Graphene has many unique properties that make it an ideal material for fundamental studies as well as for potential applications. Here we review the recent results on the Raman spectroscopy and imaging of graphene. Raman spectroscopy and imaging can be used as a quick and unambiguous method to determine the number of graphene layers. Following, the strong Raman signal of single layer graphene compared to graphite is explained by an interference enhancement model. We have also studied the effect of substrates, the top layer deposition, the annealing process, as well as folding (stacking order) on the physical and electronic properties of graphene. Finally, Raman spectroscopy of epitaxial graphene grown on SiC substrate is presented and strong compressive strain on epitaxial graphene is observed. The results presented here are closely related to the application of graphene on nano-electronic device and help on the better understanding of physical and electronic properties of graphene.
The use of Raman scattering techniques to study the mechanical properties of graphene films is reviewed here. The determination of Gruneisen parameters of suspended graphene sheets under uni- and bi-axial strain is discussed and the values are compared to theoretical predictions. The effects of the graphene-substrate interaction on strain and to the temperature evolution of the graphene Raman spectra are discussed. Finally, the relation between mechanical and thermal properties is presented along with the characterization of thermal properties of graphene with Raman spectroscopy.
We report results from two-dimensional Raman spectroscopy studies of large-area epitaxial graphene grown on SiC. Our work reveals unexpectedly large variation in Raman peak position across the sample resulting from inhomogeneity in the strain of the graphene film, which we show to be correlated with physical topography by coupling Raman spectroscopy with atomic force microscopy. We report that essentially strain free graphene is possible even for epitaxial graphene.
In this note, we report a Raman spectroscopy study of annealing-induced effects on graphene samples prepared by the microexfoliation method. It was shown that randomly located adhesive residues often contaminate nearby graphene sheets during thermal annealing. The contamination on graphene can be as thin as ~1 nm, but gives several new Raman bands of unusually strong intensity. We also find that their intensity is strongly dependent on the excitation wavelength implying that graphene-induced Raman enhancement may be operative. The current study also suggests that graphene can be selectively se…
Raman imaging on the edges of single layer micromechanical cleavage graphene (MCG) was carried out. The intensity of disorder-induced Raman feature (D band at ~1350 cm-1) was found to be correlated to the edge chirality: it is stronger at the armchair edge and weaker at the zigzag edge. This shows that Raman spectroscopy is a reliable and practical method to identify the chirality of graphene edge and to help in determination of the crystal orientation. The determination of graphene chirality is critically important for fundamental study as well as for applications.
Raman spectroscopic studies of graphene have attracted much interest. The G-band Raman intensity of a single layer graphene on Si substrate with 300 nm 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 …
The intensity ratio between two major Raman bands in graphene is one of the most important information for physics of graphene and has been believed to represent various intrinsic properties of graphene without critical assessment of extrinsic effects. We report a micro Raman spectroscopy study on the Raman intensity ratio of the 2D band to the G Raman band of graphene varying the thickness of dielectric layers (SiO_2) underneath it. The ratio is shown to change by almost 370% when the thickness is varied by 60%. The large variation in the ratio is well explained by theoretical calculations co…
We present a systematic study of the Raman spectra of optical phonons in graphene monolayers under tunable uniaxial tensile stress. Both the G and 2D bands exhibit significant red shifts. The G band splits into two distinct sub-bands (G+, G-) because of the strain-induced symmetry breaking. Raman scattering from the G+ and G- bands shows a distinctive polarization dependence that reflects the angle between the axis of the stress and the underlying graphene crystal axes. Polarized Raman spectroscopy therefore constitutes a purely optical method for the determination of the crystallographic orie…
Though graphene has been intensively studied by Raman spectroscopy, in this letter, we report a study of second-order overtone and combinational Raman modes in an unexplored range of 1690-2150 cm-1 in nonsuspended commensurate (AB-stacked), incommensurate (folded) and suspended graphene layers. Based on the double resonance theory, four dominant modes in this range have been assigned as 2oTO (M band), iTA+LO, iTO+LA and LO+LA. Differing to AB-stacked bilayer graphene or few layer graphene, the M band disappears in single layer graphene. Systematic analysis reveals that interlayer interaction i…
