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arXiv · 2105.02043

Watching a Single Fluorophore Molecule Walk into a Plasmonic Hotspot

Ling Xin·Mo Lu·Steffen Both·Markus Pfeiffer·Maximilian J. Urban·Chao Zhou·Hao Yan·Thomas Weiss·Na Liu·Klas Lindfors
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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.

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Ling Xin, Mo Lu, Steffen Both, Markus Pfeiffer, Maximilian J. Urban, Chao Zhou, Hao Yan, Thomas Weiss, Na Liu, Klas Lindfors. 2021-04-30. Watching a Single Fluorophore Molecule Walk into a Plasmonic Hotspot. https://doi.org/10.1021/acsphotonics.8b01737

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