PubMed Health⌕ Search

Biomedical subjects

Antonio M Puertas

Publications and source records attributed to Antonio M Puertas.

10 recordsLinked to original sources

Experimental phase diagram of symmetric binary colloidal mixtures with opposite charges.

The phase behavior of equimolar mixtures of oppositely charged colloidal systems with similar absolute charges is studied experimentally as a function of the salt concentration in the system and the colloid volume fraction. As the salt concentration increases, fluids of irreversible clusters, gels, liquid-gas coexistence, and finally, homogeneous fluids, are observed. Previous simulations of similar mixtures of Derjaguin-Landau-Verwey-Overbeek (DLVO) particles indeed showed the transition from homogeneous fluids to liquid-gas separation, but also predicted a reentrant fluid phase at low salt concentrations, which is not found in the experiments. Possibly, the fluid of clusters could be caused by a nonergodicity transition responsible for the gel phase in the reentrant fluid phase. Liquid-gas separation takes a delay time after the sample is prepared, whereas gels collapse from the beginning. The density of the liquid in coexistence with a vapor phase depends linearly on the overall colloid density of the system. The vapor, on the other hand, is comprised of equilibrium clusters, as expected from the simulations.

Colloids↗

Liquid-gas separation in colloidal electrolytes.

The liquid-gas transition of an electroneutral mixture of oppositely charged colloids, studied by Monte Carlo simulations, is found in the low-temperature-low-density region. The critical temperature shows a nonmonotonous behavior as a function of the interaction range, kappa(-1), with a maximum at kappasigma approximately 10, implying an island of coexistence in the kappa-rho plane. The system is arranged in such a way that each particle is surrounded by shells of particles with alternating charge. In contrast with the electrolyte primitive model, both neutral and charged clusters are obtained in the vapor phase.

Journal Article↗

Mode coupling and dynamical heterogeneity in colloidal gelation: a simulation study.

We present simulation results addressing the dynamics of a colloidal system with attractive interactions close to gelation. Our interaction also has a soft, long-range repulsive barrier that suppresses liquid-gas type phase separation at long wavelengths. The new results presented here lend further weight to an intriguing picture emerging from our previous simulation work on the same system. Whereas mode coupling theory (MCT) offers quantitatively good results for the decay of correlators, closer inspection of the dynamics reveals a bimodal population of fast and slow particles with a very long exchange time scale. This population split represents a particular form of dynamic heterogeneity (DH). Although DH is usually associated with activated hopping and/or facilitated dynamics in glasses, the form of DH observed here may be more collective in character and associated with static (i.e., structural) heterogeneity.

Journal Article↗

Colloidal aggregation induced by long range attractions.

The structure of colloidal clusters formed by long-range attractive interactions under diluted conditions is studied by means of Monte Carlo simulations. For a not-too-long attraction range, clusters show self-similar internal structure with lower density than that typical for diffusive aggregation. For long-range interactions, low kappa, nonfractal clusters are formed (dense at short scales but open at long ones). The dependence on the volume fraction shows that more-compact clusters are grown the higher the colloidal density for diffusive aggregation and attraction-driven aggregation in the fractal regime. The whole trend is explained in terms of the interpenetration among aggregates. In attraction-driven aggregations, the interpenetration of clusters competes with aggregation in the tips of the clusters, causing low-density clusters.

Journal Article↗

Dynamical heterogeneities close to a colloidal gel.

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 of two populations with different mobilities. Analyzing the statics and dynamics of both sets of particles, it is shown that the slow particles form a network of stuck particles, whereas the fast ones are able to move over long distances. Correlation functions show that the environment of the fast particles relaxes much faster than that of the slow ones, but at short times the bonds between fast particles are longer lived due to the flexibility of their structure. No stringlike motion is observed for the fast particles, but they occupy preferential sites in the surface of the structure formed by the slow ones.

Journal Article↗

Oppositely charged colloidal binary mixtures: a colloidal analog of the restricted primitive model.

