There is intense interest in graphene in fields such as physics, chemistry, and materials science, among others. Interest in graphene's exceptional physical properties, chemical tunability, and potential for applications has generated thousands of publications and an accelerating pace of research, making review of such research timely. Here is an overview of the synthesis, properties, and applications of graphene and related materials (primarily, graphite oxide and its colloidal suspensions and materials made from them), from a materials science perspective.

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Graphene and Graphene Oxide: Synthesis, Properties, and Applications

Raman spectroscopy is an integral part of graphene research. It is used to determine the number and orientation of layers, the quality and types of edge, and the effects of perturbations, such as electric and magnetic fields, strain, doping, disorder and functional groups. This, in turn, provides insight into all sp(2)-bonded carbon allotropes, because graphene is their fundamental building block. Here we review the state of the art, future directions and open questions in Raman spectroscopy of graphene. We describe essential physical processes whose importance has only recently been recognized, such as the various types of resonance at play, and the role of quantum interference. We update all basic concepts and notations, and propose a terminology that is able to describe any result in literature. We finally highlight the potential of Raman spectroscopy for layered materials other than graphene.

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Raman spectroscopy as a versatile tool for studying the properties of graphene

Raman spectroscopy in graphene

Molybdenum disulfide (MoS2) of single- and few-layer thickness was exfoliated on SiO2/Si substrate and characterized by Raman spectroscopy. The number of S−Mo−S layers of the samples was independently determined by contact-mode atomic force microscopy. Two Raman modes, E12g and A1g, exhibited sensitive thickness dependence, with the frequency of the former decreasing and that of the latter increasing with thickness. The results provide a convenient and reliable means for determining layer thickness with atomic-level precision. The opposite direction of the frequency shifts, which cannot be explained solely by van der Waals interlayer coupling, is attributed to Coulombic interactions and possible stacking-induced changes of the intralayer bonding. This work exemplifies the evolution of structural parameters in layered materials in changing from the three-dimensional to the two-dimensional regime.

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Anomalous lattice vibrations of single- and few-layer MoS2.

Every few years, a new material with unique properties emerges and fascinates the scientific community, typical recent examples being high-temperature superconductors and carbon nanotubes. Graphene is the latest sensation with unusual properties, such as half-integer quantum Hall effect and ballistic electron transport. This two-dimensional material which is the parent of all graphitic carbon forms is strictly expected to comprise a single layer, but there is considerable interest in investigating two-layer and few-layer graphenes as well. Synthesis and characterization of graphenes pose challenges, but there has been considerable progress in the last year or so. Herein, we present the status of graphene research which includes aspects related to synthesis, characterization, structure, and properties.

Graphene: The New Two-Dimensional Nanomaterial

Graphene was deposited on a transparent and flexible substrate, and tensile strain up to ∼0.8% was loaded by stretching the substrate in one direction. Raman spectra of strained graphene show significant red shifts of 2D and G band (−27.8 and −14.2 cm−1 per 1% strain, respectively) because of the elongation of the carbon−carbon bonds. This indicates that uniaxial strain has been successfully applied on graphene. We also proposed that, by applying uniaxial strain on graphene, tunable band gap at K point can be realized. First-principle calculations predicted a band-gap opening of ∼300 meV for graphene under 1% uniaxial tensile strain. The strained graphene provides an alternative way to experimentally tune the band gap of graphene, which would be more efficient and more controllable than other methods that are used to open the band gap in graphene. Moreover, our results suggest that the flexible substrate is ready for such a strain process, and Raman spectroscopy can be used as an ultrasensitive method to ...

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Uniaxial strain on graphene: Raman spectroscopy study and band-gap opening.

Graphene was deposited on a transparent andflexible substrate, and tensile strain up to0.8% was loaded by stretching the substrate in one direction. Raman spectra of strained graphene show significant red shifts of 2D and G band (27.8 and14.2 cm 1 per 1% strain, respectively) because of the elongation of the carboncarbon bonds. This indicates that uniaxial strain has been successfully applied on graphene. We also proposedthat,byapplyinguniaxialstrainongraphene,tunablebandgapatKpointcanberealized.First-principle calculations predicted a band-gap opening of300 meV for graphene under 1% uniaxial tensile strain. The strained graphene provides an alternative way to experimentally tune the band gap of graphene, which would be more efficient and more controllable than other methods that are used to open the band gap in graphene. Moreover,ourresultssuggestthattheflexiblesubstrateisreadyforsuchastrainprocess,andRamanspectroscopy can be used as an ultrasensitive method to determine the strain.

Uniaxial Strain on Graphene: Raman Spectroscopy Study and Band-Gap

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 SiO2 (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 o...

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Raman Studies of Monolayer Graphene: The Substrate Effect

Graphene is a two-dimensional material defined as a planar honeycomb lattice of close-packed carbon atoms, where the electrons exhibit a linear dispersion near Dirac K points and behave as massless Dirac fermions. However, the valence and conduction bands in an AB stacked graphene bilayer split into two parabolic branches near the K point originating from the interaction of p electrons, and the electrons are hence described by massive Dirac fermions. Moreover, a graphene bilayer is a tunable-gap semiconductor under electric-field biasing. With a further increase in the number of layers along with AB stacking, the electronic structure reveals stepwise variations that eventually approach that of the three-dimensional counterpart. Considering the close relation between the electronic properties and layer number of few-layer graphene (FLG), the ability to accurately determine the layer number and correlating this with the electronic structure is a prerequisite in understanding the evolution of the electronic properties from twoto threedimensional graphitic materials. In addition to graphene layers with AB stacking, FLG with arbitrary stacking (Figure 1) is considered to possess distinct properties arising from its different crystalline structure and p electron interactions. Experimentally, it has been observed that the electroand magnetotransport properties for folded graphene sheets are different to thoseofAB stackedbilayers. Furthermore,FLG grown on SiC, Ni, and Ru also have non-AB stacking order. Therefore, elucidating the detailed character-

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Probing layer number and stacking order of few-layer graphene by Raman spectroscopy.

Raman spectroscopic studies of graphene have attracted much interest. The G-band Raman intensity of a single layer graphene on Si substrate with 300nm SiO2 capping layer is surprisingly strong and is comparable to that of bulk graphite. To explain this Raman intensity anomaly, we show that in addition to the interference due to multiple reflection of the incident laser, the multiple reflection of the Raman signal inside the graphene layer must be also accounted for. Further studies of the role of SiO2 layer in the enhancement Raman signal of graphene are carried out and an enhancement factor of ∼30 is achievable, which is very significant for the Raman studies. Finally, we discuss the potential application of this enhancement effect on other ultrathin films and nanoflakes and a general selection criterion of capping layer and substrate is given.

Yingying Wang

Papers

Uniaxial strain on graphene: Raman spectroscopy study and band-gap opening.

Uniaxial Strain on Graphene: Raman Spectroscopy Study and Band-Gap

Raman Studies of Monolayer Graphene: The Substrate Effect

Probing layer number and stacking order of few-layer graphene by Raman spectroscopy.

Interference enhancement of Raman signal of graphene