Dresden 2014 – scientific programme
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O: Fachverband Oberflächenphysik
O 30: Surface Chemical Reactions and Heterogeneous Catalysis II
O 30.5: Talk
Tuesday, April 1, 2014, 11:30–11:45, PHY C 213
Towards Heterogeneous Catalysis Beyond the Born-Oppenheimer Approximation: LDFA and beyond — •Simon P. Rittmeyer1, J. Iñaki Juaristi2, Karsten Reuter1, and Jörg Meyer1 — 1TU München, Germany — 2Depto. & Centro de Física de Materiales (CSIC-UPV/EHU), San Sebastián, Spain
Inspired by the need of a more efficient and thus responsible use of energy, an age of light-enhanced heterogeneous catalysis is dawning. Even photons from sunlight can be used to accelerate surface reactions, if their energy is selectively and efficiently transferred into distinct nuclear degrees of freedom [1]. However, on metal catalysts resulting athermal mode populations are generally challenged by rapid energy dissipation in particular into the continuum of easily accessible electron-hole pair excitations. Ab initio molecular dynamics simulations beyond the Born-Oppenheimer approximation can assess corresponding lifetimes and therewith answer important questions as to the feasibility and efficiency of such light enhancement of catalytic reaction steps. On the way to establishing a numerically tractable approach even for complex surface processes we pursue the local density friction approach (LDFA) [2] and extend it beyond the hitherto inherent independent-atom and frozen-surface approximation. We apply this new scheme to the non-adiabatic damping of adsorbate vibrations on transition metal surfaces and critically discuss it by comparing the results to other theoretical approaches as well as experimental data.
[1] S. Linic et al., Acc. Chem. Res. 46, 1890 (2013).
[2] J. I. Juaristi et al., Phys. Rev. Lett. 100, 116102 (2008).