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Probing Chemical Bonding in Uranium Dioxide by Means of High-Resolution X-ray Absorption Spectroscopy

  • Author(s): Butorin, SM
  • Modin, A
  • Vegelius, JR
  • Kvashnina, KO
  • Shuh, DK
  • et al.
Abstract

© 2016 American Chemical Society. A systematic X-ray absorption study at the U 3d, 4d, and 4f edges of UO2 was performed, and the data were analyzed within framework of the Anderson impurity model. By applying the high-energy-resolution fluorescence-detection (HERFD) mode of X-ray absorption spectroscopy (XAS) at the U 3d3/2 edge and conducting the XAS measurements at the shallower U 4f levels, fine details of the XAS spectra were resolved resulting from reduced core-hole lifetime broadening. This multiedge study enabled a far more effective analysis of the electronic structure at the U sites and characterization of the chemical bonding and degree of the 5f localization in UO2. The results support the covalent character of UO2 and do not agree with the suggestions of rather ionic bonding in this compound as expressed in some publications.

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