Molecular reaction dynamics and chemical reactivity:
Saved in:
| Main Authors: | , |
|---|---|
| Format: | Book |
| Language: | English |
| Published: |
New York, NY [u.a.]
Oxford Univ. Press
1987
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| Subjects: | |
| Online Access: | Inhaltsverzeichnis |
| Physical Description: | XII, 535 S. graph. Darst. |
| ISBN: | 0195041399 0195053958 |
Staff View
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| 245 | 1 | 0 | |a Molecular reaction dynamics and chemical reactivity |c Raphael D. Levine ; Richard B. Bernstein |
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Record in the Search Index
| _version_ | 1804115253780283392 |
|---|---|
| adam_text | Molecular Reaction
Dynamics and
Chemical Reactivity
Raphael D Levine
The Hebrew University of Jerusalem
Richard B Bernstein
University of California, Los Angeles
New York Oxford
OXFORD UNIVERSITY PRESS
Contents
1 Understanding molecular collisions 3
1 1 What is molecular dynamics? 3
1 2 An example: Infrared chemiluminescence 4
121 Distribution of products energy states 5
122 From population inversion to chemical lasers 6
1 3 Why molecular dynamics? 6
131 The pragmatic approach 7
132 Disequilibrium 7
133 The purist approach 9
14A simple model of energy partitioning 10
141 The spectator 10
142 Product angular distribution 11
143A quantitative detour 12
144 The reverse reaction 13
145 Lasers in molecular dynamics 14
1 5 The need to know 15
151 The size of molecules 17
152 Angular distribution of elastic and reactive scattering 17
153 Energy and chemical change 18
154 The practice of molecular reaction dynamics 18
155 Energy transfer collisions 19
156 Molecular reaction dynamics 20
Suggested Reading 21
List of Edited Volumes of Relevant Review Literature 21
2 Molecular collisions 26
2 1 Molecular collisions and free-path phenomena 26
211 The concept of molecular size 26
212 Transport phenomena 27
213 Direct determination of the mean free path: A simple scattering
experiment 27
214 The collision cross section 29
215 The collision frequency 30
216 Molecules as rigid spheres 30
viii Contents
217 Realistic intermolecular potentials 32
218 The concept of molecular size 35
2 2 Dynamics of elastic molecular collisions 36
221 Elastic collisions of structureless particles 36
222 The center-of-mass system 37
223 The centrifugal energy 38
224 The impact parameter 39
225 Conservation of angular momentum; relation to impact parameter 41
226 The centrifugal barrier 43
227 The collision cross section 44
2 3 The reaction cross section 46
231 Definition of reaction cross section 47
232 The energy threshold for reaction 48
233 Trarislational energy requirements of chemical reactions 52
2 4 The reaction probability 52
241 The opacity function 52
242 Reaction cross section 53
243A simple opacity function 54
244 The steric factor 55
245 Reactive asymmetry 55
246 The centrifugal barrier to reaction 58
247 Cross sections for reactions without an energy barrier 59
248 Reactions with an energy threshold 59
249A simple model of steric requirements 61
Suggested Reading 64
3 Scattering as a probe of the collision dynamics 67
3 1 Elastic scattering as a probe of the interaction potential 68
311 The angular deflection 68
312 The deflection function 68
313 Angular distribution in the center-of-mass system 70
314 Scattering as a probe of the potential 73
315 From the potential to the deflection function 74
316 The differential cross section 76
317 The quantum mechanical approach to elastic scattering 78
318 The total cross section and the glory effect 83
319 Rainbow scattering as a probe of the potential well 86
3 1 10 Rainbows in inelastic scattering 87
Appendix 3A: Relation between scattering in the center-of-mass and
laboratory systems 91
3 2 Intermolecular potentials from experiment and theory 94
