Vibrational Population Distributions in Infrared Multiple-Photon Excitation Probed by Coherent Anti-Stokes Raman Spectroscopy

摘要

Coherent Anti stokes Raman spectroscopy has been used as a probe for molecules pumped by high-intensity Carbon Dioxide laser radiation. Ozone, sulfur hexafluoride, and chloroethane have been investigated. The intensity of the ground state CARS signal is decreased by Infrared multiphoton excitation, but signals at new vibrational origins do not appear. The observations on chloroethane are interpreted in terms of a rate equation model for IRMPE, modified to make vibrational redistribution into account. (Reprints).