Random Sequential Adsorption Model Research Articles

Tuning the Topography of Non‐Wetting Surfaces to Reduce Short‐Term Microbial Contamination Within Hospitals

AbstractMicrobial contamination of hospital surfaces is a major contributor to infectious disease transmission. This work demonstrates that superhydrophobic (Cassie‐Baxter) micro post topographies can significantly reduce cell attachment compared to flat controls. For ordered micro post arrays (post diameters 0.3 to 150 µm), the attachment of four pathogens (Pseudomonas aeruginosa, Staphylococcus aureus, Escherichia coli, and Candida albicans) from discrete contaminant droplets upon short‐term contact (15 s to 30 min) are assessed. There is a 3‐4‐log decrease in microbial attachment when reducing the micro posts diameters from 150 to 0.3 µm for all strains, with large posts (>20 µm) exhibiting similar attachment rates to flat controls. The critical, maximum feature size to prevent attachment can be tuned depending on the ratio of the cell size to post diameter. Two potential mechanisms are discussed for this size effect. First, application of the random sequential adsorption model shows that this relative post/cell size effect may be due to a reduced probability of attachment, which is theorized to be the dominant mechanism. Alternatively, a physical model is suggested for bacterial cell “pull‐off” due to surface tension forces during droplet dewetting. This work may be important for the design of non‐wetting antimicrobial surfaces within healthcare environments.

Percolation connectivity in deposits obtained usingcompetitive random sequential adsorption of binarydisk mixtures

Connectedness percolation phenomena in the two-dimensional (2D) packing of binary mixtures of disks with different diameters were studied numerically. The packings were produced using random sequential adsorption (RSA) model with simultaneous deposition of disks. The ratio of the particle diameters was varied within the range D=1-10, and the selection probability of the small disks was varied within the range 0-1. A core-shell structure of the particles was assumed for the analysis of connectivity. The packing coverages in a jamming state for different components, connectivities through small, large and both types of disks, the behavior of electrical conductivity were analyzed. The observed complex effects were explained accounting for the formation of conductive "bridges" from small disks in pores between large disks.

Density and Correlation in a Random Sequential Adsorption Model

We consider the random sequential adsorption process on the one- dimensional lattice with nearest-neighbor exclusion. In this model, each site s 2 Z starts empty and a particle will be deposited in it at time ts, where (ts)s2Z is a sequence of independent random variables uniformly distributed on the interval [0; 1]. The site will be occupied if both of its neighbors are vacant. Analytical expressions for the density of occupied sites and the pair correlation function, for all time t, are well-established and have been obtained through methods such as generating functions and differential equations. In this study, we present a method based on probabilistic arguments for the calculation of these expressions.

One-dimensional AB random sequential adsorption with one deposition per site

We investigate a modified version of the AB random sequential adsorption model. Specifically, this model involves the deposition of two distinct types of particles onto a lattice, with the constraint that different types cannot occupy neighboring sites. By restricting the deposition attempts to only one per site, we derive an analytical expression for the average densities of particles of types A and B, at all time instances, for all deposition probabilities of each particle type.

Two-stage random sequential adsorption of discorectangles and disks on a two-dimensional surface.

The different variants of two-stage random sequential adsorption (RSA) models for packing of disks and discorectangles on a two-dimensional (2D) surface were investigated. In the SD (sticks+disks) model, the discorectangles were first deposited and then the disks were added. In the DS (disks+sticks) model, the disks were first deposited and then discorectangles were added. At the first stage the particles were deposited up to the selected concentration and at the final (second) stage the particles were deposited up to the saturated (jamming) state. The main parameters of the models were the concentration of particles deposited at the first stage, aspect ratio of the discorectangles ɛ (length to diameter of ratio ɛ=l/d) and disk diameter D. All distances were measured using the value of d as a unit of measurement of linear dimensions, the disk diameter was varied in the interval D∈[1-10], and the aspect ratio value was varied in the interval ɛ∈[1-50]. The dependencies of the jamming coverage of particles deposited at the second stage versus the parameters of the models were analyzed. The presence of first deposited particles for both models regulated the maximum possible disk diameter D_{max} (SD model) or the maximum aspect ratio ɛ_{max} (DS model). This behavior was explained by the deposition of particles in the second stage into triangular (SD model) or elongated (DS model) pores formed by particles deposited at the first stage. The percolation connectivity of disks (SD model) and discorectangles (DS model) for the particles with a hard core and a soft shell structure was analyzed. The disconnectedness was ensured by overlapping of soft shells. The dependencies of connectivity versus the parameters of SD and DS models were also analyzed.

