Abstract
Collision-induced V-V energy transfer between different vibrational modes of a small polyatomic molecule in the gas phase generally occurs on the time scale of 101–103 gas-kinetic collisions. However, our infrared-ultraviolet double resonance (IRUVDR) experiments have demonstrated that collisional V-V transfer between the v6 (in-plane wag, 989-cm−1) and v4 (out-of-plane bend, 938-cm−1) vibrational modes of D2CO is remarkably rapid, occurring with approximately gas-kinetic efficiency. The general IRUVDR excitation scheme employed in this context is illustrated in Fig. 1. Earlier studies1,2 of D2CO/D2CO collisions have now been extended to a variety of collision partners (He, Ar, CH4 N2, N2O), providing some control of the relative rates of v6→v4 transfer and of rotational relaxation with respect to quantum numbers J and Ka. The extraordinary efficiency of collision-induced v6→v4 transfer in D2CO is attributable to the rovibrational mixing effect of Coriolis coupling and the availability of a number of efficient quasi-elastic relaxation channels.
© 1988 Optical Society of America
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