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Nano Research 2015, 8(3): 1026-1037 https://doi.org/10.1007/s12274-014-0584-y
Research Article | Issue | Published: 30 October 2014

Self-organized metal-semiconductor epitaxial graphene layer on off-axis 4H-SiC(0001)

Show Author's Information Debora Pierucci1,  Haikel Sediri1,  Mahdi Hajlaoui1,2,  Emilio Velez-Fort1,3,  Yannick J. Dappe4,  Mathieu G. Silly2,  Rachid Belkhou2,  Abhay Shukla3,  Fausto Sirotti2,  Noelle Gogneau1,  Abdelkarim Ouerghi1( )
CNRS-Laboratoire de Photonique et de NanostructuresRoute de Nozay91460Marcoussis, France
Synchrotron-SOLEILSaint-AubinBP48F91192Gif sur Yvette CedexFrance
Université Pierre et Marie Curie (CNRS – IMPMC)4 Pl. Jussieu75005ParisFrance
Service de Physique de l'Etat Condensé (CNRS URA2464)IRAMISCEA Saclay91191Gif-Sur-Yvette, France
Keywords:
monolayer, bilayer, electronic properties, epitaxial graphene layer, band gap opening, Bernal stacking, off-axis silicon carbide
Cite this article:
Pierucci D, Sediri H, Hajlaoui M, et al. Self-organized metal-semiconductor epitaxial graphene layer on off-axis 4H-SiC(0001). Nano Research, 2015, 8(3): 1026-1037. https://doi.org/10.1007/s12274-014-0584-y
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Abstract Full text About this article

The remarkable properties of graphene have shown promise for new perspectives in future electronics, notably for nanometer scale devices. Here we grow graphene epitaxially on an off-axis 4H-SiC(0001) substrate and demonstrate the formation of periodic arrangement of monolayer graphene on planar (0001) terraces and Bernal bilayer graphene on (1120) nanofacets of SiC. We investigate these lateral superlattices using Raman spectroscopy, atomic force microscopy/electrostatic force microscopy (AFM/EFM) and X-ray and angle resolved photoemission spectroscopy (XPS/ARPES). The correlation of EFM and ARPES reveals the appearance of permanent electronic band gaps in AB-stacked bilayer graphene on (1120) SiC nanofacets of 150 meV. This feature is confirmed by density functional theory (DFT) calculations. The charge transfer between the substrate and graphene bilayer results in an asymmetric charge distribution between the top and the bottom graphene layers opening an energy gap. This surface organization can be thus defined as self-organized metal-semiconductor graphene.


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About this article

Self-organized metal-semiconductor epitaxial graphene layer on off-axis 4H-SiC(0001)

Show Author's information Debora Pierucci1, Haikel Sediri1, Mahdi Hajlaoui1,2, Emilio Velez-Fort1,3, Yannick J. Dappe4, Mathieu G. Silly2, Rachid Belkhou2, Abhay Shukla3, Fausto Sirotti2, Noelle Gogneau1, Abdelkarim Ouerghi1( )
CNRS-Laboratoire de Photonique et de NanostructuresRoute de Nozay91460Marcoussis, France
Synchrotron-SOLEILSaint-AubinBP48F91192Gif sur Yvette CedexFrance
Université Pierre et Marie Curie (CNRS – IMPMC)4 Pl. Jussieu75005ParisFrance
Service de Physique de l'Etat Condensé (CNRS URA2464)IRAMISCEA Saclay91191Gif-Sur-Yvette, France

Abstract

The remarkable properties of graphene have shown promise for new perspectives in future electronics, notably for nanometer scale devices. Here we grow graphene epitaxially on an off-axis 4H-SiC(0001) substrate and demonstrate the formation of periodic arrangement of monolayer graphene on planar (0001) terraces and Bernal bilayer graphene on (1120) nanofacets of SiC. We investigate these lateral superlattices using Raman spectroscopy, atomic force microscopy/electrostatic force microscopy (AFM/EFM) and X-ray and angle resolved photoemission spectroscopy (XPS/ARPES). The correlation of EFM and ARPES reveals the appearance of permanent electronic band gaps in AB-stacked bilayer graphene on (1120) SiC nanofacets of 150 meV. This feature is confirmed by density functional theory (DFT) calculations. The charge transfer between the substrate and graphene bilayer results in an asymmetric charge distribution between the top and the bottom graphene layers opening an energy gap. This surface organization can be thus defined as self-organized metal-semiconductor graphene.

