Watching a Single Fluorophore Molecule Walk into a Plasmonic Hotspot

Abstract

Plasmonic nanoantennas allow for enhancing the spontaneous emission, altering the emission polarization, and shaping the radiation pattern of quantum emitters. A critical challenge for the experimental realizations is positioning a single emitter into the hotspot of a plasmonic antenna with nanoscale accuracy. We demonstrate a dynamic light-matter interaction nanosystem enabled by the DNA origami technique. A single fluorophore molecule can autonomously and unidirectionally walk into the hotspot of a plasmonic nanoantenna along a designated origami track. Successive fluorescence intensity increase and lifetime reduction are in situ monitored using single-molecule fluorescence spectroscopy, while the fluorophore walker gradually approaches and eventually enters the plasmonic hotspot. Our scheme offers a dynamic platform, which can be used to develop functional materials, investigate intriguing light-matter interaction phenomena, and serve as prototype system for examining theoretical models.

References in corpus (6)

• DNA-based Self-Assembly of Chiral Plasmonic Nanostructures with Tailored Optical Response
• On-command enhancement of single molecule fluorescence using a gold nanoparticle as an optical nano-antenna
• Atomically flat single-crystalline gold nanostructures for plasmonic nanocircuitry
• Controlled light-matter coupling for a single quantum dot embedded in a pillar microcavity using far-field optical lithography
• Controlled coupling of a single nitrogen-vacancy center to a silver nanowire
• Mode Modification of Plasmonic Gap Resonances induced by Strong Coupling with Molecular Excitons

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• Tailoring a Molecule's Optical Absorbance Using Surface Plasmonics
• LCAO-TDDFT-$k$-$\omega$: Spectroscopy in the Optical Limit
• Is there a proper figure of merit for a plasmonic structure involved in metal-enhanced fluorescence?
• Computational modeling of biological nanopores