Testing the r²SCAN Density Functional for the Thermodynamic Stability of Solids with and without a van der Waals Correction.

Content Provider	Europe PMC
Author	Kothakonda, Manish Kaplan, Aaron D. Isaacs, Eric B. Bartel, Christopher J. Furness, James W. Ning, Jinliang Wolverton, Chris Perdew, John P. Sun, Jianwei
Copyright Year	2022
Description	A central aim of materials discovery is an accurate and numerically reliable description of thermodynamic properties, such as the enthalpies of formation and decomposition. The r2SCAN revision of the strongly constrained and appropriately normed (SCAN) meta-generalized gradient approximation (meta-GGA) balances numerical stability with high general accuracy. To assess the r2SCAN description of solid-state thermodynamics, we evaluate the formation and decomposition enthalpies, equilibrium volumes, and fundamental band gaps of more than 1000 solids using r2SCAN, SCAN, and PBE, as well as two dispersion-corrected variants, SCAN+rVV10 and r2SCAN+rVV10. We show that r2SCAN achieves accuracy comparable to SCAN and often improves upon SCAN’s already excellent accuracy. Although SCAN+rVV10 is often observed to worsen the formation enthalpies of SCAN and makes no substantial correction to SCAN’s cell volume predictions, r2SCAN+rVV10 predicts marginally less accurate formation enthalpies than r2SCAN, and slightly more accurate cell volumes than r2SCAN. The average absolute errors in predicted formation enthalpies are found to decrease by a factor of 1.5 to 2.5 from the GGA level to the meta-GGA level. Smaller decreases in error are observed for decomposition enthalpies. For formation enthalpies r2SCAN improves over SCAN for intermetallic systems. For a few classes of systems—transition metals, intermetallics, weakly bound solids, and enthalpies of decomposition into compounds—GGAs are comparable to meta-GGAs. In total, r2SCAN and r2SCAN+rVV10 can be recommended as stable, general-purpose meta-GGAs for materials discovery.
Abstract	A central aim ofmaterials discovery is an accurate and numericallyreliable description of thermodynamic properties, such as the enthalpiesof formation and decomposition. The r2SCAN revision ofthe strongly constrained and appropriately normed (SCAN) meta-generalizedgradient approximation (meta-GGA) balances numerical stability withhigh general accuracy. To assess the r2SCAN descriptionof solid-state thermodynamics, we evaluate the formation and decompositionenthalpies, equilibrium volumes, and fundamental band gaps of morethan 1000 solids using r2SCAN, SCAN, and PBE, as well astwo dispersion-corrected variants, SCAN+rVV10 and r2SCAN+rVV10.We show that r2SCAN achieves accuracy comparable to SCANand often improves upon SCAN’s already excellent accuracy.Although SCAN+rVV10 is often observed to worsen the formation enthalpiesof SCAN and makes no substantial correction to SCAN’s cellvolume predictions, r2SCAN+rVV10 predicts marginally lessaccurate formation enthalpies than r2SCAN, and slightlymore accurate cell volumes than r2SCAN. The average absoluteerrors in predicted formation enthalpies are found to decrease bya factor of 1.5 to 2.5 from the GGA level to the meta-GGA level. Smallerdecreases in error are observed for decomposition enthalpies. Forformation enthalpies r2SCAN improves over SCAN for intermetallicsystems. For a few classes of systems—transition metals, intermetallics,weakly bound solids, and enthalpies of decomposition into compounds—GGAsare comparable to meta-GGAs. In total, r2SCAN and r2SCAN+rVV10 can be recommended as stable, general-purpose meta-GGAsfor materials discovery.
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Volume Number	3
DOI	10.1021/acsmaterialsau.2c00059
PubMed Central reference number	PMC9999476
Issue Number	2
PubMed reference number	38089726
Journal	ACS Materials Au [ACS Mater Au]
e-ISSN	26942461
Language	English
Publisher	American Chemical Society
Publisher Date	2022-11-09
Access Restriction	Open
Rights License	Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained (https://creativecommons.org/licenses/by/4.0/). © 2022 The Authors. Published by American Chemical Society
Subject Keyword	density functional theory meta-generalized gradient approximation (meta-GGA) van der Waals interaction formation enthalpy decomposistion enthalpy solid-state materials
Content Type	Text
Resource Type	Article
Subject	Materials Chemistry Biomaterials Polymers and Plastics Electronic, Optical and Magnetic Materials