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Hot electron effects during reactive scattering of H2 from Ag(111): assessing the sensitivity to initial conditions, coupling magnitude, and electronic temperature

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Abstract

Low-lying electronic excitations in metals, so-called hot electrons, efficiently mediate molecule-metal energy transfer and contribute to energy loss during molecular reactions at surfaces. They furthermore play an important role in plasmon-driven chemistry. Electronic friction represents a simple and effective concept to model hot electron-induced energy loss under ambient conditions. Different methods exist that vary in their description of magnitude, coordinate and directional dependence of friction during reactive molecular scattering at metal surfaces. Using molecular dynamics simulations with electronic friction, we systematically study the effect of hot electrons on measurable state-to-state scattering probabilities of molecular hydrogen from a (111) surface of silver. We assess the ability of ab initio electronic friction methods to accurately describe hot electron-mediated energy loss as a function of initial reaction conditions and electronic temperature. We furthermore find that dynamic scattering results and the ensuing energy loss are highly sensitive to the magnitude of electronic friction. Therefore, existing approximate models of electronic friction, which exhibit inherent uncertainties with respect to the magnitude of electronic friction, may not be applicable for a quantitative prediction of plasmon driven hot electron effects in their current state. We outline a development direction to potentially overcome these limitations.

Graphical abstract: Hot electron effects during reactive scattering of H2 from Ag(111): assessing the sensitivity to initial conditions, coupling magnitude, and electronic temperature

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Publication details

The article was received on 01 Oct 2018, accepted on 30 Oct 2018 and first published on 10 Dec 2018


Article type: Paper
DOI: 10.1039/C8FD00140E
Citation: Faraday Discuss., 2019, Advance Article
  • Open access: Creative Commons BY license
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    Hot electron effects during reactive scattering of H2 from Ag(111): assessing the sensitivity to initial conditions, coupling magnitude, and electronic temperature

    R. J. Maurer, Y. Zhang, H. Guo and B. Jiang, Faraday Discuss., 2019, Advance Article , DOI: 10.1039/C8FD00140E

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