CONTRIBUTORS TO VOLUME I JOHN M. ALEXANDER JACK M. HOLLANDER J. HUDIS T. D. NEWTON NORBERT T. PORILE K. S. TOTH A. ZUCKER NUCLEAR CHEMISTRY Edited hyL. Y AFFE DEPARTMENT OF CHEMISTRY MC GILL UNIVERSITY MONTREAL, QUEBEC, CANADA Volume I ACADEMIC PRESS New York and London 1968 COPYRIGHT © 1968, BY ACADEMIC PRESS INC. ALL RIGHTS RESERVED. NO PART OF THIS BOOK MAY BE REPRODUCED IN ANY FORM, BY PHOTOSTAT, MICROFILM, OR ANY OTHER MEANS, WITHOUT WRITTEN PERMISSION FROM THE PUBLISHERS ACADEMIC PRESS INC. Ill Fifth Avenue, New York, New York 10003 United Kingdom Edition published by ACADEMIC PRESS INC. (LONDON) LTD. Berkeley Square House, London W.l LIBRARY OF CONGRESS CATALOG CARD NUMBER : 67 22783 PRINTED IN THE UNITED STATES OF AMERICA LIST OF CONTRIBUTORS Numbers in parentheses indicate the pages on which the authors contributions begin. JOHN M. ALEXANDER (273), Department of Chemistry, State University of New York at Stony Brook, Stony Brook, New York JACK M. HOLLANDER (359), Lawrence Radiation Laboratory, University of California, Berkeley, California J. HUDIS (169), Chemistry Department, Brookhaven National Laboratory, Upton, Long Island, New York T. D. NEWTON (1), Atomic Energy of Canada Limited, Chalk River Nuclear Laboratories, Chalk River, Ontario, Canada NORBERT T. PORILE (57), Department of Chemistry, Purdue University, Lafayette, Indiana K. S. TOTH (409), Oak Ridge National Laboratory, Oak Ridge, Tennessee A. ZUCKER (409), Oak Ridge National Laboratory, Oak Ridge, Tennessee PREFACE The aim of these volumes is to bring to interested readers areas of topical interest in nuclear chemistry, written by experts who are actively engaged in working in these fields. The concept differs from the sequential and historical approach found in several very good nuclear chemistry texts. The material found in these chapters should be useful to research workers and graduate students and should serve as a focus of interest for those whose areas interact with nuclear chemistry. In general, each chapter is meant to be self-sufficient and referral to other chapters, while obviously unavoidable, has been kept to a minimum. Con versely application of the above principles has meant that a small unavoidable amount of repetition has been found necessary. The difference in approach used by the authors of the chapters has even made, it seems to the editor, this small amount of duplication useful. Montreal, Quebec L. YAFFE November, 1967 CONTENTS OF VOLUME II 7. NUCLEAR FISSION, J. E. Gindler and J. R. Huizenga 8. THE CHEMICAL EFFECTS OF NUCLEAR TRANSFORMATIONS, A. G. Maddock and R. Wolfgang 9. MODERN RAPID RADIOCHEMICAL SEPARATIONS, Saadia Amiel 10. ELECTROMAGNETIC SEPARATOR AND ASSOCIATED TECH NIQUES, F. Brown 11. COMPUTERS APPLIED TO NUCLEAR CHEMISTRY, David L. Morrison 12. GEO- AND COSMOCHEMISTRY, Oliver A. Schaeffer Author Index—Subject Index XI Chapter i NUCLEAR MODELS T. D. NEWTON1 Atomic Energy of Canada Limited Chalk River Nuclear Laboratories Chalk River, Ontario, Canada I. Simple Properties of Nuclei 1 II. Why Use Nuclear Models? 4 III. Relations between Nuclear Models 5 IV. The Wigner Method 7 V. The Nuclear Shell Model 13 VI. The Unified Model 25 Appendix : Transformations of Collective Coordinates 35 VII. The Optical Model and the Statistical Method 42 References 53 I. Simple Properties of Nuclei In the Rutherford-Bohr model of an atom the nucleus was simply a particle containing most of the atomic mass and having a positive charge equal to the atomic number. This simple concept was used successfully to describe the early data on scattering of a-particles by nuclei. The scattering results implied that the volume of a nucleus was proportional to its mass. After the discovery of the neutron a nucleus was pictured as a spherical collection of neutrons and protons with a radius R = r A1/3, where r is a constant length and A is 0 0 the nuclear mass number. This no longer suffices. 1 Present address: Department of Mathematics and Statistics, University of Guelph, Guelph, Ontario, Canada. 1 2 T. D. NEWTON Scattering of high-energy electrons has provided us with detailed informa tion about the distribution of charge in a nucleus (Ehrenberg et al, 1959; Meyer-Berkhout et al, 1959; Hofstadter, 1963). If we assume that the ratio of neutron to proton densities is the same throughout a nucleus then we can determine the mass distribution from the charge distribution. It appears that for all nuclei larger than 6Li the central density has the same value; one which implies that the centers of nucléons are, on the average, (1.08 ± 0.01)10~13 cm apart. There is a surface region in which the density decreases from the central value to zero. The "surface thickness" is usually specified to be the radial distance in which the density decreases from 90 to 10% of the central value. The surface thickness is about 2 x 10"13 cm. In a nucleus lighter than carbon the density decreases more or less smoothly from the central maximum value to zero. In heavier nuclei, beginning al ready with oxygen, the uniform central density extends over a significant volume. If one computes a root