expensive) M€ossbauer isotopes has been confirmed in direct experiments. By the method in our books [7, 8], the models, biophysical justification, and some possible exotic transmutation reactions with creation of gold and platinum are described: Os90 + Li7 ¼ Au197 , Re187 + Li7 ¼ Pt194 ,W186 + Be9 ¼ Pt195

Acknowledgments

227

Another possible (and more effective) transmutation reaction of gold and platinum creation is the following: Ir193 + He4 ¼ Au197 ,Ir191 + p ¼ Pt192 , Ir193 + p ¼ Pt194

We have conducted some of these reactions with participation of microbiological substances and have observed creation of gold. These results are unpublished yet. Such processes are especially important for solving the problems of accelerated deactivation of radiation-contaminated water and soil. These results can give the answer to the question of the reasons of abnormal accelerated decrease (by many times in relation to natural spontaneous decay) of environmental radioactivity in some isolated areas inside Chernobyl accident zone with initial very high level of radiation pollution. Obviously, such a phenomenon can be directly related to the activity of natural microbe syntrophic associations that are located on the ground surface. The process of nuclear transmutation is associated with controlled nuclear reactions at low energy due to the use of coherent correlated states, which contributes to a very sharp increase (by 1050 to 10500 and more times) in the transparency of the potential barrier. At atomic and molecular levels, the specificity of the interaction and motion of the microparticles is fully described by the laws of quantum mechanics and electrodynamics for both living and nonliving objects. From this point of view, there is no difference between them. We have also shown [68,69] that reactions stimulated by the formation of coherent correlated states (and formation of very large fluctuations of momentum and kinetic energy) never lead to the formation of radioactive daughter nuclei, and are characterized by the strong suppression of gamma-radiation. Such processes can be successfully implemented on any system (physical, biological, geological, etc.) if the necessary prerequisites are met. These reactions should not be called by the semimystical term “biological transmutation”. These are usual nuclear reactions (more correctly and specifically, LENR), but they are produced in growing biological systems and under the catalytic effect of dynamic electric fields accompanying atomicmolecular processes that take place with growth in these systems. Such a process can be called “nonstationary dimensional nuclear catalysis” and it can occur both in living and in nonliving physical systems. These results reveal a nontrivial nature of interactions of different microelements. By changing the makeup of the nutrient medium, it is possible to control the speed of a culture’s growth. Lacking at least one of the microelements in the nutrient medium hinders the development of the entire biological object. In any living organism, you can specify many potential places for the realization of such nuclear processes—the area between cells during its division, the surface of mitochondria, the area near the entrance to the cell membrane, the fork of DNA division and replication, and other places. All these nano-objects, if we consider them from the point of view of quantum theory and nuclear physics, are potentially effective nonstationary potential wells, within which the formation of coherent correlated states for particles present there is possible.

Acknowledgments We thank all the colleagues with whom we had very useful collaborations and discussions. Without them the essential part of conducted experiments would not have been possible. We are very grateful to Prof. V.N. Pavlovich and A. Odintsov from the Institute for Nuclear Research and the Institute for Nuclear Safety Problems in Kiev, Dr. A.B. Tashirev from the Institute of Microbiology in Kiev, Dr. S. Gaidamaka from Moscow State university, and Dr. V. Kashcheev from A.A. Bochwara High-tech Scientific Research Institute of Inorganic Materials.

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CHAPTER

Transmutations and isotopic shifts in LENR experiments

13

Mahadeva Srinivasana,∗, K.P. Rajeevb a

Bhabha Atomic Research Centre (BARC), Mumbai, India Department of Physics, IIT Kanpur, Kanpur, Indiab

Introduction and background The term “Transmutations” as used in the low-energy-nuclear reaction (LENR) field has come to refer to the occurrence of nuclear reactions between the loaded deuterium (or deuterons) or hydrogen (or protons) on the one hand, and nuclei of the host metal such as Pd, Ni, Ti, or of other higher Z nuclei present in the reaction zone such as those of alloyed elements or impurities in the cathode or even elements present in the electrolyte (in case of electrolysis experiments), on the other. Any nuclear reactions that occur among the hydrogenous isotopes themselves such as H or D present in the reactive zone would generally be classified as “fusion” reactions. Thus, as understood in the context of the present discussion the basic difference between transmutation reactions and fusion reactions is that in the former the host metal lattice nuclei participate directly in the nuclear processes taking place while in fusion reactions they only serve as passive spectators or catalytic agents but themselves do not get involved. There are also some experimental configurations wherein nuclear reactions do seem to occur among medium Z materials even when neither H nor D is explicitly introduced into the system nor is there any special metallic component that can be said to serve as a “host” as such. Some examples are the underwater Carbon Arc experiments and the phenomenon called “Biological Transmutations” which is discussed in another chapter of this book. However, in both these cases, hydrogen (and deuterium from natural abundance in water) are already present in the configuration and could be participating in transmutation type nuclear processes. There are still other configurations such as glow discharge experiments in which selected noble gases are used as the filling gas, or even “historical Alchemy” experiments where no hydrogenous isotopes are present in the experimental zone, and yet elemental transmutations seem to occur. Thirty years have gone by since the original Fleischmann & Pons (F&P) announcement of 1989. As discussed in the other chapters of this book, within a few years of the F&P announcement it was confirmed that in palladium-deuterium (Pd-D) configurations it is some variant of fusion reaction between deuterons resulting in the formation of 4He that is the source of excess heat production (the so-called “heat-helium correlation”). So, when small quantities of new elements or isotopic anomalies were ∗

Retired.

Cold Fusion. https://doi.org/10.1016/B978-0-12-815944-6.00013-0 # 2020 Elsevier Inc. All rights reserved.

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observed at localized spots on the surface of Pd cathodes in Pd-D configurations it was presumed that this could have resulted only as a result of transmutation reactions. It is of great academic interest to understand how the larger Coulomb barrier between a deuteron and a Pd nucleus could be overcome for such transmutation reactions to occur. In the mid-1990s, following the advent of the Patterson power cell (discussed in detail in “Patterson power cell and transmutation product measurements by Miley et al.” section) which deployed as cathode a packed bed of small plastic or other microspheres coated with multilayer thin films of Pd and/or Ni, and electrolyzed in light water solutions, the source of the observed excess heat posed a puzzle. Subsequent postrun analysis of the thin films clearly indicated the presence of a large variety of transmutation products and it is this observation that triggered much interest in transmutation reactions, especially in the context of Ni-H configurations. The general consensus that has emerged in the LENR field since the Patterson-Miley work was first published is that while in Pd-D systems fusion reactions are the cause of excess heat, in Ni-H configurations it is most probably transmutation reactions involving Ni that is responsible for heat production. Since the publication of the results of the Lugano experiment in 2014 and the subsequent follow up replication experiments conducted by Parkhomov and his collaborators in Russia from 2015 onwards, the Ni-H enthusiasts of the LENR community have redoubled efforts to establish a clear correlation between transmutation products, including isotopic composition changes in the elements constituting the metal powder matrix, and the integrated quantum of excess heat generated, although this has proved to be a formidable challenge. In this context, there are other researchers who speculate that the excess heat generated in light hydrogen systems could alternately have also arisen from fusion reactions between the minute quantities of deuterons which are present in the system stemming from the isotopic abundance of deuterium in natural hydrogen. On the other hand, Godes of the Brillouin Energy Corporation has postulated that in their Ni-H systems it is the stepwise capture of electrons by protons resulting in the ultimate formation of 4He that is the source of heat production [1]. To prove or disprove these hypotheses one should look for 4He in the gaseous mixture in the reactor vessel following experimental runs. To the best of our knowledge, no group has confirmed observing helium gas in Ni-H systems so far. As is evident from the discussions in the other chapters of this book, the immediate future of LENR, as far as energy production is concerned, seems to lie in high-temperature gas loaded systems wherein the fuel comprises of nanopowder mixtures of metals such as Pd, Ni, Li, Zr, etc. while the gas to which these powders are exposed at high temperatures could comprise of hydrogen, deuterium, or mixtures thereof. It is essential for us to understand whether excess heat generation in such systems is due to fusion reactions between the hydrogenous nuclei or due to transmutation reactions (which term includes isotopic composition changes) in the nuclei of the fuel powder matrix caused by protons or deuterons reacting with the metal powder nuclei. At this juncture, it is worth noting that in the above discussions it is tacitly assumed that if transmutation products are found it must be due to a nuclear reaction and the corresponding change in mass △m, must be appearing (or absorbed depending on sign) as heat according to E¼△mc2. Some recent experimental observations discussed at the end of this chapter has however thrown up yet another unexpected puzzle, namely of massive quantities of new element production but with the expected enormous energy release not manifesting as heat. One of the fascinating aspects of the LENR transmutations field is the variety of experimental conditions under which such nuclear reactions seem to be taking place, posing a great challenge to nuclear physics. The objective of this chapter is to take stock of the available experimental evidence not only

General remarks on experimental methodology

235

for the occurrence of such reactions but also to assess its relevance and importance to excess heat generation in practical LENR-based devices. In 2011, one of the authors of this chapter had carried out a review of the status of transmutation experiments in the LENR field at that time, jointly with George Miley and Edmund Storms [2]. The present effort may be considered as an update of that review paper.

General remarks on experimental methodology Transmutation experiments generally involve two steps: The experimental run during which a target or test sample is loaded with deuterons or protons by a suitable technique such as electrolysis, gas/plasma loading or other means. Loading step may at times be followed by application of a triggering stimulus which could initiate nuclear processes. In the next step, on completion of the experimental run, the test sample is analyzed offline to determine if there is any evidence for transmutation reactions having occurred. This involves measuring the elemental composition and/or isotopic distribution of various components which were present in the reaction zone. In the case of electrolysis and glow discharge experiments, the cathode would be the one mainly investigated. Obviously mere detection of traces of a “new” element which was not present prior to the run does not imply the occurrence of transmutations since, in principle, cross contamination could occur through inadvertent transport of minute quantities of elements from elsewhere in the apparatus. For example, during electrolysis trace quantities of impurities could easily get deposited from the electrolyte. In glow discharge experiments plasma etching could sputter out some elements and redeposit them on the test sample. It is therefore important to ensure that such contamination is not causing the observations. Having accurate elemental composition of the stock electrolytic solution, especially of trace elements, available prior to the commencement of the experimental runs would be essential. However, if the isotopic distribution of the newly found elements or for that matter of any of the materials not previously present in the system are found to be significantly different from their natural abundance following a run, then it would clearly point to anomalous nuclear processes taking place. Such findings are often referred to as “isotopic anomalies” or “isotopic shifts.” Advanced mass spectrometric analytic tools such as Secondary Ion Mass Spectrometry (SIMS) permit accurate isotopic distribution measurements. However, mass spectroscopy is known to be subject to errors arising from interference effects caused by molecular ion species having masses close to that of the isotope under measurement. This possibility has to be addressed before concluding that the observed “isotopic anomalies” are real. Lastly, the well-known characteristic of nonuniformity of the LENR phenomenon must be recognized while interpreting the transmutation results. In a companion chapter of this book, Ed Storms has elaborated on the very useful concept of Nuclear Active Environment (NAE), to explain the nonuniform and highly localized occurrence of nuclear reactions in samples subject to experimental stimuli. Invariably the LENR phenomenon is found to occur in one spot but not in a neighboring one. Also, a systematic variation of the reaction product concentrations is often observed as one goes from outer layers to deeper layers. Depth profiling of new element concentrations and isotopic ratios has at times influenced acceptance of the genuineness of the transmutation results. Because of these characteristics, it is very difficult for experimentalists to establish a correlation between the integrated quantity of a new element or new isotope production and total integrated quantum of thermal energy generated in an experimental run.

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Patterson power cell and transmutation product measurements by Miley et al. It was the Miley-Patterson paper published in 1996 [3] that perhaps really opened the door to the acceptance of transmutations being possibly real even within the CMNS community. Industrial chemist James Patterson had invented a pebble bed cathode, circulating solution electrolytic cell wherein the cathode was made up of a bed of Pd-Ni multilayer thin film quoted plastic microspheres (1 mm dia.). There were typically 1000 microspheres in the cell forming a four- or five-layer bed constituting the cathode. Li2SO4 solution served as an electrolyte as well as coolant. Fig. 1 is a schematic representation of this cell. As this cell showed excess heat with both D2O-based as well as H2O-based electrolytic solutions, Patterson entrusted Miley’s group at the University of Illinois to perform elemental analysis of the coating of the postrun beads to determine if any nuclear products could be identified. When Miley found what appeared to be a gamut of new elements he repeated the electrolytic runs in his lab after fabricating his own version of multilayer thin film coated cathodes as well as a fresh electrolytic cell using no metallic components, to preclude the possibility of trace elements from entering the solution and causing contamination. An advantage of thin-film cathodes (coating thicknesses varied in the range of 50–300 nm) is that high deuterium or hydrogen loadings could be obtained during electrolytic runs in time durations as short as an hour or two. Also, the nuclear products would constitute a larger fraction of the metallic mass, minimizing doubts that the new elements found could be due to impurities deposited from

Platinum contact anode(+)

Exit temperature reading O – ring

Platinum screen Coated microsphere

Industrial strength glass Microsphere bed

Platinum screen

O – ring

Platinum contact cathode(–) Input temperature reading

FIG. 1 Schematic representation of Patterson power cell. From G.H. Miley and J.A. Patterson, Nuclear transmutations in thin-film nickel coatings undergoing electrolysis, J. New Energy 1 (1996) 5–39. https://www.lenr-canr.org/acrobat/MileyGHnucleartra.pdf.

Patterson power cell and transmutation product measurements

237

the electrolyte. Miley and his colleagues carried out more than a dozen electrolytic runs with various types of coatings. Following several weeks of electrolysis, beads from the upper layers of the packed bed cathode were retrieved for analysis. A variety of measurement techniques such as SIMS, Energy Dispersive X-ray (EDX, EDXA, EDS) analysis, Auger Electron Spectroscopy (AES), and Neutron Activation Analysis (NAA) were employed. While EDX gave confirmatory data for the higher concentration elements, AES was used for depth profiling of these elements. SIMS was used to obtain an overall picture of the various nuclides present and their relative isotopic ratios while NAA gave a quantitative measure of eight key elements, namely Al, Ag, Cr, Fe, Cu, V, Co, and Zn, present in a gross sample containing 10 microspheres. In the case of Cu and Ag, NAA helped establish deviations of isotopic composition from their natural abundance values. NAA has the advantage that it circumvents the molecular ion interference problem. Since NAA typically gives an average value integrated over 10 beads, it averages out the significant bead-tobead variations in the reaction product yields, which are known to be sensitive to the location of the microspheres in the packed bed. The results confirmed the presence of a wide range of new elements in the postrun thin films. The reaction products had mass numbers ranging both below and above the atomic mass number of the host metal, spanning across the entire periodic table. Fig. 2 is a smoothened plot of the reaction product yields plotted against the atomic number (Z value) of the product elements. A characteristic fourhumped yield spectrum is evident with humps occurring at Z ¼ 6–18 (peak at Mg-Si), Z ¼ 22–30 (peak at Fe-Zn), Z ¼ 44–50 (peak at Ag-Cd), and Z ¼ 75–85 (peak at Au). In some of the runs, as much as 40% of the initial metal atoms of the thin film coating was transmuted. Miley speculates that each of these clusters of elements is derived from one of the main elemental components used in the construction of the cell such as sulfur, nickel, palladium, and platinum (which was the anode material).

FIG. 2 Reaction product yield vs Atomic number (Miley). From G.H. Miley and J.A. Patterson, Nuclear transmutations in thin-film nickel coatings undergoing electrolysis, J. New Energy 1 (1996) 5–39. https://www.lenr-canr.org/acrobat/MileyGHnucleartra.pdf.

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Chapter 13 Transmutations and isotopic shifts in LENR experiments

SIMS results indicated that the isotopic composition of most of the elements showed substantial deviation from natural abundance, whereas data of the control beads corresponded to natural isotopic ratios only. NAA data for Ag and Cu also confirmed significant deviations from natural abundance. It was however not possible to discern any systematics in the isotopic shift results since there was considerable scatter in the cathode bed. Miley’s papers have also discussed the differences in yield spectrum between different base metal coatings, differences in product yield between plastic beads and glass microspheres and differences between H2O runs and D2O runs. The similarity of this four-humped yield curve with the well-known double-humped yield curve observed in neutron-induced fission has led to speculation that there could be an analogous proton or deuteron-induced fission of the compound nucleus formed between a host metal nucleus and one or more protons or deuterons in LENR configurations. Inspired by Miley’s findings reported at the First International Conference on Low Energy Nuclear Reactions held at College Station, Texas, in June 1995, Mizuno of Hokkaido University, carried out a systematic analysis of his postrun Pd cathodes that had earlier been electrolyzed in heavy water solutions and to his pleasant surprise also found a four-humped yield spectrum similar to that of Miley (see Fig. 3). Mizuno has elaborated on the details of his transmutation quest both in his book [4] as well as a review paper [5]. Recently there has been another confirmation of the modification of host metal isotopic ratio in a Ni:H electrolysis experiment [6]. The experiment was done in an electrolytic cell with a Ni cathode and Pt anode with a K2CO3 solution in deionized water as the electrolyte. The experiment was run for several hours with voltage and current values of the order of 100 V and 5 A and a whole host of new elements were detected on the cathode using both EDS and SIMS techniques. The isotopic ratio of the Ni isotopes on the cathode surface was found to be significantly modified from their natural values by SIMS analysis which supports the fact that nuclear reactions are easily induced by electrolysis 1E + 28 Counting correction RSF/cm–3

Ne

1E + 27 Ar N

1E + 25

H

Br Se As

CI S P

1E + 24

Zn

I Cd

Te Sb

Au Pt

Hg

Pd Ni Ge Co Rh Ag Ta W Fe Be Sn Mo Mn Cu Hf Ho Nb Ti Cr La Nd Tb Er Mg Ca V Zr Yb Ba In AI Y Se Ga Rb Ce Eu Dy S Li Sm K Cs Na

1E + 23

Bi Pb

Si

1E + 22 1E + 21 1E + 20

C

Xe

Kr

O

1E + 26

0

20

40 60 Atomic number

TI

80

100

FIG. 3 Yield of elements formed on Pd surface (Mizuno). From T. Mizuno, Nuclear Transmutation: The Reality of Cold Fusion, Infinite Energy Press, Concord, NH (1998).

Lugano report and Parkhomov replications

239

experiments in certain configurations and experimental conditions. This observation suggests that some of the isotopes of Ni preferentially participate in these nuclear reactions and hence get depleted compared to other isotopes.

Lugano report and Parkhomov replications In 2013, Andrea Rossi came up with an advanced high-temperature version of his E-Cat (short for Energy Catalyzer) which he called the “Hot Cat.” An improved version of a Hot Cat module fabricated by Industrial Heat LLC was handed over to a group of seven professors (five from Sweden and two from Italy) to carry out an “independent third party” test of the Hot Cat in early 2014. It is noteworthy that this test which was conducted in an industrial laboratory in the city of Lugano in Switzerland was financed by Elforsk, the R&D wing of the Swedish Electricity Generation Companies. The results of this 32-day performance test conducted on the Hot Cat module during February–March 2014 was released in October 2014 [7]. The Hot Cat deployed in this test was basically a 2 cm diameter, 20-cm-long alumina cylinder with V-shaped ridges cut on the outer surface to facilitate convective cooling [7]. The fuel, about a gram in weight, and made of Ni powder admixed with 10% by weight of Lithium Aluminum Hydride (LiAlH4), was inserted into the alumina reactor tube which was then sealed off by means of end plugs. To trigger the onset of the nuclear reactions the temperature of the reactor tube was slowly raised by powering the solenoidal electrical heating coil wound around it. The input heating power fed into the system was in the range of 800–900 W. As there was no provision for cooling the reactor other than through radiation and convection to the ambient air, the temperature of the alumina tube rose to red hot conditions (Fig. 4), estimated to be in the 1200–1300°C range. The power dissipated from the reactor under steady-state conditions was measured using a pair of infrared cameras which had been appropriately calibrated. Full details of the experimental procedure adopted and the pyrometric measurements carried out are documented in the Lugano Test Report [7]. The coefficient of performance (COP), defined as the ratio of output to input power, was reported to be in the range of 2.5–3.5 during the test run.

FIG. 4 Photo of a red hot E-Cat tube. From the document http://www.sifferkoll.se/sifferkoll/wp-content/uploads/2014/10/LuganoReportSubmit.pdf. This is fig. 12a of the document.

