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Register a new userCharge spill-out and work function of few-layer graphene on SiC(0001)
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We report on the charge spill-out and work function of epitaxial few-layer graphene on 6H-SiC(0001). Experiments from high-resolution, energy-filtered X-ray photoelectron emission microscopy (XPEEM) are combined with ab initio Density Functional Theory calculations using a relaxed interface model. Work function values obtained from theory and experiments are in qualitative agreement, reproducing the previously observed trend of increasing work function with each additional graphene plane. Electrons transfer at the SiC/graphene interface through a buffer layer causes an interface dipole moment which is at the origin of the graphene work function modulation. The total charge transfer is independent of the number of graphene layers, and is consistent with the constant binding energy of the SiC component of the C 1s core-level measured by XPEEM. Charge leakage into vacuum depends on the number of graphene layers explaining why the experimental, layer-dependent C 1s-graphene core-level binding energy shift does not rigidly follow that of the work function. Thus, a combination of charge transfer at the SiC/graphene interface and charge spill-out into vacuum resolves the apparent discrepancy between the experimental work function and C1s binding energy.
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This paper has been withdrawn due to the adherance to the double submission policies of a refereed journal. Our apologies.
We report a Raman study of the so-called buffer layer with $(6sqrt3times6sqrt3)R30^{circ}$ periodicity which forms the intrinsic interface structure between epitaxial graphene and SiC(0001). We show that this interface structure leads to a nonvanishing signal in the Raman spectrum at frequencies in the range of the D- and G-band of graphene and discuss its shape and intensity. Ab-initio phonon calculations reveal that these features can be attributed to the vibrational density of states of the buffer-layer.
We present a structural analysis of the graphene-4HSiC(0001) interface using surface x-ray reflectivity. We find that the interface is composed of an extended reconstruction of two SiC bilayers. The interface directly below the first graphene sheet is an extended layer that is more than twice the thickness of a bulk SiC bilayer (~1.7A compared to 0.63A). The distance from this interface layer to the first graphene sheet is much smaller than the graphite interlayer spacing but larger than the same distance measured for graphene grown on the (000-1) surface, as predicted previously by ab intio calculations.
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.
The intercalation of epitaxial graphene on SiC(0001) with Ca has been studied extensively, yet precisely where the Ca resides remains elusive. Furthermore, the intercalation of Mg underneath epitaxial graphene on SiC(0001) has not been reported. Here, we use low energy electron diffraction, x-ray photoelectron spectroscopy, secondary electron cut-off photoemission and scanning tunneling microscopy to elucidate the physical and electronic structure of both Ca- and Mg-intercalated epitaxial graphene on 6H-SiC(0001). We find that Ca intercalates underneath the buffer layer and bonds to the Si-terminated SiC surface, breaking the C-Si bonds of the buffer layer i.e. freestanding the buffer layer to form Ca-intercalated quasi-freestanding bilayer graphene (Ca-QFSBLG). The situation is similar for the Mg-intercalation of epitaxial graphene on SiC(0001), where an ordered Mg-terminated reconstruction at the SiC surface and Mg bonds to the Si-terminated SiC surface are formed, resulting in Mg-intercalated quasi-freestanding bilayer graphene (Mg-QFSBLG). Ca-intercalation underneath the buffer layer has not been considered in previous studies of Ca-intercalated epitaxial graphene. Furthermore, we find no evidence that either Ca or Mg intercalates between graphene layers. However, we do find that both Ca-QFSBLG and Mg-QFSBLG exhibit very low workfunctions of 3.68 and 3.78 eV, respectively, indicating high n-type doping. Upon exposure to ambient conditions, we find Ca-QFSBLG degrades rapidly, whereas Mg-QFSBLG remains remarkably stable.
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