Modern nuclear chemistry loveland, morrissey seaborg Modern nuclear chemistry loveland, morrissey seaborg Modern nuclear chemistry loveland, morrissey seaborg Modern nuclear chemistry loveland, morrissey seaborg Modern nuclear chemistry loveland, morrissey seaborg Modern nuclear chemistry loveland, morrissey seaborg Modern nuclear chemistry loveland, morrissey seaborg Modern nuclear chemistry loveland, morrissey seaborg Modern nuclear chemistry loveland, morrissey seaborg Modern nuclear chemistry loveland, morrissey seaborg
MODERN NUCLEAR CHEMISTRY MODERN NUCLEAR CHEMISTRY WALTER D LOVELAND Oregon State University DAVID J MORRISSEY Michigan State University GLENN T SEABORG University of California, Berkeley A JOHN WILEY & SONS, INC., PUBLICATION Copyright # 2006 by John Wiley & Sons, Inc All rights reserved Published by John Wiley & Sons, Inc., Hoboken, New Jersey Published simultaneously in Canada No part of this publication may be reproduced, stored in a retrieval system, or transmitted in any form or by any means, electronic, mechanical, photocopying, recording, scanning, or otherwise, except as permitted under Section 107 or 108 of the 1976 United States Copyright Act, without either the prior written permission of the Publisher, or authorization through payment of the appropriate per-copy fee to the Copyright Clearance Center, Inc., 222 Rosewood Drive, Danvers, MA 01923, (978) 750-8400, fax (978) 750-4470, or on the web at www.copyright.com Requests to the Publisher for permission should be addressed to the Permissions Department, John Wiley & Sons, Inc., 111 River Street, Hoboken, NJ 07030, (201) 748-6011, fax (201) 748-6008, or online at http://www.wiley.com/go/permission Limit of Liability/Disclaimer of Warranty: While the publisher and author have used their best efforts in preparing this book, they make no representations or warranties with respect to the accuracy or completeness of the contents of this book and specifically disclaim any implied warranties of merchantability or fitness for a particular purpose No warranty may be created or extended by sales representatives or written sales materials The advice and strategies contained herein may not be suitable for your situation You should consult with a professional where appropriate Neither the publisher nor author shall be liable for any loss of profit or any other commercial damages, including but not limited to special, incidental, consequential, or other damages For general information on our other products and services or for technical support, please contact our Customer Care Department within the United States at (800) 762-2974, outside the United States at (317) 572-3993 or fax (317) 572-4002 Wiley also publishes its books in a variety of electronic formats Some content that appears in print may not be available in electronic formats For more information about Wiley products, visit our web site at www.wiley.com Library of Congress Cataloging-in-Publication Data Loveland, Walter D Modern nuclear chemistry / Walter D Loveland, David J Morrissey, Glenn T Seaborg p cm Includes bibliographical references and index ISBN-13 978-0-471-11532-8 (cloth: alk paper) ISBN-10 0-471-11532-0 (cloth: alk paper) Nuclear chemistry Textbooks I Morrissey, David J II Seaborg, Glenn Theodore, 1912– III