Direct observation and rational design of nucleation behavior in addressable self-assembly

Abstract

In order to optimize a self-assembly reaction, it is essential to understand the factors that govern its pathway. Here, we examine the influence of nucleation pathways in a model system for addressable, multicomponent self-assembly based on a prototypical 'DNA-brick' structure. By combining temperature-dependent dynamic light scattering and atomic force microscopy with coarse-grained simulations, we show how subtle changes in the nucleation pathway profoundly affect the yield of the correctly formed structures. In particular, we can increase the range of conditions over which self-assembly occurs by utilizing stable multi-subunit clusters that lower the nucleation barrier for assembling subunits in the interior of the structure. Consequently, modifying only a small portion of a structure is sufficient to optimize its assembly. Due to the generality of our coarse-grained model and the excellent agreement that we find with our experimental results, the design principles reported here are likely to apply generically to addressable, multicomponent self-assembly.

References in corpus (12)

• The Statistical Mechanics of Dynamic Pathways to Self-assembly
• Rational design of self-assembly pathways for complex multicomponent structures
• Numerical evidence for nucleated self-assembly of DNA brick structures
• Programmable Control of Nucleation for Algorithmic Self-Assembly
• Theoretical prediction of free-energy landscapes for complex self-assembly
• Non-Close-Packed Three-Dimensional Quasicrystals
• DNA brick self-assembly with an off-lattice potential
• Self-assembly of two-dimensional binary quasicrystals: A possible route to a DNA quasicrystal
• Design Strategies for Self-Assembly of Discrete Targets
• Multi-scale coarse-graining for the study of assembly pathways in DNA-brick self assembly
• Effects of co-ordination number on the nucleation behaviour in many-component self-assembly
• Investigating the role of boundary bricks in DNA brick self-assembly

Cited by in corpus (7)

• Pattern recognition in the nucleation kinetics of non-equilibrium self-assembly
• Temperature Protocols to Guide Selective Self-Assembly of Competing Structures
• Differentiable Molecular Simulations for Control and Learning
• Linker-mediated self-assembly of mobile DNA-coated colloids
• Simulations of DNA-origami self-assembly reveal design-dependent nucleation barriers
• Lattice models and Monte Carlo methods for simulating DNA origami self-assembly
• Controlling Fragment Competition on Pathways to Addressable Self-Assembly