Lifetime blinking in nonblinking nanocrystal quantum dots

Nanocrystal quantum dots are attractive materials for applications as nanoscale light sources. One impediment to these applications is fluctuations of single-dot emission intensity, known as blinking. Recent progress in colloidal synthesis has produced nonblinking nanocrystals; however, the physics...

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Main Authors:	Galland, Christophe, Ghosh, Yagnaseni, Steinbrück, Andrea, Hollingsworth, Jennifer A., Htoon, Han, Klimov, Victor I.
Format:	Online
Language:	English
Published:	Nature Pub. Group 2012
Online Access:	https://www.ncbi.nlm.nih.gov/pmc/articles/PMC3426359/

id	pubmed-3426359
recordtype	oai_dc
spelling	pubmed-34263592013-04-10 Lifetime blinking in nonblinking nanocrystal quantum dots Galland, Christophe Ghosh, Yagnaseni Steinbrück, Andrea Hollingsworth, Jennifer A. Htoon, Han Klimov, Victor I. Article Nanocrystal quantum dots are attractive materials for applications as nanoscale light sources. One impediment to these applications is fluctuations of single-dot emission intensity, known as blinking. Recent progress in colloidal synthesis has produced nonblinking nanocrystals; however, the physics underlying blinking suppression remains unclear. Here we find that ultra-thick-shell CdSe/CdS nanocrystals can exhibit pronounced fluctuations in the emission lifetimes (lifetime blinking), despite stable nonblinking emission intensity. We demonstrate that lifetime variations are due to switching between the neutral and negatively charged state of the nanocrystal. Negative charging results in faster radiative decay but does not appreciably change the overall emission intensity because of suppressed nonradiative Auger recombination for negative trions. The Auger process involving excitation of a hole (positive trion pathway) remains efficient and is responsible for charging with excess electrons, which occurs via Auger-assisted ionization of biexcitons accompanied by ejection of holes. Nature Pub. Group 2012-06-19 /pmc/articles/PMC3426359/ /pubmed/22713750 http://dx.doi.org/10.1038/ncomms1916 Text en Copyright © 2012, Nature Publishing Group, a division of Macmillan Publishers Limited. All Rights Reserved. http://creativecommons.org/licenses/by-nc-nd/3.0/ This work is licensed under a Creative Commons Attribution-NonCommercial-No Derivative Works 3.0 Unported License. To view a copy of this license, visit http://creativecommons.org/licenses/by-nc-nd/3.0/
repository_type	Open Access Journal
institution_category	Foreign Institution
institution	US National Center for Biotechnology Information
building	NCBI PubMed
collection	Online Access
language	English
format	Online
author	Galland, Christophe Ghosh, Yagnaseni Steinbrück, Andrea Hollingsworth, Jennifer A. Htoon, Han Klimov, Victor I.
spellingShingle	Galland, Christophe Ghosh, Yagnaseni Steinbrück, Andrea Hollingsworth, Jennifer A. Htoon, Han Klimov, Victor I. Lifetime blinking in nonblinking nanocrystal quantum dots
author_facet	Galland, Christophe Ghosh, Yagnaseni Steinbrück, Andrea Hollingsworth, Jennifer A. Htoon, Han Klimov, Victor I.
author_sort	Galland, Christophe
title	Lifetime blinking in nonblinking nanocrystal quantum dots
title_short	Lifetime blinking in nonblinking nanocrystal quantum dots
title_full	Lifetime blinking in nonblinking nanocrystal quantum dots
title_fullStr	Lifetime blinking in nonblinking nanocrystal quantum dots
title_full_unstemmed	Lifetime blinking in nonblinking nanocrystal quantum dots
title_sort	lifetime blinking in nonblinking nanocrystal quantum dots
description	Nanocrystal quantum dots are attractive materials for applications as nanoscale light sources. One impediment to these applications is fluctuations of single-dot emission intensity, known as blinking. Recent progress in colloidal synthesis has produced nonblinking nanocrystals; however, the physics underlying blinking suppression remains unclear. Here we find that ultra-thick-shell CdSe/CdS nanocrystals can exhibit pronounced fluctuations in the emission lifetimes (lifetime blinking), despite stable nonblinking emission intensity. We demonstrate that lifetime variations are due to switching between the neutral and negatively charged state of the nanocrystal. Negative charging results in faster radiative decay but does not appreciably change the overall emission intensity because of suppressed nonradiative Auger recombination for negative trions. The Auger process involving excitation of a hole (positive trion pathway) remains efficient and is responsible for charging with excess electrons, which occurs via Auger-assisted ionization of biexcitons accompanied by ejection of holes.
publisher	Nature Pub. Group
publishDate	2012
url	https://www.ncbi.nlm.nih.gov/pmc/articles/PMC3426359/
_version_	1611551876002611200

Lifetime blinking in nonblinking nanocrystal quantum dots

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