Electronic structure of UO2.12 calculated in the coherent potential approximation taking into account strong electron correlations and spin-orbit coupling
Based on the coherent potential approximation, the method of calculating the electronic structure of nonstoichiometric and hyperstoichiometric compounds with strong electron correlations and spin-orbit coupling has been developed. This method can be used to study both substitutional and interstitial impurities, which is demonstrated based on the example of the hyperstoichiometric UO2.12 compound. The influence of the coherent potential on the electronic structure of compounds has been shown for the nonstoichiometric UO1.87 containing vacancies in the oxygen sublattice as substitutional impurities, for stoichiometric UO2 containing vacancies in the oxygen sublattice and oxygen as an interstitial impurity, and for hyperstoichiometric UO2.12 with excess oxygen also as interstitial impurity. In the model of the uniform distribution of impurities, which forms the basis of the coherent potential approximation, the energy spectrum of UO2.12 has a metal-like character.
Keywordselectronic structure magnetic properties coherent potential approximation strong electron correlations spin-orbit coupling
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- 3.S. L. Dudarev, G. A. Botton, S. Y. Savrasov, Z. Szotek, W. M. Temmerman, and A. P. Sutton, “Electronic structure and elastic properties of strongly correlated metal oxides from first principles: LSDA+U, SIC-LSDA and EELS study of UO2 and NiO,” Phys. Status Solidi A 166, 429–443 (1998).CrossRefGoogle Scholar
- 6.A. Modin, M.-T. Suzuki, J. Vegelius, Y. Yun, D. K. Shuh, L. Werme, J. Nordgren, P. M. Oppeneer, and S. M. Butorin, “5 f-shell correlation effects in dioxides of light actinides studied by O 1s X-ray absorption and emission spectroscopies and first-principles calculations,” J. Phys.: Condens. Matter 27, 315503 (2015).Google Scholar
- 16.B. T. M. Willis, “Crystallographic studies of anionexcess uranium oxides,” J. Chem. Soc. 83, 1073–1081 (1987).Google Scholar
- 20.M. A. Korotin, Z. V. Pchelkina, N. A. Skorikov, E. Z. Kurmaev, and V. I. Anisimov, “The coherent potential approximation for strongly correlated systems: Electronic structure and magnetic properties of NiO–ZnO solid solutions,” J. Phys.: Condens. Matter 26, 115501 (2014).Google Scholar
- 22.M. A. Korotin, N. A. Skorikov, S. L. Skornyakov, A. O. Shorikov, and V. I. Anisimov, “Inclusion of effects of self-consistency of the electron density within the LDA+U+SO method implemented in the temperature Green’s function formalism in the basis of the Wannier functions,” JETP Lett. 100, 823–828 (2014).CrossRefGoogle Scholar
- 23.V. A. Alekseev, L. A. Anan’eva, and R. P. Rafal’skii, “Dependence of the UO2+x lattice parameter on the composition,” Izv. Akad. Nauk SSSR, Ser. Geol., No. 9, 80–89 (1979).Google Scholar
- 25.V. I. Anisimov, D. E. Kondakov, A. V. Kozhevnikov, I. A. Nekrasov, Z. V. Pchelkina, J. W. Allen, S.-K. Mo, H.-D. Kim, P. Metcalf, S. Suga, A. Sekiyama, G. Keller, I. Leonov, X. Ren, and D. Vollhardt, “Full orbital calculation scheme for materials with strongly correlated electrons,” Phys. Rev. B: Condens. Matter Mater. Phys. 71, 125119 (2005).CrossRefGoogle Scholar