Journal
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 5, Issue 11, Pages 1963-1967Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jz500728d
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Funding
- Swiss National Science Foundation [134709/1]
- Ecole Polytechnique Federale de Lausanne
- Grants-in-Aid for Scientific Research [14J07892] Funding Source: KAKEN
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Quantum state-resolved reactivity measurements probe the role of vibrational symmetry on the vibrational activation of the dissociative chemisorption of CH4 on Pt(111). IR-IR double resonance excitation in a molecular beam is used to prepare CH4 in all three different vibrational symmetry components A(1), E, and F-2 of the 2 nu(3) antisymmetric stretch overtone vibration. Methyl dissociation products chemisorbed on the cold Pt(111) surface are detected via reflection absorption infrared spectroscopy (RAIRS). We observe similar reactivity for CH4 prepared in the A(1) and F-2 sublevels but up to a factor of 2 lower reactivity for excitation of the E sublevel. It is suggested that differences in the localization of the C-H stretch amplitudes for the three states at the transition state leads to the observed difference in reactivity rather than state-specific vibrational energy transfer to electronic excitation of the metal.
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