Linker-Mediated Assembly of Virus-Like Particles into Ordered Arrays via Electrostatic Control

Nanoscale virus-like particles (VLPs), which are self-assembled from protein subunits, offer the possibility of generating hierarchically assembled functional materials such as biomimetic catalytic systems and optical metamaterials. We explore the capacity to control and tune a higher-order assembly of VLPs into ordered array materials over a wide range of ionic conditions using a combination of experimental and computational methods. The integrated methodology demonstrates that P22 VLP variants, genetically engineered to exhibit different surface charges, self-assemble into ordered arrays in the presence of PAMAM dendrimers acting as oppositely charged, macromolecular linkers. Ordered assembly occurs at an optimal ionic strength that strongly correlates with the VLP surface charge. The ordered VLP arrays exhibit the same long-range order and a similar configuration of VLP-bound dendrimers, regardless of the VLP surface charge. The experimentally validated model identifies key electrostatic and kinetic mechanisms underlying the self-assembly process and guides the modulation of dendrimer concentration as a control parameter to tune the assembly of VLPs. The integrated approach opens new design and control strategies to fabricate active functional materials via the self-assembly of engineered VLPs.