Mapping Nanoscale Hotspots with Single-Molecule Emitters Assembled into Plasmonic Nanocavities Using DNA Origami.
Published version
Peer-reviewed
Repository URI
Repository DOI
Change log
Authors
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-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 × 103 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.
Description
Keywords
Journal Title
Conference Name
Journal ISSN
1530-6992
Volume Title
Publisher
Publisher DOI
Sponsorship
European Research Council (320503)
Engineering and Physical Sciences Research Council (EP/L027151/1)
Engineering and Physical Sciences Research Council (EP/L015978/1)
Engineering and Physical Sciences Research Council (EP/G060649/1)
Engineering and Physical Sciences Research Council (EP/K028510/1)