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Synthesis of monolithic graphene–graphite integrated electronics

Abstract

Encoding electronic functionality into nanoscale elements during chemical synthesis has been extensively explored over the past decade as the key to developing integrated nanosystems1 with functions defined by synthesis2,3,4,5,6. Graphene7,8,9,10,11,12 has been recently explored as a two-dimensional nanoscale material, and has demonstrated simple device functions based on conventional top-down fabrication13,14,15,16,17,18,19,20. However, the synthetic approach to encoding electronic functionality and thus enabling an entire integrated graphene electronics in a chemical synthesis had not previously been demonstrated. Here we report an unconventional approach for the synthesis of monolithically integrated electronic devices based on graphene and graphite. Spatial patterning of heterogeneous metal catalysts permits the selective growth of graphene and graphite, with a controlled number of graphene layers. Graphene transistor arrays with graphitic electrodes and interconnects were formed from the synthesis. These functional, all-carbon structures were transferable onto a variety of substrates. The integrated transistor arrays were used to demonstrate real-time, multiplexed chemical sensing and more significantly, multiple carbon layers of the graphene–graphite device components were vertically assembled to form a three-dimensional flexible structure which served as a top-gate transistor array. These results represent substantial progress towards encoding electronic functionality through chemical synthesis and suggest the future promise of one-step integration of graphene–graphite based electronics.

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Figure 1: Synthesis of monolithic graphene–graphite structures using heterogeneously patterned metal catalyst films.
Figure 2: Synthesis and electrical characteristics of monolithic graphene–graphite back-gate FETs.
Figure 3: Real-time, multiplexed pH sensing using monolithic graphene field-effect sensor arrays with graphite electrodes.
Figure 4: Flexible and semitransparent top-gate monolithic graphene–graphite FET arrays.

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References

  1. Lu, W. & Lieber, C. M. Nanoelectronics from the bottom up. Nature Mater. 6, 841–850 (2007).

    Article  CAS  Google Scholar 

  2. Dai, H. Carbon nanotubes: Synthesis, integration, and properties. Acc. Chem. Res. 35, 1035–1044 (2002).

    Article  CAS  Google Scholar 

  3. Yang, C., Zhong, Z. & Lieber, C. M. Encoding electronic properties by synthesis of axial modulation-doped silicon nanowires. Science 310, 1304–1307 (2005).

    Article  CAS  Google Scholar 

  4. Lauhon, L. J., Gudiksen, M. S., Wang, D. & Lieber, C. M. Epitaxial core–shell and core–multishell nanowire heterostructures. Nature 420, 57–61 (2002).

    Article  CAS  Google Scholar 

  5. Kocabas, C., Shim, M. & Rogers, J. A. Spatially selective guided growth of high-coverage arrays and random networks of single-walled carbon nanotubes and their integration into electronic devices. J. Am. Chem. Soc. 128, 4540–4541 (2006).

    Article  CAS  Google Scholar 

  6. Zhou, W., Ding, L., Yang, S. & Liu, J. Orthogonal orientation control of carbon nanotube growth. J. Am. Chem. Soc. 132, 336–341 (2010).

    Article  CAS  Google Scholar 

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

    Article  CAS  Google Scholar 

  8. Zhang, Y., Tan, Y., 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 

  9. Novoselov, K. S. et al. Electric field effect in atomically thin carbon films. Science 306, 666–669 (2004).

    Article  CAS  Google Scholar 

  10. 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 

  11. Seol, J. H. et al. Two-dimensional phonon transport in supported graphene. Science 328, 213–216 (2010).

    Article  CAS  Google Scholar 

  12. Nair, R. R. et al. Fine structure constant defines visual transparency of graphene. Science 320, 1308–1308 (2008).

    Article  CAS  Google Scholar 

  13. Levendorf, M. P., Ruiz-Vargas, C. S., Garg, S. & Park, J. Transfer-free batch fabrication of single layer graphene transistors. Nano Lett. 9, 4479–4483 (2009).

