Two-stage crystallization of charged colloids under low supersaturation conditions

Kratzer, Kai; Arnold, Axel

doi:10.1039/c4sm02365j

Cited by 32 publications

(42 citation statements)

References 48 publications

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“…11), more clusters with HCP/FCC structure form, that grow over time. This result is qualitatively similar to results obtained for the Yukawa systems in [46] in which they studied the effect of the interaction energy, which can be related to S * in our model, on the crystallization dynamics. Here, we build on the knowledge about the crystallization process [46] by studying the effect of the additional degree of freedom, the particle radius.…”

Section: Structure Evolutionsupporting

confidence: 80%

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Effect of particle-size dynamics on properties of dense spongy-particle systems: Approach towards equilibrium

Zakhari¹,

Anderson

Hütter

2017

Phys. Rev. E

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Hütter, M. (2017). Effect of particle-size dynamics on properties of dense spongy-particle systems: Approach towards equilibrium. Physical Review E, 96(1), [012604]. DOI: 10.1103/PhysRevE.96.012604 General rights Copyright and moral rights for the publications made accessible in the public portal are retained by the authors and/or other copyright owners and it is a condition of accessing publications that users recognise and abide by the legal requirements associated with these rights.• Users may download and print one copy of any publication from the public portal for the purpose of private study or research.• You may not further distribute the material or use it for any profit-making activity or commercial gain • You may freely distribute the URL identifying the publication in the public portal ? Take down policyIf you believe that this document breaches copyright please contact us providing details, and we will remove access to the work immediately and investigate your claim. Open-porous deformable particles, often envisaged as sponges, are ubiquitous in biological and industrial systems (e.g. casein micelles in dairy products and microgels in cosmetics). The rich behavior of these suspensions is owing to the elasticity of the supporting network of the particle, and the viscosity of permeating solvent. Therefore, the rate-dependent size change of these particles depends on their structure, i.e. the permeability. This work aims at investigating the effect of the particle-size dynamics and the underlying particle structure, i.e. the particle permeability, on the transient and long-time behavior of suspensions of spongy particles in the absence of applied deformation, using the dynamic two-scale model developed by Hütter et al. [Faraday Discuss., 158, 407-424 (2012)]. In the high-density limit, the transient behavior is found to be accelerated by the particle-size dynamics, even at average size-changes as small as 1%. The accelerated dynamics is evidenced by (i) the higher short-time diffusion coefficient as compared to elastic-particle systems and (ii) the accelerated formation of the stable FCC crystal structure. Furthermore, after long times, the particle-size dynamics of spongy particles is shown to result in lower stationary values of the energy and normal stresses as compared to elastic-particle systems. This dependence of the long-time behavior of these systems on the permeability, that essentially is a transport coefficient and hence must not affect the equilibrium properties, confirms that full equilibration has not been reached.

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Section: Structure Evolutionsupporting

confidence: 80%

“…Particles are considered to be solid-like ifq 6 ≥ 0.29 and they are further categorized as BCC forq 4 ≤ 0.05, HCP for 0.05 <q 4 ≤ 0.1, and FCC forq 4 > 0.1 [44,46].…”

Section: A Average Local-order Parametermentioning

confidence: 99%

Effect of particle-size dynamics on properties of dense spongy-particle systems: Approach towards equilibrium

Zakhari¹,

Anderson

Hütter

2017

Phys. Rev. E

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“…6 Very recent simulations of the homogeneous liquid−fcc nucleation of charged colloids by K. Kratzer et al also show that the liquid−fcc transition involves two stages of the liquid−bcc and bcc−hcp/fcc transitions. 30 As they specially addressed, "according to Ostwald, the phase which is closest to the initial state in free energy is nucleated first, which doesn't have to be the truly stable phase. In addition, Stranski and Totomanow found that the phase with the lowest free energy barrier is nucleated first..."…”

Section: ■ Results and Discussionmentioning

confidence: 99%

Crystallization Kinetics of Concurrent Liquid–Metastable and Metastable–Stable Transitions, and Ostwald’s Step Rule

