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Mukamel S. — Principles of Nonlinear Optical Spectroscopy
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Название: Principles of Nonlinear Optical Spectroscopy
Автор: Mukamel S.
Аннотация: This textbook presents a systematic and unifying viewpoint for a wide class of nonlinear spectroscopic techniques in time domain and frequency domain. It is directed towards active researchers in physics, optics, chemistry, and materials science, as well as graduate students who enter this complex and rapidly developing field.
Nonlinear optical interactions of laser fields with matter provide powerful spectroscopic tools for the understanding of microscopic interactions and dynamic processes. One of the major obstacles facing researchers in this field, however, is the flood of experimental techniques and terminologies, which create a serious language barrier. The general microscopic correlation function approach to the nonlinear optical response developed in this book is essential for understanding the relationships among different techniques and a comparison of their information content, the design of new measurements, and for a systematic comparison of the optical response of different systems such as dyes in solutions, atoms and molecules in the gas phase, liquids, molecular aggregates and superlatives, and semiconductor nanostructures. The approach is based on formulating the nonlinear response by representing the state of matter by the density matrix and following its evolution on Liouville space. Current active research areas such as femtosecond time-domain techniques, semi-classical and wave-packet dynamics, pulse shaping, pulse locking, exciton confinement, and the interplay of electronic, nuclear and field coherence are emphasized.
The material has been developed from the author's highly successful interdisciplinary course at the University of Rochester attended byscience and engineering graduate students.
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Рубрика: Физика /
Статус предметного указателя: Готов указатель с номерами страниц
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Год издания: 1995
Количество страниц: 576
Добавлена в каталог: 20.03.2008
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Предметный указатель
Dielectric continuum approximation 237
Dielectric fluctuations, in polar medium, cumulant expansion and 234 236—237
Dielectric function 94 128 236
Differential photon scattering 267—269
Dimensionless momentum 218
Dipole 93 191
Dipole, approximation 107 112 113
Dipole, correlation functions 199
Dipole, coupling, in Heisenberg picture 139
Dipole, matrix elements 148 160
Dipole, moment 52
Dipole, moment operator 107
Dipole, operators 113 115 127 170
Dipole, time-independent, coupling in Liouville space 114
Dipole, transition, matrix elements 220 471
Dipole, transition, moments 500
Dipole-dipole interactions 295 463
Dipole-dipole interactions in Heitler — London approximation 483
Dipole-dipole interactions, coupling 479
Dipole-dipole tensor 463
Dirac -function 105 193
Direct scattering (Raman) 4f
Discrete set of oscillators 217—221
Distributions, theory of 194
Distributivity, addition rule for 40
Distributivity, multiplication rule for 40
Distributivity, scalar product rule for 41
Divergence 104
Doorway operators 375
Doorway wavepackets 369 375 376.See
Doorway wavepackets for off-resonant birefringence and dichroism 455
Doorway wavepackets in Liouville space 372
Doorway wavepackets in snapshot limit 379 396—398
Doorway wavepackets, excited-state 384
Doorway wavepackets, ground-state 362
Doorway wavepackets, ground-state, effective Hamiltonian derivation for 426 441—443
Doorway wavepackets, ground-state, off-resonance spectroscopy and 384
Doorway wavepackets, off-resonant 385
Doorway wavepackets, second-rank tensor 452
Doorway-window wavepacket representation for pump-probe spectroscopy 133 415
Doorway-window wavepacket representation for well separated pulses 373—377 375f
Doorway-window wavepacket representation in frequency domain 365—366
Doorway-window wavepacket representation in reduced space 385
Doorway-window wavepacket representation of nonlinear response function 359—363