Mechanisms of Anisotropic Particle Deposition: Prolate Spheroid Layers on Mica

Anisotropic particle deposition was investigated using the streaming potential method complemented with the atomic force microscopy (AFM) determination of the absolute particle coverage. The polymer particles were synthesized using the stretching procedure with consecutive oxidation of surface hydroxyl groups and coupling of polyethyleneimine. The bulk particle physicochemical properties were characterized by scanning electron microscopy (SEM), dynamic light scattering, and laser Doppler velocimetry. The particles were positively charged in the pH range of 3–10, exhibiting a prolate spheroid shape with an axis ratio of five. Thorough AFM and in situ optical microscopy measurements yielded the adsorption kinetics of particles under the diffusion-controlled regime. The experimental data were adequately interpreted in terms of the random sequential adsorption model with the surface blocking function derived from the scaled particle theory. The root-mean-square (rms) parameter of the layers for a broad range of particle coverage was also determined and interpreted using the topographical model developed in this work. The experiments were complemented by the measurements of the streaming potential of particle layers under various ionic strengths and pHs. The ζ (zeta)-potential data acquired in this way enabled to determine the universal hydrodynamic function describing the dependence of the streaming potential on the particle coverage. The function was used to express the ζ-potential of surfaces covered by particles in terms of substrate rms. It was argued that the acquired results, in addition to being significanct to basic science, can be exploited as useful reference systems for quantitative interpretation of bioparticle deposition on abiotic surfaces.

Study on the Influence of Reinforced Particles Spatial Arrangement on the Neutron Shielding Performance of the Composites.

Particle-reinforced composites are widely applied as nuclear radiation shielding materials for their excellent comprehensive properties. The work aimed to calculate the influence of the functional reinforced particles spatial arrangement on the neutron shielding performance of composites and attempted to explain the influence mechanism by investigating the neutron flux distribution in the materials. Firstly, four suitable physical models were established based on the Monte Carlo Particle Transport Program (MCNP) and mathematical software MATLAB, namely the RSA (Random Sequential Adsorption) Model with particles random arrangement and FCC Model, BCC Model and Staggered Arrangement Model (SA Model) with particle periodic arrangements. Later, based on these four physical models, the neutron transmittance of two kinds of typical B4C reinforced composites, 316 stainless steel matrix composite and polyethylene matrix composite, were calculated under different energy neutrons sources (0.0253 eV, 50 eV, 50 keV, fission spectrum, 241Am-Be spectrum and 14.1 MeV) and the neutron flux distribution in the 316 stainless steel composite was also analyzed under 0.0253 eV neutron and fission neutron sources. The results indicated that the spatial arrangement of B4C has an impact on the neutrons shielding performance of the composite and the influence changes with neutron energy and B4C content. It can be concluded that the RSA model and the periodic arrangement models can be used in different calculation cases in the future.

Jamming and percolation in the random sequential adsorption of a binary mixture on the square lattice

We study the competitive irreversible adsorption of a binary mixture of monomers and square-shaped particles of linear size R on the square lattice. With the random sequential adsorption model, we investigate how the jamming coverage and percolation properties depend on the size ratio R and relative flux F. We find that the onset of percolation of monomers is always lower for the binary mixture than in the case with only monomers (R = 1). Moreover, for values F below a critical value, the higher is the flux or size of the largest species, the lower is the value of the percolation threshold for monomers.

