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Title: Photoluminescence Enhancement, Blinking Suppression, and Improved Biexciton Quantum Yield of Single Quantum Dots in Zero Mode Waveguides

Abstract

The capability of quantum dots to generate both single and multiexcitons can be harnessed for a wide variety of applications, including those that require high optical gain. Here, we use time-correlated photoluminescence (PL) spectroscopy to demonstrate that the isolation of single CdSeTe/ZnS core–shell, nanocrystal quantum dots (QDs) in Zero Mode Waveguides (ZMWs) leads to a significant modification in PL intensity, blinking dynamics, and biexciton behavior. QDs in aluminum ZMWs (AlZMWs) exhibited a 15-fold increase in biexciton emission, indicating a preferential enhancement of the biexciton radiative decay rate as compared to the single exciton rate. The increase in biexciton behavior was accompanied by a decrease in blinking events due to a shortening in the dark state residence time. These results indicate that plasmon mediated enhanced decay rates of QDs in AlZMWs lead to substantial changes in the photophysical properties of single quantum dots, including an increase in biexciton behavior.

Authors:
 [1];  [2];  [2];  [1];  [1]; ORCiD logo [3];  [1];  [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [3];  [2]; ORCiD logo [1]
+ Show Author Affiliations
  1. Univ. of Kentucky, Lexington, KY (United States)
  2. Independent Univ., Bangladesh (IUB), Dhaka (Bangladesh)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1847546
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 12; Journal Issue: 13; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; 36 MATERIALS SCIENCE; Zero mode waveguides (ZMWs); quantum dots (QDs); photoluminescence (PL); photon correlation; exciton; and biexciton

Citation Formats

Masud, Abdullah Al, Arefin, S. M. Nayeem, Fairooz, Fatema, Fu, Xu, Moonschi, Faruk, Srijanto, Bernadeta R., Neupane, Khaga Raj, Aryal, Surya, Calabro, Rosemary, Kim, Doo-Young, Collier, Charles Patrick, Chowdhury, Mustafa Habib, and Richards, Christopher I. Photoluminescence Enhancement, Blinking Suppression, and Improved Biexciton Quantum Yield of Single Quantum Dots in Zero Mode Waveguides. United States: N. p., 2021. Web. doi:10.1021/acs.jpclett.1c00450.
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Masud, Abdullah Al, Arefin, S. M. Nayeem, Fairooz, Fatema, Fu, Xu, Moonschi, Faruk, Srijanto, Bernadeta R., Neupane, Khaga Raj, Aryal, Surya, Calabro, Rosemary, Kim, Doo-Young, Collier, Charles Patrick, Chowdhury, Mustafa Habib, & Richards, Christopher I. Photoluminescence Enhancement, Blinking Suppression, and Improved Biexciton Quantum Yield of Single Quantum Dots in Zero Mode Waveguides. United States. https://doi.org/10.1021/acs.jpclett.1c00450
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Masud, Abdullah Al, Arefin, S. M. Nayeem, Fairooz, Fatema, Fu, Xu, Moonschi, Faruk, Srijanto, Bernadeta R., Neupane, Khaga Raj, Aryal, Surya, Calabro, Rosemary, Kim, Doo-Young, Collier, Charles Patrick, Chowdhury, Mustafa Habib, and Richards, Christopher I. Thu . "Photoluminescence Enhancement, Blinking Suppression, and Improved Biexciton Quantum Yield of Single Quantum Dots in Zero Mode Waveguides". United States. https://doi.org/10.1021/acs.jpclett.1c00450. https://www.osti.gov/servlets/purl/1847546.
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@article{osti_1847546,
title = {Photoluminescence Enhancement, Blinking Suppression, and Improved Biexciton Quantum Yield of Single Quantum Dots in Zero Mode Waveguides},
author = {Masud, Abdullah Al and Arefin, S. M. Nayeem and Fairooz, Fatema and Fu, Xu and Moonschi, Faruk and Srijanto, Bernadeta R. and Neupane, Khaga Raj and Aryal, Surya and Calabro, Rosemary and Kim, Doo-Young and Collier, Charles Patrick and Chowdhury, Mustafa Habib and Richards, Christopher I.},
abstractNote = {The capability of quantum dots to generate both single and multiexcitons can be harnessed for a wide variety of applications, including those that require high optical gain. Here, we use time-correlated photoluminescence (PL) spectroscopy to demonstrate that the isolation of single CdSeTe/ZnS core–shell, nanocrystal quantum dots (QDs) in Zero Mode Waveguides (ZMWs) leads to a significant modification in PL intensity, blinking dynamics, and biexciton behavior. QDs in aluminum ZMWs (AlZMWs) exhibited a 15-fold increase in biexciton emission, indicating a preferential enhancement of the biexciton radiative decay rate as compared to the single exciton rate. The increase in biexciton behavior was accompanied by a decrease in blinking events due to a shortening in the dark state residence time. These results indicate that plasmon mediated enhanced decay rates of QDs in AlZMWs lead to substantial changes in the photophysical properties of single quantum dots, including an increase in biexciton behavior.},
doi = {10.1021/acs.jpclett.1c00450},
journal = {Journal of Physical Chemistry Letters},
number = 13,
volume = 12,
place = {United States},
year = {Thu Mar 25 00:00:00 EDT 2021},
month = {Thu Mar 25 00:00:00 EDT 2021}
}
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