Accelerated Discovery of a Large Family of Quaternary Chalcogenides with very Low Lattice Thermal Conductivity

Abstract: The development of efficient thermal energy management devices such as thermoelectrics, barrier coatings, and thermal data-storage disks often relies on compounds that possess very low lattice thermal conductivity ($\kappa_l$). Here, we present the computational prediction of a large family of 628 thermodynamically stable quaternary chalcogenides, AMM'Q$_3$ (A = alkali/alkaline earth/post-transition metals; M/M' = transition metals, lanthanides; Q = chalcogens) using high-throughput density functional theory (DFT) calculations. We validate the presence of low-$\kappa_l$ in this family of materials by calculating $\kappa_l$ of several predicted stable compounds using the Peierls-Boltzmann transport equation within a first-principles DFT framework. Our analysis reveals that the low-$\kappa_l$ in the AMM'Q$_3$ compounds originates from the presence of either a strong lattice anharmonicity that enhances the phonon scatterings or rattlers cations that lead to multiple scattering channels in their crystal structures. Our predictions suggest new experimental research opportunities in the synthesis and characterization of these stable, low-$\kappa_l$ compounds.