TY - JOUR

T1 - Maximizing the Accessibility in DNA Origami Nanoantenna Plasmonic Hotspots

AU - Close, Cindy

AU - Trofymchuk, Kateryna

AU - Grabenhorst, Lennart

AU - Lalkens, Birka

AU - Glembockyte, Viktorija

AU - Tinnefeld, Philip

N1 - Funding Information: The authors thank Vivien Behrendt, Dr. Benedikt Hauer, and Dr.‐Ing. Albrecht Brandenburg (Fraunhofer‐Institut für Physikalische Messtechnik IPM, Freiburg, Germany) for cooperation on the DNA origami and assay development and Prof. Tim Liedl/Prof. Joachim Rädler (Ludwig‐Maximilians‐Universität, Department für Physik, Munich, Germany) for providing access to their facilities, especially to the transmission electron microscope, and to Dr. Florian Selbach for preforming TEM measurements. C.C. thanks Maximilian Sacherer and Jakob Hartmann for help with experiments in the early project stages and Renukka Yaadav, as well as Martina Pfeiffer for fruitful cooperation on related projects. P.T. gratefully acknowledges financial support from the DFG (grant number TI 329/9‐2, project number 267681426, INST 86/1904‐1 FUGG, excellence cluster e‐conversion EXC 2089/1‐390776260), Sino‐German Center for Research Promotion (grant agreement C‐0008), BMBF (Grants POCEMON, 13N14336, and SIBOF, 03VP03891). B.L. acknowledges funding by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under Germany's Excellence Strategy—EXC‐2123 QuantumFrontiers—390837967 and “Niedersächsisches Vorab” through “Quantum‐ and Nano‐Metrology (QUANOMET)” initiative within the project NL‐1. V.G. acknowledges the support from European Union's Horizon 2020 research and innovation program under the Marie Skłodowska‐Curie actions (grant agreement No. 840741). K.T. and V.G. acknowledge the support by Humboldt Research Fellowships from the Alexander von Humboldt Foundation.

PY - 2022/8/23

Y1 - 2022/8/23

N2 - DNA nanotechnology has conquered the challenge of positioning quantum emitters in the hotspot of optical antenna structures for fluorescence enhancement. Therefore, DNA origami serves as the scaffold to arrange nanoparticles and emitters, such as fluorescent dyes. For the next challenge of optimizing the applicability of plasmonic hotspots for molecular assays, a Trident DNA origami structure that increases the accessibility of the hotspot is introduced, thereby improving the kinetics of target molecule binding. This Trident NanoAntenna with Cleared HOtSpot (NACHOS) is compared with previous DNA origami nanoantennas and improved hotspot accessibility is demonstrated without compromising fluorescence enhancement. The approach taps into the potential of Trident NACHOS for single-molecule-based plasmonic biosensing.

AB - DNA nanotechnology has conquered the challenge of positioning quantum emitters in the hotspot of optical antenna structures for fluorescence enhancement. Therefore, DNA origami serves as the scaffold to arrange nanoparticles and emitters, such as fluorescent dyes. For the next challenge of optimizing the applicability of plasmonic hotspots for molecular assays, a Trident DNA origami structure that increases the accessibility of the hotspot is introduced, thereby improving the kinetics of target molecule binding. This Trident NanoAntenna with Cleared HOtSpot (NACHOS) is compared with previous DNA origami nanoantennas and improved hotspot accessibility is demonstrated without compromising fluorescence enhancement. The approach taps into the potential of Trident NACHOS for single-molecule-based plasmonic biosensing.

KW - biosensing

KW - DNA nanotechnology

KW - nanoantenna hotspot

KW - plasmonics

KW - plasmonic hotspot accessibility

KW - single-molecule detection

KW - single-molecule fluorescence

UR - http://www.scopus.com/inward/record.url?scp=85133184362&partnerID=8YFLogxK

U2 - 10.1002/admi.202200255

DO - 10.1002/admi.202200255

M3 - Article

VL - 9

JO - Advanced materials interfaces

JF - Advanced materials interfaces

SN - 2196-7350

IS - 24

M1 - 2200255

ER -