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

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 Pb²⁺ reduces vacancy scattering, resulting in a high carrier mobility of ∼3400 cm² 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 cm² V^-1 s^-1 is obtained for Pb_1.01Te + 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 ∼10¹⁹ 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_1.01Te_0.998I_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.