Skip to main content

Thank you for visiting nature.com. You are using a browser version with limited support for CSS. To obtain the best experience, we recommend you use a more up to date browser (or turn off compatibility mode in Internet Explorer). In the meantime, to ensure continued support, we are displaying the site without styles and JavaScript.

  • Letter
  • Published:

Epitaxial growth of single-domain graphene on hexagonal boron nitride

Nature Materials volume 12, pages 792–797 (2013)Cite this article

Subjects

This article has been updated

Abstract

Hexagonal boron nitride (h-BN) has recently emerged as an excellent substrate for graphene nanodevices, owing to its atomically flat surface and its potential to engineer graphene’s electronic structure1,2. Thus far, graphene/h-BN heterostructures have been obtained only through a transfer process1, which introduces structural uncertainties due to the random stacking between graphene and h-BN substrate2,3. Here we report the epitaxial growth of single-domain graphene on h-BN by a plasma-assisted deposition method. Large-area graphene single crystals were successfully grown for the first time on h-BN with a fixed stacking orientation. A two-dimensional (2D) superlattice of trigonal moiré pattern was observed on graphene by atomic force microscopy. Extra sets of Dirac points are produced as a result of the trigonal superlattice potential and the quantum Hall effect is observed with the 2D-superlattice-related feature developed in the fan diagram of longitudinal and Hall resistance, and the Dirac fermion physics near the original Dirac point is unperturbed. The macroscopic epitaxial graphene is in principle limited only by the size of the h-BN substrate and our synthesis method is potentially applicable on other flat surfaces. Our growth approach could thus open new ways of graphene band engineering through epitaxy on different substrates.

Access through your institution
Buy or subscribe

This is a preview of subscription content, access via your institution

Access options

Access through your institution

Buy this article

  • Purchase on SpringerLink
  • Instant access to full article PDF
Buy now

Prices may be subject to local taxes which are calculated during checkout

Figure 1: Epitaxial graphene growth.
Figure 2: Moiré pattern of epitaxial graphene.
Figure 3: Transport measurements and band structure of graphene superlattice.
Figure 4: QHE of MLG and BLG superlattices.
Figure 5: QHE fan diagram of MLG superlattice.

Similar content being viewed by others

Change history

  • 26 July 2013

    In the version of this Letter originally published online, the year of the received date should have read '2012'. In Fig. 5, the numbers 10, 20, 8.5 and 17 on the colour scale bars should not have been followed by 'k'. These errors have been corrected in all versions of the Letter.

References

  1. Dean, C. R. et al. Boron nitride substrates for high-quality graphene electronics. Nature Nanotech. 5, 722–726 (2010).

    Article  CAS  Google Scholar 

  2. Xue, J. M. et al. Scanning tunneling microscopy and spectroscopy of ultra-flat graphene on hexagonal boron nitride. Nature Mater. 10, 282–285 (2011).

    Article  CAS  Google Scholar 

  3. Yankowitz, M. et al. Emergence of superlattice Dirac points in graphene on hexagonal boron nitride. Nature Phys. 8, 382–386 (2012).

    Article  CAS  Google Scholar 

  4. Dean, C. R. et al. Multicomponent fractional quantum Hall effect in graphene. Nature Phys. 7, 693–696 (2011).

    Article  CAS  Google Scholar 

  5. Mayorov, A. S. et al. Micrometer-scale ballistic transport in encapsulated graphene at room temperature. Nano Lett. 11, 2396–2399 (2011).

    Article  CAS  Google Scholar 

  6. Yu, Q. et al. Graphene segregated on Ni surfaces and transferred to insulators. Appl. Phys. Lett. 93, 113103 (2008).

    Article  Google Scholar 

  7. Wofford, J. M. et al. Extraordinary epitaxial alignment of graphene islands on Au(111). New J. Phys. 14, 053008 (2012).

    Article  Google Scholar 

  8. Sutter, P., Lahiri, J., Zahl, P., Wang, B. & Sutter, E. Scalable synthesis of uniform few-layer hexagonal boron nitride dielectric films. Nano Lett. 13, 276–281 (2012).

    Article  Google Scholar 

  9. Ding, X. L., Ding, G. Q., Xie, X. M., Huang, F. Q. & Jiang, M. H. Direct growth of few layer graphene on hexagonal boron nitride by chemical vapor deposition. Carbon 49, 2522–2525 (2011).

