M. Dell'Angela, Toyli Anniyev, Martin Beye, Ryan Coffee, Alexander Föhlisch, 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, Nomi Sorgenfrei, J. J. Turner, M. Wolf, W. Wurth, A. Nilsson
- 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.
MetadatenAuthor details: | M. Dell'Angela, Toyli Anniyev, Martin BeyeORCiDGND, Ryan 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, Nomi SorgenfreiORCiDGND, J. J. Turner, M. Wolf, W. Wurth, A. Nilsson |
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DOI: | https://doi.org/10.1126/science.1231711 |
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ISSN: | 0036-8075 |
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Title of parent work (English): | Science |
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Publisher: | American Assoc. for the Advancement of Science |
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Place of publishing: | Washington |
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Publication type: | Article |
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Language: | English |
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Year of first publication: | 2013 |
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Publication year: | 2013 |
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Release date: | 2017/03/26 |
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Volume: | 339 |
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Issue: | 6125 |
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Number of pages: | 5 |
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First page: | 1302 |
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Last Page: | 1305 |
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Funding institution: | 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 |
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Organizational units: | Mathematisch-Naturwissenschaftliche Fakultät / Institut für Physik und Astronomie |
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Peer review: | Referiert |
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