Atom-specific activation in CO oxidation

Schreck, Simon; Diesen, Elias; LaRue, Jerry; Ogasawara, Hirohito; Marks, Kess; Nordlund, Dennis; Weston, Matthew; Beye, Martin; Cavalca, Filippo; Perakis, Fivos; Sellberg, Jonas; Eilert, André; Kim, Kyung Hwan; Coslovich, Giacomo; Coffee, Ryan; Krzywinski, Jacek; Reid, Alex; Moeller, Stefan; Lutman, Alberto; Öström, Henrik; Pettersson, Lars G. M.; Nilsson, Anders

doi:10.1063/1.5044579

Title: Atom-specific activation in CO oxidation

Abstract

Here, we report on atom-specific activation of CO oxidation on Ru(0001) via resonant X-ray excitation. We show that resonant 1s core-level excitation of atomically adsorbed oxygen in the co-adsorbed phase of CO and oxygen directly drives CO oxidation. We separate this direct resonant channel from indirectly driven oxidation via X-ray induced substrate heating. Based on density functional theory calculations, we identify the valence-excited state created by the Auger decay as the driving electronic state for direct CO oxidation. We utilized the fresh-slice multi-pulse mode at the Linac Coherent Light Source that provided time-overlapped and 30 fs delayed pairs of soft X-ray pulses and discuss the prospects of femtosecond X-ray pump X-ray spectroscopy probe, as well as X-ray two-pulse correlation measurements for fundamental investigations of chemical reactions via selective X-ray excitation.

Authors:

Schreck, Simon ^[1]; Diesen, Elias ^[1];

^[2];

^[3];

^[1]; Nordlund, Dennis ^[3]; Weston, Matthew ^[1];

^[4]; Cavalca, Filippo ^[1];

^[1];

^[5]; Eilert, André ^[1]; Kim, Kyung Hwan ^[1]; Coslovich, Giacomo ^[3];

^[3]; Krzywinski, Jacek ^[3];

^[3];

^[3]; Lutman, Alberto ^[3]; Öström, Henrik ^[1] more »

Stockholm Univ., Stockholm (Sweden)
Chapman Univ., Orange, CA (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)
KTH Royal Institute of Technology, Stockholm (Sweden)

Publication Date:: Fri Dec 21 00:00:00 EST 2018

Research Org.:: SLAC National Accelerator Lab., Menlo Park, CA (United States)

Sponsoring Org.:: USDOE

OSTI Identifier:: 1493421

Grant/Contract Number:: AC02-76SF00515

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Chemical Physics

Additional Journal Information:: Journal Volume: 149; Journal Issue: 23; Journal ID: ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)

Country of Publication:: United States

Language:: English

Subject:: 74 ATOMIC AND MOLECULAR PHYSICS

Citation Formats


                    Schreck, Simon, Diesen, Elias, LaRue, Jerry, Ogasawara, Hirohito, Marks, Kess, Nordlund, Dennis, Weston, Matthew, Beye, Martin, Cavalca, Filippo, Perakis, Fivos, Sellberg, Jonas, Eilert, André, Kim, Kyung Hwan, Coslovich, Giacomo, Coffee, Ryan, Krzywinski, Jacek, Reid, Alex, Moeller, Stefan, Lutman, Alberto, Öström, Henrik, Pettersson, Lars G. M., and Nilsson, Anders. Atom-specific activation in CO oxidation.  United States: N. p., 2018. 
Web.  doi:10.1063/1.5044579.

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                    Schreck, Simon, Diesen, Elias, LaRue, Jerry, Ogasawara, Hirohito, Marks, Kess, Nordlund, Dennis, Weston, Matthew, Beye, Martin, Cavalca, Filippo, Perakis, Fivos, Sellberg, Jonas, Eilert, André, Kim, Kyung Hwan, Coslovich, Giacomo, Coffee, Ryan, Krzywinski, Jacek, Reid, Alex, Moeller, Stefan, Lutman, Alberto, Öström, Henrik, Pettersson, Lars G. M., & Nilsson, Anders. Atom-specific activation in CO oxidation.  United States.  https://doi.org/10.1063/1.5044579

