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Vapour-phase graphene epitaxy at low temperatures

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Abstract

We report an epitaxial growth of graphene, including homo- and hetero-epitaxy on graphite and SiC substrates, at a temperature as low as ∼540 °C. This vapour-phase epitaxial growth, carried out in a remote plasma-enhanced chemical vapor deposition (RPECVD) system using methane as the carbon source, can yield large-area high-quality graphene with the desired number of layers over the entire substrate surfaces following an AB-stacking layer-by-layer growth model. We also developed a facile transfer method to transfer a typical continuous one layer epitaxial graphene with second layer graphene islands on top of the first layer with the coverage of the second layer graphene islands being 20% (1.2 layer epitaxial graphene) from a SiC substrate onto SiO2 and measured the resistivity, carrier density and mobility. Our work provides a new strategy toward the growth of graphene and broadens its prospects of application in future electronics.

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References

  1. Jo, G.; Choe, M.; Cho, C. Y.; Kim, J. H.; Park, W.; Lee, S.; Hong, W. K.; Kim, T. W.; Park, S. J.; Hong, B. H. et al. Large-scale patterned multi-layer graphene films as transparent conducting electrodes for GaN light-emitting diodes. Nanotechnology 2010, 21, 175201.

    Article  Google Scholar 

  2. Kim, K. S.; Zhao, Y.; Jang, H.; Lee, S. Y.; Kim, J. M.; Kim, K. S.; Ahn, J. H.; Kim, P.; Choi, J. Y.; Hong, B. H. Large-scale pattern growth of graphene films for stretchable transparent electrodes. Nature 2009, 457, 706–710.

    Article  CAS  Google Scholar 

  3. Li, X. L.; Zhang, G. Y.; Bai, X. D.; Sun, X. M.; Wang, X. R.; Wang, E.; Dai, H. J. Highly conducting graphene sheets and Langmuir-Blodgett films. Nat. Nanotechnol. 2008, 3, 538–542.

    Article  CAS  Google Scholar 

  4. De, S.; King, P. J.; Lotya, M.; O’Neill, A.; Doherty, E. M.; Hernandez, Y.; Duesberg, G. S.; Coleman, J. N. Flexible, transparent, conducting films of randomly stacked graphene from surfactant-stabilized, oxide-free graphene dispersions. Small 2010, 6, 458–464.

    Article  CAS  Google Scholar 

  5. Wang, S. J.; Geng, Y.; Zheng, Q. B.; Kim, J. K. Fabrication of highly conducting and transparent graphene films. Carbon 2010, 48, 1815–1823.

    Article  CAS  Google Scholar 

  6. Novoselov, K. S.; Geim, A. K.; Morozov, S. V.; Jiang, D.; Zhang, Y.; Dubonos, S. V.; Grigorieva, I. V.; Firsov, A. A. Electric field effect in atomically thin carbon films. Science 2004, 306, 666–669.

    Article  CAS  Google Scholar 

  7. Hernandez, Y.; Nicolosi, V.; Lotya, M.; Blighe, F. M.; Sun, Z. Y.; De, S.; McGovern, I. T.; Holland, B.; Byrne, M.; Gun’ko, Y. K. et al. High-yield production of graphene by liquid-phase exfoliation of graphite. Nat. Nanotechnol. 2008, 3, 563–568.

    Article  CAS  Google Scholar 

  8. Bourlinos, A. B.; Georgakilas, V.; Zboril, R.; Steriotis, T. A.; Stubos, A. K. Liquid-phase exfoliation of graphite towards solubilized graphenes. Small 2009, 5, 1841–1845.

    Article  CAS  Google Scholar 

  9. Lotya, M.; Hernandez, Y.; King, P. J.; Smith, R. J.; Nicolosi, V.; Karlsson, L. S.; Blighe, F. M.; De, S.; Wang, Z. M.; McGovern, I. T. et al. Liquid phase production of graphene by exfoliation of graphite in surfactant/water solutions. J. Am. Chem. Soc. 2009, 131, 3611–3620.

    Article  CAS  Google Scholar 

  10. Gómez-Navarro, C.; Weitz, R. T.; Bittner, A. M.; Scolari, M.; Mews, A.; Burghard, M.; Kern, K. Electronic transport properties of individual chemically reduced graphene oxide sheets. Nano Lett. 2007, 7, 3499–3503.

    Article  Google Scholar 

  11. Becerril, H. A.; Mao, J.; Liu, Z.; Stoltenberg, R. M.; Bao, Z.; Chen, Y. Evaluation of solution-processed reduced graphene oxide films as transparent conductors. ACS Nano 2008, 2, 463–470.

    Article  CAS  Google Scholar 

  12. Eda, G.; Fanchini, G.; Chhowalla, M. Large-area ultrathin films of reduced graphene oxide as a transparent and flexible electronic material. Nat. Nanotechnol. 2008, 3, 270–274.

    Article  CAS  Google Scholar 

  13. Stankovich, S.; Dikin, D. A.; Piner, R. D.; Kohlhaas, K. A.; Kleinhammes, A.; Jia, Y.; Wu, Y.; Nguyen, S. T.; Ruoff, R. S. Synthesis of graphene-based nanosheets via chemical reduction of exfoliated graphite oxide. Carbon 2007, 45, 1558–1565.

