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Title: Catalysis in real time using x-ray lasers

Here, 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(0 0 0 1), 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.
Authors:
 [1] ;  [2] ;  [3] ;  [4] ;  [5] ;  [6] ;  [1] ;  [1] ;  [7] ;  [8] ;  [4] ;  [1]
  1. Stockholm Univ., Stockholm (Sweden)
  2. Chapman Univ., Orange, CA (United States)
  3. Stockholm Univ., Stockholm (Sweden); Swedish Radiation Safety, Stockholm (Sweden)
  4. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  5. CNR-IOM, Trieste (Italy)
  6. Deutsches Elektronen-Synchrotron (DESY) Photon Science, Hamburg (Germany)
  7. SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., Stanford, CA (United States)
  8. Deutsches Elektronen-Synchrotron (DESY) Photon Science, Hamburg (Germany); Univ. of Hamburg and Center for Free Electron Laser Science, Hamburg (Germany)
Publication Date:
Grant/Contract Number:
AC02-76SF00515
Type:
Published Article
Journal Name:
Chemical Physics Letters
Additional Journal Information:
Journal Volume: 675; Journal Issue: C; Journal ID: ISSN 0009-2614
Publisher:
Elsevier
Research Org:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND TECHNOLOGY
OSTI Identifier:
1347236
Alternate Identifier(s):
OSTI ID: 1349281; OSTI ID: 1372896