Long-range Attraction Research Articles

Onion‐like Multifunctional Microtrap Vehicles for Attraction–Trapping–Destruction of Biological Threats

AbstractA multifunctional motile microtrap is developed that is capable of autonomously attracting, trapping, and destroying pathogens by controlled chemoattractant and therapeutic agent release. The onion‐inspired multi‐layer structure contains a magnesium engine core and inner chemoattractant and therapeutic layers. Upon chemical propulsion, the magnesium core is depleted, resulting in a hollow structure that exposes the inner layers and serves as structural trap. The sequential dissolution and autonomous release of the chemoattractant and killing agents result in long‐range chemotactic attraction, trapping, and destruction of motile pathogens. The dissolved chemoattractant (l‐serine) significantly increases the accumulation and capture of motile pathogens (E. coli) within the microtrap structure, while the internal release of silver ions (Ag+) leads to lysis of the pathogen accumulated within the microtrap cavity.

Origin of the long-ranged attraction or repulsion between intruders in a confined granular medium

Origin of the long-ranged attraction or repulsion between intruders in a confined granular medium

Wetting transitions on soft substrates

Within mean-field theory we study wetting of elastic substrates. Our analysis is based on a grand canonical free energy functional of the fluid number density and of the substrate displacement field. The substrate is described in terms of the linear theory of elasticity, parametrized by two Lamé coefficients. The fluid contribution is of the van der Waals type. Two potentials characterize the interparticle interactions in the system. The long-ranged attraction between the fluid particles is described by a potential , and characterizes the substrate-fluid interaction. By integrating out the elastic degrees of freedom we obtain an effective theory for the fluid number density alone. Its structure is similar to the one for the wetting of an inert substrate. However, the potential is replaced by an effective potential which, in addition to , contains a term bilinear in . We discuss the corresponding wetting transitions in terms of an effective interface potential , where ℓ denotes the thickness of the wetting layer. We show that in the case of algebraically decaying interactions the elasticity of the substrate may suppress critical wetting transitions, and may even turn them first order.

Diagrammatic method for tunable interactions in colloidal suspensions in rotating electric or magnetic fields.

Tunable interactions in colloids, induced by rotating electric or magnetic fields, provide a flexible and promising tool for self-assembly of soft materials, as well as for fundamental particle-resolved studies of phase transitions and other generic phenomena in condensed matter. In the case of two-dimensional systems and the in-plane rotating fields, the interactions are known to have a long-range (dipolar) attraction and an expressed three-body part at short distances, but still remain poorly understood. Here, we show that the interactions and polarization mechanisms governing the tunable interactions can be described, calculated, and analyzed in detail with the diagrammatic method we proposed. The diagrams yield a clear illustration of different polarization processes contributing to the Keesom, Debye, London, self, and external energies, classified in colloids similarly to intermolecular interactions. The real tunable interactions, obtained with the boundary element method, can be simply and accurately interpolated with the set of basis of the diagrams attributed to different physically clear polarization processes. Calculation of large-distance behavior and interpolation of the many-body interactions (and analysis of the leading mechanisms contributing to them) excellently illustrate that the diagrammatic method provides deep insights into the nature of tunable interactions. The method can be generalized for multicomponent systems, suspensions of particles with a composite structure and a complicated shape. The results provide significant advance in theoretical methods for detailed analysis of tunable interactions in colloids and, therefore, the method is of broad interest in condensed matter, chemical physics, physical chemistry, materials science, and soft matter.

Crossover from type I to type II regime of mesoscopic superconductors of the first group

In the present work, we have studied the crossover between type I and type II superconductivity on mesoscopic superconducting thin films by numerically solving the 3D Ginzburg–Landau equations. We determined the dependence on temperature of the critical Ginzburg–Landau parameter , below which the superconductor behaves as type I for a given thickness d of the film. The effect of the sample dimensions on this crossover was also investigated. Additionally, we report a novel giant vortex configuration with a local minimum of the magnetic field at the centre of the core. Finally, we present certain results suggesting that the vortex-vortex interaction is not monotonic, varying instead from long-range attraction to short-range repulsion.

Deterministic Deposition of Nanoparticles with Sub-10 nm Resolution.

