Computational Exploration of the Binary A₁B₁ Chemical Space for Thermoelectric Performance

In spite of the emergence of chemically complex thermoelectric materials, compounds with simple binary A 1 B 1 chemistry continue to dominate the highest zT thermoelectric materials. To understand the structure–property relations that drive this propensity, we employed a descriptor that combines ab initio calculations and modeled electron and phonon transport to offer a reliable assessment of the intrinsic material properties that govern the thermoelectric figure of merit zT . We evaluated the potential for thermoelectric performance of 518 A 1 B 1 chemistries in 1508 different structures and found that good thermoelectric performance of A 1 B 1 compounds originates mainly from low valent ions in combination with cubic and orthorhombic crystal structures, which primarily offer favorable charge carrier transport properties. Additionally, we have identified promising new A 1 B 1 compounds, including their higher-energy polymorphs.