TY - JOUR
T1 - Right band gaps for the right reason at low computational cost with a meta-GGA
AU - Lebeda, Timo
AU - Aschebrock, Thilo
AU - Sun, Jianwei
AU - Leppert, Linn
AU - Kümmel, Stephan
N1 - Funding Information:
S.K. and T.L. appreciate financial support from the Deutsche Forschungsgemeinschaft, DFG Project No. KU 1410/4-1, and from the Bavarian State Ministry of Science, Research, and the Arts for the Collaborative Research Network “Solar Technologies go Hybrid.” L.L. acknowledges funding from the Dutch Research Council (NWO) under Grant No. OCENW.M20.337. S.K. and T.L. are further grateful for support from the Elite Study Program “Biological Physics” of the Elite Network of Bavaria, and T.L. acknowledges discussions with Pier Philippsen on generating data for plots with band . J.S. acknowledges the support of the U.S. DOE, Office of Science, Basic Energy Sciences Grant No. DE-SC0019350.
Publisher Copyright:
© 2023 American Physical Society.
PY - 2023/9/19
Y1 - 2023/9/19
N2 - In density functional theory, traditional explicit density functionals such as the local density approximation and generalized gradient approximations cannot accurately predict the band gap of solids for a fundamental reason: They lack the exchange-correlation derivative discontinuity. By comparing Kohn-Sham and generalized Kohn-Sham calculations, we here show that the nonempirical meta-generalized-gradient-approximation (meta-GGA) TASK from Aschebrock and Kümmel [Phys. Rev. Res. 1, 033082 (2019)2643-156410.1103/PhysRevResearch.1.033082] predicts the right gaps for the right reason, i.e., as a combination of a proper Kohn-Sham gap and a substantial derivative discontinuity contribution. For many materials from small-gap semiconductors to large-gap insulators, the proper band gap is thus obtained. We further study a group of metal-halide perovskites for which the band gap is notoriously hard to predict. For these materials, TASK yields band gaps very similar to the nonlocal screened hybrid Heyd-Scuseria-Ernzerhof functional, yet at a fraction of the hybrid functional's computational cost. We discuss the influence of correlation functionals, and open questions in the comparison of calculated band gaps with experimental ones.
AB - In density functional theory, traditional explicit density functionals such as the local density approximation and generalized gradient approximations cannot accurately predict the band gap of solids for a fundamental reason: They lack the exchange-correlation derivative discontinuity. By comparing Kohn-Sham and generalized Kohn-Sham calculations, we here show that the nonempirical meta-generalized-gradient-approximation (meta-GGA) TASK from Aschebrock and Kümmel [Phys. Rev. Res. 1, 033082 (2019)2643-156410.1103/PhysRevResearch.1.033082] predicts the right gaps for the right reason, i.e., as a combination of a proper Kohn-Sham gap and a substantial derivative discontinuity contribution. For many materials from small-gap semiconductors to large-gap insulators, the proper band gap is thus obtained. We further study a group of metal-halide perovskites for which the band gap is notoriously hard to predict. For these materials, TASK yields band gaps very similar to the nonlocal screened hybrid Heyd-Scuseria-Ernzerhof functional, yet at a fraction of the hybrid functional's computational cost. We discuss the influence of correlation functionals, and open questions in the comparison of calculated band gaps with experimental ones.
UR - http://www.scopus.com/inward/record.url?scp=85173015964&partnerID=8YFLogxK
U2 - 10.1103/PhysRevMaterials.7.093803
DO - 10.1103/PhysRevMaterials.7.093803
M3 - Article
AN - SCOPUS:85173015964
SN - 2475-9953
VL - 7
JO - Physical Review Materials
JF - Physical Review Materials
IS - 9
M1 - 093803
ER -