Improving the performance of Tao-Mo non-empirical density functional with broader applicability in quantum chemistry and material sciences

TL;DR

This paper introduces a revised Tao-Mo density functional that incorporates high-density gradient expansion modifications, significantly improving its accuracy across various quantum chemistry and material science applications.

Contribution

The paper presents a physically motivated revision of the Tao-Mo functional, enhancing its performance and applicability in quantum chemistry and solid-state physics.

Findings

Improved accuracy in thermochemistry and structural properties.

Enhanced cohesive energies and surface energies.

Preserved lattice constants and bulk moduli accuracy.

Abstract

A revised version of the semilocal exchange-correlation functional [Phys. Rev. Lett. 117, 073001 (2016)] (TM) is proposed by incorporating the modifications to its correlation content obtained from the full high-density second-order gradient expansion as proposed in the case of revised Tao-Perdew-Staroverov-Scuseria (revTPSS) [Phys. Rev. Lett. 103, 026403 (2009)] functional. The present construction improves the performance of TM functional over a wide range of quantum chemical and solid-state properties (thermochemistry and structural). More specifically, the cohesive energies, jellium surface exchange-correlation energies, and real metallic surface energies are improved by preserving the accuracy of the solid-state lattice constants and bulk moduli. The present proposition is not only physically motivated but also enhances the applicability of the TM functional. New physical insights with proper exemplification of the present modification which is presented here can further serve for more realistic non-empirical density functional construction.