4.8 Article

Low-Temperature Single Carbon Nanotube Spectroscopy of sp3 Quantum Defects

Journal

ACS NANO
Volume 11, Issue 11, Pages 10785-10796

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsnano.7b03022

Keywords

carbon nanotubes; electronic structure; diazonium doping; photoluminescence; exciton localization

Funding

  1. Los Alamos National Laboratory (LANL) Directed Research and Development Funds
  2. National Science Foundation (NSF) [DMR-1506711, ECCS-MRI-1531237]
  3. U.S. Department of Energy, Office of Science, Basic Energy Sciences, Division of Chemical Sciences, Geosciences and Biosciences [DE-AC36-08GO28308]
  4. NSF [CHE-1413614]
  5. Alfred P. Sloan Research Fellowship [BR2014-073]
  6. Office of Science of the DOE [DE-AC02-05CH11231, 86678]
  7. Directorate For Engineering
  8. Div Of Electrical, Commun & Cyber Sys [1531237] Funding Source: National Science Foundation

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Aiming to unravel the relationship between chemical configuration and electronic structure of sp(3) defects of aryl-functionalized (6,5) single-walled carbon nanotubes (SWCNTs), we perform low-temperature single nanotube photoluminescence (PL) spectroscopy studies and correlate our observations with quantum chemistry simulations. We observe sharp emission peaks from individual defect sites that are spread over an extremely broad, 1000-1350 nm, spectral range. Our simulations allow us to attribute this spectral diversity to the occurrence of six chemically and energetically distinct defect states resulting from topological variation in the chemical binding configuration of the monovalent aryl groups. Both PL emission efficiency and spectral line width of the defect states are strongly influenced by the local dielectric environment. Wrapping the SWCNT with a polyfluorene polymer provides the best isolation from the environment and yields the brightest emission with near-resolution limited spectral line width of 270 mu eV, as well as spectrally resolved emission wings associated with localized acoustic phonons. Pump-dependent studies further revealed that the defect states are capable of emitting single, sharp, isolated PL peaks over 3 orders of magnitude increase in pump power, a key characteristic of two level systems and an important prerequisite for single-photon emission with high purity. These findings point to the tremendous potential of sp(3) defects in development of room temperature quantum light sources capable of operating at telecommunication wavelengths as the emission of the defect states can readily be extended to this range via use of larger diameter SWCNTs.

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