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Article Abstract
Various isomers have been developed to regulate the morphology and reduce defects in state-of-the-art perovskite solar cells (PSCs). To insight the structure-function-effect correlations for the isomerization of thiourea derivatives on the performance of the PSCs, we developed two thiourea derivatives [(3,5-dichlorophenyl)amino]thiourea (AT) and N-(3,5-dichlorophenyl)hydrazinecarbothioamide (HB). Supported by experimental and calculated results, it was found that AT can bind with undercoordinated Pb defect through synergistic interaction between N1 and C=S group with a defect formation energy of 1.818 eV, which is much higher than that from the synergistic interaction between two -NH- groups in HB and perovskite (1.015 eV). Moreover, the stronger interaction between AT and Pb regulates the crystallization process of perovskite film to obtain a high-quality perovskite film with high crystallinity, large grain size, and low defect density. Consequently, the AT-treated FACsPbI device engenders an efficiency of 25.71 % (certified as 24.66 %), which is greatly higher than control (23.74 %) and HB-treated FACsPbI devices (25.05 %). The resultant device exhibits a remarkable stability for maintaining 91.0 % and 95.2 % of its initial efficiency after aging 2000 h in air condition or tracking at maximum power point for 1000 h, respectively.
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