Ultralow noise field-effect transistor from multilayer graphene

We present low-frequency electrical resistance fluctuations, or noise, in graphene-based field-effect devices with varying number of layers. In single-layer devices, the noise magnitude decreases with increasing carrier density, which behaved oppositely in the devices with two or larger number of layers accompanied by a suppression in noise magnitude by more than two orders in the latter case. This behavior can be explained from the influence of external electric field on graphene band structure, and provides a simple transport-based route to isolate single-layer graphene devices from those with multiple layers. ©2009 American Institute of Physics

The shear mode of multilayer graphene

The quest for materials capable of realizing the next generation of electronic and photonic devices continues to fuel research on the electronic, optical and vibrational properties of graphene. Few-layer graphene (FLG) flakes with less than ten layers each show a distinctive band structure. Thus, there is an increasing interest in the physics and applications of FLGs. Raman spectroscopy is one of the most useful and versatile tools to probe graphene samples. Here, we uncover the interlayer shear mode of FLGs, ranging from bilayer graphene (BLG) to bulk graphite, and suggest that the corresponding Raman peak measures the interlayer coupling. This peak scales from ∼43cm -1 in bulk graphite to ∼31cm -1 in BLG. Its low energy makes it sensitive to near-Dirac point quasiparticles. Similar shear modes are expected in all layered materials, providing a direct probe of interlayer interactions. © 2012 Macmillan Publishers Limited. All rights reserved.

Self-assembled multilayer graphene oxide membrane and carbon nanotubes synthesized using a rare form of natural graphite

The fabrication of flexible multilayer graphene oxide (GO) membrane and carbon nanotubes (CNTs) using a rare form of high-purity natural graphite, vein graphite, is reported for the first time. Graphite oxide is synthesized using vein graphite following Hummer's method. By facilitating functionalized graphene sheets in graphite oxide to self-assemble, a multilayer GO membrane is fabricated. Electric arc discharge is used to synthesis CNTs from vein graphite. Both multilayer GO membrane and CNTs are investigated using microscopy and spectroscopy experiments, i.e., scanning electron microscopy (SEM), atomic force microscopy (AFM), high-resolution transmission electron microscopy (HRTEM), Fourier transform infrared spectroscopy (FTIR), X-ray diffraction (XRD), thermogravimetric analysis (TGA), core level photoelectron spectroscopy, and C K-edge X-ray absorption spectroscopy (NEXAFS), to characterize their structural and topographical properties. Characterization of vein graphite using different techniques reveals that it has a large number of crystallites, hence the large number of graphene sheets per crystallite, preferentially oriented along the (002) plane. NEXAFS and core level spectra confirm that vein graphite is highly crystalline and pure. Fourier transform infrared (FT-IR) and C 1s core level spectra show that oxygen functionalities (-C-OH, -CO,-C-O-C-) are introduced into the basal plane of graphite following chemical oxidation. Carbon nanotubes are produced from vein graphite through arc discharge without the use of any catalyst. HRTEM confirm that multiwalled carbon nanotube (MWNTs) are produced with the presence of some structure in the central pipe. A small percentage of single-walled nanotubes (SWNTs) are also produced simultaneously with MWNTs. Spectroscopic and microscopic data are further discussed here with a view to using vein graphite as the source material for the synthesis of carbon nanomaterials. © 2013 American Chemical Society.

Observation of active sites for oxygen reduction reaction on nitrogen-doped multilayer graphene

Active sites and the catalytic mechanism of nitrogen-doped graphene in an oxygen reduction reaction (ORR) have been extensively studied but are still inconclusive, partly due to the lack of an experimental method that can detect the active sites. It is proposed in this report that the active sites on nitrogen-doped graphene can be determined via the examination of its chemical composition change before and after ORR. Synchrotron-based X-ray photoelectron spectroscopy analyses of three nitrogen-doped multilayer graphene samples reveal that oxygen reduction intermediate OH(ads), which should chemically attach to the active sites, remains on the carbon atoms neighboring pyridinic nitrogen after ORR. In addition, a high amount of the OH(ads) attachment after ORR corresponds to a high catalytic efficiency and vice versa. These pinpoint that the carbon atoms close to pyridinic nitrogen are the main active sites among the different nitrogen doping configurations.

