Abstract
The dynamics of small, highly polarizable molecules have been studied extensively by light scattering. We have shown that the time-resolved technique of Impulsive Stimulated Scattering (ISS) can offer distinct advantages over conventional frequency-domain light scattering.1 In particular, ISS is well-suited to the measurement and characterization of low-frequency heavily-damped modes of molecular motion. Various theories of the liquid state predict such modes at high densities as a result of molecular caging effects. As the density of a liquid is increased, nearest neighbor distances decrease on average and the short-time dynamics of molecules are expected to be dominated by repulsive intermolecular interactions. A temperature-dependent study of the transient response of CS2 showed a weakly oscillatory signal suggestive of intermolecular vibration.2 To further study intermolecular vibration in dense liquids we have combined femtosecond time resolution with diamond anvil cell technology to study the ultrafast dynamics of CS2 molecules at constant temperature as a function of pressure.
© 1990 Optical Society of America
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