Doorway-window wavepacket representation, basis for 322
Doorway-window wavepacket representation, classical simulations and 346
Doorway-window wavepacket representation, Louville space pathways and 446
Doorway-window wavepacket representation, off-resonance Raman scattering and 414
Double commutator 164
Double-sided Feynman diagrams See Feynman diagrams double-sided
Dressed states 112 182
Driven anharmonic oscillator model 13 469—475 474f
Drude oscillator 13
Drude oscillator, formula 475
Drude oscillator, model 232
Drude oscillator, picture See Harmonic oscillators
Dye resorufin in a polar solvent (DMSO) 308 308f
dynamic variables 160
Dyson equation 34 39 65
Echo response function 299
Effective Liouville operator 68 149
Eigenstates 169 215
Eigenstates and highly resolved spectra in simple quantum systems 143
Eigenstates for partitioned Hamiltonian 37
Eigenstates of Hamiltonian 17 60 65 148
Eigenstates of macroscopic systems 13
Eigenstates of single small particle 144
Eigenstates, bath Hamiltonian 176
Eigenstates, electronic, expansion of 269
Eigenstates, expansion 209 269
Eigenstates, linear response in Liouville space and 147—149
Eigenstates, nuclear, expansion of 270
Eigenstates, nuclear, Liouville space-generating function expansion 364
Eigenstates, representation of Hilbert space Green function 32
Eigenstates, representation of Liouville space Green function 147
Eigenstates, single exciton 493
Eigenstates, vibronic 345
Eigenvalues 17 19 37 60 499
Eigenvectors 17 19
Electric current operator 82
Electric displacement operator 85
electric field 113 114 324
Electric field in coherent Raman spectroscopy 415
Electric field, classical transverse 112
Electric field, polarization 86 269
electromagnetic field 79
Electromagnetism theory 79
Electronic coherences 199 441
Electronic degeneracy 210
Electronic dephasing 169 244 411 454
Electronic energy gap 225 227 240
Electronic energy gap, coherent nuclear motions and 218
Electronic energy gap, collective nuclear coordinate for 191
Electronic energy gap, solvation coordinate 236
Electronic energy gap, stochastic Gaussian Markov modulation of 225
Electronic energy gap, thermally averaged 211
Electronic polarization Kerr effect 446 447f
Electronic systems, coupling to harmonic vibrations, coherent nuclear motions and 217—221 220f
Electronic systems, two-level See Two-electronic level systems
Electronic transition 190
Electronic transition, dipole operator 189
Electronic transition, frequency 158 243
Electronic transition, static distribution of 290
Electrostatic interaction 87 236
Elementary bond breakage 11f
Emission lineshapes 250—252
Energy flux 90
entropy 134—135
Equations of motion See also specific equations of motion
Equations of motion in Hilbert space vs. Liouville space 58f
Equations of motion, semiclassical, for Liouville space-generating functions 351—355
Equilibrium two-time correlation 414
Euler angles 449 450
Euler equations 458
Evolution operator 185
Excited state, coherent anti-Stokes Raman spectroscopy (CARS) 130 280 281—282 285
Excited state, doorway wavepackets 384
Excited state, Hamiltonian 169
Excited state, inverse lifetime 271
Excited state, manifold 245
Excited state, populations 411
Excited state, resonance 283
Exciton, coherence size 506
Exciton, coherence size, temperature variation 481 482f
Exciton, confinement 480—481 481f
Exciton, dephasing 516—517
Exciton, migration 479
Exciton, population relaxation 516
Exciton, population variables 507—512 511f 512f
Exciton, population variables, for Green function solution, factorized approximations for 490
Exciton, transport 507—508
Exciton, transport, in phase space 508—510
Exciton-exciton interactions 513—514
Exciton-phonon coupling, stochastic model of 517
Exciton-phonon interaction 516
Existence of zero vector 40
Expansion of vector, in Hilbert space vs. Liouville space 58f
expectation values 354 357 414
Exponential energy gap, time-ordered 200
Extended systems, optical response, nonlocal expressions for 123—124
Extinction coefficient 95
Fast dephasing 203
Fast modulation limit 223 306
Femtosecond spectroscopy 328
Femtosecond spectroscopy, laser sources 328
Femtosecond spectroscopy, pulse shaping, high-resolution 423 423f
