Norm-conserving pseudopotentials with chemical accuracy compared to all-electron calculations

TL;DR

This paper develops improved norm-conserving pseudopotentials with non-linear core correction that achieve chemical accuracy comparable to all-electron calculations, enhancing computational efficiency for quantum chemistry and materials science.

Contribution

Introduction of non-linear core correction to Dual Space Gaussian pseudopotentials, resulting in highly accurate pseudopotentials for elements up to the third period with PBE functional.

Findings

Atomization energy errors of about 0.5 kcal/mol on G2-1 set

Reliable for high pressure phases of crystalline solids

Interaction energy errors around 0.5 kcal/mol with dispersion corrections

Abstract

By adding a non-linear core correction to the well established Dual Space Gaussian type pseudopotentials for the chemical elements up to the third period, we construct improved pseudopotentials for the Perdew Burke Ernzerhof (PBE) functional and demonstrate that they exhibit excellent accuracy. Our benchmarks for the G2-1 test set show average atomization energy errors of only half a kcal/mol. The pseudopotentials also remain highly reliable for high pressure phases of crystalline solids. When supplemented by empirical dispersion corrections the average error in the interaction energy between molecules is also about half a kcal/mol. The accuracy that can be obtained by these pseudopotentials in combination with a systematic basis set is well superior to the accuracy that can be obtained by commonly used medium size Gaussian basis sets in all-electron calculations.