Density functional study of the actinide nitrides

Abstract

The full potential all electron linearized augmented plane wave plus local orbitals (FP-LAPW + lo) method, as implemented in the suite of software WIEN2K, has been used to systematically investigate the structural, electronic, and magnetic properties of the actinide compounds AnN (An = Ac, Th, Pa, U, Np, Pu, Am). The theoretical formalism used is the generalized gradient approximation to density functional theory (GGA-DFT) with the Perdew-Burke-Ernzerhof (PBE) exchange-correlation functional. Each compound has been studied at six levels of theory: non-magnetic (NM), non-magnetic with spin-orbit coupling (NM+SOC), ferromagnetic (FM), ferromagnetic with spin-orbit coupling (FM+SOC), anti-ferromagnetic (AFM), and anti-ferromagnetic with spin-orbit coupling (AFM+SOC). The structural parameters, bulk moduli, densities of states, and charge distributions have been computed and compared to available experimental data and other theoretical calculations published in the literature. The total energy calculations indicate that the lowest energy structures of AcN, ThN, and PaN are degenerate at the NM+SOC, FM+SOC, and AFM+SOC levels of theory with vanishing total magnetic moments in the FM+SOC and AFM+SOC cases, making the ground states essentially non-magnetic with spin-orbit interaction. The ground states of UN, NpN, PuN, and AmN are found to be FM+SOC at the level of theory used in the present computations. The nature of the interactions between the actinide metals and nitrogen atom, and the implications on 5f electron delocalization and localization are discussed in detail.