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:
-
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Univ. of Texas-Austin, Austin, TX (United States)
- Publication Date:
- Research Org.:
- Los Alamos National Laboratory (LANL), Los Alamos, NM (United States); Quantum Information Science (QIS)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). 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. https://doi.org/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. https://doi.org/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 = {Mon Apr 22 00:00:00 EDT 2019},
month = {Mon Apr 22 00:00:00 EDT 2019}
}
Web of Science
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