INTERMOLECULAR VIBRATIONAL COHERENCE IN MOLECULAR LIQUIDS

The femtosecond optical heterodyne detected optical Kerr effect/Raman- induced Kerr effect (OHD OKE/RIKE) is described in detail with emphasi s on the utility for investigating the intermolecular spectra and dyna mics of liquids, The femtosecond dynamics of the liquids CS2, benzene and CCl4 are addressed through a combination of conventional time-doma in kinetic and Fourier-transform analyses, and the physical origin of the intermolecular intensity is addressed for each, The distinctions b etween the excitation mechanisms of the femtosecond OKE/RIKE and other continuous-wave and picosecond Raman techniques are described, The di stinctions between the dephasing mechanisms of intramolecular and inte rmolecular vibrational modes are discussed.