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Self-assembly in natural and synthetic molecular systems can create complexaggregates or materials whose properties and functionality rises from theirinternal structure and molecular arrangement. The key microscopic features thatcontrol such assemblies remain poorly understood, nevertheless. Using classicaldensity functional theory we demonstrate how the intrinsic length scales andtheir interplay in terms of interspecies molecular interactions can be used totune soft matter self-assembly. We apply our strategy to two different softbinary mixtures to create guidelines for tuning intermolecular interactionsthat lead to transitions from fully miscible, liquid-like uniform state toformation of simple and core-shell aggregates, and mixed aggregate structures.Furthermore, we demonstrate how the interspecies interactions and systemcomposition can be used to control concentration gradients of component specieswithin these assemblies. The insight generated by this work contributes towardsunderstanding and controlling soft multi-component self-assembly systems.Additionally, our results aid in understanding complex biological assembliesand their function and provide tools to engineer molecular interactions inorder to control polymeric and protein-based materials, pharmaceuticalformulations, and nanoparticle assemblies.

Self-assembly of binary solutions to complex structures