Reaction dynamics in polyatomic systems and cluster assemblies are often complicated by multiple competing pathways. This chapter develops a method of modeling ultrafast reaction dynamics that permits the measurement of rate coefficients as well as the determination of the branching ratios of such competing processes. This method is based on a general understanding of the rate laws of chemical kinetics and the interaction of ultrafast laser pulses with molecular targets. This approach is applied to fit pump-probe experiments on sulfur dioxide and sulfur dioxide clusters. The influence of solvation on molecular dynamics is determined. The model is based on comparing the ratio of the amplitude coefficients of competing pathways, enabling a determination of their branching ratios.
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