Preface to the Second Edition ............................. XIII
Preface to the First Edition ................................ XV
1 Preliminaries of the Interaction of Light with Matter ........ 1
2 Weak-Field Photodissociation ................................. 5
2.1 Photoexcitation of a Molecule with a Pulse of Light ..... 6
2.2 State Preparation During the Pulse ...................... 8
2.3 Photodissociation ...................................... 13
2.3.1 General Formalism ............................... 13
2.3.2 Electronic States ............................... 20
2.3.3 Energy-Resolved Quantities ...................... 21
2 A Appendix: Molecular State Lifetime in Photodissociation ... 22
3 Weak-Field Coherent Control ................................. 25
3.1 Traditional Excitation ................................. 25
3.2 Photodissociation from a Superposition State ........... 26
3.2.1 Bichromatic Control ............................. 28
3.2.2 Energy Averaging and Satellite Contributions .... 31
3.3 The Principle of Coherent Control ...................... 33
3.4 Interference between N-Photon and M-Photon Routes ...... 35
3.4.1 Multiphoton Absorption .......................... 35
3.4.2 One-vs. Three-Photon Interference ............... 39
3.4.3 One- vs. Two-Photon Interference: Symmetry
Breaking ........................................ 50
3.5 Polarization Control of Differential Cross Sections .... 56
3.6 Pump-Dump Control: Few Level Excitation ................ 57
3 A Appendix: Mode-Selective Chemistry ........................ 68
4 Control of Intramolecular Dynamics .......................... 71
4.1 Intramolecular Dynamics ................................ 71
4.1.1 Time Evolution and the Zero-Order Basis ......... 72
4.1.2 Partitioning of the Hilbert Space ............... 73
4.1.3 Initial State Control and Overlapping
Resonances ...................................... 75
5 Optimal Control Theory ...................................... 83
5.1 Pump-Dump Excitation with Many Levels: the Tannor-
Rice Scheme ............................................ 83
5.2 Optimal Control Theory ................................. 89
5.2.1 General Principles of Optimal Control Theory .... 89
6 Decoherence and Its Effects on Control ...................... 95
6.1 Decoherence ............................................ 95
6.1.1 Master Equations ................................ 98
6.2 Sample Computational Results on Decoherence ........... 100
6.2.1 Electronic Decoherence ......................... 100
6.2.2 Vibrational Decoherence in Condensed Phases .... 102
6.2.3 Decoherence: Towards the Classical Limit ....... 106
6.3 Environmental Effects on Control: Some Theorems ....... 109
6.3.1 Environment Can Limit Control .................. 109
6.3.2 Environment Can Enhance Control ................ 112
6.3.3 Environmentally Assisted One-Photon Phase
Control ........................................ 114
6.3.4 Isolated Molecules ............................. 116
6.3.5 Nonisolated Systems ............................ 117
6.4 Decoherence and Control ............................... 119
6.4.1 The Optical Bloch Equation ..................... 120
6.4.2 Countering Collisional Effects ................. 126
6.4.3 Additional Control Studies ..................... 129
6.4.4 State Stability against Decoherence ............ 133
6.4.5 Overlapping Resonances and Decoherence
Control: Qualitative Motivation ................ 135
6.4.6 Control of Dephasing ........................... 139
6.5 Countering Partially Coherent Laser Effects in
Pump-Dump Control ..................................... 142
6.6 Countering CW Laser Jitter ............................ 149
6.6.1 Laser Phase Additivity ......................... 150
6.6.2 Incoherent Interference Control ................ 151
7 Case Studies in Coherent Control ........................... 153
7.1 Two-Photon vs. Two-Photon Control ..................... 153
7.1.1 Experimental Implementation .................... 360
7.2 Control over the Refractive Index ..................... 169
7.2.1 Bichromatic Control ............................ 171
7.3 The Molecular Phase in the Presence of Resonances ..... 176
7.3.1 Theory of Scattering Resonances ................ 378
7.3.2 Three-Photon vs. One-Photon Coherent Control
in the Presence of Resonances .................. 182
7.4 Control of Chaotic Dynamics .......................... 186
