Pulsed‐Laser‐Deposition Fabricated ZnIn₂S₄ Photodetectors with Excellent ON/OFF Switching Characteristics toward High‐Temperature‐Resistant Photodetection Applications

Abstract The extensively explored unary and binary 2D layered materials (2DLMs) based photodetectors suffer from deficiencies of either poor stability, or indistinctive photoswitching, or poor scalability, or low durability to high‐temperature environment. Herein, a two‐step scenario, pulsed laser deposition (PLD) followed by post‐deposition annealing, is developed to produce centimeter‐scale 2D ZnIn₂S₄ (ZIS) nanofilms. Transport characterizations indicate that the as‐fabricated ZIS photodetectors manifest outstanding photosensitivity with an on/off switching ratio beyond 1000 upon 405 nm illumination. Beyond this, it is revealed that the photoresponse of the ZIS photodetectors increases with increasing channel thickness, where a responsivity of 1.4 A W⁻¹, an external quantum efficiency of 430% and a detectivity of 9.8 × 10⁹ Jones (1 Jones = 1 cm Hz^1/2 W^–1) are demonstrated with a pulse number of 10 000. In addition, these devices without encapsulation maintain stable within 1900 photoswitching cycles and over a one‐month storage in air. Furthermore, robust photoswitching is demonstrated under an operating temperature up to 150 °C. In summary, all these findings establish that PLD provides a powerful route to produce large‐scale multielement 2DLMs and the PLD‐derived ZIS photodetectors hold grand prospect for photoelectric technologies in specific high‐temperature environments (e.g., the lunar exploration program).