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  Observation of the adsorption and desorption of vibrationally excited molecules on a metal surface.

Shirhatti, P. R., Rahinov, I., Golibrzuch, K., Werdecker, J., Geweke, J., Altschäffel, J., et al. (2018). Observation of the adsorption and desorption of vibrationally excited molecules on a metal surface. Nature Chemistry, 10(6), 592-598. doi:10.1038/s41557-018-0003-1.

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Item Permalink: http://hdl.handle.net/21.11116/0000-0000-B345-8 Version Permalink: http://hdl.handle.net/21.11116/0000-0003-B97A-4
Genre: Journal Article

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Shirhatti, P. R.1, Author              
Rahinov, I., Author
Golibrzuch, K.1, Author              
Werdecker, J., Author
Geweke, J.1, Author              
Altschäffel, J.1, Author              
Kuma, S., Author
Auerbach, D. J.1, Author              
Bartels, C., Author
Wodtke, A.1, Author              
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1Department of Dynamics at Surfaces, MPI for biophysical chemistry, Max Planck Society, ou_578600              

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 Abstract: The most common mechanism of catalytic surface chemistry is that of Langmuir and Hinshelwood (LH). In the LH mechanism, reactants adsorb, become thermalized with the surface, and subsequently react. The measured vibrational (relaxation) lifetimes of molecules adsorbed at metal surfaces are in the range of a few picoseconds. As a consequence, vibrational promotion of LH chemistry is rarely observed, with the exception of LH reactions occurring via a molecular physisorbed intermediate. Here, we directly detect adsorption and subsequent desorption of vibrationally excited CO molecules from a Au(111) surface. Our results show that CO (v = 1) survives on a Au(111) surface for ~1 × 10-10 s. Such long vibrational lifetimes for adsorbates on metal surfaces are unexpected and pose an interesting challenge to the current understanding of vibrational energy dissipation on metal surfaces. They also suggest that vibrational promotion of surface chemistry might be more common than is generally believed.

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Language(s): eng - English
 Dates: 2018-02-262018-06
 Publication Status: Published in print
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 Rev. Method: Peer
 Identifiers: DOI: 10.1038/s41557-018-0003-1
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Title: Nature Chemistry
Source Genre: Journal
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Pages: - Volume / Issue: 10 (6) Sequence Number: - Start / End Page: 592 - 598 Identifier: -