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Vibrational relaxation of highly vibrationally excited CO scattered from Au(111): Evidence for CO- formation.

MPS-Authors
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Wagner,  R. J. V.
Department of Dynamics at Surfaces, MPI for Biophysical Chemistry, Max Planck Society;

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Henning,  N.
Department of Dynamics at Surfaces, MPI for Biophysical Chemistry, Max Planck Society;

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Krüger,  B. C.
Department of Dynamics at Surfaces, MPI for Biophysical Chemistry, Max Planck Society;

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Park,  G. B.
Department of Dynamics at Surfaces, MPI for Biophysical Chemistry, Max Planck Society;

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Altschäffel,  J.
Department of Dynamics at Surfaces, MPI for Biophysical Chemistry, Max Planck Society;

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Kandratsenka,  A.
Department of Dynamics at Surfaces, MPI for Biophysical Chemistry, Max Planck Society;

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Wodtke,  A. M.
Department of Dynamics at Surfaces, MPI for Biophysical Chemistry, Max Planck Society;

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Schäfer,  T.
Department of Dynamics at Surfaces, MPI for Biophysical Chemistry, Max Planck Society;

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Citation

Wagner, R. J. V., Henning, N., Krüger, B. C., Park, G. B., Altschäffel, J., Kandratsenka, A., et al. (2017). Vibrational relaxation of highly vibrationally excited CO scattered from Au(111): Evidence for CO- formation. The Journal of Physical Chemistry Letters, (in press). doi:10.1021/acs.jpclett.7b02207.


Cite as: https://hdl.handle.net/11858/00-001M-0000-002D-EEC9-C
Abstract
Electronically non-adiabatic dynamics can be important in collisions of molecules at surfaces; for example, when vibrational degrees of freedom of molecules are coupled to electron-hole-pair (EHP) excitation of a metal. Such dynamics have been inferred from a host of observations involving multi-quantum relaxation of NO molecules scattered from metal surfaces. Electron transfer forming transient NO- is thought to be essential to the non-adiabatic coupling. The question remains: is this behavior usual? Here, we present final vibrational state distributions resulting from the scattering of CO(νi = 17) from Au(111), which exhibits significantly less vibrational relaxation than NO(νi = 16). We explain this observation in terms of the lower electron affinity of CO compared to NO, a result that is consistent with the formation of a transient CO- ion being important to CO vibrational relaxation.