Variation of Charge Carrier Dynamics for Polycrystalline Perovskite Films by One-Step Solution and Vapor-Deposition Methods

To date, solution-processing and vapor-deposition fabrication methods have achieved huge successes in high-efficiency perovskite solar cells (PSCs) and satisfy special demanding requirements for diverse application purposes, respectively. Although people realize that the fabrication procedure is crucial in device performance, insightful studies of charge carrier dynamics in perovskite films by different methods still lack. In this work, we compare the carrier behaviors in one-step spin-coated and dual-source coevaporated MAPbI₃ perovskite films by combining time-resolved photoluminescence spectroscopy and carrier dynamics simulation. We suggest that strains, lattice orientations, and defects at buried side of perovskite films, which are associated with different preparation processes, lead to variations in carrier behaviors. Hence fabrication of perovskite layers should be elaborately designed in order to satisfy the needs of different carrier behaviors in specified device configurations of PSCs such as smooth planar or textured monolithic tandem structures.