Range-Separated Hybrid Functional Pseudopotentials

TL;DR

This paper introduces a method for constructing pseudopotentials compatible with range-separated hybrid exchange-correlation functionals, highlighting the importance of consistency for accurate property predictions in solid-state calculations.

Contribution

It presents a general scheme for creating pseudopotentials with RSH xc functionals, demonstrating their construction and impact on computational accuracy.

Findings

Pseudopotential consistency errors can reach 1.4% in property calculations.

Constructed pseudopotentials for PBE, PBE0, HSE, and sRSH functionals.

Consistency between pseudopotentials and functionals significantly affects accuracy.

Abstract

Consistency between the exchange-correlation (xc) functional used during pseudopotential construction and planewave-based electronic structure calculations is important for an accurate and reliable description of the structure and properties of condensed-phase systems. In this work, we present a general scheme for constructing pseudopotentials with range-separated hybrid (RSH) xc functionals based on the solution of the all-electron radial integro-differential equation for a spherical atomic configuration. As proof-of-principle, we demonstrate pseudopotential construction with the PBE, PBE0, HSE, and sRSH (based on LC-$\omega$PBE0) xc functionals for a select set of atoms, and then investigate the importance of pseudopotential consistency when computing band gaps, equilibrium lattice parameters, bulk moduli, and atomization energies of several solid-state systems. In doing so, we find that pseudopotential consistency errors (PSCE) tend to be systematic and can be as large as $1.4\%$ when computing these properties.