FEMTOSECOND TIME-RESOLVED COHERENT RAMAN-SCATTERING UNDER VARIOUS POLARIZATION AND RESONANCE CONDITIONS

Vibrational dephasing of the benzene 992-cm-1 mode is examined by femtosecond time-resolved coherent anti-Stokes Raman scattering with an 80-fsec pulse under various polarization conditions, and a fast dephasing process is found that is possibly related to rotation of the molecule in the liquid. Time-resolved resonance coherent anti-Stokes Raman scattering is for a benzene solution of β-carotene (preresonance) and a methanol solution of the dye DQOCI (rigorous resonance). An unexpected rise and decay signals are observed in β-carotene, but only a decay signal is observed in DQOCI, which is probably due to inhomogeneous broadening. © 1990 Optical Society of America.