Abstract
Epitaxial graphene of uniform thickness prepared on SiC is of great interest for various applications. On the Si-face, large area uniformity has been achieved, and there is a general consensus about the graphene properties. A similar uniformity has yet not been demonstrated on the C-face where the graphene has been claimed to be fundamentally different. A rotational disorder between adjacent graphene layers has been reported and suggested to explain why multilayer C-face graphene show the π-band characteristic of monolayer graphene. Utilizing low energy electron microscopy, x-ray photoelectron electron microscopy, low energy electron diffraction, and photoelectron spectroscopy, we investigated the properties of C-face graphene prepared by sublimation growth. We observe the formation of micrometer-sized crystallographic grains of multilayer graphene and no rotational disorder between adjacent layers within a grain. Adjacent grains are in general found to have different azimuthal orientations. Effects on C-face graphene by hydrogen treatment and Na exposure were also investigated and are reported. Why multilayer C-face graphene exhibits single layer electronic properties is still a puzzle, however.
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W. Lu, P. Soukiassian, and J. Boeckl: Graphene, fundamentals and functionalities. MRS Bull. 37(12), 1119–1321 (2012).
P.N. First, W.A. de Heer, T. Seyller, C. Berger, J.A. Stroscio, and J.S. Moon: Epitaxial graphenes on silicon carbide. MRS Bull. 35(4), 296 (2010).
M. Ruan, Y. Hu, Z. Guo, R. Dong, J. Palmer, J. Hankins, C. Berer, and W.A. de Heer: Epitaxial graphene on silicon carbide: Introduction to structured graphene. MRS Bull. 37(12), 1138 (2012).
L.O. Nyakiti, V.D. Wheeler, N.Y. Garces, R.L. Myers-Ward, C.R. Eddy Jr., and D.K. Gaskill: Enabling graphene-based technologies: Toward wafer-scale production of epitaxial graphene. MRS Bull. 37(12), 1149 (2012).
C. Virojanadara, M. Syväjarvi, R. Yakimova, L.I. Johansson, A.A. Zakharov, and T. Balasubramanian: Homogeneous large-area graphene layer growth on 6H-SiC(0001). Phys. Rev. B 78, 245403 (2008).
K.V. Emtsev, A. Bostwick, K. Horn, J. Jobst, G.L. Kellogg, L. Ley, J.L. McChesney, T. Ohta, S.A. Reshanov, J. Röhrl, E. Rotenberg, A.K. Schmid, D. Waldmann, H.B. Weber, and T. Seyller: Towards wafer-size graphene layers by atmospheric pressure graphitization of silicon carbide. Nat. Mater. 8, 203 (2009).
C. Virojanadara, R. Yakimova, J.R. Osiecki, M. Syväjärvi, R.I.G. Uhrberg, L.I. Johansson, and A.A. Zakharov: Substrate orientation: A way towards higher quality monolayer graphene growth on 6H-SiC(0001). Surf. Sci. 603, L87 (2009).
U. Starke, S. Forti, K.V. Emtsev, and C. Coletti: Engineering the electronic structure of epitaxial graphene by transfer doping and atomic intercalation. MRS Bull. 37(12), 1177 (2012).
Luxmi, N. Srivastava, G. He, R.M. Feenstra, and P.J. Fisher: Comparison of graphene formation on C-face and Si-face SiC{0001} surfaces. Phys. Rev. B 82, 235406 (2010).
C. Mathieu, N. Barrett, J. Rault, Y.Y. Mi, B. Zhang, W.A. de Heer, C. Berger, E.H. Conrad, and O. Renault: Microscopic correlation between chemical and electronic states in epitaxial graphene on SiC(000-1). Phys. Rev. B 83, 235436 (2011).
L.I. Johansson, S. Watcharinyanon, A.A. Zakharov, T. Iakimov, R. Yakimova, and C. Virojanadara: The stacking of adjacent graphene layers grown on C-face SiC. Phys. Rev. B. 84, 125405 (2011).
N. Srivastava, G. He, Luxmi, P.C. Mende, R.M. Feenstra, and Y. Sun: Graphene formed on SiC under various environments: Comparison of Si-face and C-face. J. Phys. D: Appl. Phys. 45, 154001 (2012).
J. Hicks, K. Shepperd, F. Wang, and E.H. Conrad: The structure of graphene grown on the SiC(000-1) surface. J. Phys. D: Appl. Phys. 45, 154002 (2012).
