Distance dependent interaction between a single emitter and a single dielectric nanoparticle using DNA origami

TL;DR

This study uses DNA origami to precisely position silicon nanoparticles near single fluorophores, revealing distance-dependent optical interactions that outperform metallic nanoantennas in fluorescence enhancement and quenching.

Contribution

It introduces a method to study single-molecule interactions with dielectric nanoantennas using DNA origami, highlighting their advantages over metallic structures.

Findings

Significant decay rate modification observed

Minimal quenching at short distances

High fluorescence quantum yield maintained

Abstract

Optical nanoantennas can manipulate light-matter interactions at the nanoscale, modifying the emission properties of nearby single photon emitters. To date, most optical antennas are based on metallic nanostructures that exhibit unmatched performance in terms of electric field enhancement but suffer from substantial ohmic losses that limit their applications. To circumvent these limitations, there is a growing interest in alternative materials. In particular, high-refractive-index dielectrics have emerged as promising candidates, offering negligible ohmic losses, and supporting both electric and magnetic resonances in the visible and near-infrared range that can unlock novel effects. Currently, the few available studies on dielectric nanoantennas focus on ensemble measurements. Here, we exploit the DNA origami technique to study the interaction between silicon nanoparticles and organic fluorophores at the single molecule level, in controlled geometries and at different spectral ranges within the visible spectrum. We characterize their distance-dependent interaction in terms of fluorescence intensity and lifetime, revealing a significant modification of the decay rate together with minimal quenching and a high fluorescence quantum yield even at short distances from the dielectric nanoparticle. This work demonstrates the advantages of dielectric nanoantennas over their metallic counterparts and paves the way for their applications in single-molecule spectroscopy and sensing.