% IMPORTANT: The following is UTF-8 encoded. This means that in the presence
% of non-ASCII characters, it will not work with BibTeX 0.99 or older.
% Instead, you should use an up-to-date BibTeX implementation like “bibtex8” or
% “biber”.
@ARTICLE{Murphy:1029087,
author = {Murphy, Gabriel L. and Bazarkina, Elena and Svitlyk,
Volodymyr and Rossberg, André and Potts, Shannon and
Hennig, Christoph and Henkes, Maximilian and Kvashnina,
Kristina O. and Huittinen, Nina},
title = {{P}robing the {L}ong- and {S}hort-{R}ange {S}tructural
{C}hemistry in the {C}-{T}ype {B}ixbyite {O}xides {T}h 0.40
{N}d 0.48 {C}e 0.12 {O} 1.76 , {T}h 0.47 {N}d 0.43 {C}e 0.10
{O} 1.785 , and {T}h 0.45 {N}d 0.37 {C}e 0.18 {O} 1.815 via
{S}ynchrotron {X}-ray {D}iffraction and {A}bsorption
{S}pectroscopy},
journal = {ACS omega},
volume = {9},
number = {25},
issn = {2470-1343},
address = {Washington, DC},
publisher = {ACS Publications},
reportid = {FZJ-2024-04948},
pages = {27397 - 27406},
year = {2024},
abstract = {The long- and short-range structural chemistry of the
C-type bixbyite compounds Th0.40Nd0.48Ce0.12O1.76,
Th0.47Nd0.43Ce0.10O1.785, and Th0.45Nd0.37Ce0.18O1.815 is
systematically examined using synchrotron X-ray powder
diffraction (S-PXRD), high-energy resolution fluorescence
detection X-ray absorption near edge (HERFD-XANES), and
extended X-ray absorption fine structure spectroscopy
(EXAFS) measurements supported by electronic structure
calculations. S-PXRD measurements revealed that the title
compounds all form classical C-type bixbyite structures in
space group Ia3̅ that have disordered cationic
crystallographic sites with further observation of
characteristic superlattice reflections corresponding to
oxygen vacancies. Despite the occurrence of oxygen
vacancies, HERFD-XANES measurements on the Ce L3-edge
revealed that Ce incorporates as Ce4+ into the structures
but involves local distortion that resembles cluster
behavior and loss of nearest-neighbors. In comparison,
HERFD-XANES measurements on the Nd L3-edge supported by
electronic structure calculations reveal that Nd3+ adopts a
local coordination environment similar to the long-range
C-type structure while providing charge balancing for the
formation of oxygen defects. Th L3-edge EXAFS analysis
reveals shorter average Th–O distances in the title
compounds in comparison to pristine ThO2 in addition to
shorter Th–O and Th–Ce distances compared to Th–Th or
Ce–Ce in the corresponding F-type binary oxides (ThO2 and
CeO2). These distances are further found to decrease with
the increased Nd content of the structures despite
simultaneous observation of the overall lattice structure
progressively expanding. Linear combination calculations of
the M-O bond lengths are used to help explain these
observations, where the role of oxygen defects, via Nd3+
incorporation, induces local bond contraction and enhanced
Th cation valence, leading to the observed increased lattice
expansion with progressive Nd3+ incorporation. Overall, the
investigation points to the significance of dissimilar
cations exhibiting variable short-range chemical behavior
and how it can affect the long-range structural chemistry of
complex oxides.},
cin = {IFN-2},
ddc = {660},
cid = {I:(DE-Juel1)IFN-2-20101013},
pnm = {1411 - Nuclear Waste Disposal (POF4-141) / BMBF 02NUK060B -
Verbundprojekt AcE: Grundlegende Untersuchungen zur
Immobilisierung von Actiniden mittels Einbau in
endlagerrelevante Festphasen, Teilprojekt B (02NUK060B)},
pid = {G:(DE-HGF)POF4-1411 / G:(BMBF)02NUK060B},
typ = {PUB:(DE-HGF)16},
pubmed = {38947849},
UT = {WOS:001246074900001},
doi = {10.1021/acsomega.4c02200},
url = {https://juser.fz-juelich.de/record/1029087},
}