Abstract
Recent femtosecond time-resolved impulsive stimulated scattering experimental results from molecular liquids are reviewed and new data are presented. Three main areas are discussed. First, the inertial molecular motions of simple liquids (CS 2 , benzene) are observed. The results can be interpreted in terms of intermolecular librations, which in some cases are clearly manifest in the form of oscillatory time-dependent responses. The temperature-dependent intermolecular librational frequency and dephasing dynamics in CS 2 liquid are determined. The data suggest that dephasing is predominantly inhomogeneous, and permit estimation of the extent of inhomogeneity in the librational frequency. Second, intramolecular vibrational oscillations are monitored directly in real time. The data are influenceed by both molecular vibrational and orientational dynamics. These experiments make possible time-resolved spectroscopy of vibrationally distorted molecules in well defined nonequilibrium configurations. Finally, the general occurrence of impulsive stimulated scat I. Etude des mouvements moleculaires inertiels de liquides simples (CS 2 , benzene); interpretation par des librations intermoleculaires qui, dans quelques cas, se manifestent par des reponses oscillatoires dependant du temps; determination de la variation temporelle de la frequence de libration et de la dynamique du dephasage pour CS 2 liquide, le dephasage etant principalement inhomogene; estimation du degre d'inhomogeneite du potentiel de libration. II. Etude des vibrations intramoleculaires en temps reel; influence des dynamiques moleculaires de vibrations et d'orientation; application a la spectroscopie resolue dans le temps de molecules vibrationnellement deformees dans des configurations bien definies hors d'equilibre. III. Discussion de l'apparition generalisee de la diffusion stimulee impulsionnelle chaque fois qu'une impulsion ultracourte traverse un milieu actif en Raman
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