Title QD601.3.L68 2005 5410 38 dc22 2005022036 Printed in the United States of America 10 CONTENTS PREFACE CHAPTER xv INTRODUCTORY CONCEPTS Introduction / The Atom / Atomic Processes / 1.3.1 Ionization / 1.3.2 X-ray Emission / 1.4 The Nucleus Nomenclature / 1.5 Survey of Nuclear Decay Types / 1.6 Modern Physical Concepts Needed in Nuclear Chemistry / 11 1.6.1 Types of Forces in Nature / 11 1.6.2 Elementary Mechanics / 12 1.6.3 Relativistic Mechanics / 13 1.6.4 De Broglie Wavelength, Wave – Particle Duality / 17 1.6.5 Heisenberg Uncertainty Principle / 19 1.6.6 Units and Conversion Factors / 19 1.7 Particle Physics / 20 1.8 Exchange Particles and Force Carriers / 24 Problems / 24 Bibliography / 26 1.1 1.2 1.3 v vi CONTENTS CHAPTER NUCLEAR PROPERTIES 29 Introduction / 30 Nuclear Masses / 30 Terminology / 32 Binding Energy Per Nucleon / 33 Separation Energy Systematics / 35 Abundance Systematics / 36 Semiempirical Mass Equation / 36 Nuclear Sizes and Shapes / 42 Quantum Mechanical Properties / 44 2.9.1 Nuclear Angular Momenta / 44 2.10 Electric and Magnetic Moments / 47 2.10.1 Magnetic Dipole Moment / 47 2.10.2 Electric Quadrupole Moment / 50 Problems / 53 References / 56 Bibliography / 56 2.1 2.2 2.3 2.4 2.5 2.6 2.7 2.8 2.9 CHAPTER RADIOACTIVE DECAY KINETICS 57 3.1 Basic Decay Equations / 58 3.2 Mixture of Two Independently Decaying Radionuclides / 65 3.3 Radioactive Decay Equilibrium / 67 3.4 Branching Decay / 75 3.5 Natural Radioactivity / 77 3.6 Radionuclide Dating / 81 Problems / 87 References / 89 Bibliography / 89 CHAPTER 4.1 4.2 4.3 RADIOTRACERS Introduction / 91 Design of a Radiotracer Experiment / 92 4.2.1 Basic Design Criteria / 92 4.2.2 Practical Considerations / 95 Preparation of Radiotracers and Their Compounds / 97 4.3.1 Chemical Synthesis / 99 4.3.2 Biosynthesis / 100 4.3.3 Tritium Labeling / 100 4.3.4 Radiolysis of Labeled Compounds / 101 91 CONTENTS vii Tracing of Physical Process / 101 Chemical Applications of Tracers / 102 Isotope Effects / 104 Biological Applications / 107 Environmental Applications / 109 Industrial Use of Radiotracers / 113 Nuclear Medicine / 113 Isotope Dilution Analysis / 122 4.11.1 Direct IDA / 122 4.11.2 Inverse IDA / 123 4.11.3 General Comments / 124 4.11.4 Special IDA Techniques / 124 4.12 Radiometric Techniques / 125 Problems / 127 References / 128 Bibliography / 128 4.4 4.5 4.6 4.7 4.8 4.9 4.10 4.11 CHAPTER NUCLEAR FORCES 129 5.1 Introduction / 129 5.2 Characteristics of the Strong Force / 130 5.3 Charge Independence of Nuclear Forces / 132 Problems / 134 Reference / 135 CHAPTER NUCLEAR STRUCTURE 137 6.1 Nuclear Potentials / 139 6.2 Schematic Shell Model / 140 6.3 Independent Particle Model / 152 6.4 Collective Model / 154 6.5 Nilsson Model / 160 6.6 Nucleus as a Fermi Gas / 163 Problems / 171 References / 174 Bibliography / 174 CHAPTER 7.1 7.2 7.3 a DECAY Energetics of a Decay / 179 Theory of a Decay / 183 Hindrance Factors / 192 177 viii CONTENTS 7.4 Heavy Particle Radioactivity / 193 7.5 Proton Radioactivity / 195 Problems / 197 References / 198 Bibliography / 198 CHAPTER b DECAY 199 8.1 Introduction / 199 8.2 Neutrino Hypothesis / 200 8.3 Derivation of Spectral Shape / 203 8.4 Kurie Plots / 207 8.5 b-Decay Rate Constant / 208 8.6 Electron Capture Decay / 213 8.7 Parity Nonconservation / 214 8.8 Neutrinos / 215 8.9 b-Delayed Radioactivities / 216 8.10 Double-b Decay / 217 Problems / 219 References / 220 Bibliography / 220 CHAPTER g-RAY DECAY 221 9.1 Introduction / 221 9.2 Energetics of g Decay / 222 9.3 Classification of Decay Types / 223 9.4 Electromagnetic Transition Rates / 226 9.5 Internal Conversion / 232 9.6 Angular Correlations / 235 9.7 Moăssbauer Effect / 241 Problems / 247 References / 248 Bibliography / 248 CHAPTER 10 10.1 10.2 10.3 10.4 NUCLEAR REACTIONS Introduction / 249 Energetics of Nuclear Reactions / 250 Reaction Types and Mechanisms / 254 Nuclear Reaction Cross Sections / 255 249 INDEX Abnormal data, 574 Absorbed dose, 531 Accelerator mass spectrometry (AMS), 84 Achromatic separation, 419 Actinide contraction, 452 Activation analysis, 366 Activity, 10 Allowed beta decay, 212 Alpha decay equation, 178 recoil, 180 coulomb energy, 182 Gamow factor, 186 hindrance factors, 192 mass parabola, 183 preformation factor, 186, 188 Q-value, 178 tunneling, 184 Alvarez accelerator, 405 Angular momentum beta decay, 200 definition, 12 intrinsic, 46 Anionic extractant, 597 Antineutrino, 202 Areal density, 498 Astrophysical S-factor, 343 Atomic mass unit, 19 Attenuation length, 526 Autoradiography, 107 B(E2), 231, 227 Background radiation, 606 Barium fluoride, 562 Barn (unit), 52 Baryons, 23 Bateman Equations, 74 Becquerel (unit), 63 Beer– Lambert Law, 256, 518 Beta decay angular momentum, 200 equation, 202 Fermi function, 207 Fermi integral, 209 parity, 214 Q-value, 203 selection rules, 211 Beta stability, 40 Bethe – Bloch stopping power, 502 Modern Nuclear Chemistry, by W.D Loveland, D.J Morrissey, and G.T Seaborg Copyright # 2006 John Wiley & Sons, Inc 667 668 INDEX Binding energy Electron Thomas– Fermi, 30, 178 nuclear, 32 Binomial distribution, 567 Bohr independence hypothesis, 272 Bohr magneton, 48 Bohr stopping power, 502 Bohr velocity, 505 Boiling water reactor (BWR), 391, 465 Boson, 20 Bragg counter, 542 Bragg peak, 506 Bragg’s rule, 506 Branching ratio, 76 Breit –Wigner function, 274, 344 Bremsstrahlung, 514, 517 Brennan –Bernstein rules, 146 Cadmium ratio, 370 CAMAC, 565 Carrier, 94 Carrier free, 64, 583 Cationic extractant, 598 Center of mass, 528 Centrifugal potential, 190, 263 Cerenkov radiation, 518, 539 Charge distribution, 45 Charged particle activation analysis (CPAA), 370 Chemical blank, 604 Chernobyl reactor, 394, 457 CNO cycle, 347 Cockcroft – Walton accelerator, 400 Cold fusion, 435 Compound nucleus, 254, 272 Compton edge, 523 Compton scattering, 522 Conversion factors, 613 Coulomb barrier, 261, 397 Coulomb excitation, 280 Critical mass, 423 Critical state, 388 Cross section, 254 Cumulative yield, 321 Curie (unit), 64 Cyclotron, 406 Data rejection, 574 Daughter activity, 68 De Broglie wavelength, 17, 386, 641 Dead time, 545, 548 Decay constant, 58 Decay law, 59 Deep inelastic reaction, 280, 286 Delayed neutrons, 390 Detection limit, 608 Deuterium, characteristics, 131,138 Differential cross section, 256 Diffractive scattering, 268 Direct reaction, 254 DNA analysis, 108 Double beta decay, 41, 217 Effective length, 415 Electric moments, 50 Electrodeposition, 587 Electromagnetic radiation angular correlation, 236 lifetime, 242 multipolarity, 224 selection rules, 225 stretched transition, 224 transition rate, 226 Electron cyclotron