Abstract
Formation of epitaxial heterostructures via post-growth self-assembly is important in the design and preparation of functional hybrid systems combining unique properties of the constituents. This is particularly attractive for the construction of metal halide perovskite heterostructures, since their conventional solution synthesis usually leads to non-uniformity in composition, crystal phase and dimensionality. Herein, we demonstrate that a series of two-dimensional and three-dimensional perovskites of different composition and crystal phase can form epitaxial heterostructures through a ligand-assisted welding process at room temperature. Using the CsPbBr3/PEA2PbBr4 heterostructure as a demonstration, in addition to the effective charge and energy transfer across the epitaxial interface, localized lattice strain was observed at the interface, which was extended to the top layer of the two-dimensional perovskite, leading to multiple new sub-bandgap emissions at low temperature. Given the versatility of our strategy, unlimited hybrid systems are anticipated, yielding composition-, interface- and/or orientation-dependent properties.
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Acknowledgements
L.W. thanks the National Key Basic Research Program of China for support (grant no. 2020YFA0308900). X.H. thanks the National Key Basic Research Program of China (grant no. 2021YFB3200302) and the National Natural Science Foundation of China (grant no. 51832001). L.W. also thanks the National Natural Science Foundation of China (grant no. 92064010), the Fundamental Research Funds for the Central Universities of China, and the funding for ‘Distinguished Professors’ and ‘High-Level Talents in Six Industries’ of Jiangsu Province (grant no. XYDXX-021). X.H. and L.W. acknowledge the Development Program of Shaanxi Province (grant nos 2020GXLH-Z-020, 2020GXLH-Z-026 and 2020GXLH-Z-027). C.Z. thanks the National Natural Science Foundation of China (grant no. 11504046). Z.L. thanks the National Research Foundation Singapore programme (NRF-CRP22-2019-0007) and Singapore Ministry of Education via AcRF Tier 3 (MOE2018-T3-1-002) for support. H.Z. thanks the Innovation and Technology Commission (ITC) via the Hong Kong Branch of National Precious Metals Material Engineering Research Center and the Start-Up Grant at the City University of Hong Kong for support.
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X.H., L.W. and W.H. proposed the research direction and supervised the project. Z.Z., Lei Yang, Q.C. J.D. and S.Z. designed and synthesized the heterostructures and performed the TEM, X-ray diffraction, steady-state PL and ultraviolet spectroscopy. C.Z. and X.H. carried out and analysed the STEM of the microstructures of the heterointerfaces. W.Z., Y.C. and L.W. performed and analysed the temperature-dependent PL spectra of the heterostructure samples. Z.Z., S.Z. and J.C. carried out time-resolved PL. C.Y. and X.W. helped to analyse the time-resolved PL results. L.Z., X.H. and J.Y. provided theoretical calculations and analyses. J.B., B.C., H.G., H.C., N.W. and G.X. performed some supporting experiments. J.D., Zeyi Wang, H.L., S.L., Zhiwei Wang, Lijuan Yang, Y.Y., Z.L. and H.Z. contributed to the revision of the manuscript.
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Nature Materials thanks Giulia Grancini, Maria Sushko and Daniel Vanmaekelbergh for their contribution to the peer review of this work.
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Zhu, Z., Zhu, C., Yang, L. et al. Room-temperature epitaxial welding of 3D and 2D perovskites. Nat. Mater. 21, 1042–1049 (2022). https://doi.org/10.1038/s41563-022-01311-4
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DOI: https://doi.org/10.1038/s41563-022-01311-4
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