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Nucleation-mediated growth of chiral 3D organic–inorganic perovskite single crystals

Nature Chemistry volume 15, pages 1581–1590 (2023)Cite this article

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Abstract

Although their zero- to two-dimensional counterparts are well known, three-dimensional chiral hybrid organic–inorganic perovskite single crystals have remained difficult because they contain no chiral components and their crystal phases belong to centrosymmetric achiral point groups. Here we report a general approach to grow single-crystalline 3D lead halide perovskites with chiroptical activity. Taking MAPbBr3 (MA, methylammonium) perovskite as a representative example, whereas achiral MAPbBr3 crystallized from precursors in solution by inverse temperature crystallization method, the addition of micro- or nanoparticles as nucleating agents promoted the formation of chiral crystals under a near equilibrium state. Experimental characterization supported by calculations showed that the chirality of the 3D APbX3 (where A is an ammonium ion and X is Cl, Br or mixed Cl–Br or Br–I) perovskites arises from chiral patterns of the A-site cations and their interaction with the [PbX6]4− octahedra in the perovskite structure. The chiral structure obeys the lowest-energy principle and thereby thermodynamically stable. The chiral 3D hybrid organic–inorganic perovskites served in a circularly polarized light photodetector prototype successfully.

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Fig. 1: Controllable growth of chiral and achiral 3D MAPbBr3 single crystals.
Fig. 2: Chiroptical properties of 3D HOIPs and CsPbBr3 single crystals.
Fig. 3: Lattices, electronic structures, energies and bond angles of MAPbBr3 unit cells and supercells.
Fig. 4: The CPL photodetection of chiral and achiral MAPbBr3 single crystals.
Fig. 5: The CPL photodetection performance of a typical MAPbBr3-R crystal.

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All data are available in the main article and supplementary information, or on request from the corresponding authors. Source data are provided with this paper.

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Acknowledgements

This work was supported by National Key R&D Program of China (2017YFA0700101 and 2021YFA1500900), the National Natural Science Foundation of China (NSFC, nos. 22241502, 22035004, 22175095, 21871143, 22075147, 61775097, 22076095 and 22222605). The calculations were performed using supercomputers at Tsinghua National Laboratory for Information Science and Technology. We thank Y. K. Wang and Q. Q. He for their help in perovskite nanocrystal synthesis; P. Wang for the discussion of CD measurement; and J. H. Li, F. J. Li and H. Bian for the help in CPL photodetection experiments.

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  1. Shibin Wang

    Present address: Institute of Industrial Catalysis, State Key Laboratory Breeding Base of Green-Chemical Synthesis Technology, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou, China

Authors and Affiliations

  1. Jiangsu Collaborative Innovation Center of Biomedical Functional Materials, Jiangsu Key Laboratory of New Power Batteries, School of Chemistry and Materials Science, Nanjing Normal University, Nanjing, China

    Gaoyu Chen, Xiaoyu Liu, Jiakun An, Xiangxing Xu & Jianchun Bao

  2. Engineering Research Center of Advanced Rare Earth Materials, Department of Chemistry, Tsinghua University, Beijing, China

    Shibin Wang, Xiaokun Zhao, Han-Shi Hu, Jun Li & Xun Wang

  3. Jiangsu Key Laboratory of Optoelectronic Technology, School of Physics and Technology, Nanjing Normal University, Nanjing, China

    Zhongzheng Gu & Caojin Yuan

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Contributions

X.X. and X.W. conceived the project and supervised the research. G.C., X.L., J.A., J.B. and X.X. performed the synthesis and characterizations of the perovskite crystals. G.C. and X.L. contributed equally on the synthesis work. J.A. measured the dark I–V curves. X.X. and G.C. did the POM characterization. X.X., G.C., X.L., J.A., Z.G. and C.Y. performed the experiments of CPL photodetection. S.W., X.Z. and H.-S.H. developed the DFT and AIMD calculation models, and performed the theoretical analyses. X.X., H.-S.H., J.L. and X.W. co-wrote the paper with help from the other authors.

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Correspondence to Xiangxing Xu, Han-Shi Hu or Xun Wang.

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Chen, G., Liu, X., An, J. et al. Nucleation-mediated growth of chiral 3D organic–inorganic perovskite single crystals. Nat. Chem. 15, 1581–1590 (2023). https://doi.org/10.1038/s41557-023-01290-2

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