Engineering of dendritic dopant-free hole transport molecules: enabling ultrahigh fill factor in perovskite solar cells

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gineering of dendritic dopant-free hole transport molecules: enabling ultrahigh fill factor in perovskite solar cells with optimized dendron construction 1,2

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Wei Chen , Yang Wang , Bin Liu , Yajun Gao , Ziang Wu , Yongqiang Shi , Yumin Tang , 1 1 1 1 3 4 Kun Yang , Yujie Zhang , Weipeng Sun , Xiyuan Feng , Frédéric Laquai , Han Young Woo , 2 1* 1* Aleksandra B. Djurišić , Xugang Guo & Zhubing He 1

Department of Materials Science and Engineering, Southern University of Science and Technology, Shenzhen 518055, China; 2 Department of Physics, The University of Hong Kong, Pokfulam, Hong Kong, China; 3 King Abdullah University of Science and Technology, KAUST Solar Center, Physical Sciences and Engineering Division, Material Science and Engineering Program, Thuwal 23955-6900, Kingdom of Saudi Arabia; 4 Department of Chemistry, Korea University, Seoul 02841, South Korea Received July 7, 2020; accepted August 25, 2020; published online October 15, 2020

Developing dopant-free hole-transporting materials (HTMs) for high-performance perovskite solar cells (PVSCs) has been a very active research topic in recent years since HTMs play a critical role in optimizing interfacial charge carrier kinetics and in turn determining device performance. Here, a novel dendritic engineering strategy is first utilized to design HTMs with a D-A type molecular framework, and diphenylamine and/or carbazole is selected as the building block for constructing dendrons. All HTMs show good thermal stability and excellent film morphology, and the key optoelectronic properties could be fine-tuned by varying the dendron structure. Among them, MPA-Cz-BTI and MCz-Cz-BTI exhibit an improved interfacial contact with the perovskite active layer, and non-radiative recombination loss and charge transport loss can be effectively suppressed. Consequently, high power conversion efficiencies (PCEs) of 20.8% and 21.35% are achieved for MPA-Cz-BTI and MCz-Cz-BTI based devices, respectively, accompanied by excellent long-term storage stability. More encouragingly, ultrahigh fill factors of 85.2% and 83.5% are recorded for both devices, which are among the highest values reported to date. This work demonstrates the great potential of dendritic materials as a new type of dopant-free HTMs for high-performance PVSCs with excellent FF. dendritic molecules, hole-transporting materials, dopant-free, ultrahigh fill factor, perovskite solar cells Citation:

Chen W, Wang Y, Liu B, Gao Y, Wu Z, Shi Y, Tang Y, Yang K, Zhang Y, Sun W, Feng X, Laquai F, Woo HY, Djurišić AB, Guo X, He Z. Engineering of dendritic dopant-free hole transport molecules: enabling ultrahigh fill factor in perovskite solar cells with optimized dendron construction. Sci China Chem, 2020, 63, https://doi.org/10.1007/s11426-020-9857-1

1 Introduction As a disruptive photovoltaic technology, perovskite solar cells (PVSCs) are gaining tremendous research interests, recently. PVSCs are generally fabricated with a sandwich structure, in which metal halide perovskite active layer is in *Corre