Cost-Effective High-Throughput Calculation Based on Hybrid Density Functional Theory: Application to Cubic, Double, and Vacancy-Ordered Halide Perovskites

Hybrid density functional theory calculations are commonly used to investigate the electronic structure of semiconductor materials but have not been ideal for high-throughput calculations due to heavy computation costs. We developed a computational approach to obtain the electronic band gap cost-effectively by employing not only non-self-consistent field calculation methods but also sparse k-point meshes for the Fock exchange potential. The benchmark calculation showed that our method is at least 30 times faster than the conventional hybrid density functional theory calculation to quickly screen materials. The band gaps of 290 materials in 5 different structures including cubic, double, and vacancy-ordered perovskites were obtained. The physical properties of Cs2WCl6 and Cs2NaInBr6, screened for optoelectronic applications, were in good agreement with the experiment.

Automated summary

A computational approach was developed to efficiently obtain electronic band gaps of semiconductor materials, showing at least 30 times faster speed compared to conventional methods, which is useful for screening materials for optoelectronic applications.