Efficient Treatment of Relativistic Effects with Periodic Density Functional Methods: Energies, Gradients, and Stress Tensors

Fuente: arXiv
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Auteurs principaux: Franzke, Yannick J., Schosser, Werner M., Pauly, Fabian
Format: Preprint
Publié: 2023
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author Franzke, Yannick J.
Schosser, Werner M.
Pauly, Fabian
author_facet Franzke, Yannick J.
Schosser, Werner M.
Pauly, Fabian
contents The implementation of an efficient self-consistent field (SCF) method including both scalar relativistic effects and spin-orbit interaction in density functional theory (DFT) is presented. We make use of Gaussian-type orbitals (GTOs) and all integrals are evaluated in real space. Our implementation supports density functional approximations up to the level of meta-generalized gradient approximations (mGGAs) for SCF energies and gradients. The latter can be used to compute the stress tensor and consequently allow us to optimize the cell structure. Considering spin-orbit interaction requires the extension of the standard procedures to a two-component (2c) formalism and a non-collinear approach for open-shell systems. Here, we implemented both the canonical and the Scalmani-Frisch non-collinear DFT formalisms, with hybrid and range-separated hybrid functionals being presently restricted to SCF energies. We demonstrate both efficiency and relevance of spin-orbit effects for the electronic structure of discrete systems and systems periodic in one to three dimensions.
format Preprint
id arxiv_https___arxiv_org_abs_2305_03817
institution arXiv
publishDate 2023
record_format arxiv
spellingShingle Efficient Treatment of Relativistic Effects with Periodic Density Functional Methods: Energies, Gradients, and Stress Tensors
Franzke, Yannick J.
Schosser, Werner M.
Pauly, Fabian
Chemical Physics
Mesoscale and Nanoscale Physics
Materials Science
Computational Physics
The implementation of an efficient self-consistent field (SCF) method including both scalar relativistic effects and spin-orbit interaction in density functional theory (DFT) is presented. We make use of Gaussian-type orbitals (GTOs) and all integrals are evaluated in real space. Our implementation supports density functional approximations up to the level of meta-generalized gradient approximations (mGGAs) for SCF energies and gradients. The latter can be used to compute the stress tensor and consequently allow us to optimize the cell structure. Considering spin-orbit interaction requires the extension of the standard procedures to a two-component (2c) formalism and a non-collinear approach for open-shell systems. Here, we implemented both the canonical and the Scalmani-Frisch non-collinear DFT formalisms, with hybrid and range-separated hybrid functionals being presently restricted to SCF energies. We demonstrate both efficiency and relevance of spin-orbit effects for the electronic structure of discrete systems and systems periodic in one to three dimensions.
title Efficient Treatment of Relativistic Effects with Periodic Density Functional Methods: Energies, Gradients, and Stress Tensors
topic Chemical Physics
Mesoscale and Nanoscale Physics
Materials Science
Computational Physics
url https://arxiv.org/abs/2305.03817