High-throughput computation of electric polarization in solids via Berry flux diagonalization

TL;DR

This paper demonstrates that Berry flux diagonalization is a robust, efficient, and automated method for calculating electric polarization in solids, outperforming traditional interpolation methods especially in high-throughput screening scenarios.

Contribution

The authors introduce and validate heuristics for Berry flux diagonalization, enabling reliable, automated polarization calculations across diverse materials with fewer interpolations.

Findings

Successfully applied to 176 ferroelectric materials

Outperforms interpolation-based methods in challenging cases

Enables high-throughput screening of polar insulators

Abstract

Electric polarization in the absence of an externally applied electric field is a key property of polar materials, but the standard interpolation-based ab initio approach to compute polarization differences within the modern theory of polarization presents challenges for automated high-throughput calculations. Berry flux diagonalization [J. Bonini et. al, Phys. Rev. B 102, 045141 (2020)] has been proposed as an efficient and reliable alternative, though it has yet to be widely deployed. Here, we assess Berry flux diagonalization using ab initio calculations of a large set of materials, introducing and validating heuristics that ensure branch alignment with a minimal number of intermediate interpolated structures. Our automated implementation of Berry flux diagonalization succeeds in cases where prior interpolation-based workflows fail due to band-gap closures or branch ambiguities. Benchmarking with ab initio calculations of 176 candidate ferroelectrics, we demonstrate the efficacy of the approach on a broad range of insulating materials and obtain accurate effective polarization values with fewer interpolated structures than prior automated interpolation-based workflows. Our real-space heuristics that can predict gauge stability a priori from ionic displacements enable a general automated framework for reliable polarization calculations and efficient high-throughput screening of chemically and structurally diverse polar insulators. These results establish Berry flux diagonalization as a robust and efficient method to compute the effective polarization of solids and to accelerate the data-driven discovery of functional polar materials.