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Fast growth of inch-sized single-crystalline graphene from a controlled single nucleus on Cu–Ni alloys

Nature Materials volume 15, pages 43–47 (2016)Cite this article

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Abstract

Wafer-scale single-crystalline graphene monolayers are highly sought after as an ideal platform for electronic and other applications1,2,3. At present, state-of-the-art growth methods based on chemical vapour deposition allow the synthesis of one-centimetre-sized single-crystalline graphene domains in ∼12 h, by suppressing nucleation events on the growth substrate4. Here we demonstrate an efficient strategy for achieving large-area single-crystalline graphene by letting a single nucleus evolve into a monolayer at a fast rate. By locally feeding carbon precursors to a desired position of a substrate composed of an optimized Cu–Ni alloy, we synthesized an ∼1.5-inch-large graphene monolayer in 2.5 h. Localized feeding induces the formation of a single nucleus on the entire substrate, and the optimized alloy activates an isothermal segregation mechanism that greatly expedites the growth rate5,6. This approach may also prove effective for the synthesis of wafer-scale single-crystalline monolayers of other two-dimensional materials.

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Figure 1: Fast growth of 1.5-inch single-crystalline graphene on Cu85Ni15 surface.
Figure 2: Characterization of the feedstock local feeding and effect of alloy composition.
Figure 3: Investigation of graphene growth mechanism by carbon isotopes.
Figure 4: Decomposition of feedstock on Cu–Ni alloy and the diffusion of carbon atoms in the alloy catalyst.

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Acknowledgements

We thank J. Chen and X. Y. Liu for help with device fabrication. We thank R. Ding and Z. Liang from the Graphene Research and Characterization Center of China for their assistance in thickness verification of our graphene. The work in Shanghai Institute of Microsystem and Information Technology, Chinese Academy of Sciences is partially supported by the National Science and Technology Major Projects of China (Grant No. 2011ZX02707), the External Cooperation Program of the Chinese Academy of Science (Grant No. GJHZ 1306), CAS International Collaboration and Innovation Program on High Mobility Materials Engineering and the National Natural Science Foundation of China (Grant No. 11304337). The work in East China Normal University is supported by an NSFC grant (Grant No. 21303056) and the Shanghai Pujiang Program (13PJ1402600). The computations were performed in the Supercomputer Centre of East China Normal University. Q. Yu thanks K. Sun and H. Chen for discussion.

Author information

Author notes

  1. Tianru Wu, Xuefu Zhang and Qinghong Yuan: These authors contributed equally to this work.

Authors and Affiliations

  1. State Key Laboratory of Functional Materials for Informatics, Shanghai Institute of Microsystem and Information Technology, Chinese Academy of Sciences, 865 Changning Road, Shanghai 200050, China

    Tianru Wu, Xuefu Zhang, Guangyuan Lu, Huishan Wang, Haomin Wang, Xiaoming Xie & Mianheng Jiang

  2. Department of Physics, East China Normal University, 500 Dongchuan Road, Minhang, Shanghai 200241, China

    Qinghong Yuan

  3. Ingram School of Engineering, and MSEC, Texas State University, San Marcos, Texas 78666, USA

    Jiachen Xue, Zhihong Liu & Qingkai Yu

  4. University of Chinese Academy of Sciences, Beijing 100049, China

    Guangyuan Lu

  5. Institute of Textiles and Clothing, Hong Kong Polytechnic University, Kowloon, Hong Kong, China

    Feng Ding

  6. School of Physical Science and Technology, ShanghaiTech University, 319 Yueyang Road, Shanghai 200031, China

    Xiaoming Xie & Mianheng Jiang

Authors
  1. Tianru Wu
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Contributions

X.X. and Q. Yu designed the project. F.D. designed the theoretical part. T.W. realized the nucleation control and inch-sized SCG with X.Z. T.W., X.Z. and G.L. performed the characterizations. Q. Yu proposed the isotope experiments and validated the isothermal segregation mechanism; the isotope growth and Raman mapping were done by J.X. and Z.L. Q. Yuan performed the first-principles calculations together with F.D. Huishan Wang made the devices and carried out transport measurements, and Haomin Wang analysed the transport results. X.X., Q.K.Y. and F.D. co-wrote the manuscript. All of the authors participated in the data analysis, discussions of results and manuscript revisions.

Corresponding authors

Correspondence to Feng Ding, Qingkai Yu or Xiaoming Xie.

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The authors declare no competing financial interests.

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Wu, T., Zhang, X., Yuan, Q. et al. Fast growth of inch-sized single-crystalline graphene from a controlled single nucleus on Cu–Ni alloys. Nature Mater 15, 43–47 (2016). https://doi.org/10.1038/nmat4477

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