2007/12/21 by Bo Sun, Ping Zhang, Sun, Bo +3
Physics and Astronomy · #FOS: Physical sciences #Materials Science (cond-mat.mtrl-sci) #Strongly Correlated Electrons (cond-mat.str-el) #cond-mat.mtrl-sci #cond-mat.str-el
paper · pdf · doi:10.48550/arxiv.0712.3623
To appear in J. Chem. Phys
arxiv created 2007/12/21 · arxiv updated 2009/12/01
The electronic structure and properties of PuO2 and Pu2O3 have been studied from first principles by the all-electron projector-augmented-wave (PAW) method. The local density approximation (LDA)+U and the generalized gradient approximation (GGA)+U formalism 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 the choice of U as well as the choice of exchange-correlation potential. Also, oxidation reaction of Pu2O3, leading to 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 promising to correctly and consistently describe structural, electronic, and thermodynamic properties of PuO2 and Pu2O3, which enables it possible the modeling of redox process involving Pu-based materials.