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

Organic color centers (OCCs) are atomic defects that can be synthetically created in single-walled carbon nanotube hosts to enable the emission of shortwave infrared single photons at room temperature. However, all known chemistries developed thus far to generate these quantum defects produce a variety of bonding configurations, posing a formidable challenge to the synthesis of identical, uniformly emitting color centers. Herein, we show that laser irradiation of the nanotube host can locally reconfigure the chemical bonding of aryl OCCs on (6,5) nanotubes to significantly reduce their spectral inhomogeneity. After irradiation the defect emission narrows in distribution by ∼26% to yield a single photoluminescence peak. We use hyperspectral photoluminescence imaging to follow this structural transformation on the single nanotube level. Density functional theory calculations corroborate our experimental observations, suggesting that the OCCs convert from kinetic structures to the more thermodynamically stable configuration. This approach may enable localized tuning and creation of identical OCCs for emerging applications in bioimaging, molecular sensing, and quantum information sciences.