scholarly journals A versatile DNA origami based plasmonic nanoantenna for label-free single-molecule SERS

2020 ◽  
Author(s):  
Kosti Tapio ◽  
Amr Mostafa ◽  
Yuya Kanehira ◽  
Antonio Suma ◽  
Anushree Dutta ◽  
...  

Abstract DNA origami technology allows for the precise nanoscale assembly of chemical entities that give rise to new functional materials. We have created a versatile DNA Origami Nanofork Antenna (DONA) by assembling Au or Ag nanoparticle dimers with 1.17 ± 0.67 nm gap size, enabling signal enhancements in surface-enhanced Raman scattering (SERS) of up to 1011. This allows for single-molecule SERS measurements, which can even be performed with larger gap sizes to accommodate differently sized molecules, and at various excitation wavelengths. A general scheme is presented to place single analyte molecules into the SERS hot spots using the DNA origami structure exploiting covalent and non-covalent coupling schemes. By using Au and Ag dimers, single-molecule SERS measurements of three dyes and cytochrome c and horseradish peroxidase proteins are demonstrated even under non-resonant excitation conditions, thus providing long photostability during time-series measurement, and enabling unprecedented optical monitoring of single molecules and DNA origami based nanomachines.

2020 ◽  
Author(s):  
Kosti Tapio ◽  
Amr Mostafa ◽  
Yuya Kanehira ◽  
Antonio Suma ◽  
Anushree Dutta ◽  
...  

Abstract DNA origami technology allows for the precise nanoscale assembly of chemical entities that give rise to new functional materials. We have created a versatile DNA Origami Nanofork Antenna (DONA) by assembling Au or Ag nanoparticle dimers with different gap sizes down to 1.17 nm, enabling signal enhancements in surface-enhanced Raman scattering (SERS) of up to 1011. This allows for single-molecule SERS measurements, which can even be performed with larger gap sizes to accommodate differently sized molecules, and at various excitation wavelengths. A general scheme is presented to place single analyte molecules into the SERS hot spots using the DNA origami structure exploiting covalent and non-covalent coupling schemes. By using Au and Ag dimers, single-molecule SERS measurements of three dyes and cytochrome c and horseradish peroxidase proteins are demonstrated even under non-resonant excitation conditions, thus providing long photostability during time-series measurement, and enabling unprecedented optical monitoring of single molecules.


Molecules ◽  
2021 ◽  
Vol 26 (6) ◽  
pp. 1684
Author(s):  
Sergio Kogikoski ◽  
Kosti Tapio ◽  
Robert Edler von Zander ◽  
Peter Saalfrank ◽  
Ilko Bald

Surface-enhanced Raman scattering is a powerful approach to detect molecules at very low concentrations, even up to the single-molecule level. One important aspect of the materials used in such a technique is how much the signal is intensified, quantified by the enhancement factor (EF). Herein we obtained the EFs for gold nanoparticle dimers of 60 and 80 nm diameter, respectively, self-assembled using DNA origami nanotriangles. Cy5 and TAMRA were used as surface-enhanced Raman scattering (SERS) probes, which enable the observation of individual nanoparticles and dimers. EF distributions are determined at four distinct wavelengths based on the measurements of around 1000 individual dimer structures. The obtained results show that the EFs for the dimeric assemblies follow a log-normal distribution and are in the range of 106 at 633 nm and that the contribution of the molecular resonance effect to the EF is around 2, also showing that the plasmonic resonance is the main source of the observed signal. To support our studies, FDTD simulations of the nanoparticle’s electromagnetic field enhancement has been carried out, as well as calculations of the resonance Raman spectra of the dyes using DFT. We observe a very close agreement between the experimental EF distribution and the simulated values.


ACS Nano ◽  
2021 ◽  
Vol 15 (4) ◽  
pp. 7065-7077
Author(s):  
Kosti Tapio ◽  
Amr Mostafa ◽  
Yuya Kanehira ◽  
Antonio Suma ◽  
Anushree Dutta ◽  
...  

ACS Nano ◽  
2016 ◽  
Vol 10 (11) ◽  
pp. 9809-9815 ◽  
Author(s):  
Sabrina Simoncelli ◽  
Eva-Maria Roller ◽  
Patrick Urban ◽  
Robert Schreiber ◽  
Andrew J. Turberfield ◽  
...  

2019 ◽  
Vol 5 (9) ◽  
pp. eaau4506 ◽  
Author(s):  
Weina Fang ◽  
Sisi Jia ◽  
Jie Chao ◽  
Liqian Wang ◽  
Xiaoyang Duan ◽  
...  

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.


Nanoscale ◽  
2016 ◽  
Vol 8 (10) ◽  
pp. 5612-5620 ◽  
Author(s):  
J. Prinz ◽  
C. Heck ◽  
L. Ellerik ◽  
V. Merk ◽  
I. Bald

DNA origami nanostructures are used to arrange gold nanoparticles into dimers with defined distance, which can be exploited as novel substrates for surface enhanced Raman scattering (SERS). Single dye molecules (TAMRA and Cy3) can be placed into the SERS hot spots, with Raman enhancement up to 1010, which is sufficient to detect single molecules by Raman scattering.


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