Transient Absorption Spectroscopy and Imaging of Individual Chirality-Assigned Single-Walled Carbon Nanotubes

Femtosecond transient absorption microscopy was employed to study the excited-state dynamics of individual semiconducting single-walled carbon nanotubes (SWNTs) with simultaneously high spatial (∼200 nm) and temporal (∼300 fs) resolution. Isolated SWNTs were located using atomic force microscopy, and Raman spectroscopy was employed to determine the chiral index of select nanotubes. This unique experimental approach removes sample heterogeneity in ultrafast measurements of these complex materials. Transient absorption spectra of the individual SWNTs were obtained by recording transient absorption images at different probe wavelengths. These measurements provide new information about the origin of the photoinduced absorption features of SWNTs. Transient absorption traces were also collected for individual SWNTs. The dynamics show a fast, ∼1 ps, decay for all the semiconducting nanotubes studied, which is significantly faster than the previously reported decay times for SWNT suspensions. We attributed this fast relaxation to coupling between the excitons created by the pump laser pulse and the substrate.