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 emphasis on the utility for investigating the intermolecular spectra and dynamics of liquids. The femtosecond dynamics of the liquids CS2, benzene and CCI4 are addressed through a combination of conventional time-domain kinetic and Fourier-transform analyses, and the physical origin of the intermolecular intensity is addressed for each. The distinctions between the excitation mechanisms of the femtosecond OKE/RIKE and other continuous-wave and picosecond Raman techniques are described. The distinctions between the dephasing mechanisms of intramolecular and intermolecular vibrational modes are discussed.