Switchable Supracolloidal Coassembly of Microgels Mediated by Host/Guest Interactions

Supramolecular engineering of multibody colloidal systems provides flexible ways of manipulating superstructures and material properties. We investigate a coassembling microgel (MG) system, in which host- and guest-modified MG partners coassemble by molecular recognition, and show in detail how electrostatic repulsion needs to be balanced for the supramolecular recognition to take place. We observe a gradual change from repellent MGs to stable clusters and ordered flocculates upon decreasing electrostatic repulsion. The adaptive nature of the multivalent interactions embedded in the soft MG shell leads to kinetically trapped scenarios and fibril formation from spherical building blocks.