Self-assembly prediction of architecture-controlled bottlebrush copolymers in solution using graph convolutional networks

Abstract

The investigation of bottlebrush copolymer self-assembly in solution involves a comprehensive approach integrating simulation and experimental research, due to their unique physical characteristics. However, the intricate architecture of bottlebrush copolymers and the diverse solvent conditions introduce a wide range of parameter spaces. In this study, we investigated the solution self-assembly behavior of bottlebrush copolymers by combining dissipative particle dynamics (DPD) simulation results and machine learning (ML) including graph convolutional networks (GCNs). The architecture of bottlebrush copolymers is encoded by graphs including connectivity, side chain length, bead types, and interaction parameters of DPD simulation. Using GCN, we accurately predicted the single chain properties of bottlebrush copolymers with over 95% accuracy. Furthermore, phase behavior was precisely predicted using these single chain properties. Shapley additive explanations (SHAP) values of single chain properties to the various self-assembly morphologies were calculated to investigate the correlation between single chain properties and morphologies. In addition, we analyzed single chain properties and phase behavior as a function of DPD interaction parameters, extracting relevant physical properties for vesicle morphology formation. This work paves the way for tailored design in solution of self-assembled nanostructures of bottlebrush copolymers, offering a GCN framework for precise prediction of self-assembly morphologies under various chain architectures and solvent conditions.