Abstract
The desirable properties of atomically thin materials (ATMs) have encouraged development of preparation methods. However, many multi-element layered and non-layered ATMs are still difficult to be fabricated in a controlled manner. Here we design a flux-assisted growth approach to overcome these limitations that can reproducibly prepare high-quality ATMs, such as metal chalcogenides, oxides, oxyhalides and phosphorous trichalcogenides, and is tolerant to growth parameters such as temperature and flow rate. In this approach, target materials nucleate and crystallize following a flux-crystallization mechanism, enabling precise control of their stoichiometry. ATMs are guaranteed by the confined synthetic space and kinetically driven growth. Eighty atomically thin composite flakes, including 48 ternary or quaternary compounds and 23 non-layered materials, have been successfully prepared by this approach. Furthermore, large single crystals or continuous films of ATMs can be prepared by the same method. This proposed flux-crystallization mechanism offers great possibilities to fabricate ATMs with good stoichiometry control and non-layered structures that possess interesting physical and chemical properties.
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The additional characterization data and experimental data are provided in the Supplementary Information and Supplementary Video. Source data are provided with this paper.
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Acknowledgements
This work was supported by the National Key R&D Program of China (grant number 2018YFA0306900), the Natural Science Foundation of China (22171016, 51872012, 21821004, 21932001) and the Beijing Outstanding Young Scientist Program (BJJWZYJH01201914430039). Part of calculations were supported by the high-performance computing (HPC) resources at Beihang University.
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Y.G., K.W. and P.Z. conceived and designed the experiments. P.Z., X.W., H.J. and Y.Z. synthesized the materials. X.W., H.J., Q.H. and H.Q. prepared the reaction powders by chemical vapour transport. P.Z., Q.H., X.W., H.J. and F.Z. performed the HRTEM characterizations of all samples, P.Z., X.W., H.J., Y.Z. and W.Z. worked on the analysis of HRTEM results. P.Z. and X.W. performed the AFM characterization of the samples. P.Z., B.L. and Y.Z. carried out Raman characterizations. K.S. performed device fabrication and measurement. A.C. and Z.H. carried out the PFM measurements. P.Z., X.W., H.J., K.W. and Y.G. wrote the paper with inputs from F.Z., Y.W., L.L., K.S. P.T. and W.Z. All authors participated in discussions and approved the manuscript.
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Nature Synthesis thanks Lei Liu, Youngdong Yoo and the other, anonymous, reviewer(s) for their contribution to the peer review of this work. Alexandra Groves, in collaboration with the Nature Synthesis team.
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Supplementary Information
Supplementary Figs. 1–155, Discussion and Tables 1–4.
Supplementary Video 1
In situ growth observation of Fe3GeTe2.
Supplementary Video 2
In situ growth observation of CoTe2.
Supplementary Video 3
In situ growth observation of NiTe2.
Source data
Source Data Fig. 1
Data used to generate histogram graphs.
Source Data Fig. 3
Data used to generate energy-dispersive spectroscopy curves.
Source Data Fig. 4
Data used to generate graphs.
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Zhang, P., Wang, X., Jiang, H. et al. Flux-assisted growth of atomically thin materials. Nat. Synth 1, 864–872 (2022). https://doi.org/10.1038/s44160-022-00165-7
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DOI: https://doi.org/10.1038/s44160-022-00165-7
