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Issue 4, 2019
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Hot-electron effects during reactive scattering of H2 from Ag(111): the interplay between mode-specific electronic friction and the potential energy landscape

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Abstract

The breakdown of the Born–Oppenheimer approximation gives rise to nonadiabatic effects in gas-surface reactions at metal surfaces. However, for a given reaction, it remains unclear which factors quantitatively determine whether these effects measurably contribute to surface reactivity in catalysis and photo/electrochemistry. Here, we systematically investigate hot electron effects during H2 scattering from Ag(111) using electronic friction theory. We combine first-principles calculations of tensorial friction by time-dependent perturbation theory based on density functional theory and an analytical neural network representation, to overcome the limitations of existing approximations and explicitly simulate mode-specific nonadiabatic energy loss during molecular dynamics. Despite sizable hot-electron-induced energy loss, no measurable nonadiabatic effects can be found for H2 scattering on Ag(111). This is in stark contrast to previous reports for vibrationally excited H2 scattering on Cu(111). By detailed analysis of the two systems, we attribute this discrepancy to a subtle interplay between the magnitude of electronic friction along intramolecular vibration and the shape of the potential energy landscape that controls the molecular velocity at impact. On the basis of this characterization, we offer guidance for the search of highly nonadiabatic surface reactions.

Graphical abstract: Hot-electron effects during reactive scattering of H2 from Ag(111): the interplay between mode-specific electronic friction and the potential energy landscape

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Article information


Submitted
05 Sep 2018
Accepted
07 Nov 2018
First published
08 Nov 2018

This article is Open Access
All publication charges for this article have been paid for by the Royal Society of Chemistry

Chem. Sci., 2019,10, 1089-1097
Article type
Edge Article

Hot-electron effects during reactive scattering of H2 from Ag(111): the interplay between mode-specific electronic friction and the potential energy landscape

Y. Zhang, R. J. Maurer, H. Guo and B. Jiang, Chem. Sci., 2019, 10, 1089
DOI: 10.1039/C8SC03955K

This article is licensed under a Creative Commons Attribution-NonCommercial 3.0 Unported Licence. Material from this article can be used in other publications provided that the correct acknowledgement is given with the reproduced material and it is not used for commercial purposes.

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    [Original citation] - Published by The Royal Society of Chemistry (RSC) on behalf of the European Society for Photobiology, the European Photochemistry Association, and RSC.
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    [Original citation] - Published by The Royal Society of Chemistry.

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