Formation of organic color centers in air-suspended carbon nanotubes using vapor-phase reaction

Abstract

Organic color centers in single-walled carbon nanotubes have demonstrated exceptional ability to generate single photons at room temperature in the telecom range. Combining the color centers with pristine air-suspended nanotubes would be desirable for improved performance, but all current synthetic methods occur in solution which makes them incompatible. Here we demonstrate the formation of color centers in air-suspended nanotubes using a vapor-phase reaction. Functionalization is directly verified by photoluminescence spectroscopy, with unambiguous statistics from more than a few thousand individual nanotubes. The color centers show strong diameter-dependent emission, which can be explained with a model for chemical reactivity considering strain along the tube curvature. We also estimate the defect density by comparing the experiments with simulations based on a one-dimensional exciton diffusion equation. Our results highlight the influence of the nanotube structure on vapor-phase reactivity and emission properties, providing guidelines for the development of high-performance near-infrared quantum light sources.

On-the-Fly Nonadiabatic Dynamics Simulations of Single-Walled Carbon Nanotubes with Covalent Defects

“…Utilizing semiempirical simulations that have been well justified in similar systems ,, and at the configuration interaction (CIS) level accounting for electrostatically bound excitonic effects, SWCNTs of more than 500 atoms were modeled. While many experimental works have explored similar physics at the sub-ps time scale, ,,,,− the conclusions found in this study will have broad impacts on both the quantum dynamics and SWCNT communities. We have rooted out the structure–property correspondence between the defect’s chemical composition and topological configuration as well as between SWCNT chiralities.…”

Reconfiguring Organic Color Centers on the sp2 Carbon Lattice of Single-Walled Carbon Nanotubes

“…We note the 3,4,5-trifluoaryl group is resistant to further chemical reactions due to its strong C–F bonds, − making it unlikely that the OCC functional group itself has changed during the irradiation process. We further prevented ultraviolet (UV) photon-triggered side reactions ,− by removing the UV photons from the incident light source using a 400 nm long path filter. The irradiation of 565 nm light on pristine (6,5)-SWCNTs under our experimental condition does not generate defect emissions (Figure S4).…”

Recent progress in controlling the photoluminescence properties of single-walled carbon nanotubes by oxidation and alkylation

“…58 Another solid-state functionalization to control the PL characteristics, an arylation reaction, was reported by Kato et al . 35…”