Antimo Marrazzo^1,2*, Nicola Colonna^3,4*

1 Scuola Internazionale Superiore di Studi Avanzati (SISSA), I-34136 Trieste, Italy

2 Dipartimento di Fisica, Universita' di Trieste, Strada Costiera 11, I-34151 Trieste, Italy

3 Laboratory for Materials Simulations, Paul Scherrer Institute (PSI), CH-5232 Villigen, Switzerland

4 National Centre for Computational Design and Discovery of Novel Materials (MARVEL), Paul Scherrer Institute (PSI), CH-5232 Villigen, Switzerland

* Corresponding authors emails: antimo.marrazzo@units.it, nicola.colonna@psi.ch

DOI10.24435/materialscloud:kp-2v [version v1]

Publication date: Jun 03, 2024

How to cite this record

Antimo Marrazzo, Nicola Colonna, Spin-dependent interactions in orbital-density-dependent functionals: non-collinear Koopmans spectral functionals, Materials Cloud Archive 2024.83 (2024), https://doi.org/10.24435/materialscloud:kp-2v

Description

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.

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Keywords

MARVEL/P4 SNSF Spin-orbit coupling Spin-dependent interactions Non-collinear magnetism Spectral functionals Transition-metal dichalcogenide Metal halide perovskite Spin-torque