arXiv subjects

A. Gama Goicochea

Publications and source records attributed to A. Gama Goicochea.

At least 19 recordsLinked to original sources

arXiv2023

Self-Diffusion and Structure of a Quasi Two-Dimensional, Classical Coulomb Gas Under Increasing Magnetic Field and Temperature

The influence of a magnetic field applied perpendicularly to the plane of a quasi two dimensional, low density classical Coulomb gas, with interparticle potential U of r as 1 over r, is studied using momentum conserving dissipative particle dynamics simulations. The self diffusion and structure of the gas are studied as functions of temperature and strength of the magnetic field. It is found that the gas undergoes a topological phase transition when the temperature is varied, in accord with the Bohr van Leeuwen BvL theorem, the structural properties being unaffected, resembling those of the strictly two dimensional Kosterlitz Thouless transition, with U of r as varying as ln r. Consistent with the BvL theorem, the transition temperature and the melting process of the condensed phase are unchanged by the field. Conversely, the self diffusion coefficient of the gas is strongly reduced by the magnetic field. At the largest values of the cyclotron frequency, the self diffusion coefficient is inversely proportional to the applied magnetic field. The implications of these results are discussed.

cond-mat.mes-hall↗

arXiv2023

Topological Phase Transition in a Quasi Two Dimensional Coulomb Gas

A system with equal number of positive and negative charges confined in a box with a small but finite thickness is modeled as a function of temperature using mesoscale numerical simulations, for various values of the charges. The Coulomb interaction is used in its three-dimensional form, U(r) ~ 1/r. A topological phase transition is found in this quasi 2d system. The translational order parameter, spatial correlation function, specific heat, and electric current show qualitatively different trends below and above a critical temperature. We find that a 2d logarithmic Coulomb interaction is not essential for the appearance of this transition. This work suggests new experimental tests of our predictions, as well as novel theoretical approaches to probe quasi 2d topological phase transitions.

cond-mat.soft↗

arXiv2021

Self assembly of model surfactants as reverse micelles in nonpolar solvents and their role as interfacial tension modifiers

The self assembly of linear surfactants into reverse micelles (RMs) in nonpolar solvents and their efficiency in reducing the interfacial tension is studied using dissipative particle dynamics simulations. Given the importance of RMs as thickeners, among many other applications, their properties are studied here when formed in oil and in supercritical carbon dioxide (scCO2). Our simulations are found to be in agreement with experimental results of surfactant self assembly in scCO2 that found viscosity increments of up to 90 percent with 10 wt percent of surfactants. The role played by a small number of water molecules in RM formation is studied as well in both solvents, corroborating experiments reporting the enhancement of RM formation with the addition of a small quantity of water. The dynamics of water surfactant aggregation in nonpolar solvents is also discussed. Lastly, the performance of the model surfactant as an interfacial tension modifier is studied in detail. The results show that RMs are more easily formed in oil than in scCO2 and that the effectiveness of the surfactant in reducing the interfacial tension lies in its preference to adsorb at interfaces rather than self association.

cond-mat.soft↗

arXiv2021

Modeling of Branched Thickening Polymers under Poiseuille Flow Gives Clues as to how to Increase a Solvent Viscosity

The viscosity enhancement of a solvent produced by the addition of thickening branched polymers is predicted as a function of polymer concentration, branch length and persistence length, and strength of the covalent bonding interactions. Non equilibrium, stationary state Poiseuille numerical simulations are performed using the dissipative particle dynamics model to obtain the viscosity of the fluid. It is found that the clustering of the polymers into aggregates raises the viscosity and that it is more strongly affected by the strength of the bonding interactions. General scaling relationships are found for the viscosity as a function of the variables studied, which are expected to be useful for the design and synthesis of new viscosifying polymers. It is argued that our results can be applied to aqueous thickeners, of importance for colloidal fluids such as paints and coatings, and also for nonpolar fluids such as supercritical CO2, which is a promising non hydraulic fracking fluid also useful in enhanced oil recovery.

cond-mat.soft↗

arXiv2018

Fractal Properties of Biophysical Models of Pericellular Brushes Can Be Used to Differentiate Between Cancerous and Normal Cervical Epithelial Cells

Fractal behavior is found on the topographies of pericellular brushes on the surfaces of model healthy and cancerous cells, using dissipative particle dynamics models and simulations. The influence of brush composition, chain stiffness and solvent quality on the fractal dimension is studied in detail. Since fractal dimension alone cannot guarantee that the brushes possess fractal properties, their lacunarity was obtained also, which is a measure of the space filling capability of fractal objects. Soft polydisperse brushes are found to have larger fractal dimension than soft monodisperse ones, under poor solvent conditions, in agreement with recent experiments on dried cancerous and healthy human cervical epithelial cells. Additionally, we find that image resolution is critical for the accurate assessment of differences between images from different cells. The images of the brushes on healthy model cells are found to be more textured than those of brushes on model cancerous cells, as indicated by the larger lacunarity of the former. These findings are helpful to distinguish monofractal behavior from multifractality, which has been found to be useful to discriminate between immortal, cancerous and normal cells in recent experiments.

