Charge-Carrier Dynamics of Evaporated Bismuth-Based Chalcogenide Thin Films Probed with Time-Resolved Microwave Conductivity

Chalcogenide-based semiconductors are emerging as a set of highly promising candidates for optoelectronic devices, owing to their low toxicity, cost-effectiveness, exceptional stability, and tunable optoelectronic properties. Nonetheless, the limited understanding of charge recombination mechanisms and trap states of these materials is impeding their further development. To fill this gap, we conducted a comprehensive study of bismuth-based chalcogenide thin films and systematically investigated the influence of post-treatments via time-resolved microwave conductivity and temperature-dependent photoluminescence. The key finding in this work is that post-treatment with Bi could effectively enhance the crystallinity and charge-carrier mobility. However, the carrier density also increased significantly after the Bi treatment. On the contrary, post-treatment of evaporated Bi₂S₃ thin films with sulfur could effectively increase the carrier lifetime and mobility by passivating the trap states on the grain boundaries, which is also consistent with the enhanced radiative recombination efficiency.