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arXiv · 1710.10910

Mapping nanoscale hotspots with single-molecule emitters assembled into plasmonic nanocavities using DNA origami

Rohit Chikkaraddy·V. A. Turek·Nuttawut Kongsuwan·Felix Benz·Cloudy Carnegie·Tim van de Goor·Bart de Nijs·Angela Demetriadou·Ortwin Hess·Ulrich F. Keyser·Jeremy J. Baumberg
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Abstract

Fabricating nanocavities in which optically-active single quantum emitters are precisely positioned, is crucial for building nanophotonic devices. Here we show that self-assembly based on robust DNA-origami constructs can precisely position single molecules laterally within sub-5nm gaps between plasmonic substrates that support intense optical confinement. By placing single-molecules at the center of a nanocavity, we show modification of the plasmon cavity resonance before and after bleaching the chromophore, and obtain enhancements of $\geq4\times10^3$ with high quantum yield ($\geq50$%). By varying the lateral position of the molecule in the gap, we directly map the spatial profile of the local density of optical states with a resolution of $\pm1.5$ nm. Our approach introduces a straightforward non-invasive way to measure and quantify confined optical modes on the nanoscale.

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Rohit Chikkaraddy, V. A. Turek, Nuttawut Kongsuwan, Felix Benz, Cloudy Carnegie, Tim van de Goor, Bart de Nijs, Angela Demetriadou, Ortwin Hess, Ulrich F. Keyser, Jeremy J. Baumberg. 2017-10-30. Mapping nanoscale hotspots with single-molecule emitters assembled into plasmonic nanocavities using DNA origami. https://doi.org/10.1021/acs.nanolett.7b04283

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