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Chapter 13 Transmutations and isotopic shifts in LENR experiments

Incidentally, it turned out that LiAlH4 was the secret additive “sauce” that Rossi did not divulge earlier but it appears to have been inadvertently revealed by the professors who wrote the final Lugano test report. The primary role of this “hydrogen storage compound” was to release hydrogen gas into the reactor tube when heated although it now appears that the Li in LiAlH4 may also have been involved in the nuclear processes. On completion of the 32-day test run, the spent fuel powder was extracted and subjected to detailed chemical and mass spectrometric analysis. A significant finding [7] of the Lugano test, besides the confirmation of excess power generation, was the observation that the isotopic composition of both the nickel and lithium contained in the fuel mixture had substantially changed from their initial natural isotopic distributions. 7Li was significantly depleted leading to the speculation that a proton-7Li reaction could have occurred. In addition, many new elements not present in the virgin fuel mixture were also detected. These results have been interpreted to indicate that the excess power production in the Hot Cat reactor is probably attributable to nuclear transmutation reactions between the protons from hydrogen and the nuclei of Ni and Li. There are also speculations that the observed preferential depletion of 7Li in comparison to 6Li could be attributed to the formation of 8Li which then could emit a beta particle and subsequently fission into two nuclei of 4He. The availability of the Lugano test report in October 2014 and the accidental revelation in this report that Rossi’s “secret sauce” in his Hot Cat was, in fact, LiAlH4 served as an impetus to Andre Parkhomov of Russia to embark on a quick replication attempt. Parkhomov indeed confirmed in January 2015 that he had succeeded in replicating the basic excess heat findings of the Lugano report and a paper on this was presented at ICCF 19 in Padua [8]. While his Padua paper elaborates on his use of a novel calorimetric technique to measure excess heat it does not contain any transmutation product results. In their paper titled “Isotopic and Elemental Composition of Substance in Nickel-Hydrogen Heat Generators” [9] Parkhomov has highlighted the problems in experimentally establishing a quantitative heat-transmutation product correlation. While the appearance of new isotopes that are not present in the initial fuel can be detected if the excess energy release is of the order of 1 MJ/g of fuel, to establish a quantitative correlation between heat and isotopic composition changes of elements already present in bulk in the fuel, Parkhomov argues that the specific energy release needs to be a hundred times larger, namely 100 MJ/g (In the Lugano experiment specific energy release was as high as 5800 MJ/g). Parkhomov also points out that ICP-MS method cannot determine the content of isotopes with mass numbers 1–5, 12–22, and 32. As already highlighted by us in “General remarks on experimental methodology” section of this chapter, Parkhomov too has cautioned that in high-temperature experiments the appearance of new elements at any local spot in the postrun fuel sample could have occurred due to migration from structural materials, which cannot be ruled out. In his latest paper [10] presented at the “25th Cold Nuclear Transmutation and Ball Lightning Conference” held in Sochi, Russia, during October 2018, Parkhomov has discussed the results of a 225days long test of a Ni-Li-Al-H high-temperature reactor which was fueled with about 1 g of powder mix. Input electrical heating power varied from 200 W to 1 kW. COP was in the range of 1.6–3.6 and excess energy produced was 4100 MJ. Elemental and isotopic analysis of the spent fuel after 7 months of continuous operation showed that while changes in the isotopic composition of Ni is insignificant there was a significant increase in calcium content. This result is indeed puzzling. It is worth pointing out that Parkhomov was able to obtain the help and cooperation of very reputed laboratories to carry out elemental and isotopic analysis of postrun fuel samples. It is obvious that a variety of transmutation reactions do take place in these high-temperature Ni-Li-Al-H fueled reactors, which indeed

Iwamura’s deuterium gas permeation experiments

241

generate measurable excess heat but so far Parkhomov’s group has not been able to come to a firm conclusion regarding the exact nuclear reaction (or reactions) responsible for the observed excess heat.

Iwamura’s deuterium gas permeation experiments One of the most spectacular of transmutation findings in the CF/LENR field is those of Yasuhiro Iwamura and his colleagues who conducted experiments at the MHI Laboratories in Japan for over two decades. They have systematically studied the nuclear products formed during the simple process of vacuum-assisted loading and “permeation” of deuterons through single- and multilayer nanostructured Pd foil complexes. As this work forms the subject matter of a separate chapter in this book it will not be discussed in detail here except to bring out the essential features of their experimental observations. Their multilayer Pd-CaO-Pd foil complex is mounted inside a deuterium-filled (at one atmosphere) chamber while the outer face of the complex is exposed to an adjoining evacuated vessel. The D2 molecule appears to undergo “dissociative chemisorption” and diffuses through the solid foil complex as deuterons. The one atmosphere pressure difference between the front and backsides of the foil complex helps the deuterons to diffuse (permeate) through the same. Iwamura’s group had earlier found that to cause nuclear reactions one needs both a decent deuterium loading as well as some mechanism to cause the deuterons to rapidly diffuse through the Pd and other layers. Instrumentation which can carry out in situ elemental analysis (using XPS) and measurement of isotopic ratios (using SIMS) without having to take the sample out for analysis is provided in the experimental chamber. The experiment involves depositing a thin layer of a specific test element on the front face of the foil complex and following the progressive formation of new elements during the D2 permeation process, over a period of 1–2 weeks, through periodic in situ measurements, using XPS. The isotopes involved were determined later using SIMS. In the first of such “designed transmutation” studies, they coated 73Li as a dopant on the surface and observed the production of 199F following the capture of six deuterons which then went on to become 27 13Al following a further capture of four more deuterons. In subsequent 141 runs [11] they studied the conversion of 133 55Cs to 59 Pr following four deuteron captures. Iwamura’s group has since laboriously carried out [11] a series of systematic experiments, using essentially the same experimental procedure described above, and investigated the occurrence of nuclear transmutation reactions with nuclides having Z values up to 56 and mass values up to 138 during D2 gas permeation. They have experimentally confirmed that such permeation-induced transmutation reactions do not occur either on pure Pd foils or with complexes wherein MgO is used as a dopant instead of CaO. Thus, the presence of CaO in the environment seems to be absolutely essential. In all these experiments, deuterons are effectively captured always in multiples of 2, namely either 4, 6, or 8. It has also been established that the phenomenon occurs only at certain “hot spots” and that too within the top 100 μm layer of the surface. The following are some of the transmutation processes which have been seen: 133 141 55 Cs ! 59

96 Pr and 88 38 Sr !42 Mo

In each of these processes, four deuterons are “effectively captured” by the initial test (or given) nuclide. Interestingly, the authors themselves do not specifically claim, anywhere in their papers that the four deuterons are directly captured by the Cs nucleus. As per their EINR (electron-induced nuclear

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Chapter 13 Transmutations and isotopic shifts in LENR experiments

reaction) theory, this reaction happens through an intermediate step of dineutron formation following electron capture by deuterons. A detailed description of their theoretical conjectures of how such a complex reaction may take place is beyond the scope of this chapter. However, one crucial experimental finding reported by their group is when they conducted the permeation experiment at the SPring 8 Synchrotron facility using a finely collimated X-ray beam to perform X-Ray Fluorescence spectroscopy (XRF) measurements, they found that such multideuteron capture reactions take place only at selected isolated hot spots on the foil surface, bringing out once again a unique feature of the LENR field, namely that for nuclear phenomena to occur a NAE has to be formed and this happens only at a few spots. Such heavy-ion nuclear reactions have never been observed even in the most advanced nuclear physics laboratories elsewhere, let alone the fact that this unbelievable reaction seems to be taking place during the simple act of deuterons diffusing through a foil complex and that too at room temperature (actually they found keeping the foil complex at a slightly higher temperature helped improve deuteron diffusion rate). In an overview [11] of their two-decade long pursuit of LENR transmutations, Iwamura has placed his findings in perspective. He confesses that he still does not understand why the addition of CaO (or Y2O3) works but not MgO and why such multideuteron captures work mostly only with intermediate layer coatings of alkali and alkaline earth elements and not others. The energy released in the above reactions, based on mass deficit calculations, works out to be in the range of several tens of MeV. But since the amount of transmuted elements is too miniscule to cause measurable heat release it is not possible to comment on whether the expected energy release manifests as heat or is lost through some other energy dissipation process.

Glow discharge studies Karabut and Savvatimova were among the earliest researchers to investigate LENR transmutation phenomena using glow discharge. Fig. 5 is a schematic representation of their glow discharge apparatus, which is basically a double-walled quartz vacuum chamber with Mo anode and cathode. The design of the setup permitted use of different cathode material inserts for study [12]. The chamber was evacuated and filled with D2 gas to a pressure of 3–10 Torr. The region of the cathode bombarded by the plasma ions was typically 1 cm2 in area. Applied voltage varied from 50 V to 1.2 kV and discharge current was 100 mA. The chamber and electrodes were water-cooled to perform calorimetric measurements. The authors have reported observing excess heat consistently with near 100% reproducibility, but not detecting the normal (d-d) fusion reaction products, such as neutrons, tritium, or even helium, commensurate with the magnitude of the heat generated. Hence their persistent quest for evidence of transmutation products. Prior to commencement, the impurity content of virgin Pd cathode material was confirmed to be under 0.01%. Postdischarge Pd cathode buttons were analyzed using scanning electron microscopy for surface topography; XRF, spark mass spectrometry, SIMS, and Thermal Ionization Mass Spectrometry (TIMS) for elemental and isotopic composition. Results consistently indicated significant deviations from natural abundance values for most elements. At the Nagoya ICCF 3 meeting (1992) Karabut et al. reported finding as much as 0.1% of Na, Mg, Br, Zn, S, Mo, and Si in the upper crust of the Pd. The top 1 μm layer of the Pd sample was examined at several spots in the front portion, the back portion, and shielded area with a spatial resolution of 1 μm

Glow discharge studies

243

FIG. 5 Glow Discharge apparatus used by Karabut et al. From A. Karabut and E. Karabut, Experimental results on excess heat power, impurity nuclides and X-ray production with high voltage discharge system, J. Condens. Matter Nucl. Sci. 6 (2012) 199–216.

using an X-ray microprobe analyzer (also known as EPMA—electron probe microanalyzer). It was found that the content of some elements increased by tens to hundreds of times relative to initial content in virgin Pd. At ICCF 5 held in Monaco in 1995, they reported finding significant spot to spot variations using an X-ray microprobe analyzer. In some spots, the Ag content was as high as 12%–15% and Mo about 5%–7%. The postrun concentration of elements such as As, Br, Rb, Sr, Y, and Cd which were not present in any of the construction materials used in the experimental apparatus was in the range of 0.1%–0.2%. A new result reported at the Monaco meeting was that even with hydrogenous plasma, they observed elements not present in the virgin cathode, but in general, the products’ yield with deuterium gas was orders of magnitude higher. At ICCF 9 held in Beijing in 2002, Karabut reported [13] new results obtained by subjecting the discharge device to an “impulsive periodical power source” (pulsed voltage), which led to the generation of intense X-ray laser beams. The main impurity nuclides (with more than 1% content altogether) registered in the top 100-nm thick surface layer were 7Li, 12C, 15N, 20Ne, 29Si, 44Ca, 48Ca, 56Fe, 57Fe, 59 Co, 64Zn, 66Zn, 75As, 107Ag, 109Ag, 110Cd, 111Cd, 112Cd, and 113Cd. They identified two broad categories of impurity elements: those with masses roughly half of that of Pd (probably caused by deuteron-induced fission) and those with masses close to but above that of Pd (possibly caused by multiple deuteron captures). At ICCF 12, held in Yokohama in December 2005, Karabut presented further results from discharges carried out with V, Nb, and Ta cathodes in the inert gases of Xe and Kr besides D2. In general, with cathodes other than Pd, “impurity” element yield was significantly lower. In these experiments, Karabut also measured the impurity content yield after peeling off some atomic layers using plasma etching and then again measuring the elemental content using SIMS.

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Chapter 13 Transmutations and isotopic shifts in LENR experiments

At the same conference in Yokohama, Savvatimova presented [14] a very detailed and exhaustive account of her independently conducted glow discharge results with hydrogen, deuterium, argon, and argon-xenon mixture plasmas. The influence of various experimental parameters such as nature of plasma gas, the total dose of bombarding ions, discharge current density, and type of applied voltage (direct or pulsed) on the yield of “additional” elements was studied systematically. This time she also used multilayer cathodes comprising several foils of 100-μm thickness stacked one on top of the other to study differences in product yield characteristics with depth. The greatest changes in “additional” element content and isotope shifts were found in certain “hot spots” (mostly near grain boundaries) where a micro-explosion or plasma micro-discharges had appeared to have taken place. The author makes special mention of elements with mass numbers 59(Co), 55(Mn), and 45(Sc), which were always found in plenty in the postdischarge samples but never in initial samples. One intriguing observation reported by the author was that the isotopic changes continued to occur for at least 3–5 months after glow discharge exposure. Several isotopes with masses less than those of W and Ta increased by factors ranging from 5 to 1000 times. On the whole, Savvatimova found that the more deeply she investigated the LENR glow discharge phenomenon, the more complex it was found to be, as brought out in the 13 tables of results included in her Yokohama paper. However, considering the relatively large quantities of transmuted elements/ isotopic changes detected in the Russian Glow Discharge studies, there does not appear to have been commensurate “excess heat” evolution over and above the input electrical power input into the system to sustain the glow discharge.

Edward Esko’s “cool fusion” Edward Esko and Alex Jack established the Quantum Rabbit (QR) Labs in the year 2004 to revive the legacy of LENR pioneers George Ohsawa, Louis Kervran, and Michio Kushi who had already been pursuing elemental transmutation studies through simple discharge experiments from the early 1960s onward, well before the advent of the Cold Fusion/LENR era as we know it following the Fleischmann-Pons announcement of 1989. Esko states in his book “Cool Fusion” published in June 2011: “After 30 years of studying how to use the vegetable world in diet, health, and healing we decided to move to the world of elements.” They were convinced from the earlier works of Ohsawa that in simple discharge experiments fusiontransmutation of elements takes place. In their 2014 book titled: “Corking the Nuclear Genie” the QR team has summarized their ambitious agenda to demonstrate that almost any elemental transmutation can be shown to occur in a simple discharge experiment, something that mainstream Nuclear Physics community will find very difficult to accept. Their goal is to show a path to nuclear waste remediation as well as producing rare elements of which the world is expected to run out of in the decades to come. Their methodology is to conduct small-scale discharge experiments in their modest labs and have the postrun test samples analyzed for elemental content/isotopic composition using ICP-MS in reputed commercial laboratories outside. Over the last 15 years or so they have carried out as many discharge experiments whose results have been reported in a series of articles of Infinite Energy magazine and also in their books. The experimental technique has steadily improved over the years.

Edward Esko’s “cool fusion”

245

Pumpout port

Quartz tube reaction zone

Metal cathode

Test material

Metal anode

FIG. 6 Electrical Discharge apparatus used by Esko of Quantum Rabbit Labs [15].

The typical experimental setup used by Esko et al. [15] is shown in Fig. 6. A quartz tube which can be evacuated is fitted with two metallic electrodes as shown in the figure. Various test materials such as lithium or sulfur, etc., are placed in the central zone of the discharge tube between the two metal electrodes. The air is then pumped out of the tube and a small amount of oxygen introduced to a pressure of a few torr. A voltage is then applied between the electrodes to strike a discharge encompassing the test material which heats up and evaporates. After the run both electrodes, as well as the test materials, are subjected to elemental/isotopic composition analysis which invariably indicates the presence of traces of new elements/isotopes not present at the beginning of the experiment and which could be identified as fusion products of the elements that were present in the reaction zone before the discharge current was passed. For example, with iron electrodes and lithium as a test material, copper was detected after the experiment. A glance at the periodic table indicates that a copper nucleus would result from combining a nucleus of iron and lithium. A sample of some of their test results is shown in Table 1. The transmutation products were found both on the test substance residues as well as on the electrodes. Isotopic analysis of the samples was got done through offsite commercial analytical labs such as New Hampshire Materials Laboratory. The results of several other experiments conducted at QR Laboratories are reported in a series of short articles in Infinite Energy Magazine and also compiled in their books. Table 1 Sample electrical discharge experimental results of quantum rabbit labs Suggested Reaction 56 26Fe 36 16S 34 16S

+

+ +

63 29Cu 65 29Cu

7 3Li

➝

63 29Cu

16 52 8O➝ 24Cr 16 50 8O ➝ 24Cr

+ 73Li ➝ +

7 3Li

➝

70 32Ge 72 32Ge

Concentration of Product

Materials in the Tube

1500 ppm (anode)

Stainless steel electrodes with Li as test material

198 ppm (sulfur residue)

Cu/Zn electrode with sulfur as test material

2190 ppm (cathode)

Cu electrode with Li as test material

From E. Esko and A. Jack, Corking the Nuclear genie: The Promise of Low Energy Transmutations, Amber Waves Press (2014); Also see Infinite Energy Issues 78 (2008) and 113 (2014).

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Chapter 13 Transmutations and isotopic shifts in LENR experiments

It may be noted that the observed reactions are actually examples of heavy-ion fusiontransmutations that does not involve H or deuterium and cannot be understood based on contemporary textbook nuclear physics. However, in view of the simplicity of the experimental setup and procedures adopted it would be worthwhile for other experimenters to try to reproduce these results.

Carbon Arc experiments In this very simple experiment, the claim is that when an arc is struck between a pair of carbon rods dipped in water by applying a voltage of some tens of volts, the powder debris that falls from the arcing region to the bottom of the vessel would contain significant amounts of iron as well as other metals in the Fe, Co, and Ni region [16]. Historically, the credit for the “invention” of this process is attributed to George Ohsawa of Japan, who was a close friend of Michio Kushi as well as Louis Kervran during the early 1960s. The word “invention” is used deliberately here because it was not an accidental discovery, but rather a carefully crafted experiment with the objective of producing iron. It is reported that the first successful synthesis was carried out in 1964, and the mixture of elements that were so generated was found to contain some Ni and Co also, so the product was called “George Ohsawa Steel.” Arcing between the carbon rods is reported to have been successfully performed both in air and underwater with comparable end results. Thus, the origin of this very simple transmutation experiment goes back almost a quarter of a century prior to the Fleischmann-Pons announcement and was inspired by the “Biological Transmutation” phenomena described by Louis Kervran in his book. One of the earliest replications of the Carbon Arc experiment was carried out by Ogura et al. at Osaka University during the early 1990s [17]. They looked for new elements in the filtrate using ICP-MS. In 1998 a group from Beijing drawn from the Chinese Academy of Science as also the Beijing University of Astronautics again replicated the Carbon Arc experiment [18]. Deploying Atomic Emission Spectroscopy (AES) they found that the iron content in the debris had increased by factors between 5.6 and 116 in 5 out of 6 runs which used carbon rods of varying initial iron content. They suspected that the pinch effect (magnetic compression of the arcing element) could be playing a role in fostering nuclear reactions. NAA indicated that the 58Fe isotopic content of Fe had increased from its natural value of 0.3%–0.5%. NAA also indicated that Cr (1130 ppm), Co (1.03 ppm), and Zn (500 ppm) had been generated during the arcing. The results of an improved experiment carried out again at Osaka University was reported at ICCF 8 conference held in Lerici in Italy in 2000 [19]. The end parts of the electrodes and debris were analyzed using proton induced X-ray emission (PIXE) and XRF which revealed a considerable increase of Fe besides a slight increase of Ca, Mn, Ti, Cu, and Zn. Roberto Monti has reported that he has independently verified the production of iron and other elements during the arcing of carbon several times [20]. It was after listening to a talk given by Monti at the Bhabha Atomic Research Center (BARC) in Mumbai in 1992 that a group at BARC set up the experiment disbelieving and challenging Monti to demonstrate the production of iron. But in the end, this group from the Spectroscopy Division confirmed finding iron in the debris [21]. Simultaneously, Sundaresan of BARC, who was a postdoctoral fellow at the Texas A&M University (TAMU) at that time, and Prof. Bockris also independently setup the Carbon Arc experiments and confirmed the production of Fe at College Station [22]. Both the BARC paper and TAMU paper were peer-reviewed simultaneously and published back to back in the same issue of Fusion Technology in 1994.

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247

Cathode

Anode

Arc discharge

Water Base FIG. 7 Schematic diagram of the Carbon Arc Experiment. From R. Sundaresan and J. Bockris, Anomalous reactions during arcing between carbon rods in water. Fusion Technol. 26 (1994) 261–265. http://lenr-canr.org/acrobat/Sundaresananomalousr.pdf.

