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Control and characterization of individual grains and grain boundaries in graphene grown by chemical vapour deposition

Abstract

The strong interest in graphene has motivated the scalable production of high-quality graphene and graphene devices. As the large-scale graphene films synthesized so far are typically polycrystalline, it is important to characterize and control grain boundaries, generally believed to degrade graphene quality. Here we study single-crystal graphene grains synthesized by ambient chemical vapour deposition on polycrystalline Cu, and show how individual boundaries between coalescing grains affect graphene’s electronic properties. The graphene grains show no definite epitaxial relationship with the Cu substrate, and can cross Cu grain boundaries. The edges of these grains are found to be predominantly parallel to zigzag directions. We show that grain boundaries give a significant Raman ‘D’ peak, impede electrical transport, and induce prominent weak localization indicative of intervalley scattering in graphene. Finally, we demonstrate an approach using pre-patterned growth seeds to control graphene nucleation, opening a route towards scalable fabrication of single-crystal graphene devices without grain boundaries.

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Figure 1: Graphene grains grown on Cu substrates.
Figure 2: Transmission electron microscopy and electron diffraction from graphene grains.
Figure 3: Scanning tunnelling microscopy of a single-crystal graphene grain on Cu.
Figure 4: Spectroscopic Raman mapping of graphene grains and grain boundaries.
Figure 5: Electronic transport cross a single grain boundary.
Figure 6: Seeded growth of graphene grains.

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Acknowledgements

Q.Y. acknowledges support from NSF and UHCAM. N.P.G. acknowledges support from DOE SISGR. E.A.S. acknowledges support from DOE BES. J.B. acknowledges support from TcSUH and the Welch Foundation. Y.P.C. acknowledges support from NSF, DTRA, DHS, IBM, the Miller Family Endowment and Midwest Institute for Nanoelectronics Discovery (MIND). STM measurements were carried out at Argonne National Laboratory under the support of the DOE user program.

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Contributions

W.W., R.C. and J.T. are equally contributing second authors. Q.Y. led the synthesis and Y.P.C. led the characterization efforts. Q.Y., W.W., Z.L. and Z.S. synthesized the graphene samples and performed SEM. R.C. and E.A.S. performed the TEM. J.T., H.C. and N.P.G. performed the STM. L.A.J. performed the Raman measurements. L.A.J. and H.C. fabricated the devices and performed electronic transport measurements. Q.Y., L.A.J., R.C., J.T., E.A.S. and Y.P.C. wrote the paper and all authors contributed to the discussions.

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Correspondence to Qingkai Yu or Yong P. Chen.

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Yu, Q., Jauregui, L., Wu, W. et al. Control and characterization of individual grains and grain boundaries in graphene grown by chemical vapour deposition. Nature Mater 10, 443–449 (2011). https://doi.org/10.1038/nmat3010

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