The room-temperature Raman signatures from graphene layers on sapphire and glass substrates were compared with those from graphene on GaAs substrate and on the standard Si/SiO2 substrate, which served as a reference. It was found that while G peak of graphene on Si/SiO2 and GaAs is positioned at 1580 cm-1 it is down-shifted by ~5 cm-1 for graphene-on-sapphire (GOS) and, in many cases, splits into doublets for graphene-on-glass (GOG) with the central frequency around 1580 cm-1. The obtained results are important for graphene characterization and its proposed graphene applications in electronic …
The unique properties of graphene offer immense opportunities for applications to many scientific fields, as well as societal needs, beyond our present imagination. One of the important features of graphene is the relatively simple tunability of its electronic structure, an asset which extends the usability of graphene even further beyond present experience. A direct injection of charge carriers into the conduction or valence bands, i.e., doping, represents a viable way of shifting the Fermi level. In particular, the electrochemical doping should be the method of choice, when higher doping lev…
Graphene has extraordinary mechanical and electronic properties, making it a promising material for membrane based nanoelectromechanical systems (NEMS). Here, chemical-vapor-deposited graphene is transferred onto target substrates to suspend it over cavities and trenches for pressure-sensor applications. The development of such devices requires suitable metrology methods, i.e., large-scale characterization techniques, to confirm and analyze successful graphene transfer with intact suspended graphene membranes. We propose fast and noninvasive Raman spectroscopy mapping to distinguish between fr…
Since graphene, a single sheet of graphite, has all of its carbon atoms on the surface, its property is very sensitive to materials contacting the surface. Herein, we report novel Raman peaks ob-served in annealed graphene and elucidate their chemical origins by Raman spectroscopy and atomic force microscopy (AFM). Graphene annealed in oxygen-free atmosphere revealed very broad additional Raman peaks overlapping the D, G and 2D peaks of graphene itself. Based on the topographic confirmation by AFM, the new Raman peaks were attributed to amorphous carbon formed on the surface of graphene by car…
In contrary to the widely reported single and symmetric peak feature of G' (or 2D) band in Raman spectrum of graphene, we herein report the observation of splitting in G' band in free standing graphene. Our experimental findings provide a direct and strong support for the previous theoretical prediction that the coexistence of the outer and inner processes in the doubleresonance Raman scattering would cause the splitting of G' mode. Our investigation of the influence of trigonal warping effect on the spectral features of G' subbands further verified the theoretical interpretation established o…
We report a Raman spectroscopy study of graphene field-effect transistors (GFET) with a controlled amount of defects introduced in graphene by exposure to electron-beam irradiation. Raman spectra are taken at T = 8 K over a range of back gate voltages (Vg) for various irradiation dosages (Re). We study effects in the Raman spectra due to Vg-induced doping and artificially created disorder at various Re. With moderate disorder (irradiation), the Raman G peak with respect to the graphene carrier density (nFE) exhibits a minimum in peak frequency and a maximum in peak width near the charge- neutr…
The properties of pristine, free-standing graphene monolayers prepared by mechanical exfoliation of graphite are investigated. The graphene monolayers, suspended over open trenches, are examined by means of spatially resolved Raman spectroscopy of the G-, D-, and 2D-phonon modes. The G-mode phonons exhibit reduced energies (1580 cm-1) and increased widths (14 cm-1) compared to the response of graphene monolayers supported on the SiO2 covered substrate. From analysis of the G-mode Raman spectra, we deduce that the free-standing graphene monolayers are essentially undoped, with an upper bound of…
The 1+1 layer folded graphene sheets that deviate from AB stacking are successfully fabricated and their electronic structures are investigated by Raman spectroscopy. Significant blue shift of the 2D band of folded graphene compared to that of single layer graphene (SLG) is observed. This is attributed to SLG-like electronic structure of folded graphene but with slowing down of Fermi velocity (as much as ~5.6%). Different amount of blue shift of 2D band is observed for different folded graphenes, which may correspond to the different twist angle and/or separation between the two layers, result…
