Quasi‐Single‐Crystal Tin Halide Perovskite Films with High Structural Integrity for Near‐Infrared Imaging Array Enabling Hidden Object Recognition

Abstract Near‐infrared (NIR) image sensors based on solution‐processed thin film are gaining prominence in various applications, including security detection, remote sensing, medical imaging, and environmental monitoring, owing to superior penetration capabilities of NIR light. However, the reported perovskite image sensors suffer from limited resolution and performance due to poor structural integrity, bioincompatibility, and constrained response wavelength range from lead‐based perovskite materials employed. In this study, we present non‐toxic quasi‐single‐crystal (QSC) CH(NH 2 ) 2 SnI 3 (FASnI 3 ) perovskite films, prepared via a simple spin‐coating technique, that demonstrate high structural integrity and effective NIR response. Through a series of in situ characterizations, we reveal that the orderly growth mode of QSC‐FASnI 3 perovskite films enables a more oriented crystal growth with reduced trap and grain boundaries. Consequently, self‐powered NIR photodetector based on QSC‐FASnI 3 films exhibited large detectivity over 10 13 Jones in the NIR range (780–890 nm). Ultimately, due to the high structural integrity, the high‐resolution 64×64 (4096) pixels NIR imaging array, exhibiting reduced photo and dark response non‐uniformity value, was fabricated on the thin‐film transistors (TFT) backplanes, enabling ultraweak NIR light (63 nW cm −2 ) real‐time imaging, fingerprint imaging, and hidden object recognition. This work pioneers the application of lead‐free perovskite for high‐resolution NIR imaging arrays.