Ground-state electronic structure of actinide monocarbides and mononitrides

Abstract

The self-interaction corrected local spin-density approximation is used to investigate the ground-state valency configuration of the actinide ions in the actinide monocarbides, AC A=U,Np,Pu,Am,Cm, and the actinide mononitrides, AN. The electronic structure is characterized by a gradually increasing degree of f electron localization from U to Cm, with the tendency toward localization being slightly stronger in the more ionic nitrides compared to the more covalent carbides. The itinerant band picture is found to be adequate for UC and acceptable for UN, while a more complex manifold of competing localized and delocalized f-electron configurations underlies the ground states of NpC, PuC, AmC, NpN, and PuN. The fully localized 5f-electron configuration is realized in CmC f 7 ,C mNf 7 , and AmN f 6 . The observed sudden increase in lattice parameter from PuN to AmN is found to be related to the localization transition. The calculated valence electron densities of states are in good agreement with photoemission data.