Detection of a Biexciton in Semiconducting Carbon Nanotubes Using Nonlinear Optical Spectroscopy

We report the observation of the biexciton in semiconducting single-wall carbon nanotubes by means of nonlinear optical spectroscopy. Our measurements reveal the universal asymmetric line shape of the Fano resonance intrinsic to the biexciton transition. For nanotubes of the (9,7) chirality, we find a biexciton binding energy of 106 meV. From the calculation of the χ⁽³⁾ nonlinear response, we provide a quantitative interpretation of our measurements, leading to an estimation of the characteristic Fano factor q of 7±3. This value allows us to extract the first experimental information on the biexciton stability and we obtain a biexciton annihilation rate comparable to the exciton-exciton annihilation one.