2021/09/02 by Botond Tyukodi, Farzaneh Mohajerani, Tyukodi, Botond +7 · 1 citation
Earth and Planetary Sciences · Materials Science · #FOS: Physical sciences #Geology and Paleoclimatology Research #Paleontology and Stratigraphy of Fossils #Pickering emulsions and particle stabilization #Soft Condensed Matter (cond-mat.soft)
paper · pdf · doi:10.48550/arxiv.2109.01174
openalex publication_date 2021/09/02 · openalex created_date 2022/07/25 · openalex updated_date 2026/07/28
We use computational modeling to investigate the assembly thermodynamics of a particle-based model for geometrically frustrated assembly, in which the local packing geometry of subunits is incompatible with uniform, strain-free large-scale assembly. The model considers discrete triangular subunits that drive assembly towards a closed, hexagonal-ordered tubule, but have geometries that locally favor negative Gaussian curvature. We use dynamical Monte Carlo simulations and enhanced sampling methods to compute the free energy landscape and corresponding self-assembly behavior as a function of experimentally accessible parameters that control assembly driving forces and the magnitude of frustration. The results determine the parameter range where finite-temperature self-limiting assembly occurs, in which the equilibrium assembly size distribution is sharply peaked around a well-defined finite size. The simulations also identify two mechanisms by which the system can escape frustration and assemble to unlimited size, and determine the particle-scale properties of subunits that suppress unbounded growth.