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Title: Low-Temperature Single Carbon Nanotube Spectroscopy of sp3 Quantum Defects

Abstract

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]; ORCiD logo [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]
+ Show Author Affiliations
  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:
Research Org.:
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States); National Renewable Energy Laboratory (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
OSTI Identifier:
1477667
Alternate Identifier(s):
OSTI ID: 1400371
Report Number(s):
LA-UR-18-25425; NREL/JA-5900-70314
Journal ID: ISSN 1936-0851
Grant/Contract Number:  
AC52-06NA25396; AC36-08GO28308; AC02-05CH11231; DMR-1506711; ECCS-MRI-1531237; CHE-1413614
Resource 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)
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY; 77 NANOSCIENCE AND NANOTECHNOLOGY; 36 MATERIALS SCIENCE; carbon nanotubes; diazonium doping; electronic structure; exciton localization; photoluminescence

Citation Formats

He, Xiaowei, Gifford, Brendan Joel, Hartmann, Nicolai, Ihly, Rachelle, Ma, Xuedan, Kilina, Svetlana V., Luo, Yue, Shayan, Kamarn, Strauf, Stefan, Blackburn, Jeffrey, Tretiak, Sergei, Doorn, Stephen K., and Htoon, Han. Low-Temperature Single Carbon Nanotube Spectroscopy of sp3 Quantum Defects. United States: N. p., 2017. Web. doi:10.1021/acsnano.7b03022.
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He, Xiaowei, Gifford, Brendan Joel, Hartmann, Nicolai, Ihly, Rachelle, Ma, Xuedan, Kilina, Svetlana V., Luo, Yue, Shayan, Kamarn, Strauf, Stefan, Blackburn, Jeffrey, Tretiak, Sergei, Doorn, Stephen K., & Htoon, Han. Low-Temperature Single Carbon Nanotube Spectroscopy of sp3 Quantum Defects. United States. https://doi.org/10.1021/acsnano.7b03022
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He, Xiaowei, Gifford, Brendan Joel, Hartmann, Nicolai, Ihly, Rachelle, Ma, Xuedan, Kilina, Svetlana V., Luo, Yue, Shayan, Kamarn, Strauf, Stefan, Blackburn, Jeffrey, Tretiak, Sergei, Doorn, Stephen K., and Htoon, Han. Thu . "Low-Temperature Single Carbon Nanotube Spectroscopy of sp3 Quantum Defects". United States. https://doi.org/10.1021/acsnano.7b03022. https://www.osti.gov/servlets/purl/1477667.
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@article{osti_1477667,
title = {Low-Temperature Single Carbon Nanotube Spectroscopy of sp3 Quantum Defects},
author = {He, Xiaowei and Gifford, Brendan Joel and Hartmann, Nicolai and Ihly, Rachelle and Ma, Xuedan and Kilina, Svetlana V. and Luo, Yue and Shayan, Kamarn and Strauf, Stefan and Blackburn, Jeffrey 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 = {Thu Sep 28 00:00:00 EDT 2017},
month = {Thu Sep 28 00:00:00 EDT 2017}
}
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https://doi.org/10.1021/acsnano.7b03022
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