Journal
NANO LETTERS
Volume 18, Issue 1, Pages 405-411Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.7b04283
Keywords
Single-molecule; DNA origami; plasmonics; nanocavities; nanoassembly; Purcell factor; strong coupling; SERS
Categories
Funding
- EPSRC [EP/G060649/1, EP/K028510/1, EP/L027151/1]
- BBSRC [BB/I022686/1]
- ERC [LINASS 320503]
- ERC Consolidator Grant [67144]
- Dr. Manmohan Singh scholarship from St. John's College
- Winton Programme for the Physics of Sustainability
- NPL [PO443073]
- Biotechnology and Biological Sciences Research Council [BB/I022686/1] Funding Source: researchfish
- Engineering and Physical Sciences Research Council [EP/K028510/1, EP/G060649/1, EP/L027151/1] Funding Source: researchfish
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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-5 nm 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 >= 4 X 10(3) with high quantum yield (>= 50%). 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 +/- 1.5 nm. Our approach introduces a straightforward noninvasive way to measure and quantify confined optical modes on the nanoscale.
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