Bifacial DNA Origami-Directed Discrete, Three-Dimensional, Anisotropic Plasmonic Nanoarchitectures with Tailored Optical Chirality

Lan, Xiang; Chen, Zhong; Dai, Guang; Lu, Xuxing; Ni, Weihai; Wang, Qiangbin

doi:10.1021/ja404354c

Cited by 210 publications

(208 citation statements)

References 25 publications

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“…Owing to close proximity, the excited plasmons in the two AuNRs can be strongly coupled 18 . The two crossed AuNRs constitute a 3D plasmonic chiral object [19][20][21][22] , which generates a theme of handedness when interacting with left-and right-handed circularly polarized light, giving rise to strong CD. …”

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Reconfigurable 3D plasmonic metamolecules

et al. 2014

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A reconfigurable plasmonic nanosystem combines an active plasmonic structure with a regulated physical or chemical control input. There have been considerable e orts on integration of plasmonic nanostructures with active platforms using topdown techniques. The active media include phase-transition materials, graphene, liquid crystals and carrier-modulated semiconductors, which can respond to thermal 1 , electrical 2 and optical stimuli 3-5 . However, these plasmonic nanostructures are often restricted to two-dimensional substrates, showing desired optical response only along specific excitation directions. Alternatively, bottom-up techniques o er a new pathway to impart reconfigurability and functionality to passive systems. In particular, DNA has proven to be one of the most versatile and robust building blocks 6-9 for construction of complex three-dimensional architectures with high fidelity 10-14 . Here we show the creation of reconfigurable three-dimensional plasmonic metamolecules, which execute DNA-regulated conformational changes at the nanoscale. DNA serves as both a construction material to organize plasmonic nanoparticles in three dimensions, as well as fuel for driving the metamolecules to distinct conformational states. Simultaneously, the threedimensional plasmonic metamolecules can work as optical reporters, which transduce their conformational changes in situ into circular dichroism changes in the visible wavelength range.Circular dichroism (CD), that is, differential absorption of left-and right-handed circularly polarized light, of natural chiral macromolecules is highly sensitive to their three-dimensional (3D) conformations 15 . Taking a similar strategy, we create 3D reconfigurable plasmonic chiral metamolecules 4,16 , whose conformation changes are highly correlated with their pronounced and distinct CD spectral changes in the visible wavelength range. Figure 1a shows the design schematic. Two gold nanorods (AuNRs) are hosted on a reconfigurable DNA origami template 7,10 , which consists of two 14-helix bundles (80 nm × 16 nm × 8 nm) folded from a long single-stranded DNA (ssDNA) scaffold with the help of hundreds of staple strands 13 . The two origami bundles are linked together by the scaffold strand passing twice between them at one point. To ensure the mobility of the DNA bundles and avoid the formation of a Holliday junction 17 , 8 unpaired bases are introduced to each ssDNA connector (Supplementary Note 1). Twelve binding sites are extended from each origami bundle for robust assembly of one AuNR (38 nm × 10 nm) functionalized with complementary DNA (Supplementary Note 2). The surface to surface distance of the two AuNRs is roughly 25 nm. Owing to close proximity, the excited plasmons in the two AuNRs can be strongly coupled 18 . The two crossed AuNRs constitute a 3D plasmonic chiral object [19][20][21][22] , which generates a theme of handedness when interacting with left-and right-handed circularly polarized light, giving rise to strong CD. Left-handedRight-handed Two gold nanorods (...

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Reconfigurable 3D plasmonic metamolecules

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“…In addition, the salient addressability of DNA origami allows us to engineer the structural handedness through precise control over the positions of the two AuNRs in the individual structure. 29,30 This is implemented by the parallel shiing of one AuNR from one to the other end of the second AuNR with spatial accuracy on the nanoscale.Inherent from the native assembly, the double stranded DNA (dsDNA) helices are unidirectionally oriented along the long …”

