Symmetry-resolved CO desorption and oxidation dynamics on O/Ru(0001) probed at the C K-edge by ultrafast X-ray spectroscopy

LaRue, Jerry; Liu, Boyang; Rodrigues, Gabriel L. S.; Liu, Chang; Garrido Torres, José A.; Schreck, Simon; Diesen, Elias; Weston, Matthew; Ogasawara, Hirohito; Perakis, Fivos; Dell'Angela, Martina; Capotondi, Flavio; Ball, Devon; Carnahan, Conner; Zeri, Gary; Giannessi, Luca; Pedersoli, Emanuele; Naumenko, Denys; Amann, Peter; Nikolov, Ivaylo; Raimondi, Lorenzo; Spezzani, Carlo; Beye, Martin; Voss, Johannes; Wang, Hsin-Yi; Cavalca, Filippo; Gladh, Jörgen; Koroidov, Sergey; Abild-Pedersen, Frank; Kolb, Manuel; Miedema, Piter S.; Costantini, Roberto; Heinz, Tony; Luntz, Alan; Pettersson, Lars G. M.; Nilsson, Anders

doi:10.1063/5.0114399

Title: Symmetry-resolved CO desorption and oxidation dynamics on O/Ru(0001) probed at the C K-edge by ultrafast X-ray spectroscopy

Journal Article · Thu Sep 29 00:00:00 EDT 2022 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/5.0114399· OSTI ID:1890467

^[1]; Liu, Boyang ^[2];

^[3]; Liu, Chang ^[2]; Garrido Torres, José A. ^[4]; Schreck, Simon ^[2];

^[5]; Weston, Matthew ^[2];

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^[7]; Capotondi, Flavio ^[8]; Ball, Devon ^[1]; Carnahan, Conner ^[1]; Zeri, Gary ^[1];

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^[2]; Nikolov, Ivaylo ^[9] more »

Chapman Univ., Orange, CA (United States)
Stockholm Univ. (Sweden)
KTH Royal Inst. of Technology, Stockholm (Sweden)
Columbia Univ., New York, NY (United States)
Stanford Univ., CA (United States). SUNCAT Center for Interface Science and Catalysis
SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
National Research Council (CNR), Trieste (Italy). Inst. of Materials (CNR-IOM)
National Research Council (CNR), Lecce (Italy). National Inst. for the Physics of Matter (INFM), National Lab. TASC
Elettra-Sincrotrone Trieste (Italy)
Consiglio Nazionale delle Ricerche (CNR), Rome (Italy). Istituto di Struttura della Materia (CNR-ISM)
Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Leiden Univ. (Netherlands)
National Research Council (CNR), Rome (Italy)
Stanford Univ., CA (United States)

In this work, we report on carbon monoxide desorption and oxidation induced by 400 nm femtosecond laser excitation on the O/Ru(0001) surface probed by time-resolved X-ray absorption spectroscopy (TR-XAS) at the carbon K-edge. The experiments were performed under constant background pressures of CO (6x10^-8 Torr) and O₂ (3x10^-8 Torr). Under these conditions, we detect two transient CO species with narrow 2π* peaks, suggesting little 2π* interaction with the surface. Based on polarization measurements, we find that these two species have opposing orientations: (1) CO favoring a more perpendicular orientation and (2) CO favoring a more parallel orientation with respect to the surface. We also directly detect gas-phase CO₂ using a mass spectrometer and observe weak signatures of bent adsorbed CO₂ at slightly higher X-ray energies than the 2π* region. These results are compared to previously reported TR-XAS results at the O K-edge where the CO background pressure was three times lower (2x10^-8 Torr) while maintaining the same O₂ pressure. At the lower CO pressure, in the CO 2π* region, we observed adsorbed CO and a distribution of OC-O bond lengths close to the CO oxidation transition state, with little indication of gas-like CO. The shift towards 'gas-like' CO species may be explained by the higher CO exposure, which blocks O adsorption, decreasing O coverage and increasing CO coverage. These effects decrease the CO desorption barrier through dipole-dipole interaction, while simultaneously increasing the CO oxidation barrier.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; Knut and Alice Wallenberg Foundation; Swedish Research Council (SRC); Helmholtz Association; SIR Foundation; USDOE

Contributing Organization:: SUNCAT

Grant/Contract Number:: AC02-76SF00515; AC02-05CH11231; FWP 100435; 2016.0042; 2013-8823; VH-NG-1005; Nr RBSI14G7TL; CUP B82I15000910001

OSTI ID:: 1890467

Alternate ID(s):: OSTI ID: 1894521

Journal Information:: Journal of Chemical Physics, Vol. 157, Issue 16; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
x-ray absorption spectroscopy
femtosecond lasers
surface and interface chemistry
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oxidation
x-ray spectroscopy
carbon monoxide
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Title: Symmetry-resolved CO desorption and oxidation dynamics on O/Ru(0001) probed at the C K-edge by ultrafast X-ray spectroscopy

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