As an illustration of this simple experiment, we describe below the Carbon Arc studies conducted by Sundaresan and Bockris [22]. Fig. 7 gives a schematic diagram of the experimental setup. The 6.14 mm diameter, 300-mm long spectroscopically pure carbon rods were procured from Johnson Matthey and were certified to have an initial iron impurity content of  2.0 ppm. (This was independently also verified by the experimenters.) The rods were mounted in a flat glass beaker as shown in the figure, with the tips being about 5 cm below the surface of the water. The voltage applied was typically  10 V. The current drawn to strike the arc was initially higher but quickly settled to a steady value of between 5 and 15 A depending on various experimental factors. A simple manually operated screw-driven arrangement, as depicted in the figure for the anode, permitted readjustment of the gap between the tips of the carbon electrodes in order to keep the arc sustained as the rods were consumed. The ultrapure distilled water was additionally passed through an ion exchange column to attain a resistivity of 13 mega-ohms. It was then further purified by percolating it through finely crushed carbon powder (made from the same stock of carbon rods), so as to minimize the dissolved iron content in the water prior to commencement of the transmutation experiments. Arcing underwater was performed for a few hours until an adequate quantity of detritus accumulated at the bottom of the vessel. For each new run, a fresh set of carbon rods was deployed. In the second series of experiments with a given pair of rods, the collected powder was taken out every few hours for analysis; at this time the vessel water too was replaced. This way it was possible to study the variation of the quantum of iron formed with time duration of arcing. The Fe content in the detritus powder was measured by a standard spectrophotometry method using a Perkins Elmer Lambda instrument. This technique measures the optical density of a solution of a colored complex of iron thiocyanate at 470 nm wavelength. Calibration was done using standard solutions having known iron content. The results of the first series of 14 runs are summarized in Table 2.

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Chapter 13 Transmutations and isotopic shifts in LENR experiments

Table 2 Results of Carbon Arc expts. Sundaresan and Bockris paper [22] (their Table III) Experiment Number

Weight of Carbon Detritus (mg)

Iron Content (μg)

Iron in Carbon (ppm)

1 4 5 7 8 9 12 13 14

269 361 103 192 183 163 130 471 477

45 45 15 11 5.5 13.5 5.5 53 196

167 125 146 57 30 80 42 112 410

It is seen that the iron concentration in the detritus powder varies in the range of 30–167 ppm, which translated to several tens of μg of total Fe production in each run, or an average the rate of about 4–5 μg of Fe per hour of arcing. The second series of runs indicated a nominally linear correlation between duration of arcing and the total quantity of iron generated. Electrode pair No. 3, which was subjected to arcing for a total of 10 h, yielded altogether about 40 μg of Fe. Before concluding that nuclear transmutation reactions were indeed responsible for the generation of iron, the authors did consider other possible modes of “adventitious” entry of iron into the system. First, ingress of iron from the water was ruled out since the total content of iron in the entire inventory of water in the trough was calculated to be well below the amounts detected in the debris. Alternately, it may be suggested that the entire initial content of iron in the carbon rods could have diffused to the tips of the rods and accumulated in the powder debris collected at the bottom of the vessel. Since the rods are immersed in water, their temperature is well under 100°C, except for the very small portion near the tips, which could have been close to 1000°C. (“The rods were cool to touch at distances beyond 2 cm from the tip.”) Even at 100°C, the diffusion coefficient of iron in carbon is so low (1026 cm2 s1) that the diffusion-concentration mechanism cannot be attributed to be the source of the iron measured in the debris. Interestingly, the authors found that when the arcing was carried out with nitrogen gas dissolved in the water in place of oxygen, no Fe was detected in the debris. This experiment thus not only ruled out the diffusion-concentration theory but also supported that dissolved oxygen is indeed necessary for the generation of iron as suggested by the multibody transmutation reaction proposed by the original proponents of this experiment. Sundaresan et al. have also pointed out in their paper that the average rate of iron production, namely 5 μg/h, implies a nuclear heat production of 135 W, assuming 55.7 MeV per atom of Fe generated. This is to be compared with an electrical power input of between 50 and 150 W, depending on the steady current level. Following simple external heating calibration, they did have an indication of detectable “excess heat.” The authors have recorded that, in general, overheating of the water was indeed a problem, requiring them to periodically stop the arcing in order to allow the water to cool down and thereby avoid reaching near-boiling temperatures.

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249

It is speculated that the basic reaction involved in the production of Fe in the Carbon Arc experiment could be a multibody heavy nucleon fusion reaction involving two carbon nuclei and two oxygen nuclei as follows:  2 126 C + 168 O ! ðintermediate compound nucleusÞ ! 56 26 Fe 12 56 16 4 or alternately 2 6 C + 8 O !26 Fe + 2 He + 56:55 MeV

As an intermediate step, an atom of oxygen and an atom of carbon may also combine to generate 28 14Si, since in some experiments, the presence of silicon in the debris was also reported.

Nano-dust fusion transmutation Dust Fusion is an improved variant of the Carbon Arc experiment and was developed by George Egely of Hungary [23]. The essential ingredient in these experiments is a dusty plasma made from nanosized carbon particles, air, and some water vapor. In its basic version, the process works at atmospheric pressure and temperatures in the region of 1000–3000°C. In his early experiments, Egely used just a conventional microwave oven. Nano-carbon which has high surface area is used as the reactions are thought to occur on the surface of the dust particles with “surface plasmon effects” playing a crucial role. In his 2012 paper, Egely has elaborated on the various physical phenomena that could be involved leading to the creation of “Nuclear Active Sites” widely discussed in LENR literature. The phenomena occurring in these dusty “crystal plasmas” could be characterized as being nonequilibrium, nonlinear, self-organized, and complex. Egely suggests that dust fusion exploits the fact that thousands of fast-moving electrons of the plasma get trapped on fine dust particles causing the surface potential and electric field to become very high. This causes the repulsive Coulomb barrier between positive ions in the plasma to be significantly lowered, improving the prospects of fusion reactions occurring. At the heart of Egely’s experimental chamber is an appropriately shaped “Electromagnetic” as well as an “Acoustic Plasma” resonator designed to amplify the ion acoustic oscillations. Thus, for success, several resonant phenomena have to be matched carefully. A 1200-W household microwave oven was used as the magnetron power source feeding into the open-ended quartz tube acoustic cavity resonator (20 cm long and 22 mm diameter) which has a small central belly where the carbon dust sample (made from reactor grade graphite) is mounted. In Egely’s experiments the carbon dust was wrapped in a thin cigarette paper and rolled into a ball prior to mounting in the sample holder. Egely has learnt by experience that the nano-carbon dust particles must have the right size and shape to couple with the resonator characteristics, neither too small nor too large. In dusty fusion plasmas, nuclear reactions can take place to form the lightest to the heaviest nuclei on account of the unique Coulomb shielding mechanism that is at play. Although Egely has researched a variety of nuclear reactions including transmutation of radioactive nuclei into stable elements, in this review we restrict ourselves to only his studies on what he has characterized as the “Ohsawa Chain” which takes place when the plasma contains only C, O, and N and results in the formation of the following transmutation products shown in the attached chain diagram (Fig. 8): Ca, Fe, K, Cu, Zn, Mg, Ti, S, and Si. Note that in these chains, secondary and tertiary products also take part in further reactions. Postrun, the grains of ash in the sample holder was analyzed using EDX. Table 3 presents a summary of

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Chapter 13 Transmutations and isotopic shifts in LENR experiments

Si 14N, 16O, 18O, 12C

N

15N, 13C

Sc

even

odd

N

14,15 41Ca

16O 14N 27Al

54Fe

31P

27Al

C

28,30Si

12,13

24Mg 16O 40Ca

16O

18O

N

C

O

16,18

46,48Ti

Sc

15N

15N 39K

32S 18O 64Zn

63Cu

FIG. 8 Ohsawa chain diagram. From G. Egely, M. Balint and F. Rosko, Change of isotopic ratios in transmutations, Infinite Energy, 142 (2018) 13–20. See also Infinite Energy, 130 (2016) 10–25.

Table 3 Results from Egely’s 2016 paper [23] Element

#1

#2

#3

#4

#6

#8

#9

#10

Average

C O Mg Al Si K Ca Fe Cu Zn Ti S

13.6 27.3 0.99 4.48 44.9 0.68 1.09 6.85 0 0 0.56 0.03

9.84 23.5 1.47 8.15 44.87 0.64 2.07 10.93 0 0 1.28 0.23

33.3 32.9 0.64 3.41 21.67 4.49 0 1.93 0 0

21.4 38.7 1.18 5.78 23.86 5.68 0 1.95 0.87 0.75

16.7 36.3 3.81 8.92 22.6 2.47 3.46 4.48 0.72 0

23.0 32.8 1.95 8.42 21.4 3.83 0 6.67 1.17 0.8

12.7 39.3 1.4 20.78 18.6 2.28 0 4.25 0.69 0.0

19.1 39.6 1.92 11.89 17.17 2.49 0 5.47 0.85 0.89

21.0 36.0 1.82 9.87 20.89 3.54 4.13 0.72 0.41

Egely’s results as given in his 2016 paper. Independently Electron Probe Microanalysis (EPMA referred to earlier) also confirmed the presence of Ohsawa chain products. Some sulfur presumably due to 16O + 16O ! 32S was also found. Otherwise, there were no other elements found other than the Ohsawa chain products.

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It is noteworthy that although no calorimetry was performed, overall there did not appear to be any extreme energy release. Egely justifies this observation on the basis that some links of the Oshawa chain could be exothermic and others endothermic a feature supported by Daniel Szumski [24].

Transmutation on an industrial scale In the period 1978–2002 the Silcal Metallurgic Ltd., a Coimbatore (India)-based company was engaged in the production of Ferrosilicon alloy deploying a 12-MVA “Submerged Carbon Arc” powered smelter. During an 11-week-long nonstop round the clock operation of the plant in 1995, daily feed of raw materials was: quartz, 33.4 t (t is the standard abbreviation for the unit tonne ¼ 1000 kg) of which Si was 15.4 t, charcoal (with fixed carbon content) of 13.2 t, and scrap steel of 5.1 t, while the daily output production of Fe-Si alloy (73.5% Si) was 24.75 t. From the total weights of Si and Fe in the input feed and assuming 100% recovery of the metals, the daily output alloy production could at best have been only 20.5 t. However, to the surprise of the plant management, throughout the 11-week period, the total daily Fe-Si alloy (with 73.5% Si) output was consistently 24.75 t, corresponding to a daily “anomalous” excess metal production of 4.25 t of FeSi alloy. In his paper presented at ICCF 20 [25] the plant owner Narayanaswamy has stated that the only source of Si entering the smelter furnace was the quartz raw material and that of Fe in the form of scrap steel (besides minor additional amounts of Fe originating from the steel casing of the consumable “Soderberg” carbon electrodes). From the records of weights of daily input feed of raw materials and output alloy drained out, as also the electrical energy consumption, it was evident that roughly 20% more metal than can be accounted for from the input feed was being produced and the management was obliged to come to the conclusion that anomalous quantities of Si (2.8 t per day) and Fe (1.45 t per day) was synthesized during those 11 weeks. Unfortunately, the plant had to be shut down within months of these observations since there were frequent power outages in the State of Tamil Nadu. Narayanaswamy has noted in his paper that although they had been observing anomalous excess production of Si and Fe ranging from 200 to 400 kg per day right from 1985 onwards, they were not sure whether these were due to errors in weighing or could be attributed to the anomalous generation of Si and Fe. However, following the consistent and repeated observation of about 4.25 t of daily excess metal production over the 11-week round the clock run in 1995, they were convinced beyond doubt that anomalous transmutation processes were indeed occurring. It was only after the 1995 incidence that they released their anomalous findings to the public through a press briefing in 1999. At that point in time, however, they were not aware either of the Carbon Arc experiment nor had they even heard of Cold Fusion/LENR. However, they were fully conscious of the fact that their claims of tons per day levels of transmutations will be met with intense skepticism. Based on the discussions presented in the immediate previous sections of this chapter on the Carbon Arc experiment and Egely’s dust fusion process, it appears reasonable to speculate that in Silcal company’s furnace too in the reaction zone where the main chemical exothermic chemical reduction takes place at 2000°C, simultaneous nucleosynthesis reactions could have occurred. In the submerged arc furnace, there are three gigantic 1-m diameter steel jacket encased consumable carbon electrodes. Intense cyclical magnetic fields are generated by the three-phase kA levels of alternating current (AC) driving the arcing between the three gigantic carbon electrodes and the carbonic hearth of the furnace, in a 2000°C temperature environment. This clearly points to the industrial smelter being a gigantic

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Chapter 13 Transmutations and isotopic shifts in LENR experiments

scaled-up version of the Carbon Arc experiment. As noted in the Carbon Arc and Dust Fusion sections above, the conditions in the reaction zone of the Arc furnace appear appropriate for the catalyzation of transmutation reactions to occur. It is therefore posited that the carbon monoxide (CO) gas formed undergoes a nuclear reaction resulting in Si and Fe as described in the Ohsawa Chain of reactions by Egely. However, the most puzzling aspect of Narayanaswamy’s findings is not only the observation of tons per day levels of transmutation having occurred but this has happened without the release of the expected massive amounts of nuclear heat that should have accompanied the tons per day quantities of transmutation reactions based on the atomic masses of the nuclei involved. His ICCF 20 paper discusses the puzzle of the missing energy in some detail. But in this chapter in view of the understandable skepticism surrounding such claims additional details of the plant and its operational parameters are given below to reinforce the fact that his claimed observations are not whimsical. Raw materials used for the production of Fe-Si alloy are low Alumina content Quartz (SiO2) of 98.7%–98.8% purity, steel scrap, and wood charcoal with low ash content which served as the reducing agent. Quartz was sourced directly from selected mines in the state of Tamil Nadu which are known to have low Alumina content. Wood charcoal on arrival was tested for moisture and fixed carbon and screened to separate fine dust and placed in indoor/outdoor storage. Steel scrap was stored in an outdoor yard. All raw materials on arrival were analyzed for purity at the in-house testing lab and the data carefully archived. The raw materials were taken by a conveyor system to the third floor of the furnace and stored in separate overhead bunkers. Each of the three raw materials was weighed according to a computerized batching system and transferred into charging buckets running on monorails in the second floor. Charging buckets containing the premixed raw materials were then discharged into the furnace every 10–15 min through chutes. Shift-wise consumption of all raw materials was totaled to obtain daily (24 h) consumption data. The molten alloy product was drained through one of the three tap holes at the bottom of the furnace every 2–2.5 h into tiltable “teeming ladles” mounted on rail tracks. The teeming ladles were then emptied into large stationary heat resistant cast iron trays to a thickness of approximately 50 mm. Next day, during the day shift the solidified Fe-Si slabs were manually broken into small pieces, weighed, and packed into 40 kg bags for domestic consumers or in 1-ton jumbo bags for export. Each batch of Fe-Si was individually analyzed adopting standard procedures prevalent in this industry. The voltage applied to the three electrodes was three-phase AC, typically in the 100–200 V region, using step-down transformers to convert from 110 kV/11 kV/ to furnace voltage from grid-supplied power. Arc currents were in the 30–60 kA region. The arc is struck between the 1-m diameter vertically mounted steel-encased consumable Soderberg electrodes and the floor of the carbon hearth. Both the carbon of the self-baking electrodes and its steel casing are consumed in the smelting process, the consumption being 50–60 kg per tonne of Fe-Si. Details of the procedure adopted to replenish the electrodes online without interrupting furnace operation is discussed in Refs. [1–4]. The whole process is slagless and the only product is molten Fe-Si alloy drained from the bottom and CO effluent gas (part of which may be used up in situ by nuclear transmutation processes) that burns at the top of the furnace, combining with atmospheric oxygen to become CO2 which is released through a stack after scrubbing as per applicable environment regulations. The 12-MVA furnace was operated round the clock at variable ratings from 7 to 12 MVA, depending on the availability of power. Various charge mix ratios and operating electrical parameters were

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experimented with in order to arrive at the optimum conditions required for achieving 73%–74% silicon content alloy. Systematic records of the total weight of the raw material feed consumed every day, as also the total weight of the product alloy tapped out daily was maintained. Cumulative daily consumption of electrical power was also recorded. A maximum daily production of 27.5 t of product alloy was achieved when the furnace was operated under full load conditions. The company was very successful and made good profits, supplying high-quality products to both local and export markets. Plant records show that to produce 1 kg of silicon content in the product alloy, about 11 kWh of electrical energy is needed. This observation also tallies with the expected energy consumption estimate based on theoretical considerations of the chemistry of the reduction reaction which is endothermic. In the Silcal plant, the product alloy contained 73%–74% silicon content. Taking an average value of 73.5%, 735 kg of Si would be present in each tonne of product alloy (the balance being Iron). Power consumption for producing 1 t of alloy thus works out to 11  735 ¼ 8085 kWh. However, dissolving iron into molten silicon is exothermic; a rough estimate of heat release due to 265 kg of iron dissolving into 735 kg of silicon is around 100 kWh of heat energy. Thus, production of 1 t of Ferrosilicon alloy of 73.5% Si content would require a net energy input of 8085–100 ¼ 7985 kWh. As already noted during early 1995, the furnace was operated continuously on a round the clock basis at a rating of between 8.5 and 8.75 MVA with a daily power consumption of 168,000 kWh per day. Thus, the total weight of the main raw materials, namely SiO2, Fe, and C consumed daily was 51.3 t. Net silicon content in product alloy works out to 24.75  0.735 t ¼ 18.2 t compared to 15.4 t in the input feed. Excess silicon was thus 2.8 t corresponding to an 18% increase. Likewise, the net weight of Fe in the product alloy works out to 24.75  0.265 ¼ 6.55 t compared to 5.1 t that was input, implying excess iron of 1.45 t or 28.4% weight gain. The most obvious source of doubt leading to an erroneous conclusion is errors in weighing of input feedstock and output alloy produced. The two main weighing points involved are the balance at the top of the furnace weighing the input feeds and the weighing machine on the ground floor where the product alloy pieces are weighed and loaded into bags for shipment to customers. These machines are made by reputed manufacturers such as Avery whose technicians visit the factory periodically to calibrate and check their accuracy as per industrial regulations. As operators of a commercial production plant, they were most conscious of maintaining proper records of material balance from an accountancy point of view. Payments were involved for raw materials received and products dispatched to customers. It is noteworthy that a 25% increase in plant output with essentially zero input manifests as a 100% increase in profits. Had there been unaccounted amounts of additional SiO2 in the feedstock, it would have shown up in the electrical power consumption records—the so-called “chemical energy signature.” The daily total power consumed would have proportionately gone up such that specific power consumed remained at the level of 7985 kWh per t of Si produced. But in the presence of nuclear transmutation processes occurring also the total power used remained the same despite the weight of product alloy having increased. This observation can be taken to be indicative of the fact that the additional Si production did not come through chemical reduction processes but must have arisen through some other cause. A significant additional qualitative observation made by the plant operators was that whenever nuclear transmutation processes appeared to take place, the heat radiated in the furnace top floor where CO burns to form CO2, was noticeably less implying that the amount of CO reaching the top of the furnace was less than expected.

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Chapter 13 Transmutations and isotopic shifts in LENR experiments

Biological transmutations In the 1960s, a book was published [26] by a French medical doctor titled “Biological Transmutations” which summarized the results of a number of prior experiments conducted over the previous couple of centuries that seemed to suggest that elemental (nuclear) transmutations do occur in plants and animals and even human beings. Of course, the techniques for analysis of the elemental composition of substances in those days were rather crude and as such the scientific community did not take the claims of biological transmutation seriously. Since the cold fusion era began many papers have been presented at various ICCF series conferences, especially on the topic of microbial transmutation. In recent years with mass spectroscopic instrumentation becoming more commonly available, isotopic anomalies in biological transmutation experiments have also been published. During the last decade, Vladimir Vysotskii of Ukraine and Jean Paul Biberian of France have conducted a series of systematic measurements carrying forward the field from where Kervran left it. 138 Vysotskii’s recent work reports on the transmutation of radioactive 137 55 Cs to stable 56 Ba using microbial colonies in light water-based cultures. A companion chapter in this book authored by Vladimir Vysotskii and his collaborators discusses recent progress in this area. This development has great significance for the nuclear industry which faces a problem of disposal of radioactive waste generated by nuclear power plants. But one basic question regarding biological transmutations, inclusive of microbial transmutation does not seem to have been answered satisfactorily. In these transmutation reactions, the expected nuclear energy release does not appear as heat. To that extent the phenomenon of biological transmutation too appears to follow the “missing energy category” that is discussed in other sections of this chapter.

