Spin-dependent interactions in orbital-density-dependent functionals: non-collinear Koopmans spectral functionals

DOI

The presence of spin-orbit coupling or non-collinear magnetic spin states can have dramatic effects on the ground-state and spectral properties of materials, in particular on the band structure. Here, we develop non-collinear Koopmans-compliant functionals based on Wannier functions and density-functional perturbation theory, targeting accurate spectral properties in the quasiparticle approximation. Our non-collinear Koopmans-compliant theory involves functionals of four-component orbitals densities, that can be obtained from the charge and spin-vector densities of Wannier functions. We validate our approach on four emblematic non-magnetic and magnetic semiconductors where the effect of spin-orbit coupling goes from small to very large: the III-IV semiconductor GaAs, the transition-metal dichalcogenide WSe₂, the cubic perovskite CsPbBr₃, and the ferromagnetic semiconductor CrI₃. The predicted band gaps are comparable in accuracy to state-of-the-art many-body perturbation theory and include spin-dependent interactions and screening effects that are missing in standard diagrammatic approaches based on the random phase approximation. While the inclusion of orbital- and spin-dependent interactions in many-body perturbation theory requires self-screening or vertex corrections, they emerge naturally in the Koopmans-functionals framework.

Identifier
DOI https://doi.org/10.24435/materialscloud:kp-2v
Related Identifier https://doi.org/10.1103/PhysRevResearch.6.033085
Related Identifier https://doi.org/10.48550/arXiv.2402.14575
Related Identifier https://archive.materialscloud.org/communities/mcarchive
Related Identifier https://doi.org/10.24435/materialscloud:2j-mn
Metadata Access https://archive.materialscloud.org/oai2d?verb=GetRecord&metadataPrefix=oai_dc&identifier=oai:materialscloud.org:2052
Provenance
Creator Marrazzo, Antimo; Colonna, Nicola
Publisher Materials Cloud
Contributor Marrazzo, Antimo; Colonna, Nicola
Publication Year 2024
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 text/plain; application/gzip; text/markdown
Discipline Materials Science and Engineering