High throughput screening of semiconductors with low lattice thermal transport induced by long-range interactions

Abstract

Semiconductors with long-range interactions (LRI) due to resonant bonding exhibit delocalized electronic states and low lattice thermal conductivity, contributing to the efficiency of heat-to-electricity conversion. Here, we build a descriptor for high-throughput screening of LRI materials from the second-order interaction force constants. We identify 75 semiconducting candidates from the binary compounds in the MatHub-3d database that contain LRI. By analyzing the bonding properties of LRI atoms, we classify LRI in materials into two categories: type I and type II. In the structural unit of type I LRI, the atoms have strong bond connections, while a weak bond exists between the two groups in the structural unit of type II LRI. We have identified atypical type I LRI formed by Sb–Sb and Mg–Mg pairs in the emerging thermoelectric material Mg₃Sb₂, resulting in the softening of TA₁ phonons and large anharmonicity. For type II LRI, the LRI of Ge–Ge and Se–Se pairs in R3m-GeSe can cross different layers. Moreover, we observe a combination of type II LRI and rattling effect in BaSe₂ to restrict thermal transport. This work is of great significance for understanding the relationship between LRI and thermal transport properties, and for designing new LRI-induced low lattice thermal conductivity materials.