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

Journal Article · · Nature Chemistry
 [1];  [2];  [1];  [3];  [3];  [4];  [1];  [5];  [2];  [1]
  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
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.
Research Organization:
Los Alamos National Laboratory (LANL)
Sponsoring Organization:
Japan Society for the Promotion of Science (JSPS); LANL Laboratory Directed Research and Development (LDRD) Program; National Science Foundation (NSF) (United States); USDOE Office of Science (SC)
Grant/Contract Number:
AC52-06NA25396
OSTI ID:
1480023
Report Number(s):
LA-UR-18-20560
Journal Information:
Nature Chemistry, Journal Name: Nature Chemistry Journal Issue: 11 Vol. 10; ISSN 1755-4330
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English

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