Ultraviolet Raman microscopy of single and multilayer graphene
TL;DR: In this paper, the authors investigated the Raman spectra of single-layer and multilayer graphene under ultraviolet laser excitation at the wavelength λ =325 nm and found that the 2D band intensity undergoes severe quenching.
Abstract: We investigated Raman spectra of single-layer and multilayer graphene under ultraviolet laser excitation at the wavelength λ=325 nm. It was found that while graphene’s G peak remains pronounced in UV Raman spectra, the 2D-band intensity undergoes severe quenching. The evolution of the ratio of the intensities of the G and 2D peaks, I(G)/I(2D), as the number of graphene layers n changes from n=1 to n=5, is different in UV Raman spectra from that in conventional visible Raman spectra excited at the 488 and 633 nm wavelengths. The 2D band under UV excitation shifts to larger wave numbers and is found near 2825 cm−1. The observed UV Raman features of graphene were explained by invoking the resonant scattering model. The obtained results contribute to the Raman nanometrology of graphene by providing an additional metric for determining the number of graphene layers and assessing its quality.
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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
TL;DR: In this paper, the use of liquid-phase-exfoliated graphene and multilayer graphene as fillers in the thermal interface materials has been discussed, and it has been demonstrated that the addition of an optimized mixture of graphene and multi-layer graphene to the composites with different matrix materials produces the record-high enhancement of the effective thermal conductivity at the small filler loading fraction (f≤10vol%).
743 citations
TL;DR: The synthesis of 2D gallium nitride (GaN) via a migration-enhanced encapsulated growth (MEEG) technique utilizing epitaxial graphene is demonstrated and it is established that graphene plays a critical role in stabilizing the direct-bandgap, 2D buckled structure.
Abstract: A method to synthesize 2D layers of gallium nitride on SiC is reported. Epitaxial graphene preliminarily grown on SiC allows intercalation of gallium atoms on the SiC substrate and stabilizes the 2D gallium nitride islands formed by ammonolysis. The spectrum of two-dimensional (2D) and layered materials ‘beyond graphene’ offers a remarkable platform to study new phenomena in condensed matter physics. Among these materials, layered hexagonal boron nitride (hBN), with its wide bandgap energy (∼5.0–6.0 eV), has clearly established that 2D nitrides are key to advancing 2D devices1. A gap, however, remains between the theoretical prediction of 2D nitrides ‘beyond hBN’2,3 and experimental realization of such structures. Here we demonstrate the synthesis of 2D gallium nitride (GaN) via a migration-enhanced encapsulated growth (MEEG) technique utilizing epitaxial graphene. We theoretically predict and experimentally validate that the atomic structure of 2D GaN grown via MEEG is notably different from reported theory2,3,4. Moreover, we establish that graphene plays a critical role in stabilizing the direct-bandgap (nearly 5.0 eV), 2D buckled structure. Our results provide a foundation for discovery and stabilization of 2D nitrides that are difficult to prepare via traditional synthesis.
594 citations
TL;DR: Generally defects degrade the figures of merit for devices, such as carrier mobility and conductivity, whereas doping provides a means to tune the carrier concentration in graphene thereby enabling the engineering of novel material systems.
Abstract: In this article we review Raman studies of defects and dopants in graphene as well as the importance of both for device applications. First a brief overview of Raman spectroscopy of graphene is presented. In the following section we discuss the Raman characterization of three defect types: point defects, edges, and grain boundaries. The next section reviews the dependence of the Raman spectrum on dopants and highlights several common doping techniques. In the final section, several device applications are discussed which exploit doping and defects in graphene. Generally defects degrade the figures of merit for devices, such as carrier mobility and conductivity, whereas doping provides a means to tune the carrier concentration in graphene thereby enabling the engineering of novel material systems. Accurately measuring both the defect density and doping is critical and Raman spectroscopy provides a powerful tool to accomplish this task.
566 citations
TL;DR: In this article, the in-plane and cross-plane thermal conductivity of reduced graphene oxide films subjected to a high-temperature treatment of up to 1000 °C was investigated.
Abstract: Thermal conductivity of free-standing reduced graphene oxide films subjected to a high-temperature treatment of up to 1000 °C is investigated. It is found that the high-temperature annealing dramatically increases the in-plane thermal conductivity, K, of the films from ≈3 to ≈61 W m−1 K−1 at room temperature. The cross-plane thermal conductivity, K⊥, reveals an interesting opposite trend of decreasing to a very small value of ≈0.09 W m−1 K−1 in the reduced graphene oxide films annealed at 1000 °C. The obtained films demonstrate an exceptionally strong anisotropy of the thermal conductivity, K/K⊥ ≈ 675, which is substantially larger even than in the high-quality graphite. The electrical resistivity of the annealed films reduces to 1–19 Ω □−1. The observed modifications of the in-plane and cross-plane thermal conductivity components resulting in an unusual K/K⊥ anisotropy are explained theoretically. The theoretical analysis suggests that K can reach as high as ≈500 W m−1 K−1 with the increase in the sp2 domain size and further reduction of the oxygen content. The strongly anisotropic heat conduction properties of these films can be useful for applications in thermal management.
457 citations
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TL;DR: Monocrystalline graphitic films are found to be a two-dimensional semimetal with a tiny overlap between valence and conductance bands and they exhibit a strong ambipolar electric field effect.