resonance (ECR), 398 Electronic stopping, 500, 514 Element synthesis, 434 Energy straggling, 508 Energy width, 63, 76 Entropy, 167 Epithermal neutrons, 370 Euler relation, 640 Evaporation residue, 434, 591 Exchange capacity, 581 Excitation function, 277 Faraday cup, 589 Fermi distribution, 43 energy, 165 function, 207 gas, 163 golden rule, 204 integral, 209 Fermi decay, 201, 204 Fermion, 20 Fission barrier, 170, 304 charge distribution, 318 isomer, 308 mass distribution, 316 TKE, 316 width, 311 Fissionability parameter, 302 Forensic activation analysis, 372 ft value, 209 Fuel cycle, 467 Fundamental constants, 613 INDEX Gamow factor, 186, 343 Gamow peak, 344 Gamow – Teller decay, 201 Gas amplification, 543 Gas flow detector, 546 Gas quenching, 548 Gaseous diffusion, 476 Gaussian distribution, 570 Geiger Muăller detector, 544, 547 Geiger – Nuttall Law, 185 Geochronometer, 83 Germanium detector, 557 Giant dipole resonance, 278 Gray (unit), 532 G-value, 582 Gyromagnetic ratio, 49 Hahn and Strassmann, 299 Half life, 10, 60 Halo nucleus, 44 Heavy cluster emission, 193 Heisenberg Uncertainty Relationship, 19, 63, 129 Hertzsprung – Russell diagram, 340 Hill – Wheeler formula, 306 Hindrance factors, 192 Hydrogen burning, 345 Impact parameter, 12, 259 Independent yield, 320 In-flight separation, 419 Interaction barrier, 264, 282 Interval distribution, 571 Intranuclear cascade, 290 Ion chamber, 540 Ion exchange, 599 Ion pair, 540 Ionization potential, 502 ISOL, 287, 417 Isomeric states, shell model, 149 Isomers, 221 Isospin, 133 Isotope dilution analysis, 122 Isotope effect, 92, 104 Isotopic abundances, 332 Kerma, 532 Kinetic isotope effect, 106 Kurie plot, 207 Lambert – Beers Law, 256, 518 Laplacian, 639 Leptons, 20 Level density, 168, 275 Level width, 273 Linear absorption coefficient, 518 Linear energy transfer (LET), 531 Liquid scintillation, 560 Lorentz force, 407 Lorentz transformations, 12 Low-level counting, 605 Low-level waste, 489 Magnetic moment, 48, 147 Magnetic rigidity, 420 Magnetic sector, 413 Mass equation Myers– Swiatecki, 39 Semi-empirical, 37 Weizsacher, 36 Mass excess, 32 Mass parabola, 183 Mass stopping power, 504 Mean free path, 289, 387 Mean life, 62 Mesons, 23 Mirror nuclei (table), 133 Mirror nuclei, coulomb, 150 Moment of inertia, 156 Monitor reaction, 589 Monopole moment, 51 Mosely, Mossbauer effect, 241 Natural decay chain, 73, 77 Natural radioactivity, 77 Natural reactor, 395 Neptunium, 439 Neutral extractant, 597 Neutrino, 200, 215 detector, 357 oscillation, 359 solar, 355 Neutron activation analysis (NAA), 370 Neutron moderator, 388 Neutron scattering, 528 Nilsson model, 160 Nuclear decay characteristics, equilibria, 70 general, rate, 10 Nuclear density, 7, 43 Nuclear fallout, 80 Nuclear force, 11 Nuclear instrumentation module (NIM), 565 669 670 INDEX Nuclear Nuclear Nuclear Nuclear Nuclear Nuclear Nuclear Nuclear Nuclear Nuclear magneton, 48 mass, 30 potential, 139 radii, 42 reaction Q-value, 251 shapes, 155 skin, 43 surface, 154 temperature, 167 waste, 484 Oklo natural reactor, 395 Optical model, 269 Packing fraction, 32 Pair production, 524 Parity, 47, 214, 655 Penning ion guage (PIG), 398 pep reactions, 345 Photoelectric absorption, 520 Photomultiplier, 562 Pickup reaction, 270 PIN diode, 555 PIXE, 373 Plutonium, 439 Poisson