arXiv subjects

Antonio M. Puertas

Publications and source records attributed to Antonio M. Puertas.

At least 19 recordsLinked to original sources

arXiv2026

Using microrheology to study dynamical heterogeneities

Dynamical heterogeneities are one of the hallmarks of supercooled liquids, and their properties and relevance have been studied with theory, simulations and experiments. In this work, we propose to monitor the dynamics of tracer particles (passive microrheology) to analyze the dynamical heterogeneities in a system of hard colloids close to the glass transition density, using Langevin dynamics simulations and mode coupling theory. Different observables, typical in the study of the dynamical heterogeneities are adapted to be calculated from the trajectory of a single tracer particle. The tracer dynamics shows a transition from a regime where it is most decoupled from the bath for small tracer size to a strong coupling regime for large tracers. Both theory and simulations show that the non-Gaussian parameter of the tracer is maximal for tracer sizes at the crossover between both regimes, and is highly dependent on the bath density. The dynamic susceptibility is also studied, but this parameter shows a minor dependence on both the tracer size or the bath density. Finally, the existence of regions with different mobility is also studied with microrheology. Although the tracer trajectory indeed shows stages with increased mobility, the estimated size of the regions decreases with the bath density, contrary to the results from cluster analysis in the bulk.

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arXiv2026

Particle-scale structure of granular suspensions

Granular suspensions are intrinsically nonequilibrium systems in which dissipative grain-grain collisions coexist with solvent-induced forcing. We study the particle-scale structure of a granular suspension modeled by inelastic hard spheres immersed in a thermal bath and compare Langevin-dynamics simulation results for the radial distribution function $g(r)$ and the static structure factor $S(q)$ with predictions of an equilibrium-inspired rational function approximation (RFA). The equilibrium hard-sphere RFA is supplied with nonequilibrium input for the contact value and a reduced isothermal-compressibility-like quantity, yielding analytical expressions for $g(r)$ in Laplace space and for $S(q)$. We find that the RFA gives a very good description of the short- and intermediate-range structure of the suspension over a broad range of densities, drag coefficients, and inelasticities. It reproduces $g(r)$ substantially better than the Percus-Yevick approximation in inelastic states, especially near contact, and gives a good account of $S(q)$ except at the smallest wave numbers. There, simulations show a drag-dependent enhancement over the RFA prediction, indicating additional long-wavelength nonequilibrium correlations beyond the present equilibrium-like description. These results show that an equilibrium-based hard-sphere approach provides an accurate description of the particle-scale structure of the present Langevin model with inelastic hard spheres (except in the smallest-$q$ region), and suggest that similar equilibrium-inspired approaches may also be useful for related nonequilibrium hard-sphere suspension models, including multicomponent systems.

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arXiv2026

Tracer Diffusion in Granular Suspensions: Testing the Enskog Kinetic Theory with DSMC and Molecular Dynamics

We investigate the diffusion of an intruder in a granular gas, with both components modeled as smooth hard spheres, both immersed in a low viscosity carrier fluid to form a particle-laden suspension. In this system, dissipative particle collisions coexist with the action of a solvent. The latter is modeled via a viscous drag force and a stochastic Langevin-like force proportional to the background fluid temperature. Building on previous kinetic theory and random-walk results of the tracer diffusion coefficient [R. Gómez González, E. Abad, S. Bravo Yuste, and V. Garzó, Phys. Rev. E \textbf{108}, 024903 (2023)], where random-walk predictions were compared with Chapman--Enskog results up to the second Sonine approximation, we assess the robustness of the Enskog framework by incorporating molecular dynamics (MD) simulations, using direct simulation Monte Carlo (DSMC) results as an intermediate reference. In particular, we focus on the intruder velocity autocorrelation function, considering intruders different masses (from 0.01 to 100 times the mass of the granular particles), and analyse the behavior of the intruder temperature and diffusion coefficient. Our results clarify the influence of the friction parameter and the conditions under which Enskog kinetic theory reliably describes intruder diffusion in granular suspensions.

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arXiv2024

Nonlinear microrheology with time-dependent forces -- Application to recoils in viscoelastic fluids

This work presents a theoretical analysis of the motion of a tracer colloid driven by a time-dependent force through a viscoelastic fluid. The recoil of the colloid after application of a strong force is determined. It provides insights into the elastic forces stored locally in the fluid and their weakening by plastic processes. We generalize the mode coupling theory of microrheology to include time-dependent forces. After deriving the equations of motion for the tracer correlator and simplifying to a schematic model we apply the theory to a switch-off force protocol that features the recoiling of the tracer after cessation of the driving. We also include Langevin dynamics simulations to compare to the results of the theory. A non-monotonic trend of the recoil amplitude is found in the theory and confirmed in the simulations. The linear-response approximation is also verified in the small-force regime. While the overall agreement between simulation and theory is good, simulation shows that the theory predicts a too strong non-monotonous dependence of the recoil distance on the applied force.