    Article  CAS  Google Scholar 

  10. Son, M., Lim, H., Hong, M. & Choi, H. C. Direct growth of graphene pad on exfoliated hexagonal boron nitride surface. Nanoscale 3, 3089–3093 (2011).

    Article  CAS  Google Scholar 

  11. Tang, S. J. et al. Nucleation and growth of single crystal graphene on hexagonal boron nitride. Carbon 50, 329–331 (2012).

    Article  CAS  Google Scholar 

  12. Zhang, L. C. et al. Vapour-phase graphene epitaxy at low temperatures. Nano Res. 5, 258–264 (2012).

    Article  CAS  Google Scholar 

  13. Zhang, L. C. et al. Catalyst-free growth of nanographene film on various substrates. Nano Res. 4, 315–321 (2011).

    Article  CAS  Google Scholar 

  14. Yang, W. et al. Characterization, and properties of nanographene. Small 8, 1429–1435 (2012).

    Article  CAS  Google Scholar 

  15. Yang, R. et al. An anisotropic etching effect in the graphene basal plane. Adv. Mater. 22, 4014–4019 (2010).

    Article  CAS  Google Scholar 

  16. Geick, R., Perry, C. H. & Rupprecht, G. Normal modes in hexagonal boron nitride. Phys. Rev. 146, 543–547 (1966).

    Article  CAS  Google Scholar 

  17. Ferrari, A. C. et al. Raman spectrum of graphene and graphene layers. Phys. Rev. Lett. 97, 187401 (2006).

    Article  CAS  Google Scholar 

  18. Malard, L. M., Pimenta, M. A., Dresselhaus, G. & Dresselhaus, M. S. Raman spectroscopy in graphene. Phys. Rep. 473, 51–87 (2009).

    Article  CAS  Google Scholar 

  19. Dresselhaus, M. S., Jorio, A., Hofmann, M., Dresselhaus, G. & Saito, R. Perspectives on carbon nanotubes and graphene Raman spectroscopy. Nano Lett. 10, 751–758 (2010).

    Article  CAS  Google Scholar 

  20. Shi, Z. W. et al. Patterning graphene with zigzag edges by self-aligned anisotropic etching. Adv. Mater. 23, 3061–3065 (2011).

    Article  CAS  Google Scholar 

  21. Yang, R., Shi, Z. W., Zhang, L. C., Shi, D. X. & Zhang, G. Y. Observation of Raman G-Peak split for graphene nanoribbons with hydrogen-terminated zigzag edges. Nano Lett. 11, 4083–4088 (2011).

    Article  CAS  Google Scholar 

  22. Koma, A. Van der Waals epitaxy for highly lattice-mismatched systems. J. Cryst. Growth 201–202, 236–241 (1999).

    Article  Google Scholar 

  23. Altshuler, B. L., Aronov, A. G. & Lee, P. A. Interaction effects in disordered Fermi systems in two dimensions. Phys. Rev. Lett. 44, 1288–1291 (1980).

    Article  CAS  Google Scholar 

  24. Park, C-H., Yang, L., Son, Y-W., Cohen, M. L. & Louie, S. G. Anisotropic behaviors of massless Dirac fermions in graphene under periodic potential. Nature Phys. 4, 213–217 (2008).

    Article  CAS  Google Scholar 

  25. Park, C-H., Yang, L., Son, Y-W., Cohen, M. L. & Louie, S. G. New generation of massless Dirac fermions in graphene under external periodic potentials. Phys. Rev. Lett. 101, 126804 (2008).

    Article  Google Scholar 

  26. Brey, L. & Fertig, H. A. Emerging zero modes for graphene in a periodic potential. Phys. Rev. Lett. 103, 046809 (2009).

    Article  CAS  Google Scholar 

  27. Novoselov, K. S. et al. Two-dimensional gas of massless Dirac fermions in graphene. Nature 438, 197–200 (2005).

    Article  CAS  Google Scholar 

  28. Zhang, Y. B., Tan, Y. W., Stormer, H. L. & Kim, P. Experimental observation of the quantum Hall effect and Berry’s phase in graphene. Nature 438, 201–204 (2005).

    Article  CAS  Google Scholar 

  29. Gusynin, V. P. & Sharapov, S. G. Unconventional integer quantum hall effect in graphene. Phys. Rev. Lett. 95, 146801 (2005).

