COHERENT ANTI-STOKES-RAMAN SPECTROSCOPY OF INFRARED MULTIPHOTON EXCITED MOLECULES

Time-resolved coherent anti-Stokes Raman spectroscopy is used to obtai n the rovibrational energy distributions in polyatomic molecules follo wing infrared multiphoton excitation. In addition to presenting new re sults on SF6, we review previously obtained data on SO2 and OCS. The d ata yield new details about infrared multiphoton excitation and intram olecular vibrational energy relaxation. In particular they show the si gnificance of collisions in redistributing vibrational energy followin g excitation. The results also clearly show stronger intermode couplin g and higher excitation in systems with increasing numbers of atoms pe r molecule.