Intermolecular vibrational coherence in molecular liquids

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Abstract
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 CCI4are 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.