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The discovery of high thermoelectric performance in n-type polycrystallineMg3(Sb,Bi)2 based Zintl compounds has ignited intensive research interest.However, some fundamental questions concerning the anisotropic transportproperties and the origin of intrinsically low thermal conductivity are stillelusive, requiring the investigation of single crystals. In this work,high-quality p-type Mg3Sb2 and Mg3Bi2 single crystals have been grown by usinga self-flux method. The electrical resistivity \r{ho} of Mg3Bi2 single crystaldisplays an anisotropy with \r{ho} in-plane twice larger than out-of-plane. Thelow-temperature heat capacity and lattice thermal conductivity of Mg3Sb2 andMg3Bi2 single crystals have been investigated by using the Debye-Callawaymodel, from which the existence of low-lying vibration mode could be concluded.Large Gr\"uneisen parameters and strong anharmonicity are found responsible forthe intrinsically low thermal conductivity. Moreover, grain boundary scatteringdoes not contribute significantly to suppress the lattice thermal conductivityof polycrystalline Mg3Sb2. Our results provide insights into the intrinsictransport properties of Mg3X2 and could pave a way to realize enhancedthermoelectric performance in single-crystalline Mg3X2-based Zintl compounds.

Growth and transport properties of Mg3X2 (X = Sb, Bi) single crystals