Keywords: monolayer, bilayer, electronic properties, epitaxial graphene layer, band gap opening, Bernal stacking, off-axis silicon carbide

References(59)

1

Costa Girão, E.; Liang, L. B.; Cruz-Silva, E.; Filho, A. G. S.; Meunier, V. Emergence of a typical properties in assembled graphene nanoribbons. Phys. Rev. Lett. 2011, 107, 135501.
DOI Google Scholar
2

Sprinkle, M.; Ruan, M.; Hu, Y.; Hankinson, J.; Rubio-Roy, M.; Zhang, B.; Wu, X.; Berger, C.; de Heer, W. A. Scalable templated growth of graphene nanoribbons on SiC. Nat. Nanotechnol. 2010, 5, 727-731.
DOI Google Scholar
3

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.; Lanzara, A. Substrate-induced bandgap opening in epitaxial graphene. Nat. Mater. 2007, 6, 770-775.
DOI Google Scholar
4

Son, Y. W.; Cohen, M. L.; Louie, S. G. Energy gaps in graphene nanoribbons. Phys. Rev. Lett. 2006, 97, 216803.
DOI Google Scholar
5

Chen, Z. H.; Lin, Y. M.; Rooks, M. J.; Avouris, P. Graphene nano-ribbon electronics. Physica E Lowdimens Syst. Nanostruct. 2007, 40, 228-232.
DOI Google Scholar
6

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 2004, 306, 666-669.
DOI Google Scholar
7

Stankovich, S.; Dikin, D. A.; Dommett, G. H. B.; Kohlhaas, K. M.; Zimney, E. J.; Stach, E. A.; Piner, R. D.; Nguyen, S. T.; Ruoff, R. S. Graphene-based composite materials. Nature 2006, 442, 282-286.
DOI Google Scholar
8

Hass, J.; de Heer, W. A.; Conrad, E. H. The growth and morphology of epitaxial multilayer graphene. J. Phys. : Condens. Matter 2008, 20, 323202.
DOI Google Scholar
9

Varchon, F.; Feng, R.; Hass, J.; Li, X.; Nguyen, B. N.; Naud, C.; Mallet, P.; Veuillen, J. Y.; Berger, C.; Conrad, E. H. et al. Electronic structure of epitaxial graphene layers on SiC: Effect of the substrate. Phys. Rev. Lett. 2007, 99, 126805.
DOI Google Scholar
10

Forbeaux, I.; Themlin, J. M.; Debever, J. M. Heteroepitaxial graphite on 6H-SiC (0001): Interface formation through conduction-band electronic structure. Phys. Rev. B 1998, 58, 396-406.
DOI Google Scholar
11

Somani, P. R.; Somani, S. P.; Umeno, M. Planer nano-graphenes from camphor by CVD. Chem. Phys. Lett. 2006, 430, 56-59.
DOI Google Scholar
12

Sutter, P. W.; Flege, J. I.; Sutter, E. A. Epitaxial graphene on ruthenium. Nat. Mater. 2008, 7, 406-411.
DOI Google Scholar
13

Reina, A.; Jia, X. T.; 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. 2009, 9, 30-35.
DOI Google Scholar
14

Wang, J. J.; Zhu, M. Y.; Outlaw, R. A.; Zhao, X.; Manos, D. M.; Holloway, B. C. Synthesis of carbon nanosheets by inductively coupled radio-frequency plasma enhanced chemical vapor deposition. Carbon 2004, 42, 2867-2872.
DOI Google Scholar
15

Wang, J. J.; Zhu, M. Y.; Outlaw, R. A.; Zhao, X.; Manos, D. M.; Holloway, B. C.; Mammana, V. P. Free-standing subnanometer graphite sheets. Appl. Phys. Lett. 2004, 85, 1265.
DOI Google Scholar
16

Berger, C.; Song, Z. M.; Li, X. B.; Wu, X. S.; Brown, N.; Naud, C.; Mayou, D.; Li, T. B.; Hass, J.; Marchenkov, A. N. et al. Electronic confinement and coherence in patterned epitaxial graphene. Science 2006, 312, 1191-1196.
DOI Google Scholar
17

Brey, L.; Fertig, H. Electronic states of graphene nanoribbons studied with the Dirac equation. Phys. Rev. B 2006, 73, 235411.
DOI Google Scholar
18

