title: Activated Dissociation of HCl on Au(111).
abstract: 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.
authors.affiliation: 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.
authors.forename: Pranav R
authors.initials: PR
authors.lastname: Shirhatti
authors.affiliation: 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.
authors.forename: Jan
authors.initials: J
authors.lastname: Geweke
authors.affiliation: 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.
authors.forename: Christoph
authors.initials: C
authors.lastname: Steinsiek
authors.affiliation: 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.
authors.forename: Christof
authors.initials: C
authors.lastname: Bartels
authors.affiliation: Department of Natural Sciences, Open University of Israel , 43553701 Raanana, Israel.
authors.forename: Igor
authors.initials: I
authors.lastname: Rahinov
authors.affiliation: 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.
authors.forename: Daniel J
authors.initials: DJ
authors.lastname: Auerbach
authors.affiliation: 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.|International Center for Advanced Studies of Energy Conversion, Georg-August University of Göttingen , Tammannstraße 6, 37077 Göttingen, Germany.
authors.forename: Alec M
authors.initials: AM
authors.lastname: Wodtke