Tailoring Cage-Like Motifs for Enhanced Thermoelectric Performance

Traditional thermoelectrics commonly achieve either promising electronic properties or low thermal conductivity but rarely excel in both. In this study, we introduce a novel approach to thermoelectric materials design that addresses the challenge of optimizing thermal and electronic properties simultaneously. Inspired by the assembly principles of molecular organic frameworks, we computationally design materials by stitching atomic clusters to enhance thermoelectric performance. Our approach introduces a new class of materials featuring transition metals, chalcogenides, and main group elements, structured with molecular frameworks embedded in a solid matrix that naturally exhibits low lattice thermal conductivity. Through structural reconstruction and electronic structure optimization, we achieve enhanced power factors that maximize the thermoelectric figure of merit (zT). These compounds represent promising candidates for next-generation thermoelectric applications, advancing atomic-scale design in energy materials.