Solvent-Hydrolysis-Driven Engineering of Ordered Single Quantum Well 2D Perovskites
Single quantum well (single-QW) two-dimensional (2D) perovskites are poised to revolutionize optoelectronic devices owing to their superior stability and optoelectronic properties. However, solution-processed 2D perovskites typically suffer from disordered multiple-QW structures, leading to inconsistent device performance. Here, we introduce a solvent-hydrolysis-driven method to control crystallization kinetics, yielding highly ordered single-QW 2D perovskite films. Dimethylamine (DMA), generated from the hydrolysis of N,N-dimethylformamide (DMF), serves as a critical mediator, preventing cluster aggregation and ensuring a uniform colloidal distribution. This approach circumvents the formation of a heterogeneous intermediate phase, thereby promoting the formation of a homogeneous (DMA,MA)PbI3 phase, which is essential for single-QW film development. The resultant photodetector exhibits outstanding performance, with a responsivity of 1153 mA/W and a detectivity of 6.98 × 10^12 Jones, along with excellent photostability under ambient conditions. These attributes render it ideal for photoelectric imaging sensors and large-scale integration. Our findings establish a scalable, solution-processed strategy for high-performance 2D perovskite materials, opening new avenues for advanced optoelectronic applications.