Self-assembly of multicomponent structures in and out of equilibrium

TL;DR

This paper investigates multicomponent self-assembly, demonstrating that certain structures cannot be formed in quasiequilibrium but can be assembled far from equilibrium using dynamic scaling techniques.

Contribution

It introduces a nonperturbative strategy for self-assembly that enables the formation of target structures far from equilibrium, beyond traditional quasiequilibrium assumptions.

Findings

Structures with non-random compositional correlations cannot be generated at finite growth rates in quasiequilibrium.

Dynamic scaling allows the creation of equilibrium-like structures far from equilibrium.

Target structures can be designed to differ from equilibrium configurations and still be assembled accurately.

Abstract

Theories of phase change and self-assembly often invoke the idea of a `quasiequilibrium', a regime in which the nonequilibrium association of building blocks results nonetheless in a structure whose properties are determined solely by an underlying free energy landscape. Here we study a prototypical example of multicomponent self-assembly, a one-dimensional fiber grown from red and blue blocks. If the equilibrium structure possesses compositional correlations different from those characteristic of random mixing, then it cannot be generated without error at any finite growth rate: there is no quasiequilibrium regime. However, by exploiting dynamic scaling, structures characteristic of equilibrium at one point in phase space can be generated, without error, arbitrarily far from equilibrium. Our results thus suggest a `nonperturbative' strategy for multicomponent self-assembly in which the target structure is, by design, not the equilibrium one.