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Title: Intrinsic limits of defect-state photoluminescence dynamics in functionalized carbon nanotubes

Abstract

Defect states introduced to single wall carbon nanotubes (SWCNTs) by covalent functionalization give rise to novel photophysics and are showing promise as sources of room-temperature quantum emission of interest for quantum information technologies. Evaluation of their ultimate potential for such needs requires a knowledge of intrinsic dynamic and coherence behaviors. Here we probe population relaxation and dephasing time (T1 and T2, respectively) of defect states following deposition of functionalized SWCNTs on polystyrene substrates that are subjected to an isopropanol rinse to remove surfactant. Low-temperature (4 K) photo-luminescence linewidths (~100 μeV) following surfactant removal are a factor of ten narrower than those for unrinsed SWCNTs. Measured recombination lifetimes, on the order of 1.5 ns, compare well with those estimated from DFT calculations, indicating that the intrinsic radiatively-limited lifetime is approached following this sample treatment. Dephasing times evaluated directly through an interferometric approach compare closely to those established by photoluminescence linewidths. Dephasing times as high as 12 ps are found; a factor of up to 6 times greater than those evaluated for band-edge exciton states. In conclusion, such enhancement of dephasing and photoluminescence lifetime behavior is a direct consequence of exciton localization at the SWCNT defect sites.

Authors:
 [1];  [2]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1];  [2]; ORCiD logo [1]; ORCiD logo [1]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  2. Univ. of Texas-Austin, Austin, TX (United States)
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Quantum Information Science (QIS)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Scientific User Facilities Division
OSTI Identifier:
1532722
Alternate Identifier(s):
OSTI ID: 1509752
Report Number(s):
LA-UR-19-21944
Journal ID: ISSN 2040-3364; NANOHL
Grant/Contract Number:  
89233218CNA000001
Resource Type:
Accepted Manuscript
Journal Name:
Nanoscale
Additional Journal Information:
Journal Volume: 11; Journal Issue: 18; Journal ID: ISSN 2040-3364
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; 36 MATERIALS SCIENCE; Quantum Information Science (QIS)

Citation Formats

He, Xiaowei, Sun, Liuyang, Gifford, Brendan Joel, Tretiak, Sergei, Piryatinski, Andrei, Li, Xiaoqin, Htoon, Han, and Doorn, Stephen K. Intrinsic limits of defect-state photoluminescence dynamics in functionalized carbon nanotubes. United States: N. p., 2019. Web. doi:10.1039/C9NR02175B.
He, Xiaowei, Sun, Liuyang, Gifford, Brendan Joel, Tretiak, Sergei, Piryatinski, Andrei, Li, Xiaoqin, Htoon, Han, & Doorn, Stephen K. Intrinsic limits of defect-state photoluminescence dynamics in functionalized carbon nanotubes. United States. doi:10.1039/C9NR02175B.
He, Xiaowei, Sun, Liuyang, Gifford, Brendan Joel, Tretiak, Sergei, Piryatinski, Andrei, Li, Xiaoqin, Htoon, Han, and Doorn, Stephen K. Mon . "Intrinsic limits of defect-state photoluminescence dynamics in functionalized carbon nanotubes". United States. doi:10.1039/C9NR02175B. https://www.osti.gov/servlets/purl/1532722.
@article{osti_1532722,
title = {Intrinsic limits of defect-state photoluminescence dynamics in functionalized carbon nanotubes},
author = {He, Xiaowei and Sun, Liuyang and Gifford, Brendan Joel and Tretiak, Sergei and Piryatinski, Andrei and Li, Xiaoqin and Htoon, Han and Doorn, Stephen K.},
abstractNote = {Defect states introduced to single wall carbon nanotubes (SWCNTs) by covalent functionalization give rise to novel photophysics and are showing promise as sources of room-temperature quantum emission of interest for quantum information technologies. Evaluation of their ultimate potential for such needs requires a knowledge of intrinsic dynamic and coherence behaviors. Here we probe population relaxation and dephasing time (T1 and T2, respectively) of defect states following deposition of functionalized SWCNTs on polystyrene substrates that are subjected to an isopropanol rinse to remove surfactant. Low-temperature (4 K) photo-luminescence linewidths (~100 μeV) following surfactant removal are a factor of ten narrower than those for unrinsed SWCNTs. Measured recombination lifetimes, on the order of 1.5 ns, compare well with those estimated from DFT calculations, indicating that the intrinsic radiatively-limited lifetime is approached following this sample treatment. Dephasing times evaluated directly through an interferometric approach compare closely to those established by photoluminescence linewidths. Dephasing times as high as 12 ps are found; a factor of up to 6 times greater than those evaluated for band-edge exciton states. In conclusion, such enhancement of dephasing and photoluminescence lifetime behavior is a direct consequence of exciton localization at the SWCNT defect sites.},
doi = {10.1039/C9NR02175B},
journal = {Nanoscale},
number = 18,
volume = 11,
place = {United States},
year = {2019},
month = {4}
}

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