Realizing High‐Ranged Out‐of‐Plane ZTs in N‐Type SnSe Crystals through Promoting Continuous Phase Transition

Thermoelectric technology enables direct conversion between heat and electricity. The conversion efficiency of a thermoelectric device is determined by the average dimensionless figure of merit ZTave. Here, a record high ZTave of ≈1.34 in the range of 300–723 K in n‐type SnSe based crystals is reported. The remarkable thermoelectric performance derives from the high power factor and the reduced thermal conductivity in the whole temperature range. The high power factor is realized by promoting the continuous phase transition in SnSe crystals through alloying PbSe, which results in a higher symmetry of the crystal structure and the correspondingly modified electronic band structure. Moreover, PbSe alloying induces mass and strain fluctuations, which enables the suppression of thermal transport. These findings provide a new strategy to enhance the thermoelectric performance for the continuous phase transition materials. SnSe–xPbSe crystals with a record high ZTave of ≈1.34 in the range of 300–723 K are presented. The outstanding thermoelectric performance derives from the countinous phase transition, which results in the significant crystal symmetry enhancement and the corresponding band structures modification. Our findings provide a new strategy to enhance the thermoelectric performance for the continuous phase transition materials.