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Showing papers on "Bilayer graphene published in 2012"


Journal ArticleDOI
11 Oct 2012-Nature
TL;DR: This work reviews recent progress in graphene research and in the development of production methods, and critically analyse the feasibility of various graphene applications.
Abstract: Recent years have witnessed many breakthroughs in research on graphene (the first two-dimensional atomic crystal) as well as a significant advance in the mass production of this material. This one-atom-thick fabric of carbon uniquely combines extreme mechanical strength, exceptionally high electronic and thermal conductivities, impermeability to gases, as well as many other supreme properties, all of which make it highly attractive for numerous applications. Here we review recent progress in graphene research and in the development of production methods, and critically analyse the feasibility of various graphene applications.

7,987 citations


Journal ArticleDOI
TL;DR: The modeling results suggest that graphene-multilayer graphene nanocomposite used as the thermal interface material outperforms those with carbon nanotubes or metal nanoparticles owing to graphene's aspect ratio and lower Kapitza resistance at the graphene-matrix interface.
Abstract: We found that the optimized mixture of graphene and multilayer graphene, produced by the high-yield inexpensive liquid-phase-exfoliation technique, can lead to an extremely strong enhancement of the cross-plane thermal conductivity K of the composite. The “laser flash” measurements revealed a record-high enhancement of K by 2300% in the graphene-based polymer at the filler loading fraction f = 10 vol %. It was determined that the relatively high concentration of the single-layer and bilayer graphene flakes (∼10–15%) present simultaneously with the thicker multilayers of large lateral size (∼1 μm) were essential for the observed unusual K enhancement. The thermal conductivity of the commercial thermal grease was increased from an initial value of ∼5.8 W/mK to K = 14 W/mK at the small loading f = 2%, which preserved all mechanical properties of the hybrid. Our modeling results suggest that graphene–multilayer graphene nanocomposite used as the thermal interface material outperforms those with carbon nanotub...

1,272 citations


Journal ArticleDOI
TL;DR: In this paper, the authors found that an optimized mixture of graphene and multilayer graphene can lead to an extremely strong enhancement of the cross-plane thermal conductivity of the composite.
Abstract: We found that an optimized mixture of graphene and multilayer graphene - produced by the high-yield inexpensive liquid-phase-exfoliation technique - can lead to an extremely strong enhancement of the cross-plane thermal conductivity K of the composite. The "laser flash" measurements revealed a record-high enhancement of K by 2300 % in the graphene-based polymer at the filler loading fraction f =10 vol. %. It was determined that a relatively high concentration of single-layer and bilayer graphene flakes (~10-15%) present simultaneously with thicker multilayers of large lateral size (~ 1 micrometer) were essential for the observed unusual K enhancement. The thermal conductivity of a commercial thermal grease was increased from an initial value of ~5.8 W/mK to K=14 W/mK at the small loading f=2%, which preserved all mechanical properties of the hybrid. Our modeling results suggest that graphene - multilayer graphene nanocomposite used as the thermal interface material outperforms those with carbon nanotubes or metal nanoparticles owing to graphene's aspect ratio and lower Kapitza resistance at the graphene - matrix interface.

896 citations


Journal ArticleDOI
TL;DR: This simple chemical vapor deposition method provides a unique approach for the synthesis of graphene heterostructures and surface functionalization of graphene and possesses great potential toward the development of new optical and electronic devices as well as a wide variety of newly synthesizable compounds for catalysts.
Abstract: We present a method for synthesizing MoS2/Graphene hybrid heterostructures with a growth template of graphene-covered Cu foil. Compared to other recent reports,(1, 2) a much lower growth temperature of 400 °C is required for this procedure. The chemical vapor deposition of MoS2 on the graphene surface gives rise to single crystalline hexagonal flakes with a typical lateral size ranging from several hundred nanometers to several micrometers. The precursor (ammonium thiomolybdate) together with solvent was transported to graphene surface by a carrier gas at room temperature, which was then followed by post annealing. At an elevated temperature, the precursor self-assembles to form MoS2 flakes epitaxially on the graphene surface via thermal decomposition. With higher amount of precursor delivered onto the graphene surface, a continuous MoS2 film on graphene can be obtained. This simple chemical vapor deposition method provides a unique approach for the synthesis of graphene heterostructures and surface funct...

