Roll-to-roll production of 30-inch graphene films for transparent electrodes (original) (raw)

Nature Nanotechnology volume 5, pages 574–578 (2010)Cite this article

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Abstract

The outstanding electrical1, mechanical2,3 and chemical4,5 properties of graphene make it attractive for applications in flexible electronics6,7,8. However, efforts to make transparent conducting films from graphene have been hampered by the lack of efficient methods for the synthesis, transfer and doping of graphene at the scale and quality required for applications. Here, we report the roll-to-roll production and wet-chemical doping of predominantly monolayer 30-inch graphene films grown by chemical vapour deposition onto flexible copper substrates. The films have sheet resistances as low as ∼125 Ω □−1 with 97.4% optical transmittance, and exhibit the half-integer quantum Hall effect, indicating their high quality. We further use layer-by-layer stacking to fabricate a doped four-layer film and measure its sheet resistance at values as low as ∼30 Ω □−1 at ∼90% transparency, which is superior to commercial transparent electrodes such as indium tin oxides. Graphene electrodes were incorporated into a fully functional touch-screen panel device capable of withstanding high strain.

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In the PDF version of this Letter originally published online, the authors were listed incorrectly. This error has now been corrected.

References

  1. Geim, A. K. & Novoselov, K. S. The rise of graphene. Nature Mater. 6, 183–191 (2007).
    Article CAS Google Scholar
  2. Lee, C., Wei, X., Kysar, J. W. & Hone, J. Measurement of the elastic properties and intrinsic strength of monolayer graphene. Science 321, 385–388 (2008).
    Article CAS Google Scholar
  3. Bunch, J. S. et al. Impermeable atomic membranes from graphene sheets. Nano Lett. 8, 2458–2462 (2008).
    Article CAS Google Scholar
  4. Elias, D. C. et al. Control of graphene's properties by reversible hydrogenation: evidence for graphene. Science 323, 610–613 (2009).
    Article CAS Google Scholar
  5. Wang, X. et al. N-doping of graphene through electrothermal reactions with ammonia. Science 324, 768–771 (2009).
    Article CAS Google Scholar
  6. Kim, K. S. et al. Large-scale pattern growth of graphene films for stretchable transparent electrodes. Nature 457, 706–710 (2009).
    Article CAS Google Scholar
  7. Kim, D.-H. et al. Stretchable and foldable silicon integrated circuits. Science 320, 507–511 (2008).
    Article CAS Google Scholar
  8. Sekitani, T. et al. A rubberlike stretchable active matrix using elastic conductors. Science 321, 1468–1472 (2008).
    Article CAS Google Scholar
  9. Reina, A. et al. Large area, few-layer graphene films on arbitrary substrates by chemical vapor deposition. Nano Lett. 9, 30–35 (2009).
    Article CAS Google Scholar
  10. Cai, W. W. et al. Large area few-layer graphene/graphite films as transparent thin conducting electrodes. Appl. Phys. Lett. 95, 123115 (2009).
    Article Google Scholar
  11. Lee, Y. et al. Wafer-scale synthesis and transfer of graphene films. Nano Lett. 10, 490–493 (2010).
    Article CAS Google Scholar
  12. Caldwell, J. D. et al. Technique for the dry transfer of epitaxial graphene onto arbitrary substrates. ACS Nano 4, 1108–1114 (2010).
    Article CAS Google Scholar
  13. Li, X. et al. Large-area synthesis of high-quality and uniform graphene films on copper foils. Science 324, 1312–1314 (2009).
    Article CAS Google Scholar
  14. Ahn, S. H. & Guo, L. J. High-speed roll-to-roll nanoimprint lithography on flexible plastic substrates. Adv. Mater. 20, 2044–2049 (2008).
    Article CAS Google Scholar
  15. Yerushalmi, R., Jacobson, Z. A., Ho, J. C., Fan, Z. & Javey, A. Large scale, highly ordered assembly of nanowire parallel arrays by differential roll printing. Appl. Phys. Lett. 91, 203104 (2007).
    Article Google Scholar
  16. Chang, Y. K. & Hong, F. C. The fabrication of ZnO nanowire field-effect transistors by roll-transfer printing. Nanotechnology 20, 195302 (2009).
    Article Google Scholar
  17. Jo, G. et al. Etching solution for etching Cu and Cu/Ti metal layer of liquid crystal display device and method of fabricating the same. US patent, 6,881,679 (2005).
  18. Hecht, D. S. et al. Carbon nanotube film on plastic as transparent electrode for resistive touch screens. J. Soc. Inf. Display 17, 941–946 (2009).
    Article CAS Google Scholar
  19. Li, X. et al. Transfer of large-area graphene films for high-performance transparent conductive electrodes. Nano Lett. 9, 4359–4363 (2009).
    Article CAS Google Scholar
  20. Hass, J. et al. Why multilayer graphene on 4H-SiC(000–1) behaves like a single sheet of graphene. Phys. Rev. Lett. 100, 125504 (2008).
    Article CAS Google Scholar
  21. Sprinkle, M. et al. First direct observation of a nearly ideal graphene band structure. Phys. Rev. Lett. 103, 226803 (2009).
    Article CAS Google Scholar
  22. Ferrari, A. C. et al. Raman spectrum of graphene and graphene layers. Phys. Rev. Lett. 97, 187401 (2006).
    Article CAS Google Scholar
  23. Nair, R. R. et al. Fine structure constant defines visual transparency of graphene. Science 320, 1308 (2008).
    Article CAS Google Scholar
  24. Das, A. et al. Monitoring dopants by Raman scattering in an electrochemically top-gated graphene transistor. Nature Nanotech. 3, 210–215 (2008).
    Article CAS Google Scholar
  25. Geng, H.-Z. et al. Effect of acid treatment on carbon nanotube-based flexible transparent conducting films. J. Am. Chem. Soc. 129, 7758–7759 (2007).
    Article CAS Google Scholar
  26. Schrivera, M., Reganb, W., Losterb, M. & Zettl, A. Carbon nanostructure–aSi:H photovoltaic cells with high open-circuit voltage fabricated without dopants. Solid State Commun. 150, 561–563 (2010).
    Article Google Scholar
  27. Wu, J. et al. Organic light-emitting diodes on solution-processed graphene transparent electrodes. ACS Nano 4, 43–48 (2010).
    Article CAS Google Scholar
  28. Lee, J.-Y., Connor, S. T., Cui, Y. & Peumans, P. Solution-processed metal nanowire mesh transparent electrodes. Nano Lett. 8, 689–692 (2008).
    Article CAS Google Scholar
  29. Cao, H. L. et al. Electronic transport in chemical vapor deposited graphene synthesized on Cu: Quantum Hall effect and weak localization. Appl. Phys. Lett. 96, 122106 (2010).
    Article Google Scholar
  30. Cairns, D. R. et al. Strain-dependent electrical resistance of tin-doped indium oxide on polymer substrates. Appl. Phys. Lett. 76, 1425–1427 (2000).
    Article CAS Google Scholar

