Photochemical Creation of Fluorescent Quantum Defects in Semiconducting Carbon Nanotube Hosts

Quantum defects are an emerging class of synthetic single‐photon emitters that hold vast potential for near‐infrared imaging, chemical sensing, materials engineering, and quantum information processing. Herein, we show that it is possible to optically direct the synthetic creation of molecularly tunable fluorescent quantum defects in semiconducting single‐walled carbon nanotube hosts through photochemical reactions. By exciting the host semiconductor with light that resonates with its electronic transition, we find that halide‐containing aryl groups can covalently bond to the sp2 carbon lattice. The introduced quantum defects generate bright photoluminescence that allows tracking of the reaction progress in situ. We show that the reaction is independent of temperature but correlates strongly with the photon energy used to drive the reaction, suggesting a photochemical mechanism rather than photothermal effects. This type of photochemical reactions opens the possibility to control the synthesis of fluorescent quantum defects using light and may enable lithographic patterning of quantum emitters with electronic and molecular precision. Creating quantum defects with light: Exciting semiconducting carbon nanotubes with light in the presence of a halide‐containing aryl molecule leads to creation of fluorescent quantum defects in the semiconductor host material. This reaction is electronically selective and efficiently driven by pumping an electron from the semiconductor to the molecular precursor.