Convective Assembly of 2D Lattices of Virus‐like Particles Visualized by In‐Situ Grazing‐Incidence Small‐Angle X‐Ray Scattering

Abstract The rapid assembly of icosohedral virus‐like particles (VLPs) into highly ordered (domain size > 600 nm), oriented 2D superlattices directly onto a solid substrate using convective coating is demonstrated. In‐situ grazing‐incidence small‐angle X‐ray scattering (GISAXS) is used to follow the self‐assembly process in real time to characterize the mechanism of superlattice formation, with the ultimate goal of tailoring film deposition conditions to optimize long‐range order. From water, GISAXS data are consistent with a transport‐limited assembly process where convective flow directs assembly of VLPs into a lattice oriented with respect to the water drying line. Addition of a nonvolatile solvent (glycerol) modified this assembly pathway, resulting in non‐oriented superlattices with improved long‐range order. Modification of electrostatic conditions (solution ionic strength, substrate charge) also alters assembly behavior; however, a comparison of in‐situ assembly data between VLPs derived from the bacteriophages MS2 and Qβ show that this assembly process is not fully described by a simple Derjaguin–Landau–Verwey–Overbeek model alone.