Semiclassical mode-coupling factorizations of coherent nonlinear optical response
| Autor: | Thomas L. C. Jansen, Shaul Mukamel |
|---|---|
| Přispěvatelé: | Theory of Condensed Matter |
| Jazyk: | angličtina |
| Rok vydání: | 2003 |
| Předmět: |
General Physics and Astronomy
Semiclassical physics Space (mathematics) 01 natural sciences NONRESONANT INTERMOLECULAR SPECTROSCOPY Normal mode 0103 physical sciences Physical and Theoretical Chemistry 010306 general physics Quantum Quantum fluctuation 5TH-ORDER RAMAN RESPONSE TIME-CORRELATION-FUNCTIONS HETERODYNE-DETECTION Physics Quantum optics 010304 chemical physics ATOMIC LIQUID MOLECULAR HYDRODYNAMIC THEORY SPATIAL CORRELATIONS Nonlinear system Classical mechanics Mode coupling INSTANTANEOUS-NORMAL-MODE LIQUID CS2 PLACZEK APPROXIMATION |
| Zdroj: | Journal of Chemical Physics, 119(15), 7979-7987. AMER INST PHYSICS |
| ISSN: | 0021-9606 |
| Popis: | The identification of relevant collective coordinates is crucial for the interpretation of coherent nonlinear spectroscopies of complex molecules and liquids. Using an h expansion of Liouville space generating functions, we show how to factorize multitime nonlinear response functions into products of lower-order correlation functions of collective coordinates, and derive closed expressions for linear, second- and third-order response functions. In addition to providing systematic quantum corrections, h offers a convenient bookkeeping device even for the purely classical response, since including quantum fluctuations allows to circumvent the expensive computation of stability matrices which is a major bottleneck in molecular dynamics simulations. The existing classical simulation strategies, including mode coupling in k space and in real space, Langevin equations, and instantaneous normal modes are compared from a unified viewpoint. (C) 2003 American Institute of Physics. |
| Databáze: | OpenAIRE |
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