cond-mat.soft↗

arXiv2017

Surfactant chain length and concentration influence on the interfacial tension of two immiscible model liquids a coarse grained approach

The interfacial tension between immiscible liquids is studied as a function of a model linear surfactant length and concentration using coarse grained, dissipative particle dynamics numerical simulations. The adsorption isotherms obtained from the simulations are found to be in agreement with Langmuir model. The reduction of the interfacial tension with increasing surfactant concentration is found to display some common characteristics for all the values of chain length modeled, with our predictions being in agreement with Szyszkowski equation. Lastly, the critical micelle concentration is predicted for all surfactant lengths, finding exponentially decaying behavior, in agreement with Kleven model. It is argued that these findings can be helpful guiding tools in the interpretation of available experiments and in the design of new ones with new surfactants and polymers.

cond-mat.soft↗

arXiv2016

Scaling features of the tribology of polymer brushes of increasing grafting density around the mushroom to brush transition

Non equilibrium coarse grained, dissipative particle dynamics simulations of complex fluids, made up of polymer brushes tethered to planar surfaces immersed in a solvent yield non monotonic behavior of the friction coefficient as a function of the polymer grating density on the substrates, Γ, while the viscosity shows a monotonically increasing dependence on Γ. This effect is shown to be independent of the degree of polymerization, N, and the size of the system. It arises from the composition and the structure of the first particle layer adjacent to each surface that results from the confinement of the fluid. Whenever such layers are made up of as close a proportion of polymer beads to solvent particles as there are in the fluid, the friction coefficient shows a minimum, while for disparate proportions the friction coefficient grows. At the mushroom to brush transition (MBT) the viscosity scales with an exponent that depends on the characteristic exponent of the MBT (6/5) and the solvent quality exponent (ν= 0.5, for theta solvent), but it is independent of the polymerization degree (N). On the other hand, the friction coefficient at the MBT scales as μ~N^(6/5), while the grafting density at the MBT scales as Γ~ N^(-6/5) when friction is minimal, in agreement with previous scaling theories. We argue these aspects are the result of cooperative phenomena that have important implications for the understanding of biological brushes and the design of microfluidics devices, among other applications of current academic and industrial interest.

cond-mat.soft↗

arXiv2016

Ab Initio Modeling Of Friction Reducing Agents Shows Quantum Mechanical Interactions Can Have Macroscopic Manifestation

Two of the most commonly encountered friction reducing agents used in plastic sheet production are the amides known as erucamide and behenamide, which despite being almost identical chemically, lead to markedly different values of the friction coefficient. To understand the origin of this contrasting behavior, in this work we model brushes made of these two types of linear chain molecules using quantum mechanical numerical simulations under the Density Functional Theory at the B97D/6-31G(d,p)level of theory. Four chains of erucamide and behenamide were linked to a 2X10 zigzag graphene sheet and optimized both in vacuum and in continuous solvent using the SMD implicit solvation model. We find that erucamide chains tend to remain closer together through ππ stacking interactions arising from the double bonds located at C13 C14, a feature behenamide lacks and thus a more spread configuration is obtained with the latter. It is argued that this arrangement of the erucamide chains is responsible for the lower friction coefficient of erucamide brushes, compared with behenamide brushes, which is a macroscopic consequence of cooperative quantum mechanical interactions. While only quantum level interactions are modeled here, we show that behenamide chains are more spread out in the brush than erucamide chains as a consequence of those interactions. The spread out configuration allows more solvent particles to penetrate the brush, leading in turn to more friction, in agreement with macroscopic measurements and mesoscale simulations of the friction coefficient reported in the literature.

cond-mat.soft↗

arXiv2016

Electrostatics in dissipative particle dynamics using Ewald sums with point charges

