Journal
SCIENCE
Volume 339, Issue 6125, Pages 1302-1305Publisher
AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/science.1231711
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Funding
- 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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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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