PubMed Health⌕ Search

Biomedical subjects

Angel J Moreno

Publications and source records attributed to Angel J Moreno.

7 recordsLinked to original sources

Relaxation scenarios in a mixture of large and small spheres: dependence on the size disparity.

We present a computational investigation on the slow dynamics of a mixture of large and small soft spheres. By varying the size disparity at a moderate fixed composition different relaxation scenarios are observed for the small particles. For small disparity density-density correlators exhibit moderate stretching. Only small quantitative differences are observed between dynamic features for large and small particles. On the contrary, large disparity induces a clear time scale separation between the large and small particles. Density-density correlators for the small particles become extremely stretched and display logarithmic relaxation by properly tuning the temperature or the wave vector. Self-correlators decay much faster than density-density correlators. For very large size disparity, a complete separation between self- and collective dynamics is observed for the small particles. Self-correlators decay to zero at temperatures where density-density correlations are frozen. The dynamic picture obtained by varying the size disparity resembles features associated with mode coupling transition lines of the types B and A at, respectively, small and very large size disparities. Both lines might merge, at some intermediate disparity, at a higher-order point, to which logarithmic relaxation would be associated. This picture resembles predictions of a recent mode coupling theory for fluids confined in matrices with interconnected voids [V. Krakoviack, Phys. Rev. Lett. 94, 065703 (2005)].

Journal Article↗

Anomalous dynamic arrest in a mixture of large and small particles.

We present molecular dynamics simulations of the slow dynamics of a mixture of large and small soft spheres with a large size disparity. The dynamics are investigated in a broad range of temperature and mixture composition. As a consequence of the large size disparity, large and small particles exhibit very different relaxation times. As previously reported for simple models of short-ranged attractive colloids and polymer blends, several anomalous dynamic features are observed: (i) sublinear behavior for mean-squared displacements, (ii) concave-to-convex crossover for density-density correlators, by varying the temperature or wave vector, and (iii) logarithmic decay for specific wave vectors of density-density correlators. These anomalous features are observed over time intervals extending up to four decades and strongly resemble predictions of the mode coupling theory (MCT) for state points close to higher-order MCT transitions, which originate from the competition between different mechanisms for dynamic arrest. For the large particles we suggest competition between soft-sphere repulsion and depletion effects induced by neighboring small particles. For the small particles we suggest competition between bulklike dynamics and confinement, respectively induced by neighboring small particles and by the slow matrix of large particles.

Journal Article↗

Logarithmic relaxation in a kinetically constrained model.

We present Monte Carlo simulations on a coarse-grained model for relaxation in binary mixtures. The liquid structure is substituted by a three-dimensional array of cells. A spin variable is assigned to each cell, with values 0 or 1 denoting, respectively, unexcited and excited local states in a mobility field. Change in local mobility (spin flip) is permitted according to kinetic constraints determined by the mobilities of neighboring cells. We introduce two types of cells ("fast" and "slow") with very different rates for spin flip. Fast cells display anomalous relaxation, characterized by a concave-to-convex crossover in dynamic correlators by changing temperature or composition. At intermediate state points logarithmic relaxation is observed over three time decades. These results display striking analogies with dynamic correlators reported in recent simulations on polymer blends.

Journal Article↗

Is there a higher-order mode coupling transition in polymer blends?

We present simulations on a binary blend of bead-spring polymer chains. The introduction of monomer size disparity yields very different relaxation times for each component of the blend. Competition between two different arrest mechanisms, namely, bulklike dynamics and confinement, leads to an anomalous relaxation scenario for the fast component, characterized by sublinear time dependence for mean squared displacements, or logarithmic decay and convex-to-concave crossover for density-density correlators. These anomalous dynamic features, which are observed over time intervals extending up to 4 decades, strongly resemble predictions of mode coupling theory for nearby higher-order transitions. Chain connectivity extends anomalous relaxation over a wide range of blend compositions.

Journal Article↗

Dynamic arrest in a liquid of symmetric dumbbells: reorientational hopping for small molecular elongations.

We present extensive equilibrium and out-of-equilibrium molecular-dynamics simulations of a liquid of symmetric dumbbell molecules, for constant packing fraction, as a function of temperature and molecular elongation. We compute diffusion constants as well as odd and even orientational correlators. The notations odd and even refer to the parity of the order l of the corresponding Legendre l polynomial, evaluated for the orientation of the molecular axis relative to its initial position. Rotational degrees of freedom of order l are arrested if, in the long-time limit, the corresponding orientational l correlator does not decay to zero. It is found that for large elongations translational and rotational degrees of freedom freeze at the same temperature. For small elongations only the even rotational degrees of freedom remain coupled to translational motions and arrest at a finite common temperature. On the contrary, the odd rotational degrees of freedom remain ergodic at all investigated temperatures. Hence, in the translationally arrested state, each molecule remains trapped in the cage formed by its neighboring molecules, but is able to perform 180 degrees rotations, which lead to relaxation only for the odd orientational correlators. The temperature dependence of the characteristic time of these residual rotations is well described by an Arrhenius law. Finally, we discuss the evidence in favor of the presence of the type-A transition for the odd rotational degrees of freedom, as predicted by mode-coupling theory for small molecular elongations. This transition is distinct from the type-B transition, associated with the arrest of the translational and even rotational degrees of freedom for small elongations, and with all degrees of freedom for large elongations. Odd orientational correlators are computed for small elongations at very low temperatures in the translationally arrested state. The obtained results suggest that hopping events restore the ergodicity of the odd rotational degrees of freedom at temperatures far below the A transition.

Journal Article↗

Evidence for the weak steric hindrance scenario in the supercooled-state reorientational dynamics.

We use molecular-dynamics computer simulations to study the translational and reorientational dynamics of a glass-forming liquid of dumbbells. For sufficiently elongated molecules the standard strong steric hindrance scenario for the rotational dynamics is found. However, for small elongations we find a different scenario--the weak steric hindrance scenario--caused by a new type of glass transition in which the orientational dynamics of the molecule's axis undergoes a dynamical transition with a continuous increase of the nonergodicity parameter. These results are in agreement with the theoretical predictions by the mode-coupling theory for the glass transition.

Journal Article↗

Relaxation dynamics of a linear molecule in a random static medium: a scaling analysis.

We present extensive molecular dynamics simulations of the motion of a single linear rigid molecule in a two-dimensional random array of fixed overlapping disklike obstacles. The diffusion constants for the center of mass translation, D(CM), and for rotation, D(R), are calculated for a wide range of the molecular length, L, and the density of obstacles, rho. The obtained results follow a master curve Drho(micro) approximately (L(2)rho)(-nu) with an exponent micro=-3/4 and 1/4 for D(R) and D(CM), respectively, that can be deduced from simple scaling and kinematic arguments. The nontrivial positive exponent nu shows an abrupt crossover at L(2)rho=zeta(1). For D(CM) we find a second crossover at L(2)rho=zeta(2). The values of zeta(1) and zeta(2) correspond to the average minor and major axis of the elliptic holes that characterize the random configuration of the obstacles. A violation of the Stokes-Einstein-Debye relation is observed for L(2)rho>zeta(1), in analogy with the phenomenon of enhanced translational diffusion observed in supercooled liquids close to the glass transition temperature.

Journal Article↗