Electronic Structure and Photoemission in Plutonium Chalcogenides

The electronic structure of Pu chalcogenides is investigated making use of static around-mean-field LDA+U and dynamical LDA+HIA (Hubbard-I) methods. The LDA+U calculations provide correct non-magnetic ground state for PuX (X = S, Se, Te) with 5 f -manifold non-integer filling (∼5.6(PuS)-5.7(PuTe)). This is an indication of a mixed valence ground state which is a combination of f 5 and f 6 multiplets. The photoelectron spectra are calculated in good agreement with experimental data. The 5 f -manifold three-peaks feature near E F is well reproduced by LDA+HIA, and follows from mixed valence character of the ground state.