Principles of the quantum control of molecular processes / Moshe Shapiro, Paul Brumer.

Format:

Book

Author/Creator:

Shapiro, Moshe.

Contributor:

Brumer, Paul.

Language:

English

Subjects (All):

Quantum optics.

Coherence (Optics).

Molecular dynamics.

Physical Description:

xiii, 354 pages : illustrations ; 25 cm

Place of Publication:

Hoboken, N.J. : Wiley-Interscience, [2003]

Summary:

The authors are among the cofounders of the field of coherent control. They have published extensively on this and related subjects in chemical physics, and have received numerous awards and worldwide recognition for their research contributions.

Contents:

1 Preliminaries of the Interaction of Light with Matter 1

1.1 Classical Electrodynamics of a Pulse of Light 1

1.1.1 Classical Hamiltonian 1

1.1.2 Free Light Field 4

1.2 Dynamics of Quantized Particles and Classical Light Fields 8

2 Weak-Field Photodissociation 11

2.1 Photoexcitation of a Molecule with a Pulse of Light 12

2.2 State Preparation During the Pulse 14

2.3 Photodissociation 19

2.3.1 General Formalism 19

2.3.2 Electronic States 27

2.3.3 Energy-Resolved Quantities 28

Appendix 2A Molecular State Lifetime in Photodissociation 29

3 Weak-Field Coherent Control 32

3.1 Photodissociation from a Superposition State 33

3.1.1 Bichromatic Control 36

3.1.2 Energy Averaging and Satellite Contributions 39

3.2 Principle of Coherent Control 41

3.3 Interference between N-Photon and M-Photon Routes 42

3.3.1 Multiphoton Absorption 42

3.3.2 One- vs. Three-Photon Interference 47

3.3.3 One- vs. Two-Photon Interference: Symmetry Breaking 57

3.4 Polarization Control of Differential Cross Sections 64

3.5 Pump-Dump Control: Few-Level Excitation 65

Appendix 3A Mode-Selective Chemistry 77

4 Optimal Control Theory 80

4.1 Pump-Dump Excitation with Many Levels: Tannor-Rice Scheme 80

4.2 Optimal Control Theory 86

4.2.1 General Principles of Optimal Control Theory 87

5 Decoherence and Loss of Control 92

5.1.1 Sample Computational Results on Decoherence 94

5.2 Coherent Control in Equilibrated Condensed Phases 97

5.2.1 Optical Bloch Equation 97

5.2.2 Countering Collisional Effects 99

5.3 Countering Partially Coherent Laser Effects in Pump-Dump Control 106

5.4 Countering cw Laser Jitter 114

5.4.1 Laser Phase Additivity 114

5.4.2 Incoherent Interference Control 114

6 Case Studies in Coherent Control 117

6.1 Two-Photon vs. Two-Photon Control 117

6.2 Control over the Refractive Index 126

6.2.1 Bichromatic Control 128

6.3 Molecular Phase in Presence of Resonances 133

6.3.1 Theory of Scattering Resonances 135

6.3.2 Three-Photon vs. One-Photon Coherent Control in Presence of Resonances 138

6.4 Control of Chaotic Dynamics 144

7 Coherent Control of Bimolecular Processes 149

7.1 Issues in Preparation of Scattering Superposition 151

7.2 Identical Particle Collisions 154

7.3 m Superpositions 157

7.3.1 Optimal Control of Bimolecular Scattering 161

7.3.2 Sculpted Imploding Waves 165

8 Coherent Control of Synthesis and Purification of Chiral Molecules 167

8.1 Principles of Electric-Dipole-Allowed Enantiomeric Control 168

8.2 Symmetry Breaking in Two-Photon Dissociation of Pure States 171

8.3 Purification of Racemic Mixtures by "Laser Distillation" 175

8.4 Enantiomer Control: Oriented Molecules 190

Appendix 8A Computation of B-A-B' Enantiomer Selectivity 192

9 Coherent Control Beyond the Weak-Field Regime: Bound States and Resonances 195

9.1 Adiabatic Population Transfer 195

9.1.1 Adiabatic States, Trapping, and Adiabatic Following 196

9.1.2 Electromagnetically Induced Transparency 203

9.1.3 EIT: A Resonance Perspective 204

9.1.4 Lasing without Inversion 214

9.2 Analytic Solution of Nondegenerate Quantum Control Problem 215

10 Photodissociation Beyond the Weak-Field Regime 219

10.1 One-Photon Dissociation with Laser Pulses 219

10.1.1 Slowly Varying Continuum 222

10.1.2 Bichromatic Control 223

10.1.3 Resonance 224

10.2 Computational Examples 230

11 Coherent Control Beyond the Weak-Field Regime: The Continuum 233

11.1 Control over Population Transfer to Continuum by Two-Photon Processes 233

11.1.1 Adiabatic Approximation for Final Continuum Manifold 235

11.2 Pulsed Incoherent Interference Control 237

11.3 Resonantly Enhanced Two-Photon Association 249

11.3.1 Theory of Photoassociation of Coherent Wave Packet 250

11.4 Laser Catalysis 258

11.4.1 Coupling of Bound State to Two Continua by Laser Pulse 259

12 Strong-Field Coherent Control 267

12.1 Quantization of the Electromagnetic Field 267

12.2 Light-Matter Interaction 269

12.3 Strong-Field Photodissociation with Continuous-Wave Quantized Fields 270

12.3.1 The Coupled-Channels Expansion 275

12.4 Quantized Fields: Pulses 279

12.4.1 Light-Induced Potentials 281

12.5 Controlled Focusing, Deposition, and Alignment of Molecules 283

12.5.1 Focusing and Deposition 283

12.5.2 Strong-Field Alignment 292

13 Case Studies in Optimal Control 299

13.1 Creating Excited States 299

13.1.1 Using Prepared States 303

13.2 Optimal Control in Perturbative Domain 304

13.3 Adaptive Feedback Control 308

13.4 Interference and Optimal Control 316.

Notes:

Includes bibliographical references (pages 322-338) and indexes.

ISBN:

0471241849

OCLC:

50479371