Midinfrared third-harmonic generation from macroscopically aligned ultralong single-wall carbon nanotubes

We report the observation of strong third-harmonic generation from a macroscopic array of aligned ultralong single-wall carbon nanotubes (SWCNTs)with intensemidinfrared radiation. Through power-dependent experiments, we determined the absolute value of the third-order nonlinear optical susceptibility !(3) of our SWCNT film to be 5.53 × 10−12 esu, three orders of magnitude larger than that of the fused silica reference we used. Taking account of the filling factor of 8.75% for our SWCNT film, we estimate a !(3) of 6.32 × 10−11 esu for a fully dense film. Furthermore, through polarization-dependent experiments, we extracted all the nonzero elements of the !(3) tensor, determining the magnitude of the weaker tensor elements to be #1/6 of that of the dominant !(3) zzzz component

Ultrafast Optical Spectroscopy of Micelle-Suspended Single-Walled Carbon Nanotubes

We present results of wavelength-dependent ultrafast pump-probe experiments on micelle-suspended single-walled carbon nanotubes. The linear absorption and photoluminescence spectra of the samples show a number of chirality-dependent peaks, and consequently, the pump-probe results sensitively depend on the wavelength. In the wavelength range corresponding to the second van Hove singularities (VHSs), we observe sub-picosecond decays, as has been seen in previous pump-probe studies. We ascribe these ultrafast decays to intraband carrier relaxation. On the other hand, in the wavelength range corresponding to the first VHSs, we observe two distinct regimes in ultrafast carrier relaxation: fast (0.3-1.2 ps) and slow (5-20 ps). The slow component, which has not been observed previously, is resonantly enhanced whenever the pump photon energy resonates with an interband absorption peak, and we attribute it to radiative carrier recombination. Finally, the slow component is dependent on the pH of the solution, which suggests an important role played by H$^+$ ions surrounding the nanotubes.Comment: 6 pages, 8 figures, changed title, revised, to be published in Applied Physics