Competitive events in fifth order time resolved coherent Raman scattering: Direct versus sequential processes

Abstract

Higher order time resolved nonlinear optical processes can often be obscured by sequential lower order processes that compete with the direct event and give similar time domain behavior though they probe different dynamics. This is true for a certain fifth order coherent anti-Stokes Raman scattering (CARS) spectroscopy designed to probe overtone vibrational dynamics. The homodyned intensity from the two competing processes is calculated and it is shown how only the direct fifth order polarization probes overtone dephasing.