Bication-Mediated Quasi-2D Halide Perovskites for High-Performance Flexible Photodetectors: From Ruddlesden–Popper Type to Dion–Jacobson Type

Quasi-2D halide perovskites, especially the Ruddlesden–Popper perovskites (RPPs), have attracted great attention because of their promising properties for optoelectronics; however, there are still serious drawbacks, such as inefficient charge transport, poor stability, and unsatisfactory mechanical flexibility, restricting further utilization in advanced technologies. Herein, high-quality quasi-2D halide perovskite thin films are successfully synthesized with the introduction of the unique bication ethylenediammonium (EDA) via a one-step spin-coating method. This bication EDA, with short alkyl chain length, can not only substitute the typically bulky and weakly van der Waals-interacted organic bilayer spacer cations forming the novel Dion–Jacobson phase to enhance the mechanical flexibility of the quasi-2D perovskite (e.g., EDA(MA)n−1PbnI3n+1; MA = CH3NH3+) but also serve as a normal cation to achieve the more intact films (e.g., (iBA)2(MA)3–2x(EDA)xPb4I13). When fabricated into photodetectors, these optimized EDA-based perovskites deliver an excellent responsivity of 125 mA/W and a fast response time down to 380 μs under 532 nm irradiation. More importantly, the device with the Dion–Jacobson phase perovskite can be bent down to a radius of 2 mm and processed with 10,000 cycles of the bending test without any noticeable performance degradation because of its superior structure to RPPs. Besides, these films do not exhibit any material deterioration after ambient storage for 30 days. All these performance parameters are already comparable or even better than those of the state-of-the-art RPPs recently reported. This work provides valuable design guidelines of the quasi-2D perovskites to obtain high-performance flexible photodetectors for next-generation optoelectronics.