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arXiv2023

Active and passive microrheology with large tracers in hard colloids

The dynamics of a tracer particle in a bath of quasi-hard colloidal spheres is studied by Langevin dynamics simulations and mode coupling theory (MCT); the tracer radius is varied from equal to up to 7 times larger than the bath particles radius. In the simulations, two cases are considered: freely diffusing tracer (passive microrheology) and tracer pulled with a constant force (active microrheology). Both cases are connected by linear response theory for all tracer sizes. It links both the stationary and transient regimes of the pulled tracer (for low forces) with the equilibrium correlation functions; the velocity of the pulled tracer and its displacement are obtained from the velocity auto-correlation function and the mean squared displacement, respectively. The MCT calculations give insight into the physical mechanisms: At short times, the tracer rattles in its cage of neighbours, with the frequency increasing linearly with the tracer radius asymptotically. The long-time tracer diffusion coefficient from passive microrheology, which agrees with the inverse friction coefficient from the active case, arises from the transport of transverse momentum around the tracer. It can be described with the Brinkman equation for the transverse flow field obtained in extension of MCT, but cannot be recovered from the MCT kernel coupling to densities only. The dynamics of the bath particles is also studied; for the unforced tracer the dynamics is unaffected, irrespective of the distance from the tracer. When the tracer is pulled, the velocity field in the bath decays with the distance from the tracer as 1/r3, as predicted by the Brinkman model, but different from the case of a Newtonian fluid.

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arXiv2021

Time-dependent active microrheology in dilute colloidal suspensions

In a microrheological set-up a single probe particle immersed in a complex fluid is exposed to a strong external force driving the system out of equilibrium. Here, we elaborate analytically the time-dependent response of a probe particle in a dilute suspension of Brownian particles to a large step-force, exact in first order of the density of the bath particles. The time-dependent drift velocity approaches its stationary state value exponentially fast for arbitrarily small driving in striking contrast to the power-law prediction of linear response encoded in the long-time tails of the velocity autocorrelation function. We show that the stationary-state behavior depends nonanalytically on the driving force and connect this behavior to the persistent correlations in the equilibrium state. We argue that this relation holds generically. Furthermore, we elaborate that the fluctuations in the direction of the force display transient superdiffusive behavior.

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arXiv2021

Microrheology of colloidal suspensions via Dynamic Monte Carlo simulations

Understanding the rheology of colloidal suspensions is crucial in the formulation of a wide selection of industry-relevant products. To characterise the viscoelastic behaviour of these soft materials, one can analyse the microscopic dynamics of colloidal tracers diffusing through the host fluid and generating local deformations and stresses. This technique, referred to as microrheology, links the bulk rheology of fluids to the microscopic dynamics at the particle scale. If tracers are subjected to external forces, rather than freely diffusing, it is called active microrheology. Motivated by the impact of microrheology in providing information on local structure in complex systems such as colloidal glasses, active matter or biological systems, we have extended the dynamic Monte Carlo (DMC) technique to investigate active microrheology in colloids. The original DMC framework, able to accurately describe the Brownian dynamics of colloids at equilibrium, is here reconsidered and expanded to describe the effects of an external force pulling a tracer embedded in isotropic colloidal suspensions at different densities. To this end, we studied the dynamics of a spherical tracer dragged by a constant external force through a bath of spherical and rod-like particles of comparable size. We could extract valuable details on its effective friction coefficient, being constant at small and large values of the external force, but otherwise displaying a nonlinear behaviour that indicates the occurrence of a force-thinning regime. Our DMC simulation results are in excellent quantitative agreement with past Langevin dynamics simulations and theoretical works for the bath of spherical colloids. The bath of rod-like particles is studied in the isotropic phase, and displays an example where DMC is more convenient than Brownian or Langevin dynamics, in this case in dealing with particle rotation.

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arXiv2020

Dynamics and friction of a large colloidal particle in a bath of hard spheres: Langevin dynamics simulations and hydrodynamic description

The analysis of the dynamics of tracer particles in a complex bath can provide valuable information about the microscopic behaviour of the bath. In this work, we study the dynamics of a forced tracer in a colloidal bath by means of Langevin dynamics simulations and a theory model within continuum mechanics. In the simulations, the bath is comprised by quasi-hard spheres with a volume fraction of 50% immersed in a featureless quiescent solvent, and the tracer is pulled with a constant small force (within the linear regime). The theoretical analysis is based on the Navier Stokes equation, where a term proportional to the velocity arises from coarse-graining the friction of the colloidal particles with the solvent. As a result, the final equation is similar to the Brinkman model, although the interpretation is different. A length scale appears in the model, 1/k_0, where the transverse momentum transport crosses over to friction with the solvent. The effective friction coefficient experienced by the tracer grows with the tracer size faster than the prediction from Stokes law. Additionally, the velocity profiles in the bath decay faster than in a Newtonian fluid. The comparison between simulations and theory points to a boundary condition of effective partial slip at the tracer surface. We also study the fluctuations in the tracer position, showing that it reaches diffusion at long times, with a subdiffusive regime at intermediate times. The diffusion coefficient, obtained from the long-time slope of the mean squared displacement, fulfills the Stokes-Einstein relation with the friction coefficient calculated from the steady tracer velocity, confirming the validity of the linear response formalism.

