Raman spectroscopy is commonly used to determine the number of layers of few-layer graphene (FLG)samples. In this work, we focus on the criteria based on the G-band integrated intensity and on the laseroptical contrast. Limitations due to stacking order are discussed and lead to the conclusion that it isnecessary to combine Raman and optical contrast to avoid misinterpretation. Both methods enable todistinguish unambiguously between single layer graphene and multilayer graphene. However, neithereach method separately nor the combination of the two enable a determination of the number of layers forall possible stacking orientations. Importantly, since the two methods always significantly disagree whenthey fail, the comparison of the values deduced by each method allows to discriminate if the determinednumber of layers can be specified or not. Other important parameters (substrate, laser wavelength,objective numerical aperture) are discussed to define a reliable method to determine the number ofgraphene layers in FLG and its domain of validity. The proposed method which combines Raman andoptical contrast measurements, carried out with a 532 nm laser and using a 100x objective with anumerical aperture of 0.9, allows the determination of the number of layers for (up to 5) FLG on thefollowing substrates: (i) glass (soda lime glass or similar with refractive index between 1.50 and 1.55) and(ii) oxidized silicon (SiO2 on silicon, with a SiO2 thickness of 90 ± 5 nm). The method is however limited tohigh quality graphene and FLG with small defect density and low residue.

Double-walled carbon nanotubes (DWNT) are made of two concentric and weakly van der Waals coupled single-walled carbon nanotubes (SWNT). DWNTs are the simplest systems for studying the mechanical and electronic interactions between concentric carbon layers.In this paper we review recent results concerning the intrinsic features of phonons of DWNTs obtained from Raman experiments performed on index-identified DWNTs. The effect of the interlayer distance on the strength of the mechanical and electronic coupling between the layers, and thus on the frequencies of the Raman-active modes, namely the radial breathinglikemodes (RBLMs) and G-modes, are evidenced and discussed.

We present experimental measurements of the features of G band in individual index-identified free-standing double-walled carbon nanotubes. We examine Raman spectra of different electronic configurations of DWNTs, namely: SC@SC, SC@M, M@SC, M@M, and clearly establish that, as in SWNTs, the profile of LO G-mode of each layer is broad (narrow) when the layer is metallic (semiconducting). The dependence of G-modes on thediameter and inter-layer distance in several SC@SC, SC@M, M@SC, M@M index-identified DWNTs is reported. We find, that, independently of the metallic or semiconducting nature of the layers, the frequencies of LO and TO G-mode of the inner and outer layers shift significantly with respect to the frequencies of the same modes in the constituent SWNTs.

We report direct and unambiguous evidence of the existence of inner semiconducting tube (ISCT) photoluminescence (PL) from measurements performed on four individual freestanding index-identified double-walled carbon nanotubes (DWNTs). Based on thorough Rayleigh scattering, Raman scattering, and PL experiments, we are able to demonstrate that the ISCT PL is observed with a quantum yield estimated to be a few 10−6 independent of the semiconducting or metallic nature of the outer tube. This result is mainly attributed to ultrafast exciton transfer from the inner to outer tube. Furthermore, by carrying out PL excitation experiments on the (14,1)@(15,12) DWNT, we show that the ISCT PL can be detected through the optical excitation of the outer tube, indicating that the exciton transfer can also occur in the opposite way.

The effects of quantum interferences on the excitation dependence of the intensity of G modes have beeninvestigated on single-walled carbon nanotubes [Duque et al., Phys. Rev. Lett. 108, 117404 (2012)]. In this work,by combining optical absorption spectroscopy and Raman scattering on individual index identified double-walledcarbon nanotubes, we examine the experimental excitation dependence of the intensity of longitudinal opticaland transverse optical G modes of the constituent inner and outer single-walled carbon nanotubes. The observedstriking dependencies are understood in terms of quantum interference effects. Considering such effects, the excitation dependence of the different components of the G modes permits us to unambiguously assign each ofthem as originating from the longitudinal or transverse G modes of inner and outer tubes.

Silicon carbide (SiC) sublimation is the most promising option to achieve transfer-free graphene at the wafer-scale. We investigated the initial growth stages from the buffer layer to monolayer graphene on SiC(0001) as a function of annealing temperature at low argon pressure (10 mbar). A buffer layer, fully covering the SiC substrate, forms when the substrate is annealed at 1600°C. Graphene formation starts from the step edges of the SiC substrate at higher temperature (1700°C). The spatial homogeneity of the monolayer graphene was observed at 1750°C, as characterized by Raman spectroscopy and magneto-transport. Raman spectroscopy mapping indicated an AG-graphene/AG-HOPG ratio of around 3.3%, which is very close to the experimental value reported for a graphene monolayer. Transport measurements fromroom temperature down to 1.7 K indicated slightly p-doped samples (p~10^10cm-2) and confirmed both continuity and thickness of the monolayer graphene film. Successive growth processes have confirmed the reproducibility and homogeneity of these monolayer films.

The experimental approach combining high resolution transmission electron microscopy (HRTEM), electron diffraction (ED) and resonant Raman spectroscopy (RRS) on the same free-standing individual carbon nanotubes (CNT) is the most efficient method to determine unambiguously the intrinsic features of the Raman-active phonons. In this paper, we review the main results obtained by the approach regarding the intrinsic features of the phonons of single-walled (SWNT) and double-walled carbon nanotubes (DWNT). First, we detail the different methods to identify the structure of SWNTs and DWNTs from the analysis of their electron diffraction patterns (EDP). In the following, we remind the principal features of the Raman response of SWNTs, unambiguously index-identified by ED. A special attention is devoted to the effect of the inter-layer interaction on the frequencies of the Raman-active phonons in index-identified DWNTs. The information obtained on index-identified SWNT and DWNT allows us to propose Raman criteria, which help identifying CNT when the ED fails to propose a single assignment. The efficiency of the Raman criteria as the complement to the ED information for the index-assignment of a few SWNTs and DWNTs is shown. The same approach to index-assign a triple-walled carbon nanotube (TWNT), by combining ED and RRS information, is reported.