Self-assembly of two-component soft systems controlled by pairwise interactions

Self-assembly in natural and synthetic molecular systems can create complex aggregates or materials whose properties and functionalities rise from their internal structure and molecular arrangement. The key microscopic features that control such assemblies remain poorly understood, nevertheless. We demonstrate how the intrinsic length scales and their interplay in terms of inter-species molecular interactions can be used to tune soft matter self-assembly. Using classical density functional theory, we apply our strategy to soft binary mixtures to create guidelines for tuning inter-molecular interactions that lead to transitions from a fully miscible, liquid-like uniform state to formation of simple and core-shell aggregates and mixed aggregate structures, as well as to a system that provides a transition from regular single-core particles to multi-core aggregates that exhibit multiple structural length scales. Our results aid in understanding complex biological assemblies and their function and provide tools to engineer molecular interactions in order to control polymeric and protein-based materials, pharmaceutical formulations, and nanoparticle assemblies.