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.

5 tables, 12 figures

References in corpus (2)

• Magnetic state of plutonium ion in metallic Pu and its compounds
• An ab initio full potential fully relativistic study of atomic carbon, nitrogen, and oxygen chemisorption on the (111) surface of delta-plutonium

Cited by in corpus (11)

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• Ab initio modeling of oxygen impurity atom incorporation into uranium mononitride surface and subsurface vacancies
• DFT calculations of point defects on UN(001) surface
• Ab initio simulations of oxygen interaction with surfaces and interfaces in uranium mononitride
• Chemisorption of a molecular oxygen on the UN (001) surface: ab initio calculations
• Advances in actinide thin films: synthesis, properties, and future directions
• Fermi-surface reconstruction at the metamagnetic high-field transition in uranium mononitride
• Ideal strengths and bonding properties of PuO2 under tension