Abstract
We introduce a novel approach to the synthesis of high-quality and highly uniform few-layer graphene on silicon wafers, based on solid source growth from epitaxial 3C-SiC films. Using a Ni/Cu catalytic alloy, we obtain a transfer-free bilayer graphene directly on Si(100) wafers, at temperatures potentially compatible with conventional semiconductor processing. The graphene covers uniformly a 2″ silicon wafer, with a Raman ID/ IG band ratio as low as 0.5, indicative of a low defectivity material. The sheet resistance of the graphene is as low as 25 Ω/square, and its adhesion energy to the underlying substrate is substantially higher than transferred graphene. This work opens the avenue for the true wafer-level fabrication of microdevices comprising graphene functional layers. Specifically, we suggest that exceptional conduction qualifies this graphene as a metal replacement for MEMS and advanced on-chip interconnects with ultimate scalability.
Similar content being viewed by others
References
K.S. Novoselov, A.K. Geim, S.V. Morozov, D. Jiang, Y. Zhang, S.V. Dubonos, I.V. Grigorieva, and A.A. Firsov: Electric field effect in atomically thin carbon films. Science 306, 666–669 (2004).
C. Berger, Z. Song, T. Li, X. Li, A.Y. Ogbazghi, R. Feng, Z. Dai, A.N. Marchenkov, E.H. Conrad, P.N. First, and W.A. De Heer: Ultrathin epitaxial graphite: 2D electron gas properties and a route toward graphene-based nanoelectronics. J. Phys. Chem. B 108, 19912–19916 (2004).
W.A. De Heer, C. Berger, M. Ruan, M. Sprinkle, X. Li, Y. Hu, B. Zhang, J. Hankinson, and E. Conrad: Large area and structured epitaxial graphene produced by confinement controlled sublimation of silicon carbide. Proc. Natl. Acad. Sci. U. S. A. 108, 16900–16905 (2011).
S. Forti and U. Starke: Epitaxial graphene on SiC: From carrier density engineering to quasi-free standing graphene by atomic intercalation. J. Phys. D: Appl. Phys. 47, 094013 (2014).
A. Ouerghi, A. Kahouli, D. Lucot, M. Portail, L. Travers, J. Gierak, J. Penuelas, P. Jegou, A. Shukla, T. Chassagne, and M. Zielinski: Epitaxial graphene on cubic SiC(111)/Si(111) substrate. Appl. Phys. Lett. 96, 191910 (2010).
B. Gupta, M. Notarianni, N. Mishra, M. Shafiei, F. Iacopi, and N. Motta: Evolution of epitaxial graphene layers on 3C SiC/Si(111) as a function of annealing temperature in UHV. Carbon 68, 563–572 (2014).
H. Fukidome, S. Abe, R. Takahashi, K. Imaizumi, S. Inomata, H. Handa, E. Saito, Y. Enta, A. Yoshigoe, Y. Tareoka, M. Kotsugi, T. Ohkouchi, T. Kinoshita, S. Ito, and M. Suemitsu: Control over structural and electronic properties of epitaxial graphene on silicon using surface termination of 3C-SiC(111)/Si. Appl. Phys. Express 4, 115104 (2011).
H. Fukidome, R. Takahashi, S. Abe, K. Imaizumi, H. Handa, C.H. Kang, H. Karasawa, T. Suemitsu, T. Otsuji, Y. Enta, A. Yoshigoe, Y. Teraoka, M. Kotsugi, T. Ohkouchi, T. Kinoshita, and M. Suemitsu: Control of epitaxy of graphene by crystallographic orientation of a Si substrate toward device applications. J. Mater. Chem. 21, 17242–17248 (2011).
N. Mishra, L. Hold, A. Iacopi, B. Gupta, N. Motta, and F. Iacopi: Controlling the surface roughness of epitaxial SiC on silicon. J. Appl. Phys. 115, 203501 (2014).
B.V. Cunning, M. Ahmed, N. Mishra, A.R. Kermany, B. Wood, and F. Iacopi: Graphitized silicon carbide microbeams: Wafer-level, self-aligned graphene on silicon wafers. Nanotechnology 25, 325301 (2014).
H. Fukidome, Y. Kawai, H. Handa, H. Hibino, H. Miyashita, M. Kotsugi, T. Ohkochi, M. Jung, T. Suemitsu, T. Kinoshita, T. Otsuji, and M. Suemitsu: Site-selective epitaxy of graphene on Si wafers. Proc. IEEE 101 (7), 1557 (2013).
L. Wang, S. Dimitrijev, P. Tanner, J. Han, A. Iacopi, L. Hold, and B.H. Harrison: Growth of 3C-SiC on 150 mm Si (100) substrates by alternating supply epitaxy at 1000°C. Thin Solid Films 519, 6443–6446 (2011).
F. Iacopi, G. Walker, L. Wang, L. Malesys, S. Ma, B.V. Cunning, and A. Iacopi: Orientation-dependent stress relaxation in hetero-epitaxial 3C-SiC films. Appl. Phys. Lett. 102, 011908 (2013).
R.H. Dauskardt, M. Lane, Q. Ma, and N. Krishna: Adhesion and debonding of multi-layer thin film structures. Eng. Fract. Mech. 61, 141–162 (1998).
