Abstract
The progress of laser depletion and Stokes growth in transient stimulated Raman scattering (TSRS) is investigated using a Rayleigh-scattering technique. High laser depletion is found to dominate the behavior of TSRS under conditions relevant to excite-and-probe vibrational dynamics experiments. The results are used to explain differences between recent vibrational dephasing experiments. Implications of the results on both energy relaxation ( T 1) and phase relaxation ( T 2) experiments utilizing TSRS excitation are discussed.
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