Abstract: We describe monocrystalline graphitic films, which are a few atoms thick but are nonetheless stable under ambient conditions, metallic, and of remarkably high quality. The films are found to be a two-dimensional semimetal with a tiny overlap between valence and conductance bands, and they exhibit a strong ambipolar electric field effect such that electrons and holes in concentrations up to 10 13 per square centimeter and with room-temperature mobilities of ∼10,000 square centimeters per volt-second can be induced by applying gate voltage.
55,532 citations
TL;DR: This study reports an experimental study of a condensed-matter system (graphene, a single atomic layer of carbon) in which electron transport is essentially governed by Dirac's (relativistic) equation and reveals a variety of unusual phenomena that are characteristic of two-dimensional Dirac fermions.
Abstract: Quantum electrodynamics (resulting from the merger of quantum mechanics and relativity theory) has provided a clear understanding of phenomena ranging from particle physics to cosmology and from astrophysics to quantum chemistry. The ideas underlying quantum electrodynamics also influence the theory of condensed matter, but quantum relativistic effects are usually minute in the known experimental systems that can be described accurately by the non-relativistic Schrodinger equation. Here we report an experimental study of a condensed-matter system (graphene, a single atomic layer of carbon) in which electron transport is essentially governed by Dirac's (relativistic) equation. The charge carriers in graphene mimic relativistic particles with zero rest mass and have an effective 'speed of light' c* approximately 10(6) m s(-1). Our study reveals a variety of unusual phenomena that are characteristic of two-dimensional Dirac fermions. In particular we have observed the following: first, graphene's conductivity never falls below a minimum value corresponding to the quantum unit of conductance, even when concentrations of charge carriers tend to zero; second, the integer quantum Hall effect in graphene is anomalous in that it occurs at half-integer filling factors; and third, the cyclotron mass m(c) of massless carriers in graphene is described by E = m(c)c*2. This two-dimensional system is not only interesting in itself but also allows access to the subtle and rich physics of quantum electrodynamics in a bench-top experiment.
18,958 citations
TL;DR: This work shows that graphene's electronic structure is captured in its Raman spectrum that clearly evolves with the number of layers, and allows unambiguous, high-throughput, nondestructive identification of graphene layers, which is critically lacking in this emerging research area.
Abstract: Graphene is the two-dimensional building block for carbon allotropes of every other dimensionality We show that its electronic structure is captured in its Raman spectrum that clearly evolves with the number of layers The D peak second order changes in shape, width, and position for an increasing number of layers, reflecting the change in the electron bands via a double resonant Raman process The G peak slightly down-shifts This allows unambiguous, high-throughput, nondestructive identification of graphene layers, which is critically lacking in this emerging research area
13,474 citations
TL;DR: The extremely high value of the thermal conductivity suggests that graphene can outperform carbon nanotubes in heat conduction and establishes graphene as an excellent material for thermal management.
Abstract: We report the measurement of the thermal conductivity of a suspended single-layer graphene. The room temperature values of the thermal conductivity in the range ∼(4.84 ± 0.44) × 103 to (5.30 ± 0.48) × 103 W/mK were extracted for a single-layer graphene from the dependence of the Raman G peak frequency on the excitation laser power and independently measured G peak temperature coefficient. The extremely high value of the thermal conductivity suggests that graphene can outperform carbon nanotubes in heat conduction. The superb thermal conduction property of graphene is beneficial for the proposed electronic applications and establishes graphene as an excellent material for thermal management.
11,878 citations
TL;DR: The bottom-up chemical approach of tuning the graphene sheet properties provides a path to a broad new class of graphene-based materials and their use in a variety of applications.
Abstract: The remarkable mechanical properties of carbon nanotubes arise from the exceptional strength and stiffness of the atomically thin carbon sheets (graphene) from which they are formed. In contrast, bulk graphite, a polycrystalline material, has low fracture strength and tends to suffer failure either by delamination of graphene sheets or at grain boundaries between the crystals. Now Stankovich et al. have produced an inexpensive polymer-matrix composite by separating graphene sheets from graphite and chemically tuning them. The material contains dispersed graphene sheets and offers access to a broad range of useful thermal, electrical and mechanical properties. Individual sheets of graphene can be readily incorporated into a polymer matrix, giving rise to composite materials having potentially useful electronic properties. Graphene sheets—one-atom-thick two-dimensional layers of sp2-bonded carbon—are predicted to have a range of unusual properties. Their thermal conductivity and mechanical stiffness may rival the remarkable in-plane values for graphite (∼3,000 W m-1 K-1 and 1,060 GPa, respectively); their fracture strength should be comparable to that of carbon nanotubes for similar types of defects1,2,3; and recent studies have shown that individual graphene sheets have extraordinary electronic transport properties4,5,6,7,8. One possible route to harnessing these properties for applications would be to incorporate graphene sheets in a composite material. The manufacturing of such composites requires not only that graphene sheets be produced on a sufficient scale but that they also be incorporated, and homogeneously distributed, into various matrices. Graphite, inexpensive and available in large quantity, unfortunately does not readily exfoliate to yield individual graphene sheets. Here we present a general approach for the preparation of graphene-polymer composites via complete exfoliation of graphite9 and molecular-level dispersion of individual, chemically modified graphene sheets within polymer hosts. A polystyrene–graphene composite formed by this route exhibits a percolation threshold10 of ∼0.1 volume per cent for room-temperature electrical conductivity, the lowest reported value for any carbon-based composite except for those involving carbon nanotubes11; at only 1 volume per cent, this composite has a conductivity of ∼0.1 S m-1, sufficient for many electrical applications12. Our bottom-up chemical approach of tuning the graphene sheet properties provides a path to a broad new class of graphene-based materials and their use in a variety of applications.
11,866 citations