Electronic structure fingerprints of visible-range excitons in $d^0$ double perovskite oxides

Abstract

Presence of excitons significantly influence the optoelectronic properties and potential applications of materials. Using combined theoretical and experimental tools, we investigate the absorption spectra of $d^0$ double perovskite oxides Ba$_{2}$Y$B'$O$_6$ ($B'$ = Nb, Ta, Sb), Ba$_{2}$Sc$B'$O$_6$ ($B'$ = Ta, Sb) and $A_{2}$ScSbO$_6$ ($A$=Ca, Sr, Ba), allowing for a systematic variation of composition. We not only show that low-energy excitons possessing large binding energies up to 3 eV are present in the visible range in all the considered wide-gap insulators, but also that the nature and properties of these excitons differs from those in double perovskite halides as well as perovskite oxides. We provide insights on the origin of such differences by a comparative analysis of the electronic structure. Our findings elucidate possible correlations between the exciton properties and the composition, via the electronic structure, towards a comprehensive understanding of correlation effects and rational design principles.