Alchemy: Myth or science? The term alchemy historically referred to attempts made by early chemists in ancient China, India, Islamic Arabia, and eventually Europe to convert base metals such as lead into the noble metal gold (and also silver). But over time the alchemical quest became embroiled in mystery, symbolism, and hermetic philosophy and the ultimate narrative that has emerged is that although very serious efforts were made by the early chemists, they never succeeded in transmuting base metals into precious gold. Available alchemical accounts can be traced back to the second century CE. The website http://www. levity.com/alchemy/, for example, contains a very comprehensive compilation of the various sublines of inquiry that were born out of this quest. It is however universally conceded by all scholars and historians of science, that it was this persistent pursuit of alchemy that eventually evolved into the modern scientific discipline we now know as chemistry [27] culminating in the classification of the properties of various elements in the form of the periodic table of elements. There exists even today a “Society for the History of Alchemy and Chemistry” [28] founded in 1935 whose peer-reviewed journal “Ambix” is published quarterly even now. Not many are aware that one of the foremost pioneers of modern science, namely Isaac Newton (1642–1727), was fascinated with alchemy and secretly carried out a large number of experiments with a view to producing gold from mercury [29]. In 2004, The Indiana University at Bloomington established a “Newton Project” [30] to catalog all of Newton’s works including his handwritten unpublished notes under the title “The Chymistry of Isaac Newton.” The Oxford University in the UK too is

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participating in the Newton Project. Newton’s contemporary in England Robert Boyle was also obsessed with alchemy and the personal correspondence between Newton and Boyle are preserved in the Archives of the Royal Society in England [31]. In 1996 a student of the Department of History of Science of Johns Hopkins University in the USA, Lawrence Principe undertook a detailed study of the Boyle-Newton correspondence including the “lost” Dialogue on the Transmutation of Metals. Lawrence Principe has since written a book titled “The Aspiring Adept: Robert Boyle and his Alchemical Quest,” which was published [32] by the Princeton University Press in 1998. Cambridge University Press has published an anthology of all the great Alchemists of the west under the title “The Alchemy Reader: From Hermes Trismegistus to Isaac Newton” (2003) [33]. Interestingly there is even an anonymously authored handbook [34] supposedly giving “Plain and Honest Directions on how to make the Philosopher’s Stone,” a quest which consumed all the energies of Isaac Newton! The concept of the philosopher’s stone is central to historical alchemical procedures. Browsing through all these references gives the unmistakable impression that both Newton and Boyle did succeed in making gold. One of the big mysteries though is why did these alchemists clothe their studies in mystical language? One reason, of course, is that in England making gold or silver was a felony ever since a law was passed by Henry IV in 1404. But the other reason was obviously power and prestige. Who is going to let out a trade secret which gives them immense power and wealth? The making of gold was only one part of the story. The other closely guarded secret was their efforts to make the so-called “elixir of life” which was sought after by the nobles. Newton had advised Boyle to keep “high silence” and not reveal alchemical secrets to the public! This probably explains why when the biography of Newton was written after his death, his decades-long involvement in alchemical experiments was suppressed and hidden.

Alchemical synthesis of silver from silicon (Peter Grandics) Peter Grandics has described [35] a very simple alchemical experiment that he has personally conducted. Grandics’ experiment comprises two steps: In the first step, NaOH is refluxed for 24 h in a borosilicate glass reactor. After cooling to room temperature, the pH is made slightly acidic (pH 4– 5) by mixing with 1:1 HCl. The solution then turns turbid. From the slightly acidic pH, the mixture is then made mildly alkaline (pH 8) with the addition NaOH. The solution now slowly clears, and a white precipitate collects at the bottom of the reactor. The precipitate is then washed with deionized water, allowed to settle, washed again repeatedly to remove residual salts, centrifuged and then air dried. Next, the precipitate is heated at 70°C for 7 h. The granular, soft white material is then crushed to a fine powder in a porcelain mortar and stored in a plastic jar at room temperature. In the second step the white powder is mixed with high-purity carbon powder at various ratios and heated in a graphite crucible to 1200°C for 1–24 h in a tubular furnace. The heating of concentrated NaOH solution and subsequent neutralization led to the formation of a white precipitate that is represented by the chemical formula Na0.07Al0.04SiO2.27. It is predominantly SiO2 with minor amounts of Na and Al along with several trace components. When heated at 1200°C in a high-purity graphite block, numerous grains appear that were absent in the starting material. Subsequent EDS analysis of the grains demonstrated Ag as the main reaction product, along with some U. No Ag or U was detected in the starting white precipitate used in the experiment or analysis setup.

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Chapter 13 Transmutations and isotopic shifts in LENR experiments

Alchemical experiments at Texas A&M University During 1992–93 Prof. John Bockris of the Dept. of Chemistry at TAMU, was given a research contract to carry out an Alchemical “mercury to gold transmutation verification experiment” for which the protocols, as well as funding, was provided by industrialist Joe Champion. Italian physicist Roberto Monti who had been involved in Alchemical studies for a long time [20] was also recruited for these experiments which was code named “Philadelphia Project.” A detailed account of the Philadelphia Project has been documented by Bockris in the Proceedings of the ICCF 11 Conference under the title “History of the Discovery of Transmutation at TAMU” [36]. The experimental method known as “Explosion method” or “Impact method” in Alchemical literature was followed. This involves mixing in the appropriate proportions certain chemicals, such as lead chloride, mercurous chloride, potassium nitrate, and graphite powder which was then ground into a very fine powder in a pestle and mortar and was kept continuously shaken overnight. This mixture of the above noted chemicals is known to be an explosive. The next day about 1.6 kg of the finely ground powder was placed in a ceramic pot and a mild explosion was set off using a propane flame. The procedure was done in a fume hood as a safety precaution. The temperature is estimated to have reached about 1000°C for a few seconds. The pot was then allowed to cool for 3 days during which, as Champion had predicted, one could measure the 18.3 h half-life of 197Pt radioactivity. 197Pt is the intermediate nucleus which forms when an alpha particle (42He) is ejected from an 201 80 Hg nucleus. The above experiment was conducted six times in all with slightly different initial compositions in Bockris’ Lab and the results are summarized in Table 4. In 5 out of 6 tests radioactivity was measured while the gold content increased by a factor of almost 1000. The full details of the experiments and results are documented in Ref. [36] It is a different matter that many of Bockris’ colleagues in the Chemistry Department of TAMU took strong exception to a University professor actually conducting an alchemical experiment in the 20th century! “Everybody knows alchemy is nonsense,” they said! The story of this scientific drama including how an inquiry was carried out and how Prof. Bockris was eventually exonerated has been published in the Journal “Accountability in Research” in 2000 [37]. Meanwhile, the Federal Bureau of Investigations (FBI) got involved and imprisoned Joe Champion for violating some financial regulations. But from prison, Joe wrote a book titled “Twentieth Century

Table 4 Main results obtained in the TAMU experiments (April to June 1992) Experiment

Main Results Obtained in April-June 1992

Thermal 1 Thermal 2 Thermal 3

Two times increase of Pt was observed. One fire assay experiment showed the existence of visible Au 250–450 ppm of gold present in the product. An increase in Pd was also observed The weight of precious metal after cupeling from the chemical mixture with Hg was three to four times heavier than that without Hg, in the original mixture A large amount of gold, about 550 ppm was found The gold concentration in the product was about 178 ppm No gold was found in either experiment (with and without Hg in the raw material)

Thermal 4 Thermal 5 Thermal 6

From J.O’M Bockris, The history of the discovery of transmutation at Texas A&M University, Proceedings of the Eleventh International Conference on Condensed Matter Nuclear Science, Marseille, France (2004).

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257

Alchemy” [38] which not only corroborates what Bockris has stated in his account of the TAMU alchemical experiments but also discusses his prior alchemical journey. The book reveals that most of the pioneer researchers who explored the untrodden path of production of gold from base metals tragically died of leukemia due to exposure to radiation and ingestion of radioactive chemicals!

Activity patterns noted in European alchemical accounts Prof. Perez-Pariente was a distinguished professor of the Institute of Catalysis and Petroleum in Madrid. From his childhood he was fascinated with Alchemy especially the “alleged” property of the socalled “Philosophers’ Stone” (PS) to change certain base metals into noble metals, often instantaneously. In view of his background and expertise in chemical catalysis, he could appreciate certain similarities between the role of the Philosophers’ stone in alchemy and catalytic agents in catalysis. He identified six basic physical parameters in the extant reports of alchemical transmutations that have been recorded in various alchemical accounts and manuscripts [39]. These are the nature and weights of the initial base metal used (Hg, Pb, Cu, Sn, etc.) and the gold or silver produced, the weight of the PS used, and the duration of the trial. Table 5 lists data from seven additional alchemical events where these six parameters were recorded, in addition to the eight cases Perez-Pariente had analyzed in his earlier paper [40]. He defines a parameter termed as “Transmuting Power” as the weight ratio of the noble metal produced and the Philosophers stone used and finds a remarkable inverse correlation between the transmuting power and the duration of the alchemical transmutation experiment (Fig. 9). Interestingly, two data points of alchemical experiments conducted in India during 1942 and 1943 (described below) which was communicated to Prof. Perez-Pariente by one of the authors of this chapter (included in Table 5), also fit nicely into his inverse correlation curve. Thus, the faster the rate of transmutation the more efficient is the process, like that displayed by many conventional chemical catalysts.

Indian alchemical texts In India, the subject of Alchemy was developed by Ayurvedic physicians and was known as Rasa Vaidya or Rasa Shastra. The word “rasa” refers to mercury which plays a crucial role in alchemy. A scholarly Indian reference for this topic is the book “Alchemy and Metallic Medicines in Ayurveda” Table 5 Data of second set of seven additional Alchemy Accounts Ex.

Year

Reference Name

Type of Transmutation

Wi

Wf

WPS

Wf/WPS

Time (min)

1 2 3 4 5 6 7

1603 1627 1675 1675 1922 1941 1942

Seton P.J. Fabre Seyler Seyler Canseliet India India

Pb ! Au Hg ! Ag

3.5 oz 1 oz

3.5 –

0.5 grain 0.5 grain

Pb ! Au Hg ! Au Hg ! Au

– 12 g 2400

120 g 12 g –

20–30 mg 125–187 mg 12 g

4000 1100 1000–4000 10,000 6000–4000 96–64 200

15 30 100 elements, Trans. Am. Nucl. Soc. 83 (2000) 369. [157] T. Mizuno, T. Ohmori, T. Akimoto, Generation of heat and products during plasma electrolysis, in: P.L. Hagelstein, S.R. Chubb (Eds.), Tenth International Conference on Cold Fusion, World Scientific Publishing Co., Cambridge, MA, 2003, pp. 73–88 [158] T. Ohmori, H. Yamada, S. Narita, T. Mizuno, Y. Aoki, Enrichment of 41K isotope in potassium formed on and in a rhenium electrode during plasma electrolysis in K2CO3/H2O and K2CO3/D2O solutions, J. Appl. Electrochem. 33 (2003) 643. [159] T. Mizuno, Y. Aoki, D.Y. Chung, F. Sesftel, Generation of heat and products during plasma electrolysis, in: J.-P. Biberian (Ed.), 11th International Conference on Cold Fusion, World Scientific Co., Marseilles, France, 2004, p. 161. [160] T. Mizuno, Y. Toriyabe, Anomalous energy generation during conventional electrolysis, in: A. Takahashi, K. Ota, Y. Iwamura (Eds.), Condensed Matter Nuclear Science, ICCF-12, World Scientific, Yokohama, Japan, 2005, p. 65.

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[161] Y. Toriyabe, T. Mizuno, T. Ohmori, Y. Aoki, Elemental analysis of palladium electrodes after Pd/Pd light water critical electrolysis, in: A. Takahashi, K. Ota, Y. Iwamura (Eds.), Condensed Matter Nuclear Science, ICCF-12, World Scientific, Yokohama, Japan, 2005, p. 253. [162] T. Mizuno, Transmutation reactions in condensed matter, in: J. Marwan, S.B. Krivit (Eds.), Low-Energy Nuclear Reactions Sourcebook, ACS Symposium Series 998American Chemical Society, Washington, DC, 2008, p. 271. [163] H. Kozima, T. Mizuno, Investigation of the cold fusion phenomenon in the surface region of hydrogen non-occlusive metal catalysts; W, Pt, and Au, Am. Phys. Soc. (2009) 16003. [164] T. Mizuno, Method of controlling a chemicallyinduced nuclear reaction in metal nanoparticles, in: ICCF-18, Columbia, MO, 2013. [165] Y. Iwamura, N. Gotoh, T. Itoh, I. Toyoda, Characteristic X-ray and neutron emissions from electrochemically deuterated palladium, in: S. Pons (Ed.), 5th International Conference on Cold Fusion, IMRA Europe, Sophia Antipolis Cedex, France, Monte-Carlo, Monaco, 1995, p. 197. [166] Y. Iwamura, H. Itoh, N. Gotoh, M. Sakano, I. Toyoda, H. Sakata, Detection of anomalous elements, X-ray and excess heat induced by continuous diffusion of deuterium through multi-layer cathode (Pd/CaO/Pd), Infinite Energy 4 (1998) 56. [167] Y. Iwamura, T. Itoh, N. Gotoh, M. Sakano, I. Toyoda, H. Sakata, Detection of anomalous elements, X-ray and excess heat induced by continous diffusion of deuterium through multi-layer cathode (Pd/CaO/Pd), in: F. Jaeger (Ed.), The Seventh International Conference on Cold Fusion, ENECO, Inc., Salt Lake City, UT, Vancouver, Canada, 1998, pp. 167–171. [168] Y. Iwamura, T. Itoh, N. Gotoh, I. Toyoda, Detection of anomalous elements, X-ray, and excess heat in a D2-Pd system and its interpretation by the electron-induced nuclear reaction model, Fusion Technol. 33 (1998) 476. [169] Y. Iwamura, T. Itoh, M. Sakano, Nuclear products and their time dependence induced by continuous diffusion of deuterium through multi-layer palladium containing low work function material, in: F. Scaramuzzi (Ed.), 8th International Conference on Cold Fusion, Italian Physical Society, Bologna, Italy, Lerici (La Spezia), Italy, 2000, pp. 141–146. [170] Y. Iwamura, T. Itoh, M. Sakano, Nuclide Transmutation Device and Nuclide Transmutation Method, Mitsubishi Heavy Industries, Ltd., USA, 2002. [171] Y. Iwamura, T. Itoh, M. Sakano, S. Sakai, Observation of low energy nuclear reactions induced by D2 gas permeation through Pd complexes, in: X.Z. Li (Ed.), The Ninth International Conference on Cold Fusion (ICCF9), Tsinghua University, Beijing, China, 2002, p. 141. [172] Y. Iwamura, M. Sakano, T. Itoh, Elemental analysis of Pd complexes: effects of D2 gas permeation, Jpn, J. Appl. Phys. A 41 (2002) 4642–4650. [173] Y. Iwamura, T. Itoh, M. Sakano, S. Sakai, S. Kuribayashi, Low energy nuclear transmutation in condensed matter induced by D2 gas permeation through Pd complexes: correlation between deuterium flux and nuclear products, in: P.L. Hagelstein, S.R. Chubb (Eds.), Tenth International Conference on Cold Fusion, World Scientific Publishing Co., Cambridge, MA, 2003, pp. 435–446. [174] A. Iwamura, T. Itoh, M. Sakano, N. Yamazaki, S. Kuribayashi, Y. Terada, T. Ishikawa, J. Kasagi, Nuclear transmutation induced by deuterium permeation through the Pd complexes detected by surface asnd bulk analysis methods, in: ICCF-11, Marseilles, France, 2004. [175] Y. Iwamura, T. Itoh, M. Sakano, N. Yamazaki, S. Kuribayashi, Y. Terada, T. Ishikawa, J. Kasagi, Observation of nuclear transmutation reactions induced by D2 gas permeation through Pd complexes, in: J.P. Biberian (Ed.), ICCF-11, International Conference on Condensed Matter Nuclear Science, World Scientific, Marseilles, France, 2004, pp. 339–350. [176] Y. Iwamura, T. Itoh, M. Sakano, N. Yamazaki, S. Kuribayashi, Y. Terada, T. Ishikawa, Observation of surface distribution of products by X-ray fluorescence spectrometry during D2 gas permeation through Pd cathodes, in: A. Takahashi, K. Ota, Y. Iwamura (Eds.), Condensed Matter Nuclear Science, ICCF-12, World Scientific, Yokohama, Japan, 2005, pp. 178–187.

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[177] A. Takahashi, F. Celani, Y. Iwamura, The Italy-Japan Project-Fundamental research on cold transmutation process for treatment of nuclear wastes, in: A. Takahashi, K. Ota, Y. Iwamura (Eds.), Condensed Matter Nuclear Science, ICCF-12, World Scientific, Yokohama, Japan, 2005, p. 289. [178] Y. Iwamura, T. Itoh, N. Yamazaki, J. Kasagi, Y. Terada, T. Ishikawa, D. Sekiba, H. Yonemura, K. Fukutani, Observation of low energy nuclear transmutation reactions induced by deuterium permeation through multilayer Pd and CaO thin film, J. Condens. Matter Nucl. Sci. 4 (2011) 132–144. [179] Y. Iwamura, T. itoh, Y. Terada, T. Ishikawa, Transmutation reactions induced by deuterium permeation through nano-structured Pd multilayer thin film, Trans. Am. Nucl. Soc. 107 (2012) 422. [180] Y. Iwamura, T. Itoh, N. Yamazaki, N. Watari, H. Yonemura, K. Fukutani, D. Sekiba, Recent advances in deuterium permeation transmutation experiments, J. Condens. Matter Nucl. Sci. 10 (2013) 63–71. [181] Y. Iwamura, S. Tsuruga, T. Itoh, Increase of transmutation products in deuterium permeation induced transmutation, in: A. Kitamura (Ed.), Proc. JCF13, Japan CF-Research Soc, WincAichi, Jap, 2012, pp. 196–213. [182] Y. Iwamura, J. Kasagi, H. Kikunaga, H. Yoshino, T. Itoh, M. Hattori, T. Mizuno, The launch of a new plan on condensed matter nuclear science at Tohoku University, JCMNS 19 (2016) 119–126. [183] L.C. Kong, X.L. Han, S.X. Zheng, H.F. Huang, Y.J. Yan, Q.L. Wu, Y. Deng, S.L. Lei, C.X. Li, X.Z. Li, Nuclear products and transmutation in a gas-loading D/Pd and H/Pd system, J. New Energy 3 (1998) 20. [184] J. Dufour, D. Murat, X. Dufour, J. Foos, Experimental observation of nuclear reactions in palladium and uranium, Trans. Am. Nucl. Soc. 83 (2000) 356. [185] E. Storms, Explaining cold fusion, J. Condens. Matter Nucl. Sci. 15 (2015) 295–304. [186] E.K. Storms, A theory of LENR based on crack formation, Infinite Energy 19 (2013) 24–27. [187] E.K. Storms, B. Scanlan, What is real about cold fusion and what explanations are plausible? in: J. Marwan (Ed.), AIP Symposium Series, American Institute of Physics, 2010. [188] M.C. McKubre, The conditions for excess heat production in the D/Pd system, in: ASTI-5, Asti, Italy, 2004, www.iscmns.org. [189] E. Wigner, H.B. Huntington, On the possibility of a metallic modification of hydrogen, J. Chem. Phys. 3 (1935) 764. [190] E.G. Brovman, Y. Kagan, A. Kholas, Properties of metallic hydrogen under pressure, Phys. JETP 35 (1972) 783–787. [191] R.L. Liboff, Fusion via metallic deuterium, Phys. Lett. 71A (1979) 361. [192] S. Badiei, P.U. Andersson, L. Holmlid, High-energy Coulomb explosions in ultra-dense deuterium: time-of-flight-mass spectrometry with variable energy and flight length, Int. J. Mass Spectrom. 282 (2009) 70–76. [193] E. Storms, How basic behavior of LENR can guide a search for an explanation, JCMNS 20 (2016) 100–138. [194] E. Storms, How the explanation of LENR can be made consistent with observed behaviour and natural laws, Curr. Sci. 108 (2015) 531–534. [195] S. Jiang, J. Liu, M. Hea, A possible in-situ 3H and 3He source in Earth’s interior: an alternative explanation of origin of 3He in deep Earth, Naturwissenschaften 97 (2010) 655–662.

