Regulation of Quantum Wells Width Distribution in Quasi-2D Perovskite Films for High-Performance Photodetectors

Dynamic optimization of the quantum-well (QW) width distribution in quasi-2D halide perovskite thin films is an effective approach for tuning the properties of photoelectric devices. Here, that the QWs width distribution in quasi-2D perovskite films can be controlled only by using hydroiodic acid (HI) as an additive is demonstrated. A uniform distribution of the colloidal particle size in the quasi-2D perovskite precursor solution is achieved through the formation of soluble iodoplumbate coordination complexes, PbI3- from the reaction of HI with PbI2, resulting in an improved phase purity in the final film. Density functional theory calculations indicate that the ideal n value quasi-2D perovskite reaction pathway through the PbI3- complex has a lower enthalpy of formation than the random nucleation pathway without the HI additive. Benefiting from this merit, a high-quality quasi-2D perovskite film with optimized phase purity delivered a balanced carrier diffusion length and improved carrier mobility. The resultant photodetectors exhibited a light on/off ratio of 50 000, a responsivity of 0.96 A W-1, and a detectivity of 5.7 x 10(12) Jones at 532 nm. In addition, the state-of-the-art device maintained more than 80% of its initial photocurrent after 720 h of storage at 30% relative humidity.

Automated summary

This study demonstrated that the quantum-well (QW) width distribution in quasi-2D perovskite films can be controlled effectively by using hydroiodic acid (HI) as an additive. The formation of soluble iodoplumbate coordination complexes, PbI3-, from the reaction of HI with PbI2 led to a uniform distribution of colloidal particle size in the precursor solution and improved phase purity in the final film. The optimized phase purity of the high-quality quasi-2D perovskite film resulted in a balanced carrier diffusion length, improved carrier mobility, and high-performance photodetectors with a light on/off ratio of 50,000, a responsivity of 0.96 A W-1, and a detectivity of 5.7 x 10(12) Jones at 532 nm. Additionally, the device showed excellent stability with more than 80% of its initial photocurrent maintained after 720 hours of storage at 30% relative humidity.