Free-Energy Functional Approach to Inverse Problems for Self-Assembly of Three-Dimensional Crystals

TL;DR

This paper introduces a variational free-energy functional method to reconstruct interparticle potentials for 3D crystal self-assembly, successfully predicting potentials for various lattices and confirming self-assembly via simulations.

Contribution

The study develops a novel variational approach to inverse self-assembly problems, enabling the reconstruction of interaction potentials for 3D crystals from their structures.

Findings

Successfully derived interaction potentials for fcc, bcc, and shx lattices.

Confirmed self-assembly of bcc and shx crystals in simulations.

Observed metastability of fcc lattice in many-particle systems.

Abstract

In this study, a variational method for the inverse problem of self-assembly, i.e., a reconstruction of the interparticle interaction potential of a given structure, is applied to three-dimensional crystals. According to the method, the interaction potential is derived as a function that maximizes the free-energy functional of the one- and two-particle density distribution functions. The interaction potentials of the target crystals, including those with face-centered cubic (fcc), body-centered cubic (bcc), and simple hexagonal (shx) lattices, are obtained by numerical maximization of the functional. Monte Carlo simulations for the systems of particles with these interactions were carried out, and the self-assembly of the target crystals was confirmed for the bcc and shx cases. However, in the many-particle system with the predicted interaction for the fcc lattice, the fcc lattice did not spontaneously form and was metastable.