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 recogniz…
In this report, we present Raman spectroscopy investigation of the thermal stability and dynamics of graphene edges. It was found that graphene edges (both armchair and zigzag) are not stable and undergo modifications even at temperature as low as 200°C. Based on polarized Raman results, we provide possible structural models on how graphene edges change during annealing. The zigzag edges rearrange and form armchair segments that are \pm30° relative to the edge direction, while armchair edges are dominated by armchair segments even at annealing temperature as high as 500°C. The modifications of…
We present a detailed calculation of intensities of two-phonon and four-phonon Raman peaks in graphene. Writing the low-energy hamiltonian of the interaction of electrons with the crystal vibrations and the electromagnetic field from pure symmetry considerations, we describe the system in terms of just a few independent coupling constants, considered to be parameters of the theory. The electron scattering rate is introduced phenomenologically as another parameter. The results of the calculation are used to extract information about these parameters from the experimentally measured Raman peak i…
We present an analysis of deep-UV Raman measurements of graphite, graphene and carbon nanotubes. For excitation energies above the strong optical absorption peak at the $M$ point in the Brillouin zone ($\approx 4.7\,\text{eV}$), we partially suppress double-resonant scattering processes and observe the two-phonon density of states of carbon nanomaterials. The measured peaks are assigned to contributions from LO, TO, and LA phonon branches, supported by calculations of the phonon dispersion. Moreover, we gain access to the infrared-active $E_{1u}$ mode in graphite. By lowering the excitation en…
The stacking faults (deviates from Bernal) will break the translational symmetry of multilayer graphenes and modify their electronic and optical behaviors to the extent depending on the interlayer coupling strength. This paper addresses the stacking-induced band splitting and folding effect on the electronic band structure of twisted bilayer graphene. Based on the first-principles density functional theory study, we predict that the band folding effect of graphene layers may enable the G band Raman double resonance in the visible excitation range. Such prediction is confirmed experimentally wi…
We report a Raman study of the so-called buffer layer with $(6\sqrt3\times6\sqrt3)R30^{\circ}$ periodicity which forms the intrinsic interface structure between epitaxial graphene and SiC(0001). We show that this interface structure leads to a nonvanishing signal in the Raman spectrum at frequencies in the range of the D- and G-band of graphene and discuss its shape and intensity. Ab-initio phonon calculations reveal that these features can be attributed to the vibrational density of states of the buffer-layer.
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 redshifts of 2D and G band (-27.8 cm^-1 and -14.2 cm^-1per 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 bandgap at K point can be realized. First principle calculations predicted a bandgap opening of ~300 meV for…
We present an \textit{ab initio} study based on density-functional theory of first- and second-order Raman spectra of graphene-based materials with different stacking arrangements and numbers of layers. Going from monolayer and bilayer graphene to periodic graphitic structures, we investigate the behavior of the first-order G-band and of the second-order 2D-band excited by the same set of photon energies. The former turns out to be very similar in all considered graphene-based materials, while in the latter we find the signatures of individual structures. With a systematic analysis of the seco…
We report a confocal Raman study on edges of single layer graphene. It is found that edge orientations could be identified by G mode besides D mode. We observe that G mode at edges of single layer graphene exhibits polar behaviors and different edges like zigzag- or armchair-dominated responses differently to the polarization of the incident laser. Moreover, G mode shows stiffening at zigzag-dominated edges, while it is softened at armchair- dominated ones. Our observations are in good agreement with recent theory (K. Sasaki, et al., J. Phys. Soc. Jpn. 79, 044603) and could be well explained b…
In a recent paper [Phys. Rev. B 78, 113407 (2008)], Poncharal et al. studied the Raman spectra of misoriented bilayer graphene. They found that the blueshift of 2D band of misoriented graphene relative to that of single layer graphene shows a strong dependence on the excitation laser energy. The blueshift increases with decreasing excitation energy. This finding contradicts our explanation of reduction of Fermi velocity of folded/misoriented graphene [Ni et al. Phys. Rev. B 77, 235403 (2008)]. In this comment, we present more experimental results from our group as well as from others to show t…