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                    Schreck, Simon, Diesen, Elias, LaRue, Jerry, Ogasawara, Hirohito, Marks, Kess, Nordlund, Dennis, Weston, Matthew, Beye, Martin, Cavalca, Filippo, Perakis, Fivos, Sellberg, Jonas, Eilert, André, Kim, Kyung Hwan, Coslovich, Giacomo, Coffee, Ryan, Krzywinski, Jacek, Reid, Alex, Moeller, Stefan, Lutman, Alberto, Öström, Henrik, Pettersson, Lars G. M., and Nilsson, Anders. Fri .  
"Atom-specific activation in CO oxidation".  United States.  https://doi.org/10.1063/1.5044579.  https://www.osti.gov/servlets/purl/1493421.

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@article{osti_1493421,

  title        = {Atom-specific activation in CO oxidation},

  author       = {Schreck, Simon and Diesen, Elias and LaRue, Jerry and Ogasawara, Hirohito and Marks, Kess and Nordlund, Dennis and Weston, Matthew and Beye, Martin and Cavalca, Filippo and Perakis, Fivos and Sellberg, Jonas and Eilert, André and Kim, Kyung Hwan and Coslovich, Giacomo and Coffee, Ryan and Krzywinski, Jacek and Reid, Alex and Moeller, Stefan and Lutman, Alberto and Öström, Henrik and Pettersson, Lars G. M. and Nilsson, Anders},

  abstractNote = {Here, we report on atom-specific activation of CO oxidation on Ru(0001) via resonant X-ray excitation. We show that resonant 1s core-level excitation of atomically adsorbed oxygen in the co-adsorbed phase of CO and oxygen directly drives CO oxidation. We separate this direct resonant channel from indirectly driven oxidation via X-ray induced substrate heating. Based on density functional theory calculations, we identify the valence-excited state created by the Auger decay as the driving electronic state for direct CO oxidation. We utilized the fresh-slice multi-pulse mode at the Linac Coherent Light Source that provided time-overlapped and 30 fs delayed pairs of soft X-ray pulses and discuss the prospects of femtosecond X-ray pump X-ray spectroscopy probe, as well as X-ray two-pulse correlation measurements for fundamental investigations of chemical reactions via selective X-ray excitation.},

  doi          = {10.1063/1.5044579},

  journal      = {Journal of Chemical Physics},

  number       = 23,

  volume       = 149,

  place        = {United States},

  year         = {Fri Dec 21 00:00:00 EST 2018},

  month        = {Fri Dec 21 00:00:00 EST 2018}

}

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Title: Atom-specific activation in CO oxidation

Abstract

Citation Formats

Chemical Bond Activation Observed with an X-ray Laser journal, September 2016

Ion Desorption by Core-Hole Auger Decay journal, April 1978

Field desorption and field evaporation of metals journal, October 1996

Dynamics of nonthermal reactions: femtosecond surface chemistry journal, January 1993

From the Sabatier principle to a predictive theory of transition-metal heterogeneous catalysis journal, August 2015

Interaction of slow Electrons with Chemisorbed Oxygen journal, May 1964

Universality in Heterogeneous Catalysis journal, July 2002

Electronically induced surface reactions: Evolution, concepts, and perspectives journal, September 2012

Integral properties of channel interference in resonant X-ray scattering journal, February 1996

Real-Time Observation of Adsorbate Atom Motion Above a Metal Surface journal, May 2000

Few-femtosecond time-resolved measurements of X-ray free-electron lasers journal, April 2014

Photochemistry at adsorbate/metal interfaces journal, January 1991

Electronic structure calculations with GPAW: a real-space implementation of the projector augmented-wave method journal, June 2010

Space-Charge Effects in Field Emission journal, October 1953

Femtochemistry at Metal Surfaces: Nonadiabatic Reaction Dynamics journal, October 2006

Theoretical approximations to X-ray absorption spectroscopy of liquid water and ice journal, March 2010

S URFACE F EMTOCHEMISTRY : Observation and Quantum Control of Frustrated Desorption of Alkali Atoms from Noble Metals journal, October 2002

