A picosecond coherent probing technique is used to determine the homogeneous vibrational linewidth in liquids. Isotope effects on the symmetric CH₃-stretching vibration in methanol and acetone provided a sensitive test for various vibrational dephasing theories. Theories based on binary-collision or hydrodynamic models do not correctly account for the observed isotope effect. Exchange theory is shown to be qualitatively consistent with the results.
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Harris et al. (1980) studied this question.
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