Capturing colloidal nano- and microplastics with plant-based nanocellulose networks

Microplastics accumulate in various aquatic organisms causing serious health issues, and have raised concerns about human health by entering our food chain. The recovery techniques for the most challenging colloidal fraction are limited, even for analytical purposes. Here we show how a hygroscopic nanocellulose network acts as an ideal capturing material even for the tiniest nanoplastic particles. We reveal that the entrapment of particles from aqueous environment is primarily a result of the network’s hygroscopic nature - a feature which is further intensified with the high surface area of nanocellulose. We broaden the understanding of the mechanism for particle capture by investigating the influence of pH and ionic strength on the adsorption behaviour. We determine the nanoplastic binding mechanisms using surface sensitive methods, and interpret the results with the random sequential adsorption (RSA) model. These findings hold potential for the explicit quantification of the colloidal nano- and microplastics from different aqueous environments, and eventually, provide solutions to collect them directly on-site where they are produced.

Relaxation of saturated random sequential adsorption packings of discorectangles aligned on a line.

Relaxation of the packing of elongated particles (discorectangles) aligned on a line was studied numerically. The aspect ratio (length-to-width ratio) for the discorectangles was varied within the range ɛ∈[1;50]. The initial jamming (saturated) state was produced using the basic variant of the random sequential adsorption model with random positions and orientations of particles. The relaxation was performed by allowing rotational and translational diffusion motions of the particles while their centers remained located on the line. The effects of the aspect ratio ɛ on the kinetics of relaxation, the orientation order parameter, and the distribution function of the distances between nearest-neighbor discorectangles were analyzed. The transport properties of the resulting one-dimensional systems were also analyzed by using the diffusion of a tracer particle (random walker) between the nearest-neighbor discorectangles. In the relaxed states the anomalous diffusion was observed having a hopping exponent d_{w}>2 dependent upon ɛ.

Confinement effects on the random sequential adsorption packings of elongated particles in a slit.

The behavior of a system of two-dimensional elongated particles (discorectangles) packed in a slit between the two parallel walls was analyzed using a simulation approach. The packings were produced using the random sequential adsorption model with continuous positional and orientational degrees of freedom. The aspect ratio (length-to-width ratio, ɛ=l/d) of the particles was varied within the range ɛ∈[1;32] while the distance between the walls was varied within the range h/d∈[1;80]. The properties of deposits in jammed state [the coverage, the order parameter, and the long-range (percolation) connectivity between particles] were studied numerically. The values of ɛ and h significantly affected the structure of the packings and the percolation connectivity. Particularly, the observed nontrivial dependencies of the jamming coverage φ(ɛ) or φ(h) were explained by the interplay of the different geometrical factors related to confinement, particle orientation degrees of freedom and excluded volume effects.

Particle Deposition to Silica Surfaces Functionalized with Cationic Polyelectrolytes

Positively charged water-solid interfaces are prepared by adsorption of a cationic polyelectrolyte poly(diallyldimethylammonium chloride) (PDADMAC) from aqueous solutions to planar silica substrates. These substrates are characterized by atomic force microscopy (AFM), optical reflectivity, and streaming current measurements. By tuning the amount of adsorbed polyelectrolyte, the surface charge of the substrate can be systematically varied. These substrates are further used to study deposition of sulfate latex nanoparticles, which is also accomplished by optical reflectivity. This deposition process is found to be consistent with an extension of the random sequential adsorption (RSA) model in a semi-quantitative fashion. Such deposition studies were further used to ascertain that the substrates obtained by in situ and ex situ functionalization behave in an identical fashion.

Large deviations in one-dimensional random sequential adsorption.

In random sequential adsorption (RSA), objects are deposited randomly, irreversibly, and sequentially; attempts leading to an overlap with previously deposited objects are discarded. The process continues until the system reaches a jammed state when no further additions are possible. We analyze a class of lattice RSA models in which landing on an empty site in a segment is allowed when at least b neighboring sites on the left and the right are unoccupied. For the minimal model (b=1), we compute the full counting statistics of the occupation number. We reduce the determination of the full counting statistics to a Riccati equation that appears analytically solvable only when b=1. We develop a perturbation procedure which, in principle, allows one to determine cumulants consecutively, and we compute the variance of the occupation number for all b.

