Photoluminescence Intensity Fluctuations and Temperature-Dependent Decay Dynamics of Individual Carbon Nanotube sp3 Defects

Kim, Younghee; Velizhanin, Kirill A.; He, Xiaowei; Sarpkaya, Ibrahim; Yomogida, Yohei; Tanaka, Takeshi; Kataura, Hiromichi; Doorn, Stephen K.; Htoon, Han

doi:10.1021/acs.jpclett.8b03732

Photoluminescence Intensity Fluctuations and Temperature-Dependent Decay Dynamics of Individual Carbon Nanotube sp³ Defects

Journal Article · Thu Mar 07 23:00:00 EST 2019 · Journal of Physical Chemistry Letters

DOI:https://doi.org/10.1021/acs.jpclett.8b03732· OSTI ID:1574797

Kim, Younghee ^[1]; ^[1]; ^[1]; Sarpkaya, Ibrahim ^[1]; ^[2]; ^[2]; ^[2]; ^[1]; ^[1]

Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
National Inst. of Advanced Industrial Science and Technology (AIST), Tsukuba (Japan)

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.

View Accepted Manuscript (DOE)

Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States); Quantum Information Science (QIS)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Scientific User Facilities Division

Grant/Contract Number:: 89233218CNA000001

OSTI ID:: 1574797

Alternate ID(s):: OSTI ID: 1581281

Journal Information:: Journal of Physical Chemistry Letters, Journal Name: Journal of Physical Chemistry Letters Journal Issue: 6 Vol. 10; ISSN 1948-7185

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Photoswitchable single-walled carbon nanotubes for super-resolution microscopy in the near-infrared Godin, Antoine G.; Setaro, Antonio; Gandil, Morgane Freie Universität Berlin https://doi.org/10.17169/refubium-25631	text	January 2019

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