Quantizing single-molecule surface-enhanced Raman scattering with DNA origami metamolecules

Abstract

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.

Gold nanoparticle-mediated non-covalent functionalization of graphene for field-effect transistors

“…S8 the Raman spectra of each step (in Fig. 1) with a 633 nm laser are shown 49,50,64,81,82 . At Raman shift between 1000 and 1700 cm -1 , we can observe the Raman peak of Au NP, which was invisible in the case of pristine graphene.…”

Exploiting Colloidal Metamaterials for Achieving Unnatural Optical Refractions

“…www.advmat.de www.advancedsciencenews.com metamolecules have inspired various experimental studies on the self-assembly of metallic colloidal clusters, as summarized in the next section. [28][29][30][31][32][33][34]39,40,[44][45][46][47][48][49][100][101][102][103]…”

“…The experimental observations of optical magnetism reported to date are still limited to the discrete unit of the well-assembled, individual 2D trimer, 2D tetramer, and 3D tetrahedral cluster. [28][29][30][31][32][33][34]39,40,[100][101][102][103] The advance in dark-field microscopic analyses has enabled these observations of magnetism from a single metamolecule. [176] This problem mainly originates from (i) low assembly yield and (ii) low robustness of the resonant modes against a few nanometer-error in the structures.…”

Highly sensitive SERS assay of DENV gene via a cascade signal amplification strategy of localized catalytic hairpin assembly and hybridization chain reaction

“…In response to the urgent need to develop new and more reliable detection methods, currently some recent advances in nanosensing have opened up new opportunities for developing novel optical and electrical methods for DENV detection, such as fluorescence [ [23] , [24] , [25] ], surface plasmon resonance (SPR) [ 26 ], surface-enhanced Raman spectroscopy (SERS) [ 27 , 28 ], and electrochemistry [ 29 , 30 ]. Among them, SERS as a molecular fingerprint spectrum which can achieve ultrasensitive detection even to single molecular level is considered to be a potential and powerful analysis tool [ [31] , [32] , [33] ]. For instance, Huh et al reported an on-chip SERS by integrating capture probe immobilized AuNPs and dye labeled target DNA for the detection of DENV-related nucleic acid sequences with a detection limit of 30 pM [ 34 ].…”