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High-resolution x-ray analysis of graphene grown on 4H–SiC (000 $\bar 1$ ) at low pressures

  • Michael A. Capano (a1), Benjamin M. Capano (a2), Dallas T. Morisette (a3), Alberto Salleo (a4), Sangwon Lee (a4) and Michael F. Toney (a5)...
Abstract
Abstract

This article explores the growth of graphene under low-pressure Ar conditions. Carbon- and silicon-face 4H–SiC samples are subjected to epitaxial graphene growth at 1600 °C in vacuum, in 1 mbar argon, or in 10 mbar of argon. High-resolution x-ray scattering is used to characterize all graphene films. On the C-face, specular scans reveal a bimodal distribution of thicknesses that decrease with increasing Ar pressure. Thin and thick regions are approximately 15 and 46 monolayers in C-face graphene grown at high vacuum, 14 and 42 monolayers thick in graphene grown at 1 mbar, and 12 and 32 monolayers thick in graphene grown at 10 mbar. Azimuthal scans confirm in all cases that graphene layers are epitaxial and display expected crystallographic relationships with the underlying SiC substrate. In-plane azimuthal scans show the rotational disorder increases as pressure increases. Peaks in radial scans are asymmetric, suggesting the grain structure has a bimodal distribution of large and small domains. The sample displaying the lowest average Hall mobility (grown at 1 mbar) has the largest population of small crystallites (coherence length on the order of ∼30 nm). Variations in structure and mobility of C-face graphene are attributed to inadequate control of Si sublimation during growth.

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a) Address all correspondence to this author. e-mail: capano@purdue.edu
References
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1. Van Bommel A.J., Crombeen J.E., and Van Tooren A.: LEED and Auger electron observations of the SiC(0001) surface. Surf. Sci. 48, 463 (1975).
2. Muehlhoff L., Choyke W.J., Bozack M.J., and Yates J.T.: Comparative electron spectroscopic studies of surface segregation on SiC(0001) and SiC(0001). J. Appl. Phys. 60, 2842 (1986).
3. Forbeaux I., Themlin J-M., and Debever J-M.: High-temperature graphitization of the 6H-SiC (000 $\bar 1$ ) face. Surf. Sci. 442, 9 (1999).
4. Tromp R.M. and Hannon J.B.: Thermodynamics and kinetics of graphene growth on SiC (0001). Phys. Rev. Lett. 102, 106104 (2009).
5. Novoselov K.S., Geim A.K., Morozov S.V., Jiang D., Zhang Y., Dubonos S.V., Grigorieva I.V., and Firsov A.A.: Electric field effect in atomically thin carbon films. Science 306, 666 (2004).
6. Berger C., Song Z.M., Li T.B., Li X.B., Ogbazghi A.Y., Feng R., Dai Z.T., Marchenkov A.N., Conrad E.H., First P.N., and de Heer W.A.: Ultrathin epitaxial graphite: 2D electron gas properties and a route toward graphene-based nanoelectronics. J. Phys. Chem. B 108, 1991219916 (2004).
7. Drowart J., De Maria G., and Inghram G.: Thermodynamic study of SiC utilizing a mass spectrometer. J. Chem. Phys. 29, 10151021 (1958).
8. Davis S.G., Anthrop D.F., and Searcy A.W.: Vapor pressure of silicon and the dissociation pressure of silicon carbide. J. Chem. Phys. 34, 659 (1961).
9. Berger C., Song Z.M., Li X.B., Wu X., Brown N., Naud C., Mayou D., Li T., Hass J., Marchenkov A.N., Conrad E.H., First P.N., and de Heer W.A.: Electronic confinement and coherence in patterned epitaxial grapheme. Science 312, 11911196 (2006).
10. Sadowski M.L., Martinez G., Potemski M., Berger C., and de Heer W.A.: Landau level spectroscopy of ultrathin graphite layers. Phys. Rev. Lett. 97, 266405 (2006).
11. Shen T., Gu J.J., Xu M., Wu Y.Q., Bolen M.L., Capano M.A., Engel L.W., and Ye P.D.: Observation of quantum-Hall effect in gated epitaxial graphene grown on SiC (0001). Appl. Phys. Lett. 95, 172105 (2009).
12. Wu X., Hu Y., Ruan M., Madiomanana N.K., Hankinson J., Sprinkle M., Berger C., and de Heer W.A.: Half integer quantum Hall effect in high mobility single layer epitaxial grapheme. Appl. Phys. Lett. 95, 223108 (2009).
