KIT | KIT-Bibliothek | Impressum | Datenschutz

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 UCx (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 M4 and L3 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 UC2. While the U M4HERFD-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 M4 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 UC2, 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.

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

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
Seitenaufrufe: 47
seit 20.12.2023
Downloads: 32
seit 23.01.2024
Cover der Publikation
KIT – Die Forschungsuniversität in der Helmholtz-Gemeinschaft
KITopen Landing Page