Thermal conductivity of ordered-disordered material: a case study of superionic Ag2Te.

Thermoelectric devices, which can generate electricity from waste heat, offer an attractive pathway for addressing an important niche in the globally growing landscape of energy demand. In the past few decades, the search for high-efficiency thermoelectrics has been guided by the concept of 'phonon-glass electron-crystal' (PGEC), i.e. an ideal thermoelectric material should have high carrier mobility and low thermal conductivity. Although remarkable progress has already been made along this line, the efficiency of thermoelectrics is still too poor to compete with other electricity producing methods. Ordered-disordered material, an emerging trend of high performance thermoelectrics under the concept of PGEC, is a new hot topic in the current thermoelectric research community. Taking superionic phase silver telluride (α-Ag2Te) as an example, we performed a comprehensive study of the thermal transport properties and of its physical mechanism by means of equilibrium molecular dynamic simulations. The results show that the thermal conductivity of α-Ag2Te is intrinsically very low. By analyzing the different contributions to the overall thermal conductivity, we revealed for the first time from atomistic simulations that the vibration of the Te(2-) sublattice dominates the thermal transport of α-Ag2Te, while the collision between the randomly diffusing Ag(+) ions and the Te(2-) sublattice yields a significant negative contribution to the thermal transport. We also studied the effect of isotropic compressive stain and carrier concentration on the thermal conductivity of α-Ag2Te. It has been found that the thermal conductivity can be largely reduced by applying compressive strain or with stoichiometric quantity modulation. Our studies shed light on the governing mechanism of thermal transport in ordered-disordered materials and could offer useful guidance for engineering the thermal transport properties of superionic conductors in terms of enhancing their thermoelectric performance.