High‐Performance (hk0)‐Oriented Sb 2 S 3 Photodetectors Toward Diversified Optoelectronic Applications

Broadband photodetectors that simultaneously combine low standby energy consumption, adequate photosensitivity, fast response rate, and scalable integration compatibility remain challenging to realize. Herein, Sb 2 S 3 thin films have been prepared through pulsed‐laser deposition (PLD). The corresponding Sb 2 S 3 photodetector exhibits a low dark current of 8.6 × 10 −12 A at 2 V, distinct UV–vis–NIR photoresponse with an optimized photo‐to‐dark current ratio of 312, a responsivity of 442 mA/W, an external quantum efficiency of 136%, and a short response/recovery time of 45/55 µs. The competitive broadband photosensitivity can be rationally ascribed to the synergy among sulfur vacancy states potentially introduced during the nonequilibrium PLD growth, light trapping by the rough surface, and efficient in‐plane carrier transport along the (hk0) texture. Benefiting from the well‐balanced performance, the PLD‐derived Sb 2 S 3 devices are further demonstrated in broadband optoelectronic imaging exceeding human vision scope, respiration monitoring, and neural‐network‐assisted high‐fidelity target recognition. In the end, on‐chip integration is demonstrated by constructing a 10 × 10 array. On the whole, this work establishes a promising growth‐to‐function pathway for developing next‐generation integrated optoelectronic chips.