Robust Wannierization including magnetization and spin-orbit coupling via projectability disentanglement

TL;DR

This paper extends the projectability-disentangled Wannier functions method to magnetic and spin-orbit coupled systems, improving robustness and automation, and demonstrates its high success rate across diverse materials.

Contribution

It introduces an extended protocol for PDWFs that automatically expands projectors, enabling reliable Wannierization for complex magnetic and spin-orbit systems.

Findings

Achieved 100% success rate in constructing accurate Wannier functions on diverse materials.

Maintained an average band distance below 15 meV up to 2 eV above Fermi level.

Successfully applied the method to 200 chemically diverse materials.

Abstract

Maximally-localized Wannier functions (MLWFs) are widely employed as an essential tool for calculating the physical properties of materials due to their localized nature and computational efficiency. Projectability-disentangled Wannier functions (PDWFs) have recently emerged as a reliable and efficient approach for automatically constructing MLWFs that span both occupied and lowest unoccupied bands. Here, we extend the applicability of PDWFs to magnetic systems and/or those including spin-orbit coupling, and implement such extensions in automated workflows. Furthermore, we enhance the robustness and reliability of constructing PDWFs by defining an extended protocol that automatically expands the projectors manifold, when required, by introducing additional appropriate hydrogenic atomic orbitals. We benchmark our extended protocol on a set of 200 chemically diverse materials, as well as on the 40 systems with the largest band distance obtained with the standard PDWF approach, showing that on our test set the present approach delivers a 100% success rate in obtaining accurate Wannier-function interpolations, i.e., an average band distance below 15 meV between the DFT and Wannier-interpolated bands, up to 2 eV above the Fermi level.