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Strategically introduced defects can be used to modify carbon nanotubes for new properties and functions. For example, chemical defects can act as atomic traps for electrons, holes, electron-hole pairs, and even molecules and ions ( 1 ). The ability to control the placement of these defects on carbon nanotubes could enable a plethora of fundamental studies and potential applications in imaging, sensing, disease diagnostics, and quantum information science ( 2 – 4 ). However, there is yet no effective way to do this with atomic precision ( 5 – 7 ). On page 535 of this issue, Lin et al. ( 8 ) report the creation of ordered defect arrays by programming DNA strands to wrap around and traverse the entire length of a single-walled carbon nanotube.more » « less
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Free, publicly-accessible full text available November 22, 2023
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Abstract We use time-dependent density functional theory to investigate the possibility of hosting organic color centers in (6, 6) armchair single-walled carbon nanotubes, which are known to be metallic. Our calculations show that in short segments of (6, 6) nanotubes ∼ 5 nm in length there is a dipole-allowed singlet transition related to the quantum confinement of charge carriers in the smaller segments. The introduction of s p 3 defects to the surface of (6, 6) nanotubes results in new dipole-allowed excited states. Some of these states are redshifted from the native confinement state of the defect-free (6, 6) segments; this is similar behavior to what is observed with s p 3 defects to exciton transitions in semiconducting carbon nanotubes. This result suggests the possibility of electrically wiring organic color centers directly through armchair carbon nanotube hosts.more » « less
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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.more » « lessFree, publicly-accessible full text available December 1, 2023