First-principles calculation of optical responses based on nonorthogonal localized orbitals

TL;DR

This paper introduces a new ab initio method for calculating optical response functions using nonorthogonal localized orbitals, avoiding Wannier function optimization, and enabling automated high throughput material property analysis.

Contribution

The authors develop a general scheme for response function calculations based on nonorthogonal localized orbitals, simplifying the process and facilitating high throughput studies.

Findings

Accurate calculation of nonlinear optical responses like shift current conductivity of monolayer WS2.

Method achieves good agreement with previous calculations.

Avoids the challenging optimization of Wannier functions.

Abstract

Based on ab initio software packages using nonorthogonal localized orbitals, we develop a general scheme of calculating response functions. We test the performance of this method by calculating nonlinear optical responses of materials, like the shift current conductivity of monolayer WS2, and achieve good agreement with previous calculations. This method bears many similarities to Wannier interpolation, which requires a challenging optimization of Wannier functions due to the conflicting requirements of orthogonality and localization. Although computationally heavier compared to Wannier interpolation, our procedure avoids the construction of Wannier functions and thus enables automated high throughput calculations of linear and nonlinear responses related to electrical, magnetic and optical material properties.