Theoretical prediction of free-energy landscapes for complex self-assembly

Abstract

We present a technique for calculating free-energy profiles for the nucleation of multicomponent structures that contain as many species as building blocks. We find that a key factor is the topology of the graph describing the connectivity of the target assembly. By considering the designed interactions separately from weaker, incidental interactions, our approach yields predictions for the equilibrium yield and nucleation barriers. These predictions are in good agreement with corresponding Monte Carlo simulations. We show that a few fundamental properties of the connectivity graph determine the most prominent features of the assembly thermodynamics. Surprisingly, we find that polydispersity in the strengths of the designed interactions stabilizes intermediate structures and can be used to sculpt the free-energy landscape for self-assembly. Finally, we demonstrate that weak incidental interactions can preclude assembly at equilibrium due to the combinatorial possibilities for incorrect association.

References in corpus (4)

• An efficient, multiple range random walk algorithm to calculate the density of states
• DNA-Programmed Mesoscopic Architecture
• Numerical evidence for nucleated self-assembly of DNA brick structures
• Growth of equilibrium structures built from a large number of distinct component types

Cited by in corpus (18)

• Rational design of self-assembly pathways for complex multicomponent structures
• The Information Capacity of Specific Interactions
• Inverse Design of Simple Pair Potentials for the Self-Assembly of Complex Structures
• Associative pattern recognition through macro-molecular self-assembly
• Temperature Protocols to Guide Selective Self-Assembly of Competing Structures
• Differentiable Molecular Simulations for Control and Learning
• DNA brick self-assembly with an off-lattice potential
• Direct observation and rational design of nucleation behavior in addressable self-assembly
• Structure-based prediction of protein-folding transition paths
• Hierarchical assembly may be a way to make large information-rich structures
• 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
• The difficulty of folding self-folding origami
• Numerical calculation of free-energy barriers for entangled polymer nucleation
• Controlling Fragment Competition on Pathways to Addressable Self-Assembly
• Moderate Point: Balanced Entropy and Enthalpy Contributions in Soft Matter