中国物理B ›› 2008, Vol. 17 ›› Issue (4): 1364-1370.doi: 10.1088/1674-1056/17/4/035

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First-principles local density approximation (LDA)+U and generalized gradient approximation (GGA)+U studies of plutonium oxides

孙博, 张平   

  1. Institute of Applied Physics and Computational Mathematics, Beijing 100088, China
  • 收稿日期:2007-09-10 修回日期:2007-10-10 出版日期:2008-04-20 发布日期:2008-04-20
  • 基金资助:
    Project supported by the National Natural Science Foundation of China (Grant No 10604010).

First-principles local density approximation (LDA)+U and generalized gradient approximation (GGA)+U studies of plutonium oxides

Sun Bo(孙博) and Zhang Ping(张平)†   

  1. Institute of Applied Physics and Computational Mathematics, Beijing 100088, China
  • Received:2007-09-10 Revised:2007-10-10 Online:2008-04-20 Published:2008-04-20
  • Supported by:
    Project supported by the National Natural Science Foundation of China (Grant No 10604010).

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摘要： The electronic structures and properties of PuO2 and Pu2O3 have been studied according to the first principles by using the all-electron projector-augmented-wave (PAW) method. The local density approximation (LDA)+U and the generalized gradient approximation (GGA)+U formalisms have been used to account for the strong on-site Coulomb repulsion among the localized Pu 5f electrons. We discuss how the properties of PuO2 and Pu2O3 are affected by choosing the values of U and exchange-correlation potential. Also, the oxidation reaction of Pu2O3, leading to the formation of PuO2, and its dependence on U and exchange-correlation potential have been studied. Our results show that by choosing an appropriate U it is possible to consistently describe structural, electronic, and thermodynamic properties of PuO2 and Pu2O3, which enable the modelling of the redox process involving Pu-based materials.

关键词: the first-principles calculation, LDA+U, GGA+U, plutonium oxides

Abstract: The electronic structures and properties of PuO2 and Pu2O3 have been studied according to the first principles by using the all-electron projector-augmented-wave (PAW) method. The local density approximation (LDA)+U and the generalized gradient approximation (GGA)+U formalisms have been used to account for the strong on-site Coulomb repulsion among the localized Pu 5f electrons. We discuss how the properties of PuO2 and Pu2O3 are affected by choosing the values of U and exchange-correlation potential. Also, the oxidation reaction of Pu2O3, leading to the formation of PuO2, and its dependence on U and exchange-correlation potential have been studied. Our results show that by choosing an appropriate U it is possible to consistently describe structural, electronic, and thermodynamic properties of PuO2 and Pu2O3, which enable the modelling of the redox process involving Pu-based materials.

Key words: the first-principles calculation, LDA+U, GGA+U, plutonium oxides

中图分类号:  (Thermal properties of crystalline solids)

  • 65.40.-b
71.15.Ap (Basis sets (LCAO, plane-wave, APW, etc.) and related methodology (scattering methods, ASA, linearized methods, etc.)) 71.15.Mb (Density functional theory, local density approximation, gradient and other corrections) 71.20.Ps (Other inorganic compounds)