Exploiting the fascinating properties of materials near soft mode phase transitions is an emerging concept in the quest to increase thermoelectric efficiency [1,2]. The underlying idea is that soft phonons lead to intrinsically low thermal conductivity, while possibly preserving electronic transport properties. Using first principles simulations, we show that driving PbTe near the transition from the rocksalt to a rhombohedral structure will significantly reduce its lattice thermal conductivity. We illustrate this concept by applying biaxial tensile (001) strain to both PbTe and its alloy with rocksalt PbSe, and also by alloying PbTe with rhombohedral GeTe [3]. Moreover, we investigate in detail how tuning the proximity to the soft optical mode phase transition via chemical composition affects the lattice thermal conductivity of (Pb,Ge)Te alloys [4]. We show that the anharmonic contribution to the lattice thermal conductivity is minimized at the phase transition due to the maximized acoustic-optical interaction. Furthermore, mass disorder shifts the conductivity minimum towards the composition at which the scattering due to mass disorder is maximized. The total lattice thermal conductivity and its anharmonic contribution vary continuously between the rocksalt and rhombohedral phases as expected for the second-order phase transition. Our results show that alloys with soft optical mode transitions are promising materials for achieving low thermal conductivity and possibly high thermoelectric efficiency.

[1] D. T. Morelli, V. Jovovic, and J. P. Heremans, Phys. Rev. Lett. 101, 035901 (2008).

[2] L.-D. Zhao et al, Nature 508, 373 (2014).

[3] R. M. Murphy, E. D. Murray, S. Fahy, and I. Savic, Phys. Rev. B 93, 104304 (2016).

[4] R. M. Murphy, E. D. Murray, S. Fahy, and I. Savic, Phys. Rev. B 95, 144302 (2017).