期刊
JOURNAL OF PHYSICAL CHEMISTRY A
卷 105, 期 34, 页码 7960-7972出版社
AMER CHEMICAL SOC
DOI: 10.1021/jp002449k
关键词
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The apparently - multicomponent subpicosecond intermolecular dynamics of carbon disulfide liquid are addressed in a unified manner in terms of an inhomogeneously broadened quantum mechanical harmonic oscillator model for a single vibrational coordinate. For an inhomogeneously broadened (Gaussian) distribution of oscillators, the model predicts naturally the bimodal character of the subpicosecond intermolecular dynamics of carbon disulfide liquid, and also the spectral evolution effects (spectral narrowing and saturation) that are observed for solutions of carbon disulfide in weakly interacting alkane solvents. The unique dynamical signature of these low-frequency vibrational coordinates is determined largely by the physical constraints on the coordinates (near equality of oscillator frequency, dephasing frequency, and inhomogeneous bandwidth), such that constructive and destructive interference effects play a dominant role in shaping the experimental observable.
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