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We perform transmission electron microscopy, electron diffraction, and Raman scattering experiments on an individual suspended double-walled carbon nanotube (DWCNT). The first two techniques allow the unambiguous determination of the DWCNT structure: (12,8)@(16,14). However, the low-frequency features in the Raman spectra cannot be connected to the derived layer diameters d by means of the 1/d power law, widely used for the diameter dependence of the radial-breathing mode of single-walled nanotubes. We discuss this disagreement in terms of mechanical coupling between the layers of the DWCNT, which results in collective vibrational modes. Theoretical predictions for the breathing-like modes of the DWCNT, originating from the radial-breathing modes of the layers, are in a very good agreement with the observed Raman spectra. Moreover, the mechanical coupling qualitatively explains the observation of Raman lines of breathing-like modes, whenever only one of the layers is in resonance with the laser energy.

The ultimate surface exposure provided by graphene monolayer makes it the ideal sensor platform but also exposes its intrinsic properties to any environmental perturbations. In this work, we demonstrate that the charge carrier density of graphene exfoliated on a SiO2/Si substrate can be finely and reversibly tuned between hole and electron doping with visible photons. This photo-induced doping happens under moderate laser power conditions but is significantly affected by the substrate cleaning method. In particular, it requires hydrophilic substrates and vanishes for suspended graphene. These findings suggest that optically gated graphene devices operating with a sub-second time scale can be envisioned and that Raman spectroscopy is not always as non-invasive as generally assumed.

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From combined Raman spectroscopy and electron diffraction studies on several freestanding single-walled carbon nanotubes (SWNTs), we define Raman criteria which correlate the main features of the Raman spectrum (radial breathing mode and G modes) and the optical transition energies with the structure of the SWNT under investigation. On this basis, we discuss the possibilities to determine the (n,m) indices of an individual SWNT from a single wavelength Raman experiment. We show the efficiency of this approach in assigning the (n,m) structure of different individual nanotubes including all types of achiral SWNTs. Finally, the limits and the accuracy of the method are discussed

We report in situ Raman scattering experiments on single-layer graphene (SLG) and Bernal bilayer graphene (BLG) during exposure to rubidium vapor. The G- and 2D-band evolutions with doping time are presented and analyzed. On SLG, the extended doping range scanned (up to about 10(14) electrons/cm(2)) allows the observation of three regimes in the evolution of the G-band frequency: a continuous upshift followed by a plateau and a downshift. Overall the measured evolution is interpreted as the signature of the competition between dynamic and adiabatic effects upon n-doping. Comparison of the obtained results with theoretical predictions indicates however that a substrate pinning effect occurs and inhibits charge-induced lattice expansion of SLG. At low doping, a direct link between electrostatic gating and Rb doping results is presented. For BLG, the added electrons are shown to be first confined in the top layer, but the system evolves with time toward a more symmetric repartition of the added electrons in both layers. The results obtained on BLG also confirm that the slope of the phonon dispersion close to the K point tends to be slightly reduced at low doping but suggest the occurrence of an unexpected increase of the phonon dispersion slope at higher electron concentration.

The experimental approach combining high resolution transmission electron microscopy (HRTEM), electron diffraction (ED) and resonant Raman spectroscopy (RRS) on the same freestanding 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 singlewalled (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 indexidentified 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.

Discrete nickel catalyst nanoparticles (NP) have been used to grow isolated single-walled carbon nanotubes by chemical vapor deposition (CVD). Atomic force microscopy (AFM), transmission electron microscopy (TEM) and micro-Raman spectroscopy are used to characterize these as-grown, isolated nanotubes. Using a conventional setup, we are able to produce narrow diameter distribution single-walled carbon nanotubes (SWNTs) (1.45 ( 0.5 nm), showing a clear mismatch with the larger broad size distribution of the catalyst nanoparticles (4.7 ( 1.5 nm). Investigation of the growth conditions allowed us to synthesize, starting with the same catalyst materials, various carbon nanotube (CNT) samples with a wide range of characteristics. The advantages of such a versatile CVD method for the study of physical properties at the single nanotube level are illustrated by means of two prospective studies on SWNTs mechanical and vibrational properties.