Abstract
We report on the study of deposition of carbon films on different substrates: (001) Si, (001) Si covered with 300 nm \(\hbox {SiO}_{2} (\hbox {Si/SiO}_{2})\) film as well as on (001) Si covered with \(\hbox {SiO}_{2}\) and diamond-like carbon layers (DLC) carried out by sublimation of pyrolytic carbon layers. It is established by Raman as well as by X-ray photoelectron spectroscopy (XPS) that the layers deposited on Si as well as on \(\hbox {Si/SiO}_{2}\) substrates consist of amorphous \(\hbox {sp}^{2}\)—bonded carbon (\(\upalpha \)-C) and the longer deposition time leads to formation of micro-sized \(\upalpha \)-C islands. The Raman studies of the films deposited on the \(\hbox {SiO}_{2}\) covered areas in the third type substrates have requisites of defected graphene (presence of clear D and weak broadening of the 2D band while the intensity ratio of 2D to G and D bands remains high: more than 2.5 and 3.1, respectively) and the films are predominantly single-layered. These films are determined as “polygraphene” (mainly single-layered graphene film consisting of mutually misoriented areas). The films deposited on the DLC paths in the third type of substrates most probably consist of few layers of mixed few-layered polygraphene and \((\hbox {sp}^{2}\hbox {C})\)- and \((\hbox {sp}^{3}\hbox {C})\)- H phases. The thorough XPS study indirectly confirms the above conclusions. The formation of polygraphene and mixed phases is explained with nucleation of many stable carbon aggregates which, once formed, are not sufficiently mobile to mutually re-orientate until forming defect-free graphene.
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Becerril, H.A., Mao, J., Liu, Z., Stoltenberg, R.M., Bao, Z., Chen, Y.: Evaluation of solution-processed reduced graphene oxide films as transparent conductors. ACS Nano 2, 463–470 (2008)
Berger, C., Song, Z., Li, T., Li, X., Ogbazghi, A.Y., Feng, R., Dai, Z., Marchenko, A.N., Conrad, E.H., First, P.N.: Ultrathin epitaxial graphite: 2D electron gas properties and a route toward graphene-based nanoelectronics. J. Phys. Chem. 108, 19912–19916 (2004)
Berger, C., Song, Z., Li, T., Li, X., Wu, X., Brown, N., Naud, C., Mayou, D., Marchenko, A.N., Conrad, E.H.: Electronic confinement and coherence in patterned epitaxial graphene. Science 312, 1191–1196 (2006)
Bradshaw, A.M., Cederbaum, S.L., Domcke, W., Krause, U.: Plasmon coupling to core hole excitations in carbon. J. Phys. C Solid State 7, 4503–4512 (1974)
Brar, V.W., Samsonidze, G.G., Dresselhaus, M.S., Dresselhaus, G., Saito, R., Swan, A.K., Ünlü, M.S., Goldberg, B.B., Souza, Filho, A.G., Jorio, A.: Second-order harmonic and combination modes in graphite, single-wall carbon nanotube bundles, and isolated single-wall carbon nanotubes. Phys. Rev. B 66, 155418-155427 (2002)
Casiraghi, C., Pisana, S., Novoselov, K.S., Geim, A.K., Ferrari, A.C.: Raman fingerprint of charged impurities in graphene. Appl. Phys. Lett. 91, 233108–233110 (2007)
Chen, J.H., Jang, C., Xiao, S., Ishigami, M., Fuhrer, M.S.: Intrinsic and extrinsic performance limits of graphene devices on \(\text{SiO}_{2}\). Nat. Nanotechnol. 3, 206–209 (2008)
