Transient absorption microscopy was employed to image charge carrier dynamics in epitaxial multilayer graphene. The carrier cooling exhibited a biexponential decay that showed a significant dependence on carrier density. The fast and slow relaxation times were assigned to coupling between electrons and optical phonon modes and the hot phonon effect, respectively. The limiting value of the slow relaxation time at high pump intensity reflects the lifetime of the optical phonons. Significant spatial heterogeneity in the dynamics was observed due to differences in coupling between graphene layers and the substrate.

The morphology of graphene formed on the ( 1 000 ) surface (the C-face) and the (0001) surface (the Si-face) of SiC, by annealing in ultra-high vacuum or in an argon environment, is studied by atomic force microscopy (AFM) and low-energy electron microscopy (LEEM). The graphene forms due to preferential sublimation of Si from the surface. In vacuum, this sublimation occurs much more rapidly for the C-face than the Si-face, so that 150°C lower annealing temperatures are required for the C-face to obtain films of comparable thickness. The evolution of the morphology as a function of graphene thickness is examined, revealing significant differences between the C-face and the Si-face. For annealing near 1320°C, graphene films of about 2 monolayers (ML) thickness are formed on the Si-face, but 16 ML is found for the C-face. In both cases, step bunches are formed on the surface and the films grow continuously (carpet-like) over the step bunches. For the Si-face in particular, layer-by-layer growth of the graphene is observed in areas between the step bunches. At 1170°C, for the C-face, a more 3-dimensional type of growth is found. The average thickness is then about 4 ML, but with a wide variation in local thickness (2 -7 ML) over the surface. The spatial arrangement of constant-thickness domains are found to be correlated with step bunches on the surface, which form in a more restricted manner than at 1320°C. It is argued that these domains are somewhat disconnected, so that no strong driving force for planarization of the film exists. In a 1-atm argon environment, permitting higher growth temperatures, the graphene morphology for the Si-face is found to become more layer-by-layer-like even for graphene thickness as low as 1 ML. However, for the C-face the morphology becomes much worse, with the surface displaying markedly inhomogeneous nucleation of the graphene. It is demonstrated that these surfaces are unintentionally oxidized, which accounts for the inhomogeneous growth.

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The formation of epitaxial graphene on SiC(0001) surfaces is studied using atomic force microscopy, Auger electron spectroscopy, electron diffraction, Raman spectroscopy, and electrical measurements. Starting from hydrogenannealed surfaces, graphene formation by vacuum annealing is observed to begin at about 1150°C, with the overall step-terrace arrangement of the surface being preserved but with significant roughness (pit formation) on the terraces. At higher temperatures near 1250°C, the step morphology changes, with the terraces becoming more compact. At 1350°C and above, the surface morphology changes into relatively large flat terraces separated by step bunches. Features believed to arise from grain boundaries in the graphene are resolved on the terraces, as are fainter features attributed to atoms at the buried graphene/SiC interface.

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 ( 1 000 ) 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 ( 1 000 ) surface is found to produce improved morphology, with relatively large areas of monolayer-thick graphene.