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Towards non-blinking colloidal quantum dots

Nature Materials volume 7, pages 659–664 (2008)Cite this article

Abstract

At a single-molecule level, fluorophore emission intensity fluctuates between bright and dark states. These fluctuations, known as blinking, limit the use of fluorophores in single-molecule experiments. The dark-state duration shows a universal heavy-tailed power-law distribution characterized by the occurrence of long non-emissive periods. Here we have synthesized novel CdSe–CdS core–shell quantum dots with thick crystalline shells, 68% of which do not blink when observed individually at 33 Hz for 5 min. We have established a direct correlation between shell thickness and blinking occurrences. Importantly, the statistics of dark periods that appear at high acquisition rates (1 kHz) are not heavy tailed, in striking contrast with previous observations. Blinking statistics are thus not as universal as thought so far. We anticipate that our results will help to better understand the physico-chemistry of single-fluorophore emission and rationalize the design of other fluorophores that do not blink.

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Figure 1: Characterization of core–shell CdSe–CdS nanocrystals with reduced blinking.
Figure 2: Intensity fluctuations and blinking behaviour of single CdSe–CdS QDs visualized with a CCD camera.
Figure 3: Intensity fluctuations of single CdSe–CdS and CdSe–ZnS QDs measured with avalanche photodiodes.
Figure 4: Cumulative distributions of off times in a logarithmic scale.

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Acknowledgements

We thank P. Guyot-Sionnest for critical and enlightening discussions concerning the work and the redaction of the manuscript. B.M. thanks T. Pons for providing the software code for the automated analysis of QD blinking. B.D. thanks the Human Frontier Science Program for funding. B.D. and J.-P.H. acknowledge funding from l’Agence Nationale de la Recherche and La Région Ile-de-France.

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Authors and Affiliations

  1. Laboratoire Photons Et Matière, CNRS UPR5, ESPCI 10 rue Vauquelin, 75231 Paris, France

    Benoit Mahler & Benoit Dubertret

  2. Laboratoire Kastler Brossel, CNRS UMR8552, Université Pierre et Marie Curie, Ecole normale supérieure, 24 rue Lhomond, 75231 Paris Cedex 05, France

    Piernicola Spinicelli & Jean-Pierre Hermier

  3. Groupe d’Etude de la Matière Condensée, CNRS UMR8635, Université de Versailles Saint-Quentin-en-Yvelines, 45 avenue des Etats-Unis, 78035 Versailles Cedex, France

    Stéphanie Buil, Xavier Quelin & Jean-Pierre Hermier

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  1. Benoit Mahler
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Correspondence to Jean-Pierre Hermier or Benoit Dubertret.

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Mahler, B., Spinicelli, P., Buil, S. et al. Towards non-blinking colloidal quantum dots. Nature Mater 7, 659–664 (2008). https://doi.org/10.1038/nmat2222

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