Crystal Morphologies of Organolead Trihalide in Mesoscopic/Planar Perovskite Solar Cells

The crystal morphology of organolead trihalide perovskite (OTP) light absorbers can have profound influence on the perovskite solar cells (PSCs) performance. Here we have used a combination of conventional transmission electron microscopy (TEM) and high-resolution TEM (HRTEM), in cross-section and plan-view, to characterize the morphologies of a solution-processed OTP (CH₃NH₃PbI₃ or MAPbI₃) within mesoporous TiO₂ scaffolds and within capping and planar layers. Studies of TEM specimens prepared with and without the use of focused ion beam (FIB) show that FIBing is a viable method for preparing TEM specimens. HRTEM studies, in conjunction with quantitative X-ray diffraction, show that MAPbI₃ perovskite within mesoporous TiO₂ scaffold has equiaxed grains of size 10–20 nm and relatively low crystallinity. In contrast, the grain size of MAPbI₃ perovskite in the capping and the planar layers can be larger than 100 nm in our PSCs, and the grains can be elongated and textured, with relatively high crystallinity. The observed differences in the performance of planar and mesoscopic-planar hybrid PSCs can be attributed in part to the striking differences in their perovskite-grain morphologies.