Chapter 3 - Cluster size effects on bound excited states of SO 2

2004 
Sulphuric acid resulting from the oxidation of atmospheric SO 2 is a major constituent of acid rain. The oxidation process is influenced by factors such as clouds and aerosol particles, light intensity, O 3 , and peroxides. Thus, the nature of the factors leading to the alteration of atmospheric SO 2 chemistry may be clarified by experimentally studying the excited state dynamics of SO 2 solvated in SO 2 clusters. It appears that the size of a particle containing SO 2 may alter its reactivity since the dynamics of (SO 2 )n clusters show a substantial dependence on n. The findings of the experiments presented in this chapter indicate that the time required for the transition from the initially excited 1 B 1 state to the double wells that result from the crossing of the 1 A 2 and 1 B 1 states is significantly greater than is found from a theoretical treatment of the transition. The study of the SO 2 F band provides experimental evidence that the SO 2 molecule remains in a bound excited state for a substantial time indicating that coupling to dissociative sates is not operative in this region of the potential energy surface. Thus, the experiments presented in this chapter provide previously unknown information about the properties of the little studied F band of SO 2 .
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