Optical absorption spectra of metal oxides from time-dependent density functional theory and many-body perturbation theory based on optimally-tuned hybrid functionals
Guy Ohad, Stephen E. Gant, Dahvyd Wing, Jonah B. Haber, María Camarasa‐Gómez, Francisca Sagredo, Marina R. Filip, Jeffrey B. Neaton, Leeor Kronik
Abstract
Using both time-dependent density functional theory (TDDFT) and the ``single-shot'' GW plus Bethe-Salpeter equation (GW-BSE) approach, we compute optical band gaps and optical absorption spectra from first principles for eight common binary and ternary closed-shell metal oxides (MgO, ${\mathrm{Al}}_{2}{\mathrm{O}}_{3}$, CaO, ${\mathrm{TiO}}_{2}, {\mathrm{Cu}}_{2}\mathrm{O}$, ZnO, ${\mathrm{BaSnO}}_{3}$, and ${\mathrm{BiVO}}_{4}$), based on the nonempirical Wannier-localization-based, optimally tuned, screened range-separated hybrid functional. Overall, we find excellent agreement between our TDDFT and GW-BSE results and experiment, with a mean absolute error smaller than 0.4 eV, including for ${\mathrm{Cu}}_{2}\mathrm{O}$ and ZnO that are traditionally considered to be challenging for both methods.