MODERN NUCLEAR CHEMISTRY WALTER D. LOVELAND Oregon State University DAVID J. MORRISSEY Michigan State University GLENN T. SEABORG University of California, Berkeley O WILEY- INTERSCIENCE A JOHN WILEY & SONS, INC., PUBLICATION
CONTENTS PREFACE xv CHAPTER 1 INTRODUCTORY CONCEPTS 1 1.1 Introduction / 1 1.2 The Atom / 2 1.3 Atomic Processes / 3 1.3.1 Ionization / 3 1.3.2 X-ray Emission / 4 1.4 The Nucleus Nomenclature / 6 1.5 Survey of Nuclear Decay Types / 8 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 v
Vi CONTENTS CHAPTER 2 NUCLEAR PROPERTIES 29 2.1 Introduction / 30 2.2 Nuclear Masses / 30 2.3 Terminology / 32 2.4 Binding Energy Per Nucleon / 33 2.5 Separation Energy Systematics / 35 2.6 Abundance Systematics / 36 2.7 Semiempirical Mass Equation / 36 2.8 Nuclear Sizes and Shapes / 42 2.9 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 CHAPTER 3 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 RADIOTRACERS 91 4.1 Introduction / 91 4.2 Design of a Radiotracer Experiment / 92 4.2.1 Basic Design Criteria / 92 4.2.2 Practical Considerations / 95 4.3 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
CONTENTS Vi I 4.4 Tracing of Physical Process / 101 4.5 Chemical Applications of Tracers / 102 4.6 Isotope Effects / 104 4.7 Biological Applications / 107 4.8 Environmental Applications / 109 4.9 Industrial Use of Radiotracers / 113 4.10 Nuclear Medicine / 113 4.11 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 CHAPTER 5 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 6 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 a DECAY 177 7.1 Energetics of a Decay / 179 7.2 Theory of a Decay / 183 7.3 Hindrance Factors / 192
Viii CONTENTS 7.4 Heavy Particle Radioactivity / 193 7.5 Proton Radioactivity / 195 Problems / 197 References / 198 Bibliography / 198 CHAPTER 8 ß 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 ß-Decay Rate Constant / 208 8.6 Electron Capture Decay / 213 8.7 Parity Nonconservation / 214 8.8 Neutrinos / 215 8.9 ß-Delayed Radioactivities / 216 8.10 Double-ß Decay / 217 Problems / 219 References / 220 Bibliography / 220 CHAPTER 9 y-ray DECAY 221 9.1 Introduction / 221 9.2 Energetics of y 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 Mössbauer Effect / 241 Problems / 247 References / 248 Bibliography / 248 CHAPTER 10 NUCLEAR REACTIONS 249 10.1 Introduction / 249 10.2 Energetics of Nuclear Reactions / 250 10.3 Reaction Types and Mechanisms / 254 10.4 Nuclear Reaction Cross Sections / 255
CONTENTS ix 10.5 Reaction Observables / 264 10.6 Rutherford Scattering / 265 10.7 Elastic (Diffractive) Scattering / 268 10.8 Direct Reactions / 270 10.9 Compound Nucleus Reactions / 272 10.10 Photonuclear Reactions / 278 10.11 Heavy Ion Reactions / 279 10.11.1 Coulomb Excitation / 280 10.11.2 Elastic Scattering / 281 10.11.3 Fusion Reactions / 282 10.11.4 Deep Inelastic Scattering / 286 10.11.5 Incomplete Fusion / 286 10.11.6 Reactions Induced by Radioactive Projectiles / 287 10.12 High-Energy Nuclear Reactions / 288 10.12.1 Spallation/Fragmentation / 288 10.12.2 Multifragmentation / 291 10.12.3 Quark Gluon Plasma / 292 Problems / 293 References / 296 Bibliography / 297 CHAPTER 11 FISSION 299 11.1 Introduction / 299 11.2 Probability of Fission / 302 11.2.1 Liquid Drop Model / 302 11.2.2 Shell Corrections / 304 11.2.3 Spontaneous Fission / 306 11.2.4 Spontaneously Fissioning Isomers / 308 11.2.5 Transition Nucleus / 310 11.3 Fission Product Distributions / 316 11.3.1 Total Kinetic Energy (TKE) Release in Fission / 316 11.3.2 Fission Product Mass Distributions / 316 11.3.3 Fission Product Charge Distributions / 318 11.4 Excitation Energy of the Fission Fragments / 322 11.5 Dynamical Properties of the Fission Fragments / 325 Problems / 329 References / 329
X CONTENTS CHAPTER 12 NUCLEAR REACTIONS IN NATURE: NUCLEAR ASTROPHYSICS 331 12.1 Introduction / 331 12.2 Elemental and Isotopic Abundances / 332 12.3 Primordial Nucleosynthesis / 336 12.4 Stellar Evolution / 338 12.5 Thermonuclear Reaction Rates / 342 12.6 Stellar Nucleosynthesis / 344 12.6.1 Introduction / 344 12.6.2 Hydrogen Burning / 345 12.6.3 Helium Burning / 348 12.6.4 Synthesis of Nuclei with A < 60 / 349 12.6.5 Synthesis of Nuclei with A > 60 / 351 12.7 Solar Neutrino Problem / 354 12.7.1 Introduction / 354 12.7.2 Expected Solar Neutrino Sources, Energies, and Fluxes / 355 12.7.3 Detection of Neutrinos / 357 12.7.4 Solar Neutrino Problem / 359 12.7.5 Solution of the Problem Neutrino Oscillations / 359 12.8 Synthesis of Li, Be, and B / 361 Problems / 362 References / 363 Bibliography / 363 CHAPTER 13 ANALYTICAL APPLICATIONS OF NUCLEAR REACTIONS 365 13.1 Activation Analysis / 366 13.1.1 Basic Description of Method / 366 13.1.2 Advantages and Disadvantages of Activation Analysis / 367 13.1.3 Practical Considerations in Activation Analysis / 368 13.1.4 Applications of Activation Analysis / 372 13.2 Particle-Induced X-ray Emission / 373 13.3 Rutherford Backscattering (RBS) / 376 Problems / 379 References / 380 Bibliography / 380
