Enhanced Performance in All-Inorganic AgBiS2 Photodetectors via Oxygen-Inhibited Spray Pyrolysis Deposition.
AgBiS2 has emerged as a promising optoelectronic material due to its broad spectral response and strong light absorption. However, the current use of high-boiling solvents and organic buffers restricts fundamental studies and further performance optimization of AgBiS2's intrinsic properties. In this study, we develop an organic buffer-free AgBiS2 photodetector prepared using a low-temperature ultrasonic spray pyrolysis technique. Our theoretical analysis revealed that oxygen doping alters the optoelectronic characteristics by enhancing the density of states near the Fermi level, leading to consequent severe nonradiative charge carrier recombination. By incorporating excess thiourea while maintaining optimal substrate temperature for enhanced crystallinity, we successfully suppress oxygen defects and consequently improve photodetection performance. The optimized device exhibits a high responsivity of 0.046 A W-1 at 1050 nm, a low noise level (<8.5 × 10-19 A2 Hz-1), and a fast response time (0.07 μs rise, 0.60 μs decay). Benefiting from the rapid response, the photodetector delivers high-resolution imaging with sharp edge definition. This work eliminates the interference of organic buffer layers to directly reveal how oxygen defect modulation affects the intrinsic optoelectronic properties of AgBiS2, offering a scalable pathway for high-performance, solution-processed photodetectors.