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Haim Diamant

Publications and source records attributed to Haim Diamant.

At least 19 recordsLinked to original sources

Phase transitions and microphases in elastomers. II. Anisotropy-driven morphologies

In swollen elastomers, elasticity can arrest macroscopic demixing between the polymer network and the solvent, producing stable domains of finite size. While previous theories have focused on isotropically swollen elastomers, anisotropy strongly influences the phase behavior of many related systems, such as gels and crosslinked polymer blends. Building on the approach developed in Part I of this two-part paper, we investigate the effects of two experimentally induced sources of anisotropy: uniaxial swelling and stiffness gradients. We show that uniaxial swelling can lead to the formation of stable lamellar microphases and modify phase behavior, while stiffness gradients can cause spatial variations in the characteristic microphase size.

cond-mat.soft

Phase transitions and microphases in elastomers. I. Emergence of stable domains

Elasticity often plays a key role in regulating phase separation in physical systems. Recent experiments have shown that elastic effects can be used to control microphase separation in swollen elastomers. Here, microphase separation arises from a mismatch between the characteristic length scales of elastic and thermodynamic interactions. In this first part of a two-part paper, we show that microphase formation in elastomers can be explained using conventional theories of elasticity through a nonlocal thermodynamic-elastic coupling arising from volume conservation. Our theory reproduces the observed dependence of phase transition temperature and domain size on elastomer stiffness in isotropically swollen elastomers. In the companion paper, we investigate the effects of anisotropic swelling and inhomogeneous elastic moduli.

cond-mat.soft

Perspective: Measuring physical entropy out of equilibrium

Entropy is one of the key thermodynamic variables reflecting changes in the state of matter. Unlike other thermodynamic variables, it is well-defined also for nonequilibrium steady states through its relation to information. Applying this relation to physical systems is an ongoing challenge, as it requires knowledge of microscopic high-dimensional continuous distributions which is generally unattainable. A set of new approaches for the measurement of entropy in nonequilibrium steady or absorbing states have been developed and successfully applied to identify dynamic structures and transitions in diverse systems, ranging from jammed packings to swarming bacteria. We briefly review these approaches, emphasizing why applications to physical systems, including those out of equilibrium, is substantially different from the general statistical challenge of entropy estimation and inference. We point at promising current and future directions.

cond-mat.stat-mech

Dielectric response as a source of viscosity in polar liquids

Transport coefficients and dielectric relaxation in liquids are often treated as distinct manifestations of molecular dynamics. We show that, in polar liquids, orientational dipolar fluctuations generate a substantial contribution to the shear viscosity that can be expressed in terms of dielectric response parameters. Using a Green-Kubo approach formulated in terms of dipolar body-force correlations, we derive an explicit relation linking the viscosity contribution to the static permittivity and the Debye relaxation time. With a single microscopic cutoff length fixed from one temperature, the theory predicts the temperature dependence of the viscosity for water and several alcohols using independently measured dielectric data. The results identify a general mechanism by which slow polarization dynamics generate an additional, and in strongly polar liquids often dominant, contribution to the viscosity, providing a quantitative bridge between dielectric spectroscopy and rheology.

cond-mat.stat-mech

The effects of ionic valency and size asymmetry on counterion adsorption

We study the effect of asymmetry in solvent and ionic size on the equilibrium properties of multivalent ionic solutions near a charged surface. For a single ionic species in solution, we derive a generalized Grahame equation at the charged surface. For general size ratio between the ions and the solvent, we obtain analytical results for the concentration profiles as a function of the distance from the surface. For weak surface charge and small ion-to-solvent size ratio, the profile follows the classical Poisson-Boltzmann equation in dilute solution conditions. However, for high surface charge and large ionic size, the concentration profile saturates near the surface, leading to distinctive dependencies of the solution properties on the surface charge density and size asymmetry. Furthermore, the crossover between dilute and saturated regimes depends on the surface charge and ionic size asymmetry. We suggest that a solution containing multiple ionic species of different valencies and sizes stratifies close to the surface in the saturation regime. This leads to the formation of layers that are ordered according to the ions' valency-to-size ratio.

