Fine Tuning of Defects Enables High Carrier Mobility and Enhanced Thermoelectric Performance of n-Type PbTe

High Resolution Image Download MS PowerPoint Slide High carrier mobility is critical to improving thermoelectric performance over a broad temperature range. However, traditional doping inevitably deteriorates carrier mobility. Herein, we develop a strategy for fine tuning of defects to improve carrier mobility. To begin, n-type PbTe is created by compensating for the intrinsic Pb vacancy in bare PbTe. Excess Pb 2+ reduces vacancy scattering, resulting in a high carrier mobility of ∼3400 cm 2 V –1 s –1 . Then, excess Ag is introduced to compensate for the remaining intrinsic Pb vacancies. We find that excess Ag exhibits a dynamic doping process with increasing temperatures, increasing both the carrier concentration and carrier mobility throughout a wide temperature range; specifically, an ultrahigh carrier mobility ∼7300 cm 2 V –1 s –1 is obtained for Pb 1.01 Te + 0.002Ag at 300 K. Moreover, the dynamic doping-induced high carrier concentration suppresses the bipolar thermal conductivity at high temperatures. The final step is using iodine to optimize the carrier concentration to ∼10 19 cm –3 . Ultimately, a maximum ZT value of ∼1.5 and a large average ZT ave value of ∼1.0 at 300–773 K are obtained for Pb 1.01 Te 0.998 I 0.002 + 0.002Ag. These findings demonstrate that fine tuning of defects with <0.5% impurities can remarkably enhance carrier mobility and improve thermoelectric performance.