Quantum spin Hall phase in multilayer graphene

The so-called quantum spin Hall phase is a topologically nontrivial insulating phase that is predicted to appear in graphene and graphenelike systems. In this paper we address the question of whether this topological property persists in multilayered systems. We consider two situations: purely multilayer graphene and heterostructures where graphene is encapsulated by trivial insulators with a strong spin-orbit coupling. We use a four-orbital tight-binding model that includes full atomic spin-orbit coupling and we calculate the Z2 topological invariant of the bulk states as well as the edge states of semi-infinite crystals with armchair termination. For homogeneous multilayers we find that even when the spin-orbit interaction opens a gap for all possible stackings, only those with an odd number of layers host gapless edge states while those with an even number of layers are trivial insulators. For heterostructures where graphene is encapsulated by trivial insulators, it turns out that interlayer coupling is able to induce a topological gap whose size is controlled by the spin-orbit coupling of the encapsulating materials, indicating that the quantum spin Hall phase can be induced by proximity to trivial insulators.

Mechanical properties of graphene : effects of layer number, temperature and isotope

Herein the mechanical properties of graphene, including Young’s modulus, fracture stress and fracture strain have been investigated by molecular dynamics simulations. The simulation results show that the mechanical properties of graphene are sensitive to the temperature changes but insensitive to the layer numbers in the multilayer graphene. Increasing temperature exerts adverse and significant effects on the mechanical properties of graphene. However, the adverse effect produced by the increasing layer number is marginal. On the other hand, isotope substitutions in graphene play a negligible role in modifying the mechanical properties of graphene.

Electrochemically exfoliated graphene for electrode films : effect of graphene flake thickness on the sheet resistance and capacitive properties

We present an electrochemical exfoliation method to produce controlled thickness graphene flakes by ultrasound assistance. Bilayer graphene flakes are dominant in the final product by using sonication during the electrochemical exfoliation process, while without sonication the product contains a larger percentage of four-layer graphene flakes. Graphene sheets prepared by using the two procedures are processed into films to measure their respective sheet resistance and optical transmittance. Solid-state electrolyte supercapacitors are made using the two types of graphene films. Our study reveals that films with a higher content of multilayer graphene flakes are more conductive, and their resistance is more easily reduced by thermal annealing, making them suitable as transparent conducting films. The film with higher content of bilayer graphene flakes shows instead higher capacitance when used as electrode in a supercapacitor.

Suppressed thermal conductivity of bilayer graphene with vacancy-initiated linkages

Through larger-scale molecular dynamics simulations, we investigated the impacts from vacancy-initiated linkages on the thermal conductivity of bilayer graphene sheets (of size L × W = 24.5 nm × 3.7 nm). Three different interlayer linkages, including divacancy bridging, “spiro” interstitial bridging and Frenkel pair defects, are considered. It is found that the presence of interlayer linkages induces a significant degradation in the thermal conductivity of the bilayer graphene sheet. The degradation is strongly dependent on the interlayer linkage type, concentration and location. More importantly, the linkages that contain vacancies lead to more severe suppression of the thermal conductivity, in agreement with theoretical predictions that vacancies induce strong phonon scattering. Our finding provides useful guidelines for the application of multilayer graphene sheets in practical thermal management.

Effect of covalent functionalisation on thermal transport across graphene-polymer interfaces

This paper is concerned with the interfacial thermal resistance for polymer composites reinforced by various covalently functionalised graphene. By using molecular dynamics simulations, the obtained results show that the covalent functionalisation in graphene plays a significant role in reducing the graphene-paraffin interfacial thermal resistance. This reduction is dependent on the coverage and type of functional groups. Among the various functional groups, butyl is found to be the most effective in reducing the interfacial thermal resistance, followed by methyl, phenyl and formyl. The other functional groups under consideration such as carboxyl, hydroxyl and amines are found to produce negligible reduction in the interfacial thermal resistance. For multilayer graphene with a layer number up to four, the interfacial thermal resistance is insensitive to the layer number. The effects of the different functional groups and the layer number on the interfacial thermal resistance are also elaborated using the vibrational density of states of the graphene and the paraffin matrix. The present findings provide useful guidelines in the application of functionalised graphene for practical thermal management.

