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• W1541341461 abstract "These imaging experiments study the formation of the methylsulfonyl radical, CH3SO2, from the photodissociation of CH3SO2Cl at 193 nm and determine the energetic barrier for the radical’s subsequent dissociation to CH3+SO2. We first state-selectively detect the angular and recoil velocity distributions of the Cl(P23/2) and Cl(P21/2) atoms to further refine the distribution of internal energy partitioned to the momentum-matched CH3SO2 radicals. The internal energy distribution of the radicals is bimodal, indicating that CH3SO2 is formed in both the ground state and low-lying excited electronic states. All electronically excited CH3SO2 radicals dissociate, while those formed in the ground electronic state have an internal energy distribution which spans the dissociation barrier to CH3+SO2. We detect the recoil velocities of the energetically stable methylsulfonyl radicals with 118 nm photoionization. Comparison of the total recoil translational energy distribution for all radicals to the distribution obtained from the detection of stable radicals yields an onset for dissociation at a translational energy of 70±2 kcal/mol. This onset allows us to derive a CH3SO2→CH3+SO2 barrier height of 14±2 kcal/mol; this determination relies on the S–Cl bond dissociation energy, taken here as the CCSD(T) predicted energy of 65.6 kcal/mol. With 118 nm photoionization, we also detect the velocity distribution of the CH3 radicals produced in this experiment. Using the velocity distributions of the SO2 products from the dissociation of CH3SO2 to CH3+SO2 presented in the following paper, we show that our fastest detected methyl radicals are not from these radical dissociation channels, but rather from a primary S–CH3 bond photofission channel in CH3SO2Cl. We also present critical points on the ground state potential energy surface of CH3SO2 at the CCSD(T)/aug-cc-pV(Q+d)Z//CCSD(T)/6-311++G(2df,p) level. We include harmonic zero-point vibrational corrections as well as core-valence and scalar-relativistic corrections. The CCSD(T) predicted barrier of 14.6 kcal/mol for CH3SO2→CH3+SO2 agrees well with our experimental measurement. These results allow us to predict the unimolecular dissociation kinetics of CH3SO2 radicals and critique the analysis of prior time-resolved photoionization studies on this system." @default.
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• W1541341461 date "2009-07-22" @default.
• W1541341461 modified "2023-09-27" @default.
• W1541341461 title "Determining the CH3SO2→CH3+SO2 barrier from methylsulfonyl chloride photodissociation at 193 nm using velocity map imaging" @default.
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• W1541341461 doi "https://doi.org/10.1063/1.3159556" @default.
• W1541341461 hasPubMedId "https://pubmed.ncbi.nlm.nih.gov/19655864" @default.
• W1541341461 hasPublicationYear "2009" @default.
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