2D Ruddlesden-Popper Perovskite with Ordered Phase Distribution for High-Performance Self-Powered Photodetectors

2D Ruddlesden-Popper perovskites exhibit great potential in optoelectronic devices for superior stability compared with their 3D counterparts. However, to achieve a high level of device performance, it is crucial but challenging to regulate the phase distribution of 2D perovskites to facilitate charge carrier transfer. Herein, using a solvent additive method (adding a small amount of dimethyl sulfoxide (DMSO) in N,N-dimethylformamide (DMF)) combined with a hot-casting process, the phase distribution of (PEA)₂ MA₃ Pb₄ I₁₃ (PEA⁺  = C₆ H₅ CH₂ CH₂ NH₃ ⁺ , MA⁺  = CH₃ NH₃ ⁺ ) perovskite can be well controlled and the Fermi level of perovskites along the film thickness direction can achieve gradient distribution. The increased built-in potential, oriented crystal, and improved crystal quality jointly contribute to the high photoresponse of devices in the entire response spectrum range. The optimum device exhibits a characteristic detection peak at 570 nm with large responsivity/detectivity (0.44 A W^-1 /3.38 × 10¹² Jones), ultrafast response speed with a rise/fall time of 20.8/20.6 µs, and improved stability. This work suggests the possibility of manipulating the ordered phase distribution of 2D perovskites toward high-performance and stable optoelectronic conversion devices.