Correlated band magnetism of cerium and actinide materials

We discuss (1) the effects to be expected by the introduction into the electronic structure of locally-based two-electron correlations between the f electrons and bonding electrons of p and d atomic origin centered off-site as well as f-f correlations, (2) the expected observable consequences of these two-electron correlations, and (3) how to perform electronic structure calculations including the two-electron correlations. We first review certain general features of the physics associated with capturing the dual energetically localized-delocalized nature of the f electron spectral density; and review model calculations involving a single on-site f electron and a single ligand p/d electron of off-site parentage which lead to the possibility of a narrow singlet and triplet (magnetic) band picture explaining heavy fermion phenomenology. We then show that the same singlet/magnetic state picture arises when we include two-electron f-l and f-f correlations for actinides, which have atomic f(n) configurations with n>1; and we describe a practical electronic structure scheme for real materials based on a sequence in which a conventional one-electron linearized combination of muffin-tin orbitals (LMTO) LDA+U calculation is followed by a calculation for the lattice with a helium like two-electron Hamiltonian at the f atom sites, i.e., two-electron atoms where initially for the core two electrons worth of charge are removed from the LMTO f-site atom. This procedure will reconstruct the LMTO bands to include two-electron texturing. (C) 1997 American Institute of Physics.