How Far Can We Push Chemical Self-Assembly?

Service, Robert F.

doi:10.1126/science.309.5731.95

Cited by 326 publications

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“…Self-assembly is nature's prescription for the creation of complex structures from simpler building blocks (10,11). Although many novel building blocks have been discovered for self-assembly, differing in shape, composition, and functionality (12,13), the basic rules that govern this process are not yet understood in sufficient detail to realize target structures routinely through a priori design of building blocks.…”

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confidence: 99%

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Rational design of helical architectures

Chakrabarti¹,

Fejer²,

Wales³

2009

Proc. Natl. Acad. Sci. U.S.A.

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Nature has mastered the art of creating complex structures through self-assembly of simpler building blocks. Adapting such a bottom-up view provides a potential route to the fabrication of novel materials. However, this approach suffers from the lack of a sufficiently detailed understanding of the noncovalent forces that hold the self-assembled structures together. Here we demonstrate that nature can indeed guide us, as we explore routes to helicity with achiral building blocks driven by the interplay between two competing length scales for the interactions, as in DNA. By characterizing global minima for clusters, we illustrate several realizations of helical architecture, the simplest one involving ellipsoids of revolution as building blocks. In particular, we show that axially symmetric soft discoids can self-assemble into helical columnar arrangements. Understanding the molecular origin of such spatial organisation has important implications for the rational design of materials with useful optoelectronic applications.anisotropic interactions ͉ columnar arrangements ͉ helix ͉ self-assembly N ature provides ubiquitous examples of helical architecture with diverse functions. Helical structures are common structural motifs in biomolecules and are involved in the storage of genetic information (1). They are also important in solid-and liquid-crystal engineering for fabricating functional materials with useful optoelectronic applications (2-5). For example, discotic molecules in crystalline or liquid crystalline states often exhibit helical order in columnar arrangements (2-6), and such materials are attractive for use in optoelectronic devices because of the exceptional 1D charge-carrier mobilities along the columns (2-4). A common route to induce helicity in columnar arrangements is inclusion of chiral centers in discotic molecules (7). Helical columnar arrangements have also been realized in a few cases with achiral discotic molecules (8, 9), although no general strategy seems to have emerged.Self-assembly is nature's prescription for the creation of complex structures from simpler building blocks (10, 11). Although many novel building blocks have been discovered for self-assembly, differing in shape, composition, and functionality (12, 13), the basic rules that govern this process are not yet understood in sufficient detail to realize target structures routinely through a priori design of building blocks. Here we ask the specific question: Can we learn from nature how to design building blocks that self-assemble into helical structures? In seeking a guiding principle from nature for obtaining helical architectures, we considered DNA, in which two competing length scales exist, one characterizing the distance between consecutive nucleotides in the sugar-phosphate backbone and the other governing the stacking of the base pairs (1). The present contribution thus explores realizations of helical architectures with achiral building blocks driven by the interplay between two competing length scales. To this end, we c...

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confidence: 99%

“…The units of energy and length are chosen as the LJ parameters 11 and 11 , respectively. For the LJ interactions, we set 11 ϭ 22 ϭ 12 ϭ 1 and 11 ϭ 1.…”

mentioning

confidence: 99%

Rational design of helical architectures

Chakrabarti¹,

Fejer²,

Wales³

2009

Proc. Natl. Acad. Sci. U.S.A.

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“…However, the emergence of supramolecular chemistry has begun to enhance our understanding of biology and capacity for creating precise, physiologically structured materials. Nobel Laureate Jean-Marie Lehn insightfully described supramolecular interactions as "chemistry beyond the molecule," (4) because they enable dynamic macromolecular interactions, as well as the self-organization necessary to form higher-order structure in proteins and tissues (5). In the body, supramolecular presentation of bio-signals is exemplified by native extracellular matrix (ECM) interactions, including receptor-ECM interactions and heparin-binding proteins.…”

Section: From Molecular To Macroscopicmentioning

confidence: 99%

Progress in material design for biomedical applications

Tibbitt

Rodell

Burdick

et al. 2015

Proc. Natl. Acad. Sci. U.S.A.

213

138

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Biomaterials that interface with biological systems are used to deliver drugs safely and efficiently; to prevent, detect, and treat disease; to assist the body as it heals; and to engineer functional tissues outside of the body for organ replacement. The field has evolved beyond selecting materials that were originally designed for other applications with a primary focus on properties that enabled restoration of function and mitigation of acute pathology. Biomaterials are now designed rationally with controlled structure and dynamic functionality to integrate with biological complexity and perform tailored, high-level functions in the body. The transition has been from permissive to promoting biomaterials that are no longer bioinert but bioactive. This perspective surveys recent developments in the field of polymeric and soft biomaterials with a specific emphasis on advances in nano-to macroscale control, static to dynamic functionality, and biocomplex materials.biomaterials | soft materials | feature control | dynamics | biocomplex

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“…Another property often found in self-assembled systems is the sensitivity to perturbations exerted by the external environment. Self-assembly has been an important method to prepare new materials and create new functions [1][2][3][4][5].…”

Section: Introductionmentioning

confidence: 99%

Macromolecular self-assembly and nanotechnology in China

Chen

Wang

et al. 2013

Phil. Trans. R. Soc. A.

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Macromolecular self-assembly refers to the assembly of synthetic polymers, biomacromolecules and supra-molecular polymers. Through macromolecular self-assembly, the fabrication of ordered structures at different scales, the control of the dynamic assembly process and the integrations of advanced functions can be realized. Macromolecular self-assembly and nanotechnology research in China has developed rapidly, from the early periods of follow-up at low to high level and progress into a stage of innovation and creation. This review selects some representative progresses achieved recently, aiming to reflect the current status of macromolecular self-assembly and nanotechnology research in China.

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How Far Can We Push Chemical Self-Assembly?

Cited by 326 publications

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Rational design of helical architectures

Rational design of helical architectures

Progress in material design for biomedical applications

Macromolecular self-assembly and nanotechnology in China

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