Lattice thermal transport in group II-alloyed PbTe

Abstract: PbTe, one of the most promising thermoelectric materials, has recently demonstrated thermoelectric figure of merit ($ZT$) of above 2.0 when alloyed with group II elements. The improvements are due mainly to significant reduction of lattice thermal conductivity ($\kappa_{l}$), which was in turn attributed to nanoparticle precipitates. However, a fundamental understanding of various phonon scattering mechanisms within the bulk alloy is still lacking. In this work, we apply the newly-developed density-functional-theory (DFT)-based compressive sensing lattice dynamics (CSLD) approach to model lattice heat transport in PbTe, MTe, and Pb${0.94}$M${0.06}$Te (M=Mg, Ca, Sr and Ba), compare our results with experimental measurements, with focus on strain effect and mass disorder scattering. We find that (1) CaTe, SrTe and BaTe in the rock-salt structure exhibit much higher $\kappa_{l}$ than PbTe, while MgTe in the same structure shows anomalously low $\kappa_{l}$; (2) lattice heat transport of PbTe is extremely sensitive to static strain induced by alloying atoms in solid solution form; (3) mass disorder scattering plays a major role in reducing $\kappa_{l}$ for Mg/Ca/Sr-alloyed PbTe through strongly suppressing the lifetimes of intermediate- and high-frequency phonons, while for Ba-alloyed PbTe, precipitated nanoparticles are also important.