Dirac's equation and its implications for density functional theory based calculations of materials containing heavy elements

Rehn, Daniel A.; Wills, John M.; Battelle, Torey E.; Mattsson, Ann E.

doi:10.1103/physrevb.101.085114

Title: Dirac's equation and its implications for density functional theory based calculations of materials containing heavy elements

Journal Article · Tue Feb 11 00:00:00 EST 2020 · Physical Review. B

DOI:https://doi.org/10.1103/physrevb.101.085114· OSTI ID:1819136

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^[1]; Battelle, Torey E. ^[2];

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Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Colorado School of Mines, Golden, CO (United States)

Electronic structure calculations based on density functional theory (DFT) give quantitatively accurate predictions of properties of most materials containing light elements. For heavy materials, and in particular for $f$ -electron systems, DFT based methods can fail both qualitatively and quantitatively for two distinct reasons: their failure to describe confinement effects arising from localized $f$ -electron behavior and their incomplete or approximate treatment of relativity. In addition, different methods for incorporating relativistic effects, which give identical results in most light materials, can give different predictions in heavy elements. In order to develop a quantitative capability for calculating the properties of these materials, it is essential to separate the predictions of the underlying equations from the uncertainty introduced in approximations used in computation. Working toward that goal, here we have developed a code, called dirac-fp, which is based directly on solving the Dirac-Kohn-Sham equations and uses the full-potential linear muffin-tin orbital (FP-LMTO) approach to electronic structure. In order to assess the performance of dirac-fp, we perform calculations on three different face-centered cubic materials using different approximate treatments of relativity: the scalar relativistic (SR) approach commonly used in most solid-state DFT codes, the scalar relativistic plus spin-orbit coupling corrections (SR+SO) approach which includes spin-orbit coupling self-consistently using the SR states inside the muffin tins, and the Dirac-Kohn-Sham (Dirac) approach implemented in dirac-fp. Performing calculations on thorium, in which relativistic effects should be strong, aluminum, in which relativistic effects should be negligible, and gold, in which relativistic effects play an intermediate role, we find that the Dirac approach is able to provide theoretically consistent results in the electronic structure and ground-state properties across all three materials.

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Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA); USDOE Laboratory Directed Research and Development (LDRD) Program

Grant/Contract Number:: 89233218CNA000001; NA0003525

OSTI ID:: 1819136

Alternate ID(s):: OSTI ID: 1599520

Report Number(s):: LA-UR-19-25303; TRN: US2214065

Journal Information:: Physical Review. B, Vol. 101, Issue 8; ISSN 2469-9950

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 5 works

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Title: Dirac's equation and its implications for density functional theory based calculations of materials containing heavy elements

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