Hybrid functional pseudopotentials

TL;DR

This paper introduces a new scheme for generating hybrid functional pseudopotentials, improving the accuracy of hybrid density functional calculations by ensuring consistency between pseudopotentials and the functional used.

Contribution

The authors develop and validate a method for creating hybrid functional pseudopotentials, addressing a key gap in current computational materials science.

Findings

PBE0 pseudopotentials improve agreement with all-electron calculations.

Using consistent pseudopotentials enhances the accuracy of hybrid functional predictions.

Benchmark results show better structural and electronic property predictions.

Abstract

The consistency between the exchange-correlation functional used in pseudopotential construction and in the actual density functional theory calculation is essential for the accurate prediction of fundamental properties of materials. However, routine hybrid density functional calculations at present still rely on GGA pseudopotentials due to the lack of hybrid functional pseudopotentials. Here, we present a scheme for generating hybrid functional pseudopotentials, and we analyze the importance of pseudopotential density functional consistency for hybrid functionals. We benchmark our PBE0 pseudopotentials for structural parameters and fundamental electronic gaps of the G2 molecular dataset and some simple solids. Our results show that using our new PBE0 pseudopotentials in PBE0 calculations improves agreement with respect to all-electron calculations.