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• W1503572283 abstract "Abstract Coherent nonlinear optical signals are commonly calculated using a semiclassical approach that assumes a quantum system interacting with classical fields. Compact expressions for the signals are then derived in terms of nonlinear susceptibilities. We present an alternative approach based on a quantum description of both matter and field. The signals are further recast in terms of transition amplitudes, which provide a clearer picture for the underlying molecular processes and may be intuitively represented by closed-time-path-loop diagrams. Unlike the semiclassical approach that treats the signal mode macroscopically using Maxwell’s equations, the present formalism allows for a fully microscopic calculation of the entire process. For example, n + 1 wave mixing appears as a concerted n + 1 photon event and all n + 1 field modes (including the signal) are treated on the same footing. Resonant contributions to nonlinear optical signals that carry useful molecule-specific information are recast as the modulus square of transition amplitudes and are clearly separated from the parametric background. Purely dissipative signals that can be measured using a collinear beam geometry and manipulated by pulse shaping techniques are proposed. The approach is demonstrated by applications to the stimulated Raman and the two-photon absorption components of pump–probe, and to coherent anti-Stokes Raman spectroscopy." @default.
• W1503572283 created "2016-06-24" @default.
• W1503572283 creator A5019093133 @default.
• W1503572283 creator A5085637107 @default.
• W1503572283 date "2010-01-01" @default.
• W1503572283 modified "2023-09-24" @default.
• W1503572283 title "Ultrafast Nonlinear Optical Signals Viewed from the Molecule’s Perspective" @default.
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• W1503572283 doi "https://doi.org/10.1016/s1049-250x(10)59006-2" @default.
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