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Anion-mediated electronic effects in reducible oxides: Tuning the valence band of ceria via fluorine doping
Charles Univ Prague, Fac Math & Phys, Dept Surface & Plasma Sci, V Holesovickach 2, Prague 18000 8, Czech Republic;Friedrich Alexander Univ Erlangen Nurnberg, Chair Interface Res & Catalysis, Egerlandstr 3, D-91058 Erlangen, Germany.
Charles Univ Prague, Fac Math & Phys, Dept Surface & Plasma Sci, V Holesovickach 2, Prague 18000 8, Czech Republic;Forschungszentrum Julich, Peter Grunberg Inst 6, D-52425 Julich, Germany.ORCID iD: 0000-0002-3035-012X
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry. Univ Bath, Dept Phys, Bath BA2 7AY, Avon, England.ORCID iD: 0000-0001-5902-4187
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.ORCID iD: 0000-0003-3570-0050
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2019 (English)In: Journal of Chemical Physics, ISSN 0021-9606, E-ISSN 1089-7690, Vol. 151, no 4, article id 044701Article in journal (Refereed) Published
Abstract [en]

Combining experimental spectroscopy and hybrid density functional theory calculations, we show that the incorporation of fluoride ions into a prototypical reducible oxide surface, namely, ceria(111), can induce a variety of nontrivial changes to the local electronic structure, beyond the expected increase in the number of Ce3+ ions. Our resonant photoemission spectroscopy results reveal new states above, within, and below the valence band, which are unique to the presence of fluoride ions at the surface. With the help of hybrid density functional calculations, we show that the different states arise from fluoride ions in different atomic layers in the near surface region. In particular, we identify a structure in which a fluoride ion substitutes for an oxygen ion at the surface, with a second fluoride ion on top of a surface Ce4+ ion giving rise to F 2p states which overlap the top of the O 2p band. The nature of this adsorbate F--Ce4+ resonant enhancement feature suggests that this bond is at least partially covalent. Our results demonstrate the versatility of anion doping as a potential means of tuning the valence band electronic structure of ceria.

Place, publisher, year, edition, pages
2019. Vol. 151, no 4, article id 044701
National Category
Theoretical Chemistry Condensed Matter Physics
Identifiers
URN: urn:nbn:se:uu:diva-393127DOI: 10.1063/1.5109955ISI: 000478625700040PubMedID: 31370552OAI: oai:DiVA.org:uu-393127DiVA, id: diva2:1353973
Funder
Swedish Research CouncileSSENCE - An eScience Collaboration
Note

M. Kettner, T. Duchoň, and M. J. Wolf contributed equally to this work.

Available from: 2019-09-24 Created: 2019-09-24 Last updated: 2019-09-24Bibliographically approved

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Wolf, Matthew J.Kullgren, JollaHermansson, Kersti

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