890 citations


Journal ArticleDOI
TL;DR: Amino-functionalized graphene quantum dots with discrete molecular weights and specific edges were self-limitedly extracted from oxidized graphene sheet and exhibit bright colorful fluorescence under a single-wavelength excitation.
Abstract: Amino-functionalized graphene quantum dots (af-GQDs) with discrete molecular weights and specific edges were self-limitedly extracted from oxidized graphene sheet. Their optical properties can be precisely controlled only by the selective and quantitative functionalization at the edge sites. The af-GQDS exhibit bright colorful fluorescence under a single-wavelength excitation.

747 citations


Journal ArticleDOI
TL;DR: Graphene, a single atomic layer of sp2 hybridized carbon, exhibits a zero-band gap with linear band dispersion at the Fermi-level, forming a Dirac-cone at the K -points of its Brillouin zone as mentioned in this paper.

743 citations


Journal ArticleDOI
TL;DR: The interlayer shear mode of FLGs, ranging from bilayer graphene (BLG) to bulk graphite, is uncovered, and it is suggested that the corresponding Raman peak measures the interlayer coupling.
Abstract: 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 43 cm 1 in bulk graphite to 31 cm 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.

601 citations


Journal ArticleDOI
15 Mar 2012-Nature
TL;DR: This work reports the emergence of Dirac fermions in a fully tunable condensed-matter system—molecular graphene—assembled by atomic manipulation of carbon monoxide molecules over a conventional two-dimensional electron system at a copper surface and shows the existence within the system of linearly dispersing, massless quasi-particles accompanied by a density of states characteristic of graphene.
Abstract: The formation of massless Dirac fermions is demonstrated in a highly tunable molecular graphene lattice, and particular distortions of the lattice are shown to endow the fermions with mass or engage the fermions with artificial electric and magnetic fields. The electronic structure of certain solids causes them to exhibit 'Dirac points', which lie at the heart of many fascinating phenomena in condensed-matter physics. In graphene, for example, they cause electrons to act as massless Dirac fermions, able to travel at the speed of light. Two very different methods for controlling the properties of Dirac fermions are presented in this issue of Nature. In conventional solids, the electronic structure of the material cannot be varied, so it is difficult to see how the properties of Dirac fermions could be controlled. To avoid this constraint, Tarruell et al. create a tunable system of ultracold quantum gases within an adjustable honeycomb optical lattice. This model simulates condensed-matter physics, with atoms in the role of electrons. The Dirac points can be moved and merged to explore the physics of exotic materials such as topological insulators and graphene. Gomes et al. describe a more direct approach, creating an artificial form of molecular graphene by arranging carbon monoxide molecules, with atomic precision, in a honeycomb pattern on top of a two-dimensional electron system. Lattice parameters are adjustable, allowing the study of the properties of Dirac electrons and even the production of 'pseudo' electric and magnetic fields. This work highlights an innovative technique for constructing artificial materials with molecular assembly, including designer Dirac materials harbouring new ground states. The observation of massless Dirac fermions in monolayer graphene has generated a new area of science and technology seeking to harness charge carriers that behave relativistically within solid-state materials1. Both massless and massive Dirac fermions have been studied and proposed in a growing class of Dirac materials that includes bilayer graphene, surface states of topological insulators and iron-based high-temperature superconductors. Because the accessibility of this physics is predicated on the synthesis of new materials, the quest for Dirac quasi-particles has expanded to artificial systems such as lattices comprising ultracold atoms2,3,4. Here we report the emergence of Dirac fermions in a fully tunable condensed-matter system—molecular graphene—assembled by atomic manipulation of carbon monoxide molecules over a conventional two-dimensional electron system at a copper surface5. Using low-temperature scanning tunnelling microscopy and spectroscopy, we embed the symmetries underlying the two-dimensional Dirac equation into electron lattices, and then visualize and shape the resulting ground states. These experiments show the existence within the system of linearly dispersing, massless quasi-particles accompanied by a density of states characteristic of graphene. We then tune the quantum tunnelling between lattice sites locally to adjust the phase accrual of propagating electrons. Spatial texturing of lattice distortions produces atomically sharp p–n and p–n–p junction devices with two-dimensional control of Dirac fermion density and the power to endow Dirac particles with mass6,7,8. Moreover, we apply scalar and vector potentials locally and globally to engender topologically distinct ground states and, ultimately, embedded gauge fields9,10,11,12, wherein Dirac electrons react to ‘pseudo’ electric and magnetic fields present in their reference frame but absent from the laboratory frame. We demonstrate that Landau levels created by these gauge fields can be taken to the relativistic magnetic quantum limit, which has so far been inaccessible in natural graphene. Molecular graphene provides a versatile means of synthesizing exotic topological electronic phases in condensed matter using tailored nanostructures.

