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Effect of carbon content on electronic structure of uranium carbides

Butorin, Sergei M.; Bauters, Stephen; Amidani, Lucia; Beck, Aaron 1; Rossberg, André; Weiss, Stephan; Vitova, Tonya ORCID iD icon 1; Kvashnina, Kristina O.; Tougait, Olivier
1 Institut für Nukleare Entsorgung (INE), Karlsruher Institut für Technologie (KIT)

Abstract:

The electronic structure of UC$_x$ (x = 0.9, 1.0, 1.1, 2.0) was studied by means of x-ray absorption spectroscopy (XAS) at the C K edge and measurements in the high energy resolution fluorescence detection (HERFD) mode at the U M$_4$ and L$_3$ edges. The full-relativistic density functional theory calculations taking into account the Coulomb interaction U and spin-orbit coupling (DFT+U+SOC) were also performed for UC and UC$_2$. While the U M$_4$HERFD-XAS spectra of the studied samples reveal little difference, the U HERFD-XAS spectra show certain sensitivity to the varying carbon content in uranium carbides. The observed gradual changes in the U M$_4$ HERFD spectra suggest an increase in the C 2p-U 5f charge transfer, which is supported by the orbital population analysis in the DFT+U+SOC calculations, indicating an increase in the U 5f occupancy in UC as compared to that in UC. On the other hand, the density of states at the Fermi level were found to be significantly lower in UC$_2$, thus affecting the thermodynamic properties. Both the x-ray spectroscopic data (in particular, the C K XAS measurements) and results of the DFT+U+SOC calculations indicate the importance of taking into account U and SOC for the description of the electronic structure of actinide carbides.


Verlagsausgabe §
DOI: 10.5445/IR/1000165736
Veröffentlicht am 19.12.2023
Originalveröffentlichung
DOI: 10.1038/s41598-023-47579-7
Scopus
Zitationen: 1
Web of Science
Zitationen: 1
Dimensions
Zitationen: 1
Cover der Publikation
Zugehörige Institution(en) am KIT Institut für Nukleare Entsorgung (INE)
Publikationstyp Zeitschriftenaufsatz
Publikationsjahr 2023
Sprache Englisch
Identifikator ISSN: 2045-2322
KITopen-ID: 1000165736
HGF-Programm 32.11.03 (POF IV, LK 01) Fundamental Scientific Aspects
Erschienen in Scientific Reports
Verlag Nature Research
Band 13
Heft 1
Seiten Art-Nr.: 20434
Vorab online veröffentlicht am 22.11.2023
Nachgewiesen in Dimensions
Web of Science
Scopus
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