CHAPTER

Models based on phonon-nuclear coupling

15 Peter L. Hagelstein

Massachusetts Institute of Technology, Cambridge, MA, United States

Introduction The claim of the observation of excess heat in the Fleischmann and Pons experiment, along with Fleischmann’s suggestion of a nuclear origin [1, 2], stimulated considerable theoretical speculation. Much of it has been focused on the problem of getting deuterons sufficiently close to fuse, and less on the perhaps more significant problem of the near total absence of energetic nuclear products which one would expect from a nuclear energy source. Notable exceptions include Schwinger, who considered the possibility of a down-conversion of the nuclear quantum to vibrations [3, 4]; and Preparata, who described a model in which the large nuclear quantum is down-converted to plasma oscillations [5, 6]. Many modern physical theories are basically simple in form. In the case of photon or phonon exchange, the basic interactions are known. To develop a fundamental model for excess heat in the Fleischmann-Pons experiment, the first problem is to determine what interaction is involved. Next, the big theoretical problem is in the down-conversion of the large nuclear quantum; hence to develop a model one needs a mechanism capable of such an extreme down-conversion. Retrospectively, these two problems are clearly the most important, and have been the focus of much of our attention. We began thinking that conventional electric and magnetic dipole interactions between the condensed matter environment and internal nuclear states would provide the interaction; but ultimately concluded that a stronger interaction was needed. In what follows, we discuss a relativistic boost interaction, which is on solid theoretical footing, but does not seem to have been considered in connection with condensed matter applications previously. We first found a mechanism for down-conversion based on many sequential interactions in the case of an oscillator coupled with many two-level systems in the presence of loss. More recently, we have noticed that no loss is needed for down-conversion if off-resonant energy shifts are present and large. The theory that results in our view applies to excess heat in the Fleischmann-Pons experiment, but also connects with many other experimental anomalies that have been reported. In addition, new effects are predicted (such as excitation transfer), which allow for tests by which the model can be verified or disproved.

Cold Fusion. https://doi.org/10.1016/B978-0-12-815944-6.00015-4 # 2020 Elsevier Inc. All rights reserved.

283

284

Chapter 15 Models based on phonon-nuclear coupling

Phonon-nuclear coupling The problem of the interaction with internal nuclear degrees of freedom with a lattice has a long history. Waller [7] considers the interaction of spins with the lattice, based on the dynamical spin-spin interaction induced by vibrations [7]. Heitler and Teller [8] suggested a generalization of the model in which an indirect coupling of the dynamical electric field and spins is included, and used this to estimate nuclear spin relaxation by coupling with lattice phonons [8]. They proposed that the coupling of nuclear spins to electrons in a metal would provide a much stronger interaction. A brief review of some of the early work is given in Ref. [9]. Deformed nuclei have a quadrupole moment that couples to electric field gradients [10, 11], which gives rise to splittings in molecules, and splittings and relaxation in crystals. Theoretical and experimental research which makes use of electric or magnetic interactions has focused on the nuclear states of a single level which would be degenerate in the absence of electric and magnetic fields. Lattice-induced transitions between nuclear states at different energies would be expected as a natural generalization of these interactions. We would expect the same physics that leads to the quadrupole splitting of a single level to produce electric dipole coupling to E1 (electric dipole) transitions between nuclear states at different energies. For the interaction between a nucleus and local electrons, we can make use of perturbation theory to write for the dipole-dipole interaction 

H^int ¼ 

X Z j e2 rj  rk 3

j, k 4πE0 jrk j

! D 

X

erk

k

4πE0 jrk j3

(1)



where Z j is the effective charge of nucleon j (due to the separation of center of mass and relative degrees of freedom) and D is the nuclear dipole operator. We would expect the strongest coupling for this electric dipole interaction, which would provide a foundation for phonon-nuclear coupling and also coupling between the nuclear transition and free electrons in a metal. The spin-lattice interaction, and also coupling between free electrons and spin, in the literature generalize directly to provide a coupling for M1 (magnetic dipole) nuclear transitions. Were we to follow this approach we might end up with a generalized hyperfine interaction Hamiltonian for electric and magnetic nuclear dipole transitions of the form i X μ0 h 2 X ^i r r Þð μ ^i r r Þ  μ ^ k δ3 ðrj  rk Þ  ^ ^ ^ ^ ^j  μ H^int ¼  μ0 3ð μ    μ μ j k j k k j k j 3 3 j, k j, k jrj  rk j X X erk Zk erk Dj  + Dj   4πE0 jrj  rk j3 j, k 4πE0 jrj  rk j3 j, k

(2)

In past years, this way of thinking provided a foundation for our view of the coupling between the lattice and nuclei. However, when we tried to develop quantitative rate estimates for up-conversion and for excitation transfer, the theoretical estimates were too low. This provided motivation to see whether there might be additional interactions, recognizing that this was unlikely since additional interactions would probably have been noticed over the past 80 years and more. Such a candidate emerged at the end of 2011 in the relativistic boost correction of the nucleon-nucleon interaction. Models for the nucleon-nucleon interaction based on meson exchange [12], and more recently models based on pion exchange in chiral effective field theory [13], lead to an interaction that depends explicitly on the nucleon momentum. Consequently, if a nucleus is moving then the nucleon-nucleon interaction will be different. This effect was first noticed by Breit [14], who considered the impact of relativity on nuclear models by considering nucleons as Dirac particles [14]. Breit focused on the

Finite basis hamiltonians

285

elimination of the boost correction for a nucleus in free space, as did some others that followed. However, for a nucleus that oscillates or accelerates the interaction due to the boost correction cannot be completely eliminated through a rotation. Consider a many-nucleon model for a nucleus made up of Dirac particles according to H^ ¼

X j

βj mc2 +

X

αj  c^ pj +

j

X

V^jk ðrj  rk Þ

j ¼ 0 and < p > ¼ 0, the wave function of the particle, which was in the ground state prior to the deformation, depends on the correlation coefficient and has the form [4–12]: 2

0

13

2 1 ir ðtÞ C7 6 q B ffiffiffiffiffiffiffiffiffiffi exp  Ψ0 ðq, tÞ ¼ p 4 @1  qffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiA5 4 4σ 2πσ q q 1  r ðtÞ2

The explicit form of the correlation coefficient:

(28b)

346

Chapter 17 Universal mechanism of LENR in physical and biological systems   ,  dε dε ε∗  r ¼ Re ε∗  dt  dt

(29)

the compression coefficient k, which determines the ratio of the dispersions of the coordinate and momentum of the particle: k ¼ σ q =σ p ¼ jε=ðdε=dtÞj2

(30)

pffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi pffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi σ q
ðħ=2Þ k=ð1  r 2 Þ, σ p
ðħ=2Þ 1=kð1  r 2 Þ

(31)

and the values of these dispersions:

can be found on the basis of the solution of the equation of a classical oscillator with a variable frequency ω(t) at the presence of an external force: d2 ε + ω2 ðtÞε ¼ f ðtÞ dt2

(32)

 dε ¼i dt 0

(33)

at initial conditions εð0Þ ¼ 1,

In Eqs. (28)–(32) and in following relations ω(t), the dimensionless frequency is normalized to the characteristic oscillator frequency ω0; t is a dimensionless (normalized to ω1 0 ) time; ε(t) is the dimenpffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi sionless (normalized to q0 ¼ ħ=Mω0 ) complex coordinate of the particle; and Mis the reduced mass of the particle. In the general case, the solution of Eq. (31) has the form ε(t) ¼ eφ(t), φ(t) ¼ α(t) + iβ(t). Substituting this solution into (29), (32), using the initial conditions following from (33): φð0Þ ¼ αð0Þ ¼ βð0Þ ¼ 0,

   dφ dα dβ ¼ i, ¼ 0, ¼1 dt 0 dt 0 dt 0

(34)

and separating the real and imaginary parts of the resulting equation, we can find:

2 ðt d2 α dα 2 +  exp ð4αÞ ¼ ω ðtÞ, βðtÞ ¼ exp f2αðt0 Þgdt0 , dt dt2

(35)

0

vffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi (  )ffi u 2 u dα dα 2 t exp ð4αÞ= 1 + exp ð4αÞ |r| ¼ dt dt

(36)

It is clear from (36) that obtaining the limiting value | r | ! 1 is possible only if the condition (dα/ dt)2 exp(4α) 1 is satisfied. The system of Eqs. (35), (36) is equivalent to Eq. (32), but it is more convenient for analysis and allows us to find from (35) the exponent of the amplitude of oscillation α(t) and then, based on the given law of variation ω(t), to find r(t) from Eq. (36).

Methods of CCS formation in realistic physical, biological, and geological systems

347

A study of specific mechanisms for CCS formation under various modes of potential well deformation, as well as an analysis of peculiarities of this state in model and real systems, has been carried out in [7–18].

Formation of CCS for periodical modulation of harmonic oscillator parameters In [8–13, 16], the features of the formation of CCS for the particle in the case of a weak periodic effect on the parameters (in particular, the frequency) of the harmonic oscillator: ωðtÞ ¼ ω0 ð1 + g cosΩtÞ

(37)

in the case |g | 1 were examined in details. From the solution of Eqs. (29)–(33), it follows that the process of CCS formation for such modulation of the parameters of the potential well is characterized by the presence of the main (for Ω  ω0) and parametric (Ω  2ω0) resonances, beyond which the efficiency of this process very sharply decreases, although it remains nonzero [11.12,15,16]. Within these resonances | r | ! 1, as the modulation duration increases, it is interesting to note that the frequency half-width of the main resonance Ω  ω0 is very small (jδ ΩjΩω0 g | ω0), and the width of parametric resonance Ω  2ω0 is much larger and equals j δ Ω jΩ2ω0 ¼ 2gω0 (see Fig. 6A). From the same calculations it follows that, as the modulation duration increases, the maximum values of the correlation coefficient j r(t)jmax also increases rapidly. The largest rate of j r(t)jmax increase corresponds to the frequency Ω ¼ 2ω0 and it rises sharply with the frequency modulation index g, reaching at g ¼ 0.1 the value j rjmax ¼ 0.998 (which corresponds to Gmax  20) at ω0t  40 and j rjmax ¼ 0.999998 (Gmax  700) at ω0t  500. When ω0t
1000 the correlation parameters at g ¼ 0.1 exceed values j rjmax  0.9999999, Gmax  3000. An additional interesting aspect of LENR production is connected with the possibility of CCS formation under low-frequency nonresonant periodic action with Ω ω0 on the parameters of potential well, in which the particle is situated. Dynamics of CCS formation for the case Ω ¼ 104ω0 is shown in Fig. 7. This result is related to the spectral region, which is much smaller than the resonance peaks Ω ¼ ω0 or Ω ¼ 2ω0 in Fig. 6A and demonstrates that the synchronizing action of prolonged low-frequency pumping at the frequency Ω  (104...105)ω0 promotes the formation of the correlated coherent state with a large correlation coefficient 1  jrjmax  105, which corresponds to a large correlation efficiency coefficient Gmax
100 and, correspondingly, to a large transparency of the potential barrier for a particle with a low average energy interacting with the neighboring atoms (nuclei). One of the simplest implementations of such a “low-frequency” method is based on the use of tunable cyclotron resonance in a low-frequency magnetic field H(t) ¼ H0 sin Ωt. It is well known that the Schr€ odinger equation for a charged particle with the mass M and charge q in a magnetic field is similar to the equation for the harmonic oscillator with the same wave-functions, a similar energy spectrum En(t) ¼ nħω(t), n ¼ 1, 2, …, and frequency ω(t) ¼ ω0 sin Ωt, ω0 ¼ qH0/Mc. The low magnetic field is a very important advantage of this method for the formation of the coherent correlated state compared to the use of direct or parametric resonance, which requires resonance pumping at high frequencies Ω ¼ ω0 or Ω ¼ 2ω0. A disadvantage of low-frequency modulation compared to high-frequency resonance pumping is a much larger time necessary for the formation of the correlated coherent state.

1.0

|r(Ω)|max

1.0

348

|r|

0.8

0.4

0.2

2|g|

0.0

0

(A)

0.5

1.0 1.5

2.0 2.5

3.0

Ω/w0

0.0

(B) 1.0

1.0

40

0

|r|

80

120

w0t

160

|r| |r|=1

0.8 0.6 0.5 0.4

0.2 0.0

(C)

0

40

80

120

160

w0t

(D)

0.0

0

1.0000

|r|

|r| max =0.998

20

40

60

80

w0t

|r|

0.9998

|r|=1

|r|=1

|r| max =0.999998

0.9996

0.5 0.9994 0.9992

(E)

41.5

42

42.5

43

43.5 w0t

(F)

501

501.5

502

502.5

503 w0t

FIG. 6 (A) resonant structure of the dependence of correlation coefficient maximum versus frequency Ω of periodic modulation ω(t) ¼ ω0(1 + g cos Ωt) of the potential well parameters; (B)–(F) the dependence of the correlation coefficient versus time when parameters of the well are modulated at the fundamental frequency Ω ¼ ω0 at g ¼ 0.1 (B), g ¼ 0.2 (C) and at the frequency of the parametric resonance Ω ¼ 2ω0 at g ¼ 0.1 in the time intervals ω0t  100 (D), ω0t  45 (E) и ω0t  500 (F) [11].

Chapter 17 Universal mechanism of LENR in physical and biological systems

0.6

0.5

Methods of CCS formation in realistic physical, biological, and geological systems

349

1.00000

|r(t)| 0.99999

0.99998

0.99997

0.99996

1.0

1.1

1.2

1.3

1.4

Ωt

FIG. 7 CCS formation under low-frequency (Ω ¼ 104ω0) harmonic modulation of potential well.

At first glance, the variant with modulation at the “industrial” frequency Ω ¼ 50...60 Hz seems to be the most optimal, does not require additional equipment, and is easily implemented in any laboratory. Furthermore, it seems strange that anomalies connected with the formation of correlated coherent states under such conditions and responsible for significant change in the internuclear and interatomic interactions for any gas have not yet been randomly observed in numerous independent diverse experiments (in particular, in chemical processes) that were performed with the use of such electromagnets and did not directly concern the particular problem of the optimization of the nuclear interaction. Unfortunately, such direct application of low-frequency modulation turns out to be inefficient due to the fact that, with such a modulation, a long time of CCS formation is required. In this case, the presence of inevitable random phase fluctuations leads to disruption of synchronization of the eigenfunctions of the particle in this magnetic field. These fluctuations can be connected, for example, with random collisions of the particle under consideration with other particles. The influence of such random processes on CCS formation will be discussed below. As a result, the process of effective CCS formation under such a low-frequency action is possible only under conditions of deep vacuum [14]. Other aspects of this process and the possibility of using low-frequency pumping under more consistent conditions are considered in detail in [14].

Experiments on LENR stimulation at resonant action on the active medium The results of a theoretical analysis of the process of LENR stimulation during resonant modulating action on the active medium are in good agreement with known successful LENR experiments: (a) Two-beam laser experiment (D. Letts, D. Cravens, P. Hagelstein) This analysis can explain the results of the experiments [32] on stimulation of LENR under the synchronized action of two laser beams generated by low-power laser diodes (P  20 mW) with close frequencies to the Pd surface of a cathode located in heavy water in an electrolytic cell at the presence of an additional external magnetic field. These results are presented in Fig. 8. When the polarization of these laser beams coincides, the generation of a difference frequency that acts on electrons in conduction band of the cathode takes place. Action of this low-frequency field leads to the periodic modulation of the potential well parameters for localized deuterium ions in the

350

Chapter 17 Universal mechanism of LENR in physical and biological systems

FIG. 8 Dependence of the power release that is generated when a cathode of palladium, saturated with deuterium in a volume of heavy water, is irradiated by difference frequency Ω from two low-power laser diodes with close frequencies [32].

palladium lattice. Selecting the appropriate pairs of such diodes, the authors investigated the dependence of the energy release in such a system on this difference frequency in the interval 5..0.25 THz and found 4 resonance peaks of energy release with frequencies Ω1  7.8...8.2 THz, Ω2  10.2...10.8 THz, Ω3  15.2...15.6 THz, and Ω4  20.2...20.8 THz, having a different amplitude. Analysis of the deuterium vibrational structure in the Pd matrix [32] shows that the frequencies ω1  7.8...8.2 THz and ω2  10.2...10.8 THz correspond to the optical phonon modes (intrinsic vibrations of deuterium ions in the Pd lattice). Each of these ions is, in fact, a harmonic oscillator. There are many fundamental questions concerning the results presented in Fig. 8: •

•

• •

Why, at the coincidence of the lasers’ beat frequency Ω with the frequency of the optical phonon modes, does the energy release sharply increase and what is the mechanism of suppression of the Coulomb potential barrier at such laser irradiation? Why do the amplitudes of the excess energy (energy release) increase with the increase of the lasers’ beat frequency Ω for the 2nd, 3rd, and 4th resonances, P(Ω2) < P(Ω3) < P(Ω4), and decrease for the 1st and 2nd resonances, P(Ω1) > P(Ω2)? What is the nature of the excess energy resonance with the frequency Ω4  20.2...20.8 THz, and why is there no optical phonon mode of deuterons in the PdD system with such a frequency? Why does the external magnetic field influence the process of the excess energy at the laser action on the PdD system?

These results are in a good agreement with the data of the calculations [11.12,15,16] presented above (Fig. 6A), if we assume that the energy release is connected with the stimulation of nuclear reactions

Methods of CCS formation in realistic physical, biological, and geological systems

351

8 < He3 + n d+d! t + p ; Pd A + d ! AgA + 2 ! … : He4

at low energy in the volume of palladium saturated with deuterium. Comparing the dependences of the power output, shown in Fig. 8, and, accordingly, the structure of the frequency dependence of the correlation coefficient (Fig. 6A), it is easy to verify that the first and the third peaks in Fig. 8 correspond to the pair determined by the basic Ω ¼ ω1  7.8...8.2 THz and parametric Ω ¼ 2ω1  15.2...15.6 THz frequency resonances of the correlation coefficient formation, and the second and the forth peaks correspond to another pair (basic Ω ¼ ω1  10.2...10.8 THz and parametric Ω ¼ 2ω1  20.2...20.8 THz frequency resonances). The ratio of the amplitudes of the maxima of energy release in Fig. 8 fully corresponds to the results presented in Fig. 6: the first, lower peak of each pair corresponds to the lower efficiency of the formation of the CCS at the frequency of the main resonance, and the second, higher—to the greater efficiency at the parametric resonance frequency. The mechanism of CCS formation in this PdD system can be connected with different processes. Most probably, in the PdD compound in “Terahertz” laser experiments [32] such a mechanism can be connected with the plasmon excitation and can be based on the following two-step process: • •

excitation of the surface electron plasmon and modulation of the electron density on a surface of the PdD compound at a combined action of two coherent laser beams with different frequencies; modulation of the frequency of the optical phonon modes of deuterons in elementary cells of the Pd matrix under the action of electron density oscillations in the volume of these elementary cells.

The possibility of second modulation is connected with the influence of the electron screening on the parameters of the parabolic potential well (e.g., on the depth of the well) in the harmonic oscillators formed by the interaction of the Pd+ and D+ ions in the PdD elementary cells. The presence of an external magnetic field leads to the formation of a nonlinear polarization in the electron plasma of a solid, needed for the generation of the difference frequency at action of two lowpower laser beams with coinciding polarization and small frequency difference. A more detailed analysis of the considered features of this experiment has been carried out in [11]. (b) Experiment with cooled deuterium in a variable magnetic field (T. Mizuno, T. Akimoto, A. Takahashi, F. Celani) Another interesting experiment on LENR stimulation [33] was conducted in cooled D2 gas in strong variable magnetic field. The scheme of the experimental installation and the results of experiments are shown in Fig. 9. The experimental setup consisted of a solenoid (magnetic coil) with a high inductance L placed in a vessel into which, in certain cases, liquid nitrogen N2 was poured. An ampoule (reactor tube) with D2 gas was placed inside the coil. In the stationary mode (with a strong current of 80 A or 100 A), the flux of detected neutrons corresponded to the background value Jn  0.01 count/sec. With a rapid change of the current in the specified interval 80 $ 100 A (or during D2 gas intake into the reactor tube) and in the presence of cooling, an intense neutron flux Jn  5 count/sec was recorded during 3–5 s (see Fig. 9, right). With a similar current switching, but at the absence of cooling, neutron emission at a level above the background was not recorded.