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arXiv2018

Active microrheology in corrugated channels

We analyze the dynamics of a tracer particle embedded in a bath of hard spheres confined in a channel of varying section. By means of Brownian dynamics simulations we apply a constant force on the tracer particle and discuss the dependence of its mobility on the relative magnitude of the external force with respect to the entropic force induced by the confinement. A simple theoretical one-dimensional model is also derived, where the contribution from particle-particle and particle-wall interactions is taken from simulations with no external force. Our results show that the mobility of the tracer is strongly affected by the confinement. The tracer velocity in the force direction has a maximum close to the neck of the channel, in agreement with the theory for small forces. Upon increasing the external force, the tracer is effectively confined to the central part of the channel and the velocity modulation decreases, what cannot be reproduced by the theory. This deviation marks the regime of validity of linear response. Surprisingly, when the channel section is not constant the effective friction coefficient is reduced as compared to the case of a plane channel. The transversal velocity, which cannot be studied with our model, follows the qualitatively the derivative of the channel section, in agreement previous theoretical calculations for the tracer diffusivity in equilibrium.

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arXiv2017

Diffusive and arrested-like dynamics in currency exchange markets

This work studies the symmetry between colloidal dynamics and the dynamics of the Euro--US Dollar currency exchange market (EURUSD). We consider the EURUSD price in the time range between 2001 and 2015, where we find significant qualitative symmetry between fluctuation distributions from this market and the ones belonging to colloidal particles in supercooled or arrested states. In particular, we find that models used for arrested physical systems are suitable for describing the EURUSD fluctuation distributions. Whereas the corresponding mean squared price displacement (MSPD) to the EURUSD is diffusive for all years, when focusing in selected time frames within a day, we find a two-step MSPD when the New York Stock Exchange market closes, comparable to the dynamics in supercooled systems. This is corroborated by looking at the price correlation functions and non-Gaussian parameters, and can be described by the theoretical model. We discuss the origin and implications of this analogy.

q-fin.ST↗

arXiv2014

Specific heat in two-dimensional melting

We report the specific heat $c_N$ around the melting transition(s) of micrometer-sized superparamagnetic particles confined in two dimensions, calculated from fluctuations of positions and internal energy, and corresponding Monte Carlo simulations. Since colloidal systems provide single particle resolution, they offer the unique possibility to compare the experimental temperatures of peak position of $c_N(T)$ and symmetry breaking, respectively. While order parameter correlation functions confirm the Kosterlitz-Thouless-Halperin-Nelson-Young melting scenario where translational and orientational order symmetries are broken at different temperatures with an intermediate so called hexatic phase, we observe a single peak of the specific heat within the hexatic phase, with excellent agreement between experiment and simulation. Thus, the peak is not associated with broken symmetries but can be explained with the total defect density, which correlates with the maximum increase of isolated dislocations. The absence of a latent heat strongly supports the continuous character of both transitions.

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arXiv2013

Influence of ripening and creaming on the aggregation rate of dodecane-in-water nanoemulsions. Is the creaming rate an appropriate measure of emulsion stability?

The behavior of four oil-in-water (O/W) ioinic nanoemulsions composed of dodecane, and mixtures of dodecane with squalene and tetra-chloro-ethylene is studied. These nanoemulsions were stabilized with sodium dodecyl sulfate (SDS). The behavior of the turbidity and the average radius of the emulsions were followed as a function of time. The results illustrate the shortcomings of characterizing the stability of emulsions by their creaming rate.

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arXiv2012

Probability densities of a forced probe particle in glass: results from mode coupling theory and simulations of active microrheology

We investigate the displacements of a probe particle inside a glass, when a strong external force is applied to the probe (active nonlinear microrheology). Calculations within mode coupling theory are presented for glasses of hard spheres and compared to Langevin and Brownian dynamics simulations. Under not too strong forces where the probe remains trapped, the probe density distribution becomes anisotropic. It is shifted towards the direction of the force, develops an enhanced tail in that direction (signalled by a positive skewness), and exhibits different variances along and perpendicular to the force direction. A simple model of an harmonically trapped probe rationalizes the low force limit, with strong strain softening setting in at forces of the order of a few thermal energies per particle radius.