Femtosecond dynamics of electronic excitations of adsorbates studied by two-photon photoemission pulse correlation: CO/Cu(111) journal, July 1995

Probing the transition state region in catalytic CO oxidation on Ru journal, February 2015

The Brønsted–Evans–Polanyi relation and the volcano curve in heterogeneous catalysis journal, May 2004

Photoexcitation of adsorbates on metal surfaces: One-step or three-step journal, September 2012

Phonon- Versus Electron-Mediated Desorption and Oxidation of CO on Ru(0001) journal, August 1999

Real-Time Observation of Surface Bond Breaking with an X-ray Laser journal, March 2013

Lifetimes of electronically excited states of molecules on oxide versus metal surfaces journal, February 1993

Interaction of Water Molecule with Au(111) and Au(110) Surfaces under the Influence of an External Electric Field journal, February 2014

Thirty years of MGR: How it came about, and what came of it journal, June 1995

Understanding Trends in Catalytic Activity: The Effect of Adsorbate–Adsorbate Interactions for CO Oxidation Over Transition Metals journal, February 2010

Fresh-slice multicolour X-ray free-electron lasers journal, October 2016

Core-hole decay studies of O/Ni(100) c (2×2) journal, October 1993

High-resolution auger spectra of adsorbates journal, January 1982

On the origin of core-level binding energy shifts journal, December 1995

X-Ray Interactions: Photoabsorption, Scattering, Transmission, and Reflection at E = 50-30,000 eV, Z = 1-92 journal, July 1993

Control of chemical reactions by core excitations journal, August 2001

Desorption from Metal Surfaces by Low‐Energy Electrons journal, December 1964

Femtosecond dynamics of chemical reactions at surfaces journal, November 2000

Catalysis in real time using X-ray lasers journal, May 2017

Adsorbate-Localized Excitation in Surface Photochemistry: Methane on Pt(111) journal, March 1996

Photon-Stimulated Desorption due to Multielectron Excitations in Chemisorbed Molecules: CO on Ni(100) journal, November 1981

Δ self-consistent field method to obtain potential energy surfaces of excited molecules on surfaces journal, August 2008

Space charge limited electron emission from a Cu surface under ultrashort pulsed laser irradiation journal, February 2010

Direct observation of electron dynamics in the attosecond domain journal, July 2005

Vacuum space charge effects in sub-picosecond soft X-ray photoemission on a molecular adsorbate layer journal, March 2015

Detailed study of pyridine at the C 1 s and N 1 s ionization thresholds: The influence of the vibrational fine structure journal, October 2001

Observation of Neutral Atomic Fragments for Specific 1 s Core Excitations of an Adsorbed Molecule journal, March 1998

High-intensity double-pulse X-ray free-electron laser journal, March 2015

Desorption from Surfaces by Slow‐Electron Impact journal, February 1964

Indication of non-thermal contribution to visible femtosecond laser-induced CO oxidation on Ru(0001) journal, August 2015

Space charge limited electron emission from a Cu surface under ultrashort pulsed laser irradiation conference, January 2010

Chemical Bond Activation Observed with an X-ray Laser text, January 2016

Delta Self-Consistent Field as a method to obtain potential energy surfaces of excited molecules on surfaces text, January 2008

Chemical Bond Activation Observed with an X-ray Laser
journal, September 2016

Ion Desorption by Core-Hole Auger Decay
journal, April 1978

Field desorption and field evaporation of metals
journal, October 1996

Dynamics of nonthermal reactions: femtosecond surface chemistry
journal, January 1993

From the Sabatier principle to a predictive theory of transition-metal heterogeneous catalysis
journal, August 2015

Interaction of slow Electrons with Chemisorbed Oxygen
journal, May 1964

Universality in Heterogeneous Catalysis
journal, July 2002

Electronically induced surface reactions: Evolution, concepts, and perspectives
journal, September 2012

Integral properties of channel interference in resonant X-ray scattering
journal, February 1996

Real-Time Observation of Adsorbate Atom Motion Above a Metal Surface
journal, May 2000

Few-femtosecond time-resolved measurements of X-ray free-electron lasers
journal, April 2014

Photochemistry at adsorbate/metal interfaces
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