352

Chapter 17 Universal mechanism of LENR in physical and biological systems

Electric current

10

Magnetic coil

5c/s; D2 gas intake

1

Counts/s

Background 0.1

0.0045 ± 0.003c/s

0.01

0.001 Detector of neutrons

0.0001 Liquid N2

Reactor tube with D2 gas

0

100

200

300

Time/min

FIG. 9 The experimental setup and the dependence of detected neutrons flux versus time for cooled D2 gas in strong variable magnetic field [9].

According to our analysis, these processes are fully consistent with the self-similar formation of CCS and their stimulating effect on the LENR reaction d + d ¼ He3 + n. The direct analysis of the used coil has shown that it was characterized by the following parameters: inductance L  10 H and parasitic (interturn) capacitance CL  100pF. The natural frequency and reactance of this coil are equal: pffiffiffiffiffiffiffiffi pffiffiffiffiffiffiffiffiffiffiffi Ω  1= LCL  30 kHz;X0 ¼ L=CL  300 kOhm

(38)

The active resistance of the copper conductor, from which the coil is made, depends on the temperature, and is equal to: ( RL 

5:::7 Ohm at T ¼ 77 K, 70:::80 Ohm at T ¼ 293 K, 100:::120 Ohm at T ¼ 373 K

(39)

From these data, it is clear that the reactance of the circuit is much higher than the active resistance and X0  RL. This ratio corresponds to the periodic mode of oscillation in the equivalent circuit. The presence of inductance, parasitic capacitance, and active resistance leads to the formation of an electric circuit, which has the form presented in Fig. 10. In the case of rapid change of electric current in the outer part of the circuit (at fast switching of resistors R1 and R2), an oscillating mode of current change takes place: I ðtÞ ¼ I2 + ðI1  I2 Þ cos ðΩtÞet=τ , τ  2L=RL >> 2π=Ω

(40a)

The flow of such an oscillating and slowly decaying electric current leads to a similar structure of the magnetic field in the volume of the reactor tube inside the coil:   H ðtÞ ¼ H2 + ðH1  H2 Þ cos ðΩtÞet=τ  H2 1 + g cos ðΩtÞet=τ , g ¼ |Hmax  Hmin |=Hmax ¼ 0:2

(40b)

Methods of CCS formation in realistic physical, biological, and geological systems

353

FIG. 10 Circuit corresponding to the current switching mode in the experimental setup.

Direct estimations showed that during the switch of the current, the stationary values of the magnetic field changed in the interval H1 $ H2 ¼ 8 $ 10 kOe. The characteristic decay time of current oscillations in the considered oscillatory circuit is determined by the value: ( τ ¼ 2L=RL 

3:::5 sec at T ¼ 77 K, 0:3  0:2 sec at T ¼ 293 K, 0:2  0:15 sec at T ¼ 377 K

(41)

Some number of D+2 ions are always present in the volume of D2 gas. The motion of these ions at the presence of a magnetic field corresponds to a harmonic oscillator: it has the same Hamilton operator, the 2 same wave functions Ψn(ξ) ¼ CnHn(ξ)e ξ /2, the same energy spectrum En ¼ (n + 1/2)ħωL, n ¼ 1, 2, …, and with a tunable cyclotron frequency: ωL ðtÞ ¼

h i |q|H ðtÞ  ωL ð0Þ 1 + g cos ðΩtÞet=τ  ωL ð0Þ½1 + g cos Ωt at t < τ Mc

(42)

Here, ωL(0)  40 MHz is the maximum cyclotron frequency in the center of the coil. At the periphery of the coil, the magnetic field decreases sharply. Since the size of the reactor tube significantly exceeded the size of the internal region of the coil, there was different cyclotron frequency amplitude ωL(0) in different parts of this tube. The most optimal (with respect to the formation of CCS) frequency ratio Ω ¼ 2ωL(0) corresponded to those ions from the gas composition, which were located at the periphery of the reactor tube. If this condition is met, then the law of frequency change (42) is fully consistent with the condition (37) of CCS formation and, accordingly, allows for effective nuclear fusion. Another possible mechanism of CCS formation can be connected with the nonresonant lowfrequency (at Ω ωL(0)) modulation of the parameters of an effective harmonic oscillator [14], which corresponds to the state of charged ions in a magnetic field. In the work [14], it has been shown that even with an extremely nonresonant ratio Ω  (104...105)ωL(0), it is possible to form an effective CCS with Gmax
103. The duration of the achievement of such a value Gmax is equal ещ topt  (1...2)/Ω  (104...105)/ωL(0) [14], which is in good agreement with the experimental results. The same agreement of the conditions of a real experiment with a theoretical model allows us to explain the unusual influence of the temperature of the system on the efficiency of nuclear fusion. It is well known that in the case of “traditional” nuclear fusion, its effectiveness always increases with an increase of temperature. In this experiment, the situation is the opposite and the probability of the fusion increases with a decrease of temperature.

354

Chapter 17 Universal mechanism of LENR in physical and biological systems

At a low temperature, T ¼ 77 K, the resistance of cooled coil is very small and does not exceed RL  7 Ohm. In this case, the duration of the oscillatory transient process is long and is equal to τ ¼ 2L/RL  3...5 sec. So, during this time the process of formation of the CCS can take place and nuclear fusion can be produced. In the opposite case (at the absence of forced cooling), the temperature of the coil during the flow of a high current can increase to T  350...370 K, which leads to a sharp increase of active resistance of the coil and, accordingly, to a very significant decrease of duration τ ¼ 2L/RL  0.2 sec of the oscillatory transient process, which leads to the impossibility of registration of reaction products. (c) Optimization of accelerator (Li + p) fusion at low proton energy (S. Lipinski, H. Lipinski) A similar mechanism of resonant formation of the CCS explains well the anomalous results of experiments on the implementation of accelerator fusion with a low-energy proton beam [31]. In these experiments, the process of alpha particles generation during the interaction of protons with a lithium target was studied at variable kinetic energy of moving protons. If we analyze this problem on the basis of “traditional” methods of accelerating nuclear (Li + p) fusion, we would expect that, at low energy, the efficiency of fusion would be very small up to an energy of about 5–10 KeV, and then it will continuously increase to an energy of >100 KeV. The actual results of this experiment are completely different, and are presented in Fig. 11. It is seen that the nuclear interaction of moving protons with lithium targets is characterized by a sharp peak. The position of this peak corresponds to the energy of particles in a narrow range near E ¼ 500 eV, where the maximum count rate of alpha particles reached J0  4 104 s1. It is easy to show that this result cannot be explained within “standard” models of a nuclear reaction involving accelerated particles. In particular, the direct use of the standard formulas: σ ðEÞ ¼ σ 0 DðEÞ,σ 0 ¼ SðEÞ=E, 9 8 > = < 2 R +ðLðEÞ pffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi > n pffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffio DðEÞ ¼ exp  2M½V ðqÞ  Edq  exp 31Z1 Z2 A=EðkeV Þ , > > ; : h R

J (counts/sec)

45,000 40,000 35,000 30,000 25,000 20,000 15,000 10,000 5000

Proton energy (eV)

0 0

500

1000

1500

2000

2500

3000

FIG. 11 Dependence of the rate of generated fast He4 nuclei versus proton energy.

3500

4000

(43)

Methods of CCS formation in realistic physical, biological, and geological systems

355

for the cross section of the nuclear reaction σ(E), involving two particles with the charges Z1e and Z2e, reduced mass M and corresponding mass number A, and the tunneling probability D(E) to the considered Li7 + p ¼ 2He4 + 17.3 MeV reaction gives an extremely small cross section σ(E)  1074 cm2, tunneling probability D(E)  1050, and the reaction rate J < 1058 s1 [18]. According to these estimations, no fusion reaction should be detected during a particular measurement (100 s) and, generally speaking, even during the time of the existence of the Universe. Here, S(E)  80 keV*barn is the astrophysical factor for the (Li7, p) reaction involving the main Li7 isotope (natural content of 92.4%) at E < 300 keV. On the other hand, the experimental rate of alpha particles in this experiment at resonant energy reached J0  4 104 s1, which is 1062 times more than the expected value. Another very interesting and surprising feature of these experiments was the complete absence of alpha particles with an energy of 1.9 MeV and 2.1 MeV, which should be formed in an alternative reaction Li6 + p ¼ He3(2.3 MeV) + He4(1.7 MeV) with other lithium isotope Li6 (see Fig. 12). It is shown in the work [18] that both of these paradoxes are easily explained if it is assumed that the fusion reaction is provided by the formation of a CCS during the passage of a proton through the periodic lithium lattice or through molecules, which are part of the lithium vapor (see Fig. 13). The results of the calculation of the change in the correlation coefficient versus distance and the average correlation efficiency coefficient versus proton velocity are presented in Fig. 14. This analysis is based on the fact that the motion of a proton in the system of potential wells and barriers is equivalent to its localization in a nonstationary harmonic oscillator. From the calculation results, it is clear that the maximum value of the correlation coefficient is produced at the optimal velocity, which (taking into account the lithium lattice parameters) corresponds to the proton energy: Topt ¼ mp v2opt =2 ¼ 2mp a2z < ω>2  400:::600 eV

that is in a good agreement with the experimental data. Another feature of these experiments (a ban on the course of the fusion reaction involving the light isotope) is also fully explained by the specificity of the nuclear reactions stimulated by the CCS. These features were discussed above.

FIG. 12 Energy spectrum of generated alpha particles He4 at proton energy E  300–500 eV [31].

356

Chapter 17 Universal mechanism of LENR in physical and biological systems

(1)

(1) (a)

(b)

(2)

(2)

V(x)

V(x)

FIG. 13 Top row: Diagrams of proton motion in the system of potential atom barriers in a diatomic Li2 molecule, a cluster of two molecules and in a Li crystal. Proton motion direction indicated by an arrow. Bottom row: Classical (a) and quantum-mechanical (b) models of channeling (proton motion in the interplanar space of a crystal) in the uncorrelated (1) and correlated (2) states.

10–9

1–|r|

10,000

8000 10–6 6000 10–3

4000 2000

10

vopt

0

(A)

0

1

2

3

N=z/az

(B)

0

1

2

3

v/(az) 4

5

6

FIG. 14 (A) The change of the correlation coefficient of a particle moving with the optimal velocity versus distance; (B) the average correlation efficiency coefficient < G > versus proton velocity.

357

Methods of CCS formation in realistic physical, biological, and geological systems

Features of CCS formation at a continuous change of parabolic potential well parameters CCS formation at limited increase of parabolic potential well width Let us find the solution of Eqs. (35), (36) with a limited increase of the width of parabolic well in the range from Lo to Lmax  L0(1 + g(+)):     LðtÞ ¼ 1 + gð +Þ = 1 + gð +Þ et=T

(44a)

that corresponds to a decrease of the frequency of the oscillator: ð +Þ

ωðtÞ ¼ ω0



   1 + gð +Þ et=T = 1 + gð +Þ

(44b)

(+) (+) from ω(0) ¼ ω(+) 0 to ω(!∞)  ωmin ¼ ω0 /(1 + g ). (+) (+) Here g ¼ (Lmax/Lo  1) and g  Lmax/Lo if Lmax > > Lo. The value of T determines the characteristic deformation time (size increase) of the well. Fig. 15 shows the dependence of the correlation coefficient on the time of a monotonic increase of the width of the potential well in the interval Lmax/Lo ¼ 11...104 for different characteristic durations

1.0

L(t)/L0 1–5 6 7

10 8

2–4

6

8 0.4

4 2 0

5

0.8 0.6

6

(A)

|r(t)| 1

0.2

ω0(+) t 0

1.0

20

40

60

80

(B) 0

1–|r(t)|

20 1

8

10–1

40

60

(+)

80 ω 0

t

1–|r(t)|

10–2

7

10–4

10–2

7

6

10–3

10–6

5 4

0

200

400

600

800

6 5 4

ω0(+)t

1–3

(C)

8

ω 0(+) t

1–3

(D) 0

5000

10,000

15,000

FIG. 15 The time dependence of the width of the potential well (A) and the correlation coefficient (B) during the expansion of the well in the interval: g(+) ¼ 10, Lmax/L0 ¼ 11 (B); 100 (C); g(+) ¼ 104, Lmax/L0  104 (D). Charts 1–8 correspond to the values Tω(+) 0 ¼ 0.1, 0.25, 0.5, 1.0, 1.33, 2, 5, 10.

358

Chapter 17 Universal mechanism of LENR in physical and biological systems

(+) T ¼ (101/ω(+) 0 )…(10/ω0 ) changes of this width. Such change of the size Lmax/Lo of the well corre4 sponds to the change of interval ω(+) 0 /ωmin ¼ 11...10 of particle oscillation frequency in the well. From these results, it follows that if the interval Lmax/Lo increases, the amplitude of the correlation coefficient oscillations also increases greatly to the maximum possible value j rjmax ! 1. Narrow dips in the graph of | r(t)| are a result of the rapid interference transitions between the values of r(t) and  r(t) with time increase. With the increase of j r jmax ! 1, the width of these gaps tends to zero. Another important factor of j r(t)jmax increase is the use of the minimum deformation time T of the well. In particular, for a relatively small change of the size of the well at Lmax/Lo ¼ 11 and T ¼ (0.1...1)/ ω(+) 0 , the maximum values of the correlation coefficient j rjmax and the correlation efficiency Gmax ¼ pffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi 2 do not exceed, respectively, j rjmax  0.98 and Gmax  5. If this interval increases to Lmax/ 1= 1  rmax 4 Lo ¼ 10 (it corresponds, for example, to an increase of the width of the microcrack from the “seed” ˚ to Lmax  5...10 μm), we have 1  jr jmax  2 107 and Gmax  1600. value Lo  5...10 A The hypothetical case of even greater change Lmax/Lo ¼ 105 corresponds to a CCS with characteristics 1 j r jmax  109 and Gmax  20, 000, that are close to ideal. We can emphasize another feature of the process of formation of the CCS. The maximum current correlation coefficient j r(t)jmax is provided through a time interval much greater than the value of T, which determines the duration of a significant change in the width of the well. It follows directly from the analysis of the data presented in Fig. 15. In particular, the first maxima of | r(t)| and G(t) correspond (+) (+) to time of CCS formation and are equal to tc  750/ω(+) 0 , 7500/ω0 , 75000/ω0 , respectively. For the appearance of the following maxima of j r(t)jmax and Gmax(t) more time is required. The scenario of LENR optimization examined above, in which the expansion of the potential agrees well with experiments in metal hydrides (in particular, with A. Rossi’s experiments [30]), when the formation of unsteady (rapidly growing) microcracks in the volume of metal, in which hydrogen ions are localized, occurs in the process of hydrogenation. In addition, such a scenario can “work” in natural dynamic systems such as biological cell division, when, for example, atoms or ions of hydrogen are in the space between dividing cells. Similar topological processes occur, for example, in the area of dividing single strand chains during DNA replication [34–37].

CCS formation at limited decrease of a width of parabolic potential well An alternative mode of CCS formation due to the influence on the parameters of the potential well, in which the particle is located, is the reduction of its width. Let us find the solution of the system of Eqs. (18), (19) with a limited decrease in the width of the potential well:     LðtÞ ¼ L0 1 + gðÞ et=T = 1 + gðÞ

(45a)

from L0 to Lmin  L0/(1 + g()), which corresponds to an increase of the frequency: ðÞ

ωðtÞ ¼ ω0

    1 + gðÞ = 1 + gðÞ et=T

(45b)

() of the oscillator from ω(0) ¼ ω() to ωmax  ω() ). 0 0 (1 + g () () Here g ¼ (L0/Lmin  1) and g  L0/Lmin if L0 > > Lmin . The results of calculation of the coefficient g() ¼ 10, 102, 103 for three values, which correspond to similar decreases of the size of the parabolic well, and, accordingly, an increase of the oscillation

Methods of CCS formation in realistic physical, biological, and geological systems

1

1.0

L(t)/L0

0.9

1 r(t)| 2 3 4 0.6

0.8

0.8

0.7 0.6

6

0.5

5

0.4

0.4

4

0.3

3

0.2

0

ω 0(–)t 0.05 0.1 0.15 0.2 0.25 0.3 0.35

0.0

(B)

1–|r(t)|

1

5

ω0(–)t 0

0.2

0.4

0.6

0.8

1–|r(t)| 1

1

4

2 3

10–1

6

0.2

0.1 1 2 0

(A)

359

5

1

2

3

4

10–1 10–2

10

–2

10–3 10–4

10–3

ω t (–) 0

(C)

0

0.05

0.1

0.15

ω 0(–)t

10–5

(D)

0

0.01

0.02

0.03

0.04

FIG. 16 The change in the width of the contracting potential well (A) and the correlation coefficient versus time for: g() ¼ 10, L0/Lmin ¼ 11 (B); g()  L0/Lmin ¼ 102 (C); g()  L0/Lmin  103 (D). Charts 1–6 correspond to the values Tω() 0 ¼ 0.001, 0.005, 0.01, 0.05, 0.1, 0.25.

frequency within this well, as well as different values of the characteristic duration T of the well compression, are shown in Fig. 16. From these results, it follows that the maximum value of the correlation coefficient, as in the case of expanding well, increases with the increase of the compression interval Lmax/Lo and decrease of the compression time T; e.g., at a relatively small compression of the well in the interval L0/Lmin ¼ 11 () and at T ¼ (0.001/ω() 0 )…(0.01/ω0 ) the maximal values of the correlation coefficient and the correpffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi 2  5. lation efficiency coefficient don’t exceed, respectively, j r jmax  0.98 and Gmax ¼ 1= 1  rmax 3 With an increase of the compression interval to L0/Lmin ¼ 10 , for example, by the reducing ˚ , we have 1  jrjmax  105 and of the width of the microcrack in the matrix from 1 μm to 10 A 4 () Gmax  220 at T ¼ 0.001/ω0 and 1  jrjmax  10 , Gmax  70 at T ¼ 0.005/ω() 0 . It should be noted that if the potential well is compressed in this interval, the initial frequency (before the compression of the well) is in L0/Lmin ¼ 103 times smaller than the initial freω0  ω() 0 quency ω0  ω(+) 0 (before the expansion) at a similar expansion of the well in the same interval from ˚ to 1 μm. This circumstance must be taken into account at the comparison of r(t) graphs, which 10 A determine the time dependence of the process of formation of CCS with the increase and decrease

360

Chapter 17 Universal mechanism of LENR in physical and biological systems

of potential well sizes. At larger value of the compression interval Lmax/Lo and with the corresponding shortening of the compression process duration T, the values of jr jmax and Gmax increase as effectively as in the case of the expansion of the well. It should be noted that the mechanism of CCS formation considered here is produced when microcracks are “healed” in a number of materials and during the growth of biological objects (in particular, during the division of DNA, on membrane surfaces, etc.). These processes of CCS formation are also related to the production of LENR and the transmutation of isotopes in growing biological objects [34–37]. In the process of growth in the volume of living systems, such nonstationary microscopic potential wells constantly arise (for example, during cell division, during DNA replication, etc.), where the conditions for the formation of CCS and the prerequisites for nuclear synthesis are fulfilled. These processes are considered in detail in Chapter 12 on biotransmutation.

