Ultrafast Quasi‐2D/3D Perovskite Photodetectors Conferred Using Interfacial Engineering of Self‐Assembled Monolayers

Abstract Quasi‐2D (q‐2D) perovskites are extensively studied due to their hybrid properties of 3D and 2D phases and have proven to be applied to a wide range of optoelectronics. Multiple device engineering methods for perovskite photodetectors are developed. However, the treatment of self‐assembled monolayer (SAM) is rarely discussed. Herein, a series of silane‐coupling agents of (3‐chloropropyl)trichlorosilane (CPTS), phenyltrichlorosilane, and (3‐aminopropyl)triethoxysilane is adopted as SAM materials and elucidated their influence on q‐2D/3D CsPbBr₃ films and their photodetector performance. The optical properties and morphology results reveal that perovskite film on CPTS‐modified surface can prolong excitons’ lifetime, produce a larger grain size and better size distribution, while also present better crystallinity and united orientation. As for the fabricated photodetectors, the device on a CPTS‐modified surface has the highest photocurrent of 5.46 × 10⁻⁸ A, a responsivity of 0.16 A W⁻¹, and an 18‐times‐higher specific detectivity than the pristine counterpart, which comes from the higher surface energy and favorable energy level alignment. The photodetector on the CPTS‐modified surface also shows better stability than that on the pristine surface. This study pioneers by using SAMs on q‐2D perovskite photodetectors and provides a facile route of device fabrication for perovskite photodetectors.