Femtosecond multipulse polarization spectroscopy of molecular vibrations and rotations in liquids

Simultaneous control over the vibrational and rotational molecular responses in ultrafast optical Kerr-effect signals in acetonitrile, toluene, and chloroform at room temperature is achieved by means of non-resonance excitation with two 30-fs orthogonal linearly polarized laser pulses. It is shown that the orientational response of the molecules can be suppressed and their vibrational response isolated by enhanced the delay between the exciting pulses and their relative intensity.