590 citations


Journal ArticleDOI
TL;DR: An inhomogeneous planar substrate (g-C(3)N(4)) promotes electron-rich and hole-rich regions, i.e., forming a well-defined electron-hole puddle, on the supported graphene layer, which can potentially allow overcoming the graphene's band gap hurdle in constructing field effect transistors.
Abstract: Opening up a band gap and finding a suitable substrate material are two big challenges for building graphene-based nanodevices. Using state-of-the-art hybrid density functional theory incorporating long-range dispersion corrections, we investigate the interface between optically active graphitic carbon nitride (g-C(3)N(4)) and electronically active graphene. We find an inhomogeneous planar substrate (g-C(3)N(4)) promotes electron-rich and hole-rich regions, i.e., forming a well-defined electron-hole puddle, on the supported graphene layer. The composite displays significant charge transfer from graphene to the g-C(3)N(4) substrate, which alters the electronic properties of both components. In particular, the strong electronic coupling at the graphene/g-C(3)N(4) interface opens a 70 meV gap in g-C(3)N(4)-supported graphene, a feature that can potentially allow overcoming the graphene's band gap hurdle in constructing field effect transistors. Additionally, the 2-D planar structure of g-C(3)N(4) is free of dangling bonds, providing an ideal substrate for graphene to sit on. Furthermore, when compared to a pure g-C(3)N(4) monolayer, the hybrid graphene/g-C(3)N(4) complex displays an enhanced optical absorption in the visible region, a promising feature for novel photovoltaic and photocatalytic applications.

532 citations


Journal ArticleDOI
TL;DR: A systematic Raman study of unconventionally stacked double-layer graphene finds that the spectrum strongly depends on the relative rotation angle between layers, and reveals changes in electronic band structure due to the interlayer interaction are responsible for the observed spectral features.
Abstract: We present a systematic Raman study of unconventionally stacked double-layer graphene, and find that the spectrum strongly depends on the relative rotation angle between layers. Rotation-dependent trends in the position, width and intensity of graphene 2D and G peaks are experimentally established and accounted for theoretically. Our theoretical analysis reveals that changes in electronic band structure due to the interlayer interaction, such as rotational-angle dependent Van Hove singularities, are responsible for the observed spectral features. Our combined experimental and theoretical study provides a deeper understanding of the electronic band structure of rotated double-layer graphene, and leads to a practical way to identify and analyze rotation angles of misoriented double-layer graphene.

529 citations


Journal ArticleDOI
TL;DR: In this paper, the electronic transport properties of a bilayer graphene contact with two monolayer nanoribbons were investigated by means of a tight-binding method and a continuum Dirac model.
Abstract: We investigate the electronic transport properties of a bilayer graphene ake contacted by two monolayer nanoribbons. This nite-size bilayer ake can be built by overlapping two semi-in nite ribbons. We study and analyze the electronic behavior of this structure by means of a tight-binding method and a continuum Dirac model. We have found that the conductance oscillates markedly between zero and the maximum value of the conductance, allowing for the design of electromechanical switches.

Journal ArticleDOI
TL;DR: A hot-electron bolometer made of bilayer graphene that is dual-gated to create a tunable bandgap and electron-temperature-dependent conductivity is demonstrated.
Abstract: An infrared bolometer made using bilayer graphene compares favourably to existing devices in terms of sensitivity, noise equivalent power and speed.

Journal ArticleDOI
TL;DR: In this paper, the authors outline different theoretical approaches developed for phonon transport in graphene, discuss contributions of the in-plane and cross-plane phonon modes and provide comparison with available experimental thermal conductivity data.
Abstract: Properties of phonons - quanta of the crystal lattice vibrations - in graphene have attracted strong attention of the physics and engineering communities. Acoustic phonons are the main heat carriers in graphene near room temperature while optical phonons are used for counting the number of atomic planes in Raman experiments with few-layer graphene. It was shown both theoretically and experimentally that transport properties of phonons, i.e. energy dispersion and scattering rates, are substantially different in the quasi two-dimensional system such as graphene compared to basal planes in graphite or three-dimensional bulk crystals. The unique nature of two-dimensional phonon transport translates to unusual heat conduction in graphene and related materials. In this review we outline different theoretical approaches developed for phonon transport in graphene, discuss contributions of the in-plane and cross-plane phonon modes and provide comparison with available experimental thermal conductivity data. Particular attention is given to analysis of recent theoretical results for the phonon thermal conductivity of graphene and few-layer graphene, and the effects of the strain, defects and isotopes on the phonon transport in these systems.