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Acknowledgements

This work was supported by the National Research Foundation of Korea (NRF), funded by the Ministry of Education, Science and Technology (2009-0081966, 2009-0082608, 2009-0083540, 2009-0090017, World Class University R33-2008-000-10138-0, National Honor Scientist Program), the Research Centre of Breakthrough Technology Program through the Korea Institute of Energy Technology Evaluation and Planning (KETEP), funded by the Ministry of Knowledge Economy (2009-3021010030-11-1), Singapore National Research Foundation (NRF-RF2008-07) & NUS NanoCore, and T.J. Park Junior Faculty Fellowship. The authors thank R. Ruoff (University of Texas at Austin) and P. Kim (Columbia University) for helpful comments, W.S. Lim, K.D. Kim and Y.D. Kim (SKKU) for assistance in XPS analysis, and Samkwang Well Tech Co. for assistance with the touch-panel fabrication.

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Author notes

  1. Sukang Bae and Hyeongkeun Kim: These authors contributed equally to this work

Authors and Affiliations

  1. SKKU Advanced Institute of Nanotechnology (SAINT) and Center for Human Interface Nano Technology (HINT), Sungkyunkwan University, Suwon, 440-746, Korea
    Sukang Bae, Hyeongkeun Kim, Youngbin Lee, Tian Lei, Young-Jin Kim, Jong-Hyun Ahn, Byung Hee Hong & Sumio Iijima
  2. Department of Chemistry, Sungkyunkwan University, Suwon, 440-746, Korea
    Hye Ri Kim & Byung Hee Hong
  3. School of Mechanical Engineering, Sungkyunkwan University, Suwon, 440-746, Korea
    Hyeongkeun Kim & Young-Jin Kim
  4. School of Advanced Materials Science and Engineering, Sungkyunkwan University, Suwon, 440-746, Korea
    Jong-Hyun Ahn
  5. NanoCore & Department of Physics, National University of Singapore, Singapore, 117576 & 117542
    Xiangfan Xu, Yi Zheng, Jayakumar Balakrishnan & Barbaros Özyilmaz
  6. Digital & IT Solution Division, Samsung Techwin, Seongnam, 462-807, Korea
    Young Il Song
  7. Department of Chemistry, Center for Superfunctional Materials, Pohang University of Science and Technology, Hyojadong, Namgu, Pohang, 790-784, Korea
    Jae-Sung Park & Kwang S. Kim
  8. Nanotube Research Center, National Institute of Advanced Industrial Science and Technology (AIST), Tsukuba 305-8565 & Faculty of Science and Engineering, Meijo University, Nagoya, 468-8502, Japan
    Sumio Iijima

Authors

  1. Sukang Bae
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  2. Hyeongkeun Kim
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  3. Youngbin Lee
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  4. Xiangfan Xu
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  5. Jae-Sung Park
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  6. Yi Zheng
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  7. Jayakumar Balakrishnan
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  8. Tian Lei
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  9. Hye Ri Kim
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  10. Young Il Song
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  11. Young-Jin Kim
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  12. Kwang S. Kim
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  13. Barbaros Özyilmaz
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  14. Jong-Hyun Ahn
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  15. Byung Hee Hong
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  16. Sumio Iijima
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Contributions

B.H.H. planned and supervised the project, with assistance in supervision from J.H.A. Y.-J.K., B.O., K.S.K. and S.I. provided advice for the project. B.H.H., S.B. and H.K. conceived and carried out the experiment. B.H.H., J.H.A. and B.O. analysed the data and wrote the manuscript. X.X., J.B., Y.Z. and B.O. fabricated the QHE devices, and carried out the measurements. Y.L. and Y.I.S. helped with the fabrication of touch-screen panels and electromechanical analysis. J.S.P., H.R.K. and T.L. helped with the doping experiment.

Corresponding authors

Correspondence toJong-Hyun Ahn or Byung Hee Hong.

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The authors declare no competing financial interests.

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Bae, S., Kim, H., Lee, Y. et al. Roll-to-roll production of 30-inch graphene films for transparent electrodes.Nature Nanotech 5, 574–578 (2010). https://doi.org/10.1038/nnano.2010.132

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