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Spin-polarized fully relativistic linear combinations of Gaussian-type orbitals calculations for fcc plutonium

Authors

  • Jonathan Carl Boettger

    Corresponding author
    1. Applied Physics Division, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, U.S.A
    • Applied Physics Division, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, U.S.A
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  • This work was performed under the auspices of the U.S. Department of Energy.

Abstract

The magnetic ordering of plutonium (Pu) in its fcc structure δ-phase is investigated using the fully relativistic linear combinations of Gaussian-type orbitals—fitting function (LCGTO-FF) method, within the generalized-gradient approximation to density functional theory. Three types of collinear spin orderings were considered: ferromagnetic, with spins aligned in the (001) direction; and two antiferromagnetic (001)-layer structures, with spins aligned either perpendicular to each plane (001) or parallel to each plane (100). For each ordering, the total energy and spin moment were calculated with and without spin-orbit coupling included. In both cases, the ground state is predicted to be antiferromagnetic. Adding spin-orbit coupling acts to stabilize the (001) orientation relative to the (100) orientation. At zero pressure, the antiferromagnetic (001) state is bound relative to the nonmagnetic state by roughly 40 mRy per atom. The zero-pressure lattice constant obtained here for the antiferromagnetic (001) state (8.69 bohr) is in substantially better agreement with the measured lattice constant (8.80 bohr) than is the nonmagnetic lattice constant (8.12 bohr). © 2003 Wiley Periodicals, Inc. Int J Quantum Chem, 2003

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