Quantifying the U 5f covalence and degree of localization in U intermetallics
Physical Review Research(2024)
摘要
A procedure for quantifying the U 5f electrons' covalence 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 5f contribution to the
valence band from the various other atomic subshells so that the computational
parameters in the DFT + DMFT can be reliably determined. Applying this method
to UGa_2 and UB_2 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 5f
configurations contributing to the ground state, as obtained from the
calculations, quantifies the correlated nature and degree of localization of
the U 5f. The findings permit answering the longstanding question why
different spectroscopic techniques give seemingly different numbers for the U
5f valence in intermetallic U compounds.
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