Abstract
Graphene, a single monolayer of graphite, has recently attracted considerable interest owing to its novel magneto-transport properties1,2,3, high carrier mobility and ballistic transport up to room temperature4. It has the potential for technological applications as a successor of silicon in the post Moore’s law era5,6,7, as a single-molecule gas sensor8, in spintronics9,10,11, in quantum computing12 or as a terahertz oscillator13. For such applications, uniform ordered growth of graphene on an insulating substrate is necessary. The growth of graphene on insulating silicon carbide (SiC) surfaces by high-temperature annealing in vacuum was previously proposed to open a route for large-scale production of graphene-based devices5,6. However, vacuum decomposition of SiC yields graphene layers with small grains (30–200 nm; refs 14–16). Here, we show that the ex situ graphitization of Si-terminated SiC(0001) in an argon atmosphere of about 1 bar produces monolayer graphene films with much larger domain sizes than previously attainable. Raman spectroscopy and Hall measurements confirm the improved quality of the films thus obtained. High electronic mobilities were found, which reach μ=2,000 cm 2 V−1 s−1 at T=27 K. The new growth process introduced here establishes a method for the synthesis of graphene films on a technologically viable basis.
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References
Novoselov, K. S. et al. Two-dimensional gas of massless Dirac fermions in graphene. Nature 438, 197–200 (2005).
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, 201–2004 (2005).
Novoselov, K. S. et al. Unconventional quantum Hall effect and Berry’s phase of 2π in bilayer graphene. Nature Phys. 2, 177–180 (2006).
Novoselov, K. S. et al. Room-temperature quantum Hall effect in graphene. Science 315, 1379 (2007).
Berger, C. et al. Ultrathin epitaxial graphite: 2D electron gas properties and a route toward graphene-based nanoelectronics. J. Phys. Chem. B 108, 19912–19916 (2004).
Berger, C. et al. Electronic confinement and coherence in patterned epitaxial graphene. Science 312, 1191–1196 (2006).
Geim, A. K. & Novoselov, K. S. The rise of graphene. Nature Mater. 6, 183–191 (2007).
Schedin, F. et al. Detection of individual gas molecules adsorbed on graphene. Nature Mater. 6, 652–655 (2007).
Son, Y.-W., Cohen, M. L. & Louie, S. G. Half-metallic graphene nanoribbons. Nature 444, 347–349 (2006).
Trauzettel, B., Bulaev, D. V., Loss, D. & Burkard, G. Spin qubits in graphene quantum dots. Nature Phys. 3, 192–196 (2007).
Yokoyama, T. Controllable spin transport in ferromagnetic graphene junctions. Phys. Rev. B 77, 073413 (2008).
Fal’ko, V. I. Graphene: Quantum information on chicken wire. Nature Phys. 3, 151–152 (2007).
Rana, F. Graphene terahertz plasmon oscillators. IEEE Trans. Nanotech. 7, 91–99 (2008).
Hass, J. et al. Highly ordered graphene for two dimensional electronics. Appl. Phys. Lett. 89, 143106 (2006).
Hibino, H. et al. Microscopic thickness determination of thin graphite films formed on SiC from quantized oscillation in reflectivity of low-energy electrons. Phys. Rev. B 77, 075413 (2008).
Ohta, T. et al. Morphology of graphene thin film growth on SiC(0001). New J. Phys. 10, 023034 (2008).
Novoselov, K. S. et al. Two-dimensional atomic crystals. Proc. Natl Acad. Sci. USA 102, 10451–10453 (2005).
Sutter, P. W., Flege, J.-I. & Sutter, E. A. Epitaxial graphene on ruthenium. Nature Mater. 7, 406–411 (2008).
Hernandez, Y. et al. High-yield production of graphene by liquid-phase exfoliation of graphite. Nature Nanotech. 3, 563–568 (2008).
Gomez-Navarro, C. et al. Electronic transport properties of individual chemically reduced graphene oxide sheets. Nano Lett. 7, 3499–3503 (2007).
McCann, E. & Fal’ko, V. I. Landau-level degeneracy and quantum Hall effect in a graphite bilayer. Phys. Rev. Lett. 96, 086805 (2006).
Ohta, T. et al. Controlling the electronic structure of bilayer graphene. Science 313, 951–954 (2006).
Emtsev, K. V. et al. Interaction, growth, and ordering of epitaxial graphene on SiC{0001} surfaces: A comparative photoelectron spectroscopy study. Phys. Rev. B 77, 155303 (2008).
Bostwick, A. et al. Quasiparticle dynamics in graphene. Nature Phys. 3, 36–40 (2007).
Ferrari, A. C. et al. Raman spectrum of graphene and graphene layers. Phys. Rev. Lett. 97, 187401 (2006).
Röhrl, J. et al. Raman spectra of epitaxial graphene on SiC(0001). Appl. Phys. Lett. 92, 201918 (2008).
Langmuir, I. Convection and conduction of heat in gases. Phys. Rev. (Series I) 34, 401–422 (1912).
Fonda, G. R. Evaporation of tungsten under various pressures of argon. Phys. Rev. (Series II) 31, 260–266 (1928).
Kedzierski, J. et al. Epitaxial graphene transistors on SiC substrates. IEEE Trans. Electron Devices 55, 2078–2085 (2008).
Seyller, Th. et al. Structural and electronic properties of graphite layers grown on SiC(0001). Surf. Sci. 600, 3906–3911 (2006).
Acknowledgements
We thank F. El Gabaly for assistance with the LEEM measurements and M. Gick for help with the sample preparation. We gratefully acknowledge support by the DFG under contract SE 1087/5-1, contract WE 4542-5-1, and within the Cluster of Excellence ‘Engineering of Advanced Materials’ (www.eam.uni-erlangen.de) at the Friedrich-Alexander-Universität Erlangen-Nürnberg, by BaCaTeC, and by the BMBF under contract 05 ES3XBA/5. A part of the work was carried out at Sandia National Laboratories, a multiprogram laboratory operated by Sandia Corporation, a Lockheed Martin company, for the United States Department of Energy, Office of Basic Energy Sciences, Division of Materials Science and Engineering, under Contract No. DE-AC04-94AL85000. The work carried out at the Advanced Light Source was supported by the Director, Office of Science, Office of Basic Energy Sciences, of the US Department of Energy under Contract No. DE-AC03-76SF00098.
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K.V.E. developed the growth process of large-area graphene with the help of S.A.R. AFM measurements were done by K.V.E. and T.O. T.O. and A.S. carried out the LEEM measurements with the help of G.K. Photoelectron spectroscopy measurements were carried out by K.V.E., T.S., A.B., J.L.M., E.R. and K.H. J.J., D.W. and H.B.W carried out lithography and electrical measurements. J.R. carried out Raman measurements. T.S., K.V.E. and L.L. wrote the manuscript with revision and input from all other co-authors.
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Emtsev, K., Bostwick, A., Horn, K. et al. Towards wafer-size graphene layers by atmospheric pressure graphitization of silicon carbide. Nature Mater 8, 203–207 (2009). https://doi.org/10.1038/nmat2382
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DOI: https://doi.org/10.1038/nmat2382
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