We proposed a novel method in molecular polarization spectroscopy, based on the ultrafast optical Kerr effect to analyze probe femtosecond signals. We demonstrated the interpretaion of the reference chloroform signal by the novel method at room temperature. It was shown that handling of the separate molecular motions by creating the constructive or destructive interference of corresponding wave packets allows one to determine directly from the experiment such constants of molecular dynamics as the relaxation times of the coherent vibrations (»1.5 ps) and those of orientational anisotropy (»1.2ps).
femtosecond spectroscopy, molecular vibrational-rotational dynamics, ultrafast optical Kerr effect, lidar