1 Department of Physics and Astronomy, Faculty of Science, Aarhus University, Aarhus University2 Teoretisk naturvidenskab, Aarhus University, Aarhus University3 Department of Physics and Astronomy, Science and Technology, Aarhus University4 Daresbury Laboratory5 Oak Ridge National Laboratory6 Department of Physics and Astronomy, Science and Technology, Aarhus University
The ground state electronic structures of the actinide oxides AO, A2O3 and AO2 (A=U, Np, Pu, Am, Cm, Bk, Cf) are determined from first-principles calculations using the selfinteraction corrected local spin-density approximation. Our study reveals a strong link between preferred oxidation number and degree of localization. The ionic nature of the actinide oxides emerges from the fact that those oxides where the ground state is calculated to be metallic do not exist in nature, as the corresponding delocalized f-states favour the accommodation of additional O atoms into the crystal lattice.
Materials Research Society Symposium Proceedings, 2010