Nakada, K.; Fujita, M.; Dresselhaus, G.; Dresselhaus, M. S. Edge state in graphene ribbons: Nanometer size effect and edge shape dependence. Phys. Rev. B 1996, 5417954.
DOI Google Scholar
19

Han, M. Y.; Özyilmaz, B.; Zhang, Y. B.; Kim, P. Energy band-gap engineering of graphene nanoribbons. Phys. Rev. Lett. 2007, 98, 206805.
DOI Google Scholar
20

Tapasztó, L.; Dobrik, G.; Lambin, P.; Biró, L. P. Tailoring the atomic structure of graphene nanoribbons by STM lithography. Nat. Nanotechnol. 2008, 3, 397-401.
DOI Google Scholar
21

Han, M. Y.; Brant, J. C.; Kim, P. Electron transport in disordered graphene nanoribbons. Phys. Rev. Lett. 2010, 104, 056801.
DOI Google Scholar
22

Bolotin, K. I.; Sikes, K. J.; Jiang, Z.; Klima, M.; Fudenberg, G.; Hone, J.; Kim, P.; Stormer, H. L. Ultrahigh electron mobility in suspended graphene. Solid State Commun. 2008, 146, 351-355.
DOI Google Scholar
23

Hwang, E. H.; Adam, S.; Das Sarma, S. Transport in chemically doped graphene in the presence of adsorbed molecules. Phys. Rev. B 2007, 76, 195421.
DOI Google Scholar
24

Moser, J.; Barreiro, A.; Bachtold, A. Current-induced cleaning of graphene. Appl. Phys. Lett. 2007, 91 163513.
DOI Google Scholar
25

Camara, N.; Rius, G.; Huntzinger, J. R.; Tiberj, A.; Mestres, N.; Godignon, P.; Camassel, J. Selective epitaxial growth of graphene on SiC. Appl. Phys. Lett. 2008, 93, 123503.
DOI Google Scholar
26

Rubio-Roy, M.; Zaman, F.; Hu, Y.; Berger, C.; Moseley, M. W.; Meindl, J. D.; de Heer, W. A. Structured epitaxial graphene growth on SiC by selective graphitization using a patterned AlN cap. Appl. Phys. Lett. 2010, 96, 082112.
DOI Google Scholar
27

Camara, N.; Huntzinger, J. R.; Rius, G.; Tiberj, A.; Mestres, N.; Pérez-Murano, F.; Godignon, P.; Camassel, J. Anisotropic growth of long isolated graphene ribbons on the C face of graphite-capped 6H-SiC. Phys. Rev. B 2009, 80, 125410.
DOI Google Scholar
28

Hicks, J.; Tejeda, A.; Taleb-Ibrahimi, A.; Nevius, M. S.; Wang, F.; Shepperd, K.; Palmer, J.; Bertran, F.; Le Fèvre, P.; Kunc, J. et al. A wide-bandgap metal-semiconductor-metal nanostructure made entirely from graphene. Nat. Phys. 2013, 9, 49-54.
DOI Google Scholar
29

Ohta, T.; Bostwick, A.; Seyller, T.; Horn, K.; Rotenberg, E. Controlling the electronic structure of bilayer graphene. Science 2006, 313, 951-954.
DOI Google Scholar
30

Ouerghi, A.; Silly, M. G.; Marangolo, M.; Mathieu, C.; Eddrief, M.; Picher, M.; Sirotti, F.; EI Moussaoui, S.; Belkhou, R. Large-area and high-quality epitaxial graphene on off-axis SiC wafers. ACS Nano 2012, 6, 6075-6082.
DOI Google Scholar
31

Nicotra, G.; Ramasse, Q. M.; Deretzis, I.; La Magna, A.; Spinella, C.; Giannazzo, F. Delaminated graphene at silicon carbide facets: Atomic scale imaging and spectroscopy. ACS Nano 2013, 7, 3045-3052.
DOI Google Scholar
32

Tanaka, S.; Morita, K.; Hibino, H. Anisotropic layer-by-layer growth of graphene on vicinal SiC(0001) surfaces. Phys. Rev. B 2010, 81, 041406.
DOI Google Scholar
33

Vecchio, C.; Sonde, S.; Bongiorno, C.; Rambach, M.; Yakimova, R.; Raineri, V.; Giannazzo, F. Nanoscale structural characterization of epitaxial graphene grown on off-axis 4H-SiC (0001). Nanoscale Res. Lett. 2011, 6, 269.
DOI Google Scholar
34