Formation of CCS at pulse modulation of potential well parameters Another alternative method of CCS excitation is connected with a pulsed change of the frequency of an equivalent harmonic oscillator—rapid deviation (usually an increase) of the frequency from a stationary value, followed by rapid return to this value. In particular, paper [17] considers the features of CCS formation for different structures, durations, and amplitudes of such a change. Fig. 17 shows the dependence of the maximum j r(t)jmax and time-averaged correlation coefficients calculated on the basis of relations of the type (18), (19) on the pulse time width τ of the frequency modulation pulse: 2

ω ¼ ω0 ð1 + f ðtÞÞ, f ðtÞ ¼ geðtt0 Þ

=2τ2

,t0 >> τ

(46)

Direct numerical calculations show that the action of such a Gaussian pulse f(t) leads to a rapid formation of the CCS characterized by periodic oscillations of the current value of the coefficient of correlation (Fig. 17A and C) between limiting values j r(t)jmax at different amplitudes g of this pulse. The similar features (oscillations and the decrease to zero for certain values of τ) characterize the dependence of the correlation coefficient averaged over the period of oscillations: < jr ðtÞj >¼

ðt2 1 |r ðtÞ|dt, ðt2  t1 Þ ¼ 10=ω0 t2  t1

(47)

t1

on the pulse duration (Fig. 17B and D). These results show that oscillations (including drop to zero) of the amplitude values of current j r(t)jmax and averaged correlation coefficients is a general tendency of the dependence of this coefficient on duration τ and amplitude g of the pulsed variation of the oscillator frequency. Analogous oscillations obviously occur when one of these parameters is fixed and another varies. Upon an increase in one of these parameters, the period of oscillations in the dependence of the correlation coefficient on another parameter rapidly decreases, and the values of j r(t)jmax and within each peak of such an oscillating dependence sharply increase, both tending to the same maximal value j r(t)jmax, < | r(t) | >max ! 1, which corresponds to a formally unlimited increase in the correlation efficiency G| r|!1 ! ∞. When amplitude g increases in the interval 5…50, the value of jrjmax increases from jr(t)jmax ¼ 0.9972 (which corresponds to Gg¼5 ¼ 3.4) to j r(t)jmax ¼ 0.9999997 and, accordingly,

361

Methods of CCS formation in realistic physical, biological, and geological systems

|r|max 1.0

|r|max

0.9982 w 0t opt =0.033

0.8

1.0

g = 20

|r| max =0.9999997

0.8

g = 50

w 0t opt =0.015

0.6

0.6 0.4

0.4

0.2

w 0t

(A)

0.0

0.4

0.8

1.2

1.6

2.0

w 0t 0.0

0.2

(C)

1.0

w 0t opt =0.033

g = 20

0.6

0.6

0.4

0.4

w 0t

0.2

0.8

0.99999

0.5

0.8

0.6

0.4

0.9975

0.8

0.2

g = 50 w 0t opt =0.015

0.2

w 0t 0.0

(B)

0.0

0.5

1.0

1.00000 |r(t)|

1.5

(D)

|r(t)|

0.6

0.8

|r|max =0.9999997

0.99999

w 0t =0.033

0.99996

g = 50

0.99998

w 0t =0.015

0.99997

0.99994

0.99996

0.99992

(E)

0.4

1.00000

g = 20

0.99998

0.99990

0.2

w 0(t–t0) 0

10

20

30

0.99995

(F)

w 0(t–t0) 0

10

20

30

FIG. 17 Dependence of the maximum j r(t)jmax(A, C) and time-averaged t (B, D) correlation coefficient on duration 2 2 τ of the frequency modulation pulse f(t) ¼ ge(tt0) /2τ (40) at different amplitudes of this pulse (g ¼ 20 (A, B), 50 (C, D)). The bottom row is a view of the correlation coefficient j r(t)j for those values of g and τ, which correspond to the main (first) maximum of the dependences j r(t)jmax and t versus duration τ: g ¼ 20, τ ¼ 0.033/ω0; g ¼ 50, τ ¼ 0.015/ω0.

362

Chapter 17 Universal mechanism of LENR in physical and biological systems

0.0

0.5

g

0

40 0.5

20

0

1.0

w 0t

FIG. 18 3D graph of the time-averaged correlation coefficient t as a function of the duration τ and amplitude g of a symmetric Gaussian pulse (40) acting on a particle.

Gg¼50 ¼ 1290. It is important to note that the increase of g also leads to a rapid increase of the timeaveraged correlation coefficient . All these features can be seen in the 3D graph of the dependence of < | r(t) | >t on τ and g [17], which is shown in Fig. 18. According to the estimations made above, such a giant increase of correlation efficiency provides an increase of the probability of the tunnel effect at the interaction of particles at low energy from Dr¼0  10500 (at the absence of correlation) to Dr¼0.9975  1035 at g ¼ 10 and to Dr¼0.9999997  0.3 at g ¼ 50. The mechanism of the formation of a CCS under a pulsed action on a particle [11, 13] can be produced, for example, by the shock deformation of the lattice under the action of shock waves, as under the action of a pulsed magnetic field on a system of free charged particles. A typical example of such an external action is an electric discharge in a gas or liquid. The  current  J(t) of the discharge is accom!

panied by the formation of a pulsed azimuthal magnetic field H r , t , in which the motion of the ions corresponds to tunable cyclotron resonance, and the system itself is a complete (formal) analog of the nonstationary harmonic oscillator. The formalism used above for the formation of a CCS in a nonstationary harmonic oscillator can be fully applied to such a system, taking into account the obvious change of the initial frequency ω(t) ¼ | q | H(t)/Mc. The results obtained above can be directly used for this case, if we assume that: ωðtÞ ¼ ω0 ð1 + f ðtÞÞ,ω0 ¼ |q|H0 =Mc, HðtÞ ¼ H0 ð1 + f ðtÞÞ, Hmax ¼ H0 ð1 + gÞ

(48)

Under the action of the pulsed magnetic field, a peculiar “deformation” of this equivalent oscillator and a very effective CCS formation take place. Such a scenario can explain well [13], for example, the

Methods of CCS formation in realistic physical, biological, and geological systems

363

generation of neutrons and other isotopes in air during both electrical discharge and lightning on the base of reactions: d + d ¼ T + p, d + d ¼ He3 + n, C12 + n ¼ 3He4 + n0 , d + d ¼ He4 , C13 + p ¼ N14 ,C12 + d ¼ N14 , N15 + p ¼ O16 ,

(49)

N14 + d ¼ O16 , O18 + p ¼ F19

In particular, the results of experiments on detection of emission at a level of approximately 2200 neutrons/pulse in a nanosecond electric discharge in gaseous deuterium at a low pressure were reported in [38]. Such a regime corresponds to the occurrence of d(d, He3)n reaction in the bulk of deuterium. An even larger number of neutrons (about 6000 neutron/pulse) were detected in the experiments [39] with an electric discharge in air. The authors did not propose a substantiated model of the observed effect. This effect can easily be explained by assuming that it is induced by the formation of the CCS of deuterons and protons contained in air. It should be noted that deuterium is present in air in the form of D2 molecules as well as (in a larger amount) in the composition of water vapor with total concentration nD
1012  1013 cm3, and the electric discharge forms ions of atomic and molecular deuterium. Such particles can stimulate a large number of reactions (49) in air. Analogous effects of self-similar CCS formation can also explain the mechanism of neutron generation in air in a lightning discharge [40, 41] due to the fusion with the participation of deuterium in the water vapor composition. According to our estimations, well-known experiments of R. Mills (J. Mols, J. Lotoski, Y. Lu, Brilliant Light Power [42]) on stimulation of large energy release in an electric discharge in a gaseous medium are also very well explained on the basis of this mechanism. Let us briefly consider the specific physical prerequisites of these effects. The conditions for the realization of maximal values of j rjmax and for g ¼ 20; 50 is presented above in Fig. 16A and C and has the form ω0τ  0.033; 0.015. This condition, taking into account the functional dependence of the optimal duration τ of the pulsed action and maximal frequency ωmax ¼ ω0(1 + g) on ω0 and g, can be written in the form of the universal relation: gω0 τ  ωmax τ  τ|q|Hmax =Mc  0:6  0:7

(50)

A similar ratio corresponds to the calculation results for other parameters: ω0τ  0.112; 0.065 at g ¼ 5; 10 [17]. The reason for such a regularity is clear and is discussed below. It was shown above that the maximal efficiency of CCS formation in a nonstationary harmonic oscillator and the possibility of obtaining large values of quantities j rjmax, and Gmax corresponds to the situation, when frequency ΩM of the periodic variation of parameters of this oscillator (modulation frequency), which is controlled by external action, is equal to the doubled frequency of this oscillator during the CCS formation [11, 12]. This condition ensures the fulfillment of the requirement of optimal phase locking of the wave eigenfunctions of the particle in the potential well. As was shown above (see Fig. 6A), it corresponds to the condition Ωmax ¼ 2ωmax. On the other hand, the Fourier spectrum of the pulse (46) has the form f(Ω) ¼ τg exp(Ω2τ2/2); it pffiffiffi pffiffiffi remains almost unchanged for Ωmax  2=τ and sharply decreases for Ωp max ffiffiffi > 2=τ. Comparison of the last two formulas leads to the relation ωmax τ  1= 2, which completely coincides with expression (48). In other words, the condition for the optimal CCS formation coincides with

364

Chapter 17 Universal mechanism of LENR in physical and biological systems

the requirement of the maximal spectral density of action at the optimal modulation frequency, which leads to synchronization of all fluctuations. This universal condition ωmaxτ  0.6  0.7 applies to all pulsed methods of CCS formation. It shows that there is a single universal mechanism for the formation of CCS, which can be interpreted on the basis of both spectral and temporal descriptions.

The influence of damping and random force on CCS formation The features of the implementation of LENR due to the formation of coherent correlated states described above did not take into account the possible effects of different stochastic processes that can change the optimal phase relations between different eigenstates of the particle. The presence of fluctuations and damping in real physical and biological systems can have a significant effect on the process of CCS formation. This problem was investigated in [9, 13, 17]. The most reasonable method for taking into account the attenuation of a quantum oscillator is the introduction of a thermostat and the use of a density matrix apparatus, which necessitates the use of a large number of longitudinal Tij and transverse τij relaxation times. These values are most often found semiempirically. This method greatly complicates the solution and makes it much less clear if we stay within the framework of a model close to the classical harmonic oscillator. On the other hand, it is well known that in a classical harmonic oscillator, damping can be taken into !

!

account by introducing a phenomenological braking force F d ¼ 2γd q =dt with a single phenomenological coefficient γ. An acceptable alternative to the density matrix method is the simulation of a phenomenological nonstationary quantum-mechanical Hamiltonian, from which an equation of motion can be obtained in the form corresponding to a classical oscillator with damping. This condition corresponds to the Caldirola-Kanai Hamiltonian [43, 44], which takes into account the effect of the external force F(t) and the phenomenological braking force on a particle in the parabolic potential, and has the form: _ _ _ _  p Mω2 ðtÞx 2 2γt _ H x , t ¼ x e2γt + e  FðtÞx e2γt 2M 2 2

(51)

_

In this relation, the canonical (generalized) momentum p x is connected with the “physical” momentum _ _ p(k)x ¼ Mdx/dt by the relation p x ¼ e2γt p ðkÞx . This Hamiltonian _ isHermitian, its eigenvalues are real and the eigenfunctions are bounded and _  normalized. The use H x , t of the form (51) does not violate the canons of quantum mechanics. The validity of the use of such Hamiltonian for the analysis of systems with dissipation at a variable frequency has been discussed_in many papers (in particular, in [9, 13, 17]). _  Based on the Hamiltonian H x , t (51) and_taking into account the general rule for constructing the equation of motion for an arbitrary operator L : _

_

i dL ∂L 1 h__ ¼ + L H ðx, tÞ dt ∂t iħ

(52) _

we can obtain the equation of motion for the coordinate operator x : i 1 hh _ i_ i d 2 x 1 ∂ h__ _  x H ðx, tÞ + 2 x H ðx, tÞ H ðx, tÞ ¼ 0 2 iħ ∂t dt ħ _

(53)

Methods of CCS formation in realistic physical, biological, and geological systems

365

which leads to the dimensionless equation of a classical harmonic oscillator with damping, an arbitrary external force, and the necessary initial conditions:  d2 ε dε dε 2 + 2γ ð t Þε ¼ f ð t Þ, ε ð 0 Þ ¼ 1, ¼ i,ωð0Þ ¼ 1 + ω dt dt 0 dt2

(54)

This equation is an obvious pffiffiffiffiffiffiffiffiffiffiffiffigeneralization of Eq. (32). In Eq. (54) and in the following relations, the function f ðtÞ ¼ FðtÞ= ħMω30 is a dimensionless external (including stochastic) force; γ is the dimensionless attenuation coefficient normalized to ω0. To solve a specific problem of the CCS formation process in the presence of damping, variable frequency, and stochastic effects, we used a more simple method of Eq. (54) analysis, which is connected with its transformation into equations for the corresponding reciprocal and mixed moments of _ _ quantities q and p q (in dimensionless form ε and dε/dt), appearing in (54), and taking into account the correlation characteristics of the functionf(t). A similar method can also be used at the presence of a random perturbation of the variable oscillator frequency ω(t). Let us consider the evolution of a nonstationary oscillator with damping under the action of a random stationary delta-correlated force f(t) with characteristics: < f ðtÞ>f ¼ 0, < f ðt1 Þ f ðt2 Þ>f ¼ 2Sδðt1  t2 Þ

(55)

corresponding to averaging over the production of a random force with the intensity S. An explicit form of the dependence S on the parameters of a low-pressure plasma or gas was obtained in [9–11]: 1 S¼ 2

∞ ð

∞

1 dτ < Δt

Δt=2 ð

f ðtÞf ðt + τÞdt>f  Δt=2

M∗ σn < ðΔvÞ2 >f < |v|>f 2ħω20

(56)

Here, 1/Δt ¼ σn | v | /ω0 is the dimensionless collision frequency of atoms in the medium (in this case, in a gas with a particle concentration n), σ  3.1016 cm2 is the total cross section for elastic scattering of atoms at low energy, M∗ ¼ M/(1 + M/Ma) is the reduced mass at the collision of the particle with another particle of the medium, and Δv is the change of particle velocity in an elastic collision. After introduction of the functions: μ00 ¼ ε∗ ε,μ01 ¼ ε∗

dε dε∗ dε∗ dε ε ¼ μ∗01 , μ11 ¼ ,μ10 ¼ dt dt dt dt

(57)

which includes a combination of dimensionless coordinate ε and mechanical momentum dε/dt of the particle, it is possible to obtain from (54) the system of equations for the mixed mii ¼ < μii > and mutual mi6¼j ¼ < μi6¼j > statistical moments of the same values ε and dε/dt corresponding to the particle. After additional averaging of all components of these equations by the production of the random force f(t), we can obtain the resulting system of equations for the moments mij ¼ < μij >f : dm00 ¼ m01 + m∗01 , dt dm01 ¼ m11  2γm01  ω2 ðtÞm00 , dt   dm11 ¼ 4γm11  ω2 ðtÞ m01 + m∗01 + 2S dt

(58a) (58b) (58c)

366

Chapter 17 Universal mechanism of LENR in physical and biological systems

The solutions of this system satisfy the initial conditions for the moments: m00 ð0Þ ¼ 1,m01 ð0Þ ¼ i, m∗01 ð0Þ ¼ i,m11 ð0Þ ¼ 1

(59)

directly following from the initial conditions (54) for ε and dε/dt. The solution of the system of Eq. (58) and the corresponding correlation coefficient:  pffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi pffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi  r ðtÞ ¼ ðm01 + m10 Þ=2 m00 m11  m01 + m∗01 =2 m00 m11

(60)

can be found for a given law of variation of the oscillator frequency ω(t). Using this coefficient and the wave function of the CCS, it is possible to calculate the fluctuation parameters of a quantum oscillator, pffiffiffiffiffiffiffiffi 2 and, using an approximate relation Dr6¼0  ðDr¼0 Þ 1r , estimate the change in the transparency of the potential barrier. Such analysis was carried out in [13, 17], where it was shown that the presence of such fluctuations (for example, due to the collision of an ion located in the field of a variable harmonic oscillator with extraneous atoms) can significantly complicate the process of CCS formation and reduce the maximum value of the correlation coefficient. Fig. 19 presents one of the many results of the analysis of the action of random force and dephasing fluctuations on the process of CCS formation with periodic modulation of parabolic potential well (at the variable frequency ω(t) ¼ ω0(1 + g cos Ωt)) on the parametric resonance frequency Ω ¼ 2ω0 at the absence and presence of random force. It can be seen that the presence of a random fluctuating force slows down the increase of the correlation coefficient, and in some cases restricts it to a fixed level. At a low intensity S of the random force, all features of both CCS formation and LENR production considered above remain unchanged. With a high intensity of the random force that destroys the phase synchronization of various eigenfunctions of the particle, the process of CCS forming will be significantly limited [9, 14]. 1

1

Dr , < Dr >

10–10

10–24 D r 10–38 10

10–24

Dr < Dr >

10–52

10–66

10–66 10–80

(A)

Dr , < Dr >

10–38

< Dr >

–52

10–10

0

20

40

60

80

t

10–80

(B)

0

50

100

150

200

t

FIG. 19 Dependence of the current (oscillating function Dr) and averaged (monotonic function ) probabilities of the tunnel effect versus duration of the periodic frequency modulation of parabolic potential well in the case of: (A) the absence of a random force and the presence of attenuation with parameters 2γ ¼ g ¼ 0.1; (B) the presence of a random force with intensity S ¼ 0.05 and attenuation with 2γ ¼ g/2 ¼ 0.05. The initial values of Dr¼0 and < Dr¼0 > are equal Dr¼0 ¼ < Dr¼0 > ¼ 1080.

References

367

Conclusions When we examine the problem of LENR production described above, based on the use of coherent correlated states, we can explain, justify, and numerically consider all known LENR paradoxes without applying new radical physical hypotheses, based only on the foundations of modern quantum theory and nuclear physics. It is important to note that a variety of LENR effects for light, medium, and heavy isotopes, observed in completely different media and systems (crystals, amorphous bodies, liquids, gases, low temperature plasma, various living systems, etc.) and under different methods (hydrogenation of metals during electrolysis and thermal exposure, glow discharge, shock waves, electric discharge, natural metabolic processes with concomitant biological phenomena, etc.) are described by a single universal mechanism [45]. Previously, different authors believed that each of the group of effects is characterized by its unique mechanism, not applicable to another group. It is also necessary to note that the acceleration of nuclear reactions by application of CCS could be a significantly more efficient and economical method compared with the acceleration of these reactions at the expense of the use of “brute force” methods, which are traditional for the thermonuclear or pycnonuclear fusion. Another undoubtedly positive aspect of the method of coherent correlated states in application to LENR processes is the ability to predict the expected effects, as well as the possibility of preliminary assessment of the potential suitability and efficiency of new designed or newly used devices, systems, and objects.

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Index Note: Page numbers followed by f indicate figures and t indicate tables.

