Fluorescence has been observed directly across the band gap of semiconducting carbon nanotubes. We obtained individual nanotubes, each encased in a cylindrical micelle, by ultrasonically agitating an aqueous dispersion of raw single-walled carbon nanotubes in sodium dodecyl sulfate and then centrifuging to remove tube bundles, ropes, and residual catalyst. Aggregation of nanotubes into bundles otherwise quenches the fluorescence through interactions with metallic tubes and substantially broadens the absorption spectra. At pH less than 5, the absorption and emission spectra of individual nanotubes show evidence of band gap-selective protonation of the side walls of the tube. This protonation is readily reversed by treatment with base or ultraviolet light.
Spectrofluorimetric measurements on single-walled carbon nanotubes (SWNTs) isolated in aqueous surfactant suspensions have revealed distinct electronic absorption and emission transitions for more than 30 different semiconducting nanotube species. By combining these fluorimetric results with resonance Raman data, each optical transition has been mapped to a specific (n,m) nanotube structure. Optical spectroscopy can thereby be used to rapidly determine the detailed composition of bulk SWNT samples, providing distributions in both tube diameter and chiral angle. The measured transition frequencies differ substantially from simple theoretical predictions. These deviations may reflect combinations of trigonal warping and excitonic effects.
Spectrofluorimetric data for identified single-walled carbon nanotubes in aqueous SDS suspension have been accurately fit to empirical expressions. These are used to obtain the first model-independent prediction of first and second van Hove optical transitions as a function of structure for a wide range of semiconducting nanotubes. To allow for convenient use in support of spectral studies, the results are presented in equation, graphical, and tabular forms. These empirical findings differ significantly from Kataura plots computed using a simple tightbinding model. It is suggested that the empirically based results should be used in preference to conventional model-based predictions in spectroscopic nanotube research.
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