321 Sources of interaction potentials 94
322 Potential curves from beam scattering 95
323 The intermolecular potential 98
324 Long-range intermolecular forces 102
3 3 Angular distribution in direct reactive collisions 104
331 Concept of a direct reactive collision 104
332 Angular distributions for direct reactions 107
333 Optical model approach to direct reactions 109
Contents ix
334 Nonreactive scattering 110
335 Angular distribution for rebound reactions 111
Suggested Reading 113
4 The polyatomic approach to chemical dynamics 117
4 1 Energy and chemical change 117
411 Energy partitioning 117
412 Energy consumption 120
4 2 Three-body potential energy functions and chemical reactions 122
421 Potential energy surfaces 122
422 The reaction path 125
423 Determining the potential energy surface 129
424 Semiempirical potential surfaces 132
425 Qualitative interpretations: The example of the harpoon
mechanism 134
426 The steric factor: Qualitative and quantitative considerations 137
427 The steric effect: Polar map representation 142
428 Unimolecular reaction and collision-induced dissociation 143
4 3 The classical trajectory approach to reaction dynamics 148
431 From the potential surface to the dynamics 148
432 The need for averaging trajectory results 149
433 Energy disposal in exoergic reactions 151
434 Energy requirements for reactions with a barrier 155
435 Dynamics by classical trajectories 157
436 Direct versus compound collisions 160
437 Monte Carlo sampling 162
Appendix 4A: Mass-weighted coordinate systems 165
Appendix 4B: Role of angular momentum 169
Appendix 4C: Kinematic models 172
4 4 From microscopic dynamics to macroscopic kinetics 173
441 State-to-state rate constants 173
442 Sum over final states, average over initial states 175
443 Detailed balance 177
444 The thermal reaction rate constant 179
445 Activation energy and the reactive reactants 181
446 The configuration of no return 182
447 Evaluating the reaction rate 183
448 Activated complex theory for k(T) 187
449 The statistical approximation 191
4 4 10 Compound collisions: Unimolecular versus bimolecular rates 192
4 4 11 Photoselective chemistry 195
Suggested Reading 198
5 The practice of molecular reaction dynamics 207
5 1 The wish and the realization 207
511 Desiderata 207
5 2 Molecules, radiation, and laser interactions 210
521 Chemiluminescence 210
522 Chemical lasers 211
X Contents
523 Laser pump and laser probe experiments 215
524 Photofragmentation spectroscopy 218
525 Lasers as effectors and detectors of chemical change 225
Appendix 5A: Laser-induced fluorescence 229
5 3 Molecular and ion beam scattering 233
531 Crossed molecular beams 233
532 Ion-molecule reactions 236
Appendix 5B: Supersonic beams 243
5 4 The collisional method 247
541 Angular distribution of reaction products 247
542 Scattering in velocity space 248
543 Intensity contour maps: Qualitative aspects of flux-velocity
distributions 253
544 Translational exoergicity and angular distributions 256
5 5 Surprisal 260
551 Measures of selectivity and specificity 260
552 Surprisal analysis of energy disposal 262
553 Surprisal analysis of energy requirements 267
554 The maximum entropy formalism 270
Appendix 5C: The prior distribution - 274
5 6 Quantum dynamics 276
561 Coupled channels 277
562 From the S matrix to the cross section 279
563 The classical path limit 281
564 The sudden approximation for fast collisions 284
565 Wave packets 285
566 Natural collision coordinates 287
567 Statistical dynamics 287
568 Concluding remarks 289
Suggested Reading 289
6 Molecular energy transfer 300
61A macroscopic description of energy transfer 300
611 Equilibrium and disequilibrium 300
612 The relaxation rate equations 301
613 The relaxation time 302
614 Overview of relaxation rates 303
