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Register a new userUltrapure Multilayer Graphene in Bromine Intercalated Graphite
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We investigate the optical properties of bromine intercalated highly orientated pyrolytic graphite (Br-HOPG) and provide a novel interpretation of the data. We observe new absorption features below 620 meV which are absent in the absorption spectrum of graphite. Comparing our results with those of theoretical studies on graphite, single and bilayer graphene as well as recent optical studies of multilayer graphene, we conclude that Br-HOPG contains the signatures of ultrapure bilayer, single layer graphene, and graphite. The observed supermetallic conductivity of Br-HOPG is identified with the presence of very high mobility (~ 121,000 cm2V-1s-1 at room temperature and at very high carrier density) multilayer graphene components in our sample. This could provide a new avenue for single and multilayer graphene research.
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Exposure of highly oriented pyrolytic graphite to bromine vapor gives rise to in-plane charge conductivities which increase monotonically with intercalation time toward values (for ~6 at% Br) that are significantly higher than Cu at temperatures down to 5 K. Magnetotransport, optical reflectivity and magnetic susceptibility measurements confirm that the Br dopes the graphene sheets with holes while simultaneously increasing the interplanar separation. The increase of mobility (~ 5E4 cm^2/Vs at T=300 K) and resistance anisotropy together with the reduced diamagnetic susceptibility of the intercalated samples suggests that the observed supermetallic conductivity derives from a parallel combination of weakly-coupled hole-doped graphene sheets.
A method to produce suspensions of graphene sheets by combining solution-based bromine intercalation and mild sonochemical exfoliation is presented. Ultrasonic treatment of graphite in water leads to the formation of suspensions of graphite flakes. The delamination is dramatically improved by intercalation of bromine into the graphite before sonication. The bromine intercalation was verified by Raman spectroscopy as well as by x-ray photoelectron spectroscopy (XPS), and density functional theory (DFT) calculations show an almost ten times lower interlayer binding energy after introducing Br2 into the graphite. Analysis of the suspended material by transmission and scanning electron microscopy (TEM and SEM) revealed a significant content of few-layer graphene with sizes up to 30 $mu$m, corresponding to the grain size of the starting material.
There has been a lot of excitement around the observation of superconductivity in twisted bilayer graphene, associated to flat bands close to the Fermi level. Such correlated electronic states also occur in multilayer rhombohedral stacked graphene (RG), which has been receiving increasing attention in the last years. In both natural and artificial samples however, multilayer stacked Bernal graphene (BG) occurs more frequently, making it desirable to determine what is their relative stability and under which conditions RG might be favored. Here, we study the energetics of BG and RG in bulk and also multilayer stacked graphene using first-principles calculations. It is shown that the electronic temperature, not accounted for in previous studies, plays a crucial role in determining which phase is preferred. We also show that the low energy states at room temperature consist of BG, RG and mixed BG-RG systems with a particular type of interface. Energies of all stacking sequences (SSs) are calculated for N = 12 layers, and an Ising model is used to fit them, which can be used for larger N as well. In this way, the ordering of low energy SSs can be determined and analyzed in terms of a few parameters. Our work clarifies inconsistent results in the literature, and sets the basis to studying the effect of external factors on the stability of multilayer graphene systems in first principles calculations.
The 2D Fermi surface of 1st stage PdAl2Cl8 acceptor-type graphite intercalation compounds (GICs) has been investigated using the Shubnikov-de Haas (SdH) effect. One fundamental frequency is observed, the angular variation of which confirms its strongly 2D nature, as previously found through electrical conductivity measurements. The energy spectrum can be described by the 2D band structure model proposed by Blinowski et al. We obtain the following parameter values: intraplane C-C interaction energy gamma_0 = 2.7 eV, Fermi energy E_F = -1.1 eV and carrier density n_SdH= 1.1x10^27 m^-3. Some fewer details are presented on stage 2 and 3 materials.
The visibility of graphene sheets on different types of substrates has been investigated both theoretically and experimentally. Although single layer graphene is observable on various types of dielectrics under an optical microscope, it is invisible when it is placed directly on most of the semiconductor and metallic substrates. We show that coating of a resist layer with optimum thickness is an effective way to enhance the contrast of graphene on various types of substrates and makes single layer graphene visible on most semiconductor and metallic substrates. Experiments have been performed to verify the results on quartz and NiFe-coated Si substrates. The results obtained will be useful for fabricating graphene-based devices on various types of substrates for electronics, spintronics and optoelectronics applications.
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