title: Generic, phenomenological, on-the-fly renormalized repulsion model for self-limited organization of terminal supraparticle assemblies.
abstract: Self-limited, or terminal, supraparticles have long received great interest because of their abundance in biological systems (DNA bundles and virus capsids) and their potential use in a host of applications ranging from photonics and catalysis to encapsulation for drug delivery. Moreover, soft, uniform colloidal aggregates are a promising candidate for quasicrystal and other hierarchical assemblies. In this work, we present a generic coarse-grained model that captures the formation of self-limited assemblies observed in various soft-matter systems including nanoparticles, colloids, and polyelectrolytes. Using molecular dynamics simulations, we demonstrate that the assembly process is self-limited when the repulsion between the particles is renormalized to balance their attraction during aggregation. The uniform finite-sized aggregates are further shown to be thermodynamically stable and tunable with a single dimensionless parameter. We find large aggregates self-organize internally into a core-shell morphology and exhibit anomalous uniformity when the constituent nanoparticles have a polydisperse size distribution.
authors.affiliation: Department of Chemical Engineering, University of Michigan, Ann Arbor, MI 48109;
authors.forename: Trung Dac
authors.initials: TD
authors.lastname: Nguyen
authors.affiliation: Department of Physics, University of Michigan, Ann Arbor, MI 48109;
authors.forename: Benjamin A
authors.initials: BA
authors.lastname: Schultz
authors.affiliation: Department of Chemical Engineering, University of Michigan, Ann Arbor, MI 48109; Department of Materials Science and Engineering, University of Michigan, Ann Arbor, MI 48109; Biointerfaces Institute, University of Michigan, Ann Arbor, MI 48109.
authors.forename: Nicholas A
authors.initials: NA
authors.lastname: Kotov
authors.affiliation: Department of Chemical Engineering, University of Michigan, Ann Arbor, MI 48109; Department of Physics, University of Michigan, Ann Arbor, MI 48109; Department of Materials Science and Engineering, University of Michigan, Ann Arbor, MI 48109; Biointerfaces Institute, University of Michigan, Ann Arbor, MI 48109 sglotzer@umich.edu.
authors.forename: Sharon C
authors.initials: SC
authors.lastname: Glotzer
mesh_terms: D003102:Colloids / Q000737:chemistry; D004247:DNA / Q000737:chemistry; D016503:Drug Delivery Systems; D004573:Electrolytes / Q000737:chemistry; D008962:Models, Theoretical; D056004:Molecular Dynamics Simulation
chemical_list: D003102:Colloids; D004573:Electrolytes; D004247:DNA
keywords: self-assembly; self-limited aggregation; terminal assemblies