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Controlling an Electron-Transfer Reaction at a Metal Surface by Manipulating Reactant Motion and Orientation

Bartels, Nils ; Krüger, Bastian C. ; Auerbach, Daniel J. ; Wodtke, Alec M. ; Schäfer, Tim

Angewandte Chemie (International ed.), 2014-12, Vol.53 (50), p.13690-13694 [Periódico revisado por pares]

Weinheim: WILEY-VCH Verlag

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  • Título:
    Controlling an Electron-Transfer Reaction at a Metal Surface by Manipulating Reactant Motion and Orientation
  • Autor: Bartels, Nils ; Krüger, Bastian C. ; Auerbach, Daniel J. ; Wodtke, Alec M. ; Schäfer, Tim
  • Assuntos: Collisions ; Degrees of freedom ; Electron transfer ; Electrons ; Gain ; Gold ; Mathematical analysis ; Mathematical models ; Metals - chemistry ; Optical pumping ; Orientation ; Surface Properties ; surface scattering ; Vibration analysis ; vibrational relaxation ; vibrationally excited molecules
  • É parte de: Angewandte Chemie (International ed.), 2014-12, Vol.53 (50), p.13690-13694
  • Notas: ArticleID:ANIE201407051
    We thank the Alexander von Humboldt Foundation for support and Alexander Kandratsenka and John Tully for useful discussions.
    Alexander von Humboldt Foundation
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    ObjectType-Article-1
    SourceType-Scholarly Journals-1
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  • Descrição: The loss or gain of vibrational energy in collisions of an NO molecule with the surface of a gold single crystal proceeds by electron transfer. With the advent of new optical pumping and orientation methods, we can now control all molecular degrees of freedom important to this electron‐transfer‐mediated process, providing the most detailed look yet into the inner workings of an electron‐transfer reaction and showing how to control its outcome. We find the probability of electron transfer increases with increasing translational and vibrational energy as well as with proper orientation of the reactant. However, as the vibrational energy increases, translational excitation becomes unimportant and proper orientation becomes less critical. One can understand the interplay of all three control parameters from simple model potentials. The transfer of vibrational energy in collisions of an NO molecule with a gold surface proceeds by electron transfer. Thanks to new optical pumping and orientation methods, all molecular degrees of freedom important to this process can be controlled. The probability of the electron‐transfer reaction is enhanced by increased translational and vibrational energy as well as by proper orientation of the reactant.
  • Editor: Weinheim: WILEY-VCH Verlag
  • Idioma: Inglês

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