Nonlinear Photoluminescence Excitation Spectroscopy of Carbon Nanotubes: Exploring the Upper Density Limit of One-Dimensional Excitons

Abstract

We have studied emission properties of high-density excitons in single-walled carbon nanotubes through nonlinear photoluminescence excitation spectroscopy. As the excitation intensity was increased, all emission peaks arising from different chiralities showed clear saturation in intensity. Each peak exhibited a saturation value that was independent of the excitation wavelength, indicating that there is an upper limit on the exciton density for each nanotube species. We developed a theoretical model based on exciton diffusion and exciton-exciton annihilation that successfully reproduced the saturation behavior, allowing us to estimate exciton densities. These estimated densities were found to be still substantially smaller than the expected Mott density even in the saturation regime, in contrast to conventional semiconductor quantum wires.

4 pages, 4 figures

References in corpus (3)

• Exciton binding energies in carbon nanotubes from two-photon photoluminescence
• Stepwise Quenching of Exciton Fluorescence in Carbon Nanotubes by Single Molecule Reactions
• Mott transition from a diluted exciton gas to a dense electron-hole plasma in a single V-shaped quantum wire

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• Exciton diffusion, end quenching, and exciton-exciton annihilation in individual air-suspended carbon nanotubes
• Ultrafast terahertz probes of interacting dark excitons in chirality-specific semiconducting single-walled carbon nanotubes
• Existence of an upper limit on the density of excitons in carbon nanotubes by diffusion-limited exciton-exciton annihilation: Experiment and theory
• Gate-controlled generation of optical pulse trains using individual carbon nanotubes
• Nonlinear spectroscopy of excitonic states in transition metal dichalcogenides
• Non-Equilibrium First-Order Exciton Mott Transition at Monolayer Lateral Heterojunctions Visualized by Ultrafast Microscopy