We have clearly discriminated the single-, bilayer-, and multiple-layer graphene (<10 layers) on Si substrate with a 285 nm SiO 2 capping layer by using contrast spectra, which were generated from the reflection light of a white light source. Calculations based on Fresnel's law are in excellent agreement with the experimental results (deviation 2%). The contrast image shows the reliability and efficiency of this new technique. The contrast spectrum is a fast, nondestructive, easy to be carried out, and unambiguous way to identify the numbers of layers of graphene sheet. We provide two easy-to-use methods to determine the number of graphene layers based on contrast spectra: a graphic method and an analytical method. We also show that the refractive index of graphene is different from that of graphite. The results are compared with those obtained using Raman spectroscopy.The recent success in extracting graphite sheets in multiple layers, and even monolayer graphene, from highly ordered pyrolytic graphite (HOPG) using a technique called micromechanical cleavage 1,2 has stimulated great interest in both the fundamental physics study and the potential applications of graphene. 3 Graphene has a two-dimensional (2D) crystal structure, which is the basic building block for other sp 2 carbon nanomaterials, such as nanographite sheets and carbon nanotubes. The peculiar properties of graphene arise from its unique electronic band structure, in which the conduction band touches the valence band at two points (K and K′) 4,5 in the Brillouin zone, and in the vicinity of these points, the electron energy has a linear relationship with the wavevector, E ) pkV f . Therefore, electrons in an ideal graphene sheet behave like massless Dirac-Fermions. 6,7 Some of these unique properties have been observed experimentally 8-21 and many new ideas 22-29 about the fundamental physics and device applications of single-and multiple-layer graphene have been proposed. Presently micromechanical cleavage is still the most effective way to produce high-quality graphene sheets, and a quick and precise method for determining the thickness of graphene sheets is essential for speeding up the research and exploration of graphene. Although atomic force microscopy (AFM) measurement is the most direct way to identify the number of layers of graphene, the method has a very slow throughput and may also cause damage to the crystal lattice during measurement. Furthermore, an instrumental offset of ∼0.5 nm (caused by different interaction forces) always exists, which is even larger than the thickness of a monolayer graphene and data fitting is required to extract the true thickness of graphene sheets. 30 Unconventional quantum Hall effects [8][9][10] are often used to differentiate monolayer and bilayer graphene from multiple layers. However, it is not a practical and efficient way. Researchers have attempted to develop more efficient ways to identify different layers of graphene without destroying the crystal lattice. Raman spectroscopy is a poten...
Graphene field effect transistors commonly comprise graphene flakes lying on SiO(2) surfaces. The gate-voltage dependent conductance shows hysteresis depending on the gate sweeping rate/range. It is shown here that the transistors exhibit two different kinds of hysteresis in their electrical characteristics. Charge transfer causes a positive shift in the gate voltage of the minimum conductance, while capacitive gating can cause the negative shift of conductance with respect to gate voltage. The positive hysteretic phenomena decay with an increase of the number of layers in graphene flakes. Self-heating in a helium atmosphere significantly removes adsorbates and reduces positive hysteresis. We also observed negative hysteresis in graphene devices at low temperature. It is also found that an ice layer on/under graphene has a much stronger dipole moment than a water layer does. Mobile ions in the electrolyte gate and a polarity switch in the ferroelectric gate could also cause negative hysteresis in graphene transistors. These findings improved our understanding of the electrical response of graphene to its surroundings. The unique sensitivity to environment and related phenomena in graphene deserve further studies on nonvolatile memory, electrostatic detection, and chemically driven applications.
Graphene has attracted a lot of interest for fundamental studies as well as for potential applications. Till now, micromechanical cleavage (MC) of graphite has been used to produce high-quality graphene sheets on different substrates. Clear understanding of the substrate effect is important for the potential device fabrication of graphene. Here we report the results of the Raman studies of micromechanically cleaved monolayer graphene on standard SiO 2 (300 nm)/Si, single crystal quartz, Si, glass, polydimethylsiloxane (PDMS), and NiFe. Our data suggests that the Raman features of monolayer graphene are independent of the substrate used; in other words, the effect of substrate on the atomic/electronic structures of graphene is negligible for graphene made by MC. On the other hand, epitaxial monolayer graphene (EMG) on SiC substrate is also investigated. Significant blueshift of Raman bands is observed, which is attributed to the interaction of the graphene sheet with the substrate, resulting in the change of lattice constant and also the electronic structure.
