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Giant light-harvesting nanoantenna for single-molecule detection in ambient light

Nature Photonics volume 11, pages 657–663 (2017)Cite this article

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A Publisher Correction to this article was published on 12 January 2018

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Abstract

Here, we explore the enhancement of single-molecule emission by a polymeric nanoantenna that can harvest energy from thousands of donor dyes to a single acceptor. In this nanoantenna, the cationic dyes are brought together, in very close proximity, using bulky counterions, thus enabling ultrafast diffusion of excitation energy (≤30 fs) with minimal losses. Our 60 nm nanoparticles containing >10,000 rhodamine-based donor dyes can efficiently transfer energy to 1–2 acceptors, resulting in an antenna effect of ~1,000. Therefore, single Cy5-based acceptors become 25-fold brighter than quantum dots QD655. This unprecedented amplification of the acceptor dye emission enables observation of single molecules at illumination powers (1–10 mW cm−2) that are >10,000-fold lower than typically required in single-molecule measurements. Finally, using a basic set-up, which includes a ×20 air objective and a scalable complementary metal-oxide–semiconductor camera, we could detect single Cy5 molecules by simply shining divergent light on the sample at powers equivalent to sunlight.

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Fig. 1: Concept of the organic nanoantenna.
Fig. 2: Spectroscopic characterization of organic nanoantennas.
Fig. 3: TEM and fluorescence microscopy images of individual nanoantennas.
Fig. 4: Fluorescence spectra and antenna effect of FRET NPs.
Fig. 5: Single-particle evaluation of nanoantennas.

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Change history

  • 12 January 2018

    Owing to a technical error, the wrong version of the Supplementary Information was published for this Article; the equation E = xcoupled donors × ElocalFRET related to Supplementary Table 6 appeared incorrectly. This error has now been corrected.

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Acknowledgements

This work was supported by the European Research Council ERC Consolidator grant BrightSens 648528. The authors thank C. Ruhlmann from the FRISBI platform (ANR-10-INBS-05) for help with electron microscopy. K.T. was supported by a fellowship from the Ministre de la Recherche (France).

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Authors and Affiliations

  1. Université de Strasbourg, Laboratoire de Biophotonique et Pharmacologie, UMR 7213 CNRS, Faculté de Pharmacie, 74, Route du Rhin, F-67401, ILLKIRCH, France

    Kateryna Trofymchuk, Andreas Reisch, Pascal Didier, Yves Mely & Andrey S. Klymchenko

  2. Université de Strasbourg, CNRS UMR 7504, Inst. Phys. & Chim. Mat. Strasbourg, F-67034, Strasbourg, France

    François Fras & Pierre Gilliot

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Contributions

A.S.K. proposed the concept. A.S.K. and K.T. designed the experiments. K.T. performed most of the experiments and data analysis. A.R. performed electron microscopy and helped with donor NP design and some data analysis. P.D. and F.F. performed time-resolved anisotropy measurements. A.S.K. helped with single-particle microscopy. A.R., Y.M., P.G. and A.S.K. contributed materials and analysis tools. A.S.K. and K.T. wrote the manuscript.

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Correspondence to Andrey S. Klymchenko.

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A European patent application has been filed under no. 17305763.9.

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A correction to this article is available online at https://doi.org/10.1038/s41566-017-0055-6.

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Supplementary Information

Additional information on FRET calculation, spectroscopic, time-resolved and single-particle data, experiment set-up and other details.

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Trofymchuk, K., Reisch, A., Didier, P. et al. Giant light-harvesting nanoantenna for single-molecule detection in ambient light. Nature Photon 11, 657–663 (2017). https://doi.org/10.1038/s41566-017-0001-7

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