Infrared Study of Charge Carrier Confinement in Doped (6,5) Carbon Nanotubes

Electronic degrees of freedom and their coupling to lattice vibrations in semiconductors can be strongly modified by doping. Accordingly, the addition of surplus charge carriers to chirality-mixed carbon nanotube samples has previously been found to give rise to a Drude-type plasmon feature as well as Fano-type antiresonances in the farto mid-infrared spectral range (FIR/MIR). Here we investigate the FIR/MIR response of redox chemically doped semiconducting (6,5) carbon nanotubes (s-SWNTs). We find that, contrary to expectations, the Drude-type plasmon shifts to lower wavenumbers with increasing doping level. By means of Monte Carlo simulations of the optical response, we attribute this behavior to the confinement of excess charge carriers at low doping levels and their progressive delocalization when approaching degenerate doping. The coupling of vibrational modes to intraband excitations in the doped s-SWNTs can be probed via a double-resonance process similar to that responsible for the Raman D-band. The resulting Fano antiresonances shed new light onto the character and coupling of electronic and vibrational degrees of freedom in these one-dimensional semiconductors.

Automated summary

This study investigates the far/mid-infrared response of redox chemically doped semiconducting carbon nanotubes. Contrary to expectations, it is found that the Drude-type plasmon shifts to lower wavenumbers with increasing doping level. Monte Carlo simulations of the optical response attribute this behavior to the confinement of excess charge carriers at low doping levels and their progressive delocalization when approaching degenerate doping. The coupling of vibrational modes to intraband excitations in the doped semiconducting carbon nanotubes can be probed via a double-resonance process, shedding new light onto the character and coupling of electronic and vibrational degrees of freedom.