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Origin and control of blinking in quantum dots

Nature Nanotechnology volume 11, pages 661–671 (2016)Cite this article

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Abstract

Semiconductor nanocrystals offer an enormous diversity of potential device applications, based on their size-tunable photoluminescence, high optical stability and 'bottom-up' chemical approaches to self-assembly. However, the promise of such applications can be seriously limited by photoluminescence intermittency in nanocrystal emission, that is, 'blinking', arising from the escape of either one or both of the photoexcited carriers to the nanocrystal surface. In the first scenario, the remaining nanocrystal charge quenches photoluminescence via non-radiative Auger recombination, whereas for the other, the exciton is thought to be intercepted before thermalization and does not contribute to the photoluminescence. This Review summarizes the current understanding of the mechanisms responsible for nanocrystal blinking kinetics as well as core–shell engineering efforts to control such phenomena. In particular, 'softening' of the core–shell confinement potential strongly suppresses non-radiative Auger processes in charged nanocrystals, with successful non-blinking implementations demonstrated in CdSe–CdS core–thick-shell nanocrystals and their modifications.

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Figure 1: Structural and optical properties of NCs.
Figure 2: Blinking of colloidal NCs.
Figure 3: Multiscale distribution of 'on' and 'off' time intervals in fluorescence trajectories of a single NC.
Figure 4: Electrochemically controlled switching between B-type and A-type blinking.
Figure 5: Schematics for describing the diffusion-controlled electron transfer model of Tang and Marcus32,40.
Figure 6: Suppression of non-radiative Auger decay by softening the shape of the NC confinement potential.
Figure 7: Suppression of the non-radiative Auger recombination in negatively charged CdSe–CdS core–thick-shell NCs with 2.5 nm core radius and 6 nm shell thickness.
Figure 8: Effect of softening the confinement potential in CdSe–CdS core–thick-shell NCs on the PL.
Figure 9: Comparison of PL quantum yields of giant and core–alloyed shell NCs.

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Acknowledgements

The authors thank C. Kagan, K. Kuno and R. Vaxenburg for help with figure preparation. Al.L.E. acknowledges the financial support of the Office of Naval Research (ONR) through the Naval Research Laboratory Basic Research Program. D.J.N. acknowledges support for this work from the National Science Foundation (CHE1266416, PHYS1125844), with additional support from the Department of Energy, Office of Basic Energy Sciences (DE-FG02-09ER16021).

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Authors and Affiliations

  1. Naval Research Laboratory, Center for Computational Material Science, 20375, Washington DC, USA

    Alexander L. Efros

  2. JILA, University of Colorado and National Institute of Standards and Technology,

    David J. Nesbitt

  3. Department of Chemistry and Biochemistry, University of Colorado, Boulder, 80309-0440, Colorado, USA

    David J. Nesbitt

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Correspondence to Alexander L. Efros.

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Efros, A., Nesbitt, D. Origin and control of blinking in quantum dots. Nature Nanotech 11, 661–671 (2016). https://doi.org/10.1038/nnano.2016.140

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