Precision and efficiency in solid-state pseudopotential calculations

TL;DR

This paper introduces a protocol for validating pseudopotential libraries in density-functional theory, resulting in curated libraries optimized for high-throughput screening and high-precision modeling, with demonstrated accuracy in equations of state.

Contribution

It presents a systematic validation protocol for pseudopotentials and develops curated libraries tailored for different computational needs.

Findings

Curated pseudopotential libraries outperform others in the Δ-factor test.

Validation protocol ensures high accuracy in equations of state and phonon calculations.

Libraries are optimized for efficiency and precision in materials simulations.

Abstract

Despite the enormous success and popularity of density-functional theory, systematic verification and validation studies are still limited in number and scope. Here, we propose a protocol to test publicly available pseudopotential libraries, based on several independent criteria including verification against all-electron equations of state and plane-wave convergence tests for phonon frequencies, band structure, cohesive energy and pressure. Adopting these criteria we obtain curated pseudopotential libraries (named SSSP or standard solid-state pseudopotential libraries), that we target for high-throughput materials screening ("SSSP efficiency") and high-precision materials modelling ("SSSP precision"). This latter scores highest among open-source pseudopotential libraries available in the $\Delta$-factor test of equations of states of elemental solids.