CONTENTS Xi CHAPTER 14 REACTORS AND ACCELERATORS 383 14.1 Nuclear Reactors / 384 14.1.1 Neutron-Induced Reactions / 384 14.1.2 Neutron-Induced Fission / 387 14.1.3 Neutron Inventory / 388 14.1.4 Light Water Reactors / 390 14.1.5 The Oklo Phenomenon / 395 14.2 Neutron Sources / 395 14.3 Neutron Generators / 396 14.4 Accelerators / 397 14.4.1 Ion Sources / 397 14.4.2 Electrostatic Machines / 399 14.4.3 Linear Accelerators / 403 14.4.4 Cyclotrons, Synchrotrons, and Rings / 406 14.5 Charged Particle Beam Transport and Analysis / 412 14.6 Radioactive Ion Beams / 417 14.7 Nuclear Weapons / 421 Problems / 426 References / 427 Bibliography / 427 CHAPTER 15 THE TRANSURANIUM ELEMENTS 429 15.1 Introduction / 429 15.2 Limits of Stability / 429 15.3 Element Synthesis / 431 15.4 History of Transuranium Element Discovery / 438 15.5 Superheavy Elements / 447 15.6 Chemistry of the Transuranium Elements / 449 15.7 Environmental Chemistry of the Transuranium Elements / 457 Problems / 462 References / 463 Bibliography / 464 CHAPTER 16 NUCLEAR REACTOR CHEMISTRY 465 16.1 Introduction / 465 16.2 Fission Product Chemistry / 466
Xii CONTENTS 16.3 Radiochemistry of Uranium / 470 16.3.1 Uranium Isotopes / 470 16.3.2 Metallic Uranium / 470 16.3.3 Uranium Compounds / 470 16.3.4 Uranium Solution Chemistry / 471 16.4 Nuclear Fuel Cycle The Front End / 472 16.4.1 Mining and Milling / 472 16.4.2 Refining and Chemical Conversion / 475 16.4.3 Enrichment / 475 16.4.4 Fuel Fabrication / 478 16.5 Nuclear Fuel Cycle The Back End / 479 16.5.1 Properties of Spent Fuel / 479 16.5.2 Fuel Reprocessing / 481 16.6 Radioactive Waste Disposal / 483 16.6.1 Classification of Radioactive Waste / 483 16.6.2 Amounts and Associated Hazards / 484 16.6.3 Storage and Disposal of Nuclear Waste / 485 16.7 Chemistry of Operating Reactors / 492 16.7.1 Radiation Chemistry of Coolants / 493 16.7.2 Corrosion / 493 16.7.3 Coolant Activities / 494 Problems / 494 References / 495 Bibliography / 496 CHAPTER 17 INTERACTION OF RADIATION WITH MATTER 497 17.1 Introduction / 497 17.2 Heavy Charged Particles (A > 1) / 499 17.3 Electrons / 514 17.4 Electromagnetic Radiation / 518 17.4.1 Photoelectric Effect / 520 17.4.2 Compton Scattering / 522 17.4.3 Pair Production / 524 17.5 Neutrons / 526 17.6 Radiation Exposure and Dosimetry / 530 Problems / 533 References / 535 Bibliography / 535
CONTENTS Xi i i CHAPTER 18 RADIATION DETECTORS 537 18.1 Detectors Based an Ionization / 540 18.1.1 Gas Ionization Detectors / 540 18.1.2 Semiconductor Detectors (Solid-State Ionization Chambers) / 548 18.2 Scintillation Detectors / 558 18.3 Nuclear Track Detectors / 564 18.4 Nuclear Electronics and Data Collection / 565 18.5 Nuclear Statistics / 567 18.5.1 Rejection of Abnormal Data / 574 18.5.2 Setting Upper Limits When No Counts are Observed / 576 Problems / 576 References / 577 Bibliography / 577 CHAPTER 19 RADIOCHEMICAL TECHNIQUES 579 19.1 Unique Aspects of Radiochemistry / 580 19.2 Availability of Radioactive Material / 584 19.3 Targetry / 584 19.4 Measuring Beam Intensity and Fluxes / 589 19.5 Recoils, Evaporation Residues (EVRs), and Heavy Residues / 591 19.6 Radiochemical Separation Techniques / 595 19.6.1 Precipitation / 595 19.6.2 Solvent Extraction / 596 19.6.3 Ion Exchange / 599 19.6.4 Extraction Chromatography / 602 19.6.5 Rapid Radiochemical Separations / 602 19.7 Low-Level Measurement Techniques / 603 19.7.1 Introduction / 603 19.7.2 Blanks / 604 19.7.3 Low-Level Counting General Principles / 605 19.7.4 Low-Level Counting Details / 605 19.7.5 Limits of Detection / 608 Problems / 609 References / 610 Bibliography / 611
XIV CONTENTS APPENDIX A FUNDAMENTAL CONSTANTS AND CONVERSION FACTORS 613 APPENDIX B NUCLEAR WALLET CARDS 617 APPENDIX C PERIODIC TABLE OF ELEMENTS 639 APPENDIX D LIST OF ELEMENTS 641 APPENDIX E ELEMENTS OF QUANTUM MECHANICS 643 INDEX 665