Cascaded nanooptics to probe microsecond atomic-scale phenomena

Marlous Kamp, Bart de Nijs, Nuttawut Kongsuwan, Matthias Saba, Rohit Chikkaraddy, Charlie A. Readman, William M. Deacon, Jack Griffiths, Steven J. Barrow, Oluwafemi S. Ojambati, Demelza Wright, Junyang Huang, Ortwin Hess, Oren A. Scherman, Jeremy J. Baumberg

Research output: Contribution to journalArticlepeer-review


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.
Original languageEnglish
JournalProceedings of the National Academy of Sciences
Issue number26
Publication statusPublished - Jun 2020


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