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Time-resolved observation of transient precursor state of CO on Ru(0001) using carbon K-edge spectroscopy
Stockholm University, Faculty of Science, Department of Physics.ORCID iD: 0000-0002-6379-9759
Stockholm University, Faculty of Science, Department of Physics.
Stockholm University, Faculty of Science, Department of Physics.
Stockholm University, Faculty of Science, Department of Physics.ORCID iD: 0000-0002-0123-631X
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2019 (English)In: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084Article in journal (Refereed) Epub ahead of print
Abstract [en]

The transient dynamics of carbon monoxide (CO) molecules on a Ru(0001) surface following femtosecond optical laser pump excitation has been studied by monitoring changes in the unoccupied electronic structure using an ultrafast X-ray free-electron laser (FEL) probe. The particular symmetry of perpendicularly chemisorbed CO on the surface is exploited to investigate how the molecular orientation changes with time by varying the polarization of the FEL pulses. The time evolution of spectral features corresponding to the desorption precursor state was well distinguished due to the narrow line-width of the C K-edge in the X-ray absorption (XA) spectrum, illustrating that CO molecules in the precursor state rotated freely and resided on the surface for several picoseconds. Most of the CO molecules trapped in the precursor state ultimately cooled back down to the chemisorbed state, while we estimate that ∼14.5 ± 4.9% of the molecules in the precursor state desorbed into the gas phase. It was also observed that chemisorbed CO molecules diffused over the metal surface from on-top sites toward highly coordinated sites. In addition, a new “vibrationally hot precursor” state was identified in the polarization-dependent XA spectra.

Place, publisher, year, edition, pages
2019.
National Category
Atom and Molecular Physics and Optics
Research subject
Theoretical Physics
Identifiers
URN: urn:nbn:se:su:diva-174692DOI: 10.1039/C9CP03677FOAI: oai:DiVA.org:su-174692DiVA, id: diva2:1359202
Available from: 2019-10-08 Created: 2019-10-08 Last updated: 2019-10-09
In thesis
1. Le Fantôme de l’Opéra - Studies on Atoms and Electrons Beneath
Open this publication in new window or tab >>Le Fantôme de l’Opéra - Studies on Atoms and Electrons Beneath
2019 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

The carbon dioxide reduction reaction is a promising candidate to tackle ecological challenges of our age. This is due to its capability of reducing carbon dioxide emission generated from the combustion of fossil fuels by converting carbon dioxide into valuable hydrocarbons. Oxide-derived metal nanostructures have been found to exhibit unique catalytic characteristics for facilitating the carbon dioxide reduction reaction. In this thesis work, the stability, influence, and effects of subsurface oxygen atoms are investigated by theoretical computations with various levels of theory and models. It is found that subsurface oxygen atoms are stable and that their presence increases the CO adsorption strength and coverage on oxide-derived Cu surface. This is explained by a reduced σ-repulsion and leads to the breaking of scaling relations. Although it does not directly reduce the CO dimerization barrier, the adsorption of H atoms is inhibited thus steering the selectivity. The presence of subsurface oxygen atoms is also concluded from a joint work with experimental and theoretical efforts of X-ray photoelectron spectroscopy. The precursor region of CO desorption from Ru(0001) is studied with the transition potential method. In contrast, for the simulation of the X-ray spectroscopy results on p4g C/Ni(100), which is a surface reconstruction when carbon atoms adsorb on Ni(100), vibrational effects are also needed for understanding the experimental data.

Place, publisher, year, edition, pages
Stockholm: Department of Physics, Stockholm University, 2019. p. 75
Keywords
Carbon dioxide reduction, Subsurface oxygen, X-ray spectroscopy, Density functional theory, CO desorption
National Category
Atom and Molecular Physics and Optics
Research subject
Theoretical Physics
Identifiers
urn:nbn:se:su:diva-174700 (URN)978-91-7797-863-3 (ISBN)978-91-7797-864-0 (ISBN)
Public defence
2019-11-22, sal FA32, AlbaNova universitetscentrum, Roslagstullsbacken 21, Stockholm, 13:00 (English)
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Available from: 2019-10-30 Created: 2019-10-08 Last updated: 2019-10-21Bibliographically approved

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Wang, Hsin-YiWeston, MatthewLiu, ChangPerakis, FivosDell’Angela, MartinaCavalca, FilippoLiu, BoyangGladh, JörgenKoroidov, SergeyCostantini, RobertoPettersson, Lars G. M.Nilsson, Anders
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