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Revealing the crystallization process and realizing uniform 1.8 eV MA-based wide-bandgap mixed-halide perovskites via solution engineering

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Abstract

Wide-bandgap perovskites are recently drawing tremendous attention in the community for high-efficiency all-perovskite tandem solar cells. However, the formamidinium (FA+) and methylammonium (MA+) based wide-bandgap mixed halide perovskites suffered from high density of traps and pin-holes, respectively. Fundamental understanding on the crystallization and film formation processes are keys to overcome those challenges but not yet clearly understood. In this study, an in-situ photoluminescence technique was used to investigate the perovskite crystallization during the thermal annealing process. It is found that the crystallization of a mixed halide perovskite with bromide (Br−) and iodine (I−) ions following the Ostward ripening crystal growth. Interestingly, it is found that the initial nucleation reaction is quickly completed in the first few seconds, however, leaving the small crystals with inhomogeneous composition. The different aggregation affinities of such inhomogeneous small crystals provoke the formation of pin-holes during the thermal annealing process. By engineering the precursor solution to control the nucleation rate, the chemical composition of the small crystals has become homogenous. Uniform pin-hole free high Br−composited wide-bandgap MA0.9Cs0.1Pb(I0.6Br0.4)3 perovskite films with bandgap energy of 1.8 eV have been realized. The corresponding photovoltaic devices have achieved an encouraging device efficiency of 15.1% with superb photostability.

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Acknowledgements

We gratefully thank the funding support from the National Natural Science Foundation of China (No. 61574120), the Guangdong province Natural Science Foundation of China (No. 2015A030313001) and the Hong Kong Innovation and Technology Commission (No. ITS/186/16).

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Authors and Affiliations

  1. Department of Materials Science and Engineering, City University of Hong Kong, Hong Kong SAR, China

    Yue-Min Xie, Chunqing Ma, Xiuwen Xu, Menglin Li, Yuhui Ma, Jing Wang, Hrisheekesh Thachoth Chandran, Chun-Sing Lee & Sai-Wing Tsang

  2. City University of Hong Kong Shenzhen Research Institute, Shenzhen, 518057, China

    Yue-Min Xie, Chunqing Ma, Xiuwen Xu, Menglin Li, Yuhui Ma, Jing Wang, Hrisheekesh Thachoth Chandran, Chun-Sing Lee & Sai-Wing Tsang

  3. Center of Super-Diamond and Advanced Films (COSDAF), City University of Hong Kong, Hong Kong SAR, China

    Yue-Min Xie, Chunqing Ma, Xiuwen Xu, Menglin Li, Yuhui Ma, Jing Wang, Hrisheekesh Thachoth Chandran, Chun-Sing Lee & Sai-Wing Tsang

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  1. Yue-Min Xie
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  2. Chunqing Ma
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Correspondence to Sai-Wing Tsang.

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Revealing the crystallization process and realizing uniform 1.8 eV MA-based wide-bandgap mixed-halide perovskites via solution engineering

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Xie, YM., Ma, C., Xu, X. et al. Revealing the crystallization process and realizing uniform 1.8 eV MA-based wide-bandgap mixed-halide perovskites via solution engineering. Nano Res. 12, 1033–1039 (2019). https://doi.org/10.1007/s12274-019-2336-5

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