M. Lane, R.H. Dauskardt, N. Krishna, and I. Hashim: Adhesion and reliability of copper interconnects with Ta and TaN barrier layers. J. Mater. Res. 15, 203–211 (2000).
A.C. Ferrari and D.M. Basko: Raman spectroscopy as a versatile tool for studying the properties of graphene. Nat. Nanotechnol. 8, 235–246 (2013).
F. Iacopi, B. Cunning, and M. Ahmed: Process for forming graphene layers on silicon carbide. PCT/AU2014/050218, 2014.
Z-Y. Juang, C-Y. Wu, C-W. Lo, W-Y. Chen, C-F. Huang, J-C. Hwang, F-R. Chen, K-C. Leou, and C-H. Tsai: Synthesis of graphene on silicon carbide substrates at low temperature. Carbon 47, 2026–2031 (2009).
A.A. Woodworth and C.D. Stinespring: Surface chemistry of Ni induced graphite formation on the 6H–SiC (0001) surface and its implications for graphene synthesis. Carbon 48, 1999–2003 (2010).
A. Lauwers, A. Steegen, M. De Potter, R. Lindsay, A. Satta, H. Bender, and K. Maex: Materials aspects, electrical performance, and scalability of Ni silicide towards sub-0.13 μm technologies. J. Vac. Sci. Technol., B 19, 2026–2037 (2001).
E. Escobedo-Cousin, K. Vassilevski, T. Hopf, N. Wright, A. O’Neill, A. Horsfall, J. Goss, and P. Cumpson: Local solid phase growth of few-layer graphene on silicon carbide from nickel silicide supersaturated with carbon. J. Appl. Phys. 113, 114309 (2013).
The Landholt-Boernstein Database, Springer Materials online database. Springer.
A. Ouerghi, R. Belkhou, M. Marangolo, M.G. Silly, S. El Moussaoui, M. Eddrief, L. Largeau, M. Portail, and F. Sirotti: Structural coherency of epitaxial graphene on 3C–SiC(111) epilayers on Si(111). Appl. Phys. Lett. 97, 161905 (2010).
A. Ouerghi, A. Balan, C. Castelli, M. Picher, R. Belkhou, M. Eddrief, M.G. Silly, M. Marangolo, A. Shukla, and F. Sirotti: Epitaxial graphene on single domain 3C-SiC (100) thin films grown on off-axis Si (100). Appl. Phys. Lett. 101, 021603 (2012).
C. Coletti, K.V. Emtsev, A.A. Zacharov, T. Ouisse, D. Chaussende, and U. Starke: Large area quasi-free standing monolayer graphene on 3C-SiC(111). Appl. Phys. Lett. 99, 081904 (2011).
G.R. Yazdi, R. Vasiliauskas, T. Iakimov, A. Zacharov, M. Syvajarvi, and R. Yakimova: Growth of large area monolayer graphene on 3C-SiC and a comparison with other SiC polytypes. Carbon 57, 477–484 (2013).
B.J. Baliga: Silicon liquid-phase epitaxy—A review. J. Electrochem. Soc. 133, C5–C14 (1986).
R.S. Wagner and W.C. Ellis: Vapor-liquid-solid mechanism of single crystal growth. Appl. Phys. Lett. 4, 89–90 (1964).
F. Iacopi, O. Richard, Y. Eichhammer, H. Bender, P.M. Vereecken, S. De Gendt, and M. Heyns: Size-dependent characteristics of indium-seeded Si nanowire growth. Electrochem. Solid-State Lett. 11, K98–K100 (2008).
S.P. Koenig, N.G. Boddeti, M.L. Dunn, and J.S. Bunch: Ultrastrong adhesion of graphene membranes. Nat. Nanotechnol. 6, 543–546 (2011).
S. Bae, H. Kim, Y. Lee, X. Xu, J-S. Park, Y. Zheng, J. Balakrishnan, T. Lei, H.R. Kim, Y.I. Song, Y-J. Kim, K.S. Kim, B. Ozyilmaz, J-H. Ahn, and S. Ijima: Roll-to-roll production of 30-inch graphene films for transparent electrodes. Nat. Nanotechnol. 5, 574–578 (2010).
G. Kaestle, H.G. Boyen, A. Schroeder, A. Plettl, and P. Ziemann: Size effect of the resistivity of thin epitaxial gold film. Phys. Rev. B 70, 165414 (2004).
H. Kanter: Slow-electron mean free path in aluminum, silver and gold. Phys. Rev. B 1 (2), 522–536 (1970).
ACKNOWLEDGMENTS
We acknowledge Glenn Walker, Philip Tanner, Alan Iacopi, and Anthony Christian for their valuable technical support. The authors acknowledge the support from the Australian National Fabrication Facility (ANFF) and the Air Force Office of Scientific Research through the grant AOARD 144045. Dr. Francesca Iacopi is the recipient of a Future Fellowship from the Australian Research Council (FT120100445).
Author information
Authors and Affiliations
Corresponding author
Additional information
This paper has been selected as an Invited Feature Paper.
Rights and permissions
About this article
Cite this article
Iacopi, F., Mishra, N., Cunning, B.V. et al. A catalytic alloy approach for graphene on epitaxial SiC on silicon wafers. Journal of Materials Research 30, 609–616 (2015). https://doi.org/10.1557/jmr.2015.3
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1557/jmr.2015.3