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

Abstract

Here, a systematic X-ray absorption study at the U 3d, 4d, and 4f edges of UO 2 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 3d 3/2 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 UO 2. The results support the covalent character of UO 2 and do not agree with the suggestions of rather ionic bonding in this compound as expressed in some publications.

Authors:
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
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division
OSTI Identifier:
1436141
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 120; Journal Issue: 51; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 47 OTHER INSTRUMENTATION

Citation Formats

Butorin, Sergei M., Modin, Anders, Vegelius, Johan R., Kvashnina, Kristina O., and Shuh, David K. Probing Chemical Bonding in Uranium Dioxide by Means of High-Resolution X-ray Absorption Spectroscopy. United States: N. p., 2016. Web. doi:10.1021/acs.jpcc.6b09335.
Butorin, Sergei M., Modin, Anders, Vegelius, Johan R., Kvashnina, Kristina O., & Shuh, David K. Probing Chemical Bonding in Uranium Dioxide by Means of High-Resolution X-ray Absorption Spectroscopy. United States. doi:10.1021/acs.jpcc.6b09335.
Butorin, Sergei M., Modin, Anders, Vegelius, Johan R., Kvashnina, Kristina O., and Shuh, David K. Wed . "Probing Chemical Bonding in Uranium Dioxide by Means of High-Resolution X-ray Absorption Spectroscopy". United States. doi:10.1021/acs.jpcc.6b09335. https://www.osti.gov/servlets/purl/1436141.
@article{osti_1436141,
title = {Probing Chemical Bonding in Uranium Dioxide by Means of High-Resolution X-ray Absorption Spectroscopy},
author = {Butorin, Sergei M. and Modin, Anders and Vegelius, Johan R. and Kvashnina, Kristina O. and Shuh, David K.},
abstractNote = {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.},
doi = {10.1021/acs.jpcc.6b09335},
journal = {Journal of Physical Chemistry. C},
number = 51,
volume = 120,
place = {United States},
year = {Wed Nov 30 00:00:00 EST 2016},
month = {Wed Nov 30 00:00:00 EST 2016}
}

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