Universal Integration of 2D Organic Single Crystals With Fluorinated Polymer Dielectrics for High‐Performance Transistors and Single‐Pixel Imaging Applications

ABSTRACT Organic single‐crystal field‐effect transistors (OSCFETs) are regarded as an ideal platform for investigating intrinsic charge transport behaviors and developing high‐performance organic electronic devices, thanks to their ordered molecular stacking and minimal grain boundary defects. However, conventional integration methods frequently introduce impurities that induce interface defects or crystal damage, significantly impairing charge transport efficiency‐a long‐standing limitation plaguing diverse organic semiconductors. To address this critical challenge, we propose a universal strategy for the integration of two‐dimensional (2D) organic single crystals with fluorinated polymer dielectrics. This approach synergistically combines an in‐house microspacing in‐air sublimation (MAS) growth technique with a gentle, damage‐free transfer process, effectively eliminating interfacial imperfections. The resulting high‐quality crystal‐dielectric interfaces enable OSCFETs to achieve exceptional comprehensive performance: a record‐high mobility of 18.9 cm 2 V −1 s −1 , ultralow operating voltage of −5 V, ultrafast photoresponse of 30 µs, outstanding high‐speed image acquisition capability, and robust dual‐mode driving performance for organic light‐emitting diodes (OLED). This work establishes a universal method for constructing high‐quality single crystals on polymer dielectrics, which holds broad implications for advancing high‐speed sensing, imaging technologies, flexible displays, and integrated logic circuits.