Material specific optimization of Gaussian basis sets against plane wave data

TL;DR

This paper introduces a material-specific Gaussian basis set optimization method for solids that improves accuracy by tailoring basis sets to specific materials, outperforming existing sets in various periodic systems.

Contribution

The paper presents a novel optimization scheme for Gaussian basis sets that accounts for material-specific properties, enhancing simulation accuracy for periodic systems.

Findings

Optimized basis sets for diamond, graphite, and silicon show improved accuracy.

The scheme outperforms existing basis sets for MoS2 and NiO.

Material-specific basis sets reduce simulation errors in periodic systems.

Abstract

Since in periodic systems, a given element may be present in different spatial arrangements displaying vastly different physical and chemical properties, an elemental basis set that is independent of physical properties of materials may lead to significant simulation inaccuracies. To avoid such a lack of material specificity within a given basis set, we present a material-specific Gaussian basis optimization scheme for solids, which simultaneously minimizes the total energy of the system and optimizes the band energies when compared to the reference plane wave calculation while taking care of the overlap matrix condition number. To assess this basis set optimization scheme, we compare the quality of the Gaussian basis sets generated for diamond, graphite, and silicon via our method against the existing basis sets. The optimization scheme of this work has also been tested on the existing Gaussian basis sets for periodic systems such as MoS$_2$ and NiO yielding improved results.