Performance improvement of deorbitalized exchange-correlation functionals

DOI

<p>Deorbitalization of a conventional meta-generalized-gradient exchange-correlation approximation replaces its dependence upon the Kohn-Sham kinetic energy density with a dependence on the density gradient and Laplacian. In principle, that simplification should provide improved computational performance relative to the original meta-GGA form because of the shift from an orbital-dependent generalized Kohn-Sham potential to a true KS local potential. Often that prospective gain is lost because of problematic roughness in the density caused by the density Laplacian and consequent roughness in the exchange-correlation potential from the resulting higher-order spatial derivatives of the density in it. We address the problem by constructing a deorbitalizer based on the RPP deorbitalizer [Phys. Rev. Mater. 6, 083803 (2022)] with comparative smoothness of the potential along with retention of constraint satisfaction as design goals. Applied to the r<sup>2</sup>SCAN exchange-correlation functional [J. Phys. Chem. Lett. 11, 8208 (2020)], we find substantial timing improvements for solid-state calculations over both r<sup>2</sup>SCAN and its earlier deorbitalization for high precision calculations of structural properties, while improving upon the accuracy of RPP deorbitalization for both solids and molecules.</p> <p>Data archive includes data needed to reproduce the figures and tables of this work, and input scripts for test set calculations performed using VASP and NWChem electronic structure codes.</p>

Identifier
DOI https://doi.org/10.24435/materialscloud:ga-tb
Related Identifier https://arxiv.org/abs/2509.00953
Related Identifier https://archive.materialscloud.org/communities/mcarchive
Related Identifier https://doi.org/10.24435/materialscloud:zk-py
Metadata Access https://archive.materialscloud.org/oai2d?verb=GetRecord&metadataPrefix=oai_dc&identifier=oai:materialscloud.org:tq12m-bzc76
Provenance
Creator Francisco, Hector; Thapa, Bishal; Trickey, S. B.; Cancio, Antonio
Publisher Materials Cloud
Contributor Cancio, Antonio
Publication Year 2025
Rights info:eu-repo/semantics/openAccess; Creative Commons Attribution 4.0 International; https://creativecommons.org/licenses/by/4.0/legalcode
OpenAccess true
Contact archive(at)materialscloud.org
Representation
Language English
Resource Type info:eu-repo/semantics/other
Format application/gzip; text/plain
Discipline Materials Science and Engineering