Abstract
Variable-time neutralization−reionization mass spectrometry is used to generate isotopomers of metastable hydrosulfonium radicals, H3S•, of lifetimes ranging between 0.2 and 2.8 μs. The fractions of metastable H332S•, H334S•, D332S•, D334S•, and D2H32S• increase with the increasing internal energy of the precursor cations. Intramolecular isotope effects favor less of H from D2HS•. Ab initio calculations at the MP2/6-311++G(3df,2p) level indicate existence of symmetry-restricted 2A‘ and 2A‘‘ electronic states of H3S•. Formation of metastable radicals from vibrationally excited precursor ions is discussed.
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