We present spatially resolved Raman images of the G and 2D lines of single-layer graphene flakes. The spatial fluctuations of G and 2D lines are correlated and are thus shown to be affiliated with local doping domains. We investigate the position of the 2D line -- the most significant Raman peak to identify single-layer graphene -- as a function of charging up to |n|~4 10^12 cm^-2. Contrary to the G line which exhibits a strong and symmetric stiffening with respect to electron and hole-doping, the 2D line shows a weak and slightly asymmetric stiffening for low doping. Additionally, the line wi…
We report strong variations in the Raman spectra for different single-layer graphene samples obtained by micromechanical cleavage, which reveals the presence of excess charges, even in the absence of intentional doping. Doping concentrations up to ~10^13 cm-2 are estimated from the G peak shift and width, and the variation of both position and relative intensity of the second order 2D peak. Asymmetric G peaks indicate charge inhomogeneity on the scale of less than 1 micron.
Theory has predicted rich and very distinct physics for graphene devices with boundaries that follow either the armchair or zigzag crystallographic directions. A prerequisite to disclose this physics in experiment is to be able to produce devices with boundaries of pure chirality. Exfoliated flakes frequently exhibit corners with an odd multiple of 30°, which raised expectations that their boundaries follow pure zigzag and armchair directions. The predicted Raman behavior at such crystallographic edges however failed to confirm pure edge chirality. Here, we perform confocal Raman spectroscopy …
Vibrational properties of graphene nanoribbons are examined with density functional based tight-binding method and non-resonant bond polarization theory. We show that the recently discovered reconstructed zigzag edge can be identified from the emergence of high-energy vibrational mode due to strong triple bonds at the edges. This mode is visible also in the Raman spectrum. Total vibrational density of states of the reconstructed zigzag edge is observed to resemble the vibrational density of states of armchair, rather than zigzag, graphene nanoribbon. Edge-related vibrational states increase in…
Graphene edges are of particular interest, since their chirality determines the electronic properties. Here we present a detailed Raman investigation of graphene flakes with well defined edges oriented at different crystallographic directions. The position, width and intensity of G and D peaks at the edges are studied as a function of the incident light polarization. The D-band is strongest for light polarized parallel to the edge and minimum for perpendicular orientation. Raman mapping shows that the D peak is localized in proximity of the edge. The D to G ratio does not always show a signifi…
As the synthesis of graphene on copper became one of the primary preparation methods for both fundamental research and industrial application, Raman spectra of graphene/Cu systems need to be quantitatively understood regarding how their interactions affect the electronic structure of graphene. Using multi-wavelength Raman spectroscopy, we investigated three types of graphene bound on Cu: graphene grown on Cu foils and Cu film/SiO2, and Cu-evaporated exfoliated graphene. 2D peak frequencies of the first two samples were ~17 cm-1 higher than expected for 1.96 eV excitation even when the effect o…
The fabrication of epitaxial graphene (EG) on SiC substrate by annealing has attracted a lot of interest as it may speed up the application of graphene for future electronic devices. The interaction of EG and the SiC substrate is critical to its electronic and physical properties. In this work, Raman spectroscopy was used to study the structure of EG and its interaction with SiC substrate. All the Raman bands of EG blue shift from that of bulk graphite and graphene made by micromechanical cleavage, which was attributed to the compressive strain induced by the substrate. A model containing 13 x…
Raman spectroscopy plays a key role in studies of graphene and related carbon systems. Graphene is perhaps the most promising material of recent times for many novel applications, including electronics. In this paper, the traditional and well established Kramers-Heisenberg-Dirac (KHD) Raman scattering theory (1925-1927) is extended to crystalline graphene for the first time. It demands different phonon production mechanisms and phonon energies than does the popular "double resonance" Raman scattering model. The latter has never been compared to KHD. Within KHD, phonons are produced instantly a…
