Multiple low-energy excitons and optical response of $d^0$ double perovskite Ba$_2$ScTaO$_6$

Abstract

Large bandgap insulators are considered promising for applications such as photocatalysts, dielectric resonators and interference filters. Based on synchrotron X-ray diffraction, diffuse reflectance measurement and density functional theory, we report the crystal structure, optical response, and electronic properties of the synthesized $d^0$ double perovskite Ba$_2$ScTaO$_6$. In contrast to earlier prediction, the electronic bandgap is found to be large, $\sim 4.66$ eV. The optical response is characterized by the presence of multiple exciton modes extending up to the visible range. A detailed investigation of the direct gap excitons based on the Elliot formula is presented. Density functional theory based investigation of the electronic properties within generalized gradient approximation severely underestimates the electronic gap. To reach a quantitative agreement, we consider different available flavors of the modified-Becke-Johnson exchange-correlation potential and discuss their effects on the electronic and optical properties.