Simulations reveal that ISRS models of pump-probe signals require coherences between non-adjacent vibrational levels for agreement with wavepacket dynamics, and that the coherent anti-Stokes pathway dominates for the chosen pump and probe bandwidths.
Slow intramolecular vibrational relaxation leads to long-lived excited-state wavepackets
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Comparing and Contrasting Vibrational Wavepacket Dynamics and Impulsive Stimulating Raman Scattering Descriptions of Pump-Probe Spectroscopy: A Theoretical Study
Simulations reveal that ISRS models of pump-probe signals require coherences between non-adjacent vibrational levels for agreement with wavepacket dynamics, and that the coherent anti-Stokes pathway dominates for the chosen pump and probe bandwidths.