Journal ArticleDOI
TL;DR: In this paper, the surface of graphene was decorated with lithium atoms, and it was shown that it could be made to superconduct, despite many attempts to find ways to induce it, superconductivity is not one of them.
Abstract: Graphene exhibits many extraordinary properties. But, despite many attempts to find ways to induce it, superconductivity is not one of them. First-principles calculations suggest that by decorating the surface of graphene with lithium atoms, it could yet be made to superconduct.

Journal ArticleDOI
TL;DR: In this article, van Hove singularities due to interlayer coupling are ubiquitously present in a broad range of rotation angles in twisted graphene layers and they survive in the presence of a third graphene layer, and test the role of the periodic modulation and absolute value of the interlayer distance.
Abstract: Extensive scanning tunneling microscopy and spectroscopy experiments complemented by first-principles and parametrized tight binding calculations provide a clear answer to the existence, origin, and robustness of van Hove singularities (vHs) in twisted graphene layers Our results are conclusive: vHs due to interlayer coupling are ubiquitously present in a broad range (from 1\ifmmode^\circ\else\textdegree\fi{} to 10\ifmmode^\circ\else\textdegree\fi{}) of rotation angles in our graphene on $6H$-SiC(000-1) samples From the variation of the energy separation of the vHs with the rotation angle we are able to recover the Fermi velocity of a graphene monolayer as well as the strength of the interlayer interaction The robustness of the vHs is assessed both by experiments, which show that they survive in the presence of a third graphene layer, and by calculations, which test the role of the periodic modulation and absolute value of the interlayer distance Finally, we clarify the role of the layer topographic corrugation and of electronic effects in the apparent moir\'e contrast measured on the STM images

Journal ArticleDOI
Yu Liu1, Gang Wang1, Qingsong Huang1, Liwei Guo1, Xiaolong Chen1 
TL;DR: T graphene, a two-dimensional carbon allotrope with tetrarings, is investigated by first-principles calculations in this article, and it is shown that buckled T graphene has Dirac-like fermions and a high Fermi velocity similar to graphene even though it has nonequivalent bonds and possesses no hexagonal honeycomb structure.
Abstract: T graphene, a two-dimensional carbon allotrope with tetrarings, is investigated by first-principles calculations. We demonstrate that buckled T graphene has Dirac-like fermions and a high Fermi velocity similar to graphene even though it has nonequivalent bonds and possesses no hexagonal honeycomb structure. New features of the linear dispersions that are different from graphene are revealed. π and π* bands and the two comprising sublattices are the key factors for the emergence of Dirac-like fermions. T graphene and its two types of nanoribbon are expected to possess additional properties over graphene due to its different band structure.

Journal ArticleDOI
TL;DR: This work combines two direct imaging techniques, dark-field transmission electron microscopy (DF-TEM) and widefield Raman imaging, to establish a robust, one-to-one correlation between twist angle and Raman intensity in twisted bilayer graphene (tBLG).
Abstract: Few-layer graphene is a prototypical layered material, whose properties are determined by the relative orientations and interactions between layers. Exciting electrical and optical phenomena have been observed for the special case of Bernal-stacked few-layer graphene, but structure–property correlations in graphene which deviates from this structure are not well understood. Here, we combine two direct imaging techniques, dark-field transmission electron microscopy (DF-TEM) and widefield Raman imaging, to establish a robust, one-to-one correlation between twist angle and Raman intensity in twisted bilayer graphene (tBLG). The Raman G band intensity is strongly enhanced due to a previously unreported singularity in the joint density of states of tBLG, whose energy is exclusively a function of twist angle and whose optical transition strength is governed by interlayer interactions, enabling direct optical imaging of these parameters. Furthermore, our findings suggest future potential for novel optical and op...