cond-mat.soft

STL-to-Stokeslet Computation of Mobility Tensors and Sedimentation Dynamics for Shaped Particles

Sedimentation is extremely common in nature, occurring throughout the atmosphere and oceans, and in every laboratory centrifuge. The shape and mass distribution of a particle uniquely determines its motion at low Reynolds number, and complex dynamics can emerge from even simple particle shapes. The dynamics are governed by the particle's hydrodynamic mobility tensor, which dictates the translational and rotational velocities given the forces and torques. However, to date the inference of the mobility tensor from the object shape has been cumbersome and tricky. Starting with an input file representing an object for a 3D printer, such as an STL file, here we present an efficient numerical framework to compute the mobility tensor by discretizing the particle surface into distributed point drag forces called stokeslets. We validate our results against analytical solutions of simple geometries and recent experimental measurements. With our calculated mobility tensors in hand, using standard transformation laws, we demonstrate the dramatic effect of shifting the center of mass from a center of symmetry: all initial orientations evolve into one, two, or three particular final motions dictated by the object. By providing a user-friendly and efficient framework to compute the mobility tensor and resulting particle dynamics, this work offers a broadly applicable tool for the soft-matter, fluid-mechanics, and biophysics communities, and facilitates the design of steerable particles under diverse external forces, with relevance to colloidal transport, biological locomotion, diffusion, and self-assembly.

cond-mat.soft

Collapse of a single polymer chain: Effects of chain stiffness and attraction range

Chain-like macromolecules in solution, whether biological or synthetic, transform from an extended conformation to a compact one when temperature or other system parameters change. This collapse transition is relevant in various phenomena, including DNA condensation, protein folding, and the behavior of polymers in solution. We investigate the interplay of chain stiffness and range of attraction between monomers in the collapse of a single polymer chain. We use Monte Carlo simulations based on the pruned-enriched Rosenbluth method. We demonstrate that the competition between the persistence length, l_p, and the range of attraction, r_c, determines whether the chain's collapse behavior resembles that of flexible chains or stiff ones. When l_p is larger than r_c, the chain collapses sharply with decreasing temperature, whereas if l_p is smaller than r_c, it contracts gradually. Notably, in the regime of small l_p and large r_c, this rounding into a gradual compaction persists upon increasing the chain length and may remain in place in the limit of infinite chain length. Furthermore, for small r_c, the transition temperature (theta-temperature) increases with l_p, whereas for large r_c the theta-temperature decreases with l_p. Thus, stiffness promotes collapse for small r_c but suppresses it for large r_c. Our findings are in agreement with recent experiments on the contraction of single-stranded RNA as compared to double-stranded DNA, and provide valuable insights for understanding polymer collapse and the essential polymer parameters affecting it.

cond-mat.soft

Theory of Microphase Separation in Elastomers

Inspired by recent experiments, we present a phase-field model of microphase separation in an elastomer swollen with a solvent. The imbalance between the molecular scale of demixing and the mesoscopic scale beyond which elasticity operates produces effective long-range interactions, forming stable finite-sized domains. Our predictions concerning the dependence of the domain size and transition temperature on the stiffness of the elastomer are in good agreement with the experiments. Analytical phase diagrams, aided by numerical findings, capture the richness of the microphase morphologies, paving the way to create stable, patterned elastomers for various applications.

cond-mat.soft

Model-free hydrodynamic theory of the colloidal glass transition

We present a phenomenological, model-free theory for the large-distance hydrodynamic response of a viscous fluid hosting colloidal particles. The flow of the host fluid is affected by the presence of the particles, thus reflecting their liquid or solid state. On the liquid side of the glass transition we identify a dynamic length scale $\ell$ beyond which the host fluid's response is that of a viscous fluid with increased effective viscosity $\eta$. As the glass transition is approached, $\ell$ increases indefinitely as $\ell \sim \eta^{1/2}$. At the transition the large-distance response changes qualitatively, marking the host fluid's loss of translation invariance. On the solid side of the transition we identify another dynamic length, $\ell_s$, beyond which the host fluid responds as a viscous fluid of increased effective viscosity $\eta^+$, confined in a porous medium of effective pore size $\ell_s$. As the glass transition is approached from the solid side, $\ell_s$ grows indefinitely, more sharply than $(\eta^+)^{1/2}$. We discuss various experimental implications of the results and their possible relation to microscopic theories of the colloidal glass transition.

