摘要
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.
基金
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
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
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。
