Advances in multi-photon processes and spectroscopy

This book presents the latest developments and issues in both experimental and theoretical studies of multi-photon processes and the spectroscopy of atoms, ions and molecules in physics, chemistry, biology and material science. It contains review papers suitable for both active researchers and non-experts who wish to enter the field.Special attention is paid to the recent progress of non-linear photon-matter interactions in atoms, molecules and interfaces: XUV/soft X-ray, high-order harmonic generation in attosecond regime, high-order harmonic generation, sum frequency generation, four-wave mixing spectroscopy and molecular orientation with combined electrostatic and intense, non-resonant laser fields.

Yasuo Nabekawa and Katsumi MidorikawaManfred Lein and Ciprian C. ChirilaHirofumi SakaiMary Jane ShultzJose Luis PazKunihito Hoki and Yuichi Fujimura

Preface	p. v
1 Nonlinear Optics for Characterizing XUV/Soft X-ray High-order Harmonic Fields in Attosecond Regime	p. 1
1 Introduction	p. 1
1.1 Nonlinear phenomena in XUV/soft X-ray region for ultrafast optics	p. 1
1.2 Autocorrelation measurement	p. 3
2 Generation of Intense Harmonic Fields	p. 5
2.1 Single atom response	p. 6
2.2 Propagation of the harmonic fields with pumping laser field: Phase matching	p. 9
2.3 Development of intense high-order harmonic generator	p. 13
3 Two-Photon Double Ionization	p. 20
4 Measurement of Attosecond Pulse Train with Two-Photon ATI	p. 30
5 Interferometric Autocorrelation of APT with Two-Photon Coulomb Explosion	p. 45
5.1 Similarity of APT with mode-locked laser pulses	p. 45
5.2 Why do we need interferometric autocorrelation?	p. 48
5.3 Two-photon Coulomb explosion	p. 49
5.4 Interferometric autocorrelation	p. 52
6 Summary and Prospects	p. 61
Acknowledgements	p. 63
References	p. 64
2 Signatures of Molecular Structure and Dynamics in High-Order Harmonic Generation	p. 69
1 Introduction	p. 69
2 Theory of High-Order Harmonic Generation	p. 73
2.1 Basic theory	p. 73
2.2 Three-step model	p. 76
2.3 The strong-field approximation	p. 79
2.4 Odd and even harmonics	p. 84
3 Influence of Molecular Structure on HHG	p. 86
3.1 Ionization step	p. 86
3.2 Recombination step	p. 89
4 Dynamical Effects	p. 97
5 Conclusions	p. 102
Acknowledgments	p. 103
References	p. 103
3 Molecular Manipulation Techniques and Their Applications	p. 107
1 Introduction	p. 107
2 Theoretical Background	p. 109
3 Molecular Orientation with Combined Electrostatic and Intense, Nonresonant Laser Fields	p. 110
3.1 One-dimensional molecular orientation	p. 110
3.2 Three-dimensional molecular orientation	p. 114
4 Applications with a Sample of Aligned Molecules	p. 118
4.1 Optimal control of multiphoton ionization processes in aligned I[subscript 2] molecules with time-dependent polarization pulses	p. 118
4.2 High-order harmonic generation from aligned molecules	p. 123
5 Summary and Outlook	p. 129
Acknowledgments	p. 130
References	p. 130
4 Sum Frequency Generation: An Introduction with Recent Developments and Current Issues	p. 133
1 Introduction	p. 133
2 Electric Fields and Orientation Factors	p. 136
2.1 Fresnel factors and propagation direction	p. 141
2.2 Orientation factors	p. 144
2.2.1 Simplification of the orientation tensor	p. 146
2.3 Observed intensity	p. 147
2.3.1 Molecular examples	p. 150
3 Recent Developments	p. 151
3.1 Absolute orientation determination with a reference	p. 151
3.2 Orthogonal resonances	p. 154
3.3 Null angle	p. 156
3.3.1 Visible angle null, VAN	p. 158
3.3.2 Polarization angle null, PAN	p. 161
3.3.3 Connection with previous work	p. 164
3.3.4 Example	p. 165
4 Current Issues in Sum Frequency Generation	p. 168
4.1 Interfacial optical constants and bulk contributions	p. 168
4.2 Collective modes - a theoretical challenge	p. 171
4.3 Probe depth	p. 174
4.4 Nanoparticle SFG	p. 176
4.5 Time resolution	p. 177
4.6 Surface 2D imaging	p. 178
5 Selected Results	p. 180
5.1 Ions at aqueous surfaces: The case for surface H[subscript 3]O[superscript +]	p. 180
5.2 Interactions at nanostructured interfaces	p. 184
6 Summary	p. 185
Acknowledgments	p. 189
Appendix A	p. 189
A.1 Tensor product	p. 189
A.2 Null angle	p. 195
References	p. 195
5 Propagation and Intramolecular Coupling Effects in the Four-Wave Mixing Spectroscopy	p. 201
1 Introduction	p. 201
2 Four-Wave Mixing Spectroscopy	p. 206
2.1 Study and characterization of FWM signal in the frequency space	p. 206
2.2 Effects of solute concentration, field intensity, and spectral inhomogeneous broadening on FWM	p. 215
2.2.1 Propagation effects	p. 215
2.2.2 Topological studies for the FWM signal surfaces	p. 218
2.2.3 Spectra in the frequency space	p. 223
2.3 Approximation levels for the study of the propagation in FWM	p. 226
3 Intramolecular Coupling	p. 229
3.1 Molecular models	p. 229
3.2 Theoretical characteristics of the model	p. 231
3.3 Signal response	p. 233
3.4 Results and discussion	p. 236
4 Final Remarks	p. 241
Acknowledgments	p. 242
References	p. 242
6 Control of Molecular Chirality by Lasers	p. 245
1 Introduction	p. 245
2 Fundamental Issues in Laser Control of Molecular Chirality	p. 247
2.1 Laser control of an ensemble of racemic mixtures	p. 247
2.2 Photon polarizations of lasers	p. 248
2.3 Density matrix treatment of a racemic mixture	p. 253
3 Control Scenarios	p. 257
3.1 Pump-dump control via an electronic excited state	p. 258
3.2 Control of molecular chirality in a randomly oriented racemic mixture using three polarization components of electric fields	p. 266
3.3 Stimulated Raman adiabatic passage method	p. 275
3.4 Sequential pump-dump control of chirality transformation competing with photodissociation in an electronic excited state	p. 280
4 Conclusions	p. 287
Acknowledgments	p. 288
References	p. 288

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