cond-mat.soft

Fluids with power-law repulsion: Hyperuniformity and energy fluctuations

We revisit the equilibrium statistical mechanics of a classical fluid of point-like particles with repulsive power-law pair interactions, focusing on density and energy fluctuations at finite temperature. Such long-range interactions, decaying with inter-particle distance $r$ as $1/r^s$ in $d$ dimensions, are known to fall into two qualitatively different categories. For $s d$ ("weakly" long-range interactions) screening and hyperuniformity do not occur. Using scaling arguments, variational analysis, and Monte Carlo simulations, we find another qualitative distinction. For $s\geq d/2$ the strong repulsion at short distances leads to enhanced small-wavelength density fluctuations, decorrelating particle positions. This prevents indefinitely negative entropy and large energy fluctuations. The distinct behaviors for $s\geq d/2$ and $s<d/2$ give rise to qualitatively different dependencies of the entropy, heat capacity, and energy fluctuations on temperature and density. We investigate the effect of introducing an upper cutoff distance in the pair-potential. The effect of the cutoff on energy fluctuations is strong for $s<d/2$ and negligible for $s\geq d/2$.

cond-mat.stat-mech

Second Law of Thermodynamics without Einstein Relation

Materials that are constantly driven out of thermodynamic equilibrium, such as active and living systems, typically violate the Einstein relation. This may arise from active contributions to particle fluctuations which are unrelated to the dissipative resistance of the surrounding medium. We show that in these cases the widely used relation between informatic entropy production and heat dissipation does not hold. Consequently, fluctuation relations for the mechanical work, such as the Jarzynski and Crooks theorems, are invalid. We relate the breaking of the correspondence between entropy production and heat dissipation to departure from the fluctuation-dissipation theorem. We propose a temperaturelike variable that restores this correspondence and gives rise to a generalized second law of thermodynamics, whereby the dissipated heat is necessarily non-negative and vanishes at equilibrium. The Clausius inequality, Carnot maximum efficiency theorem, and relation between the extractable work and the change of free energy are recovered as well.

cond-mat.stat-mech

Universal Relation between Entropy and Kinetics

Relating thermodynamic and kinetic properties is a conceptual challenge with many practical benefits. Here, based on first principles, we derive a rigorous inequality relating the entropy and the dynamic propagator of particle configurations. It is universal and applicable to steady states arbitrarily far from thermal equilibrium. Applying the general relation to diffusive dynamics yields a relation between the entropy and the (normal or anomalous) diffusion coefficient. The relation can be used to obtain useful bounds for the late-time diffusion coefficient from the calculated steady-state entropy or, conversely, to estimate the entropy based on measured diffusion coefficients. We demonstrate the validity and usefulness of the relation through several examples and discuss its broad range of applications, in particular, for systems far from equilibrium.

cond-mat.stat-mech

Detecting and characterizing phase transitions in active matter using entropy

A major challenge in the study of active matter lies in quantitative characterization of phases and transitions between them. We show how the entropy of a collection of active objects can be used to classify regimes and spatial patterns in their collective behavior. Specifically, we estimate the contributions to the total entropy from correlations between the degrees of freedom of position and orientation. This analysis pin-points the flocking transition in the Vicsek model while clarifying the physical mechanism behind the transition. When applied to experiments on swarming Bacillus subtilis with different cell aspect ratios and overall bacterial area fractions, the entropy analysis reveals a rich phase diagram with transitions between qualitatively different swarm statistics. We discuss physical and biological implications of these findings.

