| Description |
This work is a study of the optical properties of single-wall carbon nanotubes (SWNTs) using continuous wave (CW) modulation spectroscopy and resonant Raman scattering. SWNTs comprise a nanoscale, quasi-1D system in which the electrons are strongly interacting, resulting in the photo-generation of excitons. Our optical studies have revealed the behavior of these excitons under a number of di fferent perturbations to the system. We have used absorption, reflectance, electro-absorption (EA), photo-induced absorption (PA), charge-induced absorption (CIA), and resonant Raman scattering (RRS) on films of SWNTs. Our EA results provide strong evidence for the dominance of excitons in the optical absorption spectra of SWNT films. The absence of Franz-Keldysh oscillations and the presence of a derivative-like structure of the EA spectra indicate that the oscillator strength goes to the generation of excitons and not to interband electronic transitions. Furthermore, some of the photo-generated excitons are long-lived due to charge trapping in individual tubes within bundles, and this leads to a PA spectrum that is extraordinarily similar to the EA signal. When SWNTs are electrochemically doped we see that the exciton absorption is bleached due to k-space fi lling and screening of the excitons by the modi ed local dielectric, while there is very little shift in the exciton transition energies due to band-gap renormalization. Simultaneously the infrared absorption, which is due to Drude free-carriers absorption, is enhanced. A similar behavior is observed in the case of direct charge injection. The RRS of doped SWNT samples shows a frequency shift of many of the Raman-active modes that is commensurate with the macroscopic actuation observed in nanotube-based electrochemical devices. This indicates that doping-induced changes in the lattice are connected with softening and sti ening of the vibrational modes. Our results impact many proposed technologies that exploit the unique prop-erties of SWNTs. Displays, batteries, and even photovoltaics that incorporate nanotubes are already in development. The performance and robustness of these devices could be improved when our results are taken into account. |
