Charge transport and ion migration in perovskite-incorporated conjugated polymer semiconductor

The migration of intrinsic ions in metal halide perovskites and their interfaces has been shown to contribute to hysteresis and performance degradation in perovskite-based electronic devices, particularly in photovoltaics and transistors. Accordingly, controlling the film morphology, microstructure, and ionic defects in perovskite semiconductors is essential for advancing and achieving high-performance perovskite field-effect transistors (FETs). In this study, we demonstrate a well-controlled method to systematically probe the structure-property relationships, origin of hysteresis, and intrinsic ion migration effects in formamidinium iodide and lead iodide (FAI + PbI₂)-based perovskite by incorporating it in a semicrystalline conjugated poly(3-hexylthiophene) (P3HT) polymer. Optimized FETs exhibited over 100% hole mobility enhancement owing to unperturbed edge-on crystalline orientation of the P3HT chains caused by the incorporated perovskite, P3HT-(FAI + PbI₂) interactions, and better charge injection properties. However, the optimized devices exhibited improved current modulation with dual-sweep hysteresis, which was attributed to the ion migration effect contributed by the polarization of the lead/iodine-related ions and defects. Furthermore, operational stability investigation of the P3HT-(FAI + PbI₂) FETs in the air revealed gradual current decay owing to charge trapping in contrast to the control P3HT FETs. This work provides a fundamental understanding of the origin of hysteresis and instabilities in metal perovskite materials and their transistor-based devices.