Excitations in layered materials from a non-empirical Wannier-localized optimally- tuned screened range-separated hybrid functional

María Camarasa-Gómez*, Stephen E. Gant, Guy Ohad, Jeffrey B. Neaton, Ashwin Ramasubramaniam*, Leeor Kronik*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

Abstract

Accurate prediction of electronic and optical excitations in van der Waals (vdW) materials is a long-standing challenge for density functional theory. The recent Wannier-localized optimally-tuned screened range-separated hybrid (WOT-SRSH) functional has proven successful in non-empirical determination of electronic band gaps and optical absorption spectra for covalent and ionic crystals. However, for vdW materials the tuning of the material- and structure-dependent functional parameters has only been attained semi-empirically. Here, we present a non-empirical WOT-SRSH approach applicable to vdW materials, with the optimal functional parameters transferable between monolayer and bulk. We apply this methodology to prototypical vdW materials: black phosphorus, molybdenum disulfide, and hexagonal boron nitride (in the latter case including zero-point renormalization). We show that the WOT-SRSH approach consistently achieves accuracy levels comparable to experiments and many-body perturbation theory (MBPT) calculations for band structures and optical absorption spectra, both on its own and as an optimal starting point for MBPT calculations.

Original languageEnglish
Article number288
Journalnpj Computational Materials
Volume10
DOIs
Publication statusPublished - 19 Dec 2024

Funding

We thank Prof. Bartomeu Monserrat for very helpful input regarding the effects of ZPR and Dr. Daniel Hernang\u00F3mez-P\u00E9rez for useful discussions. This work was supported by the U.S.-Israel NSF-Binational Science Foundation Grant No. DMR-2015991, by the US Air Force through the grant AFOSR grant FA8655-20-1-7041, and by the Israel Science Foundation. A.R. gratefully acknowledges support from the National Science Foundation (NSF-BSF 2150562). M.C.-G. is grateful to the Azrieli Foundation for the award of an Azrieli International Postdoctoral Fellowship. This work used Frontera at TACC in part through allocation TG-DMR190070 from the Extreme Science and Engineering Discovery Environment (XSEDE), which was supported by National Science Foundation grant number #1548562 and the Advanced Cyberinfrastructure Coordination Ecosystem: Services & Support (ACCESS) program, which is supported by National Science Foundation grants #2138259, #2138286, #2138307, #2137603, and #2138296. Additional computational resources were provided by the Weizmann Institute of Science at Chemfarm. L.K. acknowledges support from the Aryeh and Mintzi Katzman Professorial Chair, and the Helen and Martin Kimmel Award for Innovative Investigation.

All Science Journal Classification (ASJC) codes

  • Modelling and Simulation
  • General Materials Science
  • Mechanics of Materials
  • Computer Science Applications

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