Self-assembling Ordered Arrays of Virus-like Particles Mediated by Linkers*

Virus-like particles (VLPs), themselves self-assembled from protein subunits, can be exploited to generate hierarchical functional materials for applications in catalysis and photonics. We present an integrated experimental and computational method to understand and control higher-order VLP assembly into three dimensional, ordered arrays that is applicable to a variety of VLP-linker systems. Specifically, we study the assembly of bacteriophage P22 VLPs mediated by oppositely-charged, macromolecular dendrimers. The integrated approach demonstrates VLPs self-assemble into ordered arrays in the presence of dendrimers as the ionic strength is lowered below a threshold value. This threshold may be tuned by genetically engineering the VLP surface charge. At threshold, the common lattice structure exhibits the same long-range order and a similar configuration of bridging dendrimers, regardless of the VLP surface charge. The experimentally-validated model identifies key electrostatic and kinetic mechanisms, predicting dendrimer concentration as a control parameter for modulating assembly. The integrated approach opens new design and control strategies to fabricate active hierarchical materials.