TY  - JOUR
AU  - Marino, Andrea
AU  - Christovam, Denise S.
AU  - Takegami, Daisuke
AU  - Falke, Johannes
AU  - Carvalho, Miguel M. F.
AU  - Okauchi, Takaki
AU  - Chang, Chun-Fu
AU  - Altendorf, Simone G.
AU  - Amorese, Andrea
AU  - Sundermann, Martin
AU  - Gloskovskii, Andrei
AU  - Gretarsson, Hlynur
AU  - Keimer, Bernhard
AU  - Andreev, Alexandr V.
AU  - Havela, Ladislav
AU  - Leithe-Jasper, Andreas
AU  - Severing, Andrea
AU  - Kuneš, Jan
AU  - Tjeng, Liu Hao
AU  - Hariki, Atsushi
TI  - Quantifying the U 5f covalence and degree of localization in U intermetallics
JO  - Physical review research
VL  - 6
IS  - 3
SN  - 2643-1564
CY  - College Park, MD
PB  - APS
M1  - PUBDB-2024-05102
SP  - 033068
PY  - 2024
AB  - A procedure for quantifying the U 5⁢𝑓 electronic covalency and degree of localization in U intermetallic compounds is presented. To this end, bulk sensitive hard and soft x-ray photoelectron spectroscopy were utilized in combination with density-functional theory (DFT) plus dynamical mean-field theory (DMFT) calculations. The energy dependence of the photoionization cross sections allows the disentanglement of the U 5⁢𝑓 contribution to the valence band from the various other atomic subshells so the computational parameters in the DFT+DMFT can be reliably determined. Applying this method to UGa<sub>2</sub> and UB<sub>2</sub>  as model compounds from opposite ends of the (de)localization range, we have achieved excellent simulations of the valence band and core-level spectra. The width in the distribution of atomic U 5⁢𝑓 configurations contributing to the ground state, as obtained from the calculations, quantifies the correlated nature and degree of localization of the U 5⁢𝑓. The findings permit answering the longstanding question why different spectroscopic techniques give seemingly different numbers for the U 5⁢𝑓 valence in intermetallic U compounds. 
LB  - PUB:(DE-HGF)16
UR  - <Go to ISI:>//WOS:001270715500006
DO  - DOI:10.1103/PhysRevResearch.6.033068
UR  - https://bib-pubdb1.desy.de/record/611888
ER  -