Cong, C., Yu, T., Saito, R., Dresselhaus, G.F., Dresselhaus, M.S.: Second-order overtone and combination Raman modes of graphene layers in the range of 1690–2150 \(\text{cm}^{-1}\). ACS Nano 5, 1600–1605 (2011)
Díaz, J., Paolicelli, G., Ferrer, S., Comin, F.: Separation of the sp3 and sp2 components in the C1s photoemission spectra of amorphous carbon films. Phys. Rev. B 54, 8064–8069 (1996)
Ding, X., Ding, G., Xie, X., Huang, F., Jiang, M.: Direct growth of few layer graphene on hexagonal boron nitride by chemical vapor deposition. Carbon 49, 2522–2525 (2011)
Dwivedi, N., Kumar, S., Malik, H.K., Govind, Rauthan, C.M.S., Panwar, O.S.: Correlation of \(\text{sp}^{3}\) and \(\text{sp}^{2}\) fraction of carbon with electrical, optical and nano-mechanical properties of argondiluted diamond-like carbon films. Appl. Surf. Sci. 257, 6804–6810 (2011)
Ferrari, A.C.: Raman spectroscopy of graphene and graphite: disorder, electron phonon coupling, doping and nonadiabatic effects. Solid State Commun. 143, 47–57 (2007)
Ferrari, A.C., Basko, D.M.: Raman spectroscopy as a versatile tool for studying the properties of graphene. Nat. Nanotechnol. 8, 235–246 (2013)
Ferrari, A.C., Meyer, J.C., Scardaci, V., Casiraghi, C., Lazzeri, M., Mauri, F., Piscanec, S., Jiang, D., Novoselov, K.S., Roth, S., Geim, A.K.: Raman spectrum of graphene and graphene layers. Phys. Rev. Lett. 97, 187401–187404 (2007)
Ferrari, A.C., Robertson, J.: Interpretation of Raman spectra of disordered and amorphous carbon. Phys. Rev. B 61, 14095–14107 (2000)
Ferrari, A.C., Robertson, J.: Resonant Raman spectroscopy of disordered, amorphous, and diamondlike carbon. Phys. Rev. B 64, 075414–075426 (2001)
Geim, A.K., MacDonald, A.H.: Graphene: exploring carbon flatland. Phys. Today 60, 35–41 (2007)
Haerle, R., Riedo, E., Pasquarello, A., Baldereschi, A.: \(\text{sp}^{2}/\text{sp}^{3}\) hybridization ratio in amorphous carbon from C 1 s corelevel shifts: X-ray photoelectron spectroscopy and firstprinciples calculation. Phys. Rev. B 65, 045101 (2001)
Hawaldar R., Merino P., Correia M.R., Bdikin I., Grácio J., Méndez J., Martín-Gago J.A., Singh M.K.: Large-area high-throughput synthesis of monolayer graphene sheet by hot filament thermal chemical vapor deposition. Nat. Sci. Rep. 2, Art.Nr. 682, p. 1–9 (2012)
Han, W., Zettl, A.: An efficient route to graphitic carbon-layer-coated gallium nitride nanorods. Adv. Mater. 14, 1560–1562 (2002)
Heersche, H.B., Jarillo-Herrero, P., Oostinga, J.B., Vandersypen, L.M.K., Morpurgo, A.F.: Bipolar supercurrent in graphene. Nature 446, 56–59 (2007)
Hofrichter, J., Szafranek, B.N., Otto, M., Echtermeyer, T.J., Baus, M., Majerus, A., Geringer, V., Ramsteiner, M., Kurz, H.: Synthesis of graphene on silicon dioxide by a solid carbon source. Nano Lett. 10, 36–42 (2010)
Ismach, A., Druzgalski, C., Penwell, S., Schwartzberg, A., Zheng, M., Javey, A., Bokor, J., Zhang, Y.: Direct chemical vapor deposition of graphene on dielectric surfaces. Nano Lett. 10, 1542–1548 (2010)
Jiao, L., Wang, X., Diankov, G., Wang, H., Dai, H.: Facile synthesis of high-quality graphene nanoribbons. Nat. Nanotechnol. 5, 321–325 (2010)
