Narrow-band single-photon emission through selective aryl functionalization of zigzag carbon nanotubes

Saha, Avishek; Gifford, Brendan J.; He, Xiaowei; Ao, Geyou; Zheng, Ming; Kataura, Hiromichi; Htoon, Han; Kilina, Svetlana; Tretiak, Sergei; Doorn, Stephen K.

doi:10.1038/s41557-018-0126-4

Title: Narrow-band single-photon emission through selective aryl functionalization of zigzag carbon nanotubes

Journal Article · Mon Sep 03 00:00:00 EDT 2018 · Nature Chemistry

DOI:https://doi.org/10.1038/s41557-018-0126-4· OSTI ID:1480023

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Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Los Alamos National Lab. (LANL), Los Alamos, NM (United States); North Dakota State Univ., Fargo, ND (United States). Dept. of Chemistry and Biochemistry
National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States). Materials Science and Engineering Division
National Inst. of Advanced Industrial Science and Technology (AIST), Tsukuba (Japan). Nanomaterials Research Inst.
North Dakota State Univ., Fargo, ND (United States). Dept. of Chemistry and Biochemistry

The introduction of sp³ defects into single-walled carbon nanotubes through covalent functionalization can generate new light-emitting states and thus dramatically expand their optical functionality. This may open up routes to enhanced imaging, photon upconversion, and room-temperature single-photon emission at telecom wavelengths. However, a significant challenge in harnessing this potential is that the nominally simple reaction chemistry of nanotube functionalization introduces a broad diversity of emitting states. Precisely defining a narrow band of emission energies necessitates constraining these states, which requires extreme selectivity in molecular binding configuration on the nanotube surface. We show that such selectivity can be obtained through aryl functionalization of so-called ‘zigzag’ nanotube structures to achieve a threefold narrowing in emission bandwidth. Accompanying density functional theory modelling reveals that, because of the associated structural symmetry, the defect states become degenerate, thus limiting emission energies to a single narrow band. Finally, we show that this behaviour can only result from a predominant selectivity for ortho binding configurations of the aryl groups on the nanotube lattice.

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Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE Office of Science (SC); LANL Laboratory Directed Research and Development (LDRD) Program; National Science Foundation (NSF); Japan Society for the Promotion of Science (JSPS)

Grant/Contract Number:: AC52-06NA25396; CHE-1413614; JP25220602

OSTI ID:: 1480023

Report Number(s):: LA-UR-18-20560

Journal Information:: Nature Chemistry, Vol. 10, Issue 11; ISSN 1755-4330

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 59 works

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