Abstract
It is shown that time-resolved nonlinear optical techniques can be extended to the selective study of the dynamics of vibrational overtones and two-phonon states in condensed media. In a primary application the first experimental demonstration of coherent anti-Stokes higher order Raman scattering (CAHORS) on the overtone and bound two-phonon state of the v2 vibration in liquid and crystalline CS2 , respectively. Is presented. The CAHORS technique is subsequently employed to measure the coherence relaxation times of both components of the Fermi doublet {v1 ,2v2 } in condensed CO2 , as a function of temperature up to and across the melting point. Several possible mechanisms for the loss of coherence of bound two-phonon states are described and discussed.
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