Organic-inorganic hybrid perovskites (OIHPs) with superior optoelectronic properties have emerged as revolutionary semiconductor materials for diverse applications. A fundamental understanding of the interplay between the microscopic molecular-level structure and the macroscopic optoelectronic properties is essential to boost device performance toward theoretical limits. Here, we reveal the critical role of CH3NH3+ (MA) in the regulation of the physicochemical and optoelectronic properties of a MAPbI3 film irradiated by an electron beam at 130 K. The order-to-disorder transformation of the MA cation not only leads to a notably enhanced photoluminescence emission but also results in the suppression of the orthorhombic phase down to 85 K. Taking advantage of the regulation of MA cation dynamics, we demonstrate a perovskite photodetector with 100% photocurrent enhancement and long-term stability exceeding one month. Our study provides a powerful tool for regulating the optoelectronic properties and stabilities of perovskites and highlights potential opportunities related to the organic cation in OIHPs.
Keywords: MA cations; cryogenic e-beam; order−disorder transformation; phase transition; photoluminescence.