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1.
Proc Natl Acad Sci U S A ; 118(3)2021 01 19.
Article in English | MEDLINE | ID: mdl-33397813

ABSTRACT

Despite the omnipresence of colloidal suspensions, little is known about the influence of colloid shape on phase transformations, especially in nonequilibrium. To date, real-space imaging results at high concentrations have been limited to systems composed of spherical colloids. In most natural and technical systems, however, particles are nonspherical, and their structural dynamics are determined by translational and rotational degrees of freedom. Using confocal microscopy of fluorescently labeled core-shell particles, we reveal that suspensions of ellipsoidal colloids form an unexpected state of matter, a liquid glass in which rotations are frozen while translations remain fluid. Image analysis unveils hitherto unknown nematic precursors as characteristic structural elements of this state. The mutual obstruction of these ramified clusters prevents liquid crystalline order. Our results give insight into the interplay between local structures and phase transformations. This helps to guide applications such as self-assembly of colloidal superstructures and also gives evidence of the importance of shape on the glass transition in general.

2.
J Colloid Interface Sci ; 514: 694-703, 2018 Mar 15.
Article in English | MEDLINE | ID: mdl-29310099

ABSTRACT

HYPOTHESIS: Hetero-aggregation of inorganic colloids is influenced by numerous parameters, which dictate the suspension properties. When particles are different in size, the suspension can be either stable or unstable according to concentration of components, ionic strength, and pH. Experimentally, understanding the role of each parameter is sometimes difficult because parameters cannot easily be modified independently. Numerical simulations are thus very useful to discriminate between different effects. SIMULATIONS: Brownian dynamics simulations are used here to study the heteroaggregation of dilute suspensions composed of two populations of colloids with large size asymmetry. Special attention is paid to the effect of small-particle concentration, surface potentials, and ionic strength. FINDINGS: The simulation results show that hetero-aggregation can be tuned by modifying these different parameters, and that the resulting aggregate structures depend more on the surface properties of small particles than on those of large particles. The simulations shed light on a further parameter crucially influencing hetero-aggregation, i.e. the mobility of small particles when adsorbed on large ones. The present results rationalize numerous experimental observations reported in the literature and can be used as reference to explain future experimental observations.

3.
Soft Matter ; 13(21): 3909-3917, 2017 May 31.
Article in English | MEDLINE | ID: mdl-28488709

ABSTRACT

We employ the reverse non-equilibrium molecular dynamics method (RNEMD) of Müller-Plathe [Phys. Rev. E, 1999, 59, 4894] to calculate the shear viscosity of colloidal suspensions within the stochastic rotation dynamics-molecular dynamics (SRD-MD) simulation method. We examine the influence of different coupling schemes in SRD-MD on the colloidal volume fraction ϕc dependent viscosity from the dilute limit up to ϕc = 0.3. Our results demonstrate that the RNEMD method is a robust and reliable method for calculating rheological properties of colloidal suspensions. To obtain quantitatively accurate results beyond the dilute regime, the hydrodynamic interactions between the effective fluid particles in the SRD and the MD colloidal particles must be carefully considered in the coupling scheme. We benchmark the method by comparing with the hard sphere suspension case, and then calculate relative viscosities for colloids with mutually attractive interactions. We show that the viscosity displays a sharp increase at the onset of aggregation of the colloidal particles with increasing volume fraction and attraction.

4.
Phys Chem Chem Phys ; 18(4): 3073-9, 2016 Jan 28.
Article in English | MEDLINE | ID: mdl-26739745

ABSTRACT

The adsorption of colloidal particles from a suspension on a solid surface is of fundamental importance to many physical and biological systems. In this work, Brownian Dynamics simulations are performed to study the aggregation in a suspension of oppositely charged colloidal particles in the presence of an attractive wall. For sufficiently strong attractions, the wall alters the microstructure of the aggregates so that B2 (CsCl-type) structures are more likely obtained instead of B1 (NaCl-type) structures. The probability of forming either B1 or B2 crystallites depends also on the inverse interaction range κa. Suspensions with small κa are more likely to form B2 crystals than suspensions with larger κa, even if the energetic stability of the B2 phase decreases with decreasing κa. The mechanisms underlying this aggregation and crystallization behaviour are analyzed in detail.

5.
J Colloid Interface Sci ; 458: 241-6, 2015 Nov 15.
Article in English | MEDLINE | ID: mdl-26232284

ABSTRACT

The percolation behavior of alumina suspensions is studied by computer simulations. The percolation threshold ϕc is calculated, determining the key factors that affect its magnitude: the strength of colloid-colloid attraction and the presence of hydrodynamic interactions (HIs). To isolate the effects of HIs, we compare the results of Brownian Dynamics, which do not include hydrodynamics, with those of Stochastic Rotation Dynamics-Molecular Dynamics, which include hydrodynamics. Our results show that ϕc decreases with the increase of the attraction between the colloids. The inclusion of HIs always leads to more elongated structures during the aggregation process, producing a sizable decrease of ϕc when the colloid-colloid attraction is not too strong. On the other hand, the effects of HIs on ϕc tend to become negligible with increasing attraction strength. Our ϕc values are in good agreement with those estimated by the yield stress model by Flatt and Bowen.


Subject(s)
Aluminum Oxide/chemistry , Colloids/chemistry , Hydrodynamics , Molecular Dynamics Simulation , Rheology , Suspensions
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