A nanoscale perspective of the coexistence of multidimensional defects in the AgCuTe system

Abstract

AgCuTe, a p-type medium-temperature thermoelectric material, exhibits great potential as a candidate for converting waste heat into electricity owing to its low thermal conductivity and high thermoelectric performance. However, an unstable phase structure of the material system has hindered the direct observation of various point defects contacting with high performance, despite their predicted possibilities solely based on first-principles calculations. Here, we present the novel observation of Te interstitial atoms together with other point defects, planar defects, and nanoscale atomic aggregation for the first time in the Zn-doped and Te non-stoichiometric AgCuTe system, employing a nanoscale perspective. Through our investigation, we disclose the remarkable coexistence of multidimensional defects, thereby resolving the previously conflicting opinions regarding point defects in this system. The effective control of these defects is crucial for achieving high thermoelectric performance. The ZnCu point defects regulate carrier concentration and Seebeck coefficient by influencing phase proportion and carrier effective mass. While maintaining the material's inherently large power factor (PF), thermal conductivity is effectively reduced through grain refinement and multiscale defect scattering. As a result, the dimensionless thermoelectric figure of merit (ZT) of approximately ∼ 1.16 is achieved at 773 K. By altering Te content, a coexistence of diverse defects is introduced, leading to intricate microstructures and phase structures. Consequently, a significant reduction in thermal conductivity is observed. The coexistence of multidimensional defects, as well as their impact on microstructure and thermoelectric transport properties, holds significant implications for the performance control of functional materials.