Wafer-scale single-crystalline graphene monolayers are highly sought after as an ideal platform for electronic and other applications. At present, state-of-the-art growth methods based on chemical vapour deposition allow the synthesis of one-centimetre-sized single-crystalline graphene domains in ∼12 h, by suppressing nucleation events on the growth substrate. Here we demonstrate an efficient strategy for achieving large-area single-crystalline graphene by letting a single nucleus evolve into a monolayer at a fast rate. By locally feeding carbon precursors to a desired position of a substrate composed of an optimized Cu-Ni alloy, we synthesized an ∼1.5-inch-large graphene monolayer in 2.5 h. Localized feeding induces the formation of a single nucleus on the entire substrate, and the optimized alloy activates an isothermal segregation mechanism that greatly expedites the growth rate. This approach may also prove effective for the synthesis of wafer-scale single-crystalline monolayers of other two-dimensional materials.
Hexagonal boron nitride (h-BN) has attracted significant attention because of its superior properties as well as its potential as an ideal dielectric layer for graphene-based devices. The h-BN films obtained via chemical vapour deposition in earlier reports are always polycrystalline with small grains because of high nucleation density on substrates. Here we report the successful synthesis of large single-crystal h-BN grains on rational designed Cu-Ni alloy foils. It is found that the nucleation density can be greatly reduced to 60 per mm 2 by optimizing Ni ratio in substrates. The strategy enables the growth of single-crystal h-BN grains up to 7,500 mm 2 , approximately two orders larger than that in previous reports. This work not only provides valuable information for understanding h-BN nucleation and growth mechanisms, but also gives an effective alternative to exfoliated h-BN as a high-quality dielectric layer for large-scale nanoelectronic applications.
Graphene has many unique properties which make it an attractive material for fundamental study as well as for potential applications. In this paper, we report the first experimental study of process-induced defects and stress in graphene using Raman spectroscopy and imaging. While defects lead to the observation of defect-related Raman bands, stress causes shift in phonon frequency. A compressive stress (as high as 2.1 GPa) was induced in graphene by depositing a 5 nm SiO(2) followed by annealing, whereas a tensile stress ( approximately 0.7 GPa) was obtained by depositing a thin silicon capping layer. In the former case, both the magnitude of the compressive stress and number of graphene layers can be controlled or modified by the annealing temperature. As both the stress and thickness affect the physical properties of graphene, this study may open up the possibility of utilizing thickness and stress engineering to improve the performance of graphene-based devices. Local heating techniques may be used to either induce the stress or reduce the thickness selectively.
To grow precisely aligned graphene on h-BN without metal catalyst is extremely important, which allows for intriguing physical properties and devices of graphene/h-BN hetero-structure to be studied in a controllable manner. In this report, such hetero-structures were fabricated and investigated by atomic resolution scanning probe microscopy. Moiré patterns are observed and the sensitivity of moiré interferometry proves that the graphene grains can align precisely with the underlying h-BN lattice within an error of less than 0.05°. The occurrence of moiré pattern clearly indicates that the graphene locks into h-BN via van der Waals epitaxy with its interfacial stress greatly released. It is worthy to note that the edges of the graphene grains are primarily oriented along the armchair direction. The field effect mobility in such graphene flakes exceeds 20,000 cm2·V−1·s−1 at ambient condition. This work opens the door of atomic engineering of graphene on h-BN, and sheds light on fundamental research as well as electronic applications based on graphene/h-BN hetero-structure.
The effect of vacuum annealing on the properties of graphene is investigated by using Raman spectroscopy and electrical measurement. Heavy hole doping on graphene with concentration as high as 1.5 × 10 13 cm −2 is observed after vacuum annealing and exposed to an air ambient. This doping is due to the H 2 O and O 2 adsorption on graphene, and graphene is believed to be more active to molecular adsorption after annealing. Such observation calls for special attention in the process of fabricating graphene-based electronic devices and gas sensors. On the other hand, because the quality of graphene remains high after the doping process, this would be an efficient and controllable method to introduce heavy doping in graphene, which would greatly help on its application in future electronic devices.
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