• search hit 2 of 5
Back to Result List

Strong Influence of Coadsorbate Interaction on CO Desorption Dynamics on Ru(0001) Probed by Ultrafast X-Ray Spectroscopy and Ab Initio Simulations

  • We show that coadsorbed oxygen atoms have a dramatic influence on the CO desorption dynamics from Ru(0001). In contrast to the precursor-mediated desorption mechanism on Ru(0001), the presence of surface oxygen modifies the electronic structure of Ru atoms such that CO desorption occurs predominantly via the direct pathway. This phenomenon is directly observed in an ultrafast pump-probe experiment using a soft x-ray free-electron laser to monitor the dynamic evolution of the valence electronic structure of the surface species. This is supported with the potential of mean force along the CO desorption path obtained from density-functional theory calculations. Charge density distribution and frozen-orbital analysis suggest that the oxygen-induced reduction of the Pauli repulsion, and consequent increase of the dative interaction between the CO 5 sigma and the charged Ru atom, is the electronic origin of the distinct desorption dynamics. Ab initio molecular dynamics simulations of CO desorption from Ru(0001) and oxygen-coadsorbedWe show that coadsorbed oxygen atoms have a dramatic influence on the CO desorption dynamics from Ru(0001). In contrast to the precursor-mediated desorption mechanism on Ru(0001), the presence of surface oxygen modifies the electronic structure of Ru atoms such that CO desorption occurs predominantly via the direct pathway. This phenomenon is directly observed in an ultrafast pump-probe experiment using a soft x-ray free-electron laser to monitor the dynamic evolution of the valence electronic structure of the surface species. This is supported with the potential of mean force along the CO desorption path obtained from density-functional theory calculations. Charge density distribution and frozen-orbital analysis suggest that the oxygen-induced reduction of the Pauli repulsion, and consequent increase of the dative interaction between the CO 5 sigma and the charged Ru atom, is the electronic origin of the distinct desorption dynamics. Ab initio molecular dynamics simulations of CO desorption from Ru(0001) and oxygen-coadsorbed Ru(0001) provide further insights into the surface bond-breaking process.show moreshow less

Export metadata

Additional Services

Share in Twitter Search Google Scholar Statistics
Metadaten
Author:Hong Xin, Jerry LaRue, Henrik Oberg, Martin Beye, J. J. Turner, Jörgen Gladh, May L. Ng, Jonas A. Sellberg, Sarp Kaya, G. Mercurio, F. Hieke, Dennis Nordlund, William F. Schlotter, Georgi L. Dakovski, Michael P. Minitti, Alexander FöhlischORCiDGND, Martin Wolf, Wilfried Wurth, Hirohito Ogasawara, Jens K. Norskov, Henrik Ostrom, Lars G. M. Pettersson, Anders Nilsson, F. Abild-Pedersen
DOI:https://doi.org/10.1103/PhysRevLett.114.156101
ISSN:0031-9007 (print)
ISSN:1079-7114 (online)
Pubmed Id:http://www.ncbi.nlm.nih.gov/pubmed?term=25933322
Parent Title (English):Physical review letters
Publisher:American Physical Society
Place of publication:College Park
Document Type:Article
Language:English
Year of first Publication:2015
Year of Completion:2015
Release Date:2017/03/27
Volume:114
Issue:15
Pagenumber:6
Funder:US Department of Energy, Basic Energy Science; Swedish Research Council (VR); Department of Energy, Laboratory Directed Research and Development [DE-AC02-76SF00515]; VolkswagenStiftung; LCLS, Stanford University; Lawrence Berkeley National Laboratory (LBNL); University of Hamburg [FSP 301]; Center for Free Electron Laser Science (CFEL)
Organizational units:Mathematisch-Naturwissenschaftliche Fakultät / Institut für Physik und Astronomie
Peer Review:Referiert