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@ARTICLE{Kettner:864241,
author = {Kettner, Miroslav and Duchoň, Tomáš and Wolf, Matthew J.
and Kullgren, Jolla and Senanayake, Sanjaya D. and
Hermansson, Kersti and Veltruská, Kateřina and Nehasil,
Václav},
title = {{A}nion-mediated electronic effects in reducible oxides:
{T}uning the valence band of ceria via fluorine doping},
journal = {The journal of chemical physics},
volume = {151},
number = {4},
issn = {1089-7690},
address = {Melville, NY},
publisher = {American Institute of Physics},
reportid = {FZJ-2019-04075},
pages = {044701 -},
year = {2019},
abstract = {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},
cin = {PGI-6},
ddc = {530},
cid = {I:(DE-Juel1)PGI-6-20110106},
pnm = {522 - Controlling Spin-Based Phenomena (POF3-522)},
pid = {G:(DE-HGF)POF3-522},
typ = {PUB:(DE-HGF)16},
pubmed = {pmid:31370552},
UT = {WOS:000478625700040},
doi = {10.1063/1.5109955},
url = {https://juser.fz-juelich.de/record/864241},
}