Xin, Ling, Lu, Mo, Both, Steffen, Pfeiffer, Markus, Urban, Maximilian J., Zhou, Chao ORCID: 0000-0003-1185-9964, Yan, Hao, Weiss, Thomas, Liu, Na and Lindfors, Klas ORCID: 0000-0002-6482-5605 (2019). Watching a Single Fluorophore Molecule Walk into a Plasmonic Hotspot. ACS Photonics, 6 (4). S. 985 - 1002. WASHINGTON: AMER CHEMICAL SOC. ISSN 2330-4022

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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.

Item Type: Journal Article
Creators:
CreatorsEmailORCIDORCID Put Code
Xin, LingUNSPECIFIEDUNSPECIFIEDUNSPECIFIED
Lu, MoUNSPECIFIEDUNSPECIFIEDUNSPECIFIED
Both, SteffenUNSPECIFIEDUNSPECIFIEDUNSPECIFIED
Pfeiffer, MarkusUNSPECIFIEDUNSPECIFIEDUNSPECIFIED
Urban, Maximilian J.UNSPECIFIEDUNSPECIFIEDUNSPECIFIED
Zhou, ChaoUNSPECIFIEDorcid.org/0000-0003-1185-9964UNSPECIFIED
Yan, HaoUNSPECIFIEDUNSPECIFIEDUNSPECIFIED
Weiss, ThomasUNSPECIFIEDUNSPECIFIEDUNSPECIFIED
Liu, NaUNSPECIFIEDUNSPECIFIEDUNSPECIFIED
Lindfors, KlasUNSPECIFIEDorcid.org/0000-0002-6482-5605UNSPECIFIED
URN: urn:nbn:de:hbz:38-151836
DOI: 10.1021/acsphotonics.8b01737
Journal or Publication Title: ACS Photonics
Volume: 6
Number: 4
Page Range: S. 985 - 1002
Date: 2019
Publisher: AMER CHEMICAL SOC
Place of Publication: WASHINGTON
ISSN: 2330-4022
Language: English
Faculty: Faculty of Mathematics and Natural Sciences
Divisions: Faculty of Mathematics and Natural Sciences > Department of Chemistry > Institute of Physical Chemistry
Subjects: no entry
Uncontrolled Keywords:
KeywordsLanguage
DNA ORIGAMI; QUANTUM DOTS; FLUORESCENCE ENHANCEMENT; NANOPARTICLE DIMERS; ROOM-TEMPERATURE; EMISSION; NANOSTRUCTURES; NANOANTENNAS; PRECISION; DNAZYMEMultiple languages
Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Optics; Physics, Applied; Physics, Condensed MatterMultiple languages
Refereed: Yes
URI: http://kups.ub.uni-koeln.de/id/eprint/15183

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