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.
ABSTRACT
The effect of TiO2 interfacial morphology on perovskite crystallinity was investigated by modifying the micro and nanoscale surface roughness of compact TiO2. While surface treatments of the compact TiO2 layer are recognized as effective strategies to enhance the photovoltaic performance of perovskite solar cells, the discussion regarding the crystallinity of perovskite atop TiO2 has been limited. In this study, we explored the impact of micro and nano scale interface morphology on perovskite crystal formation and its subsequent effects on device performance. Surprisingly, despite the absence of noticeable voids at the interface between the compact TiO2 and perovskite layers, the perovskite crystal morphology exhibited significant improvement following either micro or nanoscale interfacial modification. This enhancement ultimately led to improved photoconversion efficiency and reduced I-V hysteresis. These results emphasize the importance of underlayer surface morphology in the perovskite crystallization and suggest that the presence of grain boundaries within the perovskite layer may also contribute to I-V hysteresis in perovskite solar cells.
