Quantifying the U 5f covalence and degree of localization in U intermetallics

Research output: Contribution to journalResearch articleContributedpeer-review

Contributors

  • Andrea Marino - , Faculty of Physics, Max Planck Institute for Chemical Physics of Solids, TUD Dresden University of Technology, Stellbrink and Partner Patentanwälte MbB (Author)
  • Denise S. Christovam - , Max Planck Institute for Chemical Physics of Solids (Author)
  • Daisuke Takegami - , Max Planck Institute for Chemical Physics of Solids, Waseda University (Author)
  • Johannes Falke - , Max Planck Institute for Chemical Physics of Solids (Author)
  • Miguel M.F. Carvalho - , Max Planck Institute for Chemical Physics of Solids, University of Cologne (Author)
  • Takaki Okauchi - , Osaka Metropolitan University (Author)
  • Chun Fu Chang - , Max Planck Institute for Chemical Physics of Solids (Author)
  • Simone G. Altendorf - , Max Planck Institute for Chemical Physics of Solids (Author)
  • Andrea Amorese - , Max Planck Institute for Chemical Physics of Solids, University of Cologne, ASML Netherlands BV (Author)
  • Martin Sundermann - , Max Planck Institute for Chemical Physics of Solids, German Electron Synchrotron (DESY) (Author)
  • Andrei Gloskovskii - , German Electron Synchrotron (DESY) (Author)
  • Hlynur Gretarsson - , German Electron Synchrotron (DESY), Max Planck Institute for Solid State Research (Author)
  • Bernhard Keimer - , Max Planck Institute for Solid State Research (Author)
  • Alexandr V. Andreev - , Czech Academy of Sciences (Author)
  • Ladislav Havela - , Charles University Prague (Author)
  • Andreas Leithe-Jasper - , Max Planck Institute for Chemical Physics of Solids (Author)
  • Andrea Severing - , Max Planck Institute for Chemical Physics of Solids, University of Cologne (Author)
  • Jan Kuneš - , Masaryk University (Author)
  • Liu Hao Tjeng - , Max Planck Institute for Chemical Physics of Solids (Author)
  • Atsushi Hariki - , Osaka Metropolitan University (Author)

Abstract

A procedure for quantifying the U 5f 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 5f 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 UGa2 and UB2 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.

Details

Original languageEnglish
Article number033068
JournalPhysical Review Research
Volume6
Issue number3
Publication statusPublished - Jun 2024
Peer-reviewedYes

Keywords

ASJC Scopus subject areas