Thin film thermoelectric technology has immense potential to become a next-generation power source for small-scale electronics. However, the rapid development of thin film thermoelectric still lacks a controllable structural design to improve the performance of thermoelectric devices for required temperature applications. This work presented a controlled thermoelectric design of ZnO-based thin films by Al and Mg co-doping using ALD. Herein, the Mg-doped ZnO sample exhibits the highest Seebeck coefficient of −311.83 μVK−1 at 500oC, while the maximum thermoelectric power factor of 3.68 μWcm−1K−2 is obtained at 300oC, which drops for higher temperatures. This decrease in power factor resulted from the reduction in electrical conductivity above 300oC. Similarly, the Al and Mg co-doped ZnO sample (Mg/Al ≈2 at%) exhibits a high thermoelectric power factor of 3.85 μWcm−1K−2 for ZnO based material due to its moderate electrical conductivity and Seebeck coefficient value at 325oC and behave monotonically for elevated temperatures. Scanning electron microscope (SEM) images show the formation of wedge-shaped structures for Al-incorporated samples, which helps to boost the overall thermoelectric performance. Additionally, we performed XRD, UV–Vis, Hall, and AFM analysis to get a deep insight into structural, optical, electrical, and surface features of the grown thin films and their linkage with the thermoelectric properties.
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