The equilibrium phase diagram of a colloidal system composed of 1:1 mixture of positive and negative particles with equal charge is studied by means of Monte Carlo simulations. The system is the colloidal analog of the restricted primitive model (RPM) for ionic fluids. A liquid-gas transition is found in the low-temperature-low-density region, similar to the liquid-gas transition in the RPM. The fluid-crystal transition is also studied, and the liquid phase is shown to be stable in a narrow range of temperatures. In the liquid, the pair distribution function shows alternating layers of particles with opposite sign of charge surrounding every particle. In the vapor phase, clusters of particles are observed, again in agreement with the RPM. However, a decreasing distribution of clusters is obtained, instead of the discrimination between charged and neutral clusters found in the RPM.

Journal Article↗

Internal structure of clusters from charge heteroaggregation.

The internal structure of clusters formed by colloidal heteroaggregation of particles with opposite signs of charge is studied by means of computer simulations. Every particle is surrounded by a layer of particles of opposite sign, a second neighbors shell of particles mainly with the same sign, a third one of opposite sign, etc. As the distance from the particle increases, the system becomes more homogeneous and no difference between the numbers of particles with similar or opposite signs of charge can be noticed for distances larger than ten times the particle radius. For low ionic concentrations the local environment of particles is formed by quasi-straight branches, where the sign of charge alternates, and at high concentrations the structure of the cluster is typical of DLCA and the alternation is restricted to very short distances. However, this effect is not responsible for the low fractal dimensions observed in charge heteroaggregates.

Journal Article↗

Induced asymmetries in the heteroaggregation of oppositely charged colloidal particles.

Heterocoagulation of cationic and carboxylated polystyrene latexes is studied for a wide range of salt concentrations by static light scattering. The weak character of the surface groups providing the charges allows variation of the relative charge of the systems. Two situations are studied: both latexes with similar surface charges and with very different ones. In both cases at low ionic concentration pure heteroaggregation takes place, whereas diffusive aggregation is observed at high kappa, above the critical coagulation concentration (C.C.C.) of both latexes. The overall rate of aggregation describes a minimum at intermediate salt concentrations when both latexes bear similar charges. The heterocoagulation rate constant decreases continuously to reach the diffusive value at high salt. An interesting behavior is observed when the latexes have very different charge. The heterocoagulation kinetic constant becomes diffusive above the C.C.C. of the less charged latex.

Journal Article↗

Simulation study of nonergodicity transitions: gelation in colloidal systems with short-range attractions.

Computer simulations were used to study the gel transition occurring in colloidal systems with short-range attractions. A colloid-polymer mixture was modeled and the results were compared with mode coupling theory (MCT) expectations and with the results for other systems (hard-spheres system and Lennard-Jones system). The self-intermediate scattering function and the mean squared displacement were used as the main dynamical quantities. Two different colloid packing fractions have been studied. For the lower packing fraction, alpha-scaling holds and the wave-vector analysis of the correlation function shows that gelation is a regular nonergodicity transition within MCT. The leading mechanism for the novel nonergodicity transition is identified as the bond formation caused by the short-range attraction. The time scale and diffusion coefficient also show qualitatively the expected behavior, although different exponents are found for the power-law divergences of these two quantities. The non-Gaussian parameter was also studied and a very large correction to Gaussian behavior was found. The system with higher colloid packing fraction shows indications of a nearby high-order singularity, causing alpha scaling to fail, but the general expectations for nonergodicity transitions still hold.

Journal Article↗

Comparative simulation study of colloidal gels and glasses.

Using computer simulations, we identify the mechanisms causing aggregation and structural arrest of colloidal suspensions interacting with a short-ranged attraction at moderate and high densities. Two different nonergodicity transitions are observed. As the density is increased, a glass transition takes place, driven by excluded volume effects. In contrast, at moderate densities, gelation is approached as the strength of the attraction increases. At high density and interaction strength, both transitions merge, and a logarithmic decay in the correlation function is observed. All of these features are correctly predicted by mode coupling theory.

Journal Article↗