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Characteristics of chemical bonding of pentavalent uranium in La-doped UO2
Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and Condensed Matter Physics.
European Synchrotron, CS40220, F-38043 Grenoble 9, France.;HZDR, Inst Resource Ecol, POB 510119, D-01314 Dresden, Germany..
European Commiss, Inst Transuranium Elements, Joint Res Ctr, POB 2340, D-76125 Karlsruhe, Germany..
Univ Lille, CNRS, Cent Lille,ENSL, Univ Artois,UMR 8181,UCCS,Unite Catalyse & Chim S, F-59000 Lille, France..
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2017 (English)In: Chemical Communications, ISSN 1359-7345, E-ISSN 1364-548X, Vol. 53, no 1, p. 115-118Article in journal (Refereed) Published
Abstract [en]

The effect of La doping on the electronic structure of U in UO2 was studied using an advanced technique, namely, X-ray absorption spectroscopy (XAS) in the high-energy-resolution fluorescence-detection (HERFD) mode, at the U 3d(3/2) (M-4) edge. Thanks to a significant reduction of the core-hole lifetime broadening and distinct chemical shifts of the HERFD-XAS lines, the U(v) formation as a result of La doping was identified. The isolated contribution of U(v) in the M-4 HERFD-XAS spectrum reveals the so-called charge-transfer satellites due to the U 5f-O 2p hybridization. The analysis of the experimental data within the framework of the Anderson impurity model (AIM) indicates a significant change in the characteristics and degree of covalency for the chemical bonding in the U(v) subsystem of UO2 as compared to undoped UO2, which is a Mott-Hubbard system. The results are also supported by AIM calculations of X-ray photoelectron and optical absorption data.

Place, publisher, year, edition, pages
2017. Vol. 53, no 1, p. 115-118
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Chemical Sciences
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URN: urn:nbn:se:uu:diva-315832DOI: 10.1039/c6cc07684jISI: 000391607100012OAI: oai:DiVA.org:uu-315832DiVA, id: diva2:1075993
Available from: 2017-02-21 Created: 2017-02-21 Last updated: 2017-11-29Bibliographically approved

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Butorin, Sergei. M.

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