distribution, 569 Positron emission tomography (PET), 117 Potential Energy, Coulomb, 12 pp1 reaction, 346 pp2 reaction, 346 p-process, 353 Preformation factor, 186, 188 Pressurized water reactor (PWR), 391, 465 Primordial nucleosynthesis, 337 Proton activation analysis (PAA), 370 Proton emission, 195 Quadrupole moment, 50 Quarks, 23 Q-value alpha decay, 178 beta decay, 203 equation, 252 nuclear reaction, 31, 251 Rad, 531 Radiation exposure, 531 Radiative stopping, 514 Radioactive decay law, 59 Radiocarbon, 79 Radioimmunoassay, 108 Radiolysis, 101, 493 Radiopharmaceuticals (table), 116 Radiotracer label, 99 Radiotracers (table), 98, 111 Range, 513 Range straggling, 509 Reactor poisons, 390 Relativistic mass, 14 REM (unit), 533 Residual interaction, 153 Resonance, 274 Roentgen (unit), 531 Rotational energy, 155 r-process, 352 rp process, 353 Rutherford backscattering, 376 Rutherford scattering, 265 Saddle point, 300 Saturation activity, 258 Scavengers, 583 Schmidt limit, 148 Scintillation, 559 Scission point, 300 Secular equilibrium, 72 Segre diagram, 36 Selection rules, 225 Semiconductor detector, 549 Semi-empirical mass, 37 Separation energy, 32 Shell model, 141 Sievert (unit), 533 Silicon surface detector, 554 Sodium iodide, 561 Solar abundances, 335 neutrinos, 355 reactions, 346 Spallation, 288 Specific activity, 64 Spent fuel, 479, 484, 488 Spherical coordinates, 649 Spontaneous fission, 306 s-process, 351 Stable nuclides, 36 Standard model, 20 Statistical equilibrium, 169 Stellar populations, 340 Stopping power, 500 Straggling, 508 Stripping reaction, 270 Strong force, 130 Strutinsky method, 305 Subcritical state, 390 Superallowed beta decay, 212 INDEX Supercritical mass, 423 Superdeformed nuclei, 157, 161 Superheavy nuclei, 447 Synchrocyclotron, 410 Synchrotron, 410 Tandem accelerator, 402 Thermonuclear reactions, 342, 424 Three-Mile Island reactor, 394, 457 Threshold energy, 253 Time projection chamber (TPC), 542 Townsend avalanche, 543 Track detectors, 499, 564 Transient equilibrium, 70 Transmutation, 491 Triple alpha reaction, 348 Tunneling, 184, 646 Uncertainties, 573 Uranium enrichment, 475 Uranium metal, 470 671 Van de Graff accelerator, 400 Vibrational motion, 158 Virtual photon, 130 Water dilution volume, 485 Watt energy spectrum, 324, 387 Wave function, 637 Weisskopf transition rate, 227, 229 Weizsacher mass equation, 36 Wheeler angular distribution, 326 Wideroe accelerator, 405 Wilzbach reaction, 94, 101 Woods– Saxon potential, 132, 153, 263 X-ray, Yellowcake, 474 Yrast states, 286 Yucca mountain, 487 Yukawa potential, 132 Zeeman splitting, 236 COLOR PLATES Figure 1.4 Two artist’s conceptions of the standard model (a) From New York Times, 22 September, 1998 Reprinted by permission of the New York Times (b) From “Nuclear Science”, Contemporary Physics Education Project (CPEP), LBNL Figure 2.10 Nuclear density distribution: (a) in a schematic view and (b) in an artist’s conception from R Mackinfosh, J Al-Khalili, B Jonson and T Pena, Nucleus: A Trip to the Heart of Matter Copyright # 2001 by The Johns Hopkins University Press, 2001; reprinted by permission of Johns Hopkins Figure 2.12 Schematic representation of the relative sizes of the halo nucleus 11Li and 208Pb Figure 4.2 Schematic view of DNA fingerprinting Figure 4.6 PET pictures of