Abstract
The femtosecond optical-heterodyne-detected optical Kerr effect/Raman-induced Kerr effect (OHD OKE/RIKE) dynamics of CS2 dissolved in a series of alkane solvents are reported. The data reveal that the nondiffusive (subpicosecond) dynamics of simple molecular liquids are determined largely by the details of the local, microscopic environment, rather than by the bulk solution properties, with no correlation observed between the short-time, nondiffusive dynamics and the bulk solution viscosity. For each solvent investigated, the vibrational spectral density is observed to narrow and shift to lower frequency with increasing dilution. While the same general trend is observed for each solvent, deviations of magnitude are observed for the longer-chain n-alkanes. This, coupled with the markedly nonexponential decay of the orientational anisotropy observed for the higher-alkane dilutions, suggests the presence of two distinct environments in which isolated pockets of CS2 exist. The observed spectral evolution is d...
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