Accurate deposition of nanoparticles at defined positions on a substrate is still a challenging task, because it requires simultaneously stable long-range transport and attraction to the target site and precise short-range orientation and deposition. Here we present a method based on geometry-induced energy landscapes in a nanofluidic slit for particle manipulation: Brownian motors or electro-osmotic flows are used for particle delivery to the target area. At the target site, electrostatic trapping localizes and orients the particles. Finally, reducing the gap distance of the slit leads sequentially to a focusing of the particle position and a jump into adhesive contact by several nanometers. For 60 nm gold spheres, we obtain a placement accuracy of 8 nm. The versatility of the method is demonstrated further by a stacked assembly of nanorods and the directed deposition of InAs nanowires.

Self-Assembly Formed by Spherical Patchy Particles with Long-Range Attraction

We report on self-assemblies formed from spherical patchy particles interacting by a long-range attraction through a patch region in a two-dimensional system. We performed Monte Carlo simulations to find stable structures in a system with constant number of particles under constant temperature and constant pressure (NPT system), in which particles interact via the Kern–Frenkel potential. For long-range attractive potentials, we describe how these stable structures and their formation depend on the coverage of the patch. Under high pressure, when the coverage is small, triangular lattices are formed as reported in previous papers. From our simulations, we find when the pressure is low short chain-like structures, in which the distance between particles is long, and square clusters, which are not formed with a short-range attractive potential, are formed. When the coverage of the patch region is large, square clusters are formed since the interaction between particles is stronger than that for with small coverage. When the coverage ratio is larger than 0.5, the direction of the patch is perpendicular to the plane in which the particles are placed.

Structure of Dense Adsorption Layers of Escin at the Air-Water Interface Studied by Molecular Dynamics Simulations.

Saponins are natural surfactants with high surface activity and unique surface properties. Escin is a triterpenoid saponin which has unusually high surface viscoelasticity [Golemanov et al. Soft Matter 2013, 9, 5738] and low permittivity to molecular gas diffusion of its adsorption layers. In our previous study [Tsibranska et al. Langmuir 2017, 33, 8330], we investigated the molecular origin of this unconventional behavior and found that escin molecules rapidly assemble in a compact and stable surface cluster. This behavior was explained with long-range attraction between the hydrophobic aglycones combined with intermediate dipole-dipole attraction and strong short-range hydrogen bonds between the sugar residues in the adsorbed escin molecules. In this study, we performed atomistic molecular simulations of escin molecules in dense adsorption layers with two different areas per molecule. The results show that the surfactant molecules in these systems are much less submerged in water and adopt a more upright position compared to the dilute layers studied previously. A significant number of trapped water molecules are located around the hydrophilic groups placed above the water equimolecular surface to solvate them in the dense layer. To maintain the preferred orientation of the escin molecules with respect to the interface, the most compact adsorption layer acquires a significant spontaneous curvature. The substantial elasticity of the neutral escin layers, as in our previous study, is explained with the presence of a specific interaction, which is intermediate between hydrogen bonding and dipole-dipole attraction (populated lengths in the range 0.16 to >0.35 nm), supplemented by substantial flexibility of the surfactant heads, optimal curvature of the interface, and significant normal displacement of the molecules to allow their tight surface packing. The simulations reveal long-range order within the layers, which signifies the role of the collective behavior of the saponin molecules in such dense adsorption layers.

Stable emergent formations for a swarm of autonomous car-like vehicles

A biological swarm is an ideal multi-agent system that collectively self-organizes into bounded, if not stable, formations. A mathematical model, developed appropriately from some principle of swarming, should enable one, therefore, to study formation strategies for multiple autonomous robots. In this article, based on the hypothesis that swarming is an interplay between long-range attraction and short-range repulsion between the individuals in the swarm, a planar individual-based or Lagrangian swarm model is constructed using the Direct Method of Lyapunov. While attraction ensures the swarm is cohesive, meaning that the individuals in the swarm remain close to each other at all times, repulsion ensures that the swarm is well-spaced, meaning that no two individuals in the swarm occupy the same space at the same time. Via a novel Lyapunov-like function with attractive and repulsive components, the article establishes the global existence, uniqueness, and boundedness of solutions about the centroid. This paves the way to prove that the swarm model, governed by a system of first-order ordinary differential equations (ODEs), is cohesive and well-spaced. The article goes on to show that the artificial swarm can collectively self-organize into two stable formations: (i) a constant arrangement about the centroid when the system has equilibrium points, and (ii) a highly parallel formation when the system does not have equilibrium points. Computer simulations not only illustrate these but also reveal other emergent patterns such as swirling structures and random-like walks. As an application, we tailor the model accordingly and propose new autonomous steering laws giving rise to pattern-forming for multiple nonholonomic car-like vehicles.

