We present a new fabrication method for epitaxial graphene on SiC which enables the growth of ultrasmooth defect-and bilayer-free graphene sheets with an unprecedented reproducibility, a necessary prerequisite for wafer-scale fabrication of high quality graphene-based electronic devices. The inherent but unfavorable formation of high SiC surface terrace steps during high temperature sublimation growth is suppressed by rapid formation of the graphene buffer layer which stabilizes the SiC surface. The enhanced nucleation is enforced by decomposition of polymer adsorbates which act as a carbon source. With most of the steps well below 0.75 nm pure monolayer graphene without bilayer inclusions is formed with lateral dimensions only limited by the size of the substrate. This makes the polymer assisted sublimation growth technique the most promising method for commercial wafer scale epitaxial graphene fabrication. The extraordinary electronic quality is evidenced by quantum resistance metrology at 4.2 K with until now unreached precision and high electron mobilities on mm scale devices. Main TextThe success of graphene as a basis for new applications depends crucially on the reliability of the available technologies to fabricate large areas of homogenous high quality graphene layers. Epitaxial growth on metals as well as on SiC substrates is employed with specific benefits and drawbacks.Single graphene layers epitaxially grown on SiC offer a high potential for electronic device applications. They combine excellent properties, e.g. high electron mobilities, with the opportunity for wafer-scale fabrication and direct processing on semi-insulating substrates without the need to transfer the graphene to a suitable substrate (Avouris & Dimitrakopoulos 2012). Some progress has been achieved during the recent years. In particular, high temperature sublimation growth under Ar atmosphere (Virojanadara et al. 2008),(Emtsev et al. 2009 or by confinement control (Heer et al. 2011), (Real et al. 2012) was a breakthrough for synthesizing large-area graphene on SiC substrates.The coverage of graphene bilayers could be reduced from wide stripes formed along the terraces to small micrometer-sized bilayer patches (Virojanadara et al. 2009). Further it was found that beyond pure sublimation growth from SiC graphene formation can be assisted by additional carbon supply from external sources (Al-Temimy et al. 2009;Moreau et al. 2010). In particular, by using propane in
We report on electronic transport measurements in rotational square probe configuration in combination with scanning tunneling potentiometry of epitaxial graphene monolayers which were fabricated by polymer-assisted sublimation growth on SiC substrates. The absence of bilayer graphene on the ultralow step edges of below 0.75 nm scrutinized by atomic force microscopy and scanning tunneling microscopy result in a not yet observed resistance isotropy of graphene on 4H- and 6H-SiC(0001) substrates as low as 2%. We combine microscopic electronic properties with nanoscale transport experiments and thereby disentangle the underlying microscopic scattering mechanism to explain the remaining resistance anisotropy. Eventually, this can be entirely attributed to the resistance and the number of substrate steps which induce local scattering. Thereby, our data represent the ultimate limit for resistance isotropy of epitaxial graphene on SiC for the given miscut of the substrate.
Graphene, the first true two-dimensional material still reveals the most remarkable transport properties among the growing class of two-dimensional materials. Although many studies have investigated fundamental scattering processes, the surprisingly large variation in the experimentally determined resistances associated with a localized defect is still an open issue. Here, we quantitatively investigate the local transport properties of graphene prepared by polymer assisted sublimation growth (PASG) using scanning tunneling potentiometry. PASG graphene is characterized by a spatially homogeneous current density, which allows to analyze variations in the local electrochemical potential with high precision. We utilize this possibility by examining the local sheet resistance finding a significant variation of up to 270% at low temperatures. We identify a correlation of the sheet resistance with the stacking sequence of the 6H-SiC substrate as well as with the distance between the graphene
In this study, we first show that the argon flow during epitaxial graphene growth is an important parameter to control the quality of the buffer and the graphene layer. Atomic force microscopy (AFM) and low-energy electron diffraction (LEED) measurements reveal that the decomposition of the SiC substrate strongly depends on the Ar mass flow rate while pressure and temperature are kept constant. Our data are interpreted by a model based on the competition of the SiC decomposition rate, controlled by the Ar flow, with a uniform graphene buffer layer formation under the equilibrium process at the SiC surface. The proper choice of a set of growth parameters allows the growth of defect-free, ultra-smooth and coherent graphene-free buffer layer and bilayer-free monolayer graphene sheets which can be transformed into large-area high-quality quasi-freestanding monolayer and bilayer graphene (QFMLG and QFBLG) by hydrogen intercalation. AFM, scanning tunneling microscopy (STM), Raman spectroscopy and electronic transport measurements underline the excellent homogeneity of the resulting quasi-freestanding layers. Electronic transport measurements in four-point probe configuration reveal a homogeneous low resistance anisotropy on both μm-and mm scales.
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