Librational echo: Subpicosecond intermolecular interactions in liquid

The ultrafast optical Kerr effect observed in liquids upon two-pulse laser excitation is studied theoretically. It is shown that a Raman echo on librational frequencies (librational echo) can be excited in liquid. The librational echo has the following features: its shape and amplitude strongly depend on the local inhomogeneity of a medium and the form of local potentials; and the echo signal can be separated into the contributions of the phase and irreversible relaxation of coherent molecular librations. These properties of the librational echo can be used for studying the specific features of the local structure of liquids by the method of selective subpicosecond spectroscopy of molecular librations.