8 Coherent Control of Bimolecular Processes .................. 191
8.1 Fixed Energy Scattering: Entangled Initial States ..... 191
8.1.1 Issues in the Preparation of the Scattering
Superposition .................................. 193
8.1.2 Identical Particle Collisions .................. 195
8.1.3 Sample Control Results ......................... 198
8.1.4 Experimental Implementation: Fixed Total
Energy ......................................... 211
8.1.5 Optimal Control of Bimolecular Scattering ...... 212
8.1.6 Sculpted Imploding Waves ....................... 236
8.2 Time Domain: Fast Timed Collisions .................... 237
8.2.1 Nonentangled Wave Packet Superpositions:
Time-Dependent Scattering ...................... 237
8.2.2 Entangled or Wave Packets? ..................... 220
9 The Interaction of Light with Matter: a Closer Look ........ 223
9.1 Classical Electrodynamics of a Pulse of Light ......... 223
9.1.1 The Classical Hamiltonian ...................... 223
9.1.2 The Free Light Field ........................... 226
9.2 The Dynamics of Quantized Particles and Classical
Light Fields .......................................... 228
10 Coherent Control with Quantum Light ........................ 233
10.1 The Quantization of the Electromagnetic Field ......... 233
10.1.1 Light-Matter Interactions ...................... 235
10.2 Quantum Light and Quantum Interference ................ 236
10.2.1 One-Photon vs. Two-Photon Quantum Field
Control ........................................ 238
10.2.2 Pump-Dump Coherent Control ..................... 240
10.3 Quantum Field Control of Entanglement ................. 245
10.4 Control of Entanglement in Quantum Field Chiral
Separation ............................................ 250
11 Coherent Control beyond the Weak-Field Regime: Bound
States and Resonances ...................................... 253
11.1 Adiabatic Population Transfer ......................... 253
11.1.1 Adiabatic States, Trapping, and Adiabatic
Following ...................................... 254
11.1.2 The Multistate Extension of STIRAP ............. 260
11.2 An Analytic Solution of the Nondegenerate Quantum
Control Problem ....................................... 261
11.3 The Degenerate Quantum Control Problem ................ 266
11.4 Adiabatic Encoding and Decoding of Quantum
Information ........................................... 271
11.5 Multistate Piecewise Adiabatic Passage ................ 275
11.5.1 Multistate Piecewise Adiabatic Passage -
Experiments .................................... 280
11.6 Electromagnetically Induced Transparency .............. 290
11.6.1 EIT: a Resonance Perspective ................... 291
11.6.2 EIT as Emerging from the Interference between
Resonances ..................................... 293
11.6.3 Photoabsorption ................................ 301
11.6.4 The Resonance Description of Slowing Down of
Light by EIT ................................... 306
12 Photodissociation Beyond the Weak-Field Regime ............. 315
12.1 One-Photon Dissociation with Laser Pulses ............. 315
12.1.1 Slowly Varying Continuum ....................... 318
12.1.2 Bichromatic Control ............................ 319
12.1.3 Resonance ...................................... 319
12.2 Computational Examples ................................ 325
13 Coherent Control Beyond the Weak-Field Regime: the
Continuum .................................................. 329
13.1 Control over Population Transfer to the Continuum by
Two-Photon Processes .................................. 329
13.1.1 The Adiabatic Approximation for a Final
Continuum Manifold ............................. 330
13.2 Pulsed Incoherent Interference Control ................ 335
13.3 Resonantly Enhanced Photoassociation .................. 345
13.3.1 Theory of Photoassociation of a Coherent Wave
Packet ......................................... 346
13.3.2 Photoassociation by the Consecutive
Application of APC and STIRAP .................. 353
13.3.3 Interference between Different Pathways ........ 357
13.3.4 Experimental Realizations ...................... 359
13.4 Laser Catalysis ....................................... 363
13.4.1 The Coupling of a Bound State to Two Continua
by a Laser Pulse ............................... 364
14 Coherent Control of the Synthesis and Purification of
