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Cascaded nanooptics to probe microsecond atomic-scale phenomena
Ist Teil von
Proceedings of the National Academy of Sciences - PNAS, 2020-06, Vol.117 (26), p.14819-14826
Ort / Verlag
United States: National Academy of Sciences
Erscheinungsjahr
2020
Quelle
EZB Electronic Journals Library
Beschreibungen/Notizen
Plasmonic nanostructures can focus light far below the diffraction limit, and the nearly thousandfold field enhancements obtained routinely enable few- and single-molecule detection. However, for processes happening on the molecular scale to be tracked with any relevant time resolution, the emission strengths need to be well beyond what current plasmonic devices provide. Here, we develop hybrid nanostructures incorporating both refractive and plasmonic optics, by creating SiO₂ nanospheres fused to plasmonic nanojunctions. Drastic improvements in Raman efficiencies are consistently achieved, with (single-wavelength) emissions reaching 10⁷ counts·mW−1·s−1 and 5 × 10⁵ counts·mW−1·s−1·molecule−1, for enhancement factors >1011. We demonstrate that such high efficiencies indeed enable tracking of single gold atoms and molecules with 17-μs time resolution, more than a thousandfold improvement over conventional high-performance plasmonic devices. Moreover, the obtained (integrated) megahertz count rates rival (even exceed) those of luminescent sources such as single-dye molecules and quantum dots, without bleaching or blinking.