mean square (rms) radius for these systems one finds that R JA1/3 is not constant but decreases with A, changing rapidly for rm A < 16. On the other hand if one defines the nuclear size by the radius R(£) at which the density reaches \ the central value then R{\)jA113 increases with A, again rapidly for A < 16 (see Fig. 1). This merely reflects the fact that a greater fraction of the mass of a light nucleus lies in the region R > R{\). The final break with the simple picture of the nucleus occurred when we found that the nucleus was not spherical. The angular dependence of electron scattering from nB and 14N indicates that these nuclei have nonspherical shapes (Meyer-Berkhout et al, 1959). The deformation of nuclei has been demonstrated in many ways, most commonly by the occurrence of rotational bands in the energy level spectra. To summarize, we now have a picture of an assemblage of nucléons, usually not spherical, containing a central region in which the nucléons are so closely spaced that their charge distributions overlap and a surface region in which this density falls gradually to zero. This description arises almost directly from observation. Some mathematics is needed to interpret the electron scattering results but no theory of the nucleus need be involved. Another set of simple nuclear properties can be deduced from the masses of nuclei in their ground states. The Bethe-Weizsacher formula expresses the nuclear binding energy E as a simple sum of terms representing the volume, B surface, Coulomb, and symmetry energies E = -aA + a A2/3 + a Z(Z - 1)/T1/3 + 0.25a (N - Z)2A~l. (1) B x 2 3 4 Green and Engler (1953) obtained a = 16 MeV, a = 18 MeV, a = 100 MeV, x 2 4 and the fit was good enough to predict at so early a date that in the radius 1. NUCLEAR MODELS 3 formula R = r A1/3, one required r less than the then fashionable value 0 0 1.4 x 10~13 cm (cf. value 1.08 from electron experiments). The data from ground states of nuclei, as summarized in (1) must be kept in mind during all nuclear calculations. For example, for a long time shell model calculations were unable to predict reasonable binding energies. Also formula 1.8 -1/3 A R 1/3 Fig. 1. The equivalent uniform nuclear radius R= [5<r2>/3]1/2 and the radius R. at 05 which the nuclear density is half the central value, each divided by Al/2, are shown as functions of Al/3. Some of the errors of estimation are shown. 4 T. D. NEWTON (1) is frequently corrected by a term representing the odd-even mass difference. This was the first, and very strong, evidence for the effect of short-range correlations now frequently represented in nuclear theory by the "pairing force." Departures from the Bethe-Weizsacher formula show the effects of nuclear shells and of nuclear deformations. In order to study collections of nucléons without these perturbing effects, the concept of nuclear matter, i.e., an extended medium supposed to have the properties of matter in the central regions of nuclei, has been extensively discussed. These discussions test whether or not various assumed inter nucleon forces (including those which fit the two-body data) provide a (volume) binding energy of 16 MeV at a density corresponding to r = 1.08 0 l(T13cm. These calculations have been quite successful, and will undoubtedly con tinue until our understanding of internucleon forces and our methods of calculating with them are considerably improved. So far, however, the methods used for nuclear matter have had only limited success for finite nuclei, so they cannot yet be said to supply a theory of nuclei. II. Why Use Nuclear Models? Experiment has shown what the nucleus looks like and experiment also tells us quite precisely how pairs of nucléons interact, at least in those energy regions of interest for the purposes of this chapter, i.e., from the bound state of the deuteron to, say, 200 MeV. While our knowledge of the interaction between two nucléons is not yet complete it is established that the data below 200 MeV can be quite adequately represented by a potential function (Signell and Marshak, 1958; Gammell and Thaler, 1957; Hamada and Johnston, 1962). The potential is complicated, but can be used. We believe that for energies of interest for problems of nuclear structure the equations of ordinary nonrelativistic quantum theory should be valid. Despite all the information available this chapter is called "Nuclear Models" and not "Theory of Nuclear Structure." Why do we continue to use models? The answer is, most simply, that the problem is too hard. All of our theories avoid the difficulty of a complete solution of the nuclear structure problem by one means or another. In most cases one makes a set of simplifying assumptions which defines a model; i.e., an imaginary object which is not a nucleus, but which we hope may display properties of interest which are the same as those of a nucleus. We seek to avoid the situation that every calcula tion uses a different model. One fundamental difficulty is that a complex nucleus may not be describ- able as an assemblage of neutrons and protons, at least if a nucléon is defined