615A hierachy of relaxation times 305
616 Laser-induced fluorescence spectroscopy 305
617 V-V processes in poly atomics 306
618 The COz laser 311
6 2 Simple models of energy transfer 312
621 Two extremes of vibrational energy transfer 312
622 The adiabaticity parameter 314
623 The exponential gap 316
624 Intermolecular potential for vibrational excitation 320
625 Vibrational energy transfer for the Landau-Teller model 322
626 Classical trajectories for the Landau-Teller model 324
627 Rotational energy transfer in the sudden limit 327
Contents xi
6 3 State-to-state inelastic collisions 331
631 State-to-state rate constants 332
632 Molecular beam studies of inelastic collisions 335
633 Angular distribution 337
6 4 Collisions of molecules with surfaces 338
641 Surface scattering 340
642 Inelastic atom-surface collisions 340
643 Experimental studies of molecule-surface scattering 344
6 5 Bimolecular spectroscopy 348
651 The importance of collisions 348
652 Collision-induced light absorption 349
653 Quasi-bound states and predissociation 351
654 Pressure broadening of spectral lines 353
655 Bimolecular emission spectroscopy 356
656 Laser-assisted collision processes 359
6 6 Electronic energy transfer 368
661 Collisions of electronically excited species 368
662 Quenching processes 369
663 The He-Ne laser 371
664 Radiationless transitions 373
665 Curve crossing 375
666 The adiabaticity parameter 376
667 The Landau-Zener transition probability 377
668 Angular distribution in the curve-crossing problem 378
669 Steric effects in collisions of electronically excited reagents 380
6 6 10 Back to chemistry 382
Appendix 6A: Stimulated emission, laser action, and molecular lasers 383
Suggested Reading 387
7 Reaction dynamics and chemical reactivity 396
71A case study of an elementary reaction 396
711 The F + H2 reaction 396
712 Early experiments: In the beginning 3 9 6
713A landmark: Crossed molecular beam study 397
714 Theoretical attacks on the dynamics 398
715 Definitive product state distributions at last! 401
716 Angular distribution of products and the resonances 407
7 2 Collision complexes: Their formation and decay 411
721A union of bimolecular-unimolecular concepts 411
722A simple model of the angular distribution 412
723 Qualitative criteria for complex formation: Structure and stability 417
724 Quantitative considerations: The available energy 421
725 The RRKM unimolecular reaction rate 426
726 Energy disposal and energy consumption in compound collisions 427
7 3 Multiphoton dissociation 429
731 Intramolecular vibrational energy redistribution 430
732 Infrared multiphoton dissociation 432
733 Molecular beam studies 436
xii Contents
734 Multiphoton ionization and fragmentation 440
Appendix 7A: Beyond RRKM/QET 443
7 4 Van der Waals molecules and clusters 444
741 Beams of molecular clusters 446
742 Spectroscopic and structural studies 448
743 Chemical reactivity of clusters 452
744 Reaction dynamics 454
7 5 Molecular dynamics of gas-surface reactions 459
751 Adsorption and desorption 460
752 Dissociative adsorption 463
753 Heterogeneous chemical reactivity 467
754 Dynamics of gas-surface reactions 469
755 Laser-induced processes 473
7 6 Stereospecific dynamics 473
761 Orientation and alignment of reactant molecules 476
762 Orbital control 483
763 Alignment of reaction products 484
764 Repulsive energy release 490
765 Photopolarization 490
7 7 New frontiers 495
771 Understanding chemical reactivity 496
772 Future directions 497
Suggested Reading 502
General Appendix 511
Subject Index 513
Author Index 525
|
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| id | DE-604.BV000802482 |
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| indexdate | 2024-07-09T15:19:41Z |
| institution | BVB |
| isbn | 0195041399 0195053958 |
| language | English |
