Ab initio determination of the localized/delocalized f-manifold in UPd2Al3

The electronic structure of UPd2Al3 is described using the self-interaction–corrected local-spin-density approximation to density functional theory. The ground state is found to be characterized by the coexistence of localized (f2) and delocalized U f electrons, in agreement with experimental evidence. We observe significant difference in electronic structure between UPd2Al3 and the previously studied UPt3 compound. Even though a trend towards localization exists in UPt3, the total energies and the density of states at the Fermi level favor a ground state with localized f1, rather than f2 U ions.