Journal ArticleDOI
TL;DR: The extra states sometimes observed in graphene's quantum Hall characteristics have been presumed to be the result of broken SU(4) symmetry as discussed by the authors, and magnetotransport measurements of high-quality graphene in a tilted magnetic field finally prove this is indeed the case.
Abstract: The extra states sometimes observed in graphene’s quantum Hall characteristics have been presumed to be the result of broken SU(4) symmetry. Magnetotransport measurements of high-quality graphene in a tilted magnetic field finally prove this is indeed the case.

01 Jan 2012
TL;DR: Graphene is a material that invites superlatives as mentioned in this paper, and it has been much in the news recently, especially following the 2010 Nobel Prize to Andre Geim and Konstantin Novaselov for their groundbreaking experiments on graphene.
Abstract: Graphene is a material that invites superlatives. It has been much in the news recently, especially following the 2010 Nobel Prize to Andre Geim and Konstantin Novaselov for their ‘groundbreaking experiments’ on graphene. A two-dimensional sheet of carbon atoms linked in a hexagonal lattice, just one atom thick, it is the thinnest known material, is harder than diamond and stronger than steel, while still very stretchable (by up to 20%), has an electrical conductivity higher than copper, and has an exceptionally high thermal conductivity.

Journal ArticleDOI
TL;DR: D density functional theory calculations demonstrate that divacancies and higher order defects have reasonable diffusion barrier heights allowing lithium diffusion through the basal plane but neither monovacancies nor Stone-Wales defect.
Abstract: Coexistence of both edge plane and basal plane in graphite often hinders the understanding of lithium ion diffusion mechanism. In this report, two types of graphene samples were prepared by chemical vapor deposition (CVD): (i) well-defined basal plane graphene grown on Cu foil and (ii) edge plane-enriched graphene layers grown on Ni film. Electrochemical performance of the graphene electrode can be split into two regimes depending on the number of graphene layers: (i) the corrosion-dominant regime and (ii) the lithiation-dominant regime. Li ion diffusion perpendicular to the basal plane of graphene is facilitated by defects, whereas diffusion parallel to the plane is limited by the steric hindrance that originates from aggregated Li ions adsorbed on the abundant defect sites. The critical layer thickness (lc) to effectively prohibit substrate reaction using CVD-grown graphene layers was predicted to be ∼6 layers, independent of defect population. Our density functional theory calculations demonstrate that...

Journal ArticleDOI
Tianrong Zhan1, Xi Shi1, Yunyun Dai1, Xiaohan Liu1, Jian Zi1 
TL;DR: A transfer matrix method is developed for optical calculations of non-interacting graphene layers, revealing well-defined photonic band structures and evenphotonic bandgaps and a simple way to tune the plasmon dispersion.
Abstract: A transfer matrix method is developed for optical calculations of non-interacting graphene layers. Within the framework of this method, optical properties such as reflection, transmission and absorption for single-, double- and multi-layer graphene are studied. We also apply the method to structures consisting of periodically arranged graphene layers, revealing well-defined photonic band structures and even photonic bandgaps. Finally, we discuss graphene plasmons and introduce a simple way to tune the plasmon dispersion.

Journal ArticleDOI
TL;DR: In this article, the authors investigated the electronic structure and the quantum Hall effect in twisted bilayer graphenes with various rotation angles in the presence of magnetic field and computed the energy spectrum and quantized Hall conductivity in a wide range of magnetic fields.
Abstract: We investigate the electronic structure and the quantum Hall effect in twisted bilayer graphenes with various rotation angles in the presence of magnetic field. Using a low-energy approximation, which incorporates the rigorous interlayer interaction, we computed the energy spectrum and the quantized Hall conductivity in a wide range of magnetic field from the semiclassical regime to the fractal spectrum regime. In weak magnetic fields, the low-energy conduction band is quantized into electronlike and holelike Landau levels at energies below and above the van Hove singularity, respectively, and the Hall conductivity sharply drops from positive to negative when the Fermi energy goes through the transition point. In increasing magnetic field, the spectrum gradually evolves into a fractal band structure called Hofstadter's butterfly, where the Hall conductivity exhibits a nonmonotonic behavior as a function of Fermi energy. The typical electron density and magnetic field amplitude characterizing the spectrum monotonically decrease as the rotation angle is reduced, indicating that the rich electronic structure may be observed in a moderate condition.

