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Mode-Specific Chemisorption of CH4 on Pt{110}-(1 × 2) Explored by First-Principles Molecular Dynamics

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journal contribution
posted on 10.11.2011, 00:00 by M. Sacchi, D. J. Wales, S. J. Jenkins
The chemisorption of CH4 on Pt{110}-(1 × 2) has been studied by vibrational analysis of the reaction pathway defined by the potential energy surface and, in time reversal, by first-principles molecular dynamics simulations of CH4 associative desorption, with the electronic structure treated explicitly using density functional theory. We find that the symmetric stretch vibration ν1 is strongly coupled to the reaction coordinate; our results therefore provide a firm theoretical basis for recently reported state-resolved reactivity measurements, which show that excitation of the ν1 normal mode is the most efficient way to enhance the reaction probability.