Microscopic Mechanism of 1/f Noise in Graphene: Role of Energy Band Dispersion

A distinctive feature of single-layer graphene is the linearly dispersive energy bands, which in the case of multilayer graphene become parabolic. A simple electrical transport-based probe to differentiate between these two band structures will be immensely valuable, particularly when quantum Hall measurements are difficult, such as in chemically synthesized graphene nanoribbons. Here we show that the flicker noise, or the 1/f noise, in electrical resistance is a sensitive and robust probe to the band structure of graphene. At low temperatures, the dependence of noise magnitude on the carrier density was found to be opposite for the linear and parabolic bands. We explain our data with a comprehensive theoretical model that clarifies several puzzling issues concerning the microscopic origin of flicker noise in graphene field-effect transistors (GraFET).

The parameter space of graphene chemical vapor deposition on polycrystalline Cu

A systematic study of the parameter space of graphene chemical vapor deposition (CVD) on polycrystalline Cu foils is presented, aiming at a more fundamental process rationale in particular regarding the choice of carbon precursor and mitigation of Cu sublimation. CH 4 as precursor requires H 2 dilution and temperatures ≥1000 °C to keep the Cu surface reduced and yield a high-quality, complete monolayer graphene coverage. The H 2 atmosphere etches as-grown graphene; hence, maintaining a balanced CH 4/H 2 ratio is critical. Such balance is more easily achieved at low-pressure conditions, at which however Cu sublimation reaches deleterious levels. In contrast, C 6H 6 as precursor requires no reactive diluent and consistently gives similar graphene quality at 100-150 °C lower temperatures. The lower process temperature and more robust processing conditions allow the problem of Cu sublimation to be effectively addressed. Graphene formation is not inherently self-limited to a monolayer for any of the precursors. Rather, the higher the supplied carbon chemical potential, the higher the likelihood of film inhomogeneity and primary and secondary multilayer graphene nucleation. For the latter, domain boundaries of the inherently polycrystalline CVD graphene offer pathways for a continued carbon supply to the catalyst. Graphene formation is significantly affected by the Cu crystallography; i.e., the evolution of microstructure and texture of the catalyst template form an integral part of the CVD process. © 2012 American Chemical Society.

Experimental demonstration of a transparent graphene millimetre wave absorber with 28% fractional bandwidth at 140 GHz.

The development of transparent radio-frequency electronics has been limited, until recently, by the lack of suitable materials. Naturally thin and transparent graphene may lead to disruptive innovations in such applications. Here, we realize optically transparent broadband absorbers operating in the millimetre wave regime achieved by stacking graphene bearing quartz substrates on a ground plate. Broadband absorption is a result of mutually coupled Fabry-Perot resonators represented by each graphene-quartz substrate. An analytical model has been developed to predict the absorption performance and the angular dependence of the absorber. Using a repeated transfer-and-etch process, multilayer graphene was processed to control its surface resistivity. Millimetre wave reflectometer measurements of the stacked graphene-quartz absorbers demonstrated excellent broadband absorption of 90% with a 28% fractional bandwidth from 125-165 GHz. Our data suggests that the absorbers' operation can also be extended to microwave and low-terahertz bands with negligible loss in performance.

Spatio-temporal resolution studies on a highly compact ultrafast electron diffractometer

Time-resolved diffraction with femtosecond electron pulses has become a promising technique to directly provide insights into photo induced primary dynamics at the atomic level in molecules and solids. Ultrashort pulse duration as well as extensive spatial coherence are desired, however, space charge effects complicate the bunching of multiple electrons in a single pulse.Weexperimentally investigate the interplay between spatial and temporal aspects of resolution limits in ultrafast electron diffraction (UED) on our highly compact transmission electron diffractometer. To that end, the initial source size and charge density of electron bunches are systematically manipulated and the resulting bunch properties at the sample position are fully characterized in terms of lateral coherence, temporal width and diffracted intensity.Weobtain a so far not reported measured overall temporal resolution of 130 fs (full width at half maximum) corresponding to 60 fs (root mean square) and transversal coherence lengths up to 20 nm. Instrumental impacts on the effective signal yield in diffraction and electron pulse brightness are discussed as well. The performance of our compactUEDsetup at selected electron pulse conditions is finally demonstrated in a time-resolved study of lattice heating in multilayer graphene after optical excitation.