Electronic-structure theory of plutonium chalcogenides

Abstract The correlated band theory methods, the around-mean-field LDA + U and dynamical LDA + HIA (Hubbard-I), are applied to investigate the electronic structure of Pu chalcogenides. The LDA + U calculations for PuX (X = S, Se, Te) provide non-magnetic ground state in agreement with the experimental data. Non-integer filling of 5 f -manifold (from approx. 5.6 in PuS to 5.7 PuTe). indicates a mixed valence ground state which combines f 5 and f 6 multiplets. Making use of the dynamical LDA+HIA method the photoelectron spectra are calculated in good agreement with experimental data. The three-peak feature near E F attributed to 5 f -manifold is well reproduced by LDA + HIA, and follows from mixed valence character of the ground state.