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Structural transformations in graphene studied with high spatial and temporal resolution

Nature Nanotechnology volume 4, pages 500–504 (2009)Cite this article

Abstract

Graphene has remarkable electronic properties, such as ballistic transport and quantum Hall effects1,2,3, and has also been used as a support for samples in high-resolution transmission electron microscopy4,5 and as a transparent electrode in photovoltaic devices6. There is now a demand for techniques that can manipulate the structural and physical properties of graphene, in conjunction with the facility to monitor the changes in situ with atomic precision. Here, we show that irradiation with an 80 kV electron beam can selectively remove monolayers in few-layer graphene sheets by means of electron-beam-induced sputtering. Aberration-corrected, low-voltage, high-resolution transmission electron microscopy with sub-ångström resolution is used to examine the structural reconstruction occurring at the single atomic level. We find preferential termination for graphene layers along the zigzag orientation for large hole sizes. The temporal resolution can also be reduced to 80 ms, enabling real-time observation of the reconstruction of carbon atoms during the sputtering process. We also report electron-beam-induced rapid displacement of monolayers, fast elastic distortions and flexible bending at the edges of graphene sheets. These results reveal how energy transfer from the electron beam to few-layer graphene sheets leads to unique structural transformations.

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Figure 1: HRTEM imaging of monolayer and few-layer graphene.
Figure 2: Selective destruction of graphene monolayer.
Figure 3: Zipper-like removal of carbon atoms.
Figure 4: Stepwise movement of carbon atoms.

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Acknowledgements

J.H.W. thanks the Violette and Samuel Glasstone Fund and Brasenose College, Oxford, for support. This work was supported in part by the Engineering and Physical Sciences Research Council (EPSRC) through the Quantum Information Processing Interdisciplinary Research Collaboration (GR/S82176/01). G.A.D.B. thanks the EPSRC for a Professorial Research Fellowship (GR/S15808/01). We thank J. H. Jefferson for discussions.

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Authors and Affiliations

  1. Department of Materials, Quantum Information Processing Interdisciplinary Research Collaboration, University of Oxford, Parks Road, Oxford, OX1 3PH, UK

    Jamie H. Warner, Ling Ge & G. Andrew D. Briggs

  2. IFW Dresden, PO Box 270116, Dresden, D-01171, Germany

    Mark H. Rümmeli, Thomas Gemming & Bernd Büchner

  3. STFC Rutherford Appleton Laboratory, Didcot, Oxfordshire, OX11 0QX, UK

    Barbara Montanari

  4. Department of Chemistry, Imperial College, London, SW7 2AZ, UK

    Nicholas M. Harrison

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  1. Jamie H. Warner
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  8. G. Andrew D. Briggs
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Contributions

J.H.W. designed and conducted the experiments, analysed the results and wrote the paper. M.R., T.G. and B.B. assisted with the HRTEM measurements. L.G., B.M. and N.M.H. performed the density functional theory (DFT). G.A.D.B. assisted in the analysis of the results.

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Correspondence to Jamie H. Warner.

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Warner, J., Rümmeli, M., Ge, L. et al. Structural transformations in graphene studied with high spatial and temporal resolution. Nature Nanotech 4, 500–504 (2009). https://doi.org/10.1038/nnano.2009.194

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