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Register a new userSurfactant-Mediated Epitaxial Growth of Single-Layer Graphene in an Unconventional Orientation on SiC
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Fran\\c{c}ois C. Bocquet
Publication date
2018
fields
Physics
and research's language is
English
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We report the use of a surfactant molecule during the epitaxy of graphene on SiC(0001) that leads to the growth in an unconventional orientation, namely $R0^circ$ rotation with respect to the SiC lattice. It yields a very high-quality single-layer graphene with a uniform orientation with respect to the substrate, on the wafer scale. We find an increased quality and homogeneity compared to the approach based on the use of a pre-oriented template to induce the unconventional orientation. Using spot profile analysis low energy electron diffraction, angle-resolved photoelectron spectroscopy, and the normal incidence x-ray standing wave technique, we assess the crystalline quality and coverage of the graphene layer. Combined with the presence of a covalently-bound graphene layer in the conventional orientation underneath, our surfactant-mediated growth offers an ideal platform to prepare epitaxial twisted bilayer graphene via intercalation.
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An in vacuo thermal desorption process has been accomplished to form epitaxial graphene (EG) on 4H- and 6H-SiC substrates using a commercial chemical vapor deposition reactor. Correlation of growth conditions and the morphology and electrical properties of EG are described. Raman spectra of EG on Si-face samples were dominated by monolayer thickness. This approach was used to grow EG on 50 mm SiC wafers that were subsequently fabricated into field effect transistors with fmax of 14 GHz.
Epitaxial graphene layers were grown on the C-face of 4H- and 6H-SiC using an argon-mediated growth process. Variations in growth temperature and pressure were found to dramatically affect the morphological properties of the layers. The presence of argon during growth slowed the rate of graphene formation on the C-face and led to the observation of islanding. The similarity in the morphology of the islands and continuous films indicated that island nucleation and coalescence is the growth mechanism for C-face graphene.
In recent years, graphene growth optimization has been one of the key routes towards large-scale, high-quality graphene production. We have measured in-situ residual gas content during epitaxial graphene growth on silicon carbide (SiC) to find detrimental factors of epitaxial graphene growth. The growth conditions in high vacuum and purified argon are compared. The grown epitaxial graphene is studied by Raman scattering mapping and mechanical strain, charge density, number of graphene layers and graphene grain size are evaluated. Charge density and carrier mobility has been studied by Hall effect measurements in van der Pauw configuration. We have identified a major role of chemical reaction of carbon and residual water. The rate of the reaction is lowered when purified argon is used. We also show, that according to time varying gas content, it is preferable to grow graphene at higher temperatures and shorter times. Other sources of growth environment contamination are also discussed. The reaction of water and carbon is discussed to be one of the factors increasing number of defects in graphene. The importance of purified argon and its sufficient flow rate is concluded to be important for high-quality graphene growth as it reduces the rate of undesired chemical reactions and provides more stable and defined growth ambient.
The thermal decomposition of SiC surface provides, perhaps, the most promising method for the epitaxial growth of graphene on a material useful in the electronics platform. Currently, efforts are focused on a reliable method for the growth of large-area, low-strain epitaxial graphene that is still lacking. We report here a novel method for the fast, single-step epitaxial growth of large-area homogeneous graphene film on the surface of SiC(0001) using an infrared CO2 laser (10.6 {mu}m) as the heating source. Apart from enabling extreme heating and cooling rates, which can control the stacking order of epitaxial graphene, this method is cost-effective in that it does not necessitate SiC pre-treatment and/or high vacuum, it operates at low temperature and proceeds in the second time scale, thus providing a green solution to EG fabrication and a means to engineering graphene patterns on SiC by focused laser beams. Uniform, low-strain graphene film is demonstrated by scanning electron microscopy and x-ray photoelectron, secondary ion mass, and Raman spectroscopies. Scalability to industrial level of the method described here appears to be realistic, in view of the high rate of CO2-laser induced graphene growth and the lack of strict sample-environment conditions.
Growth of epitaxial graphene on the C-face of SiC has been investigated. Using a confinement controlled sublimation (CCS) method, we have achieved well controlled growth and been able to observe propagation of uniform monolayer graphene. Surface patterns uncover two important aspects of the growth, i.e. carbon diffusion and stoichiometric requirement. Moreover, a new stepdown growth mode has been discovered. Via this mode, monolayer graphene domains can have an area of hundreds of square micrometers, while, most importantly, step bunching is avoided and the initial uniformly stepped SiC surface is preserved. The stepdown growth provides a possible route towards uniform epitaxial graphene in wafer size without compromising the initial flat surface morphology of SiC.
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