L.I. Johansson, C. Xia, J. Ul Hassan, T. Iakimov, A.A. Zakharov, S. Watchari-nyanon, R. Yakimova, E. Janzen, and C. Virojanadara: Is the registry between adjacent graphene layers grown on C-face SiC different compared to that on Si-face SiC. Crystals 3, 1 (2013).
I. Forbeaux, J-M. Themlin, A. Charrier, F. Thibaudau, and J-M. Debever: Solid state graphitization mechanisms of silicon carbide 6H-SiC polar faces. Appl. Surf. Sci. 162–163, 406 (2000).
J. Hass, R. Feng, J.E. Millan-Otoya, X. Li, M. Sprinkle, P.N. First, W.A. de Heer, E.H. Conrad, and C. Berger: Structural properties of the multilayer graphene/4H-SiC(000-1) system as determined by surface x-ray diffraction. Phys. Rev. B 75, 214109 (2007).
J. Hass, F. Varchon, J.E. Millan-Otoya, M. Sprinkle, N. Sharma, W.A. de Heer, C. Berger, P.N. First, L. Magaud, and E.H. Conrad: Why multilayer graphene on 4H-SiC(000-1) behaves like a single sheet of graphene. Phys. Rev. Lett. 100, 125504 (2008).
J. Hass, W.A. de Heer, and J. Conrad: The growth and morphology of epitaxial multilayer graphene. J. Phys. Condens. Matter 20, 323202 (2008).
K.V. Emtsev, F. Speck, T. Seyller, L. Ley, and J.D. Riley: Interaction, growth, and ordering of epitaxial graphene on SiC{0001} surfaces: A comparative photoelectron spectroscopy study. Phys. Rev. B 77, 155303 (2008).
M. Sprinkle, D. Siegel, Y. Hu, J. Hicks, A. Tejeda, A. Taleb-Ibrahimi, P. Le Fèvre, F. Bertran, S. Vizzini, H. Enriquez, S. Chiang, P. Soukiassian, C. Berger, W.A. de Heer, A. Lanzara, and E.H. Conrad: First direct observation of a nearly ideal graphene band structure. Phys. Rev. Lett. 103, 226803 (2009).
D.L. Miller, K.D. Kubista, G.M. Rutter, M. Ruan, W.A. de Heer, P.N. First, and J.A. Stroscio: Structural analysis of multilayer graphene via atomic moire interferometry. Phys. Rev. B 81, 125427 (2010).
T. Ohta, A. Bostwick, J.L. McChesney, T. Seyller, K. Horn, and E. Rotenberg: Interlayer interaction and electronic screening in multilayer graphene investigated with angle-resolved photoemission spectroscopy. Phys. Rev. Lett. 98, 206802 (2007).
C. Riedl, C. Coletti, T. Iwasaki, A.A. Zakharov, and U. Starke: Quasi-free standing epitaxial graphene on SiC obtained by hydrogen intercalation. Phys. Rev. Lett. 103, 246804 (2009).
C. Virojanadara, A.A. Zakharov, R. Yakimova, and L.I. Johansson: Buffer layer free large area bi-layer graphene on SiC(0001). Surf. Sci. 604, L4 (2010).
S. Watcharinyanon, C. Virojanadara, J.R. Osiecki, A.A. Zakharov, R. Yakimova, R.I.G. Uhrberg, and L.I. Johansson: Hydrogen intercalation of graphene grown on 6H-SiC(0001). Surf. Sci. 605, 1662 (2011).
S. Watcharinyanon, L.I. Johansson, C. Xia, and C. Virojanadara: Changes in structural and electronic properties of graphene grown on 6H-SiC(0001) by Na. J. Appl. Phys. 111, 083711 (2012).
A. Sandin, T. Jayasekera, J.E. Rowe, K.W. Kim, M.B. Nardelli, and D.B. Dougherty: Multiple coexisting intercalation structures of sodium in epitaxial graphene-SiC interfaces. Phys. Rev. B 85, 125410 (2012).
C. Xia, S. Watcharinyanon, A.A. Zakharov, L.I. Johansson, R. Yakimova, and C. Virojanadara: Detailed studies of Na intercalation on furnace grown graphene on 6H-SiC(0001). Surf. Sci. 613, 88 (2013).
A. Bostwick, F. Speck, T. Seyller, K. Horn, M. Polini, R. Asgari, A.H. MacDonald, and E. Rotenberg: Observation of plasmarons in quasi-freestanding graphene. Science 328, 999 (2010).
