Abstract
Accurate prediction of fundamental band gaps of crystalline solid-state systems entirely within density functional theory is a long-standing challenge. Here, we present a simple and inexpensive method that achieves this by means of nonempirical optimal tuning of the parameters of a screened range-separated hybrid functional. The tuning involves the enforcement of an ansatz that generalizes the ionization potential theorem to the removal of an electron from an occupied state described by a localized Wannier function in a modestly sized supercell calculation. The method is benchmarked against experiment for a set of systems ranging from narrow band-gap semiconductors to large band-gap insulators, spanning a range of fundamental band gaps from 0.2 to 14.2 electronvolts (eV), and is found to yield quantitative accuracy across the board, with a mean absolute error of ∼0.1 eV and a maximal error of ∼0.2 eV.
| Original language | English |
|---|---|
| Article number | e2104556118 |
| Number of pages | 8 |
| Journal | Proceedings of the National Academy of Sciences of the United States of America |
| Volume | 118 |
| Issue number | 34 |
| Early online date | 20 Aug 2021 |
| DOIs | |
| Publication status | Published - 24 Aug 2021 |
Funding
This work was supported via US-Israel NSF-Binational Science Foundation (BSF) Grant DMR-1708892 and by the Israel Ministry of Defense. Computational resources were provided by the National Energy Research Scientific Computing Center, DOE Office of Science User Facilities supported by the Office of Science of the US Department of Energy under Contract DE-AC02-05CH11231. Additional computational resources were provided by the Extreme Science and Engineering Discovery Environment (XSEDE) supercomputer Stampede2 at the Texas Advanced Computing Center (TACC) through the allocation TG-DMR190070. Publisher Copyright: © 2021 National Academy of Sciences. All rights reserved.
All Science Journal Classification (ASJC) codes
- General