Chiral Molecules ........................................... 373
14.1 Principles of Electric Dipole Allowed Enantiomeric
Control ............................................... 374
14.2 Symmetry Breaking in the Two-Photon Dissociation of
Pure States ........................................... 376
14.3 Purification of Racemic Mixtures by "Laser
Distillation" ......................................... 381
14.4 Enantiomer Control: Oriented Molecules ................ 395
14.5 Adiabatic Purification of Mixtures of Right-Handed
and Left-Handed Chiral Molecules ...................... 397
14.5.1 Vibrational State Discrimination of Chiral
Molecules ...................................... 399
14.5.2 Spatial Separation of Enantiomers .............. 404
14.5.3 Internal Hamiltonian and Dressed States ........ 405
14.5.4 Laser Configuration ............................ 408
14.5.5 Spatial Separation Using a Cold Molecular
Trap ........................................... 409
14.4 Appendix: Computation of B- A- B' Enantiomer
Selectivity ........................................... 413
15 Strong-Field Coherent Control .............................. 415
15.1 Strong-Field Photodissociation with Continuous Wave
Quantized Fields ...................................... 415
15.1.1 The Coupled-Channels Expansion ................. 419
15.1.2 Number States vs. Classical Light .............. 423
15.2 Strong-Field Photodissociation with Pulsed Quantized
Fields ................................................ 425
15.2.1 Light-Induced Potentials ....................... 426
15.3 Controlled Focusing, Deposition, and Alignment of
Molecules ............................................. 429
15.3.1 Focusing and Deposition ........................ 429
15.3.2 Strong-Field Molecular Alignment ............... 435
16 Coherent Control with Few-Cycle Pulses ..................... 443
16.1 The Carrier Envelope Phase ............................ 443
16.2 Coherent Control and the CEO Frequency Measurement .... 445
16.3 The Recollision Model ................................. 446
16.3.1 Step 1: Tunnel Ionization ...................... 447
16.3.2 Step 2: Classical "Swing" Motion ............... 448
16.3.3 Step 3: Recollision ............................ 448
16.3.4 Step 4: Emission of a Photon ................... 450
16.4 CEP Stabilization and Control ......................... 451
16.4.1 The Attosecond Streak Camera ................... 452
16.5 Coherent Control of Sample Molecular Systems .......... 453
16.5.1 One-Photon vs. Two-Photon Control with Few-
Cycle Pulses ................................... 453
16.5.2 Control of the Generation of High-Harmonics .... 455
16.5.3 Control of Electron Transfer Processes ......... 456
16.5.4 Electron Transfer in Alkali Halides ............ 457
17 Case Studies in Optimal Control ............................ 463
17.1 Creating Excited States ............................... 463
17.1.1 Using Prepared States .......................... 467
17.2 Optimal Control in the Perturbative Domain ............ 468
17.3 Adaptive Feedback Control ............................. 471
17.4 Analysis of Adaptive Feedback Experiments ............. 480
17.4.1 trans-cis Isomerization in 3,3'-Diethyl-2,2'-
thiacyanine Iodide ............................. 480
17.4.2 Controlled Stokes Emission vs. Vibrational
Excitation in Methanol ......................... 486
17.5 Interference and Optimal Control ...................... 487
18 Coherent Control in the Classical Limit .................... 491
18.1 The One-Photon vs. Two-Photon Scenario Revisited ...... 491
18.1.1 Resonant Regime ................................ 491
18.1.2 Off-Resonant Extension ......................... 492
18.1.3 A Three-State Example .......................... 494
18.1.4 Quantum Features ............................... 495
18.2 The Quartic Oscillator ................................ 496
18.3 Control in an Optical Lattice ......................... 499
18.3.1 Equivalence with Dipole Driving ................ 503
18.3.2 Computational Results .......................... 502
Appendix Common Notation Used in the Book (in Order of
Appearance) ................................................... 507
References ................................................. 533
Subject Index .............................................. 537
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