Scrutinizing the Stability and Exploring the Dependence of Thermoelectric Properties on Band Structure of 3d Metal-Based Double Perovskites: An ab-initio Analysis

Abstract Through the conventional DFT computation, we have designed new oxide double perovskites Ba2BNiO6 (B = Fe and Co). The structural and thermodynamic stabilities are defined by optimizing the crystal energy and determination of tolerance factor and cohesive energies. Thereafter, at the optimized lattice constant, we have explored the different physical properties. The GGA+mBJ electronic band-structure depicts the semiconducting nature for Ba2CoNiO6 while half-metallic with 100% spin polarization for Ba2FeNiO6. The origin of such a diverse band profile upon changing Fe to Co is explained with the help of the orbital diagram and exchange interaction. The eg-eg interaction is strong in these perovskites compared to eg-t2g and t2g-t2g hybridization. The strong exchange interaction among eg states via O-p states happens because the B-O-Ni angle is strictly 180°. Furthermore, due to the narrow bandgaps, we have explored the transport properties to express the applicability of these materials towards thermoelectric technology. Also, herein we have investigated the dependency of transport properties on band profile. The semiconducting nature in Ba2CoNiO6 results in a high ZT~0.8 at room temperature makes it suitable for energy restoration.