From compact to fractal crystalline clusters in concentrated systems of monodisperse hard spheres

Abstract

We address the crystallization of monodisperse hard spheres in terms of the properties of finite- size crystalline clusters. By means of large scale event-driven Molecular Dynamics simulations, we study systems at different packing fractions ϕ ranging from weakly supersaturated state points to glassy ones, covering different nucleation regimes. We find that such regimes also result in different properties of the crystalline clusters: compact clusters are formed in the classical-nucleation-theory regime (ϕ \leq 0.54), while a crossover to fractal, ramified clusters is encountered upon increasing packing fraction (ϕ \geq 0.56), where nucleation is more spinodal-like. We draw an analogy between macroscopic crystallization of our clusters and percolation of attractive systems to provide ideas on how the packing fraction influences the final structure of the macroscopic crystals. In our previous work (Phys. Rev. Lett., 106, 215701, 2011), we have demonstrated how crystallization from a glass (at ϕ > 0.58) happens via a gradual (many-step) mechanism: in this paper we show how the mechanism of gradual growth seems to hold also in super-saturated systems just above freezing showing that static properties of clusters are not much affected by dynamics.

arXiv commentSoft Matter, 2012

References in corpus (32)

• Colloidal Gels: Equilibrium and Non-Equilibrium Routes
• Spatial Correlations of Mobility and Immobility in a Glassforming Lennard-Jones Liquid
• Equilibrium cluster phases and low-density arrested disordered states: The role of short-range attraction and long-range repulsion
• Dynamical Arrest in Attractive Colloids: The Effect of Long-Range Repulsion
• Probing the equilibrium dynamics of colloidal hard spheres above the mode-coupling glass transition
• Hard Spheres: Crystallization and Glass Formation
• Crystallization of hard-sphere glasses
• On measuring colloidal volume fractions
• Precursor-mediated crystallization process in suspensions of hard spheres
• Crystal nucleation of hard spheres using molecular dynamics, umbrella sampling and forward flux sampling: A comparison of simulation techniques
• Phase behavior of a fluid with competing attractive and repulsive interactions
• Colloidal systems with competing interactions: from an arrested repulsive cluster phase to a gel
• Confirmation of Anomalous Dynamical Arrest in attractive colloids: a molecular dynamics study
• A cluster mode-coupling approach to weak gelation in attractive colloids
• Equilibrium phase behavior of polydisperse hard spheres
• Modeling Equilibrium Clusters in Lysozyme Solutions
• Structural and dynamical features of multiple metastable glassy states in a colloidal system with competing interactions
• Evidence for out-of-equilibrium crystal nucleation in suspensions of oppositely charged colloids
• Crystalline phases of polydisperse spheres
• The Ultimate Fate of Supercooled Liquids
• Crystallization Mechanism of Hard Sphere Glasses
• Clusters in Simple Fluids
• Phase behavior and far-from-equilibrium gelation of charged attractive colloids
• Effect of bond lifetime on the dynamics of a short-range attractive colloidal system
• A unifying model for chemical and colloidal gels
• Equilibration of Concentrated Hard Sphere Fluids
• Monomer-resolved simulations of cluster-forming dendrimers
• Arrest of flow and emergence of activated processes at the glass transition of a suspension of particles with hard sphere-like interactions
• Crystallization in suspensions of hard spheres: A Monte Carlo and Molecular Dynamics simulation study
• Comment on "Probing the equilibrium dynamics of colloidal hard spheres above the mode-coupling glass transition"
• Dynamical Study of Polydisperse Hard-Sphere System
• Jamming, relaxation and crystallization of a super-cooled fluid in a three-dimensional lattice

Cited by in corpus (11)

• The role of local structure in dynamical arrest
• Crystal nucleation as the ordering of multiple order parameters
• Colloidal Hard Spheres: Triumphs, Challenges and Mysteries
• Morphology of clusters of attractive dry and wet self-propelled spherical particle suspensions
• Nucleation in sheared granular matter
• Non-classical pathways of crystallization in colloidal systems
• Crystal-to-crystal transition of ultrasoft colloids under shear
• The interplay of sedimentation and crystallization in hard-sphere suspensions
• Homogeneous Nucleation of Sheared Liquids: Advances and Insights from Simulations and Theory
• Orientational order and morphology of clusters of self-assembled Janus swimmers
• Crystallization in Glassy Suspensions of Hard Ellipsoids