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Cascaded nanooptics to probe microsecond atomic-scale phenomena.

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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.



few-molecule sensing, microsecond integration times, nanolensing, nanophotonics, surface-enhanced Raman scattering (SERS)

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Proc Natl Acad Sci U S A

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Proceedings of the National Academy of Sciences


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Engineering and Physical Sciences Research Council (EP/L027151/1)
European Commission Horizon 2020 (H2020) Marie Sk?odowska-Curie actions (702005)
Isaac Newton Trust (18.08(K))
Leverhulme Trust (ECF-2018-021)
European Commission (658360)
Engineering and Physical Sciences Research Council (EP/L015978/1)
European Research Council (726470)
Engineering and Physical Sciences Research Council (EP/R020965/1)
Engineering and Physical Sciences Research Council (EP/G060649/1)
MK is grateful to the European Commission for a Marie Curie fellowship (grant 7020005, SPARCLEs). BdN acknowledges financial support from the Leverhulme Trust through an Early Career Fellowship and from the Newton Trust through matching funding. MK and BdN are also grateful for a Pump Prime grant from the Winton Programme for the Physics of Sustainability. RC acknowledges support from Trinity College, University of Cambridge. SJB thanks the European Commission for a Marie Curie fellowship (grant 658360, NANOSPHERE). OSO acknowledges the support of a Rubicon fellowship from the Netherlands Organisation for Scientific Research. JJB acknowledges support from the Engineering and Physical Sciences Research Council (EPSRC) UK through grants EP/L027151/1, EP/R020965/1, and NanoDTC EP/L015978/1. O.A.S. acknowledges the ERC-2016 Consolidator Grant (CAM-RIG, 726470) and EPSRC Programme Grant (NOtCH, EP/L027151/1) for funding. O.H. also acknowledges support from the EPSRC through grants EP/L024926/1 and EP/L027151/1.
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