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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...
Autores principales: | , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
American Chemical Society
2023
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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. |
format | Online Article Text |
id | pubmed-10278138 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2023 |
publisher | American Chemical Society |
record_format | MEDLINE/PubMed |
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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