Exploiting classical nucleation theory for reverse self-assembly

TL;DR

This paper presents a novel method leveraging classical nucleation theory to design interparticle interactions for targeted self-assembly of specific crystal structures, demonstrating its application to cubic and square symmetries.

Contribution

It introduces a new approach to reverse-engineer interparticle interactions based on nucleation free-energy barriers for desired crystal structures.

Findings

Successfully designed interactions for cubic and square crystal structures

Exploited nucleation barrier curvature to optimize self-assembly

Proposed a general model for infinite interaction geometries

Abstract

In this paper we introduce a new method to design interparticle interactions to target arbitrary crystal structures via the process of self-assembly. We show that it is possible to exploit the curvature of the crystal nucleation free-energy barrier to sample and select optimal interparticle interactions for self-assembly into a desired structure. We apply this method to find interactions to target two simple crystal structures: a crystal with simple cubic symmetry and a two-dimensional plane with square symmetry embedded in a three-dimensional space. Finally, we discuss the potential and limits of our method and propose a general model by which a functionally infinite number of different interaction geometries may be constructed and to which our reverse self-assembly method could in principle be applied.