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Raman spectroscopy is a fast, non-destructive means to characterize graphene samples. In particular, the Raman spectra show a significant dependence on doping. While the change in position and width of the G peak can be explained by the non-adiabatic Kohn anomaly at $\Gamma$, the significant doping dependence of the 2D peak intensity has not been explained yet. Here we show that this is due to a combination of electron-phonon and electron-electron scattering. Under full resonance, the photogenerated electron-hole pairs can scatter not just with phonons, but also with doping-induced electrons or holes, and this changes the intensity. We explain the doping dependence and show how it can be used to determine the corresponding electron-phonon coupling. This is higher than predicted by density-functional theory, as a consequence of renormalization by Coulomb interactions., Comment: Refs added, typos corrected, submitted to PRB

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 significant dependence on edge orientation. Thus, even though edges can appear macroscopically smooth and oriented at well defined angles, they are not necessarily microscopically ordered.

We report phonon renormalisation in bilayer graphene as a function of doping. The Raman G peak stiffens and sharpens for both electron and hole doping, as a result of the non-adiabatic Kohn anomaly at the $\Gamma$ point. The bilayer has two conduction and valence subbands, with splitting dependent on the interlayer coupling. This results in a change of slope in the variation of G peak position with doping, which allows a direct measurement of the interlayer coupling strength., Comment: 5 figures

We measure the temperature dependence of the Raman spectra of metallic and semiconducting nanotubes. We show that the different trend in metallic tubes is due to phonon re-normalization induced by the variation in electronic temperature, which is modeled including non-adiabatic contributions to account for the dynamic, time dependent nature, Comment: 5 pages, 3 figures

Graphene nanoribbons are the counterpart of carbon nanotubes in graphene-based nanoelectronics. We investigate the electronic properties of chemically modified ribbons by means of density functional theory. We observe that chemical modifications of zigzag ribbons can break the spin degeneracy. This promotes the onset of a semiconducting-metal transition, or of an half-semiconducting state, with the two spin channels having a different bandgap, or of a spin-polarized half-semiconducting state -where the spins in the valence and conduction bands are oppositely polarized. Edge functionalization of armchair ribbons gives electronic states a few eV away from the Fermi level, and does not significantly affect their bandgap. N and B produce different effects, depending on the position of the substitutional site. In particular, edge substitutions at low density do not significantly alter the bandgap, while bulk substitution promotes the onset of semiconducting-metal transitions. Pyridine-like defects induce a semiconducting-metal transition., Comment: 12 pages, 5 figures

We demonstrate electrochemical top gating of graphene by using a solid polymer electrolyte. This allows to reach much higher electron and hole doping than standard back gating. In-situ Raman measurements monitor the doping. The G peak stiffens and sharpens for both electron and hole doping, while the 2D peak shows a different response to holes and electrons. Its position increases for hole doping, while it softens for high electron doping. The variation of G peak position is a signature of the non-adiabatic Kohn anomaly at $\Gamma$. On the other hand, for visible excitation, the variation of the 2D peak position is ruled by charge transfer. The intensity ratio of G and 2D peaks shows a strong dependence on doping, making it a sensitive parameter to monitor charges., Comment: 7 pages, 8 figures

Graphene is the two-dimensional (2d) building block for carbon allotropes of every other dimensionality. It can be stacked into 3d graphite, rolled into 1d nanotubes, or wrapped into 0d fullerenes. Its recent discovery in free state has finally provided the possibility to study experimentally its electronic and phonon properties. Here we show that graphene's electronic structure is uniquely captured in its Raman spectrum that clearly evolves with increasing number of layers. Raman fingerprints for single-, bi- and few-layer graphene reflect changes in the electronic structure and electron-phonon interactions and allow unambiguous, high-throughput, non-destructive identification of graphene layers, which is critically lacking in this emerging research area.

We prove that Electron-phonon coupling (EPC) is the major source of broadening for the Raman G and G- peaks in graphite and metallic nanotubes. This allows us to directly measure the optical-phonon EPCs from the G and G- linewidths. The experimental EPCs compare extremely well with those from density functional theory. We show that the EPC explains the difference in the Raman spectra of metallic and semiconducting nanotubes and their dependence on tube diameter. We dismiss the common assignment of the G- peak in metallic nanotubes to a Fano resonance between phonons and plasmons. We assign the G+ and G- peaks to TO (tangential) and LO (axial) modes., Comment: 5 pages, 4 figures (correction in label of fig 3)

We demonstrate the key role of phonon occupation in limiting the high-field ballistic transport in metallic carbon nanotubes. In particular, we provide a simple analytic formula for the electron transport scattering length, that we validate by accurate first principles calculations on (6,6) and (11,11) nanotubes. The comparison of our results with the scattering lengths fitted from experimental I-V curves indicates the presence of a non-equilibrium optical phonon heating induced by electron transport. We predict an effective temperature for optical phonons of thousands Kelvin., Comment: 4 pages, 1 figure

We demonstrate that graphite phonon dispersions have two Kohn anomalies at the Gamma-E_2g and K-A'1 modes. The anomalies are revealed by two sharp kinks. By an exact analytic derivation, we show that the slope of these kinks is proportional to the square of the electron-phonon coupling (EPC). Thus, we can directly measure the EPC from the experimental dispersions. The Gamma-E_2g and K-A'1 EPCs are particularly large, whilst they are negligible for all the other modes at Gamma and K., Comment: 4 pages, 2 figures