Engineered Core-Shell Nanostructures through Bio-Inspired Self-Assembly

From the crystal structure of a ribosome to viral capsids, self-assembly is a fundamental principle in nature for forming complex and functional structures. The self-assembly of nanomaterials offers a bottom-up approach to the development of functional materials with optical, electromagnetic, and biological properties. These include applications such as polymeric nanocontainers for targeted drug delivery, 3D electrical networks, photonic crystals, and field-effect transistors. We investigate the self-assembly of multiple types of nanoparticles in a one-pot mixture using a system of charged virus-like particles (VLPs) and oppositely charged dendritic polymers. Using coarse-grained molecular dynamics simulations we demonstrate that salt dialysis, VLP stoichiometry, and temperature can be leveraged to self-assemble different macrostructures of core-shell morphology starting from a solution of multiple types of VLPs. Our in silico predictions include the experimentally-validated ordered core-shell arrays, where each layer is formed by a single type of VLPs, as well as novel bio-inspired materials such as hybrid core-shell structures with multicomponent cores and one-component shells, and patchy core-shell structures with cores enveloped by a patchy shell of two distinct VLP types, creating a multifunctional outer layer. Our simulations elucidate how modulation of solution conditions alters the linker-VLP interactions that give rise to these distinct macrostructures, opening pathways to engineer complex nanomaterials with tunable functionality, driven by principles of biological self-assembly.