Raman spectroscopy is a powerful tool for characterizing the local properties of graphene. Here, we introduce a method for evaluating unknown strain configurations and simultaneous doping. It relies on separating the effects of hydrostatic strain (peak shift) and shear strain (peak splitting) on the Raman spectrum of graphene. The peak shifts from hydrostatic strain and doping are separated with a correlation analysis of the 2D and G frequencies. This enables us to obtain the local hydrostatic strain, shear strain and doping without any assumption on the strain configuration prior to the analy…
The electronic structure and structural evolution of hydrogenated graphene are investigated by Raman spectroscopy with multiple excitations. The excitation energy dependent saturation effect on the ratio of integrated intensities of D and G modes (ID/IG) is revealed and further developed as a quick method for estimation of inter-defect distance and defect density in hydrogenated graphene. At low hydrogen coverage, the chemisorbed H atoms behave like defects in sp2 C=C matrix; while for a high hydrogen coverage, the sp3 C-H bonds become coalescent clusters, resulting in confinement effect on th…
Accurate and simple local strain assessment in graphene is one of the crucial tasks in device characterization. Raman spectroscopy is often used for that purpose through monitoring of the G and 2D modes. However, the shifts of those two bands might be biased, especially under uniaxial strain, by the effects of charge-transfer doping. Therefore, it is extremely desirable to use another Raman band, less affected by doping, but with a defined and measurable behavior under strain. The Raman 2D' mode is in this sense the ideal feature for the evaluation of strain levels in stretched graphene monola…
The symmetry group analysis is applied to classify the phonon modes of $N$-stacked graphene layers (NSGL's) with AB- and AA-stacking, particularly their infra-red and Raman properties. The dispersions of various phonon modes are calculated in a multi-layer vibrational model, which is generalized from the lattice vibrational potentials of graphene to including the inter-layer interactions in NSGL's. The experimentally reported red shift phenomena in the layer number dependence of the intra-layer optical C-C stretching mode frequencies are interpreted. An interesting low frequency inter-layer op…
Charged impurity (CI) scattering is one of the dominant factors that affect the carrier mobility in graphene. In this paper, we use Raman spectroscopy to probe the charged impurities in suspended graphene. We find that the 2D band intensity is very sensitive to the CI concentration in graphene, while the G band intensity is not affected. The intensity ratio between the 2D and G bands, I2D/IG, of suspended graphene is much stronger compared to that of non-suspended graphene, due to the extremely weak CI scattering in the former. This finding is consistent with the ultra-high carrier mobility in…
The absolute integrated intensity of the single-phonon Raman peak at 1580 cm^{-1} is calculated for a clean graphene monolayer. The resulting intensity is determined by the trigonal warping of the electronic bands and the anisotropy of the electron-phonon coupling, and is proportional to the second power of the excitation frequency. The main contribution to the process comes from the intermediate electron-hole states with typical energies of the order of the excitation frequency, contrary to what has been reported earlier. This occurs because of strong cancellations between different terms of …
We report the growth of thickness-controlled rotationally faulted multilayer graphene (rf-MLG) on Ni foils by low-pressure chemical vapor deposition and their characterization by micro-Raman spectroscopy. The surface morphology and thickness were investigated by scanning electron microscope, X-ray diffraction, and transmittance measurements. These results have revealed that the thickness of rf-MLG can be effectively controlled by the thickness of the Ni foil rather than the flow rate of CH$_4$, H$_2$, Ar. In the Raman spectroscopy measurements, we observed most Raman peaks of the graphitic mat…
In this paper, we report our study on gold (Au) films with different thicknesses deposited on single layer graphene (SLG) as surface enhanced Raman scattering (SERS) substrates for the characterization of rhodamine (R6G) molecules. We find that an Au film with a thickness of ~7 nm deposited on SLG is an ideal substrate for SERS, giving the strongest Raman signals for the molecules and the weakest photoluminescence (PL) background. While Au films effectively enhance both the Raman and PL signals of molecules, SLG effectively quenches the PL signals from the Au film and molecules. The former is …
