New results on ultrafast coherent excitation of molecular vibrations in liquids

Coherent Raman probe scattering experiments are performed to study dynamical processes of polyatomic liquids at 300 K. For single homogeneous transitions the dephasing time T₂ is readily obtained from time resolved investigations. Spectral studies show an interesting time dependent shift in scattered frequency. After the excitaiton the vibrating molecules are shown to relax freely with their resonance frequency. Multiple, equally spaced transitions exhibit a beating phenomenon which provides the dephasing time and the frequency interval between neighboring vibrational states. Inhomogeneously broadened systems do not allow a ready determination of the dephasing time by the present probing technique. Previous experiments on the subject have to be reconsidered.