Probing Carrier Dynamics in sp³-Functionalized Single-Walled Carbon Nanotubes with Time-Resolved Terahertz Spectroscopy

The controlled introduction of covalent sp³ 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 sp³ 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 sp³ 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, sp³ defect scattering and inter-nanotube carrier hopping to the overall charge transport properties of nanotube networks.