Photochemical spin-state control of binding configuration for tailoring organic color center emission in carbon nanotubes

• DOI: 10.1038/s41467-022-31921-0
• Publication Date: 2022-08-01T09:08:04Z
• Authors: Yu Zheng; Yulun Han; Braden M. Weight; Zhiwei Lin; Brendan J. Gifford; Ming Zheng; Dmitri Kilin; Svetlana Kilina; Stephen K. Doorn; Han Htoon; Sergei Tretiak
• Keywords: Center (category theory); Visible spectrum

Abstract Incorporating fluorescent quantum defects in the sidewalls of semiconducting single-wall carbon nanotubes (SWCNTs) through chemical reaction is an emerging route to predictably modify nanotube electronic structures and develop advanced photonic functionality. Applications such as room-temperature single-photon emission high-contrast bio-imaging have been aryl-functionalized SWCNTs, which binding configurations aryl group define energies emitting states. However, chemistry with atomic precision at single-bond level tunable control over are yet be achieved. Here, we explore recently reported photosynthetic protocol find that it can defects, often referred organic color centers, spin multiplicity photoexcited intermediates. Specifically, aromatics react SWCNT undergo a singlet-state pathway presence dissolved oxygen, leading ortho on nanotube. In contrast, oxygen-free photoreaction activates previously inaccessible para triplet-state mechanism. These experimental results corroborated by first principles simulations. Such spin-selective photochemistry diversifies tunability controlling morphology sites.