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Biexciton Blinking in CdSe-Based Quantum Dots

[Image: see text] Experiments on single colloidal quantum dots (QDs) have revealed temporal fluctuations in the emission efficiency of the single-exciton state. These fluctuations, often termed “blinking”, are caused by opening/closing of charge-carrier traps and/or charging/discharging of the QD. I...

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Autores principales: Vonk, Sander J. W., Rabouw, Freddy T.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2023
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10278138/
https://www.ncbi.nlm.nih.gov/pubmed/37276380
http://dx.doi.org/10.1021/acs.jpclett.3c00437
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author Vonk, Sander J. W.
Rabouw, Freddy T.
author_facet Vonk, Sander J. W.
Rabouw, Freddy T.
author_sort Vonk, Sander J. W.
collection PubMed
description [Image: see text] Experiments on single colloidal quantum dots (QDs) have revealed temporal fluctuations in the emission efficiency of the single-exciton state. These fluctuations, often termed “blinking”, are caused by opening/closing of charge-carrier traps and/or charging/discharging of the QD. In the regime of strong optical excitation, multiexciton states are formed. The emission efficiencies of multiexcitons are lower because of Auger processes, but a quantitative characterization is challenging. Here, we quantify fluctuations of the biexciton efficiency for single CdSe/CdS/ZnS core–shell QDs. We find that the biexciton efficiency “blinks” significantly. The additional electron due to charging of a QD accelerates Auger recombination by a factor of 2 compared to the neutral biexciton, while opening/closing of a charge-carrier trap leads to an increase of the nonradiative recombination rate by a factor of 4. To understand the fast rate of trap-assisted recombination, we propose a revised model for trap-assisted recombination based on reversible trapping. Finally, we discuss the implications of biexciton blinking for lasing applications.
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spelling pubmed-102781382023-06-20 Biexciton Blinking in CdSe-Based Quantum Dots Vonk, Sander J. W. Rabouw, Freddy T. J Phys Chem Lett [Image: see text] Experiments on single colloidal quantum dots (QDs) have revealed temporal fluctuations in the emission efficiency of the single-exciton state. These fluctuations, often termed “blinking”, are caused by opening/closing of charge-carrier traps and/or charging/discharging of the QD. In the regime of strong optical excitation, multiexciton states are formed. The emission efficiencies of multiexcitons are lower because of Auger processes, but a quantitative characterization is challenging. Here, we quantify fluctuations of the biexciton efficiency for single CdSe/CdS/ZnS core–shell QDs. We find that the biexciton efficiency “blinks” significantly. The additional electron due to charging of a QD accelerates Auger recombination by a factor of 2 compared to the neutral biexciton, while opening/closing of a charge-carrier trap leads to an increase of the nonradiative recombination rate by a factor of 4. To understand the fast rate of trap-assisted recombination, we propose a revised model for trap-assisted recombination based on reversible trapping. Finally, we discuss the implications of biexciton blinking for lasing applications. American Chemical Society 2023-06-05 /pmc/articles/PMC10278138/ /pubmed/37276380 http://dx.doi.org/10.1021/acs.jpclett.3c00437 Text en © 2023 The Authors. Published by American Chemical Society https://creativecommons.org/licenses/by/4.0/Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained (https://creativecommons.org/licenses/by/4.0/).
spellingShingle Vonk, Sander J. W.
Rabouw, Freddy T.
Biexciton Blinking in CdSe-Based Quantum Dots
title Biexciton Blinking in CdSe-Based Quantum Dots
title_full Biexciton Blinking in CdSe-Based Quantum Dots
title_fullStr Biexciton Blinking in CdSe-Based Quantum Dots
title_full_unstemmed Biexciton Blinking in CdSe-Based Quantum Dots
title_short Biexciton Blinking in CdSe-Based Quantum Dots
title_sort biexciton blinking in cdse-based quantum dots
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10278138/
https://www.ncbi.nlm.nih.gov/pubmed/37276380
http://dx.doi.org/10.1021/acs.jpclett.3c00437
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