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Register a new userFormation of Graphene atop a Si adlayer on the C-face of SiC
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The structure of the SiC(000-1) surface, the C-face of the {0001} SiC surfaces, is studied as a function of temperature and of pressure in a gaseous environment of disilane (Si2H6). Various surface reconstructions are observed, both with and without the presence of an overlying graphene layer (which spontaneously forms at sufficiently high temperatures). Based on cross-sectional scanning transmission electron microscopy measurements, the interface structure that forms in the presence of the graphene is found to contain 1.4 - 1.7 monolayers (ML) of Si, a somewhat counter-intuitive result since, when the graphene forms, the system is actually under C-rich conditions. Using ab initio thermodynamics, it is demonstrated that there exists a class of Si-rich surfaces containing about 1.3 ML of Si that are stable on the surface (even under C-rich conditions) at temperatures above about 400 K. The structures that thus form consist of Si adatoms atop a Si adlayer on the C-face of SiC, with or without the presence of overlying graphene.
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The morphology of graphene on SiC {0001} surfaces formed in various environments including ultra-high vacuum, 1 atm of argon, and 10^-6 to 10^-4 Torr of disilane is studied by atomic force microscopy, low-energy electron microscopy, and Raman spectroscopy. The graphene is formed by heating the surface to 1100 - 1600 C, which causes preferential sublimation of the Si atoms. The argon atmosphere or the background of disilane decreases the sublimation rate so that a higher graphitization temperature is required, thus improving the morphology of the films. For the (0001) surface, large areas of monolayer-thick graphene are formed in this way, with the size of these areas depending on the miscut of the sample. Results on the (000-1) surface are more complex. This surface graphitizes at a lower temperature than for the (0001) surface and consequently the growth is more three-dimensional. In an atmosphere of argon the morphology becomes even worse, with the surface displaying markedly inhomogeneous nucleation, an effect attributed to unintentional oxidation of the surface during graphitization. Use of a disilane environment for the (000-1) surface is found to produce improved morphology, with relatively large areas of monolayer-thick graphene.
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.
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.
We present electronic structure calculations of few-layer epitaxial graphene nanoribbons on SiC(0001). Trough an atomistic description of the graphene layers and the substrate within the extended H{u}ckel Theory and real/momentum space projections we argue that the role of the heterostructures interface becomes crucial for the conducting capacity of the studied systems. The key issue arising from this interaction is a Fermi level pinning effect introduced by dangling interface bonds. Such phenomenon is independent from the width of the considered nanostructures, compromising the importance of confinement in these systems.
The results of micro-Raman scattering measurements performed on three different ``graphitic materials: micro-structured disks of highly oriented pyrolytic graphite, graphene multi-layers thermally decomposed from carbon terminated surface of 4H-SiC and an exfoliated graphene monolayer are presented. Despite its multi-layer character, most parts of the surface of the graphitized SiC substrates shows a single-component, Lorentzian shape, double resonance Raman feature in striking similarity to the case of a single graphene monolayer. Our observation suggests a very weak electronic coupling between graphitic layers on the SiC surface, which therefore can be considered to be graphene multi-layers with a simple (Dirac-like) band structure.
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