13. Shen T., Neal A.T., Bolen M.L., Gu J.J., Engel L.W., Capano M.A., and Ye P.D.: Quantum-Hall plateau-plateau transition in top-gated epitaxial graphene grown on SiC (0001). J. Appl. Phys. 111, 013716 (2012).
14. Forbeaux I., Themlin J.M., and Debever J.M.: Heteroepitaxial graphite on 6H-SiC (0001): Interface formation through conduction-band electronic structure. Phys. Rev. B 58, 1639616406 (1998).
15. Hannon J.B. and Tromp R.M.: Pit formation during graphene synthesis on SiC (0001): In-situ electron microscopy. Phys. Rev. B 77, 241404 (2008).
16. Emtsev K.V., Speck F., Seyller T., Riley J.D., and Ley L.: Interaction, growth, and ordering of epitaxial graphene on SiC {0001} surfaces: A comparative photoelectron spectroscopy study. Phys. Rev. B 77, 155303 (2008).
17. de Heer W.A., Berger C., Ruan M., Sprinkle M., Li X., Hu Y., Zhang B., Hankinson J., and Conrad E.: Large area and structured epitaxial graphene produced by confinement controlled sublimation of silicon carbide. Proc. Natl. Acad. Sci. U.S.A. 108, 1690016905 (2011).
18. Wu Y.Q., Ye P.D., Capano M.A., Xuan Y., Sui Y., Qi M., Cooper J.A., Shen T., Pandey D., Prakash G., and Reifenberger R.: Top-gated graphene field-effect-transistors formed by decomposition of SiC. Appl. Phys. Lett. 92, 092102 (2008).
19. Emtsev K.V., Bostwick A., Horn K., Jobst J., Kellogg G.L., Ley L., McChesney J.L., Ohta T., Reshanov S.A., Rohrl J., Rotenberg E., Schmid A.K., Waldmann D., Weber H.B., and Seyller T.: Towards wafer-size graphene layers by atmospheric pressure graphitization of silicon carbide. Nat. Mater. 8, 203 (2009).
20. Bolen M.L., Shen T., Gu J., Colby R., Stach E., Ye P.D., and Capano M.A.: Empirical study of Hall bars on few-layer graphene on c-face 4H-SiC. J. Electron. Mater. 39, 2696 (2010).
21. Tedesco J.L., VanMil B., Myers-Ward R.L., Culbertson J., Jernigan G., Campbell P., McCrate J.M., Kitt S.A., Eddy C. Jr., and Gaskill D.K.: Improvement of Morphology and Free Carrier Mobility through Argon-Assisted Growth of Epitaxial Graphene on Silicon Carbide. ECS Trans. 19, 137 (2009).
22. Bolen M.L., Harrison S.E., Biedermann L.B., and Capano M.A.: Graphene formation mechanisms on 4H-SiC(0001). Phys. Rev. B 80, 115433 (2009).
23. Lee S., Toney M.F., Ko W., Randel J.C., Jung H.J., Munakata K., Lu J., Geballe T.H., Beasley M.R., Sinclair R., Manoharan H.C., and Salleo A.: Laser-synthesized epitaxial graphene. ACS Nano 4, 75247530 (2010).
24. Sutter P.: Epitaxial graphene: How silicon leaves the scene. Nat. Mater. 8, 171172 (2009).
25. Virojanadara C., Syväjarvi M., Yakimova R., Johansson L.I., Zakharov A.A., and Balasubramanian T.: Homogeneous large-area graphene layer growth on 6H-SiC(0001). Phys. Rev. B 78, 245403 (2008).
26. Hass J., Feng R., Li T., Li X., Zong Z., de Heer W.A., First P.N., Conrad E.H., Jeffrey C.A., and Berger C.: Highly ordered graphene for two dimensional electronics. Appl. Phys. Lett. 89, 143106 (2006).
27. de Heer W.A., Berger C., Wu X., First P.N., Conrad E.H., Li X., Li T., Sprinkle M., Hass J., Sadowski M.L., Potemski M., and Martinez G.: Epitaxial graphene. Solid State Commun. 143, 92100 (2007).
28. Jernigan G.G., VanMil B.L., Tedesco J.L., Tischler J.G., Glaser E.R., Davidson A. III, Campbell P.M., and Gaskill D.K.: Comparison of epitaxial graphene on Si-face and C-face 4H SiC formed by ultrahigh vacuum and RF furnace production. Nano Lett. 9, 26052609 (2009).
