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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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).
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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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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