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Real-time observation of surface bond breaking with an X-ray Laser

  • We used the Linac Coherent Light Source free-electron x-ray laser to probe the electronic structure of CO molecules as their chemisorption state on Ru(0001) changes upon exciting the substrate by using a femtosecond optical laser pulse. We observed electronic structure changes that are consistent with a weakening of the CO interaction with the substrate but without notable desorption. A large fraction of the molecules (30%) was trapped in a transient precursor state that would precede desorption. We calculated the free energy of the molecule as a function of the desorption reaction coordinate using density functional theory, including van der Waals interactions. Two distinct adsorption wells-chemisorbed and precursor state separated by an entropy barrier-explain the anomalously high prefactors often observed in desorption of molecules from metals.

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Author:M. Dell'Angela, Toyli Anniyev, Martin Beye, R. Coffee, Alexander FöhlischORCiDGND, J. Gladh, T. Katayama, S. Kaya, O. Krupin, J. LaRue, A. Mogelhoj, D. Nordlund, J. K. Norskov, H. Oberg, H. Ogasawara, H. Ostrom, Lars G. M. Pettersson, W. F. Schlotter, J. A. Sellberg, F. Sorgenfrei, J. J. Turner, M. Wolf, W. Wurth, A. Nilsson
ISSN:0036-8075 (print)
Parent Title (English):Science
Publisher:American Assoc. for the Advancement of Science
Place of publication:Washington
Document Type:Article
Year of first Publication:2013
Year of Completion:2013
Release Date:2017/03/26
First Page:1302
Last Page:1305
Funder:U.S. Department of Energy (DOE), Office of Basic Energy Sciences, Division of Materials Sciences and Engineering [DE-AC02-76SF00515]; DOE, Basic Energy Science through the SUNCAT Center for Interface Science and Catalysis; Swedish National Research Council; Danish Center for Scientific Computing; Volkswagen Stiftung; Alexander von Humboldt Foundation; Lundbeck Foundation; LCLS; Stanford University through SIMES; Lawrence Berkeley National Laboratory, University of Hamburg through the BMBF [FSP 301]; Center for Free Electron Laser Science
Organizational units:Mathematisch-Naturwissenschaftliche Fakultät / Institut für Physik und Astronomie
Peer Review:Referiert