Generalized Kohn-Sham Approach for the Electronic Band Structure of Spin-Orbit Coupled Materials

TL;DR

This paper introduces an extended Kohn-Sham formalism within spin-current density functional theory to accurately compute electronic band structures in spin-orbit coupled materials, demonstrating improved agreement with experiments.

Contribution

It develops a non-local potential extension of the Kohn-Sham approach within SCDFT, enabling self-consistent treatment of spin currents in spin-orbit coupled systems.

Findings

Accurately predicts spin-orbit-induced band splittings in MoSe₂ and MoTe₂.

Achieves quantitative agreement with experimental data using hybrid functionals.

Outperforms second-variational methods in capturing spin-orbit effects.

Abstract

Spin-current density functional theory (SCDFT) is a formally exact framework designed to handle the treatment of interacting many-electron systems including spin-orbit coupling at the level of the Pauli equation. In practice, robust and accurate calculations of the electronic structure of these systems call for functional approximations that depend not only on the densities, but also on spin-orbitals. Here we show that the call can be answered by resorting to an extension of the Kohn-Sham formalism, which admits the use of non-local effective potentials, yet it is firmly rooted in SCDFT. The power of the extended formalism is demonstrated by calculating the spin-orbit-induced band-splittings of inversion-asymmetric MoSe$_2$ monolayer and inversion-symmetric bulk $\alpha$-MoTe$_2$. We show that quantitative agreement with experimental data is obtainable via global hybrid approximations by setting the fraction of Fock exchange at the same level which yields accurate values of the band gap. Key to these results is the ability of the method to self-consistently account for the spin currents induced by the spin-orbit interaction. The widely used method of refining spin-density functional theory by a second-variational treatment of spin-orbit coupling is unable to match our SCDFT results.