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Large-area single-crystal AB-bilayer and ABA-trilayer graphene grown on a Cu/Ni(111) foil

Abstract

High-quality AB-stacked bilayer or multilayer graphene larger than a centimetre has not been reported. Here, we report the fabrication and use of single-crystal Cu/Ni(111) alloy foils with controllable concentrations of Ni for the growth of large-area, high-quality AB-stacked bilayer and ABA-stacked trilayer graphene films by chemical vapour deposition. The stacking order, coverage and uniformity of the graphene films were evaluated by Raman spectroscopy and transmission electron microscopy including selected area electron diffraction and atomic resolution imaging. Electrical transport (carrier mobility and band-gap tunability) and thermal conductivity (the bilayer graphene has a thermal conductivity value of about 2,300 W m−1 K−1) measurements indicated the superior quality of the films. The tensile loading response of centimetre-scale bilayer graphene films supported by a 260-nm thick polycarbonate film was measured and the average values of the Young’s modulus (478 GPa) and fracture strength (3.31 GPa) were obtained.

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Fig. 1: Preparation and characterization of Cu/Ni(111) foils.
Fig. 2: Raman measurements of the bilayer and trilayer graphene.
Fig. 3: TEM and LEED characterization of a bilayer graphene film.
Fig. 4: Electrical transport measurements, thermal conductivity measurements and tensile tests of AB-stacked bilayer graphene film.

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 acknowledge support from the Institute for Basic Science (IBS-R019-D1).

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Contributions

R.S.R. proposed and supervised the research project. M.H. prepared the single-crystalline alloy foils, performed the graphene growth, conducted characterizations and data analyses. M.H. wrote the manuscript. M.H., P.V.B. and R.S.R. revised the manuscript. M.B. participated in graphene growth and Raman characterization. Z.J.-W. and M.-G.W. performed the in situ observation of the hydrogen etching of graphene. S.J. and Y.K. prepared the single-crystal copper foils. H.-J.P. and Z.L. carried out the HRTEM analysis. Z.Y., Y.L., D.Q. and W.-J.Y. made graphene devices and conducted transport measurements. B.W. and M.H. performed the tensile tests. P.V.B., X.C. and S.W.L. provided critical insights for the analysis and discussion. All authors discussed the results and commented on the manuscript.

Corresponding author

Correspondence to Rodney S. Ruoff.

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Peer review information Nature Nanotechnology thanks Jeremy Robinson and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary Information

Supplementary methods and notes, Figs. 1–26, Tables 1–5 and refs. 1–40.

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Huang, M., Bakharev, P.V., Wang, ZJ. et al. Large-area single-crystal AB-bilayer and ABA-trilayer graphene grown on a Cu/Ni(111) foil. Nat. Nanotechnol. 15, 289–295 (2020). https://doi.org/10.1038/s41565-019-0622-8

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