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Title: Chemical bond activation observed with an x-ray laser

Journal Article · · Journal of Physical Chemistry Letters
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  1. Helmholtz-Zentrum Berlin fur Materialien und Energie GmbH, Berlin (Germany); SLAC National Accelerator Lab., Menlo Park, CA (United States); Deutsches Elektronen-Synchrotron (DESY) Photon Science, Hamburg (Germany)
  2. Stockholm Univ., Stockholm, (Sweden)
  3. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  4. Univ. Hamburg and Center for Free-Electron Laser Science, Hamburg (Germany)
  5. Helmholtz-Zentrum Berlin fur Materialien und Energie GmbH, Berlin (Germany); Univ. Potsdam, Potsdam (Germany)
  6. Helmholtz-Zentrum Berlin fur Materialien und Energie GmbH, Berlin (Germany)
  7. SLAC National Accelerator Lab., Menlo Park, CA (United States); Chapman Univ., Orange, CA (United States)
  8. SLAC National Accelerator Lab., Menlo Park, CA (United States); Stockholm Univ., Stockholm, (Sweden)
  9. The Univ. of Liverpool, Liverpool (United Kingdom)
  10. SLAC National Accelerator Lab., Menlo Park, CA (United States); Stockholm Univ., Stockholm, (Sweden); KTH Royal Institute of Technology, Stockholm (Sweden)
  11. Fritz-Haber Institut der Max-Planck-Gesellschaft, Berlin (Germany)
  12. Deutsches Elektronen-Synchrotron (DESY) Photon Science, Hamburg (Germany); Univ. Hamburg and Center for Free-Electron Laser Science, Hamburg (Germany)

The concept of bonding and anti-bonding orbitals is fundamental in chemistry. The population of those orbitals and the energetic difference between the two reflect the strength of the bonding interaction. Weakening the bond is expected to reduce this energetic splitting, but the transient character of bond-activation has so far prohibited direct experimental access. Lastly, we apply time-resolved soft X-ray spectroscopy at a free-electron laser to directly observe the decreased bonding–anti-bonding splitting following bond-activation using an ultra short optical laser pulse.

Research Organization:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC02-76SF00515
OSTI ID:
1349302
Journal Information:
Journal of Physical Chemistry Letters, Vol. 7, Issue 18; ISSN 1948-7185
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 22 works
Citation information provided by
Web of Science

References (23)

Why Must Oxygen Atoms Be Activated from Hollow Sites to Bridge Sites in Catalytic CO Oxidation? journal March 2000
Fundamental Concepts in Heterogeneous Catalysis book January 2014
Phonon- Versus Electron-Mediated Desorption and Oxidation of CO on Ru(0001) journal August 1999
Indication of non-thermal contribution to visible femtosecond laser-induced CO oxidation on Ru(0001) journal August 2015
Chemical bonding on surfaces probed by X-ray emission spectroscopy and density functional theory journal October 2004
Real-Time Observation of Surface Bond Breaking with an X-ray Laser journal March 2013
Probing the transition state region in catalytic CO oxidation on Ru journal February 2015
Ultrafast soft X-ray emission spectroscopy of surface adsorbates using an X-ray free electron laser journal April 2013
Time-resolved X-ray spectroscopies of chemical systems: New perspectives journal May 2016
Local aspects of the adsorbate-substrate chemical bond in N/Cu(100) and O/Cu(100) journal July 1998
Femtochemistry at Metal Surfaces:  Nonadiabatic Reaction Dynamics journal October 2006
Ultra-fast dynamics of electron thermalization, cooling and transport effects in Ru(001) journal January 2004
The soft x-ray instrument for materials studies at the linac coherent light source x-ray free-electron laser journal April 2012
X-ray pulse preserving single-shot optical cross-correlation method for improved experimental temporal resolution journal March 2012
NEXAFS Spectroscopy book January 1992
Thermal evolution of the band edges of 6H-SiC: X-ray methods compared to the optical band gap journal December 2014
A climbing image nudged elastic band method for finding saddle points and minimum energy paths journal December 2000
Precursor-mediated adsorption and desorption: a theoretical analysis journal March 1988
Dynamics of precursor‐mediated chemisorption journal June 1991
Electronic structure calculations with GPAW: a real-space implementation of the projector augmented-wave method journal June 2010
Calculations of X-ray Emission Spectra of Molecules and Surface Adsorbates by Means of Density Functional Theory journal December 1998
Calculations of near-edge x-ray-absorption spectra of gas-phase and chemisorbed molecules by means of density-functional and transition-potential theory journal September 1998
An implementation of core level spectroscopies in a real space Projector Augmented Wave density functional theory code journal November 2011

Cited By (7)

Short-wavelength free-electron laser sources and science: a review text January 2017
In Situ/Operando Characterization Techniques to Probe the Electrochemical Reactions for Energy Conversion journal April 2018
Quantum-Sized Metal Catalysts for Hot-Electron-Driven Chemical Transformation journal August 2018
Theoretical X‐ray spectroscopy of transition metal compounds journal July 2019
Atom-specific activation in CO oxidation journal December 2018
Atom-specific activation in CO oxidation text January 2018
Short-wavelength free-electron laser sources and science: a review journal October 2017

Figures / Tables (4)