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Register a new userSynthesis of nitrogen doped single wall carbon nanotubes with caffeine
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Nitrogen doped single wall carbon nanotubes have many functional benefits. Doping opens the possibility to control the electronic energy levels, surface energy, surface reactivity and charge carrier density. The additional electron in the outer shell changes the electronic properties of the nanotubes when introduced into the carbon lattice. Here we present the latest findings in the in-situ doping during synthesis of single wall carbon nanotubes using caffeine as a precursor of both carbon and nitrogen. A special furnace with two heating elements allowed us to sublimate and decompose the solid precursor. Caffeine allowed us to reach a high doping percentage with high quality nanotubes directly in a one-step synthesis procedure.
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Having access to the chemical environment at the atomic level of a dopant in a nanostructure is crucial for the understanding of its properties. We have performed atomically-resolved electron energy-loss spectroscopy to detect individual nitrogen dopants in single-walled carbon nanotubes and compared with first principles calculations. We demonstrate that nitrogen doping occurs as single atoms in different bonding configurations: graphitic-like and pyrrolic-like substitutional nitrogen neighbouring local lattice distortion such as Stone-Thrower-Wales defects. The stability under the electron beam of these nanotubes has been studied in two extreme cases of nitrogen incorporation content and configuration. These findings provide key information for the applications of these nanostructures.
Photoluminescence (PL) measurements of porphyrin-doped single wall carbon nanotubes (SWNT) were studied in sodium dodecylbenzenesulfonate (NaDDBS) aqueous dispersions. The PL spectra were used to draw PL maps were the maxima corresponds to absorption-emission excitonic processes related to (E11, E22) first Van Hove singularities of the SWNT electronic structure. The influence of the net charge of the porphyrin was a determinant factor in the energy map maximum shifts (EMMS) compared to the energy map of a pristine NaDDBS/SWNT dispersion. A non-interacting porphyrin is used as a reference to discard the influence of the dielectric constant of the medium in the EMMS.
The circular dichroism (CD) spectra of single-wall carbon nanotubes are calculated using a dipole approximation. The calculated CD spectra show features that allow us to distinguish between nanotubes with different angles of chirality, and diameters. These results provide theoretical support for the quantification of chirality and its measurement, using the CD lineshapes of chiral nanotubes. It is expected that this information would be useful to motivate further experimental studies.
A novel method is presented which allows the characterization of diameter selective phenomena in SWCNTs. It is based on the transformation of fullerene peapod materials into double-wall carbon nanotubes and studying the diameter distribution of the latter. The method is demonstrated for the diameter selective healing of nanotube defects and yield from C$_{70}$ peapod samples. Openings on small diameter nanotubes are closed first. The yield of very small diameter inner nanotubes from C$_{70}$ peapods is demonstrated. This challenges the theoretical models of inner nanotube formation. An anomalous absence of mid-diameter inner tubes is observed and explained by the suppressed amount of C$_{70}$ peapods due to the competition of the two almost equally stable standing and lying C$_{70}$ peapod configurations.
While addition of electrolyte to sodium dodecyl sulfate suspensions of single-wall carbon nanotubes has been demonstrated to result in significant brightening of the nanotube photoluminescence (PL), the brightening mechanism has remained unresolved. Here, we probe this mechanism using time-resolved PL decay measurements. We find that PL decay times increase by a factor of 2 on addition of CsCl as the electrolyte. Such an increase directly parallels an observed near-doubling of PL intensity, indicating the brightening results primarily from changes in nonradiative decay rates associated with exciton diffusion to quenching sites. Our findings indicate that a reduced number of these sites results from electrolyte-induced reorientation of the surfactant surface structure that partially removes pockets of water from the tube surface where excitons can dissociate, and thus underscores the contribution of interfacial water in exciton recombination processes.
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