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Title: Performance of the strongly constrained and appropriately normed density functional for solid-state materials

Abstract

Constructed to satisfy 17 known exact constraints for a semilocal density functional, the strongly constrained and appropriately normed (SCAN) meta-generalized-gradient-approximation functional has shown early promise for accurately describing the electronic structure of molecules and solids. One open question is how well SCAN predicts the formation energy, a key quantity for describing the thermodynamic stability of solid-state compounds. To answer this question, we perform an extensive benchmark of SCAN by computing the formation energies for a diverse group of nearly 1000 crystalline compounds for which experimental values are known. Due to an enhanced exchange interaction in the covalent bonding regime, SCAN substantially decreases the formation energy errors for strongly bound compounds, by approximately 50% to 110 meV/atom, as compared to the generalized gradient approximation of Perdew, Burke, and Ernzerhof (PBE). However, for intermetallic compounds, SCAN performs moderately worse than PBE with an increase in formation energy error of approximately 20%, stemming from SCAN's distinct behavior in the weak bonding regime. The formation energy errors can be further reduced via elemental chemical potential fitting. We find that SCAN leads to significantly more accurate predicted crystal volumes, moderately enhanced magnetism, and mildly improved band gaps as compared to PBE. Altogether, SCAN represents amore » significant improvement in accurately describing the thermodynamics of strongly bound compounds.« less

Authors:
ORCiD logo [1];  [1]
  1. Northwestern Univ., Evanston, IL (United States)
Publication Date:
Research Org.:
Northwestern Univ., Evanston, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1457131
Alternate Identifier(s):
OSTI ID: 1456297
Grant/Contract Number:  
SC0015106; AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review Materials
Additional Journal Information:
Journal Volume: 2; Journal Issue: 6; Journal ID: ISSN 2475-9953
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Isaacs, Eric B., and Wolverton, Chris. Performance of the strongly constrained and appropriately normed density functional for solid-state materials. United States: N. p., 2018. Web. doi:10.1103/PhysRevMaterials.2.063801.
Isaacs, Eric B., & Wolverton, Chris. Performance of the strongly constrained and appropriately normed density functional for solid-state materials. United States. doi:10.1103/PhysRevMaterials.2.063801.
Isaacs, Eric B., and Wolverton, Chris. Fri . "Performance of the strongly constrained and appropriately normed density functional for solid-state materials". United States. doi:10.1103/PhysRevMaterials.2.063801. https://www.osti.gov/servlets/purl/1457131.
@article{osti_1457131,
title = {Performance of the strongly constrained and appropriately normed density functional for solid-state materials},
author = {Isaacs, Eric B. and Wolverton, Chris},
abstractNote = {Constructed to satisfy 17 known exact constraints for a semilocal density functional, the strongly constrained and appropriately normed (SCAN) meta-generalized-gradient-approximation functional has shown early promise for accurately describing the electronic structure of molecules and solids. One open question is how well SCAN predicts the formation energy, a key quantity for describing the thermodynamic stability of solid-state compounds. To answer this question, we perform an extensive benchmark of SCAN by computing the formation energies for a diverse group of nearly 1000 crystalline compounds for which experimental values are known. Due to an enhanced exchange interaction in the covalent bonding regime, SCAN substantially decreases the formation energy errors for strongly bound compounds, by approximately 50% to 110 meV/atom, as compared to the generalized gradient approximation of Perdew, Burke, and Ernzerhof (PBE). However, for intermetallic compounds, SCAN performs moderately worse than PBE with an increase in formation energy error of approximately 20%, stemming from SCAN's distinct behavior in the weak bonding regime. The formation energy errors can be further reduced via elemental chemical potential fitting. We find that SCAN leads to significantly more accurate predicted crystal volumes, moderately enhanced magnetism, and mildly improved band gaps as compared to PBE. Altogether, SCAN represents a significant improvement in accurately describing the thermodynamics of strongly bound compounds.},
doi = {10.1103/PhysRevMaterials.2.063801},
journal = {Physical Review Materials},
number = 6,
volume = 2,
place = {United States},
year = {2018},
month = {6}
}

Journal Article:
Free Publicly Available Full Text
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Cited by: 18 works
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Figures / Tables:

FIG. 1. FIG. 1.: Jacob’s ladder framework for describing different levels of sophistication and accuracy of Exc in density functional theory. Starting from the Hartree level of theory (Exc = 0)and attempting to climb towards chemical accuracy, each rung of the ladder labeled on the left corresponds to additional dependencies of Excmore » indicated on the right. The top rung listed is the random phase approximation (RPA). Figure is based on Refs. 3 and 4. We note that additional methodologies have been described as rungs in between meta- and hyper-GGA not shown here [5, 6].« less

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    Works referencing / citing this record:

    Rationalizing accurate structure prediction in the meta-GGA SCAN functional
    journal, July 2019


      Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.