Second-and third-harmonic generation by carbon nanotubes irradiated with femtosecond laser pulses

Femtosecond pulses of a Cr:forsterite laser are used to study second-and third-harmonic generation in a layer of single-wall carbon nanotubes produced by low-velocity spraying. The harmonic amplitude in our experiments scales as (Ip)n as a function of the pump intensity Ip, with n=2 and 3 for the second and third harmonics, respectively. This scaling law holds up to pump intensities on the order of 1012W/cm2. The ratio of the maximum signal to the averaged background in the spectra of the second and third harmonics is estimated as 50 and 30, respectively. The second and third harmonics produced by a linearly polarized pump field are also linearly polarized, with their polarization vectors oriented along the polarization direction of the pump field. The capabilities of nonlinear-optical methods for structural and morphological analysis of carbon nanotubes are discussed, as well as ways to create solid-state carbon-nanotube generators of optical harmonic.