Resonances in the entrance channel of the elementary chemical reaction of fluorine and methane

Till Westermann, Jongjin B. Kim, Marissa L. Weichman, Christian Hock, Tara I. Yacovitch, Juliana Palma, Daniel M. Neumark, Uwe Manthe

Research output: Contribution to journalArticle

45 Scopus citations

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. Chemical reactivity: Experimental and theoretical data consistently demonstrate the existence of resonances in the entrance channel of the F+CH4→HF+CH 3 reaction shown by transition-state spectroscopy (see picture; ΔSO=atomic spin-orbit splitting). Based on full-dimensional quantum dynamics simulations, a clear picture is drawn explaining the resonances.

Original languageEnglish (US)
Pages (from-to)1122-1126
Number of pages5
JournalAngewandte Chemie - International Edition
Volume53
Issue number4
DOIs
StatePublished - Jan 20 2014
Externally publishedYes

All Science Journal Classification (ASJC) codes

  • Catalysis
  • Chemistry(all)

Keywords

  • ab initio calculations
  • molecular dynamics
  • photoelectron spectroscopy
  • potential-energy surfaces
  • van der Waals complexes

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