Effects of co-ordination number on the nucleation behaviour in many-component self-assembly

Abstract

We report canonical and grand-canonical lattice Monte Carlo simulations of the self-assembly of addressable structures comprising hundreds of distinct component types. The nucleation behaviour, in the form of free-energy barriers to nucleation, changes significantly as the co-ordination number of the building blocks is changed from 4 to 8 to 12. Unlike tetrahedral structures - which roughly correspond to DNA bricks that have been studied in experiment - the shapes of the free-energy barriers of higher co-ordination structures depend strongly on the supersaturation, and such structures require a very significant driving force for structure growth before nucleation becomes thermally accessible. Although growth at high supersaturation results in more defects during self-assembly, we show that high co-ordination number structures can still be assembled successfully in computer simulations and that they exhibit self-assembly behaviour analogous to DNA bricks. In particular, the self-assembly remains modular, enabling in principle a wide variety of nanostructures to be assembled, with a greater spatial resolution than is possible in low co-ordination structures.

Faraday Discussions 2015

References in corpus (6)

• Rational design of self-assembly pathways for complex multicomponent structures
• Multifarious Assembly Mixtures: Systems Allowing Retrieval of Diverse Stored Structures
• Theoretical prediction of free-energy landscapes for complex self-assembly
• Growth of equilibrium structures built from a large number of distinct component types
• Hierarchical assembly may be a way to make large information-rich structures
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Cited by in corpus (5)

• Direct observation and rational design of nucleation behavior in addressable self-assembly
• DNA brick self-assembly with an off-lattice potential
• Simulations of DNA-origami self-assembly reveal design-dependent nucleation barriers
• Multi-scale coarse-graining for the study of assembly pathways in DNA-brick self assembly
• Investigating the role of boundary bricks in DNA brick self-assembly