Microparticle Deposition on Human Serum Albumin Layers: Unraveling Anomalous Adsorption Mechanism

Human serum albumin (HSA) layers are adsorbed on mica under controlled diffusion transport at pH 3.5 and various ionic strengths. The surface concentration of HSA is directly determined by AFM imaging of single molecules. It is shown that the adsorption kinetics derived in this way is quantitatively described using the random sequential (RSA) adsorption model. The electrokinetic characteristics of the HSA layers at various pHs comprising their zeta potential are acquired in situ while using the streaming potential method. It is shown that at pH 3.5 the zeta potential of mica becomes positive for HSA concentrations above 3000 μm−2. At larger pHs, HSA layers exhibit negative zeta potential for the entire range of coverage. Thorough characteristics of these monolayers at various pHs were performed applying the colloid deposition method involving negatively charged polystyrene microparticles. The kinetics of their deposition and their maximum coverage are determined as a function of the HSA layer surface concentration, pH, and ionic strength. An anomalous deposition of microparticles on substrates also exhibiting a negative zeta potential is observed, which contradicts the Derjaguin, Landau, Vervey, Overbeek (DLVO) theory. This effect is interpreted in terms of heterogeneous charge distribution that results from molecule concentration fluctuations. It is also shown that the maximum concentration of microparticles abruptly decreases with the electric double-layer thickness that is regulated by changing ionic strength, which indicates that their deposition is governed by electrostatic interactions. One can argue that the results obtained in this work can be exploited as useful reference data for the analysis of deposition phenomena of bioparticles on protein layers.

Adsorption kinetic of myoglobin on mica and silica – Role of electrostatic interactions

Adsorption kinetics of myoglobin molecules on mica and silica was studied using the atomic force microscopy (AFM), the colloid enhancement and the quartz microbalance (QCM) methods. Measurements were carried out for the NaCl concentration of 0.01 and 0.15 M as a function of pH comprising pH 7.4 stabilized by the PBS buffer. The electrophoretic mobility measurements enabled to derive the molecules zeta potential as a function of pH. The isoelectric point appearing at pH 5, is lower than that predicted from the theoretical calculations of the nominal dissociation charge. The AFM investigations confirmed that myoglobin molecules irreversibly adsorb at pH 3.5 yielding well-defined layers of single molecules. These layers were characterized using the colloid enhancement method involving polymer microparticles for pH range 3–9. The microparticle deposition kinetics was adequately interpreted in terms of a hybrid random sequential adsorption model. It is confirmed that the myoglobin layers exhibit a negligible zeta potential at pH equal to 5 in accordance with the electrophoretic mobility measurements. Analogous adsorption kinetic measurements were performed for the silica substrate using QCM and AFM. It is observed that myoglobin molecules irreversibly adsorb at pH 3.5 forming stable layers of single molecules. On the other hand, its adsorption kinetics at larger pHs was much slower exhibiting a poorly defined maximum coverage. This was attributed to aggregation of the myoglobin solutions due to their vanishing charge. The kinetic QCM runs were adequately interpreted in terms of a theoretical model combining the Smoluchowski aggregation theory with the convective diffusion mass transfer theory.

Random model for radiation shielding calculation of particle reinforced metal matrix composites and its application

The work aimed to calculate the radiation biological shielding performance of particle reinforced metal matrix composite (PRMMCs) using more reasonable model instead of conventional Uniform Filling Model, also attempted to provide a basis for the radiation shielding optimal design of such materials. Firstly, RSA (Random Sequential Adsorption) Model and GRM (Grid Random Model) were established based on MATLAB and Monte Carlo Particle transport program MCNP, and then advantages and disadvantages of them were compared. Later, the influences of metal matrix type, particle (B4C) content, particle shape and particle shape parameters on the biological shielding performance of materials were calculated under different energy neutrons and different thickness shield using random models. Finally, the optimal aspect ratio of regular hexahedral B4C was calculated by Genetic Algorithm combined with MATLAB and MCNP. It indicated that GRM could be applied to radiation shielding calculation of PRMMCs.