    Article  CAS  Google Scholar 

  14. Kim, K. S.; Zhao, Y.; Jang, H.; Lee, S. Y.; Kim, J. M.; Kim, K. S.; Ahn, J. H.; Kim, P.; Choi, J. Y.; Hong, B. H. Large-scale pattern growth of graphene films for stretchable transparent electrodes. Nature 2009, 457, 706–710.

    Article  CAS  Google Scholar 

  15. Reina, A.; Jia, X. T.; Ho, J.; Nezich, D.; Son, H. B.; Bulovic, V.; Dresselhaus, M. S.; Kong, J. Large area, few-layer graphene films on arbitrary substrates by chemical vapor deposition. Nano Lett. 2009, 9, 30–35.

    Article  CAS  Google Scholar 

  16. Yu, Q. K.; Lian, J.; Siriponglert, S.; Li, H.; Chen, Y. P.; Pei, S. S. Graphene segregated on Ni surfaces and transferred to insulators. Appl. Phys. Lett. 2008, 93, 113103.

    Article  Google Scholar 

  17. Li, X. S.; Cai, W. W.; An, J. H.; Kim, S.; Nah, J.; Yang, D. X.; Piner, R.; Velamakanni, A.; Jung, I.; Tutuc, E. et al. Large-area synthesis of high-quality and uniform graphene films on copper foils. Science 2009, 324, 1312–1314.

    Article  CAS  Google Scholar 

  18. Emtsev, K. V.; Bostwick, A.; Horn, K.; Jobst, J.; Kellogg, G. L.; Ley, L.; McChesney, J. L.; Ohta, T.; Reshanov, S. A.; Röhrl, J. et al. Towards wafer-size graphene layers by atmospheric pressure graphitization of silicon carbide. Nat. Mater. 2009, 8, 203–207.

    Article  CAS  Google Scholar 

  19. Bolen, M. L.; Harrison, S. E.; Biedermann, L. B.; Capano, M. A. Graphene formation mechanisms on 4H-SiC(0001). Phys. Rev. B 2009, 80, 115433.

    Article  Google Scholar 

  20. Jernigan, G. G.; VanMil, B. L.; Tedesco, J. L.; Tischler, J. G.; Glaser, E. R.; Davidson, A.; Campbell, P. M.; Gaskill, D. K. Comparison of epitaxial graphene on Si-face and C-face 4H SiC formed by ultrahigh vacuum and RF furnace production. Nano Lett. 2009, 9, 2605–2609.

    Article  CAS  Google Scholar 

  21. Cambaz, Z. G.; Yushin, G.; Osswald, S.; Mochalin, V.; Goyotsi, Y. Noncatalytic synthesis of carbon nanotubes, graphene and graphite on SiC. Carbon 2008, 46, 841–849.

    Article  CAS  Google Scholar 

  22. Chae, S. J; Günes, F.; Kim, K. K.; Kim, E. S.; Han, G. H.; Kim, S. M.; Shin, H. J.; Yoon, S. M.; Choi, J. Y.; Park, M. H. et al. Synthesis of large-area graphene layers on poly-nickel substrate by chemical vapor deposition: Wrinkle formation. Adv. Mater. 2009, 21, 2328–2333.

    Article  CAS  Google Scholar 

  23. Zhang, L. C.; Shi, Z. W.; Wang, Y.; Yang, R.; Shi, D. X.; Zhang, G. Y. Catalyst-free growth of nanographene films on various substrates. Nano Res. 2011, 4, 315–321.

    Article  CAS  Google Scholar 

  24. Lee, D. S.; Riedl, C.; Krauss, B.; von Klitzing, K.; Starke, U.; Smet, J. H. Raman spectra of epitaxial graphene on SiC and of epitaxial graphene transferred to SiO2. Nano Lett. 2008, 8, 4320–4325.

    Article  CAS  Google Scholar 

  25. Yang, R.; Zhang, L. C.; Wang, Y.; Shi, Z. W.; Shi, D.X.; Gao, H. J.; Wang, E. G.; Zhang, G. Y. An anisotropic etching effect in the graphene basal plane. Adv. Mater. 2010, 22, 4014–4019.

    Article  CAS  Google Scholar 

  26. Unarunotai, S.; Murata, Y.; Chialvo, C. E.; Kim, H. S.; MacLaren, S.; Mason, N.; Petrov, I.; Rogers, J. A. Transfer of graphene layers grown on SiC wafers to other substrates and their integration into field effect transistors. Appl. Phys. Lett. 2009, 95, 202101.

    Article  Google Scholar 

  27. Romero, H. E.; Shen, N.; Joshi, P.; Gutierrez, H. R.; Tadigadapa, S. A.; Sofo, J. O.; Eklund, P. C. N-Type behavior of graphene supported on Si/SiO2 substrates. ACS Nano 2008, 2, 2037–2044.

    Article  CAS  Google Scholar 

  28. Morozov, S. V.; Novoselov, K. S.; Katsnelson, M. I.; Schedin, F.; Elias, D. C.; Jaszczak, J. A.; Geim, A. K. Giant intrinsic carrier mobilities in graphene and its bilayer. Phys. Rev. Lett. 2008, 100, 016602.

    Article  CAS  Google Scholar 

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Correspondence to Guangyu Zhang.

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Zhang, L., Shi, Z., Liu, D. et al. Vapour-phase graphene epitaxy at low temperatures. Nano Res. 5, 258–264 (2012). https://doi.org/10.1007/s12274-012-0205-6

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  • DOI: https://doi.org/10.1007/s12274-012-0205-6

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