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)