Reliable Density Functional Theory Predictions of Bandgaps for Materials

Fuente: arXiv
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Main Authors: Lu, Chenxi, Li, Musen, Ford, Michael J., Kobayashi, Rika, Amos, Roger, Reimers, Jeffrey R.
Format: Preprint
Published: 2025
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_version_ 1866908649199239168
author Lu, Chenxi
Li, Musen
Ford, Michael J.
Kobayashi, Rika
Amos, Roger
Reimers, Jeffrey R.
author_facet Lu, Chenxi
Li, Musen
Ford, Michael J.
Kobayashi, Rika
Amos, Roger
Reimers, Jeffrey R.
contents We consider methods for optimizing the bandgap calculation of 3D materials, considering 340 sample materials. Examined are the effects of the choice of the pseudopotential to describe core electrons, the plane-wave basis set cutoff energy, and the Brillouin zone integration. Cost-saving calculations in which the structure is optimized using reduced-quality Brillouin zone integrations and cutoff energies were found to lead to experimentally significant errors exceeding 0.1 eV in 18% of cases using the PBE functional and 21% of cases using PBE0. Such cost-savings approaches are therefore not recommended for general applications. Also, the current practice of using unoptimized grids to perform the Brillouin-zone integrations in bandgap calculations is found to be unreliable for 16% of materials using PBE and for 23% using PBE0. A k-space optimization scheme is introduced that interpolates extensive PBE results to determine a generally useful approach that when used in PBE0 calculations is found to be inadequate for only 1.6% of the materials studied.
format Preprint
id arxiv_https___arxiv_org_abs_2501_15811
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Reliable Density Functional Theory Predictions of Bandgaps for Materials
Lu, Chenxi
Li, Musen
Ford, Michael J.
Kobayashi, Rika
Amos, Roger
Reimers, Jeffrey R.
Materials Science
We consider methods for optimizing the bandgap calculation of 3D materials, considering 340 sample materials. Examined are the effects of the choice of the pseudopotential to describe core electrons, the plane-wave basis set cutoff energy, and the Brillouin zone integration. Cost-saving calculations in which the structure is optimized using reduced-quality Brillouin zone integrations and cutoff energies were found to lead to experimentally significant errors exceeding 0.1 eV in 18% of cases using the PBE functional and 21% of cases using PBE0. Such cost-savings approaches are therefore not recommended for general applications. Also, the current practice of using unoptimized grids to perform the Brillouin-zone integrations in bandgap calculations is found to be unreliable for 16% of materials using PBE and for 23% using PBE0. A k-space optimization scheme is introduced that interpolates extensive PBE results to determine a generally useful approach that when used in PBE0 calculations is found to be inadequate for only 1.6% of the materials studied.
title Reliable Density Functional Theory Predictions of Bandgaps for Materials
topic Materials Science
url https://arxiv.org/abs/2501.15811