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  Observation of orientation-dependent electron transfer in molecule–surface collisions.

Bartels, N., Golibrzuch, K., Bartels, C., Chen, L., Auerbach, D. J., Wodtke, A. M., et al. (2013). Observation of orientation-dependent electron transfer in molecule–surface collisions. Proceedings of the National Academy of Sciences of the United States of America, 110(44), 17738-17743. doi:10.1073/pnas.1312200110.

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Item Permalink: http://hdl.handle.net/11858/00-001M-0000-0014-A227-1 Version Permalink: http://hdl.handle.net/11858/00-001M-0000-0028-80DF-D
Genre: Journal Article

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 Creators:
Bartels, N., Author
Golibrzuch, K., Author
Bartels, C., Author
Chen, L.1, Author              
Auerbach, D. J.1, Author              
Wodtke, A. M.1, Author              
Schäfer, T., Author
Affiliations:
1Department of Dynamics at Surfaces, MPI for biophysical chemistry, Max Planck Society, ou_578600              

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 Abstract: Molecules typically must point in specific relative directions to participate efficiently in energy transfer and reactions. For example, Förster energy transfer favors specific relative directions of each molecule’s transition dipole [Förster 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.

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Language(s): eng - English
 Dates: 2013-10-042013-10-29
 Publication Status: Published in print
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 Rev. Method: Peer
 Identifiers: DOI: 10.1073/pnas.1312200110
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Title: Proceedings of the National Academy of Sciences of the United States of America
Source Genre: Journal
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Pages: - Volume / Issue: 110 (44) Sequence Number: - Start / End Page: 17738 - 17743 Identifier: -