Zhou

Qin

et al. 2015

Langmuir

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Experimental measurements of colloidal crystallization in a wide range of volume fractions of charged particles were performed to investigate the liquid−metastable−stable transition process. To fit the obtained experimental data, we developed a theoretical model to formulate the kinetics of the concurrent liquid− metastable and metastable−stable transitions. This model is wellsupported by our observations. We found that when the ratio of the metastable−stable transition rate to the liquid−metastable rate is very large, the metastable state can become undetectable, although it still exists, offering a possible explanation for very few exceptions to Ostwald's step rule. ■ INTRODUCTIONColloidal crystallization has attracted a great deal of attention as a model system for mimicking the atomic or molecular counterparts, and also for assessing the validity of classical crystal growth theories.1−5 Understanding the nature of the structural evolution during nucleation and growth is still a fundamental and challenging issue in condensed-matter science.6,7 One of the major relevant topics is Ostwald's step rule, 8 first proposed in 1897 as an empirical rule, stating that in general it is not the most stable, but the least stable, polymorph that crystallizes first.However, Ostwald's step rule is not yet a universal law for two reasons. First, there are exceptions (although very few) to the rule. Second, an undisputed theoretical basis for the rule has not been formulated successfully. Over the past 100 years, various attempts were made to reach the goal, but none of them were successful. In 1978, on the basis of the mean-field treatment, Alexander and McTague 9 published their striking result predicting that a body-centered cubic (bcc) structure should be formed first regardless of whether a more thermodynamically stable one exists, as long as the first-order nature of the transition from the liquid is not too distinct. Since then, a great deal of research attention has been devoted to finding the existence of the metastable bcc phase in various systems.10,11 Among these efforts, our previous studies focused more on the issues of the structural evolution in colloidal crystallization. 12,13 We quantitatively demonstrated bcc's formation and face-centered cubic (fcc)'s growth at the expense of metastable bcc, confirming the existence of the metastable bcc phase. However, determining how to explain the exceptions to the step rule is still an interesting issue. To explore this more deeply, we conducted a series of experiments in an extended range of volume fractions, Φ, covering the phase behavior involved in entire liquid−metastable−stable (L−M−S) transitions. To fit the obtained experimental data, we also proposed a new theoretical model and found that the model fits the data very well.Analyzing our experimental data with an appropriate theoretical model is critical for a better understanding of the phase transition kinetics. Dating back to 1940s, the Kolmogorov, Mehl, Johnson, and Avrami (KMJA) phenomenological mo...

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“…Evidence of bond orientational foreshadowing of crystallization has been suggested for colloidal systems both in simulations [11,12,31,60,64,73] and experiments [65,66,74]. Interestingly, the role of structural fluctuations has been investigated also in a variety of different systems, like water [75], metallic melts [76,77], anisotropic particles [78][79][80], and polymers [81,82].…”

Section: Two-step Nucleation and Precursorsmentioning

confidence: 99%

Nonclassical pathways of crystallization in colloidal systems

Russo

Tanaka

2016

MRS Bull.

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Colloidal systems offer the ideal conditions to study the nucleation process, both from an experimental viewpoint, due to their relative large size and long time-scales, and from a modeling point of view, due to the tunability of their interactions. Here we review some recent works that study the process of colloidal crystallization from a microscopic perspective. We focus in particular on non-classical pathways to nucleation where the appearance of the solid crystals involves fluctuations of two (or more) order parameters. We interpret the non-classical behavior as a decoupling of positional and orientational symmetry breaking. We then consider how the nucleation pathway determines which polymorph is selected upon nucleation from the melt. Moreover we show how the study of nucleation pathways not only sheds new light on the microscopic mechanism of nucleation, but also provides important information regarding its avoidance, thus suggesting a deep link between crystallization and vitrification.

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Two-stage crystallization of charged colloids under low supersaturation conditions

Cited by 32 publications

References 48 publications

Effect of particle-size dynamics on properties of dense spongy-particle systems: Approach towards equilibrium

Effect of particle-size dynamics on properties of dense spongy-particle systems: Approach towards equilibrium

Crystallization Kinetics of Concurrent Liquid–Metastable and Metastable–Stable Transitions, and Ostwald’s Step Rule

Nonclassical pathways of crystallization in colloidal systems

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