Journal
CHEMICAL PHYSICS LETTERS
Volume 675, Issue -, Pages 145-173Publisher
ELSEVIER
DOI: 10.1016/j.cplett.2017.02.018
Keywords
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Funding
- Swedish Research Council
- U.S. Department of Energy, Basic Energy Science through the SUNCAT Center
- Swedish Energy Agency (Energirnyndigheten)
- Knut and Alice Wallenberg Foundation
- U.S. Department of Energy [DE-ACO2-76SF00515]
- Volkswagen Stiftung
- Deutsche Forschungsgemeinschaft within the excellence cluster
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-ACO2-76SF00515]
- LCLS
- Stanford University through the Stanford Institute for Materials Energy Sciences (SIMES)
- Lawrence Berkeley National Laboratory (LBNL)
- University of Hamburg [FSP 301]
- Center for Free Electron Laser Science (CFEL)
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We describe how the unique temporal and spectral characteristics of X-ray free-electron lasers (XFEL) can be utilized to follow chemical transformations in heterogeneous catalysis in real time. We highlight the systematic study of CO oxidation on Ru(0001), which we initiate either using a femtosecond pulse from an optical laser or by activating only the oxygen atoms using a THz pulse. We find that CO is promoted into an entropy-controlled precursor state prior to desorbing when the surface is heated in the absence of oxygen, whereas in the presence of oxygen, CO desorbs directly into the gas phase. We monitor the activation of atomic oxygen explicitly by the reduced split between bonding and antibonding orbitals as the oxygen comes out of the strongly bound hollow position. Applying these novel XFEL techniques to the full oxidation reaction resulted in the surprising observation of a significant fraction of the reactants at the transition state through the electronic signature of the new bond formation. (c) 2017 The Authors. Published by Elsevier B.V.
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