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

Abdullah Al Masud; S. M.Nayeem Arefin; Fatema Fairooz; Xu Fu; Faruk Moonschi; Bernadeta R. Srijanto; Khaga Raj Neupane; Surya Aryal; Rosemary Calabro; Doo Young Kim; C. Patrick Collier; Mustafa Habib Chowdhury; Christopher I. Richards

doi:10.1021/acs.jpclett.1c00450

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

Abdullah Al Masud, S. M.Nayeem Arefin, Fatema Fairooz, Xu Fu, Faruk Moonschi, Bernadeta R. Srijanto, Khaga Raj Neupane, Surya Aryal, Rosemary Calabro, Doo Young Kim, C. Patrick Collier, Mustafa Habib Chowdhury, Christopher I. Richards

Nanofabrication Research Laboratory

Research output: Contribution to journal › Article › peer-review

11 Scopus citations

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.

Original language	English
Pages (from-to)	3303-3311
Number of pages	9
Journal	Journal of Physical Chemistry Letters
Volume	12
Issue number	13
DOIs	https://doi.org/10.1021/acs.jpclett.1c00450
State	Published - Apr 8 2021

Funding

C.I.R. acknowledges support from HFSP (RGY0081/2014) and NIH (DA038817). Zero-mode waveguides were fabricated at the Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility.

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Al Masud, A., Arefin, S. M. N., Fairooz, F., Fu, X., Moonschi, F., Srijanto, B. R., Neupane, K. R., Aryal, S., Calabro, R., Kim, D. Y., Collier, C. P., Chowdhury, M. H., & Richards, C. I. (2021). Photoluminescence Enhancement, Blinking Suppression, and Improved Biexciton Quantum Yield of Single Quantum Dots in Zero Mode Waveguides. Journal of Physical Chemistry Letters, 12(13), 3303-3311. https://doi.org/10.1021/acs.jpclett.1c00450

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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.",

author = "{Al Masud}, Abdullah and Arefin, {S. M.Nayeem} and Fatema Fairooz and Xu Fu and Faruk Moonschi and Srijanto, {Bernadeta R.} and Neupane, {Khaga Raj} and Surya Aryal and Rosemary Calabro and Kim, {Doo Young} and Collier, {C. Patrick} and Chowdhury, {Mustafa Habib} and Richards, {Christopher I.}",

note = "Publisher Copyright: {\textcopyright} 2021 American Chemical Society.",

year = "2021",

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doi = "10.1021/acs.jpclett.1c00450",

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Al Masud, A, Arefin, SMN, Fairooz, F, Fu, X, Moonschi, F, Srijanto, BR, Neupane, KR, Aryal, S, Calabro, R, Kim, DY, Collier, CP, Chowdhury, MH & Richards, CI 2021, 'Photoluminescence Enhancement, Blinking Suppression, and Improved Biexciton Quantum Yield of Single Quantum Dots in Zero Mode Waveguides', Journal of Physical Chemistry Letters, vol. 12, no. 13, pp. 3303-3311. https://doi.org/10.1021/acs.jpclett.1c00450

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AU - Al Masud, Abdullah

AU - Arefin, S. M.Nayeem

AU - Fairooz, Fatema

AU - Fu, Xu

AU - Moonschi, Faruk

AU - Srijanto, Bernadeta R.

AU - Neupane, Khaga Raj

AU - Aryal, Surya

AU - Calabro, Rosemary

AU - Kim, Doo Young

AU - Collier, C. Patrick

AU - Chowdhury, Mustafa Habib

AU - Richards, Christopher I.

PY - 2021/4/8

Y1 - 2021/4/8

N2 - 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.

AB - 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.

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ER -

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

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