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It has been proposed that introducing the chlorine anion into a CH3NH3PbI3 perovskite material can substantially improve the materials properties as well as the solar cell performance. To elucidate the role of chlorine in perovskite solar cells (PSCs), here we introduced PbCl2 into the precursor, and studied the chlorine configuration evolution during perovskite film formation and the associated influence on PSC performance in detail. We found that chlorine could be successfully incorporated into the precursor film in the form of PbICl or PbCl2 through a properly designed preparation, and it was conserved in the final perovskite film with a configuration of MAPbCl(3), PbICl or PbCl2 depending on the fabrication process. However, no evidence of a MAPbI(3-x)Cl(x) phase was observed, and it is considered that MAPbI(3-x)Cl(x) might be metastable or possesses a higher formation energy. In addition, we demonstrate that the formation of a porous PbICl scaffold in the precursor film plays a key role in high quality perovskite film realization, benefiting from an effective stress release during structure expansion after methylammonium iodide dripping. Moreover, we propose that residual amorphous PbCl2 can effectively passivate defects in perovskite film, and dramatically improve the film's electrical properties. Finally, n-i-p type planar PSCs with efficiencies up to 19.45% were achieved. It should be mentioned that the whole process for the formation of the PSCs is performed at less than 100 degrees C, which is beneficial for a wide range of applications, such as flexible and tandem solar cells.
Felix Thomas Eickemeyer, Lukas Pfeifer, Hiroaki Jinno, Tommaso Marcato
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