29. Tedesco J.L., VanMil B.L., Myers-Ward R.L., McCrate J.M., Kitt S.A., Campbell P.M., Jernigan G.G., Culbertson J.C., Eddy C.R., and Gaskill D.K.: Hall effect mobility of epitaxial graphene grown on silicon carbide. Appl. Phys. Lett. 95, 122102 (2009).
30. Hass J., Feng R., Millán-Otoya J.E., Li X., Sprinkle M., First P.N., de Heer W.A., Conrad E.H., and Berger C.: Structural properties of the multilayer graphene/4H-SiC(000 $\bar 1$ ) system as determined by surface x-ray diffraction. Phys. Rev. B 75, 214109 (2007).
31. Hass J., Varchon F., Millán-Otoya J.E., Sprinkle M., Sharma N., de Heer W.A., Berger C., First P.N., Magaud L., and Conrad E.H.: Why multilayer graphene on 4H-SiC(000 $\bar 1$ ) behaves like a single sheet of graphene. Phys. Rev. Lett. 100, 125504 (2008).
32. Luxmi N.S., Guowei H., Feenstra R.M., and Fisher P.J.: Comparison of graphene formation on C-face and Si-face SiC {0001} surfaces. Phys. Rev. B 82, 235406 (2010).
33. Sprinkle M., Hicks J., Tejeda A., Taleb-Ibrahimi A., Fèvre P.L., Bertran F., Tinkey H., Clark M.C., Soukiassian P., Martinotti D., Hass J., and Conrad E.H.: Multilayer epitaxial graphene grown on the SiC(000-1) surface; structure and electronic properties. J. Phys. D: Appl. Phys. 43, 374006 (2010).
34. Franklin R.: The structure of graphitic carbons. Acta Crystall. 4, 253261 (1951).
35. Baskin Y. and Meyer L.: Lattice constants of graphite at low temperatures. Phys. Rev. 100, 544545 (1955).
36. Wallace P.R.: The band theory of graphite. Phys. Rev. 71, 622634 (1947).
37. Röhrl J., Hundhausen M., Emtsev K.V., Seyller T., Graupner R., and Ley L.: Raman spectra of epitaxial graphene on SiC(0001). Appl. Phys. Lett. 92, 201918 (2008).
38. Ferralis N., Maboudian R., and Carraro C.: Evidence of structural strain in epitaxial graphene layers on 6H-SiC(0001). Phys. Rev. Lett. 101, 156801 (2008).
39. Robinson J.A., Wetherington M., Tedesco J.L., Campbell P.M., Weng X., Stitt J., Fanton M.A., Frantz E., Snyder D., VanMil B.L., Jernigan G.G., Myers-Ward R.L., Eddy C.R. Jr., and Gaskill D.K.: Correlating Raman spectral signatures with carrier mobility in epitaxial graphene: A guide to achieving high mobility on the wafer scale. Nano Lett. 9, 28732876 (2009).
40. Choi S-M., Jhi S-H., and Son Y-W.: Effects of strain on electronic properties of graphene. Phys. Rev. B 81, 081407 (2010).
41. Huang M., Yan H., Heinz T.F., and Hone J.: Probing strain-induced electronic structure change in graphene by Raman spectroscopy. Nano Lett. 10, 40744079 (2010).
42. Robinson J.A., Puls C.P., Staley N.E., Stitt J.P., and Fanton M.A.: Raman topography and strain uniformity of large-area epitaxial graphene. Nano Lett. 9, 964968 (2009).
43. Tedesco J.L., Jernigan G.G., Culbertson J.C., Hite J.K., Yang Y., Daniels K.M., Myers-Ward R.L., Eddy C.R., Robinson J.A., Trumbull K.A., Wetherington M.T., Campbell P.M., and Gaskill D.K.: Morphology characterization of argon-mediated epitaxial graphene on C-face SiC. Appl. Phys. Lett. 96, 222103 (2010).
44. Prakash G., Capano M.A., Bolen M.L., Zemlyanov D., and Reifenberger R.G.: AFM study of ridges in few-layer epitaxial graphene grown on the carbon-face of 4H–SiC. Carbon 48, 23832393 (2010).
45. Colby R., Bolen M.L., Capano M.A., and Stach E.A.: Amorphous interface layer in thin graphite films grown on the carbon face of SiC. Appl. Phys. Lett. 99, 101904 (2011).
46. Zhou S.Y., Gweon G.H., Fedorov A.V., First P.N., de Heer W.A., Lee D.H., Guinea F., Castro Neto A.H., and Lanzara A.: Substrate-induced bandgap opening in epitaxial graphene. Nat. Mater. 6, 770775 (2007).
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