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Inverse Design of Ultralow Lattice Thermal Conductivity Materials Via Lone Pair Cation Coordination Environment

The presence of lone pair (LP) electrons is strongly associated with the disruption of lattice heat transport, which is a critical component of strategies to achieve efficient thermoelectric energy conversion. By exploiting an empirical relationship between lattice thermal conductivity $κ_L$ and the bond angles of pnictogen group LP cation coordination environments, we develop an inverse design strategy based on a materials database screening to identify chalcogenide materials with ultralow $κ_L$ for thermoelectrics. Screening the $\sim$ 635,000 real and hypothetical inorganic crystals of the Open Quantum Materials Database based on the constituent elements, nominal electron counting, LP cation coordination environment, and synthesizability, we identify 189 compounds expected to exhibit ultralow $κ_L$. As a validation, we explicitly compute the lattice dynamical properties of two of the compounds (Cu$_2$AgBiPbS$_4$ and MnTl$_2$As$_2$S$_5$) using first-principles calculations and successfully find both achieve ultralow $κ_L$ values at room temperature of $\sim$ 0.3--0.4 W/(m$\cdot$K) corresponding to the amorphous limit. Our data-driven approach provides promising candidates for thermoelectric materials and opens new avenues for the design of phononic properties of materials.