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

Autor: LaRue J; Schmid College of Science and Technology, Chapman University, Orange, California 92866, USA., Liu B; Department of Physics, AlbaNova University Center, Stockholm University, SE-10691 Stockholm, Sweden., Rodrigues GLS; Department of Physics, AlbaNova University Center, Stockholm University, SE-10691 Stockholm, Sweden., Liu C; Department of Physics, AlbaNova University Center, Stockholm University, SE-10691 Stockholm, Sweden., Garrido Torres JA; SLAC National Accelerator Laboratory, SUNCAT Center for Interface Science and Catalysis, 2575 Sand Hill Road, Menlo Park, California 94025, USA., Schreck S; Department of Physics, AlbaNova University Center, Stockholm University, SE-10691 Stockholm, Sweden., Diesen E; SLAC National Accelerator Laboratory, SUNCAT Center for Interface Science and Catalysis, 2575 Sand Hill Road, Menlo Park, California 94025, USA., Weston M; Department of Physics, AlbaNova University Center, Stockholm University, SE-10691 Stockholm, Sweden., Ogasawara H; SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, USA., Perakis F; Department of Physics, AlbaNova University Center, Stockholm University, SE-10691 Stockholm, Sweden., Dell'Angela M; CNR-IOM, SS 14-km 163.5, 34149 Basovizza, Trieste, Italy., Capotondi F; FERMI, Elettra-Sincrotrone Trieste, SS 14-km 163.5, 34149 Basovizza, Trieste, Italy., Ball D; Schmid College of Science and Technology, Chapman University, Orange, California 92866, USA., Carnahan C; Schmid College of Science and Technology, Chapman University, Orange, California 92866, USA., Zeri G; Schmid College of Science and Technology, Chapman University, Orange, California 92866, USA., Giannessi L; FERMI, Elettra-Sincrotrone Trieste, SS 14-km 163.5, 34149 Basovizza, Trieste, Italy., Pedersoli E; FERMI, Elettra-Sincrotrone Trieste, SS 14-km 163.5, 34149 Basovizza, Trieste, Italy., Naumenko D; FERMI, Elettra-Sincrotrone Trieste, SS 14-km 163.5, 34149 Basovizza, Trieste, Italy., Amann P; Scienta Omicron AB, Danmarksgatan 22, 75323 Uppsala, Sweden., Nikolov I; FERMI, Elettra-Sincrotrone Trieste, SS 14-km 163.5, 34149 Basovizza, Trieste, Italy., Raimondi L; FERMI, Elettra-Sincrotrone Trieste, SS 14-km 163.5, 34149 Basovizza, Trieste, Italy., Spezzani C; FERMI, Elettra-Sincrotrone Trieste, SS 14-km 163.5, 34149 Basovizza, Trieste, Italy., Beye M; Deutsches Elektronen-Synchrotron DESY, Notkestrasse 85, 22607 Hamburg, Germany., Voss J; SLAC National Accelerator Laboratory, SUNCAT Center for Interface Science and Catalysis, 2575 Sand Hill Road, Menlo Park, California 94025, USA., Wang HY; Department of Physics, AlbaNova University Center, Stockholm University, SE-10691 Stockholm, Sweden., Cavalca F; Department of Physics, AlbaNova University Center, Stockholm University, SE-10691 Stockholm, Sweden., Gladh J; SLAC National Accelerator Laboratory, SUNCAT Center for Interface Science and Catalysis, 2575 Sand Hill Road, Menlo Park, California 94025, USA., Koroidov S; Department of Physics, AlbaNova University Center, Stockholm University, SE-10691 Stockholm, Sweden., Abild-Pedersen F; SLAC National Accelerator Laboratory, SUNCAT Center for Interface Science and Catalysis, 2575 Sand Hill Road, Menlo Park, California 94025, USA., Kolb M; Department of Physics, AlbaNova University Center, Stockholm University, SE-10691 Stockholm, Sweden., Miedema PS; Deutsches Elektronen-Synchrotron DESY, Notkestrasse 85, 22607 Hamburg, Germany., Costantini R; CNR-IOM, SS 14-km 163.5, 34149 Basovizza, Trieste, Italy., Heinz TF; SLAC National Accelerator Laboratory, SUNCAT Center for Interface Science and Catalysis, 2575 Sand Hill Road, Menlo Park, California 94025, USA., Luntz AC; SLAC National Accelerator Laboratory, SUNCAT Center for Interface Science and Catalysis, 2575 Sand Hill Road, Menlo Park, California 94025, USA., Pettersson LGM; Department of Physics, AlbaNova University Center, Stockholm University, SE-10691 Stockholm, Sweden., Nilsson A; Department of Physics, AlbaNova University Center, Stockholm University, SE-10691 Stockholm, Sweden.
Jazyk: angličtina
Zdroj: The Journal of chemical physics [J Chem Phys] 2022 Oct 28; Vol. 157 (16), pp. 164705.
DOI: 10.1063/5.0114399
Abstrakt: 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 (6 × 10 -8 Torr) and O 2 (3 × 10 -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 CO 2 using a mass spectrometer and observe weak signatures of bent adsorbed CO 2 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 (2 × 10 -8 Torr) while maintaining the same O 2 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 toward "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.
Databáze: MEDLINE
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