DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Time-resolved x-ray absorption spectroscopy probe in ultrafast surface chemistry

Journal Article · · Structural Dynamics
DOI: https://doi.org/10.1063/4.0000289 · OSTI ID:2511171
ORCiD logo [1]
  1. Stockholm University (Sweden); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). SUNCAT Center for Interface Science and Catalysis

To celebrate the scientific achievement of Jo Stöhr, I present here a personal account of the use of x-ray absorption spectroscopy to probe dynamics on surfaces using x-ray lasers. In particular, I will review the investigation of ultrafast processes in adsorbates on surfaces using an optical pump and an x-ray absorption spectroscopy probe. Here, it is shown that it is possible to gain insight into the effects of electronic excitations in metals on adsorbates as well as laser-induced vibrational motions. Furthermore, the ultrafast optical pump allows the detection of the CO precursor state in the desorption channel, species close to the transition state in CO oxidation, and the transient HCO intermediate during CO hydrogenation on Ru(0001).

Research Organization:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Organization:
Swedish National Research Council (VR); USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)
Grant/Contract Number:
AC02-76SF00515
OSTI ID:
2511171
Journal Information:
Structural Dynamics, Journal Name: Structural Dynamics Journal Issue: 1 Vol. 12; ISSN 2329-7778
Publisher:
American Crystallographic Association/AIPCopyright Statement
Country of Publication:
United States
Language:
English

References (33)

Handbook of Heterogeneous Catalysis book March 2008
Ultra-fast dynamics of electron thermalization, cooling and transport effects in Ru(001) journal January 2004
The electronic structure effect in heterogeneous catalysis journal April 2005
The sticking probabilities of gases chemisorbed on the surfaces of solids journal January 1957
Rate expressions for adsorption and desorption kinetics with precursor states and lateral interactions journal January 1981
Catalysis in real time using X-ray lasers journal May 2017
Ultrafast soft X-ray emission spectroscopy of surface adsorbates using an X-ray free electron laser journal April 2013
Chemical bonding on surfaces probed by X-ray emission spectroscopy and density functional theory journal October 2004
Chemical Bond Activation Observed with an X-ray Laser journal September 2016
Real-Time Elucidation of Catalytic Pathways in CO Hydrogenation on Ru journal August 2017
Direct Observation of the Transition State journal March 1995
Femtosecond Time-Resolved Photoelectron Spectroscopy journal April 2004
Femtochemistry at Metal Surfaces:  Nonadiabatic Reaction Dynamics journal October 2006
CO Chemisorption and Dissociation at High Coverages during CO Hydrogenation on Ru Catalysts journal April 2013
Direct versus Hydrogen-Assisted CO Dissociation journal September 2009
Precursor-mediated adsorption and desorption: a theoretical analysis journal March 1988
Time-resolved observation of transient precursor state of CO on Ru(0001) using carbon K-edge spectroscopy journal January 2020
Dynamics of precursor‐mediated chemisorption journal June 1991
Vacuum space charge effects in sub-picosecond soft X-ray photoemission on a molecular adsorbate layer journal March 2015
Atom-specific activation in CO oxidation journal December 2018
Symmetry-resolved CO desorption and oxidation dynamics on O/Ru(0001) probed at the C K-edge by ultrafast x-ray spectroscopy journal October 2022
Electronic structure of atomic adsorbates from x-ray-absorption spectroscopy: Threshold effects and higher excited states journal July 1993
Selective Ultrafast Probing of Transient Hot Chemisorbed and Precursor States of CO on Ru(0001) journal May 2013
Strong Influence of Coadsorbate Interaction on CO Desorption Dynamics on Ru(0001) Probed by Ultrafast X-Ray Spectroscopy and Ab Initio Simulations journal April 2015
Ultrafast Adsorbate Excitation Probed with Subpicosecond-Resolution X-Ray Absorption Spectroscopy journal June 2021
Atom-Specific Probing of Electron Dynamics in an Atomic Adsorbate by Time-Resolved X-Ray Spectroscopy journal December 2022
Anisotropic atomic motions in structural analysis by low energy electron diffraction journal January 1993
Direct Observation of Surface Chemistry Using Ultrafast Soft-X-Ray Pulses journal June 2001
Real-Time Observation of Nonadiabatic Surface Dynamics: The First Picosecond in the Dissociation of NO on Iridium journal November 2006
Real-Space Observation of Molecular Motion Induced by Femtosecond Laser Pulses journal July 2004
Real-Time Observation of Molecular Motion on a Surface journal December 2005
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