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WIREs Nanomed Nanobiotechnol
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DNA‐based plasmonic nanoarchitectures: from structural design to emerging applications

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Abstract Plasmonic nanoarchitectures refer to the well‐defined groupings of elementary metallic nanoparticle building blocks. Such nanostructures have a plethora of technical applications in diagnostics, energy‐harvesting, and nanophotonic circuits, to name a few. Nevertheless, it remains challenging to construct plasmonic nanoarchitectures at will inexpensively. Bottom‐up self‐assembly is promising to overcome these limitations, but such methods often produce defects and low‐yields. For these purposes, DNA has emerged as a powerful nanomaterial beyond its genetic function in biology to either program or template synthesis of plasmonic nanostructures, or act as a ligand to mediate large‐area self‐assembly. In conjunction with top‐down lithography, DNA‐based strategies can afford excellent control over internal and overall structures of plasmonic nanoarchitectures. In this review, we outline the representative methodologies for building various well‐defined plasmonic nanoarchitectures and cover their recent exciting applications. WIREs Nanomed Nanobiotechnol 2012, 4:587–604. doi: 10.1002/wnan.1184 This article is categorized under: Diagnostic Tools > Diagnostic Nanodevices Diagnostic Tools > In Vitro Nanoparticle-Based Sensing Nanotechnology Approaches to Biology > Nanoscale Systems in Biology

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Plasmonic nanostructures derived from mono‐DNA and site‐specific DNA conjugates. (a) Schematic and TEM images for 10 nm AuNPs homodimer and 5/10/10 nm AuNPs heterotrimer constructed from mono‐DNA conjugates. (b) Chiral nanostructures built by using DNA‐AuNPs monoconjugats with four different sizes at DNA pyramids tips. (c) Dendrimer‐like nanostructures formed by asymmetric functionalized AuNPs. (d) End, side, and satellite nanostructures formed by AuNPs and Au nanorods after selective modification using DNA. (e) Stepwise surface modification of AuNPs and formation of two‐faced cluster with anisotropic nanostructures.

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Applications of DNA‐based plasmonic nanostructures. (a) Colorimetric DNA detection method using DNA‐functionalized particles as probes and the complementary DNA strands as target molecules. (b) Plasmon ruler used in the detection of the hybridization of complementary DNA to the ssDNA linkers. After hybridization, the particles were pushed apart due to the more rigid nature of dsDNA than ssDNA, which resulted in a blue‐shift of ∼2.1 nm measured by monitoring the spectrum of single AuNPs dimer. (c) SERS‐active Au–Ag core–shell nanodumbbells assembled by DNA hybridization. In this nanostructure, a single Raman‐active Cy3 dye molecule is located in the gap of this heterodimer, followed by Ag shells deposition on the surface of the dimeric nanodumbbell. Left figure shows Raman spectra taken from Cy3‐modified oligonucleotides (red line) and Cy3‐free oligonucleotides (black line) in NaCl‐aggregated silver colloids.

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Top‐down lithography integrates with bottom‐up DNA‐programmed self‐assembly. (a) Cross‐sectional scheme of a microdroplet confined in a micromould showing center dewetting. Localized assembly of the AuNPs microdiscs was then achieved by DNA‐programmed crystallization. (b) SEM image of nanoparticle disks pattern with highly ordered internal structures. (c) Large‐area patterning of AuNPs (5 nm) onto spatially ordered, 2D arrays through the site‐selective deposition of triangular DNA origami onto lithographically patterned substrates.

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DNA as entropic ligands in drying‐mediated self‐assembly. (a) Free‐standing monolayered DNA‐AuNPs superlattice sheets. Three‐dimensional STEM tomography reconstruction of a folded sheet (left) and TEM image (right) showing hexagonal ordering. (b) Drying‐mediated deformation of DNA corona in 3D supercrystals.

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DNA‐templated self‐assembly constructed by using DNA tiles and DNA origami. (a) DNA‐functionalized AuNPs were organized into closely packed rows with precisely defined regular inter‐row spacings templated by the DNA scaffolding. (b) Three‐dimensional plasmonic tubular spirals of AuNPs using DNA tile‐mediated self‐assembly. (c) Encapsulated ‘nanopeapod’ AuNPs 1D chains using triangular DNA nanotubes with longitudinal variation as host. TEM image (right side) shows that encapsulated AuNPs could be spontaneously released from the nanotubes by simple addition of specific DNA strands. (d) Six‐nanoparticle self‐similar chain nanostructures using triangular DNA‐origami templates. (e) DNA origami‐templated AuNRs dimer that form with various predetermined inter‐rod angles.

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(a) DNA‐functionalized nanoparticles/nanoshells into heteropentamer clusters (pentamers), which consist of a smaller gold nanosphere (74 nm) surrounded by a ring of four larger nanoshells ([r1, r2] = [62.5, 92.5] nm). (b) Schematic illustration of RCA on DNA‐AuNPs that served as a scaffold for the formation of satellite 3D nanostructures. AFM image (right) showed superstructures constructed from 5 and 15 nm AuNPs (large bright spots).

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(a) DNA‐functionalized AuNPs can be assembled into different crystallographic lattice structures programmed by the sequence of the DNA linkers. (b) Schematic of hexagonal superlattice of standing AuNRs with corresponding TEM images. (c) Scheme illustration of using 3D hollow DNA spacers in AuNP crystallization. TEM images of a bcc lattice (left) formed from AuNPs (20 nm) and DNA spacer (10 nm), and ‘Lattice X’ (right) structure formed from AuNPs (10 nm) and DNA spacer (20 nm). (d) Controllable switching of interparticle distances by using a reconfigurable DNA device (ld) that acts as an interparticle linkage. After addition of set DNA strands (s1, s2), ld structure can be reversibly transformed from a flexible C configuration to stem loop RS and linear RL morphologies.

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Diagnostic Tools > In Vitro Nanoparticle-Based Sensing
Diagnostic Tools > Diagnostic Nanodevices
Nanotechnology Approaches to Biology > Nanoscale Systems in Biology

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