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

Journal Article · · Journal of Physical Chemistry. C
ORCiD logo [1];  [1];  [1];  [2];  [3]
  1. Uppsala Univ. (Sweden). Dept. of Physics and Astronomy
  2. European Synchrotron Radiation Facility (ESRF), Grenoble (France); Helmholtz-Zentrum Dresden-Rossendorf (HZDR), Inst. of Resource Ecology, Dresden (Germany)
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division
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Here, 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.

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division
Grant/Contract Number:
AC02-05CH11231
OSTI ID:
1436141
Journal Information:
Journal of Physical Chemistry. C, Vol. 120, Issue 51; ISSN 1932-7447
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 21 works
Citation information provided by
Web of Science

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Cited By (3)

Heteroleptic samarium( iii ) halide complexes probed by fluorescence-detected L 3 -edge X-ray absorption spectroscopy journal January 2018
A Novel Metastable Pentavalent Plutonium Solid Phase on the Pathway from Aqueous Plutonium(VI) to PuO 2 Nanoparticles journal December 2019
A Novel Metastable Pentavalent Plutonium Solid Phase on the Pathway from Aqueous Plutonium(VI) to PuO 2 Nanoparticles journal October 2019

Figures / Tables (5)

Figure 1(p. 5)figure Figure 1
Figure 2(p. 6)figure Figure 2
Table 1(p. 7)table Table 1
Figure 3(p. 8)figure Figure 3
Figure 4(p. 9)figure Figure 4

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