Journal ArticleDOI
TL;DR: An ultrasensitive and flexible field-effect transistor (FET) olfactory system, namely, a bioelectronic nose (B-nose), based on plasma-treated bilayer graphene conjugated with an olf factory receptor, which can recognize a target odorant with single-carbon-atom resolution.
Abstract: Rapid and precise discrimination of various odorants is vital to fabricating enhanced sensing devices in the fields of disease diagnostics, food safety, and environmental monitoring. Here, we demonstrate an ultrasensitive and flexible field-effect transistor (FET) olfactory system, namely, a bioelectronic nose (B-nose), based on plasma-treated bilayer graphene conjugated with an olfactory receptor. The stable p- and n-type behaviors from modified bilayer graphene (MBLG) took place after controlled oxygen and ammonia plasma treatments. It was integrated with human olfactory receptors 2AG1 (hOR2AG1: OR), leading to the formation of the liquid-ion gated FET-type platform. ORs bind to the particular odorant amyl butyrate (AB), and their interactions are specific and selective. The B-noses behave as flexible and transparent sensing devices and can recognize a target odorant with single-carbon-atom resolution. The B-noses are ultrasensitive and highly selective toward AB. The minimum detection limit (MDL) is as...

Journal ArticleDOI
13 Jan 2012-ACS Nano
TL;DR: This study demonstrates the ability of graphene nanostructures to host well-defined plasmons down to sizes below 10 nm, and it delineates a roadmap for understanding their main characteristics, including the role of finite size and nonlocality, thus providing a solid background for the emerging field of graphene Nanoplasmonics.
Abstract: Graphene plasmons are emerging as an alternative solution to noble metal plasmons, adding the advantages of tunability via electrostatic doping and long lifetimes. These excitations have been so far described using classical electrodynamics, with the carbon layer represented by a local conductivity. However, the question remains, how accurately is such a classical description representing graphene? What is the minimum size for which nonlocal and quantum finite-size effects can be ignored in the plasmons of small graphene structures? Here, we provide a clear answer to these questions by performing first-principles calculations of the optical response of doped nanostructured graphene obtained from a tight-binding model for the electronic structure and the random-phase approximation for the dielectric response. The resulting plasmon energies are in good agreement with classical local electromagnetic theory down to ∼10 nm sizes, below which plasmons split into several resonances that emphasize the molecular c...

Journal ArticleDOI
TL;DR: In this paper, the Young's modulus of graphene is estimated by measuring the strain applied by a pressure difference across graphene membranes using Raman spectroscopy, which can be estimated directly from the peak shift of the Raman G band.
Abstract: The Young’s modulus of graphene is estimated by measuring the strain applied by a pressure difference across graphene membranes using Raman spectroscopy. The strain induced on pressurized graphene balloons can be estimated directly from the peak shift of the Raman G band. By comparing the measured strain with numerical simulation, we obtained the Young’s modulus of graphene. The estimated Young’s modulus values of single- and bilayer graphene are 2.4 ± 0.4 and 2.0 ± 0.5 TPa, respectively.

Journal ArticleDOI
TL;DR: The normal and inverted devices based on GO hole- and GO-Cs electron-extraction layers both outperform the corresponding standard BHJ solar cells.
Abstract: : Graphene, having a single-atom-thick sheet of carbon atoms packed in a 2D honeycomb lattices, possesses excellent electronic, thermal, and mechanical properties attractive for a large variety of potential applications, including transparent electrodes and/or active materials in electronic devices, solar cells, supercapacitors, batteries, fuel cells, actuators, and sensors. Graphene has also been found to be useful as the platform of biomedical sensors. The recent availability of solution processable graphene by exfoliation of graphite into graphene oxides (GOs), followed by solution reduction, has allowed the functionalization, characterization, and processing of graphene sheets via various solution methods. It has been demonstrated that GO consists of epoxy and hydroxyl groups on the basal plane and carboxylic groups at the edge. The C O bonds on the basal plane disrupt the conjugation of the hexagonal graphene lattice to render GO insulator or semiconductor. Due to strong interactions between the hexagonally sp 2 -bonded carbon layers in graphite, the solution oxidation of graphite requires strong oxidizing reagents (e.g., HNO 3 , KMnO 4 , and/ or H 2 SO 4 ) under harsh conditions. This often leads to severe damage to the carbon basal plane, and hence a poorly defi ned electronic structure. It remains a big challenge to design GO-based materials with controlled electronic properties for high-performance device applications. Further to our work on functionalization of graphene (oxide), we have recently found that simple charge neutralization of the COOH groups in GO with Cs 2 CO 3 could tune the electronic structure of GO, making GO derivatives useful as both hole- and electron-extraction layers in bulk heterojunction (BHJ) solar cells.

