Observation of orientation-dependent electron transfer in molecule-surface collisions
2013 | journal article. A publication with affiliation to the University of Göttingen.
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Observation of orientation-dependent electron transfer in molecule-surface collisions
Bartels, N.; Golibrzuch, K.; Bartels, C.; Chen, L. I.; Auerbach, D. J.; Wodtke, A. M. & Schaefer, T. (2013)
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 110(44) pp. 17738-17743. DOI: https://doi.org/10.1073/pnas.1312200110
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Details
- Authors
- Bartels, Nils; Golibrzuch, Kai; Bartels, Christof; Chen, L. I.; Auerbach, Daniel J.; Wodtke, Alec Michael; Schaefer, Tim
- Abstract
- Molecules typically must point in specific relative directions to participate efficiently in energy transfer and reactions. For example, Forster energy transfer favors specific relative directions of each molecule's transition dipole [Forster T (1948) Ann Phys 2(1-2):55-75] and electron transfer between gas- phase molecules often depends on the relative orientation of orbitals [Brooks PR, et al. (2007) J Am Chem Soc 129(50):15572-15580]. Surface chemical reactions can be many orders of magnitude faster than their gas-phase analogs, a fact that underscores the importance of surfaces for catalysis. One reason surface reactions can be so fast is the labile change of oxidation state that commonly takes place upon adsorption, a process involving electron transfer between a solid metal and an approaching molecule. By transferring electrons to or from the adsorbate, the process of bond weakening and/or cleavage is initiated, chemically activating the reactant [Yoon B, et al. (2005) Science 307(5708):403-407]. Here, we show that the vibrational relaxation of NO-an example of electronically nonadiabatic energy transfer that is driven by an electron transfer event [Gadzuk JW (1983) J Chem Phys 79(12):6341-6348]-is dramatically enhanced when the molecule approaches an Au(111) surface with the N atom oriented toward the surface. This represents a rare opportunity to investigate the steric influences on an electron transfer reaction happening at a surface.
- Issue Date
- 2013
- Status
- published
- Publisher
- Natl Acad Sciences
- Journal
- PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
- ISSN
- 0027-8424
- Sponsor
- Alexander von Humboldt Foundation