Johnson, J.A., Holland, D., Woodford, J.B., Zinovev, A., Gee, I.A., Eryilmaz, O.L., Erdemir, A.: Top surface characterization of a near frictionless carbon film. Diam. Relat. Mater. 16, 209–215 (2007)
Kosynkin, D.V., Higginbotham, A.L., Sinitskii, A., Lomeda, J.R., Dimiev, A., Price, B.K., Tour, J.M.: Longitudinal unzipping of carbon nanotubes to form graphene nanoribbons. Nature 458, 872–876 (2009)
Lascovich, J.C., Giorgi, R., Scaglione, S.: Evaluation of the \(\text{sp}^{2}/\text{sp}^{3}\) ratio in amorphous carbon structure by XPS and XAES. Appl. Surf. Sci. 47, 17–21 (1991)
Li, X., Cai, W., An, J., Kim, S., Nah, J., Yang, D., Piner, R., Velamakanni, A., Jung, I., Tutuc, E., Banerjee, S.K., Colombo, L., Ruoff, R.S.: Large-area synthesis of high-quality and uniform graphene films on copper foils. Science 324, 1312–1314 (2009)
Lundeberg, M.B., Folk, J.A.: Spin-resolved quantum interference in graphene. Nat. Phys. 5, 894–897 (2009)
Malard, L.M., Pimenta, M.A., Dresselhaus, G.F., Dresselhaus, M.S.: Raman spectroscopy in graphene. Phys. Rep. 473, 51–87 (2009)
Michaelson, Sh, Hoffman, A.: Hydrogen bonding, content and thermal stability in nano-diamond films. Diam. Relat. Mater. 15, 486–497 (2006)
Milenov, T.I.: Chemical-vapour-deposition-initiated growth and characterization of diamond and diamond-like micro-crystals. J. Cryst. Growth 310, 5447–5452 (2008)
Morar, J.F., Himpsel, F.J., Hollinger, G., Jordan, J.L., Hughes, G., McFeely, F.R.: Carbon 1s excitation studies of diamond (111). I. Surface core levels. Phys. Rev. B 33, 1340–1345 (1986)
Nemanich, R.J., Solin, S.A.: First- and second-order Raman scattering from finite-size crystals of graphite. Phys. Rev. B 20, 392–401 (1979)
Ni, Z., Wang, Y., Yu, T., Shen, Z.: Raman spectroscopy and imaging of graphene. Nano Res. 1, 273–291 (2008)
Novoselov, K.S., Geim, A.K., Morozov, S.V., Jiang, D., Zhang, Y., Dubonos, S.V., Grigorieva, I.V., Firsov, A.A.: Electric field effect in atomically thin carbon films. Science 306, 666–669 (2004)
Novoselov, K.S., Geim, A.K., Morozov, S.V., Jiang, D., Katsnelson, M.I., Grigorieva, I.V., Dubonos, S.V., Firsov, A.A.: Two-dimensional gas of massless Dirac fermions in graphene. Nature 438, 197–200 (2005)
Poncharal, P., Ayari, A., Michel, T., Sauvajol, J.-L.: Raman spectra of misoriented bilayer graphene. Phys. Rev. B 78, 113407 (2008)
Reina, A., Jia, X., Ho, J., Nezich, D., Son, H., Bulovic, V., Dresselhaus, M.S., Kong, J.: Large area, few-layer graphene films on arbitrary substrates by chemical vapor deposition. Nano Lett. 9, 30–35 (2009)
Rummeli, M.H., Bachmatiuk, A., Scott, A., Borrnert, F., Warner, J.H., Hoffman, V., Lin, J.-H., Cuniberti, G., Büchner, B.: Direct low-temperature nanographene CVD synthesis over a dielectric insulator. ACS Nano 4, 4206–4210 (2010)
Rutherford R.B., Dudman R.L.: US Patent 6 667 100 B2 (2003)
Stankovich, S., Dikin, D.A., Piner, R.D., Kohlhaas, K.A., Kleinhammes, A., Jia, Y., Wu, Y., Nguyen, S.B.T., Ruoff, R.S.: Synthesis of graphene-based nanosheets via chemical reduction of exfoliated graphite oxide. Carbon 45, 1558–1565 (2007)