Journal ArticleDOI
02 Mar 2012-ACS Nano
TL;DR: It is demonstrated that, in general, multilayer graphene will give rise to higher levels of reinforcement than monolayer material, with the optimum number of layers depending upon the separation of the graphene flakes in the nanocomposite.
Abstract: The stress transfer between the internal layers of multilayer graphene within polymer-based nanocomposites has been investigated from the stress-induced shifts of the 2D Raman band. This has been undertaken through the study of the deformation of an ideal composite system where the graphene flakes were placed upon the surface of a polymer beam and then coated with an epoxy polymer. It is found that the rate of band shift per unit strain for a monolayer graphene flake is virtually independent of whether it has one or two polymer interfaces (i.e., with or without an epoxy top coating). In contrast, the rate of band shift is lower for an uncoated bilayer specimen than a coated one, indicating relatively poor stress transfer between the graphene layers. Mapping of the strain in the coated bilayer regions has shown that there is strain continuity between adjacent monolayer and bilayer regions, indicating that they give rise to similar levels of reinforcement. Strain-induced Raman band shifts have also been eva...

Journal ArticleDOI
TL;DR: It is predicted that there exists no Li arrangement that stabilizes Li absorption on the surface of single layer graphene unless that surface includes defects, and it follows that defect-poorsingle layer graphene exhibits significantly inferior capacity compared to bulk graphite.
Abstract: We present an exhaustive first-principles investigation of Li absorption and intercalation in single layer graphene and few layer graphene, as compared to bulk graphite. For single layer graphene, the cluster expansion method is used to systemically search for the lowest energy ionic configuration as a function of absorbed Li content. It is predicted that there exists no Li arrangement that stabilizes Li absorption on the surface of single layer graphene unless that surface includes defects. From this result follows that defect-poor single layer graphene exhibits significantly inferior capacity compared to bulk graphite. For few layer graphene, we calibrate a semiempirical potential to include the effect of van der Waals interactions, which is essential to account for the contribution of empty (no Li) gallery to the total energy. We identify and analyze the Li intercalation mechanisms in few layer graphene and map out the sequence in stable phases as we move from single layer graphene, through few layer, to bulk graphite.

Journal ArticleDOI
TL;DR: In this paper, the authors review the electronic properties of bilayer graphene and derive the effective Hamiltonian describing massive chiral quasiparticles in two parabolic bands at low energy.
Abstract: We review the electronic properties of bilayer graphene, beginning with a description of the tight-binding model of bilayer graphene and the derivation of the effective Hamiltonian describing massive chiral quasiparticles in two parabolic bands at low energy. We take into account five tight-binding parameters of the Slonczewski-Weiss-McClure model of bulk graphite plus intra- and interlayer asymmetry between atomic sites which induce band gaps in the low-energy spectrum. The Hartree model of screening and band-gap opening due to interlayer asymmetry in the presence of external gates is presented. The tight-binding model is used to describe optical and transport properties including the integer quantum Hall effect, and we also discuss orbital magnetism, phonons and the influence of strain on electronic properties. We conclude with an overview of electronic interaction effects.

Journal ArticleDOI
24 Aug 2012-ACS Nano
TL;DR: It is shown that the self-limiting effect of graphene growth on Cu foil can be broken by using a high H(2)/CH(4) ratio in a low-pressure CVD process to enable the continued growth of bilayer graphene.
Abstract: Bernal-stacked (AB-stacked) bilayer graphene is of significant interest for functional electronic and photonic devices due to the feasibility to continuously tune its band gap with a vertical electric field. Mechanical exfoliation can be used to produce AB-stacked bilayer graphene flakes but typically with the sizes limited to a few micrometers. Chemical vapor deposition (CVD) has been recently explored for the synthesis of bilayer graphene but usually with limited coverage and a mixture of AB- and randomly stacked structures. Herein we report a rational approach to produce large-area high-quality AB-stacked bilayer graphene. We show that the self-limiting effect of graphene growth on Cu foil can be broken by using a high H2/CH4 ratio in a low-pressure CVD process to enable the continued growth of bilayer graphene. A high-temperature and low-pressure nucleation step is found to be critical for the formation of bilayer graphene nuclei with high AB stacking ratio. A rational design of a two-step CVD process...