Putting error bars on density functional theory

Simuck F. Yuk; Irmak Sargin; Noah Meyer; Jaron T. Krogel; Scott P. Beckman; Valentino R. Cooper

doi:10.1038/s41598-024-69194-w

Putting error bars on density functional theory

Simuck F. Yuk, Irmak Sargin, Noah Meyer, Jaron T. Krogel, Scott P. Beckman, Valentino R. Cooper

Research output: Contribution to journal › Article › peer-review

3 Scopus citations

Abstract

Predicting the error in density functional theory (DFT) calculations due to the choice of exchange–correlation (XC) functional is crucial to the success of DFT, but currently, there are limited options to estimate this a priori. This is particularly important for high-throughput screening of new materials. In this work, the structure and elastic properties of binary and ternary oxides are computed using four XC functionals: LDA, PBE-GGA, PBEsol, and vdW-DF with C09 exchange. To analyze the systemic errors inherent to each XC functional, we employed materials informatics methods to predict the expected errors. The predicted errors were also used to better the DFT-predicted lattice parameters. Our results emphasize the link between the computed errors and the electron density and hybridization errors of a functional. In essence, these results provide “error bars” for choosing a functional for the creation of high-accuracy, high-throughput datasets as well as avenues for the development of XC functionals with enhanced performance, thereby enabling the accelerated discovery and design of new materials.

Original language	English
Article number	20219
Journal	Scientific Reports
Volume	14
Issue number	1
DOIs	https://doi.org/10.1038/s41598-024-69194-w
State	Published - Dec 2024

Funding

S.F.Y., J.T.K. and V.R.C. (first principles calculations and high-throughput workflow efforts) were supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. I.S. and S.P.B. (data analytics) were supported in part by the U.S. Department of Energy under contract 89304017CEM000001. N.M. acknowledges summer support through the ORNL HERE Program, sponsored by the U.S. Department of Energy and administered by the Oak Ridge Institute for Science and Education. We gratefully acknowledge the computational resources provided by the National Energy Research Scientific Computing Center (NERSC), which is supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. The opinions expressed herein are those of the authors and not necessarily representative of those of the Department of the Army, Department of Defense (DoD), or U.S. Government.

Funders	Funder number
Basic Energy Sciences
Oak Ridge National Laboratory
U.S. Department of Energy
Office of Science
U.S. Department of Defense
Division of Materials Sciences and Engineering	89304017CEM000001
Oak Ridge Institute for Science and Education	DE-AC02-05CH11231

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title = "Putting error bars on density functional theory",

abstract = "Predicting the error in density functional theory (DFT) calculations due to the choice of exchange–correlation (XC) functional is crucial to the success of DFT, but currently, there are limited options to estimate this a priori. This is particularly important for high-throughput screening of new materials. In this work, the structure and elastic properties of binary and ternary oxides are computed using four XC functionals: LDA, PBE-GGA, PBEsol, and vdW-DF with C09 exchange. To analyze the systemic errors inherent to each XC functional, we employed materials informatics methods to predict the expected errors. The predicted errors were also used to better the DFT-predicted lattice parameters. Our results emphasize the link between the computed errors and the electron density and hybridization errors of a functional. In essence, these results provide “error bars” for choosing a functional for the creation of high-accuracy, high-throughput datasets as well as avenues for the development of XC functionals with enhanced performance, thereby enabling the accelerated discovery and design of new materials.",

author = "Yuk, {Simuck F.} and Irmak Sargin and Noah Meyer and Krogel, {Jaron T.} and Beckman, {Scott P.} and Cooper, {Valentino R.}",

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doi = "10.1038/s41598-024-69194-w",

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AU - Sargin, Irmak

AU - Meyer, Noah

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AU - Beckman, Scott P.

AU - Cooper, Valentino R.

PY - 2024/12

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Putting error bars on density functional theory

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