Semiclassical Mode-Coupling Factorizations of Coherent Nonlinear Optical Response

dc.creatorJansen, Thomas la Cour
dc.creatorMukamel, Shaul
dc.date2003-07-25
dc.date.accessioned2026-07-07T02:52:37Z
dc.date.available2026-07-07T02:52:37Z
dc.descriptionThe identification of relevant collective coordinates is crucial for the interpretation of coherent nonlinear spectroscopies of complex molecules and liquids. Using an $\hbar$ 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, $\hbar$ 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 (MD) simulations. The existing classical simulation strategies, including Mode-Coupling in $\mathbf{k}$ space and in real-space, Langevin equations, and Instantaneous Normal Modes are compared from a unified viewpoint.
dc.identifierhttps://arxiv.org/abs/cond-mat/0307654
dc.identifierhttp://arxiv.org/abs/cond-mat/0307654
dc.identifier.urihttp://salesiana.dossiersoluciones.com/handle/123456789/21908
dc.subjectMaterials Science
dc.titleSemiclassical Mode-Coupling Factorizations of Coherent Nonlinear Optical Response
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