Direct observation of cross-polarized excitons in aligned single-chirality single-wall carbon nanotubes

摘要： Optical properties of single-wall carbon nanotubes (SWCNTs) for light polarized parallel to the nanotube axis have been studied extensively, whereas their response to light polarized perpendicular to the nanotube axis has not been well explored. Here, by using a macroscopic film of highly aligned single-chirality (6,5) SWCNTs, we performed a systematic polarization-dependent optical absorption spectroscopy study. In addition to the commonly observed angular-momentum-conserving interband absorption of parallel-polarized light, which generates E11 and E22 excitons, we observed a small but unambiguous absorption peak whose intensity is maximum for perpendicular-polarized light. We attribute this feature to the lowest-energy cross-polarized interband absorption processes that change the angular momentum along the nanotube axis by ±1, generating E12 and E21 excitons. Unlike previous observations of cross-polarized excitons in polarization-dependent photoluminescence and circular dichroism spectroscopy experiments, our direct observation using absorption spectroscopy allowed us to quantitatively analyze this resonance. Specifically, we determined the energy and oscillator strength of this resonance to be 1.54 and 0.05, respectively, compared with the values for the E11 exciton peak. These values, in combination with a comparison with theoretical calculations, in turn led to an assessment of the environmental effect on the strength of Coulomb interactions in this aligned single-chirality SWCNT film.