TY - JOUR AU - Gao, Zhi AU - Hou, Shuaihang AU - Liu, Xinqi AU - Xue, Yuli AU - Li, Zhipeng AU - Zhao, Qi AU - Wang, Jianglong AU - Li, Zhiliang AU - Wang, Shufang PY - 2026 TI - Post-selenization tailored carrier-crystallographic synergy in c-axis Bi2Se3 thin films for advanced thermoelectrics JO - Journal of Materiomics SN - 2352-8478 VL - 12 IS - 1 AB - Bi2Se3 has emerged as a promising thermoelectric (TE) material due to its environmentally benign composition and earth-abundant constituents. However, the practical implementation of Bi2Se3-based systems remains challenging due to suboptimal TE performance. This study demonstrates the fabrication of c-axis oriented Bi2Se3 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 × 1019 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 Bi2Se3 thin films selenized for about 60 min, outperforming the reported state-of-the-art Bi2Se3 films. Demonstrating practical applicability, an 8-leg planar thin-film device generates an exceptional power density of 441.3 μW/cm2 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. UR - https://doi.org/10.1016/j.jmat.2025.101099 DO - 10.1016/j.jmat.2025.101099