A proper treatment of electrostatic interactions is crucial for the accurate calculation of forces in computer simulations. Electrostatic interactions are typically modeled using Ewald based methods, which have become one of the cornerstones upon which many other methods for the numerical computation of electrostatic interactions are based. However, their use with charge distributions rather than point charges requires the inclusion of ansatz for the solutions of the Poisson equation, since there is no exact solution known for smeared out charges. The interest for incorporating electrostatic interactions at the scales of length and time that are relevant for the study the physics of soft condensed matter has increased considerably. Using mesoscale simulation techniques, such as dissipative particle dynamics (DPD), allows us to reach longer time scales in numerical simulations, without abandoning the particulate description of the problem. The main problem with incorporating electrostatics into DPD simulations is that DPD particles are soft and those particles with opposite charge can form artificial clusters of ions. Here we show that one can incorporate the electrostatic interactions through Ewald sums with point charges in DPD if larger values of coarse graining degree are used, where DPD is truly mesoscopic. Using point charges with larger excluded volume interactions the artificial formation of ionic pairs with point charges can be avoided, and one obtains correct predictions. We establish ranges of parameters useful for detecting boundaries where artificial formation of ionic pairs occurs. Lastly, using point charges we predict the scaling properties of polyelectrolytes in solvents of varying quality and obtain predictions that are in agreement with calculations that use other methods, and with recent experimental results.

cond-mat.soft↗

arXiv2016

Adsorption of polyelectrolytes on silica and gold surfaces

The results of a study that helps understand the mechanisms of adsorption of polyelectrolytes on particles, using numerical simulation methods, specifically the one known as dissipative particle dynamics are reported here. The adsorption of cationic polyelectrolytes of two different polymerization degrees interacting with two types of surfaces, one made of gold and the other of silica is predicted and compared. We find that a more negatively charged wall does not necessarily adsorb more cationic polyelectrolytes because the electrostatic repulsion between the wall and the polyelectrolytes is stronger. Additionally, intra chain repulsion plays an important role, because the largest polyelectrolyte chains have larger excluded volume than the shorter ones. In regard to the adsorption dependence on the polyelectrolyte polymerization degree we find that the excluded volume drives the adsorption throughout the intrachain electrostatic repulsion, because the SiO2 surface is strongly negative. These results are expected to be useful for several nanotechnological applications of current interest, such as in gene therapy and in the improvement of drug delivering mechanisms.

cond-mat.soft↗

arXiv2016

Friction coefficient and viscosity of polymer brushes with and without free polymers as slip agents

There is ample evidence that polymer brushes reduce friction between surfaces. Several industrial applications take advantage of this fact, such as those in plastic bag production, where the brushes act as slip agents; however, the complex mechanisms that give rise to such reduction of friction are not yet fully understood. In this work we report coarse grained, dissipative particle dynamics simulations carried out for surfaces functionalized with erukamide brushes, a polymer commonly used in the plastics industry as a slip agent between surfaces. We calculate their rheological properties, such as the coefficient of friction (COF) and the viscosity, η, as functions of the number of chains grafted on the surfaces under the influence of stationary, Couette flow. Moreover, we consider also the case when a fraction of the erukamide chains is not adsorbed and moves freely between the surfaces. We show that the COF reaches an equilibrium value of about 0.29 in these two cases, in agreement with experimental results. On other hand, the viscosity grows monotonically, as a result of the increasing collisions when the erukamide content is increased. The force between brushes is found to be in agreement with predictions from scaling theories. We find that the addition to free chains helps stabilize the film formed by the brushes and the solvent, as others have found experimentally. The mechanisms that give rise to these phenomena are studied in detail.

cond-mat.soft↗

arXiv2015

A new effective potential for colloidal dispersions with polymer chains emerging from mesoscopic scale interactions

A new potential of mean force is proposed for colloidal dispersions, which is obtained from coarse grained, pair interactions between colloidal particles formed by the explicit grouping of particles that are themselves groups of atoms and molecules. Using numerical simulations, we start by constructing colloidal particles made up of 250 mesoscopic particles joined by springs and interacting with each other through short range forces. Afterward we proceed to model several colloidal concentrations and obtain the colloidal particles pair correlation function, from which we derive the potential of mean force. In our second case study, we add linear polymer chains of the same length that attach by one of their ends to the colloids, at a fixed colloidal concentration, and carry out numerical simulations at increasing concentrations of polymer chains, from which we obtain the potential of mean force once again following the same procedure as in the previous case. For the last case study we fixed both the colloids and the polymer chains concentration, while increasing the length of the polymer chains and obtain again the potential of mean force. In all of these simulations, the solvent particles are included explicitly. Using these data we propose a new effective potential of interaction for colloidal dispersion whose parameters can be obtained from mesoscopic scale parameters and carry out standard molecular dynamics simulations with this new potential, thereby providing a route for more fundamentally obtained, coarse grained approaches to model colloidal dispersions.

cond-mat.soft↗

arXiv2015

Rheological properties of brushes on cancerous epithelial cells under the influence of an external oscillatory force

