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Title: Photoluminescence Intensity Fluctuations and Temperature-Dependent Decay Dynamics of Individual Carbon Nanotube sp 3 Defects

Abstract

Recent demonstration of room temperature, telecommunication wavelength single photon generation by sp 3 defects of single wall carbon nanotubes established these defects as a new class of quantum materials. However, their practical utilization in development of quantum light sources calls for a significant improvement in their imperfect quantum yield (QY~10–30%). PL intensity fluctuations observed with some defects also need to be eliminated. Aiming toward attaining fundamental understanding necessary for addressing these critical issues, we investigate PL intensity fluctuation and PL decay dynamics of aryl sp 3 defects of (6,5), (7,5), and (10,3) single wall carbon nanotubes (SWCNTs) at temperatures ranging from 300 to 4 K. By correlating defect-state PL intensity fluctuations with change (or lack of change) in PL decay dynamics, we identified random variations in the trapping efficiency of E 11 band-edge excitons (likely resulting from the existence of a fluctuating potential barrier in the vicinity of the defect) as the mechanism mainly responsible for the defect PL intensity fluctuations. Furthermore, by analyzing the temperature dependence of PL intensity and decay dynamics of individual defects based on a kinetic model involving the trapping and detrapping of excitons by optically allowed and forbidden (bright and dark) defect states, we estimatemore » the height of the potential barrier to be in the 3–22 meV range. Our analysis also provides further confirmation of recent DFT simulation results that the emissive sp 3 defect state is accompanied by an energetically higher-lying optically forbidden (dark) exciton state.« less

Authors:
 [1]; ORCiD logo [1]; ORCiD logo [1];  [1]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [1]; ORCiD logo [1]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  2. National Inst. of Advanced Industrial Science and Technology (AIST), Tsukuba (Japan)
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; USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
1574797
Alternate Identifier(s):
OSTI ID: 1581281
Report Number(s):
LA-UR-19-29770
Journal ID: ISSN 1948-7185
Grant/Contract Number:  
89233218CNA000001
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 10; Journal Issue: 6; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; Quantum Information Science (QIS); Material Science

Citation Formats

Kim, Younghee, Velizhanin, Kirill A., He, Xiaowei, Sarpkaya, Ibrahim, Yomogida, Yohei, Tanaka, Takeshi, Kataura, Hiromichi, Doorn, Stephen K., and Htoon, Han. Photoluminescence Intensity Fluctuations and Temperature-Dependent Decay Dynamics of Individual Carbon Nanotube sp3 Defects. United States: N. p., 2019. Web. doi:10.1021/acs.jpclett.8b03732.
Kim, Younghee, Velizhanin, Kirill A., He, Xiaowei, Sarpkaya, Ibrahim, Yomogida, Yohei, Tanaka, Takeshi, Kataura, Hiromichi, Doorn, Stephen K., & Htoon, Han. Photoluminescence Intensity Fluctuations and Temperature-Dependent Decay Dynamics of Individual Carbon Nanotube sp3 Defects. United States. doi:10.1021/acs.jpclett.8b03732.
Kim, Younghee, Velizhanin, Kirill A., He, Xiaowei, Sarpkaya, Ibrahim, Yomogida, Yohei, Tanaka, Takeshi, Kataura, Hiromichi, Doorn, Stephen K., and Htoon, Han. Fri . "Photoluminescence Intensity Fluctuations and Temperature-Dependent Decay Dynamics of Individual Carbon Nanotube sp3 Defects". United States. doi:10.1021/acs.jpclett.8b03732. https://www.osti.gov/servlets/purl/1574797.
@article{osti_1574797,
title = {Photoluminescence Intensity Fluctuations and Temperature-Dependent Decay Dynamics of Individual Carbon Nanotube sp3 Defects},
author = {Kim, Younghee and Velizhanin, Kirill A. and He, Xiaowei and Sarpkaya, Ibrahim and Yomogida, Yohei and Tanaka, Takeshi and Kataura, Hiromichi and Doorn, Stephen K. and Htoon, Han},
abstractNote = {Recent demonstration of room temperature, telecommunication wavelength single photon generation by sp3 defects of single wall carbon nanotubes established these defects as a new class of quantum materials. However, their practical utilization in development of quantum light sources calls for a significant improvement in their imperfect quantum yield (QY~10–30%). PL intensity fluctuations observed with some defects also need to be eliminated. Aiming toward attaining fundamental understanding necessary for addressing these critical issues, we investigate PL intensity fluctuation and PL decay dynamics of aryl sp3 defects of (6,5), (7,5), and (10,3) single wall carbon nanotubes (SWCNTs) at temperatures ranging from 300 to 4 K. By correlating defect-state PL intensity fluctuations with change (or lack of change) in PL decay dynamics, we identified random variations in the trapping efficiency of E11 band-edge excitons (likely resulting from the existence of a fluctuating potential barrier in the vicinity of the defect) as the mechanism mainly responsible for the defect PL intensity fluctuations. Furthermore, by analyzing the temperature dependence of PL intensity and decay dynamics of individual defects based on a kinetic model involving the trapping and detrapping of excitons by optically allowed and forbidden (bright and dark) defect states, we estimate the height of the potential barrier to be in the 3–22 meV range. Our analysis also provides further confirmation of recent DFT simulation results that the emissive sp3 defect state is accompanied by an energetically higher-lying optically forbidden (dark) exciton state.},
doi = {10.1021/acs.jpclett.8b03732},
journal = {Journal of Physical Chemistry Letters},
issn = {1948-7185},
number = 6,
volume = 10,
place = {United States},
year = {2019},
month = {3}
}

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