    Article  CAS  Google Scholar 

  14. 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 

  15. Jobst, J., Waldmann, D., Emtsev, K. V., Seyller, Th. & Weber, H. B. Transport properties of single-layer epitaxial graphene on 6H-SiC (0001). Mater. Sci. Forum 645–648, 637–641 (2010).

    Article  Google Scholar 

  16. Mattevi, C., Kim, H. & Chhowalla, M. A review of chemical vapour deposition of graphene on copper. J. Mater. Chem. 21, 3324–3334 (2010).

    Article  Google Scholar 

  17. 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 

  18. 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 

  19. Jauregui, L. A., Cao, H., Wu, W., Yu, Q. & Chen, Y. P. Electronic properties of grains and grain boundaries in graphene grown by chemical vapor deposition. Solid State Commun. 151, 1100–1104 (2011).

    Article  CAS  Google Scholar 

  20. Han, M. Y., Ozyilmaz, B., Zhang, Y. & Kim, P. Energy band-gap engineering of graphene nanoribbons. Phys. Rev. Lett. 98, 206805 (2007).

    Article  Google Scholar 

  21. Li, X., Cai, W., Colombo, L. & Ruoff, R. S. Evolution of graphene growth on Ni and Cu by carbon isotope labeling. Nano Lett. 9, 4268–4272 (2009).

    Article  CAS  Google Scholar 

  22. Blake, P. et al. Making graphene visible. Appl. Phys. Lett. 91, 063124 (2007).

    Article  Google Scholar 

  23. 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 

  24. Bae, S. et al. Roll-to-roll production of 30 inch graphene films for transparent electrodes. Nature Nanotech. 5, 574–578 (2010).

    Article  CAS  Google Scholar 

  25. Bhaviripudi, S., Jia, X., Dresselhaus, M. S. & Kong, J. Role of kinetic factors in chemical vapor deposition synthesis of uniform large area graphene using copper catalyst. Nano Lett. 10, 4128–4133 (2010).

    Article  CAS  Google Scholar 

  26. Zhang, Y., Small, J. P., Pontius, W. V. & Kim, P. Fabrication and electric-field-dependent transport measurements of mesoscopic graphite devices. Appl. Phys. Lett. 86, 073104 (2005).

    Article  Google Scholar 

  27. Yazyev, O. V. & Louie, S. G. Electronic transport in polycrystalline graphene. Nature Mater. 9, 806–809 (2010).

    Article  CAS  Google Scholar 

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

    Article  CAS  Google Scholar 

  29. Ohno, Y., Maehashi, K., Yamashiro, Y. & Matsumoto, K. Electrolyte-gated graphene field-effect transistors for detecting pH and protein adsorption. Nano Lett. 9, 3318–3322 (2009).

    Article  CAS  Google Scholar 

  30. Cohen-Karni, T., Qing, Q., Li, Q., Fang, Y. & Lieber, C. M. Graphene and nanowire transistors for cellular interfaces and electrical recording. Nano Lett. 10, 1098–1102 (2010).

    Article  CAS  Google Scholar 

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Acknowledgements

We thank L. Wang for assistance on electrical measurements, Y. K. Kim for TEM characterization, and J. Cahoon and Q. Qing for helpful discussions. J-U.P. thanks UNIST for support through the 2010 Research Fund, and S.N. thanks the Samsung Scholarship. This research was supported by a research project of National Research Foundation of Korea (Grant number: 20110014111), and by a NIH Director’s Pioneer Award (5DP1OD003900).

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J-U.P., S.N. and C.M.L. designed the experiments. J-U.P., S. N. and M-S. L. performed the experiments. J-U.P., S.N. and C.M.L. analysed the data and wrote the paper.

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Correspondence to Jang-Ung Park or SungWoo Nam.

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The authors declare no competing financial interests.

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Park, JU., Nam, S., Lee, MS. et al. Synthesis of monolithic graphene–graphite integrated electronics. Nature Mater 11, 120–125 (2012). https://doi.org/10.1038/nmat3169

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