Multilayered ordered arrays self-assembled from a mixed population of nanoparticles

Ordered self-assembled structures composed of multiple building blocks are ubiquitous in nature and have inspired many bottom-up strategies for the synthesis of nanomaterials with applications in drug delivery, biomimetic catalysts, and sensing, among others. We explore the synthesis of bio-inspired nanomaterials through the self-assembly of up to 4 different types of nanoscale virus-like particles (VLPs) derived from bacteriophage P22, which can be genetically engineered to express different surface charges. We develop a coarse-grained model to capture the assembly behavior over a broad range of VLP surface charges (-500e to -2000e) and salt concentrations (10 mM to 1000 mM). Molecular dynamics simulations based on this experimentally-validated model are used to probe the self-assembly of mixtures of multiple types of VLPs in the presence of oppositely-charged dendrimers that act as linkers. Through different combinations of two-component mixtures, we demonstrate that the self-assembly of multilayered ordered arrays, where each layer is composed of a single type of building block, can be engineered over a broad range of salt concentrations. The coarse-grained model also enables the investigation of three- and four-component mixtures, which are presented. The reversible nature of assembly and the effects of gradual vs rapid lowering of ionic strength are also discussed.