Quantizing single-molecule surface-enhanced Raman scattering with DNA origami metamolecules
Tailored metal nanoclusters have been actively developed to manipulate light at the subwavelength scale for nanophotonic applications. Nevertheless, precise arrangement of molecules in a hot spot with fixed numbers and positions remains challenging. Here, we show that DNA origami metamolecules with...
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| Main Authors: | , , |
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| Format: | Article (Journal) |
| Language: | English |
| Published: |
[27 September 2019]
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| In: |
Science advances
Year: 2019, Volume: 5, Issue: 9 |
| ISSN: | 2375-2548 |
| DOI: | 10.1126/sciadv.aau4506 |
| Online Access: | Verlag, Volltext: https://doi.org/10.1126/sciadv.aau4506 Verlag, Volltext: https://advances.sciencemag.org/content/5/9/eaau4506 
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| Author Notes: | Weina Fang, Sisi Jia, Jie Chao, Liqian Wang, Xiaoyang Duan, Huajie Liu, Qian Li, Xiaolei Zuo, Lihua Wang, Lianhui Wang, Na Liu, Chunhai Fan |
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| 520 | |a Tailored metal nanoclusters have been actively developed to manipulate light at the subwavelength scale for nanophotonic applications. Nevertheless, precise arrangement of molecules in a hot spot with fixed numbers and positions remains challenging. Here, we show that DNA origami metamolecules with Fano resonances (DMFR) can precisely localize single dye molecules and produce quantified surface-enhanced Raman scattering (SERS) responses. To enable tailored plasmonic permutations, we develop a general and programmable method for anchoring a set of large gold nanoparticles (L-AuNPs) on prescribed n-tuple docking sites of super-origami DNA frameworks. A tetrameric nanocluster with four spatially organized 80-nm L-AuNPs exhibits peak-and-dip Fano characteristics. The drastic enhancement at the wavelength of the Fano minimum allows the collection of prominent SERS spectrum for even a single dye molecule. We expect that DMFR provides physical insights into single-molecule SERS and opens new opportunities for developing plasmonic nanodevices for ultrasensitive sensing, nanocircuits, and nanophotonic lasers. - Plasmonic nanostructures supporting strong spatially confined field enhancement are developed to probe single-molecule SERS. - Plasmonic nanostructures supporting strong spatially confined field enhancement are developed to probe single-molecule SERS. | ||
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