Noncollinear DFT+U and Hubbard parameters with fully-relativistic ultrasoft pseudopotentials

DOI

The magnetic, noncollinear parametrization of Dudarev's DFT+U method is generalized to fully-relativistic ultrasoft pseudopotentials. We present the definition of the DFT+U total energy functional, and the calculation of forces and stresses in the case of orthogonalized atomic orbitals defining the localised Hubbard manifold, where additional contributions arising from the derivative of the inverse square root of the overlap matrix appear. We further extend the perturbative calculation of the Hubbard U parameters within density-functional perturbation theory to the noncollinear relativistic case, by exploiting an existing and recently developed theoretical approach that takes advantage of the time-reversal operator to solve a second Sternheimer equation. We validate and apply the new scheme by studying the electronic structure and the thermodynamics of the binary compounds EuX (where X = O, S, Se, Te is a chalcogen atom), as representative simple crystals, and of the pyrochlore Cd2Os2O7, representative of a more structurally complex oxide.

Identifier
DOI https://doi.org/10.24435/materialscloud:3d-ww
Related Identifier https://doi.org/10.48550/arXiv.2304.10178
Related Identifier https://doi.org/10.1103/PhysRevB.108.115157
Related Identifier https://archive.materialscloud.org/communities/mcarchive
Related Identifier https://doi.org/10.24435/materialscloud:f1-7k
Metadata Access https://archive.materialscloud.org/oai2d?verb=GetRecord&metadataPrefix=oai_dc&identifier=oai:materialscloud.org:1740
Provenance
Creator Binci, Luca; Marzari, Nicola
Publisher Materials Cloud
Contributor Binci, Luca; Marzari, Nicola
Publication Year 2023
Rights info:eu-repo/semantics/openAccess; Creative Commons Attribution 4.0 International; https://creativecommons.org/licenses/by/4.0/legalcode
OpenAccess true
Contact archive(at)materialscloud.org
Representation
Language English
Resource Type info:eu-repo/semantics/other
Format application/zip; text/markdown; text/plain
Discipline Materials Science and Engineering