Accelerated single photon emission from dye molecule-driven nanoantennas assembled on DNA

Abstract

A photon interacts efficiently with an atom when its frequency corresponds exactly to the energy between two eigenstates. But at the nanoscale, homogeneous and inhomogeneous broadenings strongly hinder the ability of solid-state systems to absorb, scatter or emit light. By compensating the impedance mismatch between visible wavelengths and nanometre-sized objects, optical antennas can enhance light-matter interactions over a broad frequency range. Here we use a DnA template to introduce a single dye molecule in gold particle dimers that act as antennas for light with spontaneous emission rates enhanced by up to two orders of magnitude and single photon emission statistics. Quantitative agreement between measured rate enhancements and theoretical calculations indicate a nanometre control over the emitterparticle position while 10 billion copies of the target geometry are synthesized in parallel. optical antennas can thus tune efficiently the photo-physical properties of nano-objects by precisely engineering their electromagnetic environment.

DNA origami based assembly of gold nanoparticle dimers for surface-enhanced Raman scattering

“…A particularly exciting sensing application utilizing plasmons has been the creation of metallic nanostructures using doublestranded DNA (dsDNA) linkers 22,23 as well as DNA origami 24 . The oscillations of conduction electrons create localized surface plasmons in metal nanoparticles (NPs) which enhance local fields in a small volume around the NP 25,26 .…”

Metal Nanoparticles for Microscopy and Spectroscopy

“…According to electrodynamic calculations, the field enhancement in the 1-2 nm gaps can be as high as 100, corresponding to a 10 4 times enhancement. Recent measurements of spontaneous emission of dye molecules localized in the gap [41] confirm the presence of very strongly enhanced fields. The compatibility of Au with DNA chemistry and the emergence of techniques like DNA origami means that arbitrary scaffolds for bottom-up fabrication of plasmon structures with ultrasmall gaps can be created.…”

Plasmonic Purcell factor and coupling efficiency to surface plasmons. Implications for addressing and controlling optical nanosources

“…Moreover, optical nanoantenna could efficiently interface molecular fluorescent emission and a nanophotonic waveguide [73] with possible applications to realize a platform for quantum optics. In addition, coupling a single photon source to an optical nano-antenna permits to control its emission cadency [74,75,76,77,78,79,80,81,82,83]. Realization of indistiguishable single photons is also a major issue [84,85].…”