The rheological properties of brushes of different length on the surface of human epithelial cancerous cells are studied here by means of coarse grained numerical simulations, where the surface of the cell is subjected to an external oscillatory force acting on the plane of the cell surface. We model explicitly the tip of an atomic force microscope and the cancerous cell as a surface covered by brushes of different length, and take into account the interactions of the brush chains with the tip and with each other, leading to complex rheological behavior as displayed by the profiles of viscosity and the friction coefficient of this complex system. We comment briefly on how these findings can help in the experimental effort to understand the nature of the cancer growth in human epithelial cells.

cond-mat.soft↗

arXiv2015

Importance of molecular interactions in colloidal dispersions

We review briefly the concept of colloidal dispersions, their general properties and some of their most important applications, as well as the basic molecular interactions that give rise to their properties in equilibrium. Similarly, we revisit Brownian motion and hydrodynamic interactions associated with the concept of viscosity of colloidal dispersion. It is argued that the use of modern research tools, such as computer simulations, allows one to predict accurately some macroscopically measurable properties by solving relatively simple models of molecular interactions for a large number of particles. Lastly, as a case study, we report the prediction of rheological properties of polymer brushes using state of the art, coarse grained computer simulations, which are in excellent agreement with experiments.

cond-mat.soft↗

arXiv2015

Importance of pore length and geometry in the adsorption/desorption process: a molecular simulation study

Discrete potentials can describe properly the liquid vapor boundary that is necessary to model the adsorption of gas molecules in mesoporous systems with computer simulations. Although there are some works in this subject, the simulations are still highly time - consuming. Here we show that an efficient alternative is to use the three - dimensional Ising model, which allows one to model large systems, with geometries as complex as required that accurately represent the liquid vapor boundary. In particular, we report molecular simulations of cylindrical pores of two different geometry, using a discrete potential. The effect of the length of the pore in the hysteresis loop for a finite pore and infinite one is studied in detail. Lastly, we compare our predictions with experimental results and find excellent agreement between the area of the hysteresis loop predicted for the finite pore and that found in adsorption/desorption experiments.

cond-mat.soft↗

arXiv2015

On the computational modeling of the viscosity of colloidal dispersions and its relation with basic molecular interactions

The connection between fundamental interactions acting in molecules in a fluid and macroscopically measured properties, such as the viscosity between colloidal particles coated with polymers, is studied here. The role that hydrodynamic and Brownian forces play in colloidal dispersions is also discussed. It is argued that many body systems in which all these interactions take place can be accurately solved using computational simulation tools. One of those modern tools is the technique known as dissipative particle dynamics, which incorporates Brownian and hydrodynamic forces, as well as basic conservative interactions. A case study is reported, as an example of the applications of this technique, which consists of the prediction of the viscosity and friction between two opposing parallel surfaces covered with polymer chains, under the influence of a steady flow. This work is intended to serve as an introduction to the subject of colloidal dispersions and computer simulations, for last year undergraduate students and beginning graduate students who are interested in beginning research in soft matter systems. To that end, a computational code is included that students can use right away to study complex fluids in equilibrium.

cond-mat.soft↗

arXiv2015

Adsorption desorption processes on mesoscopic pores conected to microscopic pores of complex geometry using the Ising model

In this work we report studies of nitrogen adsorption and desorption onto solid surfaces using computer simulations of the three dimensional Ising model, for systems with complex porous structures at the mesoscopic and microscopic levels. A hysteresis cycle between the adsorption and desorption processes appears and we find that its characteristics are dependent on the geometry of the pore and on the strength of the surface fluid interaction. We obtained also an average adsorption isotherm, which represents a combination of differently shaped pores, and shows robust jumps at certain values of the chemical potential as a consequence of the structures of the pores. Lastly, we compare our results with experimental data and also report the filling process of microscopic pores connected with mesopores. It is argued that these predictions are useful for researchers working on the enhanced recovery of oil and for the design of new nanomaterials, among others.

cond-mat.soft↗

arXiv2014

The role of the dissipative and random forces in the calculation of the pressure of simple fluids with dissipative particle dynamics

The role of viscous forces coupled with Brownian forces in momentum conserving computer simulations is studied here in the context of their contribution to the total average pressure of a simple fluid as derived from the virial theorem, in comparison with the contribution of the conservative force to the total pressure. The specific mesoscopic model used is the one known as dissipative particle dynamics, although our conclusions apply to similar models that obey the fluctuation dissipation theorem for short range interactions and have velocity dependent viscous forces. We find that the average contribution of the random and dissipative forces to the pressure is negligible for long simulations, provided these forces are appropriately coupled and when the finite time step used in the integration of the equation of motion is not too small. Finally, we study the properties of the fluid when the random force is made equal to zero and find that the system freezes as a result of the competition of the dissipative and conservative forces.

physics.chem-ph↗