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Wafer-scale single-crystal monolayer graphene grown on sapphire substrate

Abstract

The growth of inch-scale high-quality graphene on insulating substrates is desirable for electronic and optoelectronic applications, but remains challenging due to the lack of metal catalysis. Here we demonstrate the wafer-scale synthesis of adlayer-free ultra-flat single-crystal monolayer graphene on sapphire substrates. We converted polycrystalline Cu foil placed on Al2O3(0001) into single-crystal Cu(111) film via annealing, and then achieved epitaxial growth of graphene at the interface between Cu(111) and Al2O3(0001) by multi-cycle plasma etching-assisted–chemical vapour deposition. Immersion in liquid nitrogen followed by rapid heating causes the Cu(111) film to bulge and peel off easily, while the graphene film remains on the sapphire substrate without degradation. Field-effect transistors fabricated on as-grown graphene exhibited good electronic transport properties with high carrier mobilities. This work breaks a bottleneck of synthesizing wafer-scale single-crystal monolayer graphene on insulating substrates and could contribute to next-generation graphene-based nanodevices.

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Fig. 1: Wafer-scale single-crystal Cu(111) film formed on Al2O3(0001).
Fig. 2: Growth of single-crystal graphene at the Cu(111)–Al2O3(0001) interface.
Fig. 3: Synthesis of wafer-scale single-crystal graphene film on Al2O3(0001).
Fig. 4: DFT simulations and carbon diffusion model.
Fig. 5: Electronic transport properties of GFETs.

Data availability

The data that support the findings of this study are available from the corresponding author on reasonable request.

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Acknowledgements

We thank A. Chen for providing suggestions on device fabrication. We thank F. Laquai and Y. Gao for help with UV–vis spectrum measurements, and N. Wehbe for help with D-SIMS measurements. We thank D. Luo and M. Wang for comments. X.Z. acknowledges the support from KAUST, under award numbers OSR-2018-CRG7-3717 and OSR-2016-CRG5-2996, and R.S.R. acknowledges the support from IBS-R-019-D1.

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Authors and Affiliations

Authors

Contributions

J.L. and B.T. conceived the experiments. X.Z. supervised the project. J.L. and H.D. performed the annealing of the Cu foils and their characterizations. J.L., M.C., X.J. and H.D. performed the graphene growth and transfer experiments. J.L., H.D. and B.T. performed the Raman, SEM, AFM and XRD characterizations. J.Z. performed the TEM characterization for 2D materials. C.C., Y.H. and B.T. performed the focused ion beam analysis, HR–TEM, HAADF–STEM and energy dispersive spectroscopy characterizations for the cross-section. J.D. and T.F. performed the LEED and STM characterizations. A.S., A.R. and U.S. performed the DFT simulations. B.T. performed the fabrication of GFETs and electronic transport property measurements. R.S.R. provided various insights and particularly about the role of nitrogen in causing deformation of the Cu(111) film. U.S., T.F., R.S.R. and X.Z. provided comments on the paper. R.S.R. did a major revision of the paper and Supplementary Information document. J.L. and B.T. wrote the paper. All coauthors revised and commented on the paper.

Corresponding authors

Correspondence to Bo Tian or Xixiang Zhang.

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Supplementary information

Supplementary Information

Supplementary Figs. 1–35, Discussion and Tables 1–4.

Supplementary Video 1

Schematic animation of direct growth of single-crystalline graphene on insulating substrates by MPE–CVD.

Supplementary Video 2

Schematic animation of the liquid nitrogen-assisted separation methods.

Supplementary Video 3

A video recording of the sample immersion in liquid nitrogen followed by its rapid heating to 500 °C.

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Li, J., Chen, M., Samad, A. et al. Wafer-scale single-crystal monolayer graphene grown on sapphire substrate. Nat. Mater. 21, 740–747 (2022). https://doi.org/10.1038/s41563-021-01174-1

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