Post-selenization tailored carrier-crystallographic synergy in c-axis Bi2Se3 thin films for advanced thermoelectrics

Bi 2 Se 3 has emerged as a promising thermoelectric (TE) material due to its environmentally benign composition and earth-abundant constituents. However, the practical implementation of Bi 2 Se 3 -based systems remains challenging due to suboptimal TE performance. This study demonstrates the fabrication of c -axis oriented Bi 2 Se 3 thin films through pulsed laser deposition, with subsequent selenization treatment significantly enhancing TE performance through dual optimization of carrier concentration and crystallographic alignment. A strategic post-deposition selenization process effectively mitigates selenium vacancies and correspondingly reduces the carrier concentration to 2.0×10 19 cm -3 while improving in-plane carrier mobility. A high power factor (PF) of about 9.5 μW⸱cm -1 ⸱K -2 is achieved at 475 K in the highly c -axis oriented Bi 2 Se 3 thin films selenized for about 60 min, outperforming the reported state-of-the-art Bi 2 Se 3 films. Demonstrating practical applicability, an 8-leg planar thin-film device generates an exceptional power density of 441.3 μW/cm 2 under a 25 K temperature gradient, establishing new performance benchmarks for chalcogenide-based microgenerators. These findings provide crucial insights into defect engineering and structural optimization strategies for developing high-performance TE devices compatible with self-powered microelectronic applications. • Highly oriented Bi 2 Se 3 thin films were prepared by PLD technology and selenization. • By applying efficient selenization strategy, vacancy concentration was controllably adjusted, enhancing the power factor. • The maximum power factor of 9.5 μW⸱cm –1 ⸱K –2 is achieved at 475 K.