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

Manish Kothakonda, Aaron D. Kaplan, Eric B. Isaacs, Christopher J. Bartel, James W. Furness, Jinliang Ning, Chris Wolverton, John P. Perdew, Jianwei Sun

Research output: Contribution to journalArticlepeer-review

14 Scopus citations

Abstract

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.

Original languageEnglish (US)
Pages (from-to)102-111
Number of pages10
JournalACS Materials Au
Volume3
Issue number2
DOIs
StatePublished - Mar 8 2023

Bibliographical note

Publisher Copyright:
© 2022 The Authors. Published by American Chemical Society.

Keywords

  • decomposistion enthalpy
  • density functional theory
  • formation enthalpy
  • meta-generalized gradient approximation (meta-GGA)
  • solid-state materials
  • van der Waals interaction

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