Mapping Nanoscale Hotspots with Single-Molecule Emitters Assembled into Plasmonic Nanocavities Using DNA Origami.
File(s)1710.10910.pdf (1.14 MB)
Accepted version
Author(s)
Type
Journal Article
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.
Date Issued
2017-11-22
Online Publication Date
2018-11-22T07:00:18Z
Date Acceptance
2017-11-22
ISSN
1530-6984
Publisher
American Chemical Society
Start Page
405
End Page
411
Journal / Book Title
Nano Letters
Volume
18
Issue
1
Copyright Statement
© 2017 American Chemical Society
Source Database
pubmed
Subjects
DNA origami
Purcell factor
SERS
Single-molecule
nanoassembly
nanocavities
plasmonics
strong coupling
MD Multidisciplinary
Nanoscience & Nanotechnology
Publication Status
Published