Femtosecond spectroscopy, pulse shaping, techniques 423
Femtosecond spectroscopy, Raman techniques 294 417—418 428
Fermi Golden Rule 146 250
fermions 514
Feynman diagrams 137 144 156
Feynman diagrams, double-sided 153—154 154f—155f 157f 159
Feynman diagrams, double-sided, for phase-locked spontaneous light emission 311
Feynman diagrams, double-sided, for probe absorption 327f 374
Feynman diagrams, double-sided, for response function in RWA 298f 326
Feynman diagrams, double-sided, for sequential pump-probe spectroscopy 326—327 327f
Feynman diagrams, double-sided, for spontaneous light emission processes 267 268f
Feynman diagrams, double-sided, for time-domain four-wave mixing in two-level system 297 298f
Feynman diagrams, double-sided, in three-level system 394 394f 396
Feynman diagrams, double-sided, of absorption 220 220f
Feynman diagrams, double-sided, of relaxed fluorescence 220 220f
Feynman diagrams, one-sided 156
Feynman — Vernon influence functional 356
Field amplitudes 375
Field intensity 90 95 174
Field operators 91
Fifth-order polarization 434
First-order perturbation theory 483
Floquet expansion 112
Fluctuation-dissipation theorem 143 144f 242 423
Fluctuation-dissipation theorem in semiclassical simulations 242
Fluctuation-dissipation theorem, Brownian oscillator parameters for polar solvent and 253—254
Fluctuation-dissipation theorem, description of 146 147f
Fluctuation-dissipation theorem, multimode Brownian oscillator model and 228
Fluctuation-dissipation theorem, spectral density and 215
Fluctuation-dissipation theorem, stochastic models and 225
Fluorescence 133 261—262
Fluorescence, absorption of quantum field 262—264 263f
Fluorescence, anisotropy 445 453
Fluorescence, emission 250
Fluorescence, excitation spectrum 9f 10f 290
Fluorescence, excitation spectrum, of rhodamine 194 195f
Fluorescence, line narrowing 338 388—389
Fluorescence, line narrowing, inhomogeneous broadening and 294
Fluorescence, line narrowing, time-dependent Stokes shift 372
Fluorescence, Raman spectroscopy and 271—279 272f 274f—279f
Fluorescence, spontaneous light emission spectroscopy and See Spontaneous light emission spectroscopy (SLE)
Fokker — Planck equation for doorway-window representation of nonlinear response function 362
Fokker — Planck equation for Liouville space wavepackets 357 358 359
Fokker — Planck equation, rotational 446 453 458—459
Forster energy transfer 479
Forward propagation 32
Four-mode system, photon echoes for 306 307f 308
Four-wave mixing 4f 116 295
Four-wave mixing in semiconductor 7 9f
Four-wave mixing, coherent Raman spectroscopy See Coherent Raman spectroscopy
Four-wave mixing, degenerate 175 282 509
Four-wave mixing, degenerate, time-domain analogue of 510—512 511f 512f
Four-wave mixing, femtosecond 432
Four-wave mixing, pressure-induced extra resonance in 282
Four-wave mixing, resonant, frequency factors for 297t
Four-wave mixing, resonant, in time-domain 322
Four-wave mixing, resonant, non-time-ordered 323—324
Four-wave mixing, resonant, paths for 297;
Four-wave mixing, resonant, wavevectors for 297r
Four-wave mixing, tensorial aspects of 446
Four-wave mixing, third-order nonlinearities and 4—5
Four-wave mixing, three-pulse time-domain 296 296f
Four-wave mixing, time-domain, classification of 295—299 296f 297f 298f
Four-wave mixing, time-domain, in two-level system, double-sided Feynman diagrams for 297 298f
Four-wave mixing, time-domain, resonant 322
Four-wave mixing, time-integrated 474 474f
Four-wave mixing, transient grating See Transient grating
Fourier decomposition 125
Fourier transforms 34
Fourier transforms for nonlinear response functions 129
Fourier transforms for off-resonance Raman scattering 430—432
Fourier transforms in nonlinear spectroscopies 322
Fourier transforms in phase averaging 191 199
Fourier transforms in Raman techniques 414
Fourier transforms in semiclassical simulations 242
Fourier transforms of time evolution operator 31—32
Fourier transforms, absorption lineshape and 290
Fourier transforms, definition of 228
Fourier transforms, Green function, in Hilbert space 33 34
Fourier transforms, Green function, in Liouville space vs. Hilbert space 64 65
Fourier transforms, nonlinear response in momentum (k) space 124—125
Fourier transforms, of correlation function 256
