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Reliable Density Functional Theory Predictions of Bandgaps for Materials

2025/01/27 by Chenxi Lu, Lu, Chenxi, Musen Li +9 · 1 citation
Materials Science · #FOS: Physical sciences #Materials Science (cond-mat.mtrl-sci) #Thermal Expansion and Ionic Conductivity

paper · pdf · doi:10.48550/arxiv.2501.15811

openalex publication_date 2025/01/27 · openalex created_date 2025/10/10 · openalex updated_date 2026/07/30

Abstract

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.

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