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Title: Low-Temperature Single Carbon Nanotube Spectroscopy of sp 3 Quantum Defects

Aiming to unravel the relationship between chemical configuration and electronic structure of sp3 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. Here, 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 ueV, 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. Our findings point to themore » tremendous potential of sp3 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.« less
Authors:
ORCiD logo [1] ;  [2] ; ORCiD logo [1] ; ORCiD logo [3] ;  [1] ; ORCiD logo [4] ;  [5] ;  [5] ; ORCiD logo [5] ; ORCiD logo [3] ; ORCiD logo [6] ; ORCiD logo [1] ; ORCiD logo [1]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Center for Integrated Nanotechnologies
  2. Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Theoretical Division and Center for Nonlinear Studies; North Dakota State Univ., Fargo, ND (United States). Dept. of Chemistry and Biochemistry
  3. National Renewable Energy Lab. (NREL), Golden, CO (United States). National Center for Photovoltaics. Chemical and Materials Science Center
  4. North Dakota State Univ., Fargo, ND (United States). Dept. of Chemistry and Biochemistry
  5. Stevens Inst. of Technology, Hoboken, NJ (United States). Dept. of Physics
  6. Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Center for Integrated Nanotechnologies, Theoretical Division and Center for Nonlinear Studies
Publication Date:
Report Number(s):
NREL/JA-5900-70314; LA-UR-18-25425
Journal ID: ISSN 1936-0851
Grant/Contract Number:
AC36-08GO28308; AC02-05CH11231; DMR-1506711; ECCS-MRI-1531237; CHE-1413614; AC52-06NA25396
Type:
Accepted Manuscript
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 11; Journal Issue: 11; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society (ACS)
Research Org:
National Renewable Energy Lab. (NREL), Golden, CO (United States); Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation (NSF)
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY; 77 NANOSCIENCE AND NANOTECHNOLOGY; carbon nanotubes; diazonium doping; electronic structure; exciton localization; photoluminescence; 36 MATERIALS SCIENCE
OSTI Identifier:
1477667
Alternate Identifier(s):
OSTI ID: 1400371

He, Xiaowei, Gifford, Brendan J., Hartmann, Nicolai F., Ihly, Rachelle, Ma, Xuedan, Kilina, Svetlana V., Luo, Yue, Shayan, Kamran, Strauf, Stefan, Blackburn, Jeffrey L., Tretiak, Sergei, Doorn, Stephen K., and Htoon, Han. Low-Temperature Single Carbon Nanotube Spectroscopy of sp 3 Quantum Defects. United States: N. p., Web. doi:10.1021/acsnano.7b03022.
He, Xiaowei, Gifford, Brendan J., Hartmann, Nicolai F., Ihly, Rachelle, Ma, Xuedan, Kilina, Svetlana V., Luo, Yue, Shayan, Kamran, Strauf, Stefan, Blackburn, Jeffrey L., Tretiak, Sergei, Doorn, Stephen K., & Htoon, Han. Low-Temperature Single Carbon Nanotube Spectroscopy of sp 3 Quantum Defects. United States. doi:10.1021/acsnano.7b03022.
He, Xiaowei, Gifford, Brendan J., Hartmann, Nicolai F., Ihly, Rachelle, Ma, Xuedan, Kilina, Svetlana V., Luo, Yue, Shayan, Kamran, Strauf, Stefan, Blackburn, Jeffrey L., Tretiak, Sergei, Doorn, Stephen K., and Htoon, Han. 2017. "Low-Temperature Single Carbon Nanotube Spectroscopy of sp 3 Quantum Defects". United States. doi:10.1021/acsnano.7b03022. https://www.osti.gov/servlets/purl/1477667.
@article{osti_1477667,
title = {Low-Temperature Single Carbon Nanotube Spectroscopy of sp 3 Quantum Defects},
author = {He, Xiaowei and Gifford, Brendan J. and Hartmann, Nicolai F. and Ihly, Rachelle and Ma, Xuedan and Kilina, Svetlana V. and Luo, Yue and Shayan, Kamran and Strauf, Stefan and Blackburn, Jeffrey L. and Tretiak, Sergei and Doorn, Stephen K. and Htoon, Han},
abstractNote = {Aiming to unravel the relationship between chemical configuration and electronic structure of sp3 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. Here, 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 ueV, 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. Our findings point to the tremendous potential of sp3 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.},
doi = {10.1021/acsnano.7b03022},
journal = {ACS Nano},
number = 11,
volume = 11,
place = {United States},
year = {2017},
month = {9}
}