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

Abstract

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.

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [1]; ORCiD logo [3]; ORCiD logo [3];  [4]; ORCiD logo [1];  [5]; ORCiD logo [2]; ORCiD logo [1]
+ Show Author Affiliations
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  2. Los Alamos National Lab. (LANL), Los Alamos, NM (United States); North Dakota State Univ., Fargo, ND (United States). Dept. of Chemistry and Biochemistry
  3. National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States). Materials Science and Engineering Division
  4. National Inst. of Advanced Industrial Science and Technology (AIST), Tsukuba (Japan). Nanomaterials Research Inst.
  5. North Dakota State Univ., Fargo, ND (United States). Dept. of Chemistry and Biochemistry
Publication Date:
Research Org.:
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
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)
OSTI Identifier:
1480023
Report Number(s):
LA-UR-18-20560
Journal ID: ISSN 1755-4330
Grant/Contract Number:  
AC52-06NA25396; CHE-1413614; JP25220602
Resource Type:
Accepted Manuscript
Journal Name:
Nature Chemistry
Additional Journal Information:
Journal Volume: 10; Journal Issue: 11; Journal ID: ISSN 1755-4330
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Material Science

Citation Formats

Saha, Avishek, Gifford, Brendan J., He, Xiaowei, Ao, Geyou, Zheng, Ming, Kataura, Hiromichi, Htoon, Han, Kilina, Svetlana, Tretiak, Sergei, and Doorn, Stephen K. Narrow-band single-photon emission through selective aryl functionalization of zigzag carbon nanotubes. United States: N. p., 2018. Web. doi:10.1038/s41557-018-0126-4.
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Saha, Avishek, Gifford, Brendan J., He, Xiaowei, Ao, Geyou, Zheng, Ming, Kataura, Hiromichi, Htoon, Han, Kilina, Svetlana, Tretiak, Sergei, & Doorn, Stephen K. Narrow-band single-photon emission through selective aryl functionalization of zigzag carbon nanotubes. United States. https://doi.org/10.1038/s41557-018-0126-4
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Saha, Avishek, Gifford, Brendan J., He, Xiaowei, Ao, Geyou, Zheng, Ming, Kataura, Hiromichi, Htoon, Han, Kilina, Svetlana, Tretiak, Sergei, and Doorn, Stephen K. Mon . "Narrow-band single-photon emission through selective aryl functionalization of zigzag carbon nanotubes". United States. https://doi.org/10.1038/s41557-018-0126-4. https://www.osti.gov/servlets/purl/1480023.
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@article{osti_1480023,
title = {Narrow-band single-photon emission through selective aryl functionalization of zigzag carbon nanotubes},
author = {Saha, Avishek and Gifford, Brendan J. and He, Xiaowei and Ao, Geyou and Zheng, Ming and Kataura, Hiromichi and Htoon, Han and Kilina, Svetlana and Tretiak, Sergei and Doorn, Stephen K.},
abstractNote = {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.},
doi = {10.1038/s41557-018-0126-4},
journal = {Nature Chemistry},
number = 11,
volume = 10,
place = {United States},
year = {Mon Sep 03 00:00:00 EDT 2018},
month = {Mon Sep 03 00:00:00 EDT 2018}
}
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