Mode specific excitation of SO2 by resonant energy transfer from laser excited CH3F

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Abstract
The rate of rise of the ν3 (7.4 μ) fluorescence in S16O2 and S18O2 has been measured in CH3F/SO2/Ar mixtures subsequent to laser pumping of the 0–ν3 C–F stretching transition in CH3F. The risetimes were analyzed with the aid of a kinetic model which explicitly includes the collisional coupling between nearby vibrational states. The risetime of the S16O2 (ν2) fluorescence near 19 μ has also been measured and found to be almost two orders of magnitude slower than the risetime of the SO2 (ν3) stretching mode fluorescence. These results are consistent with mode specific excitation of SO2 by resonant energy transfer from CH3F and indicate that on the time scale of V–V crossover between CH3F and SO2 the stretching modes in SO2 (ν1 and ν3) are vibrationally hot with respect to the bending mode (ν2) in SO2.

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