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.