Abstract
Photofragmentation of acetone at 193 nm is known to produce predominantly two methyl radicals and a CO molecule. Infrared emission is collected for the CO fragment at time delays of 6-30 ..mu..s after the exciting laser pulse by a time-resolved Fourier transform spectrometer. High-resolution vibration-rotation spectra are obtained both under collision-free and rotationally relaxed conditions. The observed vibrational distribution is, for v = 1/2/3, 0.73 /plus minus/ 0.04/0.23 /plus minus/ 0.02/0.04 /plus minus/ 0.01. This distribution fits a temperature of /approximately/ 2030/sub /minus/430//sup +730/ K, in approximate agreement with previous low-resolution results from this laboratory. The observed rotational distribution is highly excited, approximating a temperature of 3360/sub /minus/800//sup +1540/ K. Both the vibrational and rotational distributions can be successfully modeled by using a pure impulsive mechanism for the fragmentation of an initial bent acetyl fragment. Thus, the observed distribution supports previous arguments that the dissociation occurs by a two-step fragmentation mechanism following single-photon excitation.
Published Version
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