The Origin of the Chemical Elements

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2 P.K Kuroda The Origin of the Chemical Elements and the Oklo Phenomenon with 24 Figures and 48 Tables Springer-Verlag Berlin Heidelberg New York 1982

3 Prof. Paul K Kuroda, Dept of Chemistry, Chemistry Building, University of Arkansas Fayetteville, AR 72701, USA ISBN-13: DOl: / e-isbn-13: Library of Congress Cataloging in Publication Data. Main entry under title: Kuroda, P.K. (paul K.), The origin of the chemical elements and t;qe Oklo phenomenon. Bibliography: p. Includes index. 1. Chemical elements. 2. Cosmochemistry. 3. Nuclear reactions. I. Title. QD 466.K ISBN-13 : (U.S.) AACR2 This work is subject to copyright. All rights are reserved, whether the whole or part of material is concerned, specifically those of translation, reprinting, re-use of illustrations, broadcasting, reproduction by photocopying machine or similar means, and stomge in data banks. Under 54 of the German Copyright Law where copies are made for other than private use, a fee is payable to ''Verwertungsgesellschaft Wort", Munich. Springer-Verlag Berlin Heidelberg 1982 Softcover reprint of the hardcover 1st edition 1982 The use of registered names, trademarks, etc. in this publication does not imply, even in the absence of a specific statement, that such names are exempt from the relevant protective laws and regulations and therefore free for general use. Composition: Schreibsatz-Service Weihrauch, Wiirzburg 2152/

4 To Professor Kenjiro Kimura

5 Contents Preface XI 1. Introduction Abundance of the Elements Mendeleeff and the Periodic Law The Ideas of Crookes...' Richards and Atomic Weights Clarke's Numbers The Rule of Harkins The 1930 Estimates by Noddack The 1938 Estimates by Goldschmidt Geochemical Classification of the Elements The 1956 Estimates by Suess and Urey Elements 43 and 61 in Nature The All-Present Theory of Noddack Discoveries of Elements 43 and 61 by Artificial Means Magic Numbers Technetium in Stars Long-Lived Isotopes of Technetium Reported Discoveries of Technetium in Terrestrial Minerals Absence of Primordial Technetium in the Earth's Crust Molybdenum-99 in Non-Irradiated Uranium Salts Technetium in Pitchblende Promethium-147 in Non-Irradiated Uranium Salts Promethium in Pitchblende The Oklo Phenomenon Discovery of Spontaneous Fission., Plutonium-239 in Nature Large-Scale Nuclear Processes on the Earth Xenon Isotopes in Radioactive Minerals VII

6 4.5. Radioactive Strontium Isotopes in Pitchblende... " Iodine-129 in Pitchblende Radioactive Iodine Isotopes in Aqueous Uranium Solutions Resonance Capture of Neutrons in Pitchblende The Theory of Natural Reactors The Uranium-238 to -235 Ratio in Nature The Uranium-234 to -238 Ratio in Nature Discovery of the Oklo Reactor Promethium-147 in the Oklo Reactor Plutonium-239 in the Oklo Reactor Technetium-99 in the Oklo Reactor Search for Additional Natural Reactors Synthesis of the Elements in Stars Discovery of Helium in the Sun The Concept of Frozen Thermodynamic Equilibria Deficient Elements The Rate of Thermonuclear Reactions The CoN Cycle and the Proton-Proton Chain Synthesis of the Elements in a Neutron-Rich Environment The Big-Bang Theory of Gamow The Polyneutron Hypothesis of Mayer and Teller The Proton-Neutron Ratio Prior to the Big-Bang Theories on the Evolution of Stars Supernovae and Californium Synthesis of the Elements in Stars The e-process According to B2FH The s- andr-processes According to B2FH Cosmic Black-Body Radiation Pulsars or Neutron Stars The World of Antimatter Possible Climatic Effect of Supernova Explosion Search for Neutrinos from the Sun Temperature of the Sun... " Further Studies on Nucleosynthesis in Stars Plutonium-244 in the Early Solar System Rutherford and Soddy's View on the Transuranium Elements Rutherford's Calculation of the Age of the Elements The Concept of Extinct Radioactivity Half-life ofiodine-129 and the Age of the Elements Excess 129Xe in Meteorites The Plutonium-244 Hypothesis... " Chronology of Nucleosynthesis Plutonium-244 in the Early Solar System Unsolved Problems in Xenology VIII

7 6.10. Search for Superheavy Elements in Nature Superheavy Elementary Particles and Quarks in Nature Isotopic Anomalies in the Early Solar System The Origin of Lithium, Beryllium and Boron Isotopic Anomalies in Meteorites A Unified Theory of Isotopic Anomalies Neon Argon Krypton Xenon Barium Gadolinium Other Elements Appendices Appendix I. Goldschmidt's table of the abundance of the elements (Originally compiled in 1938 and up-dated to 1954) Appendix II. The 1956 Suess-Urey abundance table for the individual nuclei Appendix III. The 1965 abundance table compiled by Virginia Trimble Subject Index IX

8 Preface At about the time I was a student in the 1930's, it had become increasingly evident that all the elements existing on the Earth today had already been discovered. Scientists then began "discovering" new elements by means of their artificial synthesis and some of the man-made elements found important military as well as industrial applications. I have often wondered, however, if the importance of these artificial elements may not have been overly emphasized by contemporary scientists for their practical applications. It seemed to me that these man-made elements were destined to play an important role during the second half of the 20th century in the study of the origin of the elements in the Universe. This subject of study, which dates back to the days of ancient Greek philosophers, may be regarded as the most fundamental in the entire compass of our modetn science. Since I joined the faculty of the University of Arkansas in the early 1950's, I have had the good fortune of being able to maintain a long-range research project, the ultimate goal of which was to elucidate the origin of the elements. I have presented the results from these and related investigations on numerous occasions. While serving as a tour speaker of the American Chemical Society for many years, I have had the privilege of visiting many ofthe local sections to present a lecture on the origin ofthe elements. A Japanese;language version of the talk has been presented at universities and research laboratories throughout Japan. When I was invited to Nagoya University in Japan in the summer of 1977, I was asked by Professor Hideo Yamatera to write a monograph to be published by the Springer Verlag in Germany. The year 1977 happened to be the 100th anniversary of the births of Francis Aston and Frederick Soddy and it appeared to be an appropriate time to undertake such a project. This monograph could not have been written if it were not for the fact that Professor Yamatera was kind enough to provide strong support for the project. It is a real pleasure to express my deep gratitude to him for his encouragement and patience; and to Dr. F. Boschke of the Springer Verlag for his kindness in deciding to publish the manuscript. Special thanks are also due to the U. S. Atomic Energy Commission and the National Science Foundation for the generous support of the writer's research projects at the University of Arkansas; to Dr. Michiaki Furukawa of Nagoya University for reviewing the manuscript; to Dr. James N. Beck of McNeese State University for his assistance; and to Mrs. Marge Bright for her excellent typing work. Fayetteville, Arkansas May 5,1981 P.K. Kuroda

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