We demonstrate the growth of high quality graphene layers by chemical vapor deposition (CVD) on insulating and conductive SiC substrates. This method provides key advantages over the well-developed epitaxial graphene growth by Si sublimation that has been known for decades. (1) CVD growth is much less sensitive to SiC surface defects resulting in high electron mobilities of ∼1800 cm(2)/(V s) and enables the controlled synthesis of a determined number of graphene layers with a defined doping level. The high quality of graphene is evidenced by a unique combination of angle-resolved photoemission spectroscopy, Raman spectroscopy, transport measurements, scanning tunneling microscopy and ellipsometry. Our measurements indicate that CVD grown graphene is under less compressive strain than its epitaxial counterpart and confirms the existence of an electronic energy band gap. These features are essential for future applications of graphene electronics based on wafer scale graphene growth.
We show that optical reflection microscopy is a reliable method to simultaneously locate and count graphene layers deposited on bulk, transparent substrates such as soda-lime glass. The visible contrast in optical reflection versus graphene layer number is resolvable on bulk substrates. A simple Fresnel theory based on the universal optical conductance of graphene layers accurately models optical reflection images taken at a wavelength of 550±5 nm. We directly count one to nine layers of graphene using reflection microscopy.
The optical reflection contrast and optical transmission contrast of graphitic films on glass ranging in thickness from a monolayer to the limit of bulk graphite have been experimentally measured. For samples with more than 10 graphene layers where optical contrast quantization becomes difficult to observe, atomic force microscopy was used to measure the sample thickness. The visible optical reflection and transmission of thin graphitic films is found to depend strongly on the real component of the optical conductance per graphene layer, and comparatively weakly on the imaginary component of optical conductance. This observation in part explains the significant variation in the refractive index of graphene and graphite reported in the literature to date. Spectroscopic measurements reveal a strong dispersion in the optical conductance of even a 10 layer film, consistent with an imaginary conductance arising from virtual transitions at the band edges of the pi and sigma bands at the M and Gamma points, respectively.
Composites of tin nanoparticles (Sn NP) and graphene are candidate materials for high capacity and mechanically stable negative electrodes in rechargeable Li ion batteries. A uniform dispersion of Sn NP with controlled size is necessary to obtain high electrochemical performance. We show that the nucleation of Sn particles on highly ordered pyrolitic graphite (HOPG) from solution can be controlled by functionalizing the HOPG surface by aryl groups prior to Sn deposition. On the contrary, we observe heterogeneous deposition of micrometer sized Sn islands on HOPG subjected to oxidation prior to deposition in the same conditions. We demonstrate that functional groups act as nucleation sites for Sn NP nucleation, and that homogeneous nucleation of small particles can be achieved by combining surface functionalization with diazonium chemistry and appropriate stabilizers in solution.
The quantum Hall effect is observed in a two-dimensional electron gas formed in millimeter-scale hydrogenated graphene, with a mobility less than 10 cm2/V·s and corresponding Ioffe-Regel disorder parameter (k(F)λ)(-1) ≫ 1. In a zero magnetic field and low temperatures, the hydrogenated graphene is insulating with a two-point resistance of the order of 250h/e2. The application of a strong magnetic field generates a negative colossal magnetoresistance, with the two-point resistance saturating within 0.5% of h/2e2 at 45 T. Our observations are consistent with the opening of an impurity-induced gap in the density of states of graphene. The interplay between electron localization by defect scattering and magnetic confinement in two-dimensional atomic crystals is discussed.
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