the heart of a patient with acute myocardial infarction treated with a thrombolytic agent Top row shows scans after administration of water containing 15 O to trace blood flow Bottom row shows tomograms obtained after administration of acetate containing 11C to trace the heart’s metabolism, that is, its rate of oxygen use The defects are clearly visible on day 1, both in the impaired blood flow (top left) and the impaired metabolic use of oxygen (bottom left) Recovery of blood circulation has taken place on day and is maintained 5+ 5.2 yr 60 27 Co Q = 2823.9 4+ 2505.77 1173 99.025% 2+ 1332.52 1332 0.057% stable 2.0x104 yr (6)+ 94 41 Nb Q = 2045.1 4+ 1573.72 2+ 71 98.1% 02 60 28 Ni 0+ 0+ 94 42 Mo 871.10 stable Figure 6.8 (a) Energy level diagram showing the rst (lowest energy) 2ỵ and 4ỵ states in 60 Ni The high-spin ground state, 5ỵ, of 60Co b decays primarily to the 4ỵ state and initiates a well-known g-ray cascade to the 2ỵ state and then the 0ỵ ground state (b) For comparison, the energy level diagram showing the rst (lowest energy) 2ỵ and 4ỵ states in 94Mo The highspin ground state, 6ỵ, of 94Nb also primarily feeds the 4ỵ state initiating a g-ray cascade Figure 7.5 A (reasonably accurate) one-dimensional potential energy diagram for 238U indicating the energy and calculated distances for a decay into 234Th Fermi energy %30 MeV, Coulomb barrier %28 MeV at 9.3 fm, Qa 4.2 MeV, distance of closest approach 62 fm 6+ 4+ (254 W.u.) (358 W.u.) 2+ 0+ 103 ps (1098 W.u.) 2026 ps 160 Figure 9.4 18.6 ps Dy Schematic diagram of the ground-state rotational band transitions for 160 Dy Figure 9.10 Energy level diagram of two members of the A ¼ 57 mass chain 57Co decays À to excited states of 57Fe, which result in the M1 transition from the 32 state at 14.41 keV to the 1À ground state Fission Isomers Fm 100 Es 99 Cf 98 Bk 97 Cm 96 Am 95 Pu 94 Np 93 U 92 Pa 91 Th 90 140 Figure 11.6 152 148 144 Position of the known spontaneously fissioning isomers in the nuclide chart Figure 12.1 Abundances of the first 40 elements as a percentage by mass of Earth’s crust (filled squares) and in the solar system (open circles) Data from the CRC Handbook of Chemistry and Physics, 75th ed., 1994 Fraction of critical density 0.25 0.24 0.23 0.22 He Mass fraction 0.05 0.02 0.01 D –4 Number relative to H 10 10–5 He 10–9 LI 10–10 –31 Baryon density (10 –3 g cm ) Figure 12.6 Variation of the relative abundances of the Big Bang nuclei and the 4He mass fraction versus the baryon density The boxes indicate the measured data and an estimate of the uncertainty The curves indicate the dependence of the yield on the baryon density in the Big Bang; the vertical bar indicates the region of concordence ... Cataloging-in-Publication Data Loveland, Walter D Modern nuclear chemistry / Walter D Loveland, David J Morrissey, Glenn T Seaborg p cm Includes bibliographical references and index ISBN-13 97 8-0 -4 7 1-1 153 2-8 ... references and index ISBN-13 97 8-0 -4 7 1-1 153 2-8 (cloth: alk paper) ISBN-10 0-4 7 1-1 153 2-0 (cloth: alk paper) Nuclear chemistry Textbooks I Morrissey, David J II Seaborg, Glenn Theodore, 1912– III Title... MODERN NUCLEAR CHEMISTRY MODERN NUCLEAR CHEMISTRY WALTER D LOVELAND Oregon State University DAVID J MORRISSEY Michigan State University GLENN T SEABORG University of California,