A

B

Air-flow calorimetry, 98, 115 blower paper cylinder, 117, 117f rubber O-ring, 116–117, 117f wind velocity, 117 blower input vs. airflow velocity, 121–122f air flow rate, 121 air inlet and outlet, 121–122 resistance temperature devices (RTDs), 122 Reynolds number, 120 turbulence, 120 wind velocity distribution, 120–121 blower input vs. air outlet temperature, 123f calibration data, 129, 130f heat applied, 123, 124f heat loss out, 127, 128f heat recovery rate and reactor temperature, 129, 129f logger data, 124, 125t reactor body temperature, 127, 128f wind velocity, 126 insulated box active and control reactors, 115–116, 116f air inlet and outlets, 115–116 resistance temperature devices (RTDs), 115–116 sensor readings, 115–116, 116f measurement and data acquisition data logger, 118, 118t exhaust and gas supply piping, 119, 119f spreadsheet columns, 118, 118f thermal measurements, 119, 120f Alchemy, 205 European alchemical accounts, 257, 257t, 258f Indian alchemical texts, 257–259 silver from silicon, 255 Texas A&M University (TAMU), 256–257, 256t Anaerobic syntrophic association, 218–223, 219f, 222f, 222t Angular quantum number, 306, 315 Anomalous heat effects (AHE), 101, 104, 107–110, 157 Anomalous magnetic momentum (AMM), 319 Anomalous solutions, 302, 305–307 Arata’s double cathode double-structure (DS) cathode, 95, 95–96f light water and heavy water, 96, 96f Asbestos, 101–102 Auger Electron Spectroscopy (AES), 237 Avogadro’s number, 5

Bhabha Atomic Research Center (BARC), 246 Biological transmutations, 205, 233, 246, 254 physical foundation, 225–226 Boltzmann constant, 105–106 Bragg neutron, 294–295 Brown-Ravenhall disease, 285, 314

C CalTech, 4, 13, 63–64 Carbon arc experiments, 247f Atomic Emission Spectroscopy (AES), 246 Bhabha Atomic Research Center (BARC), 246 Perkins Elmer Lambda instrument, 247 results, 247, 248t Texas A&M University (TAMU), 246 ultrapure distilled water, 247 CCM. See Cooperative colliding mechanism (CCM) Cell cooling experiments calorimetric differential equation, 61 differential equation, 62 heat-after-death, 62 initial cell cooling rate, 61 Child-Langmuir law, 106 China Lake, 3–4, 11–12, 64 experiments, 5, 6t Clausius-Clapeyron equations, 64–65 Coefficient of performance (COP), 239–240 Coherent correlated states (CCS), 225, 334 anomalous features and mechanism, 340–341 birth and disappearance of virtual fluctuation, 341, 341f Coulomb potential barrier, 343 Oppenheimer-Phillips reaction, 344 standard Heisenberg uncertainty relation, 343 continuous change of parabolic potential well parameters limited decrease, 358–360, 359f limited increase, 357–358, 357f correlation coefficient, 345–346 damping and random force, 364–366, 366f giant energy fluctuations and barrier transparency, 339f averaged distributions, of probability density, 339–340, 340f

371

372

Index

Coherent correlated states (CCS) (Continued) large fluctuations, 337, 337f periodic modulation, of probability density, 338, 339f physical mechanism, 336 population coefficients, 338 Schr€ odinger-Robertson uncertainty relation, 334–335 periodical modulation of harmonic oscillator parameters, 348f accelerator fusion, low proton energy, 354, 354–356f cooled deuterium, variable magnetic field, 351, 352–353f low-frequency harmonic modulation of potential well, 347, 349f two-beam laser experiment, 349, 350f pulse modulation of potential well parameters, 360–364, 361–362f Cold fusion effect, 265 Coulomb barrier, 271 D-D fusion, 270 experimental studies, 266–268, 267f Gaussian error equation, 269–270 helium production, 270–271 hot fusion process, 268 measured tritium/neutron ratio, 270–271, 271f radiation, 271 Colloidal palladium, 101–102 Condensed matter nuclear reaction (CMNR), 157 Constantan wires, 105, 107–108, 107–108f Continuum dissolution problem, 314 Conventional electric dipole, 285–286 Cooperative colliding mechanism (CCM), 180f, 185–186 Coulomb scattering, 181 energy spectrum of proton, 181, 182f excitation function, 182, 183f Moliere potential and ZBL potential, 181 reaction yield, 181 reduced proton and triton yields, 183, 183–184f Rutherford scattering formula, 181 Coulomb potential, 168–169, 181, 316, 320, 324 anomalous magnetic momentum (AMM), 319 electron deep orbits (EDOs), 302–303 square-integrability, 303 Coulomb wave function, 168–169 CR-39, 25, 25f, 27–28, 31

D Debye model, 172, 176, 185 Deep Dirac Levels (DDLs) anomalous solutions, 305–307 criticisms, 314 discontinuity, 313–314 lack of dependence, 312–313 deep orbits ansatz, 308–309 Kummer’s equation, 307

orthogonality criterion, 309 steps, 307–308 normalized electron probability density (NEPD), 311, 312f orbital mean radii, 309–310 parameters, 311–312 Deformed nuclei, 284 Deuterated thick Pd rod, long-term electrolysis count rate of neutron (CRN), 72–73 electrode interior, 76, 77f electrode surface earthquake, 75 mantle movement, 74 plain terrace appearing slip bands, 73, 75f surface hole mechanism, 73–74, 76f vortex, 76 0.1M LiOD electrode and electric leads, 71 electrolyte and experimental cell, 70–71 experimental, 70, 70f microstructure characterization, 72 working-electrode and counter-electrode configuration, 71–72, 71t postelectrolysis Pd electrode, 73, 74f radial dilation, 72–73, 72f Dewar-type cells, 55 Dielectric barrier discharge (DBD), 108–109 Dipole-dipole interaction, 284 Dirac equation, 313, 319 anomalous solutions, 305–307 square-integrability, 303 Dirac particles, 284–285 Double-structure (DS) cathode, 95, 95–96f Ductile-to-brittle transition hydrogen concentration (DBTC), 82 Duoplasmatron ion source, 169

E EDOs. See Electron deep orbits (EDOs) Electrically induced anomalous thermal phenomena, 110 gas mixtures, 106–107 gas-phase experiments, 103–104 history, 101–102 iron, 105 nickel alloys, 104–105 reactor design and anomalous heat effects (AHE) control alternating current (AC), 108 Constantan wire, 107–108, 107–108f dielectric barrier discharge (DBD), 108–109 reactor configuration, 107–108, 109f thermionic-like behavior, 105–106, 106f Electric dipole coupling, 284 Electrochemistry, 38–39, 97

Index

Electron deep orbits (EDOs), 325–328 anomalous solution, 302 deep Dirac Levels (DDLs), 305–314 Heisenberg uncertainty relation (HUR) coefficient γ, 322 effective potential energy Veff, 322–323 hydrino, 302 low-energy-nuclear reaction (LENR) femto-molecule/molecular ion, 301 hydrogen atom, 301–302 nuclear fusion process, 302 magnetic interactions diamagnetic terms, 319 electron spin, 317–318 nuclear spin, 318 Vigier-Barut (V-B) model, 319–322 special relativity relativistic and nonrelativistic Schr€ odinger equation, 315 term α2 appearing, 316 stability question local energy minimum, 325, 326f potential energy terms, 324 states and possible solutions anomalous solutions, 303 fine-structure constant, 303 Klein-Gordon (K-G) equation, 303 orthogonality criterion, 304 quantum equations, 302–303 relativistic Schr€ odinger equation, 303 wave function, 303 Electron spin resonance (ESR), 286–287 Energetic particles 12 C(n, n’)3α reaction, 27–28, 28f composite cathode, 26 CR-39, 25, 25f, 27–28 energy distribution, of particles, 26–27, 27f linear energy transfer (LET) spectrum analysis, 26–27 Ni screen, 25–26, 25f triple tracks comparison, 27–28, 28f Excess heat generation, fusion reactions air-flow calorimetry, 115–129 direct deposition, 145 material, 145–146, 145–147f results, 146–150, 148t, 149–150f temperature dependence, 151–153, 151–152f hydrogen solubility, 154, 154f plasma deposition, 129–145 Explosion method, 256

373

F Faraday constant, 5 Fine-structure constant, 303 Finite basis Hamiltonians, 285–287 Fleischmann-Pons heat effect (FPHE), 37 highly reproducible excess heat production energetics/ENEA replication cells ETI 35–61, 42 excess energy density vs. maximum loading obtained, 44, 45f excess energy vs. maximum loading obtained, 44, 44f experimental conditions, 46, 47t Fleischmann-Pons replication SRI cells P 12–22, 41 Mode A, 46, 48f Mode B, 46, 49f, 50 Mode C, 46, 49f, 50 principal factors, 46 resistance ratio and derived loading values, 43, 43f resistance ratio and temperature coefficient, 42–43, 42f SRI exploding wire, 42 Tripodi conjecture, 46, 48f progress, 40 anode, 41 bulk-phase Pd metallurgy, 41 electrified metal-electrolyte interface, 41 electrochemical current, 41 electrolyte, 41 questions, 41 variability bulk metallurgy, 40 electrochemical cell, 38, 39f electrochemistry, 38–39 surface structure, 39–40 Foldy-Wouthuysen transformation, 285 FPHE. See Fleischmann-Pons heat effect (FPHE) Fukushima disaster, 157, 191 Fusion reaction, 3–4, 12 Fusion/transmutation, of stable isotopes microbe syntrophin associations, 214f Ba134 isotope, 216, 217f Cs133 isotope, 216, 217f heavy stable isotopes, 215, 216f mass-spectroscopy investigation, 214, 215f, 215t M€ ossbauer isotope Fe57, 213–214 relative efficiency rate, 214 nuclear reactions, light and meddle mass isotopes Bacillus subtilis, 211 Deinococcus radiodurans, 209, 210f E. coli and Saccharomyces cerevisiae T-8, 209, 210f logical premises, 208 Mn55 to Fe57, 209, 209f M€ ossbauer isotope Fe57, 208 nutrient composition, 209, 209t time-of-flight mass-spectrometric analysis, 211, 212f

374

Index

G Gamow energy, 168 Gas phase, 23 deuterium diffusion Biberian, 92–93, 93f Brillouin, 95, 95f Fralick, 91–92, 92f Iwamura, 93–94 Li, 93, 94f Piantelli, 94, 94f experiments, 103–104 hydrogen and deuterium loading Arata’s double cathode, 95–97 Leslie Case catalyst, 98 Mizuno, 98–99, 99f NEDO, 97, 97f Gaussian error equation, 269–270 Geiger-M€ uller (GM) detector, 29 George Ohsawa Steel, 246 Global warming, 157 Greenhouse gases, 157

H Harwell, 3, 63–64 Heat generation experiments, 157 blank run, 159–160 evaluation, 159–160, 161f excess heat generation, 160–161, 162f excess power dependence, 162–163, 163f fabrication process, 158 heat burst, 163 hydrogen gas, 158, 159f input electric power, 159–160, 160f Ni based multilayer thin films, 158, 159f radiation thermometer, 160, 164f released excess energy per hydrogen, 161–162, 162t set-up, 158, 158f thermocouple, 158 Heat-helium correlation, 233–234 Heisenberg uncertainty relation (HUR), 305, 316 coefficient γ, 322 effective potential energy Veff, 322–323 Helium-3 (He-3), 4 Helium-4 (He-4), 4–6, 11–13, 98 background corrections, 10–11, 11t experimental measurement, 7–8, 7t, 11t Helium measurements, 3 first set, 3–5 analysis, 5–6, 6t second set, 8–10, 8t third set, 10–11, 11t Hot Cat, 239, 239f Hot fusion process, 268

Hydrogen electrode characteristics, 84–85, 84t electrolysis conditions, 84–85, 84t Hydrogen embrittlement (HE), 82, 83f Hydrogen solubility, 154, 154f

I Impact method, 256 In situ small punch (SP) testing, 82 International Cold Fusion Conference (ICCF-1), 3–4 Isoperibolic calorimeter CalTech, 63–64 cell cooling experiments calorimetric differential equation, 61 differential equation, 62 heat-after-death, 62 initial cell cooling rate, 61 Clausius-Clapeyron equations, 64–65 cold fusion experiments Dewar calorimeters, 57 D2O electrolytes, 57 excess power, 57 lower bound coefficient, 56 platinum cathode, 57 total cell heat capacity, 56–57 Dewar-type cells, 55 D2O vapor pressure, 64, 65f equations and possible simplifications, 56 Harwell, 63–64 lower bound heat transfer coefficient, 57–58 MIT, 63–64 PG term, 58–59, 64 PW term, 58–59 radiative heat transfer coefficient, 60–61 size and shape, 55 Stefan-Boltzmann constant, 55–56 straight-line method, 59, 60f trade-offs, 55 Isotopic anomalies, 235 Isotopic shifts, 235 Iwamura’s deuterium gas permeation experiments, 241–242

J J-M palladium (J-M Pd) rod, 3

K Klein-Gordon (K-G) equation, 303, 306 Kummer’s equation, 307

L Lamb shift, 325 Laser-induced breakdown spectroscopy (LIBS), 19 Lattice-induced transitions, 284

Index

Leslie Case catalyst, 98, 98f Linear energy transfer (LET) spectrum analysis, 26–27 Lithium chloride, 17 Los Alamos National Laboratory (LANL), 266 Low-energy-nuclear reaction (LENR), 85, 157, 265 coherent correlated states (CCS), 334 anomalous features and mechanism, 340–345 correlation coefficient, 345–346 giant energy fluctuations and barrier transparency, 334–340 periodical modulation of harmonic oscillator parameters, 347–356 Coulomb potential barrier, 333 model, 272–273 problems, 333 radioactive Cs137 isotope and aerobic syntrophic association, 223–225, 224f transmutation reactions (see Transmutation reactions) Lower bound heat transfer coefficient, 57–58

M Magnetic dipole interactions, 285–286 MIT, 4, 13, 63–64 Monovacancy, 296 M€ ossbauer isotope Fe57, 208, 213–214

N Nano-dust fusion transmutation, 249–251, 250f, 250t Nernst equation, 91 Neutron Activation Analysis (NAA), 200, 237 Newton Project, 254–255 Nickel alloys, 104–105 Nonrelativistic Schr€ odinger equation, 315 Nontransparent quartz, 70–71 Normalized electron probability density (NEPD), 311, 312f Nuclear-active environment (NAE), 40, 235 Nuclear magnetic resonance (NMR), 286–287 Nuclear reaction cycle model, 78f benefits, 77 sequential processes, 77 Nucleon-nucleon interaction, 284–285

O Oppenheimer-Phillips reaction, 344 Orthogonality criterion, 309

P Palladium (Pd), 3, 10–11, 91–95 nickel-net reactant, 145, 145f repeated cathodic and anodic electrolysis, 78–79, 81f experimental, 79 macro void formation, 81–82, 81f

375

micro voids and macro voids, 81–82, 81f phases and voids, 79, 80f slip bands in crystal, 81–82, 81f tangled dislocation cell, 81–82, 81f surface features, 102 Palladium chloride, 17 Palladium-deuterium (Pd-D), 3–4, 37, 233–234 Palladium-deuterium co-deposition, 32–33 cell configurations, 17 energetic particles, 25–28 geometries, 17 heat calorimetric measurements, 19–20 cell temperature and cell potential curves, 19–20, 20f cryogenic calorimeter, 22 excess power measurements, 19–20, 20–21f infrared image, 17–19, 19f laser-induced breakdown spectroscopy (LIBS), 19 Ni screen cathode, 17–19 positive feedback effect, 19–20 spiral-wound palladium cathode, 20–21, 21f thermocouples, 17–19 lithium chloride, 17 long incubation times, 17 palladium chloride, 17 researchers, 17, 18t transmutation, 30–32 tritium, 23–24 working electrode surfaces, 17 γ-/X-ray emissions, 28–29, 30f Palladium-hydrogen, 37 Patterson power cell, 236f, 238f measurement techniques, 237 reaction product yield vs. atomic number, 237, 237f thin-film cathodes, 236–237 Pebble bed cathode, 236 Permeation-induced nuclear transmutation reaction, 192f commercial transmutation apparatus, 202–203, 202f detection sensitivity, 200, 200f deuterium permeation, 198 D2 gas, 191–192, 202–203 examples, 198, 198t experimental method and results, 197f control experiments, 193 Cs into Pr, 193, 193f field emission transmission electron microscope (FE-TEM), 193–194, 194f Silicon Drift Detector (SDD), 194–195 150 Sm and 149Sm, 195–198 SPring-8, 194–195, 196f time-of-flight secondary ion mass spectrometry (TOF-SIMS), 194, 195f x-ray photoelectron spectroscopy (XPS), 193 key factors, 200–201, 201f

376

Index

Permeation-induced nuclear transmutation reaction (Continued) replication experiments, 198–199, 199t transmutation apparatus, 191–192, 192f Perturbation theory, 284 Philosophers’ Stone (PS), 257 Phonon-mediated nuclear excitation transfer applications, 288–290 destructive interference effect, 288 deuteron binding energy, 288, 289f Fleischmann-Pons experiment, 287 loss and phase decoherence, 288 nucleon-nucleon potential, 288 second-order perturbation theory, 287–288 single-phonon exchange, 287 Phonon-mediated off-resonant neutron transfer reaction, 294–295 Phonon-nuclear coupling, 283 active sites, 295–296 deformed nuclei, 284–285 dipole-dipole interaction, 284 finite basis Hamiltonians, 285–287 lattice-induced transitions, 284 nuclear effects, 294–295 phonon-mediated nuclear excitation transfer applications, 288–290 destructive interference effect, 288 deuteron binding energy, 288, 289f Fleischmann-Pons experiment, 287 loss and phase decoherence, 288 nucleon-nucleon potential, 288 second-order perturbation theory, 287–288 single-phonon exchange, 287 spin-lattice interaction, 284 subdivision and down-conversion, 293–294 transformed Hamiltonian, 285 up-conversion and down-conversion applications, 293 dimensionless coupling constant, 291–292 scaled indirect coupling matrix element, 291–292, 292f spin-boson model, 291 Plasma deposition, 129–130 activation, 131–133 excess heat example, 143f Arrhenius plot, 143–145, 144f calibration data, 142, 143f input and output power, 142, 142f vs. reactor body temperature, 142, 144f excess heat generation, 135 hydrogen pressure, 136, 136f input power, 136, 136f internal heater temperature and reactor body temperature, 136, 138f O/I ratio, 136, 137f reactor surface temperature, 136, 137f

gas pressure, 139, 140f input time indication, 141, 141f plasma discharge description, 135, 135f process, 134, 134f reactants, 131 reactor cruciform reactor, 131, 133f glow discharge electrodes, 130–131, 132f lid and equipment attached, 130, 131f R-type thermocouple, 130–131 reactor temperature and variation, 138–139, 139f temperature settings, 139–140, 140f Positive feedback effect, 19–20 Positronium, 319–320 Potassium transmutation, 205 Prenuclear period, 205

Q Quantum Rabbit (QR) Labs, 244

R Radiative heat transfer coefficient, 60–61 Radioactive material, 191 Radioactive waste, 157, 217–225 Rasaratnakara, 257–258 Rasa Shastra, 257–258 Rasa Vaidya, 257–258 Relativistic Schr€ odinger equation, 303, 315 Real-time detectors, 29 Renewable energy, 157 Resistance temperature devices (RTDs), 115–116, 122 Resonant nuclear excitation transfer, 287 Reynolds number, 120 Richardson law, 105–106 Rutherford scattering formula, 181

S Saccharomyces cerevisiae T-8, 209, 210f Schr€ odinger-Robertson uncertainty relations, 225, 334–335 Screened Coulomb potential, 169 Screening energy, 167–168 cooperative colliding mechanism (CCM), 180f Coulomb scattering, 181 energy spectrum of proton, 181, 182f excitation function, 182, 183f Moliere potential and ZBL potential, 181 reaction yield, 181 reduced proton and triton yields, 183, 183–184f Rutherford scattering formula, 181 d+d reaction, metals Debye model, 172 deduced values, 172, 173f excitation function, 171, 171f

Index

hydrogen nuclei, 172–173 low-energy deuteron beams, 170–172 screened electrostatic potential, 172 Thomas-Fermi screening, 172 experimental procedure, 169–170, 170f Li+d reaction, solid and liquid metal Li enhancement factor (EF), 174–175 nuclear reaction yield, 174, 175f thick target yield, 174–175, 176–177f Thomas-Fermi screening, 175–176 Wigner-Seitz radius, 174 and nuclear reaction cross section astrophysical S-factor, 168 Coulomb barrier, 168 Coulomb wave function, 168–169 Gamow energy, 168 screened Coulomb potential, 169 Sommerfeld parameter, 168 temperature dependence, of Us, 177–179, 178f, 180f Secondary Ion Mass Spectrometry (SIMS), 235, 237 Silicon Drift Detector (SDD), 194–195 Single-phonon exchange, 287 Smith-Johnson potential, 307 Solid-state nuclear track detector (SSNTD), 25 Spin-boson model, 291 Spin-lattice interaction, 284 SPring-8, 194–195, 196f SSNTD. See Solid-state nuclear track detector (SSNTD) Stefan-Boltzmann constant, 55–56, 159–160 Straight-line method, 59, 60f Strontium, 103 Submerged Carbon Arc, 251 Super abundant vacancies (SAV), 52

T Teflon, 70–71 Texas A&M University (TAMU), 246 Thermal Desorption Analysis (TDA), 83 Thomas-Fermi screening, 172, 175–176 Thorium, 103 Transformed Hamiltonian, 285 Transmutations, 233–235 109 Ag, 31 alchemy, 254–259 Au/Pd cathode, 31, 32f biological transmutations, 254 biophysical aspects, 207–208 carbon arc experiments, 246–249 Edward Esko’s cool fusion, 244–246, 245t, 245f experimental methodology, 235 glow discharge

377

additional elements, 244 apparatus, 242, 243f double-walled quartz vacuum chamber, 242 ICCF 5, 243 ICCF 9, 243 ICCF 12, 243 impulsive periodical power source, 243 Iwamura’s deuterium gas permeation experiments, 241–242 Lugano report and Parkhomov replications coefficient of performance (COP), 239–240 Hot Cat, 239–240, 239f Lithium Aluminum Hydride (LiAlH4), 239–240 secret sauce, 240 microbe syntrophin associations, 213–217 nano-dust fusion transmutation, 249–251 Patterson power cell, 236f, 238f measurement techniques, 237 reaction product yield vs. atomic number, 237, 237f thin-film cathodes, 236–237 109 Pd decay, 31 Pt/Pd electrode, 30, 31f radioactive isotopes and reactor waste, 217–218 long-lived reactor Cs137 isotope, anaerobic syntrophic association, 219–223, 222f, 222t low-energy-nuclear reaction (LENR), 223–225, 224f reactor Ba140 isotope, anaerobic syntrophic association, 218–219, 219f Si and Fe, arc furnace-driven industrial ferrosilicon smelting plant, 251–253 Transmuting Power, 257 Transparent quartz, 70–71 Tritium, 85, 266, 270–271, 273 closed system, 24, 24t measurements, 23–24, 23f open system, 24t results, 24t scintillation technique, 23–24 Tunneling effect probability, 343

V Vigier-Barut (V-B) model anomalous magnetic momentum (AMM), 319 positronium, 319–320 two potential wells, 319–320, 320f

W Weak trap site, 83

X

γ-/X-ray emissions, 28–29, 30f