Probing Carrier Dynamics in sp(3)-Functionalized Single-Walled Carbon Nanotubes with Time-Resolved Terahertz Spectroscopy

[Image: see text] The controlled introduction of covalent sp(3) defects into semiconducting single-walled carbon nanotubes (SWCNTs) gives rise to exciton localization and red-shifted near-infrared luminescence. The single-photon emission characteristics of these functionalized SWCNTs make them interesting candidates for electrically driven quantum light sources. However, the impact of sp(3) defects on the carrier dynamics and charge transport in carbon nanotubes remains an open question. Here, we use ultrafast, time-resolved optical-pump terahertz-probe spectroscopy as a direct and quantitative technique to investigate the microscopic and temperature-dependent charge transport properties of pristine and functionalized (6,5) SWCNTs in dispersions and thin films. We find that sp(3) functionalization increases charge carrier scattering, thus reducing the intra-nanotube carrier mobility. In combination with electrical measurements of SWCNT network field-effect transistors, these data enable us to distinguish between contributions of intra-nanotube band transport, sp(3) defect scattering and inter-nanotube carrier hopping to the overall charge transport properties of nanotube networks.