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Probing the transition state region in catalytic CO oxidation on Ru

  • Femtosecond x-ray laser pulses are used to probe the carbon monoxide (CO) oxidation reaction on ruthenium (Ru) initiated by an optical laser pulse. On a time scale of a few hundred femtoseconds, the optical laser pulse excites motions of CO and oxygen (O) on the surface, allowing the reactants to collide, and, with a transient close to a picosecond (ps), new electronic states appear in the OK-edge x-ray absorption spectrum. Density functional theory calculations indicate that these result from changes in the adsorption site and bond formation between CO and O with a distribution of OC-O bond lengths close to the transition state (TS). After 1 ps, 10% of the CO populate the TS region, which is consistent with predictions based on a quantum oscillator model.

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Metadaten
Author:H. Ostrom, H. Oberg, H. Xin, J. Larue, Martin Beye, J. Gladh, M. L. Ng, J. A. Sellberg, S. Kaya, G. Mercurio, D. Nordlund, M. Hantschmann, F. Hieke, D. Kuehn, W. F. Schlotter, G. L. Dakovski, J. J. Turner, M. P. Minitti, A. Mitra, S. P. Moeller, Alexander Foehlisch, M. Wolf, W. Wurth, Mats Persson, J. K. Norskov, F. Abild-Pedersen, Hirohito Ogasawara, Lars G. M. Pettersson, A. Nilsson
DOI:https://doi.org/10.1126/science.1261747
ISSN:0036-8075 (print)
ISSN:1095-9203 (online)
Pubmed Id:http://www.ncbi.nlm.nih.gov/pubmed?term=25722407
Parent Title (English):Science
Publisher:American Assoc. for the Advancement of Science
Place of publication:Washington
Document Type:Article
Language:English
Year of first Publication:2015
Year of Completion:2015
Release Date:2017/03/27
Volume:347
Issue:6225
Pagenumber:5
First Page:978
Last Page:982
Funder:U.S. Department of Energy, Basic Energy Science through SUNCAT Center for Interface Science and Catalysis; Swedish Research Council; Knut and Alice Wallenberg foundation; U.S. Department of Energy through SLAC Laboratory Directed Research and Development program [DE-AC02-76SF00515]; Volkswagen Stiftung; Deutsche Forschungsgemeinschaft within the excellence cluster "Center for Ultrafast Imaging (CUI)"; LCLS, Stanford University through Stanford Institute for Materials Energy Sciences (SIMES); Lawrence Berkeley National Laboratory (LBNL), University of Hamburg through the Bundesministerium fur Bildung, Wissenschaft; Forschung und Technologie priority program [FSP 301]; Center for Free Electron Laser Science (CFEL)
Organizational units:Mathematisch-Naturwissenschaftliche Fakultät / Institut für Physik und Astronomie
Peer Review:Referiert