Projectability disentanglement for accurate and automated electronic-structure Hamiltonians

Abstract

AbstractMaximally-localized Wannier functions (MLWFs) are broadly used to characterize the electronic structure of materials. Generally, one can construct MLWFs describing isolated bands (e.g. valence bands of insulators) or entangled bands (e.g. valence and conduction bands of insulators, or metals). Obtaining accurate and compact MLWFs often requires chemical intuition and trial and error, a challenging step even for experienced researchers and a roadblock for high-throughput calculations. Here, we present an automated approach, projectability-disentangled Wannier functions (PDWFs), that constructs MLWFs spanning the occupied bands and their complement for the empty states, providing a tight-binding picture of optimized atomic orbitals in crystals. Key to the algorithm is a projectability measure for each Bloch state onto atomic orbitals, determining if that state should be kept identically, discarded, or mixed into the disentanglement. We showcase the accuracy on a test set of 200 materials, and the reliability by constructing 21,737 Wannier Hamiltonians.