Composition-agnostic prediction of self-assembly in multicomponent amphiphile mixtures from molecular structure

TL;DR

This paper introduces a machine-learning framework that predicts self-assembly behaviors of multicomponent amphiphiles directly from molecular structures, regardless of component number or identity, enabling efficient material design.

Contribution

It extends the critical packing parameter to multi-component systems and develops a graph convolutional network model with strong extrapolative capabilities for predicting self-assembly.

Findings

GCN-GCN architecture outperforms other models

Model accurately predicts for unseen components

Framework enables virtual screening of amphiphilic materials

Abstract

Predicting self-assembly in multi-component amphiphilic systems is challenging due to the complexity of intercomponent interactions and the combinatorial growth of possible formulations. In this study, we develop a unified machine-learning framework that directly predicts self-assembly behavior from the molecular structures of constituent components, independent of the number or identity of those components. We extend the critical packing parameter (CPP) to multi-component systems and generate a large dataset of self-assembled morphologies using dissipative particle dynamics (DPD) simulations. By systematically evaluating twelve combinations of feature extraction methods and model architectures, we find that models incorporating a fully connected graph convolutional network (GCN) layer achieve superior performance, with the GCN-GCN architecture accurately capturing both intramolecular relationships and intercomponent interactions. Notably, this model exhibits strong extrapolative capability: it accurately predicts CPP values for five-component mixtures even when trained only on systems with fewer components, and it maintains high accuracy for mixtures composed of molecular species that are entirely absent from the training data. These results demonstrate that a composition-agnostic predictive framework can enable efficient virtual screening and provide a foundation for the rational design of complex amphiphilic materials.