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Ultrafast growth of single-crystal graphene assisted by a continuous oxygen supply

Abstract

Graphene has a range of unique physical properties1,2 and could be of use in the development of a variety of electronic, photonic and photovoltaic devices3,4,5. For most applications, large-area high-quality graphene films are required and chemical vapour deposition (CVD) synthesis of graphene on copper surfaces has been of particular interest due to its simplicity and cost effectiveness6,7,8,9,10,11,12,13,14,15. However, the rates of growth for graphene by CVD on copper are less than 0.4 μm s–1, and therefore the synthesis of large, single-crystal graphene domains takes at least a few hours. Here, we show that single-crystal graphene can be grown on copper foils with a growth rate of 60 μm s–1. Our high growth rate is achieved by placing the copper foil above an oxide substrate with a gap of 15 μm between them. The oxide substrate provides a continuous supply of oxygen to the surface of the copper catalyst during the CVD growth, which significantly lowers the energy barrier to the decomposition of the carbon feedstock and increases the growth rate. With this approach, we are able to grow single-crystal graphene domains with a lateral size of 0.3 mm in just 5 s.

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Figure 1: Growth of graphene on Cu foils assisted by a continuous oxygen supply.
Figure 2: Single-crystal confirmation and quality characterization of the as-grown graphene domains.
Figure 3: Time evolution of graphene domain growth.
Figure 4: The theoretical exploration of the mechanism of oxygen-assisted fast graphene growth on the Cu surface.

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Acknowledgements

We are grateful to Z. Liu for the helpful comments. We thank F. Wang and T. Cao for their help revising the manuscript. This work was supported by the NSFC (51522201, 11474006, 21525310, 11234001, 11327902, 91433102, 91021007 and 11074005), the National Basic Research Program of China (2016YFA0300903, 2013CBA01603, 2014CB932500, 2012CB921300) and the National Program for Thousand Young Talents of China.

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Contributions

K.L. and X.X. conceived the project. K.L. supervised the project. X.X., Z.Z. and Z.H. conducted the growth experiment. X.X. performed STM, AES and LEED experiments. X.X., K.L., H.P., F.D., D.Y. and E.W. analysed the experimental data. Z.Z. and H.W. performed the transfer of the graphene. R.Q. and P.G. conducted the TEM experiments. Z.L., L.L., L.Z., H.S. and C.L. performed the electrical measurements. F.D., L.Q. and J.Z. performed theoretical calculations. All of the authors discussed the results and wrote the paper.

Corresponding authors

Correspondence to Feng Ding, Hailin Peng or Kaihui Liu.

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The authors declare no competing financial interests.

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Xu, X., Zhang, Z., Qiu, L. et al. Ultrafast growth of single-crystal graphene assisted by a continuous oxygen supply. Nature Nanotech 11, 930–935 (2016). https://doi.org/10.1038/nnano.2016.132

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