Infrared multiphoton excitation of CF3I. I. Transient ultraviolet absorption study of after-pulse dissociation and excited state populations

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Abstract
Transient UV absorption spectra of CF3I were recorded during the IR multiphoton excitation of this molecule. Short laser pulses (20–50 ns) without longer tails were employed. Pressure effects were analyzed in the 10–100 mTorr range. Unimolecular dissociation rates (in the 106–107 s−1 range) after the pulse were identified unambiguously by time‐resolved low‐pressure observations and collisional quenching experiments. Marked laser intensity effects on the rates are attributed to intensity‐dependent changes of rotational state distributions of the reacting molecules. Excited state distributions have been resolved in direct observations. Bimodal distributions were identified.