Journal
SCIENCE
Volume 347, Issue 6225, Pages 978-982Publisher
AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/science.1261747
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Funding
- 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)
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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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