Non-empirical prediction of electronic and optical properties of van der Waals materials from a Wannier-localized Optimally Tuned Screened Range-Separated Hybrid functional*

There is wide interest in the electronic and optical properties of van der Waals (vdW) materials. Accurately predicting these properties with density functional theory, however, has been difficult. Wannier-localized, optimally tuned, screened range-separated hybrid (WOT-SRSH) functionals [1] have been used successfully for determining the electronic band gaps and optical absorption spectra of a variety of materials [1-3]. However, for vdW materials only semi-empirical approaches have been used, to date, to tune the material- and structure-dependent functional parameters [4, 5]. Here, we develop and apply a fully non-empirical WOT-SRSH approach for determining the functional parameters and we show, using several prototypical vdW materials, that this approach yields a level of accuracy comparable to that of ab initio many-body perturbation theory.

 

[1] Wing et al., PNAS 118, e2104556118 (2021)

[2] Ohad et al., Phys. Rev. Materials 6, 104606 (2022)

[3] Ohad et al., arXiv:2309.02117 (2023)

[4] Ramasubramaniam et al., Phys. Rev. Materials 3, 084007 (2019)

[5] Camarasa-Gómez et al., Phys. Rev. Materials 7, 104001 (2023)