The Raman shift, broadening, and relative Raman intensities of bilayer graphene are computed as functions of the electron concentration. We include dynamic effects for the phonon frequencies and we consider the gap induced in the band structure of bilayer graphene by an external electric field. We show that from the analysis of the Raman spectra of gated bilayer graphene it is possible to quantitatively identify the amount of charges coming from the atmosphere and from the substrate. These findings suggest that Raman spectroscopy of bilayer graphene can be used to characterize the electrostati…
The effect of grain boundaries and wrinkles on the electrical properties of polycrystalline graphene is pronounced. Here we investigate the stitching between grains of polycrystalline graphene, specifically, overlapping of layers at the boundaries, grown by chemical vapor deposition (CVD) and subsequently doped by the oxidized Cu substrate. We analyze overlapped regions between 60 and 220 nm wide via Raman spectroscopy, and find that some of these overlapped boundaries contain AB stacked bilayers. The Raman spectra from the overlapped grain boundaries are distinctly different from bilayer grap…
We describe Raman spectroscopy based method of measuring thermal conductivity of thin films, and review significant results achieved with this technique pertinent to graphene and other two-dimensional materials. The optothermal Raman method was instrumental for the discovery of unique heat conduction properties of graphene. In this method, Raman spectroscopy is used to determine the local temperature of the sample while the excitation laser is utilized as a heat source. The success of Raman spectroscopy in investigating thermal conductivity of suspended graphene and graphene-based thin films m…
Raman spectra were measured for mono-, bi- and trilayer graphene grown on SiC by solid state graphitization, whereby the number of layers was pre-assigned by angle-resolved ultraviolet photoemission spectroscopy. It was found that the only unambiguous fingerprint in Raman spectroscopy to identify the number of layers for graphene on SiC(0001) is the linewidth of the 2D (or D*) peak. The Raman spectra of epitaxial graphene show significant differences as compared to micromechanically cleaved graphene obtained from highly oriented pyrolytic graphite crystals. The G peak is found to be blue-shift…
Nanometer-scale graphene objects are attracting much research interest because of newly emerging properties originating from quantum confinement effects. We present Raman spectroscopy studies of graphene nanoribbons (GNRs) which are known to have nonzero electronic bandgap. GNRs of width ranging from 15 nm to 100 nm have been prepared by e-beam lithographic patterning of mechanically exfoliated graphene followed by oxygen plasma etching. Raman spectra of narrow GNRs can be characterized by upshifted G band and prominent disorder-related D band originating from scattering at ribbon edges. The D…
The vibrational properties of twisted bilayer graphene (tBLG) show complex features, due to the intricate energy landscape of its low-symmetry configurations. A machine learning-based approach is developed to provide a continuous model between the twist angle and the simulated Raman spectra of tBLGs. Extracting the structural information of the twist angle from Raman spectra corresponds to solving a complicated inverse problem. Once trained, the machine learning regressors (MLRs) quickly provide predictions without human bias and with an average of 98% of the data variance being explained by t…
We present detailed multi frequency resonant Raman measurements of potassium graphite intercalation compounds (GICs). From a well controlled and consecutive in-situ intercalation and high temperature de-intercalation approach the response of each stage up to stage VI is identified. The positions of the G and 2D lines as a function of staging depend on the charge transfer from K to the graphite layers and on the lattice expansion. Ab-initio calculations of the density and the electronic band-structure demonstrate that most (but not all) of the transferred charge remains on the graphene sheets a…
We review the different results obtained in the last decade in the field of Raman scattering of graphene based systems, with an applied magnetic field. Electronic properties of graphene based systems with an applied magnetic field will first be described. The phonon response in magnetic field, the magneto-phono resonance, will then be introduced and described in different systems, including graphene, multilayer graphene and bulk graphite. Electronic Raman scattering is then be discussed in the context of Landau level spectroscopy, of electron phonon interaction and of electron-electron interac…
We synthesized three-dimensional nanoporous graphene films by a chemical vapor deposition method with nanoporous copper as a catalytic substrate. The resulting nanoporous graphene has the same average pore size as the underlying copper substrate. Our surface-enhanced Raman scattering (SERS) investigation indicates that the nanoporosity of graphene significantly improves the SERS efficiency of graphene as a substrate as compared to planar graphene substrates.
