Two-photon Raman excitation and coherent anti-Stokes Raman spectroscopy probing of population changes in polyatomic molecules: a novel nonlinear optical technique for vibrational-relaxation studies.
Two-photon Raman excitation is used to populate selectively vibrational states in CO(2) and SF(6). The collisional population of 01(1)0, 02(2)0, 03(1)0, 11(1)0, etc. by means of 10 degrees 0 and 02 degrees 0 states in CO(2) gas is studied by coherent anti-Stokes Raman spectroscopy. No population transfer is observed between Fermi-resonant CO(2)(10 degrees 0) and CO(2)(02 degrees 0) states with the rate constant K greater, similar 7 10(4) sec(-1) Torr(-1). The lifetime of the SF(6)(100000) state is found to be taurho greater, similar 15 microsec Torr.
Gladkov
S M
SM
Karimov
M G
MG
Koroteev
N I
NI