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3D plasmonic chiral colloids

et al. 2014

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3D plasmonic chiral colloids are synthesized through deterministically grouping of two gold nanorod AuNRs on DNA origami. These nanorod crosses exhibit strong circular dichroism (CD) at optical frequencies which can be engineered through position tuning of the rods on the origami. Our experimental results agree qualitatively well with theoretical predictions.The asset of DNA as nature's designer toolkit for structural technology has been explored for several decades. 1-5 The excellent control over topology and superior accuracy in templated synthesis bestow DNA the most successful molecule for programmable assembly of matter on the nanoscale. 6-10 The DNA origami technique, introduced by Rothemund, 11 relies on the nanoscale folding of a single-stranded viral DNA by numerous helper strands to create arbitrary 2D or 3D shapes. [11][12][13][14][15][16][17][18] Due to the fact that each individual helper strand can be modied and extended to produce a sequence-dependent surface tag, DNA origami can serve as a template to assemble functionalized nanoparticles. [19][20][21][22][23][24] Signicant progress in DNA origami technology has been concurrent with the prompt spanning of the scope of utility and diversity of possible conjugate materials. Among them, metal nanoparticles are one of the most exciting materials, whose versatile contributions in multiple disciplines have been indisputably witnessed. 25 A metal nanoparticle supports localized surface plasmons, which are associated with the collective oscillation of the conductive electrons in the nanoparticle. The localized nature of particle plasmons enables a vast range of useful applications, including surface-enhanced optical spectroscopies and subwavelength photonic devices, as well as medical diagnostics and therapeutics.Recently, considerable effort has been directed towards DNA origami templated assembly of gold nanoparticles into assortments of functional nanostructures. 26,27 Optical chirality in the visible spectral range is one of the most important pursuits in that it generally does not occur in natural chiral molecules. Recent seminal work was carried out by organizing gold spherical nanoparticles in a helical staircase on a DNA origami bundle. 28 However, due to the weak interaction between tiny gold nanoparticles, CD of these plasmonic helices was rather small. Alternatively, AuNRs have been considered owing to their excellent optical properties and stronger oscillator strength. For example, AuNRs were assembled on DNA origami to form chiral nanostructures. 29 However, the achieved CD response was still quite weak and the induced chiral effect due to the presence of DNA was not considered.Here we demonstrate 3D plasmonic chiral colloids assembled by DNA origami. Assemblies of crossed AuNRs templated by DNA origami are dispersed in a water-based solution. In each structure, two AuNRs are assembled on the opposite surfaces of a planar DNA origami sheet, forming a 90 twisting angle (see Fig. 1). Such crossed AuNRs constitute the simplest chiral object i...

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“…Liedl and co-workers 32 organized AuNPs into chirality-controlled nanohelices on a rod-like DNA origami template, resulting in defined circular dichroism and optical rotatory dispersion effects ( Figure 1b). As simpler alternatives, pronounced circular dichroism is also observed from chiral AuNP (Figure 1d) 33,34 and nanorod 35 arrays assembled on planar rectangular DNA origami templates. Furthermore, multiscaffold DNA origami ribbons have been shown to be powerful tools for the assembly of plasmonic waveguides consisting of linear AuNP arrays.…”

Section: Formation Of Plasmonic Patterns From Metal Npsmentioning

confidence: 99%

Spatial regulation of synthetic and biological nanoparticles by DNA nanotechnology

Yang

Liu

2015

NPG Asia Mater

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Nanoparticles are among the most fascinating materials because of their unique size-dependent properties. The spatial positioning of the nanoparticles with a nanoscale precision will greatly enhance their potential for use in the fabrication of functional materials and devices. Recently, the development of DNA nanotechnology has enabled the construction of two-and three-dimensional, precisely addressable nanostructures and devices based on DNA sequence design and programmable assembly. Advances in conjugating DNA with nanoparticles can bridge these two technologies and provide scientists with a new tool to study material transportation and energy transfer at a nanometer scale. In this review, we summarize the recent progress in this emerging research field, which includes not only the static arrangements of inorganic nanoparticles but also the dynamic regulation of organic and biological units at a nanometer scale. With the rapid development in this field, new challenges and new possibilities will emerge and bring about fruitful achievements with a significant impact on future work.

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Bifacial DNA Origami-Directed Discrete, Three-Dimensional, Anisotropic Plasmonic Nanoarchitectures with Tailored Optical Chirality

Cited by 210 publications

References 25 publications

Reconfigurable 3D plasmonic metamolecules

Reconfigurable 3D plasmonic metamolecules

3D plasmonic chiral colloids

Spatial regulation of synthetic and biological nanoparticles by DNA nanotechnology

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