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Title: Ab initio molecular dynamics study of the Eley-Rideal reaction of H + Cl–Au(111) → HCl + Au(111): Impact of energy dissipation to surface phonons and electron-hole pairs

Abstract

The reaction between an impinging H atom and a Cl atom adsorbed on Au(111), which is a prototype for the Eley-Rideal mechanism, is investigated using ab initio molecular dynamics at different incidence angles. The reaction yielding gaseous HCl with large internal excitation proceeds via both direct and hot-atom mechanisms. Significant energy exchange with both surface phonons and electron-hole pairs has been observed. Furthermore, their impact on the reactivity and final state distributions was found to be limited, thanks to the large exothermicity and small barrier of the reaction.

Authors:
 [1];  [2]; ORCiD logo [3];  [2]; ORCiD logo [4]; ORCiD logo [1]
  1. Univ. of New Mexico, Albuquerque, NM (United States). Dept. of Chemistry and Chemical Biology
  2. Univ. of Science and Technology of China, Hefei (China). Dept. of Chemical Physics
  3. Centro de Física de Materiales Centro Mixto, CSIC-UPV/EHU, San Sebastián (Spain); Donostia International Physics Center DIPC, San Sebastián (Spain)
  4. Univ. of Science and Technology of China, Hefei (China). Department of Chemical Physics
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center
Sponsoring Org.:
USDOE
OSTI Identifier:
1498065
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 148; Journal Issue: 1; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Zhou, Linsen, Zhou, Xueyao, Alducin, Maite, Zhang, Liang, Jiang, Bin, and Guo, Hua. Ab initio molecular dynamics study of the Eley-Rideal reaction of H + Cl–Au(111) → HCl + Au(111): Impact of energy dissipation to surface phonons and electron-hole pairs. United States: N. p., 2018. Web. doi:10.1063/1.5016054.
Zhou, Linsen, Zhou, Xueyao, Alducin, Maite, Zhang, Liang, Jiang, Bin, & Guo, Hua. Ab initio molecular dynamics study of the Eley-Rideal reaction of H + Cl–Au(111) → HCl + Au(111): Impact of energy dissipation to surface phonons and electron-hole pairs. United States. doi:10.1063/1.5016054.
Zhou, Linsen, Zhou, Xueyao, Alducin, Maite, Zhang, Liang, Jiang, Bin, and Guo, Hua. Wed . "Ab initio molecular dynamics study of the Eley-Rideal reaction of H + Cl–Au(111) → HCl + Au(111): Impact of energy dissipation to surface phonons and electron-hole pairs". United States. doi:10.1063/1.5016054. https://www.osti.gov/servlets/purl/1498065.
@article{osti_1498065,
title = {Ab initio molecular dynamics study of the Eley-Rideal reaction of H + Cl–Au(111) → HCl + Au(111): Impact of energy dissipation to surface phonons and electron-hole pairs},
author = {Zhou, Linsen and Zhou, Xueyao and Alducin, Maite and Zhang, Liang and Jiang, Bin and Guo, Hua},
abstractNote = {The reaction between an impinging H atom and a Cl atom adsorbed on Au(111), which is a prototype for the Eley-Rideal mechanism, is investigated using ab initio molecular dynamics at different incidence angles. The reaction yielding gaseous HCl with large internal excitation proceeds via both direct and hot-atom mechanisms. Significant energy exchange with both surface phonons and electron-hole pairs has been observed. Furthermore, their impact on the reactivity and final state distributions was found to be limited, thanks to the large exothermicity and small barrier of the reaction.},
doi = {10.1063/1.5016054},
journal = {Journal of Chemical Physics},
issn = {0021-9606},
number = 1,
volume = 148,
place = {United States},
year = {2018},
month = {1}
}

Journal Article:
Free Publicly Available Full Text
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Cited by: 15 works
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Figures / Tables:

Figure 1 Figure 1: Energetics (in eV) of the ER (H + Cl* HCl) and LH (H* + Cl* HCl) reaction paths along the reaction coordinate. Geometries of the stationary points along the reaction path are shown.

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    Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.