| oai_aleph_id | oai:aleph.bib-bvb.de:BVB01-000502798 |
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| physical | XII, 535 S. graph. Darst. |
| publishDate | 1987 |
| publishDateSearch | 1987 |
| publishDateSort | 1987 |
| publisher | Oxford Univ. Press |
| record_format | marc |
| spelling | Levine, Raphael D. 1938- Verfasser (DE-588)133914887 aut Molecular reaction dynamics and chemical reactivity Raphael D. Levine ; Richard B. Bernstein New York, NY [u.a.] Oxford Univ. Press 1987 XII, 535 S. graph. Darst. txt rdacontent n rdamedia nc rdacarrier Dynamique moléculaire Réactions chimiques - Mécanismes Chemical reaction, Conditions and laws of Molecular Biology Molecular dynamics Theorie (DE-588)4059787-8 gnd rswk-swf Molekulardynamik (DE-588)4170370-4 gnd rswk-swf Chemische Reaktion (DE-588)4009853-9 gnd rswk-swf Reaktionskinetik (DE-588)4048655-2 gnd rswk-swf Molekülphysik (DE-588)4039979-5 gnd rswk-swf Reaktionsdynamik (DE-588)4301792-7 gnd rswk-swf Reaktionsdynamik (DE-588)4301792-7 s DE-604 Chemische Reaktion (DE-588)4009853-9 s Theorie (DE-588)4059787-8 s Molekülphysik (DE-588)4039979-5 s Reaktionskinetik (DE-588)4048655-2 s Molekulardynamik (DE-588)4170370-4 s 1\p DE-604 Bernstein, Richard B. 1923-1990 Verfasser (DE-588)135778778 aut HEBIS Datenaustausch application/pdf http://bvbr.bib-bvb.de:8991/F?func=service&doc_library=BVB01&local_base=BVB01&doc_number=000502798&sequence=000002&line_number=0001&func_code=DB_RECORDS&service_type=MEDIA Inhaltsverzeichnis 1\p cgwrk 20201028 DE-101 https://d-nb.info/provenance/plan#cgwrk |
| spellingShingle | Levine, Raphael D. 1938- Bernstein, Richard B. 1923-1990 Molecular reaction dynamics and chemical reactivity Dynamique moléculaire Réactions chimiques - Mécanismes Chemical reaction, Conditions and laws of Molecular Biology Molecular dynamics Theorie (DE-588)4059787-8 gnd Molekulardynamik (DE-588)4170370-4 gnd Chemische Reaktion (DE-588)4009853-9 gnd Reaktionskinetik (DE-588)4048655-2 gnd Molekülphysik (DE-588)4039979-5 gnd Reaktionsdynamik (DE-588)4301792-7 gnd |
| subject_GND | (DE-588)4059787-8 (DE-588)4170370-4 (DE-588)4009853-9 (DE-588)4048655-2 (DE-588)4039979-5 (DE-588)4301792-7 |
| title | Molecular reaction dynamics and chemical reactivity |
| title_auth | Molecular reaction dynamics and chemical reactivity |
| title_exact_search | Molecular reaction dynamics and chemical reactivity |
| title_full | Molecular reaction dynamics and chemical reactivity Raphael D. Levine ; Richard B. Bernstein |
| title_fullStr | Molecular reaction dynamics and chemical reactivity Raphael D. Levine ; Richard B. Bernstein |
| title_full_unstemmed | Molecular reaction dynamics and chemical reactivity Raphael D. Levine ; Richard B. Bernstein |
| title_short | Molecular reaction dynamics and chemical reactivity |
| title_sort | molecular reaction dynamics and chemical reactivity |
| topic | Dynamique moléculaire Réactions chimiques - Mécanismes Chemical reaction, Conditions and laws of Molecular Biology Molecular dynamics Theorie (DE-588)4059787-8 gnd Molekulardynamik (DE-588)4170370-4 gnd Chemische Reaktion (DE-588)4009853-9 gnd Reaktionskinetik (DE-588)4048655-2 gnd Molekülphysik (DE-588)4039979-5 gnd Reaktionsdynamik (DE-588)4301792-7 gnd |
| topic_facet | Dynamique moléculaire Réactions chimiques - Mécanismes Chemical reaction, Conditions and laws of Molecular Biology Molecular dynamics Theorie Molekulardynamik Chemische Reaktion Reaktionskinetik Molekülphysik Reaktionsdynamik |
| url | http://bvbr.bib-bvb.de:8991/F?func=service&doc_library=BVB01&local_base=BVB01&doc_number=000502798&sequence=000002&line_number=0001&func_code=DB_RECORDS&service_type=MEDIA |
| work_keys_str_mv | AT levineraphaeld molecularreactiondynamicsandchemicalreactivity AT bernsteinrichardb molecularreactiondynamicsandchemicalreactivity |