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Sensitivity to Actinide Doping of Uranium Compounds by Resonant Inelastic X-ray Scattering at Uranium L3 Edge.
- Source :
-
Analytical Chemistry . 9/1/2015, Vol. 87 Issue 17, p8772-8780. 9p. - Publication Year :
- 2015
-
Abstract
- Valence-to-core resonant inelastic X-ray scattering (RIXS) and high energy resolution fluorescence detection (HERFD) X-ray absorption measurements were performed at the U L3 edges of UO2 and UO2(NO3)2(H2O)6. The results are compared with model calculations based on the local-density-approximation formalism, taking into account Coulomb interaction U (LDA + U). We show that despite strong 5f-5f electronic correlations in the studied systems and the use of core-level excitations in the intermediate stage of the spectroscopic process, the RIXS technique probes a convolution of the single-particle densities of states in the valence and conduction bands. For UO2, the detected crystal-field splitting between the U 6d eg and t2g orbitals from the RIXS spectra (~3.5 eV) is larger than that previously derived from optical spectroscopy. Furthermore, by using an example of the U0.75Pu0.25O2 mixed oxide, we show that the RIXS technique at the U L3 edges is sensitive to the substitution of U with other actinide, in contrast to conventional X-ray absorption methods. That is, due to changes in the occupied part rather than in the unoccupied part of the U 6d states caused by the substitution. [ABSTRACT FROM AUTHOR]
Details
- Language :
- English
- ISSN :
- 00032700
- Volume :
- 87
- Issue :
- 17
- Database :
- Academic Search Index
- Journal :
- Analytical Chemistry
- Publication Type :
- Academic Journal
- Accession number :
- 109925811
- Full Text :
- https://doi.org/10.1021/acs.analchem.5b01699