Abstract
The uranium valence electronic structure in the prototypical undistorted perovskite KUO3 is reported on the basis of a comprehensive experimental study using multi-edge HERFD-XAS and relativistic quantum chemistry calculations based on density functional theory. Very good agreement is obtained between theory and experiments, including the confirmation of previously reported Laporte forbidden f-f transitions and X-ray photoelectron spectroscopic measurements. Many spectral features are clearly identified in the probed U-f, U-p and U-d states and the contribution of the O-p states in those features could be assessed. The octahedral crystal field strength, 10Dq, was found to be6.6 (1.5) eV and 6.9 (4) eV from experiment and calculations, respectively. Calculated electron binding energies down to U-4f states are alsoreported.
Highlights
Uranium compounds are usually associated with nuclear applications, such as nuclear fission for energy generation, but for many decades they triggered interest from more fundamental aspects
We are reporting here results of our study on the uranium valence electronic structure in KUO3 by means of multi-edge high energy resolution fluorescence detected X-ray absorption spectroscopy (HERFD-XAS) and state-of-the-art relativistic quantum chemistry calculations based on density functional theory (DFT)
Uranium L1- and L3-edge XANES measurements were performed at BM20 (The Rossendorf Beamline) (Matz et al, 1999; Scheinost et al, 2021) of the European Synchrotron Radiation Facility (ESRF) operating at an electron beam energy of 6 GeV, in Grenoble, France
Summary
Uranium compounds are usually associated with nuclear applications, such as nuclear fission for energy generation, but for many decades they triggered interest from more fundamental aspects. Experimental studies typically require dedicated laboratories, owing to the natural radioactivity of uranium, and, in addition, theoretical calculations are revealed to be extremely complicated because of comparable magnitudes of the crystal field, spin–orbit coupling and the electron–electron repulsion interactions. The influence of the latter effect can be significantly reduced by exploring pure pentavalent U(V) compounds. We are reporting here results of our study on the uranium valence electronic structure in KUO3 by means of multi-edge high energy resolution fluorescence detected X-ray absorption spectroscopy (HERFD-XAS) and state-of-the-art relativistic quantum chemistry calculations based on DFT
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