Supporting Information

Activated Dissociation of HCl on Au(111)

Terms & Conditions

- Hide

Electronic Supporting Information files are available without a subscription to ACS Web Editions. The American Chemical Society holds a copyright ownership interest in any copyrightable Supporting Information. Files available from the ACS website may be downloaded for personal use only. Users are not otherwise permitted to reproduce, republish, redistribute, or sell any Supporting Information from the ACS website, either in whole or in part, in either machine-readable form or any other form without permission from the American Chemical Society. For permission to reproduce, republish and redistribute this material, requesters must process their own requests via the RightsLink permission system. Information about how to use the RightsLink permission system can be found at http://pubs.acs.org/page/copyright/permissions.html.

Activated Dissociation of HCl on Au(111)

Institute for Physical Chemistry, Georg-August University of Göttingen, Tammannstraße 6, 37077 Göttingen, Germany
Department of Dynamics at Surfaces, Max Planck Institute for Biophysical Chemistry, Am Faßberg 11, 37077 Göttingen, Germany
§ Max-Planck - EPFL Center for Molecular Nanoscience and Technology, Institute of Chemical Sciences and Engineering (ISIC), Station 6, École Polytechnique Fédérale de Lausanne, CH-1015 Lausanne, Switzerland
Department of Natural Sciences, Open University of Israel, 43553701 Raanana, Israel
International Center for Advanced Studies of Energy Conversion, Georg-August University of Göttingen, Tammannstraße 6, 37077 Göttingen, Germany
J. Phys. Chem. Lett., 2016, 7 (7), pp 1346–1350
DOI: 10.1021/acs.jpclett.6b00289
Publication Date (Web): March 18, 2016
Copyright © 2016 American Chemical Society
*E-mail: pshirha@gwdg.de.


Abstract Image

We report zero-coverage reaction probabilities (S0) for HCl dissociative adsorption on Au(111) obtained by the seeded molecular beam hot-nozzle method. For measurements at normal incidence with mean translational energies ranging from 0.94 to 2.56 eV (nozzle temperatures 296 to 1060 K), S0 increased from 6 × 10–6 to 2 × 10–2. S0 also increased with increasing nozzle temperature for fixed incidence energy associated with the motion normal to the surface. Accounting for the influence of the vibrational state population and translational energy distributions in the incident beam, we are able to compare the experimental results to recent theoretical predictions. These calculations, performed employing 6-D quantum dynamics on an electronically adiabatic potential energy surface obtained using density functional theory at the level of the generalized gradient approximation and the static surface approximation, severely overestimate the reaction probabilities when compared with our experimental results. We discuss some possible reasons for this large disagreement.

The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.jpclett.6b00289

  • (1) Parameters for incidence beam translational energy and vibrational state distributions. (2) Measurement of the hydrodynamic enrichment factor. (3) Calculation of the Cl coverage from the Auger electron spectroscopy measurements. (4) Notes regarding the measurement of the nozzle temperature and vibrational state distributions. (5) Estimating the loss of Cl coverage at Ts = 170 K due to recombinative desorption. (PDF)

Explore by:


Received 9 February 2016
Date accepted 18 March 2016
Published online 18 March 2016
Published in print 7 April 2016