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Resonances in the Entrance Channel of the Elementary Chemical Reaction of Fluorine and Methane

Authors


  • The experimental part of this research is funded by the Air Force Office of Scientific Research under grant number FA9550-12-1-0160 and the Defense University Research Instrumentation Program under grant number FA9550-11-1-0300. M.L.W. thanks the National Science Foundation for a graduate research fellowship. For the theoretical part, financial support by the Deutsche Forschungsgemeinschaft and the Alexander von Humboldt Foundation is gratefully acknowledged.

Abstract

Extending the fully quantum-state-resolved description of elementary chemical reactions beyond three or four atom systems is a crucial issue in fundamental chemical research. Reactions of methane with F, Cl, H or O are key examples that have been studied prominently. In particular, reactive resonances and nonintuitive mode-selective chemistry have been reported in experimental studies for the F+CH4→HF+CH3 reaction. By investigating this reaction using transition-state spectroscopy, this joint theoretical and experimental study provides a clear picture of resonances in the F+CH4 system. This picture is deduced from high-resolution slow electron velocity-map imaging (SEVI) spectra and accurate full-dimensional (12D) quantum dynamics simulations in the picosecond regime.

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