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arXiv2012

Nanoemulsion stability: experimental evaluation of the flocculation rate from turbidity measurements

The coalescence of liquid drops induces a higher level of complexity compared to the classical studies about the aggregation of solid spheres. Yet, it is commonly believed that most findings on solid dispersions are directly applicable to liquid mixtures. Here, the state of the art in the evaluation of the flocculation rate of these two systems is reviewed. Special emphasis is made on the differences between suspensions and emulsions. In the case of suspensions, the stability ratio is commonly evaluated from the initial slope of the absorbance as a function of time under diffusive and reactive conditions. Puertas and de las Nieves (1997) developed a theoretical approach that allows the determination of the flocculation rate from the variation of the turbidity of a sample as a function of time. Here, suitable modifications of the experimental procedure and the referred theoretical approach are implemented in order to calculate the values of the stability ratio and the flocculation rate corresponding to a dodecane-in-water nanoemulsion stabilized with sodium dodecyl sulfate. Four analytical expressions of the turbidity are tested, basically differing in the optical cross section of the aggregates formed. The first two models consider the processes of: a) aggregation (as described by Smoluchowski) and b) the instantaneous coalescence upon flocculation. The other two models account for the simultaneous occurrence of flocculation and coalescence. The latter reproduce the temporal variation of the turbidity in all cases studied (380 \leq [NaCl] \leq 600 mM), providing a method of appraisal of the flocculation rate in nanoemulsions.

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arXiv2010

Schematic Models for Active Nonlinear Microrheology

We analyze the nonlinear active microrheology of dense colloidal suspensions using a schematic model of mode-coupling theory. The model describes the strongly nonlinear behavior of the microscopic friction coefficient as a function of applied external force in terms of a delocalization transition. To probe this regime, we have performed Brownian dynamics simulations of a system of quasi-hard spheres. We also analyze experimental data on hard-sphere-like colloidal suspensions [Habdas et al., Europhys. Lett., 2004, 67, 477]. The behavior at very large forces is addressed specifically.

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arXiv2009

Comparison of structure and transport properties of concentrated hard and soft sphere fluids

Using Newtonian and Brownian dynamics simulations, the structural and transport properties of hard and soft spheres have been studied. The soft spheres were modeled using inverse power potentials ($V\sim r^{-n}$, with $1/n$ the potential softness). Although the pressure, diffusion coefficient and viscosity depend at constant density on the particle softness up to extremely high values of $n$, we show that scaling the density with the freezing point for every system effectively collapses these parameters for $n\geq 18$ (including hard spheres), for large densities. At the freezing points, the long range structure of all systems is identical, when the distance is measured in units of the interparticle distance, but differences appear at short distances (due to the different shape of the interaction potential). This translates into differences at short times in the velocity and stress autocorrelation functions, although they concur to give the same value of the corresponding transport coefficient (for the same density to freezing ratio); the microscopic dynamics also affects the short time behaviour of the correlation functions and absolute values of the transport coefficients, but the same scaling with the freezing density works for Newtonian or Brownian dynamics. For hard spheres, the short time behaviour of the stress autocorrelation function has been studied in detail, confirming quantitatively the theoretical forms derived for it.

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arXiv2008

Glasses in Colloidal Systems. Attractive Interactions and Gelation

In this chapter, a study of the glass transitions in colloidal systems is presented, in connection with gelation, mainly from theoretical and simulation results. Mode Coupling Theory, which anticipated the existence of attraction driven glasses, is reviewed, and its predictions concerning attractive glasses discussed. Results from computer simulations will be presented for different models and the predictions of the theory will be tested. Starting from high density, where reasonable agreement is found, the study will be extended to low density, where new modes for the decay of density correlation functions appear. In all cases, the results will be also be brought into connection with experiments, and we will conclude with a discussion of the present understanding of the mechanisms leading to gelation.

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arXiv2007

Viscoelasticity and Stokes-Einstein relation in repulsive and attractive colloidal glasses

We report a numerical investigation of the visco-elastic behavior in models for steric repulsive and short-range attractive colloidal suspensions, along different paths in the attraction-strength vs packing fraction plane. More specifically, we study the behavior of the viscosity (and its frequency dependence) on approaching the repulsive glass, the attractive glass and in the re-entrant region where viscosity shows a non monotonic behavior on increasing attraction strength. On approaching the glass lines, the increase of the viscosity is consistent with a power-law divergence with the same exponent and critical packing fraction previously obtained for the divergence of the density fluctuations. Based on mode-coupling calculations, we associate the increase of the viscosity with specific contributions from different length scales. We also show that the results are independent on the microscopic dynamics by comparing newtonian and brownian simulations for the same model. Finally we evaluate the Stokes-Einstein relation approaching both glass transitions, finding a clear breakdown which is particularly strong for the case of the attractive glass.

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