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Thermal activation of non-radiative Auger recombination in charged colloidal nanocrystals

Nature Nanotechnology volume 8, pages 206–212 (2013)Cite this article

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Abstract

Applications of semiconductor nanocrystals such as biomarkers and light-emitting optoelectronic devices require that their fluorescence quantum yield be close to 100%. However, such quantum yields have not been obtained yet, in part, because non-radiative Auger recombination in charged nanocrystals could not be suppressed completely. Here, we synthesize colloidal core/thick-shell CdSe/CdS nanocrystals with 100% quantum yield and completely quenched Auger processes at low temperatures, although the nanocrystals are negatively photocharged. Single particle and ensemble spectroscopy in the temperature range 30–300 K shows that the non-radiative Auger recombination is thermally activated around 200 K. Experimental results are well described by a model suggesting a temperature-dependent delocalization of one of the trion electrons from the CdSe core and enhanced Auger recombination at the abrupt CdS outer surface. These results point to a route for the design of core/shell structures with 100% quantum yield at room temperature.

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Figure 1: TEM images of nanocrystals and single-nanocrystal fluorescent traces.
Figure 2: Single nanocrystal lifetime evolution versus temperature, and charge determination.
Figure 3: Model of temperature-dependent electron localization.

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Acknowledgements

Al.L.E. acknowledges financial support from the Office of Naval Research and Alexander-von-Humboldt Foundation. A.S. acknowledges support from the Center for Advanced Solar Photophysics (CASP), an Energy Frontier Research Center founded by the Office of Basic Energy Sciences (OBES), Office of Science (OS), US Department of Energy (US DOE). C.J., B.D. and J-P.H. acknowledge support from the Agence Nationale de la Recherche, and the Région Ile-de-France. B.D. acknowledges support from the ESPCI and J-P.H acknowledges support from the Institut Universitaire de France. F.L. and D.R.Y. acknowledge support from the EU Seventh Framework Programme (grant no. 237252, Spin-optronics). The authors thank T. Pons, N. Lequeux, E. Cassette, M. Tessier, I. Maksimovic, N. Bergeal and R. Lobo for stimulating discussions and advice. The authors are also grateful to Xiangzhen Xu for expert help with TEM measurements.

Author information

Authors and Affiliations

  1. Laboratoire de Physique et d'Etude des Matériaux, CNRS, ESPCI, 10 rue Vauquelin, Paris, 75231, France

    C. Javaux, B. Mahler & B. Dubertret

  2. George Mason University, Fairfax, 22030, Virginia, USA

    A. Shabaev

  3. Ioffe Physical-Technical Institute, Russian Academy of Sciences, 194021 St., Petersburg, Russia

    A. V. Rodina & D. R. Yakovlev

  4. Naval Research Laboratory, Washington, Washington, 20375, DC, USA

    Al. L. Efros

  5. Experimentelle Physik 2, TU Dortmund University, Dortmund, 44227, Germany

    D. R. Yakovlev, F. Liu & M. Bayer

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

    G. Camps, L. Biadala, S. Buil, X. Quelin & J-P. Hermier

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  1. C. Javaux
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Contributions

C.J. and B.M. synthesized the nanocrystals. C.J. and G.C. performed the single particle measurements under the guidance of B.D., S.B., X.Q. and J-P.H. L.B and F.L. performed the measurements in magnetic fields under the guidance of D.Y. and M.B. Al.L.E., A.R. and A.S. developed the theoretical model. C.J., B.D., J-P.H., L.B., D.Y. and Al.L.E. analysed and interpreted the data. C.J., B.D. and Al.L.E. wrote the manuscript with the assistance of all other co-authors.

Corresponding authors

Correspondence to B. Dubertret, Al. L. Efros or J-P. Hermier.

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The authors declare no competing financial interests.

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Javaux, C., Mahler, B., Dubertret, B. et al. Thermal activation of non-radiative Auger recombination in charged colloidal nanocrystals. Nature Nanotech 8, 206–212 (2013). https://doi.org/10.1038/nnano.2012.260

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