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Over the past two decades, a large number of studies addressed the topic of crystal nucleation in suspensions of hard spheres. The shared result of all these efforts is that, at low super-saturations, experimentally observed nucleation…

Soft Condensed Matter · Physics 2022-06-22 Wilkin Wöhler , Tanja Schilling

The crystallization of a metastable melt is one of the most important non equilibrium phenomena in condensed matter physics, and hard sphere colloidal model systems have been used for several decades to investigate this process by…

Soft Condensed Matter · Physics 2015-05-20 Tanja Schilling , Sven Dorosz , Hans Joachim Schoepe , George Opletal

In the study of crystal nucleation via computer simulations, hard spheres are arguably the most extensively explored model system. Nonetheless, even in this simple model system, the complex thermodynamics of crystal nuclei can sometimes…

Soft Condensed Matter · Physics 2025-02-19 Marjolein de Jager , Carlos Vega , Pablo Montero de Hijes , Frank Smallenburg , Laura Filion

We study crystal nucleation under the influence of sedimentation in a model of colloidal hard spheres via Brownian Dynamics simulations. We introduce two external fields acting on the colloidal fluid: a uniform gravitational field (body…

Soft Condensed Matter · Physics 2013-07-03 John Russo , Anthony C. Maggs , Daniel Bonn , Hajime Tanaka

We report on a large scale computer simulation study of crystal nucleation in hard spheres. Through a combined analysis of real and reciprocal space data, a picture of a two-step crystallization process is supported: First dense, amorphous…

Soft Condensed Matter · Physics 2015-05-18 T. Schilling , H. J. Schope , M. Oettel , G. Opletal , I. Snook

We determined bulk crystal nucleation rates in aqueous suspensions of charged spheres at low metastability. Experiments were performed in dependence on electrolyte concen-tration and for two different particle number densities. The…

Soft Condensed Matter · Physics 2021-11-04 Jürgen Schwarz , Paul Leiderer , Thomas Palberg

Motivated by old experiments on colloidal suspensions, we report molecular dynamics simulations of assemblies of hard spheres, addressing crystallization and glass formation. The simulations cover wide ranges of polydispersity s (standard…

Materials Science · Physics 2015-05-13 P. N. Pusey , E. Zaccarelli , C. Valeriani , E. Sanz , W. C. K. Poon , M. E. Cates

The nucleation of crystals in liquids is one of nature's most ubiquitous phenomena, playing an important role in areas such as climate change and the production of drugs. As the early stages of nucleation involve exceedingly small time and…

Crystallization is often assumed to be a quasi-static process that is unaffected by details of particle transport other than the bulk diffusion coefficient. Therefore colloidal suspensions are frequently argued to be an ideal toy model for…

Statistical Mechanics · Physics 2013-04-16 Dominic Roehm , Stefan Kesselheim , Axel Arnold

The discrepancy in nucleation rate densities between simulated and experimental hard spheres remains staggering and unexplained. Suggestively, more strongly sedimenting colloidal suspensions of hard spheres nucleate much faster than weakly…

Soft Condensed Matter · Physics 2021-12-08 Nicholas Wood , John Russo , Francesco Turci , C. Patrick Royall

Over the last number of years several simulation methods have been introduced to study rare events such as nucleation. In this paper we examine the crystal nucleation rate of hard spheres using three such numerical techniques: molecular…

Soft Condensed Matter · Physics 2012-08-17 Laura Filion , Michiel Hermes , Ran Ni , Marjolein Dijkstra

We have carried out molecular dynamics simulations of the crystallization of hard spheres modelling colloidal systems that are studied in conventional and space-based experiments. We use microscopic probes to investigate the effects of…

Condensed Matter · Physics 2009-11-07 Igor Volkov , Marek Cieplak , Joel Koplik , Jayanth R. Banavar

Hard-sphere model systems are well-suited in both experiment and simulations to investigate fundamental aspects of the crystallization of fluids. In experiments on colloidal models of hard-sphere fluids, the uid is unavoidably at contact…

Soft Condensed Matter · Physics 2021-04-28 Jorge R. Espinosa , Carlos Vega , Chantal Valeriani , Daan Frenkel , Eduardo Sanz

We investigate the early part of the crystal nucleation process in the hard sphere fluid using data produced by computer simulation. We find that hexagonal order manifests continuously in the overcompressed liquid, beginning approximately…

Soft Condensed Matter · Physics 2016-06-29 Joshua T. Berryman , Muhammad Anwar , Sven Dorosz , Tanja Schilling

A widely spread method of crystal preparation is to precipitate it from a supersaturated solution. In such a process, control of solution concentration is of paramount importance. Nucleation process, polymorph selection, and crystal habits…

Soft Condensed Matter · Physics 2019-07-10 Tarak Karmakar , Pablo M. Piaggi , Michele Parrinello

We study the spontaneous nucleation and crystallization of linear and cyclic chains of flexibly connected hard spheres using extensive molecular dynamics simulations. To this end, we present a novel event-driven molecular dynamics…

Soft Condensed Matter · Physics 2012-06-27 Ran Ni , Marjolein Dijkstra

We consider homogeneous crystallisation rates in confocal microscopy experiments on colloidal nearly hard spheres at the single particle level. These we compare with Brownian dynamics simuations by carefully modelling the softness in the…

Soft Condensed Matter · Physics 2017-12-27 Jade Taffs , Stephen R. Williams , Hajime Tanaka , C. Patrick Royall

We study numerically the crystallization process in a supersaturated suspension of repulsive colloidal particles driven by simple shear flow. The effect of the shear flow on crystallization is two-fold: while it suppresses the initial…

Soft Condensed Matter · Physics 2013-07-02 Boris Lander , Udo Seifert , Thomas Speck

Dynamical heterogeneities in a colloidal fluid close to gelation are studied by means of computer simulations. A clear distinction between some fast particles and the rest, slow ones, is observed, yielding a picture of the gel composed by…

Soft Condensed Matter · Physics 2009-11-10 Antonio M. Puertas , Matthias Fuchs , Michael E. Cates

In supercooled liquids, vitrification generally suppresses crystallization. Yet some glasses can still crystallize despite the arrest of diffusive motion. This ill-understood process may limit the stability of glasses, but its microscopic…

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