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Abstract Organic-inorganic hybrid lead halide perovskite has shown to be one of the best light-harvesting materials for solar cell in the last decade. However, there still is needed a deeper understanding of phase and film formation for better control of device fabrication. In this work, we visualise the formation mechanism of Cs0.15(MA0.7FA0.3)0.85PbI3 perovskite by the sequential spin-coating method and how changes in the dispensing timing and substrate motion affect the formation process and properties of the final film quality. In particular, this is the first time that we are able to visualise and identify the different stages of the film formation: i) “initial formation”; ii) “perovskite deconstruction” and iii) “perovskite re-crystallisation”. This particularly applies to films that are sequentially spin-coated and involve the use of dimethyl sulfoxide (DMSO) as the “deconstruction” is caused by the formation of intermediate-DMSO-complex. These findings are validated by FTIR and XRD measurements. Comparison among processes also suggests that motion causes an earlier onset of deconstruction, which will lead to a slower re-crystallisation resulting in better quality perovskite film with less non-perovskite phase. This can be achieved by motion dispensing and dynamic processing (where there is no stoppage between the two sequential steps). Reasons for the earlier onset of deconstruction are the higher kinetic energy supplied by the dynamic process. This work has provided more insights into the complex stages involved in perovskite conversion specific to sequential processing. The knowledge will aid future process optimisation for better device fabrication.

AbstractOrganic–inorganic hybrid metal halide perovskite materials have attracted exponentially increased attention for photovoltaic applications in the past few years, while the toxic lead component remains a big concern. Herein, we present the recent progress in researching lead‐free perovskite light absorbers for solar cell application, and the challenges in this field are also discussed, which may shed light on further investigation of low‐toxic, lead‐free and efficient perovskite solar cells for sustainable solar energy utilization. © 2016 Curtin University of Technology and John Wiley & Sons, Ltd.

Abstract Perovskite solar cells (PSCs) have been attracting tremendous attention due to ease of processing, flexibility, and high performance. Dimethyl sulfoxide (DMSO) and N, N-dimethylformamide (DMF) are the two most widely used solvents to dissolve perovskite precursors. Here, we investigate the impact of residual amount and evaporation rate of the DMSO inside the precursor films on the microstructure of the ultimate perovskite films. We decouple the DMSO and DMF solvents and demonstrate that DMSO component exhibits great and dominant influence on the final film morphology by using quasi in-situ photoluminescence (PL) measurement and X-ray diffraction (XRD) characterization of the wet films after spin-coating. Much more smooth and uniform perovskite films are obtained by careful management of remanent solvent, including decreasing residual amount by shelving the precursor films prior to heating and retarding the evaporation of the solvent via adopting a gradient annealing (GA) process. In consequence, the as-prepared PEDOT: PSS-based inverted PSCs yield a champion efficiency of 15.59% with high reproducibility. This work shows great potential in preparing high-quality perovskite films through a simple remanent solvent management engineering.