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

Yu Zheng (), Yulun Han, Braden M. Weight, Zhiwei Lin, Brendan J. Gifford, Ming Zheng, Dmitri Kilin, Svetlana Kilina, Stephen K. Doorn, Han Htoon () and Sergei Tretiak ()
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Yu Zheng: Center for Integrated Nanotechnologies, Materials Physics and Applications Division, Los Alamos National Laboratory
Yulun Han: North Dakota State University
Braden M. Weight: Center for Integrated Nanotechnologies, Materials Physics and Applications Division, Los Alamos National Laboratory
Zhiwei Lin: Materials Science and Engineering Division, National Institute of Standards and Technology
Brendan J. Gifford: Center for Nonlinear Studies, and Theoretical Division Los Alamos National Laboratory
Ming Zheng: Materials Science and Engineering Division, National Institute of Standards and Technology
Dmitri Kilin: North Dakota State University
Svetlana Kilina: North Dakota State University
Stephen K. Doorn: Center for Integrated Nanotechnologies, Materials Physics and Applications Division, Los Alamos National Laboratory
Han Htoon: Center for Integrated Nanotechnologies, Materials Physics and Applications Division, Los Alamos National Laboratory
Sergei Tretiak: Center for Integrated Nanotechnologies, Materials Physics and Applications Division, Los Alamos National Laboratory

Nature Communications, 2022, vol. 13, issue 1, 1-9

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

Date: 2022
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DOI: 10.1038/s41467-022-31921-0

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