    Article  CAS  Google Scholar 

  30. Novoselov, K. S. et al. Unconventional quantum Hall effect and Berry’s phase of 2π in bilayer graphene. Nature Phys. 2, 177–180 (2006).

    Article  Google Scholar 

Download references

Acknowledgements

The authors would like to thank H. Dai and F. Wang and Y. Yu for helpful discussions. G.Z. acknowledges supports from the 973 Program (2013CB934500 and 2012CB921302), the NSFC (91223204), and the ‘100 talents project’ of CAS. Y.Z. acknowledges supports from the 973 Program (2011CB921802) and NSFC (11034001). Y.Y. acknowledges supports from 973 Program (2011CBA00100) and NSFC (10974231, 11174337 and 11225418).

Author information

Authors and Affiliations

  1. Beijing National Laboratory for Condensed Matter Physics and Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China

    Wei Yang, Zhiwen Shi, Cheng-Cheng Liu, Lianchang Zhang, Guibai Xie, Meng Cheng, Duoming Wang, Rong Yang, Dongxia Shi & Guangyu Zhang

  2. State Key Laboratory of Surface Physics and Department of Physics, Fudan University, Shanghai 200433, China

    Guorui Chen & Yuanbo Zhang

  3. School of Physics, Beijing Institute of Technology, Beijing 100081, China

    Cheng-Cheng Liu & Yugui Yao

  4. Department of Physics, Kunming University, Kunming 650214, China

    Lianchang Zhang

  5. Advanced Materials Laboratory, National Institute for Materials Science, 1-1 Namiki, Tsukuba, 305-0044, Japan

    Kenji Watanabe & Takashi Taniguchi

Authors
  1. Wei Yang
    View author publications

    You can also search for this author inPubMed Google Scholar

  2. Guorui Chen
    View author publications

    You can also search for this author inPubMed Google Scholar

  3. Zhiwen Shi
    View author publications

    You can also search for this author inPubMed Google Scholar

  4. Cheng-Cheng Liu
    View author publications

    You can also search for this author inPubMed Google Scholar

  5. Lianchang Zhang
    View author publications

    You can also search for this author inPubMed Google Scholar

  6. Guibai Xie
    View author publications

    You can also search for this author inPubMed Google Scholar

  7. Meng Cheng
    View author publications

    You can also search for this author inPubMed Google Scholar

  8. Duoming Wang
    View author publications

    You can also search for this author inPubMed Google Scholar

  9. Rong Yang
    View author publications

    You can also search for this author inPubMed Google Scholar

  10. Dongxia Shi
    View author publications

    You can also search for this author inPubMed Google Scholar

  11. Kenji Watanabe
    View author publications

    You can also search for this author inPubMed Google Scholar

  12. Takashi Taniguchi
    View author publications

    You can also search for this author inPubMed Google Scholar

  13. Yugui Yao
    View author publications

    You can also search for this author inPubMed Google Scholar

  14. Yuanbo Zhang
    View author publications

    You can also search for this author inPubMed Google Scholar

  15. Guangyu Zhang
    View author publications

    You can also search for this author inPubMed Google Scholar

Contributions

G.Z. and Y.Z. designed the research; W.Y. performed the growth, structural characterization, device fabrication and electrical transport measurements; Z.S. helped with QHE measurements; G.C provided the h-BN substrates and helped with QHE measurements; K.W. and T.T. synthesized h-BN crystals; and C-C.L. carried out the band structure calculations. W.Y., G.C., Z.S., R.Y., D.S., Y.Y., Y.Z and G.Z. analysed data; W.Y., G.C., Y.Z. and G.Z. wrote, and all authors commented on, the manuscript.

Corresponding author

Correspondence to Guangyu Zhang.

Ethics declarations

Competing interests

The authors declare no competing financial interests.

Supplementary information

Supplementary Information

Supplementary Information (PDF 1490 kb)

Rights and permissions

Reprints and permissions

About this article

Cite this article

Yang, W., Chen, G., Shi, Z. et al. Epitaxial growth of single-domain graphene on hexagonal boron nitride. Nature Mater 12, 792–797 (2013). https://doi.org/10.1038/nmat3695

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1038/nmat3695

Search

Advanced search

Quick links

Nature Briefing

Sign up for the Nature Briefing newsletter — what matters in science, free to your inbox daily.

Get the most important science stories of the day, free in your inbox. Sign up for Nature Briefing