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The functionalization of single-walled carbon nanotubes (SWCNTs) withluminescent sp$^{3}$ defects has greatly improved their performance inapplications such as quantum light sources and bioimaging. Here, we report thecovalent functionalization of purified semiconducting SWCNTs with stableorganic radicals (perchlorotriphenylmethyl, PTM) carrying a net spin. Thismodel system allows us to use the near-infrared photoluminescence arising fromthe defect-localized exciton as a highly sensitive probe for the short-rangeinteraction between the PTM radical and the SWCNT. Our results point toward anincreased triplet exciton population due to radical-enhanced intersystemcrossing, which could provide access to the elusive triplet manifold in SWCNTs.Furthermore, this simple synthetic route to spin-labeled defects could enablemagnetic resonance studies complementary to in vivo fluorescence imaging withfunctionalized SWCNTs and facilitate the scalable fabrication of spintronicdevices with magnetically switchable charge transport.

Interaction of Luminescent Defects in Carbon Nanotubes with Covalently Attached Stable Organic Radicals