Crystallisation in Melts of Short, Semi-Flexible Hard-Sphere Polymer Chains: The Role of the Non-Bonded Interaction Range

A melt of short semi-flexible polymers with hard-sphere-type non-bonded interaction undergoes a first-order crystallisation transition at lower density than a melt of hard-sphere monomers or a flexible hard-sphere chain. In contrast to the flexible hard-sphere chains, the semi-flexible ones have an intrinsic stiffness energy scale, which determines the natural temperature scale of the system. In this paper, we investigate the effect of weak additional non-bonded interaction on the phase transition temperature. We study the system using the stochastic approximation Monte Carlo (SAMC) method to estimate the micro-canonical entropy of the system. Since the density of states in the purely hard-sphere non-bonded interaction case already covers 5600 orders of magnitude, we consider the effect of weak interactions as a perturbation. In this case, the system undergoes the same ordering transition with a temperature shift non-uniformly depending on the additional interaction. Short-range attractions impede ordering of the melt of semi-flexible polymers and decrease the transition temperature, whereas relatively long-range attractions assist ordering and shift the transition temperature to higher values, whereas weak repulsive interactions demonstrate an opposite effect on the transition temperature.

Real-Space Mapping of the Two-Dimensional Phase Diagrams in Attractive Colloidal Systems

Video microscopy reveals the full 2D phase diagram of a colloid with short- and long-range attractions, which could lead to a better understanding of the phase behavior of real-world 2D materials such as biological membranes and graphene.

Chemical Bond Mechanism for Helium Revealed by Electronic Excitation.

Helium chemistry is notoriously very impervious. It is therefore certainly no surprise that, for example, beryllium and helium atoms, in their ground state, do not bind. Full configuration-interaction calculations show that the same turns out to be true, save for a long-range shallow attraction, for the Be+ + He system. However, quite astonishingly, when one electron is re-added to Be+ in an excited 2pπ or 3s orbital (Be 1P or 1S), a bound adduct with He is formed, at an interatomic separation as short as 1.5 Å. Understanding why this happens reveals an unsuspected chemical mechanism that stabilizes helium compounds at the molecular level.

Local interactions and their group-level consequences in flocking jackdaws.

As one of nature's most striking examples of collective behaviour, bird flocks have attracted extensive research. However, we still lack an understanding of the attractive and repulsive forces that govern interactions between individuals within flocks and how these forces influence neighbours' relative positions and ultimately determine the shape of flocks. We address these issues by analysing the three-dimensional movements of wild jackdaws ( Corvus monedula) in flocks containing 2-338 individuals. We quantify the social interaction forces in large, airborne flocks and find that these forces are highly anisotropic. The long-range attraction in the direction perpendicular to the movement direction is stronger than that along it, and the short-range repulsion is generated mainly by turning rather than changing speed. We explain this phenomenon by considering wingbeat frequency and the change in kinetic and gravitational potential energy during flight, and find that changing the direction of movement is less energetically costly than adjusting speed for birds. Furthermore, our data show that collision avoidance by turning can alter local neighbour distributions and ultimately change the group shape. Our results illustrate the macroscopic consequences of anisotropic interaction forces in bird flocks, and help to draw links between group structure, local interactions and the biophysics of animal locomotion.