We investigated Raman spectra of single-layer and multi-layer graphene under ultraviolet laser excitation at the wavelength of 325 nm. It was found that while the G peak of graphene 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 nm and 633 nm wavelengths. The 2D band under UV excitation shifts to larger wave number…
We calculate the probabilities of two- and four-phonon Raman scattering in graphene and show how the relative intensities of the overtone peaks encode information about relative rates of different inelastic processes electrons are subject to. If the most important processes are electron-phonon and electron-electron scattering, the rate of the latter can be deduced from the Raman spectra.
Graphene layers placed on SrTiO3 single-crystal substrates were investigated using temperature-dependent confocal Raman spectroscopy. This approach successfully resolved distinct Raman modes of graphene that are often untraceable in conventional measurements due to the strong Raman scattering background of SrTiO3. Information on defects and strain states was obtained for a few graphene/SrTiO3 samples that were synthesized by different techniques. This confocal Raman spectroscopic approach can shed light on the investigation of not only this graphene/SrTiO3 system but also various two-dimension…
The results of micro-Raman scattering measurements performed on three different ``graphitic'' materials: micro-structured disks of highly oriented pyrolytic graphite, graphene multi-layers thermally decomposed from carbon terminated surface of 4H-SiC and an exfoliated graphene monolayer are presented. Despite its multi-layer character, most parts of the surface of the graphitized SiC substrates shows a single-component, Lorentzian shape, double resonance Raman feature in striking similarity to the case of a single graphene monolayer. Our observation suggests a very weak electronic coupling bet…
We show the evolution of Raman spectra with number of graphene layers on different substrates, SiO$_{2}$/Si and conducting indium tin oxide (ITO) plate. The G mode peak position and the intensity ratio of G and 2D bands depend on the preparation of sample for the same number of graphene layers. The 2D Raman band has characteristic line shapes in single and bilayer graphene, capturing the differences in their electronic structure. The defects have a significant influence on the G band peak position for the single layer graphene: the frequency shows a blue shift upto 12 cm$^{-1}$ depending on th…
The paper reports a theoretical study of scattering of electrons by edges in graphene and its effect on Raman scattering. First, effective models are discussed for translationally invariant and rough edges. Second, they are used in a calculation of the edge-activated Raman D peak intensity and its dependence on the polarization of the incident/scattered light, as well as on the position of the excitation spot. Manifestations of the quasiclassical character of electron motion in Raman scattering are discussed.
A simple, non-invasive method using Raman spectroscopy for the estimation of the thickness of graphene layers grown epitaxially on silicon carbide (SiC) is presented, enabling simultaneous determination of thickness, grain size and disorder using the spectra. The attenuation of the substrate Raman signal due to the graphene overlayer is found to be dependent on the graphene film thickness deduced from X-ray photoelectron spectroscopy and transmission electron microscopy of the surfaces. We explain this dependence using an absorbing overlayer model. This method can be used for mapping graphene …
Surface enhanced Raman scattering (SERS) exploits surface plasmons induced by the incident field in metallic nanostructures to significantly increase the Raman intensity. Graphene provides the ideal prototype two dimensional (2d) test material to investigate SERS. Its Raman spectrum is well known, graphene samples are entirely reproducible, height controllable down to the atomic scale, and can be made virtually defect-free. We report SERS from graphene, by depositing arrays of Au particles of well defined dimensions on graphene/SiO$_2$(300nm)/Si. We detect significant enhancements at 633nm. To…
