Modified Sequential Deposition Route through Localized-Liquid-Liquid-Diffusion for Improved Perovskite Multi-Crystalline Thin Films with Micrometer-Scaled Grains for Solar Cells.

High-class perovskite film with beautiful surface morphology (such as large-size grain, low defect density, good continuity and flatness) is normally believed to be a very important factor for high-efficiency perovskite solar cells (PSCs). Here, we report a modified sequential deposition route through localized-liquid-liquid-diffusion (LLLD) for qualified perovskite multi-crystalline thin films with micrometer-scaled grains for solar cells. We adopted a contact-type drop method to drop Methylammonium iodide (MAI) solution and have successfully used high-concentration MAI solution (73 mg/mL) to transform PbI₂ film into high-class perovskite film via our route. A high efficiency of 10.7% was achieved for the device with spongy carbon film deposited on a separated FTO-substrate as a counter electrode under one sun illumination, which is the highest efficiency (as 2.5 times as previous efficiency) ever recorded in perovskite solar cells with a such spongy carbon/FTO composite counter electrode. The preparation techniques of high-class perovskite thin films under ambient conditions and the cheap spongy carbon/FTO composite counter electrode are beneficial for large-scale applications and commercialization.