Mechanistic and experimental models of cell migration reveal the importance of cell-to-cell pushing in cell invasion

Moving fronts of cells are essential for development, repair and disease progression. Therefore, understanding and quantifying the details of the mechanisms that drive the movement of cell fronts is of wide interest. Quantitatively identifying the role of intercellular interactions, and in particular the role of cell pushing, remains an open question. In this work, we report a combined experimental-modelling approach showing that intercellular interactions contribute significantly to the spatial spreading of a population of cells. We use a novel experimental data set with PC-3 prostate cancer cells that have been pretreated with Mitomycin-C to suppress proliferation. This allows us to experimentally separate the effects of cell migration from cell proliferation, thereby enabling us to focus on the migration process in detail as the population of cells recolonizes an initially-vacant region in a series of two-dimensional experiments. We quantitatively model the experiments using a stochastic modelling framework, based on Langevin dynamics, which explicitly incorporates random motility and various intercellular forces including: (i) long range attraction (adhesion); and (ii) finite size effects that drive short range repulsion (pushing). Quantitatively comparing the ability of this model to describe the experimentally observed population-level behaviour provides us with quantitative insight into the roles of random motility and intercellular interactions. To quantify the mechanisms at play, we calibrate the stochastic model to match experimental cell density profiles to obtain estimates of cell diffusivity, D, and the amplitude of intercellular forces, f0. Our analysis shows that taking a standard modelling approach which ignores intercellular forces provides a poor match to the experimental data whereas incorporating intercellular forces, including short-range pushing and longer range attraction, leads to a faithful representation of the experimental observations. These results demonstrate a significant role of cell pushing during cell front movement and invasion.

Enhancing phase contrast for bimodal AFM imaging in low quality factor environments

Since the invention of atomic force microscopy (AFM), there have been extensive studies with the goal of expanding its capabilities beyond topographical imaging. These studies have made AFM capable of providing material compositional mapping, magnetic or electrical properties, subsurface imaging not only in air environment but also in the liquid environment. Being able to perform AFM imaging in the liquid environment is advantageous since it can provide the true environment for various samples. However, it can also cause experimental challenges while tuning the dynamics of the cantilever for proper imaging. This issue can also be more problematic when performing multifrequency AFM in liquid environments. This paper focuses on providing both numerical and experimental procedures for selection of oscillation amplitudes for bimodal AFM in liquid with the goal of enhancing the higher eigenmode's phase channel. The numerical work has considered different models (vdW and DLVO) for long-range attraction models and DMT for short-range interactions. The oscillation amplitudes for both eigenmodes that provide the highest 2nd eigenmode's phase contrast have been selected. Simulations are done on three different polymers: low-density polyethylene (LDPE), polystyrene (PS) and polytetrafluoroethylene (PTFE). Correspondingly, the experimental results have verified that the selected configuration enhances the phase signal. The experiments are done on a polyethylene (LDPE) and polystyrene (PS) polymer blends in both air and liquid environment.

Hydration and Dispersion Forces in Hydroxypropylcellulose Phase Behavior.

Many-body polarization and hydration forces can strongly affect the equilibrium structure and energetics of mixed phases. Accurately reproducing both forces presents a challenge to force field models because it requires balancing hydrogen bonding at short range with many-body orientational order and dispersive attraction at long range. This work reports the first comparison of experimental measurements of the pressure-area isotherm for hydroxypropylcellulose (HPC) against molecular dynamics results with four different force field models-united-atom, all-atom (OPLS and CHARMM), and Drude oscillator models. All force fields exhibit the experimentally determined, exponentially shaped repulsive force at short range. Above a critical temperature of about 40 °C and a lattice spacing of around 14 Å, HPC experiments show a reversible, heat-induced polymer aggregation into an ordered phase driven by loss of water. The nonpolarizable force fields do not display the critical point and instead show biphasic behavior at all temperatures tested. This indicates net attractive forces at intermediate lattice spacings. In contrast, the Drude polarizable force field shows positive osmotic pressure and a single, homogeneous phase over all temperatures and spacings tested. Analysis of structural data from our simulations provides several clues to help interpret these findings. Although all force fields show similar water-water hydrogen bond numbers in the mixed phase, the polarizable model predicts that water-HPC hydrogen bonds are much more favorable than HPC-HPC hydrogen bonds when polymers are dispersed. At high density, water is driven out and replaced by HPC-HPC hydrogen bonds. The polarizable force field shows that both effects have a stronger dependence on polymer density than any of the nonpolarizable models. Our observations support the conclusion that hydration forces are coupled to the polymer coordination number by local, structural waters and that long-range dispersive attraction is overestimated by pairwise additive models.

Rapid Assembly of Colloidal Crystals under Laser Illumination on a GeSbTe Substrate.

