Poly(amic acid)-Polyimide Copolymer Interfacial Layers for Self-Powered CH3NH3PbI3 Photovoltaic Photodiodes

Hybrid organohalide perovskites have received considerable attention due to their exceptional photovoltaic (PV) conversion efficiencies in optoelectronic devices. In this study, we report the development of a highly sensitive, self-powered perovskite-based photovoltaic photodiode (PVPD) fabricated by incorporating a poly(amic acid)-polyimide (PAA-PI) copolymer as an interfacial layer between a methylammonium lead iodide (CH₃NH₃PbI₃, MAPbI₃) perovskite light-absorbing layer and a poly(3,4-ethylenedioxythiophene)-poly(styrene sulfonate) (PEDOT: PSS) hole injection layer. The PAA-PI interfacial layer effectively suppresses carrier recombination at the interfaces, resulting in a high power conversion efficiency (<i>PCE</i>) of 11.8% compared to 10.4% in reference devices without an interfacial layer. Moreover, applying the PAA-PI interfacial layer to the MAPbI₃ PVPD significantly improves the photodiode performance, increasing the specific detectivity by 49 times to 7.82 × 10¹⁰ Jones compared to the corresponding results of reference devices without an interfacial layer. The PAA-PI-passivated MAPbI₃ PVPD also exhibits a wide linear dynamic range of ~103 dB and fast response times, with rise and decay times of 61 and 18 µs, respectively. The improved dynamic response of the PAA-PI-passivated MAPbI₃ PVPD enables effective weak-light detection, highlighting the potential of advanced interfacial engineering with PAA-PI interfacial layers in the development of high-performance, self-powered perovskite photovoltaic photodetectors for a wide range of optoelectronic applications.