Time-resolved broadband Raman spectroscopies; A unified six-wave-mixing representation
arXiv:1308.6622 · doi:10.1063/1.4821228
Abstract
Excited-state vibrational dynamics in molecules can be studied by an electronically off-resonant Raman process induced by a probe pulse with variable delay with respect to an actinic pulse. We establish the connection between several variants of the technique that involve either spontaneous or stimulated Raman detection and different pulse configurations. By using loop diagrams in the frequency domain we show that all signals can be described as six wave mixing which depend on the same four point molecular correlation functions involving two transition dipoles and two polarizabilities and accompanied by a different gating. Simulations for the stochastic two-state-jump model illustrate the origin of the absorptive and dispersive features observed experimentally.
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- Detecting Electronic Coherence by Multidimensional Broadband Stimulated X-Ray Raman Signals
- Time-and-frequency gated photon coincidence counting; a novel multidimensional spectroscopy tool
- Stochastic Liouville Equations for Femtosecond Stimulated Raman Spectroscopy
- Detection of squeezed phonons in pump-probe spectroscopy
- Stimulated Raman lineshapes in the large light-matter interaction limit
- Stimulated Raman Spectroscopy with Entangled Light; Enhanced Resolution and Pathway Selection