Sun, J., Lindvall, N., Cole, M.T., Teo, K.B.K., Yurgens, A.: Large-area uniform graphene-like thin films grown by chemical vapor deposition directly on silicon nitride. Appl. Phys. Lett. 98, 252107–252109 (2011)
Sun, J., Lindvall, N., Cole, M.T., Wang, T., Booth, T.J., Bøggild, P., Teo, K.B.K., Liu, J., Yurgens, A.: Controllable chemical vapor deposition of large area uniform nanocrystalline graphene directly on silicon dioxide. J. Appl. Phys. 111, 044103–044106 (2012)
Sun, Z., Yan, Z., Yao, J., Beitler, E., Zhu, Y., Tour, J.M.: Growth of graphene from solid carbon sources. Nature 468, 549–552 (2010)
Svensson, S., Eriksson, B., Maartensson, N., Wendin, G., Gelius, U.: Electron shake-up and correlation satellites and continuum shake-off distributions in X-ray photoelectron spectra of the rare gas atoms. J. Electron Spectrosc. Relat. Phenom. 47, 327–384 (1988)
Thomsen, C., Reich, S.: Double resonant Raman scattering in graphite. Phys. Rev. Lett. 85, 5214–5217 (2000)
Tsen, A.W., Brown, L., Levendorf, M.P., Ghahari, F., Huang, P.Y., Havener, R.W., Ruiz-Vargas, C.S., Muller, D.A., Kim, P., Park, J.: Tailoring electrical transport across grain boundaries in polycrystalline graphene. Science 336, 1143–1146 (2012)
Tuinstra, F., Koenig, J.L.: Raman spectrum of graphite. J. Chem. Phys. 53, 1126–1130 (1970)
Vo-Van, C., Kimouche, A., Reserbat-Plantey, A., Fruchart, O., Bayle-Guillemaud, P., Bendiab, N., Coraux, J.: Epitaxial graphene prepared by chemical vapor deposition on single crystal thin iridium films on sapphire. Appl. Phys. Lett. 98, 181903–181903 (2011)
Wang, Y., Ni, Z., Yu, T., Shen, Z., Wang, H., Wu, Y., Chen, W., Wee, A.T.S.: Raman studies of monolayer graphene: the substrate effect. J. Phys. Chem. C 112, 10637–10640 (2008)
Wei, D., Liu, Y., Zhang, H., Huang, L., Wu, B., Chen, J., Yu, G.: Scalable synthesis of few-layer graphene ribbons with controlled morphologies by a template method and their applications in nanoelectromechanical switches. J. Am. Chem. Soc. 131, 11147–11154 (2009)
Wilson, J.I.B., Walton, J.S., Beamson, G.: Analysis of chemical vapour deposited diamond films by X-ray photoelectron spectroscopy. J. Electron Spectrosc. Relat. Phenom. 121, 183–201 (2001)
Yazyev, O.V., Louie, S.G.: Electronic transport in polycrystalline graphene. Nat. Mater. 9, 806–809 (2010)
Zhang, Y., Tan, Y.W., Stormer, H.L., Kim, P.: Experimental observation of the quantum Hall effect and Berry’s phase in graphene. Nature 438, 201–204 (2005)
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The authors gratefully acknowledge Assoc. Prof. E.P. Valcheva (Faculty of Physics, Sofia University, Sofia) for help with the Raman measurements as well as support from MPNS COST ACTION MP1204 - TERA-MIR Radiation: Materials, Generation, Detection and Applications.
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Milenov, T., Avramova, I. Deposition of graphene by sublimation of pyrolytic carbon. Opt Quant Electron 47, 851–863 (2015). https://doi.org/10.1007/s11082-014-0015-z
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DOI: https://doi.org/10.1007/s11082-014-0015-z