Abstract
The influence of chloride integration on perovskite film deposition, encompassing both the structures of intermediate phases and the properties of the final films, was explored. Our methodology involved the fabrication of perovskite intermediate-phase films with varying concentrations of methylammonium chloride (MACl). Subsequently, we conducted an analysis employing X-ray diffraction and Rietveld refinement, incorporating the March-Dollase correction, to gain insights into how chloride-induced intermediate phases impact film morphology. Remarkably, a distinct preferred orientation was observed in the (020) lattice plane perpendicular to the substrate surface, and this orientation was found to be directly correlated to the MACl concentration. This distinctive arrangement of chloride-induced intermediate-phase complexes facilitated controlled crystallization, leading to highly oriented crystals and an improved film morphology. As a consequence, perovskite solar cell devices incorporating chloride-containing methylammonium lead iodide achieved a power conversion efficiency exceeding 20%. These findings suggest a crucial link between the preferred orientation observed in the final chlorine-derived perovskite films and the intermediate-phase structure formed during the initial stages of perovskite formation. These results suggest a profound impact of intermediate phase compositions and crystal structures on perovskite formation, emphasizing the importance of a comprehensive understanding of these factors to enable precise control over ideal structures and the subsequent transformation into high-quality perovskite films.