Picosecond Photofragmentation of Tri- and Tetraatomlc Molecules: Measurement of "State-to-State" Reaction Rates

In this Letter, we report our first results on the picosecond measurements of state-to-state rates of reactions, involving three and four-atom molecules. These photofragment reactions are ICN → I + CN and NCNO → NO + CN. In these experiments, we use one picosecond pulse to initiate the photolysis and a second pulse to probe the produced fragments in their internal vibrational/rotational states. Results are presented for molecules in bulbs and beams, and comparisons with unimolecular theories are given.