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Abstract

The intrinsically low lattice thermal conductivity κL is essentially important for thermoelectric technology to maintain large working temperature difference, in order to enlarge the output power. In principle, high density and complex structure at atomic and nano scale are typical features for thermoelectric materials with low lattice thermal conductivities (κLs). However, many 122-phase Zintl compounds with promising thermoelectric properties defy these paradigms. They adopt three relatively simple structures with comparably small mean atomic mass, while these compounds exhibit considerably low lattice thermal conductivities κLs. Herein we unveil the origins of low κLs in 122-phase Zintl compounds, ascribed from the important aspects including atomic constituents, their arrangements and chemical bonding. The coupling between the acoustic branches and low-frequency optical branches, as well as the anisotropic chemical bonding are responsible for the high anharmonicity, favoring for the low phonon velocity and small relaxation time. This work offers a guidance to design high-performance Zintl thermoelectric materials with ultralow lattice thermal conductivity. © 2021