Stochastic Yield Catastrophes and Robustness in Self-Assembly

Abstract

A guiding principle in self-assembly is that, for high production yield, nucleation of structures must be significantly slower than their growth. However, details of the mechanism that impedes nucleation are broadly considered irrelevant. Here, we analyze self-assembly into finite-sized target structures employing mathematical modeling. We investigate two key scenarios to delay nucleation: (i) by introducing a slow activation step for the assembling constituents and, (ii) by decreasing the dimerization rate. These scenarios have widely different characteristics. While the dimerization scenario exhibits robust behavior, the activation scenario is highly sensitive to demographic fluctuations. These demographic fluctuations ultimately disfavor growth compared to nucleation and can suppress yield completely. The occurrence of this stochastic yield catastrophe does not depend on model details but is generic as soon as number fluctuations between constituents are taken into account. On a broader perspective, our results reveal that stochasticity is an important limiting factor for self-assembly and that the specific implementation of the nucleation process plays a significant role in determining the yield.

References in corpus (10)

• Rational design of self-assembly pathways for complex multicomponent structures
• Mechanisms of kinetic trapping in self-assembly and phase transformation
• Understanding the Concentration Dependence of Viral Capsid Assembly Kinetics - the Origin of the Lag Time and Identifying the Critical Nucleus Size
• Numerical evidence for nucleated self-assembly of DNA brick structures
• Analyzing mechanisms and microscopic reversibility of self-assembly
• First passage times in homogeneous nucleation and self-assembly
• Growth of equilibrium structures built from a large number of distinct component types
• Stochastic self-assembly of incommensurate clusters
• Do hierarchical structures assemble best via hierarchical pathways?
• Hierarchical assembly may be a way to make large information-rich structures

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