Optical techniques have been actively studied for manipulating nano- to microsized objects. However, long-range attraction and rapid transport of particles within thin quasi-two-dimensional systems are difficult because of the weak thermophoretic forces. Here, we introduce an experimental system that can rapidly generate quasi-two-dimensional colloidal crystals in deionized water, sandwiched between two hard plates. When a pulsed laser is irradiated on a chalcogenide phase-change material spattered on one side of the plates, the induced Marangoni-like flow causes a colloidal self-assembly in the order of tens of micrometers within the laser spot, with a transport velocity of a few tens of micrometers per second. This is due to the large thermal gradient induced by chalcogenide characteristicsof high laser absorption and low thermal conductivity, and a strong hydrodynamic slip flow at the hydrophobic chalcogenide interface. Moreover, the colloidal crystals exhibit various lattice structures, depending on the laser intensity and chamber distance. For a certain range of the chamber distance, the colloidal crystal phases can be alternated by tuning the laser intensity in real time. Our system forms and deforms quasi-two-dimensional colloidal crystals at an on-demand location on a GeSbTe substrate.

Phase diagram of two-dimensional colloids with Yukawa repulsion and dipolar attraction.

We study the phase diagram of a two-dimensional (2D) system of colloidal particles, interacting via an isotropic potential with a short-ranged Yukawa repulsion and a long-ranged dipolar attraction. Such interactions in 2D colloidal suspensions can be induced by rapidly rotating in-plane magnetic (or electric) fields. Using computer simulations and liquid integral equation theory, we calculate the bulk phase diagram, which contains gas, crystalline, liquid, and supercritical fluid phases. The densities at the critical and triple points in the phase diagram are governed by the softness of Yukawa repulsion and can therefore be largely tuned. We observe that the liquid-gas binodals exhibit universal behavior when the effective temperature (given by the inverse magnitude of the dipolar attractions) is normalized by its value at the critical point and the density is normalized by the squared Barker-Henderson diameter. The results can be verified in particle-resolved experiments with colloidal suspensions.

Assessing Pair Interaction Potentials of Nanoparticles on Liquid Interfaces.

The pair interaction potentials of polymer-grafted silica nanoparticles (NPs) at liquid surfaces were determined by scanning electron microscopy, exploiting the nonvolatility of ionic liquids to stabilize the specimens against microscope vacuum. Even at near contact, individual, two-dimensionally well-dispersed NPs were resolved. The potential of mean force, reduced to the pair interaction potential for dilute NPs, was extracted with good accuracy from the radial distribution function, as both NP diameter and grafted polymer chain length were varied. While NP polydispersity somewhat broadened the core repulsion, the pair potential well-approximated a hard sphere interaction, making these systems suitable for model studies of interfacially bound NPs. For short (5 kDa) poly(ethylene glycol) ligands, a weak (< kB T) long-range attraction was discerned, and for ligands of identical length, pair potentials overlapped for NPs of different diameter; the attraction is suggested to arise from ligand-induced menisci. To understand better the interactions underlying the pair potential, NP surface-binding energies were measured by interfacial tensiometry, and NP contact angles were assessed by atomic force microscopy and transmission electron microscopy.

Breakup of ultra-thin liquid films on vertical fiber enhanced by Marangoni effect

An ultra-thin liquid film flowing down a vertical uniformly heated cylinder under the influence of gravity is investigated. A thin liquid film model is derived, assuming that the film thickness h is much smaller than the fiber radius a. To predict the breakup of film, the van der Waals attraction, proportional to h-3, is taken into account. Linear stability analysis shows that the Rayleigh-Plateau instability is enhanced by the long-range attractions and Marangoni effect. The spatial-temporal stability analysis shows that the instability is absolute when A+M>0.17 (A is a composite Hamaker number accounting for the strength of van der Waals attractions and M is the Marangoni number). A self-similarity analysis shows that the film thins as h∼(tr-t)1/5 (tr is the breakup time), which is supported by the numerical simulations of the thin film model. Although the scaling is independent on the Marangoni effect, nonlinear simulations demonstrate that the breakup time tr decreases as the Marangoni effect becomes stronger, demonstrating that the breakup process is accelerated by the Marangoni effect. Nonlinear simulation also shows that the thin heated or non-heated film mainly breaks up in the absolutely unstable regime.