cond-mat.soft

Resolving entropy contributions in nonequilibrium transitions

We derive a functional for the entropy contributed by any microscopic degrees of freedom as arising from their measurable pair correlations. Applicable both in and out of equilibrium, this functional yields the maximum entropy which a system can have given a certain correlation function. When applied to different correlations, the method allows us to identify the degrees of freedom governing a certain physical regime, thus capturing and characterizing dynamic transitions. The formalism applies also to systems whose translational invariance is broken by external forces and whose number of particles may vary. We apply it to experimental results for jammed bidisperse emulsions, capturing the crossover of this nonequilibrium system from crystalline to disordered hyperuniform structures as a function of mixture composition. We discover that the cross-correlations between the positions and sizes of droplets in the emulsion play the central role in the formation of the disordered hyperuniform states. We discuss implications of the approach for entropy estimation out of equilibrium and for characterizing transitions in disordered systems.

cond-mat.stat-mech

Electrostatics of Patchy Surfaces

In the study of colloidal, biological and electrochemical systems, it is customary to treat surfaces, macromolecules and electrodes as homogeneously charged. This simplified approach is proven successful in most cases, but fails to describe a wide range of heterogeneously charged surfaces commonly used in experiments. For example, recent experiments have revealed a long-range attraction between overall neutral surfaces, locally charged in a mosaic-like structure of positively and negatively charged domains ("patches"). Here we review experimental and theoretical studies addressing the stability of heterogeneously charged surfaces, their ionic strength in solution, and the interaction between two such surfaces. We focus on electrostatics, and highlight the important new physical parameters appearing in the heterogeneous case, such as the largest patch size and inter-surface charge correlations

cond-mat.soft

Structured viscoelastic substrates as linear foundations

The linear (Winkler) foundation is a simple model widely used for decades to account for the surface response of elastic bodies. It models the response as purely local, linear, and perpendicular to the surface. We extend this model to the case where the foundation is made of a structured material such as a polymer network, which has characteristic scales of length and time. We use the two-fluid model of viscoelastic structured materials to treat a film of finite thickness, supported on a rigid solid and subjected to a concentrated normal force at its free surface. We obtain the foundation modulus (Winkler constant) as a function of the film's thickness, intrinsic correlation length, and viscoelastic moduli, for three choices of boundary conditions. The results can be used to readily extend earlier applications of the Winkler model to more complex, microstructured substrates. They also provide a way to extract the intrinsic properties of such complex materials from mechanical surface measurements.

cond-mat.soft

Parametric excitation of wrinkles in elastic sheets on elastic and viscoelastic substrates

Thin elastic sheets supported on compliant media form wrinkles under lateral compression. Since the lateral pressure is coupled to the sheet's deformation, varying it periodically in time creates a parametric excitation. We study the resulting parametric resonance of wrinkling modes in sheets supported on semi-infinite elastic or viscoelastic media, at pressures smaller than the critical pressure of static wrinkling. We find distinctive behaviors as a function of excitation amplitude and frequency, including (a) a different dependence of the dynamic wrinkle wavelength on sheet thickness compared to the static wavelength; and (b) a discontinuous decrease of the wrinkle wavelength upon increasing excitation frequency at sufficiently large pressures. In the case of a viscoelastic substrate, resonant wrinkling requires crossing a threshold of excitation amplitude. The frequencies for observing these phenomena in relevant experimental systems are of the order of a kilohertz and above. We discuss experimental implications of the results.

cond-mat.soft

Symmetry properties of nonlinear hydrodynamic interactions between responsive particles

Two identical particles driven by the same steady force through a viscous fluid may move relative to one another due to hydrodynamic interactions. The presence or absence of this relative translation has a profound effect on the dynamics of a driven suspension consisting of many particles. We consider a pair of particles which, to linear order in the force, do not interact hydrodynamically. If the system possesses an intrinsic property (such as the shape of the particles, their position with respect to a boundary, or the shape of the boundary) which is affected by the external forcing, hydrodynamic interactions that depend nonlinearly on the force may emerge. We study the general properties of such nonlinear response. Analysis of the symmetries under particle exchange and under force reversal leads to general conclusions concerning the appearance of relative translation and the motion's time-reversibility. We demonstrate the applicability of the conclusions in three specific examples: (a) two spheres driven parallel to a wall; (b) two deformable objects driven parallel to their connecting line; and (c) two spheres driven along a curved path. The breaking of time-reversibility suggests a possible use of nonlinear hydrodynamic interactions to disperse or assemble particles by an alternating force.

cond-mat.soft