Self-assembly of magnetite nanocubes into helical superstructures.

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Abstract

Organizing inorganic nanocrystals into complex architectures is challenging and typically relies on preexisting templates, such as properly folded DNA or polypeptide chains. We found that under carefully controlled conditions, cubic nanocrystals of magnetite self-assemble into arrays of helical superstructures in a template-free manner with >99% yield. Computer simulations revealed that the formation of helices is determined by the interplay of van der Waals and magnetic dipole-dipole interactions, Zeeman coupling, and entropic forces and can be attributed to spontaneous formation of chiral nanocube clusters. Neighboring helices within their densely packed ensembles tended to adopt the same handedness in order to maximize packing, thus revealing a novel mechanism of symmetry breaking and chirality amplification.

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Anisotropy of building blocks and their assembly into complex structures.

Sharon C. Glotzer, Michael Solomon (2007)

A revolution in novel nanoparticles and colloidal building blocks has been enabled by recent breakthroughs in particle synthesis. These new particles are poised to become the 'atoms' and 'molecules' of tomorrow's materials if they can be successfully assembled into useful structures. Here, we discuss the recent progress made in the synthesis of nanocrystals and colloidal particles and draw analogies between these new particulate building blocks and better-studied molecules and supramolecular objects. We argue for a conceptual framework for these new building blocks based on anisotropy attributes and discuss the prognosis for future progress in exploiting anisotropy for materials design and assembly.

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DNA-guided crystallization of colloidal nanoparticles.

Dmytro Nykypanchuk, Mathew Maye, Daniel van der Lelie … (2008)

Many nanometre-sized building blocks will readily assemble into macroscopic structures. If the process is accompanied by effective control over the interactions between the blocks and all entropic effects, then the resultant structures will be ordered with a precision hard to achieve with other fabrication methods. But it remains challenging to use self-assembly to design systems comprised of different types of building blocks-to realize novel magnetic, plasmonic and photonic metamaterials, for example. A conceptually simple idea for overcoming this problem is the use of 'encodable' interactions between building blocks; this can in principle be straightforwardly implemented using biomolecules. Strategies that use DNA programmability to control the placement of nanoparticles in one and two dimensions have indeed been demonstrated. However, our theoretical understanding of how to extend this approach to three dimensions is limited, and most experiments have yielded amorphous aggregates and only occasionally crystallites of close-packed micrometre-sized particles. Here, we report the formation of three-dimensional crystalline assemblies of gold nanoparticles mediated by interactions between complementary DNA molecules attached to the nanoparticles' surface. We find that the nanoparticle crystals form reversibly during heating and cooling cycles. Moreover, the body-centred-cubic lattice structure is temperature-tuneable and structurally open, with particles occupying only approximately 4% of the unit cell volume. We expect that our DNA-mediated crystallization approach, and the insight into DNA design requirements it has provided, will facilitate both the creation of new classes of ordered multicomponent metamaterials and the exploration of the phase behaviour of hybrid systems with addressable interactions.

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DNA-based Self-Assembly of Chiral Plasmonic Nanostructures with Tailored Optical Response

Alexander Högele, Günther Pardatscher, Zhiyuan Fan … (2011)

Surface plasmon resonances generated in metallic nanostructures can be utilized to tailor electromagnetic fields. The precise spatial arrangement of such structures can result in surprising optical properties that are not found in any naturally occurring material. Here, the designed activity emerges from collective effects of singular components equipped with limited individual functionality. Top-down fabrication of plasmonic materials with a predesigned optical response in the visible range by conventional lithographic methods has remained challenging due to their limited resolution, the complexity of scaling, and the difficulty to extend these techniques to three-dimensional architectures. Molecular self-assembly provides an alternative route to create such materials which is not bound by the above limitations. We demonstrate how the DNA origami method can be used to produce plasmonic materials with a tailored optical response at visible wavelengths. Harnessing the assembly power of 3D DNA origami, we arranged metal nanoparticles with a spatial accuracy of 2 nm into nanoscale helices. The helical structures assemble in solution in a massively parallel fashion and with near quantitative yields. As a designed optical response, we generated giant circular dichroism and optical rotary dispersion in the visible range that originates from the collective plasmon-plasmon interactions within the nanohelices. We also show that the optical response can be tuned through the visible spectrum by changing the composition of the metal nanoparticles. The observed effects are independent of the direction of the incident light and can be switched by design between left- and right-handed orientation. Our work demonstrates the production of complex bulk materials from precisely designed nanoscopic assemblies and highlights the potential of DNA self-assembly for the fabrication of plasmonic nanostructures.

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Journal

Journal ID (iso-abbrev): Science

Title: Science (New York, N.Y.)

ISSN (Electronic): 1095-9203

ISSN (Print): 0036-8075

Publication date (Electronic): Sep 5 2014

Volume: 345

Issue: 6201

Affiliations

[1 ] Department of Organic Chemistry, Weizmann Institute of Science, Rehovot 76100, Israel.

[2 ] Department of Chemistry, University of Illinois, Chicago, IL 60607, USA.

[3 ] Department of Chemistry, University of Illinois, Chicago, IL 60607, USA. Department of Physics, University of Illinois, Chicago, IL 60607, USA. rafal.klajn@weizmann.ac.il pkral@uic.edu.

[4 ] Department of Organic Chemistry, Weizmann Institute of Science, Rehovot 76100, Israel. rafal.klajn@weizmann.ac.il pkral@uic.edu.

Article

Publisher Item ID: science.1254132

DOI: 10.1126/science.1254132

PubMed ID: 25061133

SO-VID: 2400f3cc-28c4-4af8-98bd-7df0ed5b731c

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Self-assembly of magnetite nanocubes into helical superstructures.

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Most cited references 68

Anisotropy of building blocks and their assembly into complex structures.

DNA-guided crystallization of colloidal nanoparticles.

DNA-based Self-Assembly of Chiral Plasmonic Nanostructures with Tailored Optical Response

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