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 often relies on semiconductors with very low lattice thermal conductivity (κ_L). Here, we present the discovery of 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 very large number of thermodynamically stable chalcogenides. Our materials design strategy relies on successive phase stability screening based on the calculated enegetics of all known crystallographic prototypes in the family of experimentally known AMM'Q₃ compounds. We validate the presence of very low κ_L in this chalcogenides family by calculating the κ_L of several predicted stable compounds using the Peierls-Boltzmann transport equation for phonos in a first-principles framework. Our predictions suggest new experimental research opportunities in the synthesis and characterization of these stable, low-κ_L compounds.