C. Virojanadara, S. Watcharinyanon, A.A. Zakharov, and L.I. Johansson: Epitaxial graphene on 6H-SiC(0001) and Li intercalation. Phys. Rev. B 82, 205402 (2010).
C. Virojanadara, A.A. Zakharov, S. Watcharinyanon, R. Yakimova, and L.I. Johansson: A LEEM and XPEEM study of Li intercalated into graphene on SiC(0001). New J. Phys. 12, 125015 (2010).
A.L. Walter, A. Bostwick, K-J. Jeon, F. Speck, M. Ostler, T. Seyller, L. Moreschini, Y.J. Chang, M. Polini, R. Asgari, A.H. MacDonald, K. Horn, and E. Rotenberg: Effective screening and plasmaron bands in graphene. Phys. Rev. B 84, 085410 (2011).
S. Watcharinyanon, C. Virojanadara, and L.I. Johansson: Rb and Cs deposition on epitaxial graphene grown on 6H-SiC(0001). Surf. Sci. 605, 1918 (2011).
D.A. Siegel, C.G. Hwang, A.W. Fedorov, and A. Lanzara: Quasifreestanding multilayer graphene films on the carbon face of SiC. Phys. Rev. B 81, 241417 (2010).
L.I. Johansson, C. Xia, and C. Virojanadara: Na induced changes in the electronic band structure of graphene grown on C-face SiC. Graphene 2, 1 (2013).
A.A. Zakharov, C. Virojanadara, S. Watcharinyanon, R. Yakimova, and L.I. Johansson: Nano-scale 3D(E, kx, ky) band structure imaging on graphene and intercalated graphene. IBM J. Res. Dev. 55(4), 6 (2011).
H. Hibino, K. Kagashima, F. Maeda, M. Nagase, Y. Kobayashi, and H. Yamaguchi: 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).
L.I. Johansson, F. Owman, and P. Mårtensson: High-resolution core level study of 6H-SiC(0001). Phys. Rev. B 53, 13793 (1996).
S. Latil, V. Meunier, and L. Henrard: Massless fermions in multilayer graphitic systems with misoriented layers: Ab initio calculations and experimental fingerprints. Phys. Rev. B 76, 201402 (2007).
S. Latil and L. Henrard: Charge carriers in few-layer graphene films. Phys. Rev. Lett. 97, 036803 (2006).
T. Ohta, T.E. Beechem, J.T. Robinson, and G.L. Kellogg: Long-range atomic ordering and variable interlayer interactions in two overlapping graphene lattices with stacking misorientations. Phys. Rev. B 85, 075415 (2012).
J. Ul Hassan, C. Virojanadara, A. Meyer, I.G. Ivanov, J.I. Flege, S. Watcharinyanon, J. Falta, L.I. Johansson, and E. Janzén: Control of epitaxial graphene thickness on 4H-SiC(0001) and buffer layer removal through hydrogen intercalation. Mater. Sci. Forum 717–720, 605 (2012).
M. Mucha-Kruczyński, O. Tsyplyatyev, A. Grishin, E. McCann, V.I. Fal’ko, A. Bostwick, and E. Rotenberg: Characterization of graphene through anisotropy of constant-energy maps in angle-resolved photoemission. Phys. Rev. B 77, 195403 (2008).
I. Gierz, J. Henk, H. Hàchst, C.R. Ast, and K. Kern: Illuminating the dark corridor in graphene: Polarization dependence of angle-resolved photoemission spectroscopy on graphene. Phys. Rev. B 83, 121408 (2011).
J. Avila, I. Razado, S. Lorcy, B. Lagarde, J-L. Giorgetta, F. Polack, and M.C. Asensio: ANTARES, a scanning photoemission microscopy beamline at SOLEIL. J. Phys. Conf. Ser. 425, 192023 (2013).
O. Pankratov, S. Hensel, P. Gàtzfried, and M. Bockstedte: Graphene on cubic and hexagonal SiC: A comparative theoretical study. Phys. Rev. B 86, 155432 (2012).
ACKNOWLEDGMENTS
The authors gratefully acknowledge support from the European Science Foundation, within the EuroGRAPHENE (EPIGRAT) program and the Swedish Research Council (Grant No. 621-2011-4252 and Linnaeus Grant).
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Johansson, L.I., Virojanadara, C. Properties of epitaxial graphene grown on C-face SiC compared to Si-face. Journal of Materials Research 29, 426–438 (2014). https://doi.org/10.1557/jmr.2013.261
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DOI: https://doi.org/10.1557/jmr.2013.261