Computational Discovery of an Enormous Class of Stable Quaternary Chalcogenides with Very Low Lattice Thermal Conductivity

The development of efficient thermal energy management devices such as thermoelectrics, barrier coatings, and thermal data storage disks relies on compounds which possess low lattice thermal conductivity (κ_l ). Here, we present an enormous class of thermodynamically stable quaternary chalcogenides AMM'Q₃ (A=Alkali, alkaline earth, post transition metals; M,M'=transition metals, lanthanides; Q= chalcogens) that possess intrinsically low κ_l using high-throughput DFT calculations. Leveraging the computed energetics of hundreds of thousands of multinary compounds in the Open Quantum Materials Database (OQMD), we discovered a large number (nearly 1000) of thermodynamically stable chalcogenides through successive screening based on the calculations on multiple crystallographic prototypes of the experimentally known AMM'Q₃ compounds. We validate the low-κ_l in this family of compounds by calculating the lattice thermal conductivity taking several representative compounds using the highly accurate anharmonic lattice dynamics methods. Our predictions suggest new experimental research opportunities in the synthesis and characterization of these stable, low-κ_l compounds.