Mechanism of lysozyme adsorption onto gold surface determined by quartz crystal microbalance and surface plasmon resonance

In this study, the physicochemical characterization of lysozyme adsorbed on gold was investigated. Through the use of MP-SPR it was possible to establish that the orientation of molecules changes from side-on to between or end-on with increasing surface coverage. The data confirms that the process of adsorption is driven primarily by electrostatic interactions but also by hydrophobic forces. MP-SPR data was compared with the Random Sequential Adsorption model for a molecule with an ellipsoidal shape. Contact angle measurements showed that higher surface coverage also translates in more hydrophilic properties of obtained lysozyme layer. Comparison of CD and PM-IRRAS spectra in solution and adsorbed state respectively showed changes in the secondary structures of lysozyme. These changes are dependent on pH, but fundamentally they go in the direction of the increase of β-turn/random content with a simultaneous decrease in β-sheet fraction, which suggests that aggregation is not occurring. The combination of MP-SPR and QCM-D measurements allowed the estimation of the number of water molecules associated with the lysozymes films. It has been observed that hydration decreases from 70% in pH = 4 to 30% in pH = 11. This data indicates that hydration is driven mainly by the degree of protonation of lysozyme molecules.

Hydrodynamic Solvent Coupling Effects in Quartz Crystal Microbalance Measurements of Nanoparticle Deposition Kinetics.

Hydrodynamic coupling effects pertinent to quartz crystal microbalance (QCM) investigation of nanoparticle adsorption kinetics were evaluated using atomic force microscopy and the theoretical modeling. Monodisperse polymer particles of the size between 26 and 140 nm and the density of 1.05 g cm–3 were used. The ζ-potential of particles was opposite to the substrate ζ-potential that promoted their irreversible adsorption on the silica sensor. The experimental kinetic data were interpreted in terms of theoretical calculations derived from the hybrid random sequential adsorption model. This allowed us to determine the amount of hydrodynamically coupled solvent (electrolyte) for the absolute particle coverage range up to 0.5. The coupling function representing the ratio of the solvent to the particle volumes was also determined and used to explicitly calculate the solvent level in particle monolayers. It is shown that the solvent level abruptly increases with the particle coverage attaining values comparable with the particle size. One can expect that these results can serve as useful reference data for the interpretation of protein adsorption kinetics on rough surfaces where the presence of stagnant solvent is inevitable.

Percolation in random sequential adsorption of mixtures on a triangular lattice

Percolation properties of two-component mixtures are studied by Monte Carlo simulations. Objects are deposited onto a substrate according to the random sequential adsorption model. Various shapes making the mixtures are made by self-avoiding walks on a triangular lattice. Percolation threshold for mixtures of objects covering the same number of sites is always lower than for the more compact object, and it can be even lower than for both components. Mixtures of percolating and non-percolating objects almost always percolate, but the percolation threshold is higher than for the percolating component. Adding a shape of high connectivity to a system of compact non-percolating objects, makes the deposit percolate. Lowest percolation thresholds are obtained for mixtures with elongated angled objects. Dependence of on the object length exhibits a minimum, so it could be estimated that the angled objects of length give the largest contribution to the percolation.

Relaxation in two-dimensional suspensions of rods as driven by Brownian diffusion.

Relaxation in a two-dimensional suspensions containing rods was studied by using dynamic Monte Carlo simulations. An off-lattice model with continuous positional and orientational degrees of freedom was considered. The initial state was produced by using a random sequential adsorption model. During the relaxation, the rods underwent translational and rotational Brownian motions. The simulations were run at different values of number density ρ (the number of rods per unit area) and of the initial orientation order parameter S_{i}. The rods were assumed to have core-shell structures. The evolutions of both the connectivity and the order parameter have revealed different relaxation behavior.