Lalmi, B.; Girard, J. C.; Pallecchi, E.; Silly, M.; David, C.; Latil, S.; Sirotti, F.; Ouerghi, A. Flower-shaped domains and wrinkles in trilayer epitaxial graphene on silicon carbide. Sci. Rep. 2014, 4, 4066.
DOI Google Scholar
35

Pallecchi, E.; Lafont, F.; Cavaliere, V.; Schopfer, F.; Mailly, D.; Poirier, W.; Ouerghi, A. High electron mobility in epitaxial graphene on 4H-SiC(0001) via post-growth annealing under hydrogen. Sci. Rep. 2014, 4, 4558.
DOI Google Scholar
36

Polack, F.; Silly, M.; Chauvet, C.; Lagarde, B.; Bergeard, N.; Izquierdo, M.; Chubar, O.; Krizmancic, D.; Ribbens, M.; Duval, J. P. et al. TEMPO: A new insertion device beamline at SOLEIL for time resolved photoelectron spectroscopy experiments on solids and interfaces. AIP Conf. Proc. 2010, 1234, 185-188.
DOI Google Scholar
37

Bergeard, N.; Silly, M. G.; Krizmancic, D.; Chauvet, C.; Guzzo, M.; Ricaud, J. P.; Izquierdo, M.; Stebel, L.; Pittana, P.; Sergo, R. et al. Time-resolved photoelectron spectroscopy using synchrotron radiation time structure. J. Synchrotron Radiat. 2011, 18, 245-250.
DOI Google Scholar
38

Lewis, J. P.; Glaesemann, K. R.; Voth, G. A.; Fritsch, J.; Demkov, A. A.; Ortega, J.; Sankey, O. F. Further developments in the local-orbital density-functional-theory tight-binding method. Phys. Rev. B 2001, 64, 195103.
DOI Google Scholar
39

Lewis, J. P.; Jelínek, P.; Ortega, J.; Demkov, A. A.; Trabada, D. G.; Haycock, B.; Wang, H.; Adams, G.; Tomfohr, J. K.; Abad, E. et al. Advances and applications in the FIREBALL ab initio tight-binding molecular-dynamics formalism. Phys. Status Solidi B 2011, 248, 1989-2007.
DOI Google Scholar
40

Jelínek, P.; Wang, H.; Lewis, J. P.; Sankey, O. F.; Ortega, J. Multicenter approach to the exchange-correlation interactions in ab initio tight-binding methods. Phys. Rev. B 2005, 71, 235101.
DOI Google Scholar
41

Sankey, O. F.; Niklewski, D. J. Ab initio multicenter tight-binding for molecular-dynamics simulations and other applications in covalent systems. Phys. Rev. B 1989, 40, 3979-3995.
DOI Google Scholar
42

Basanta, M. A.; Dappe, Y. J.; Jelínek, P.; Ortega, J. Optimized atomic-like orbitals for first-principles tight-binding molecular dynamics. Comp. Mater. Sci. 2007, 39, 759-766.
DOI Google Scholar
43

Dappe, Y. J.; Ortega, J.; Flores, F. Intermolecular interaction in density functional theory: Application to carbon nanotubes and fullerenes. Phys. Rev. B 2009, 79, 165409.
DOI Google Scholar
44

Švec, M.; Merino, P.; Dappe, Y. J.; González, C.; Abad, E.; Jelínek, P.; Martin-Gago, J. A. van der Waals interactions mediating the cohesion of fullerenes on graphene. Phys. Rev. B 2012, 86, 121407.
DOI Google Scholar
45

Ouerghi, A.; Balan, A.; Castelli, C.; Picher, M.; Belkhou, R.; Eddrief, M.; Silly, M. G.; Marangolo, M.; Shukla, A.; Sirotti, F. Epitaxial graphene on single domain 3C-SiC (100) thin films grown on off-axis. Appl. Phys. Lett. 2012, 101, 021603.
DOI Google Scholar
46

Michon, A.; Vézian, S.; Ouerghi, A.; Zielinski, M.; Chassagne, T.; Portail, M. Direct growth of few-layer graphene on 6H-SiC and 3C-SiC/Si via propane chemical vapor deposition. Appl. Phys. Lett. 2010, 97, 171909.
DOI Google Scholar
47