Fourier transforms, one-sided 120
Fourier transforms, relationships between pump-probe and hole-burning spectroscopies 340—343 342f
Fourier transforms, spatial 105
Fourier transforms, time- vs. frequency-domain techniques 5 13 134
Fourier transforms, using contour integration 229
Franck — Condon principle 202—203 338 398 403—406
Free radiation-field Hamiltonian 81
Freedom, degrees of 132
Frenkel exciton model 504 513 514
Frequency sum generation 116
Frequency-dependent dielectric function, of solid 253
Frequency-dependent wavepackets 416
Frequency-domain spectroscopy 31—32 117 124 127 145 168 171 214 219 244 322
Frequency-domain spectroscopy, advanced Green function in 33
Frequency-domain spectroscopy, coherent Raman scattering 417—429
Frequency-domain spectroscopy, doorway-window picture 365—366
Frequency-domain spectroscopy, homogeneous broadening 343
Frequency-domain spectroscopy, ideal 129
Frequency-domain spectroscopy, impulsive coherent anti-Stokes Raman 420 421f
Frequency-domain spectroscopy, inhomogeneous broadening and 343
Frequency-domain spectroscopy, lineshape function 150
Frequency-domain spectroscopy, Liouville space pathways in 120—122
Frequency-domain spectroscopy, Liouville space pathways in, linear response 121
Frequency-domain spectroscopy, Liouville space pathways in, second-order response 121
Frequency-domain spectroscopy, Liouville space pathways in, third-order response 122
Frequency-domain spectroscopy, nth order response function in 120—121
Frequency-domain spectroscopy, nuclear susceptibility 360
Frequency-domain spectroscopy, optical susceptibilities 244 245
Frequency-domain spectroscopy, Raman measurements 412
Frequency-domain spectroscopy, Raman techniques, dynamic approach to coherent Raman Frequency-domain spectroscopy, scattering and 414—422 421f
Frequency-domain spectroscopy, spontaneous light emission 267—271
Frequency-domain spectroscopy, spontaneous Raman scattering 417—429
Frequency-domain spectroscopy, techniques 13
Function, of an operator 17—18
Gauge transformation 80 84
Gaussian distribution 224 287 293
Gaussian distribution of transition frequencies 187
Gaussian distribution with Stokes shift 223
Gaussian distribution, inhomogeneous broadening 232 235f 338
Gaussian distribution, lineshape 194
Gaussian distribution, lineshape, Brownian oscillator model and 388
Gaussian distribution, profiles 173 222 292 293 386
Gaussian distribution, stochastic random variable 226 517
Gaussian wavepackets in coordinate space 233
Gaussian wavepackets in phase space 354
General relaxation matrices 149
Generalized master equations 442
Grating configurations 12
Grating signal, polarization-dependent 451—455 454f—455f
Grating, heterodyne-detected, probe field in 453
Green function 36 67 167 172 190 280 303 358
Green function for third-order variables 488
Green function of transverse electromagnetic field in vacuum 495
Green function, advanced 33—34 64
Green function, anharmonic oscillator picture and 513
Green function, coherence 203 204—205 403
Green function, coherence, semiclassical expansion with reference Hamiltonian 199—200 204—205
Green function, contour integration 32—33
Green function, exciton population 488 519
Green function, expression, for four-wave mixing signal including radiative decay 493—496
Green function, expression, for molecular assembly with arbitrary geometry 496
Green function, expression, for nonlinear response 485—486
Green function, expression, frequency domain, in Hilbert space vs. Liouville space 58t
Green function, expression, in general solution of Heisenberg equation of motion 139
Green function, expression, in Hilbert space 31—34 137
Green function, expression, in Liouville space 64—67
Green function, expression, noninteracting, for pure dephasing 519
Green function, expression, of optical response of molecular nanostructures with arbitrary geometry 483—488 484f
Green function, expression, of optical response of molecular nanostructures with arbitrary geometry, in frequency domain 150
Green function, expression, one-exciton 487
Green function, expression, one-sided Fourier transform 120
Green function, expression, partitioning of 35—36
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