Abstract
The kinetic Wulff shape, determined by the crystal structure and growth rates of different crystal facets, is ubiquitous in classical crystal growth. However, its utilization for heterostructure integration remains largely unexplored. Here we report the discovery of kinetic Wulff-shaped heteroepitaxial growth in halide perovskites, which enables the realization of well-defined phase-pure 2D halide perovskite epitaxial heterostructures with deterministic slab thickness (n = 1–3). This approach allows modulation of the interfacial lattice mismatch from 0% to >11%. Two-___domain and complex heterostructures synthesized using this approach have well-defined chemical compositions and electronic structures that may enable the development of ultranarrow domains (less than the de Broglie wavelength of carriers) for solution-processed lateral quantum wells and superlattices. Finally, devices based on these heterostructures demonstrate substantial rectification ratios and reliable switching behaviours under optical or electrical inputs. This study presents the universality of kinetic Wulff-shaped epitaxy in achieving 2D halide perovskite epitaxial heterostructures with high phase purity.
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Data availability
The X-ray crystallographic coordinates for structures reported in this study have been deposited at the Cambridge Crystallographic Data Centre (CCDC), under deposition numbers CCDC 2376612 for (3T)2PbI4, CCDC 2376613 for (3T)2MAPb2I7, CCDC 2376614 for (3T)2SnI4, CCDC 2376615 for (3T)2MASn2I7, CCDC 2376616 for (3T)2PbCl4 and CCDC 2376617 for (3T)2PbBr4. These data can be obtained free of charge from The Cambridge Crystallographic Data Centre via www.ccdc.cam.ac.uk/data_request/cif. The additional data that substantiate the study’s findings and contribute to the assessment of the paper’s conclusions can be accessed within the Article and its Supplementary Information. Source data are provided with this paper.
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Acknowledgements
We thank J. Zhu and B. Pentice for helpful discussions. E.S. acknowledges the support from Research Center for Industries of the Future at Westlake University, Zhejiang Baima Lake Laboratory Co., Ltd., National Natural Science Foundation of China (grant no. 52272164), and the technical support from both the Instrumentation and Service Center for Molecular Science and the Instrumentation and Service Center for Physical Science at Westlake University. L.D. acknowledges the support from US Department of Energy, Office of Basic Energy Sciences under award number DE-SC0022082. J.D. acknowledges the support from National Natural Science Foundation of China (no. 22173109) and the CAS Project for Young Scientists in Basic Research (no. YSBR-053). Y.Y. acknowledges the support from the National Natural Science Foundation of China (52222311). The TEM characterizations were supported by the Center for high-resolution Electron Microscopy (ChEM) at ShanghaiTech University.
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Contributions
E.S. conceived the idea. M.X. and T.W. synthesized the 2D perovskite materials and heterostructures. T.W. performed device fabrication and measurements. J.D. performed phase-field simulation. Y. Lu and Y.Y. performed TEM characterization and data analysis. Y. Li, B.L., H.S., Y.G., Y. Liu and L.D. participated in data analysis and discussion. M.X., T.W. and E.S. wrote the manuscript. All authors read and revised the manuscript.
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Competing interests
E.S., M.X. and T.W. are applying for a patent based on the findings in this work. The other authors declare no competing interests.
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Nature Synthesis thanks Jin-Wook Lee and the other, anonymous, reviewer(s) for their contribution to the peer review of this work. Primary handling editor: Alexandra Groves, in collaboration with the Nature Synthesis team.
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Supplementary information
Supplementary Information
Supplementary Discussions, Figs. 1–30 and Tables 1–5.
Supplementary Data 1
The cif file of (3T)2PbCl4.
Supplementary Data 2
The cif file of (3T)2PbBr4.
Supplementary Data 3
The cif file of (3T)2PbI4.
Supplementary Data 4
The cif file of (3T)2MAPb2I7.
Supplementary Data 5
The cif file of (3T)2SnI4.
Supplementary Data 6
The cif file of (3T)2MASn2I7.
Source data
Source Data Fig. 1
The source data for Fig. 1g.
Source Data Fig. 2
The source data for Fig. 2 panels a (right), b (right), c (right), d (bottom), e (bottom), f (bottom) and g.
Source Data Fig. 3
The source data for Fig. 4c–e.
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Xia, M., Wang, T., Lu, Y. et al. Kinetic Wulff-shaped heteroepitaxy of phase-pure 2D perovskite heterostructures with deterministic slab thickness. Nat. Synth 4, 380–390 (2025). https://doi.org/10.1038/s44160-024-00692-5
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DOI: https://doi.org/10.1038/s44160-024-00692-5