Giannazzo, F.; Deretzis, I.; Nicotra, G.; Fisichella, G.; Spinella, C.; Roccaforte, F.; La Magna, A. Electronic properties of epitaxial graphene residing on SiC facets probed by conductive atomic force microscopy. Appl. Surf. Sci. 2014, 291, 53-57.
DOI Google Scholar
48

Huang, H.; Wong, S. L.; Tin, C. C.; Luo, Z. Q.; Shen, Z. X.; Chen, W.; Wee, A. T. S. Epitaxial growth and characterization of graphene on free-standing polycrystalline 3C-SiC. J. Appl. Phys. 2011, 110, 014308.
DOI Google Scholar
49

Pimenta, M. A.; Dresselhaus, G.; Dresselhaus, M. S.; Cançado, L. G.; Jorio, A.; Saito, R. Studying disorder in graphite-based systems by Raman spectroscopy. Phys. Chem. Chem. Phys. 2007, 9, 1276-1291.
DOI Google Scholar
50

Burnett, T.; Yakimova, R.; Kazakova, O. Mapping of local electrical properties in epitaxial graphene using electrostatic force microscopy. Nano Lett. 2011, 11, 2324-2328.
DOI Google Scholar
51

Gogneau, N.; Balan, A.; Ridene, M.; Shukla, A.; Ouerghi, A. Control of the degree of surface graphitization on 3C-SiC(100)/Si(100). Surf. Sci. 2012, 606, 217-220.
DOI Google Scholar
52

Filleter, T.; Emtsev, K. V.; Seyller, T.; Bennewitz, R. Local work function measurements of epitaxial graphene. Appl. Phys. Lett. 2008, 93, 133117.
DOI Google Scholar
53

Coletti, C.; Emtsev, K. V.; Zakharov, A. A.; Ouisse, T.; Chaussende, D.; Starke, U. Large area quasi-free standing monolayer graphene on 3C-SiC(111). Appl. Phys. Lett. 2011, 99, 081904.
DOI Google Scholar
54

Emtsev, K. V.; Speck, F.; Seyller, T.; Ley, L.; Riley, J. D. Interaction, growth, and ordering of epitaxial graphene on SiC{0001} surfaces: A comparative photoelectron spectroscopy study. Phys. Rev. B 2008, 77, 155303.
DOI Google Scholar
55

Penuelas, J.; Ouerghi, A.; Lucot, D.; David, C.; Gierak, J.; Estrade-Szwarckopf, H.; Andreazza-Vignolle, C. Surface morphology and characterization of thin graphene films on SiC vicinal substrate. Phys. Rev. B 2009, 79, 033408.
DOI Google Scholar
56

Jabakhanji, B.; Michon, A.; Consejo, C.; Desrat, W.; Portail, M.; Tiberj, A.; Paillet, M.; Zahab, A.; Cheynis, F.; Lafont, F. et al. Tuning the transport properties of graphene films grown by CVD on SiC(0001): Effect of in situ hydrogenation and annealing. Phys. Rev. B 2014, 89, 085422.
DOI Google Scholar
57

Ostler, M.; Deretzis, I.; Mammadov, S.; Giannazzo, F.; Nicotra, G.; Spinella, C.; Seyller, T.; La Magna, A. Direct growth of quasi-free-standing epitaxial graphene on nonpolar SiC surfaces. Phys. Rev. B 2013, 88, 085408.
DOI Google Scholar
58

Jayasekera, T.; Xu, S.; Kim, K. W.; Nardelli, M. B. Electronic properties of the graphene/6H-SiC(000-1) interface: A first-principles study. Phys. Rev. B 2011, 84, 035442.
DOI Google Scholar
59

Ohta, T.; Bostwick, A.; Mcchesney, J. L.; Seyller, T.; Horn, K.; Rotenberg, E. Interlayer interaction and electronic screening in multilayer graphene investigated with angle-resolved photoemission spectroscopy. Phys. Rev. Lett. 2007, 98, 206802.
DOI Google Scholar
Publication history
Copyright
Acknowledgements

Publication history

Received: 26 June 2014
Revised: 13 August 2014
Accepted: 15 September 2014
Published: 30 October 2014
Issue date: March 2015

Copyright

© Tsinghua University Press and Springer-Verlag Berlin Heidelberg 2014

Acknowledgements

Acknowledgements

The authors thank the French National Research Agency (ANR) SUPERTRAMP project and LABEX NanoSaclay for funding.

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