Condensed Matter

Incompressible nonlinearly hyperelastic materials are rarely simulated in Finite Element numerical experiments as being perfectly incompressible because of the numerical difficulties associated with globally satisfying this constraint. Most commercial Finite Element packages therefore assume that the material is slightly compressible. It is then further assumed that the corresponding strain-energy function can be decomposed additively into volumetric and deviatoric parts. We show that this decomposition is not physically realistic, especially for anisotropic materials, which are of particular interest for simulating the mechanical response of biological soft tissue. The most striking illustration of the shortcoming is that with this decomposition, an anisotropic cube under hydrostatic tension deforms into another cube instead of a hexahedron with non-parallel faces. Furthermore, commercial numerical codes require the specification of a `compressibility parameter' (or `penalty factor'), which arises naturally from the flawed additive decomposition of the strain-energy function. This parameter is often linked to a `bulk modulus', although this notion makes no sense for anisotropic solids; we show that it is essentially an arbitrary parameter and that infinitesimal changes to it result in significant changes in the predicted stress response. This is illustrated with numerical simulations for biaxial tension experiments of arteries, where the magnitude of the stress response is found to change by several orders of magnitude when infinitesimal changes in `Poisson's ratio' close to the perfect incompressibility limit of 1/2 are made.

We consider a microscopic field theoretical approach for interacting active nematic particles. With only steric interactions the self-propulsion strength in such systems can lead to different collective behaviour, e.g., synchronized self-spinning and collective translation. The different behaviour results from the delicate interplay between internal nematic structure, particle shape deformation and particle-particle interaction. For intermediate active strength an asymmetric shape emerges and leads to chirality and self-spinning crystals. For larger active strength the shape is symmetric and translational collective motion emerges. Within circular confinements, depending on the packing fraction, the self-spinning regime either stabilizes positional and orientational order or can lead to edge currents and global rotation which destroys the synchronized self-spinning crystalline structure.

Microcapsules are a key class of microscale materials with applications in areas ranging from personal care to biomedicine, and with increasing potential to act as extracellular matrix (ECM) models of hollow organs or tissues. Such capsules are conventionally generated from non-ECM materials including synthetic polymers. Here, we fabricated robust microcapsules with controllable shell thickness from physically- and enzymatically-crosslinked gelatin and achieved a core-shell architecture by exploiting a liquid-liquid phase separated aqueous dispersed phase system in a one-step microfluidic process. Microfluidic mechanical testing revealed that the mechanical robustness of thicker-shell capsules could be controlled through modulation of the shell thickness. Furthermore, the microcapsules demonstrated environmentally-responsive deformation, including buckling by osmosis and external mechanical forces. A sequential release of cargo species was obtained through the degradation of the capsules. Stability measurements showed the capsules were stable at 37 °C for more than two weeks. Finally, all-aqueous liquid-liquid phase separated and multiphase liquid-liquid phase separated systems were generated with the gel-sol transition of microgel precursors. These smart capsules are promising models of hollow biostructures, microscale drug carriers, and building blocks or compartments for active soft materials and robots.

Using a minimal algebraic model for the thermodynamics of binary rod--polymer mixtures, we provide evidence for a quintuple phase equilibrium; an observation that seems to be at odds with the Gibbs phase rule for two-component systems. Our model is based on equations of state for the relevant liquid crystal phases that are in quantitative agreement with computer simulations. We argue that the appearance of a quintuple equilibrium, involving an isotropic fluid, a nematic and smectic liquid crystal, and two solid phases can be reconciled with a generalized Gibbs phase rule in which the two intrinsic length scales of the athermal colloid--polymer mixture act as additional field variables.

This work investigates dense packings of congruent hard infinitesimally--thin circular arcs in the two-dimensional Euclidean space. It focuses on those denotable as major whose subtended angle θ∈(π,2π] . Differently than those denotable as minor whose subtended angle θ∈[0,π] , it is impossible for two hard infinitesimally-thin circular arcs with θ∈(π,2π] to arbitrarily closely approach once they are arranged in a configuration, e.g. on top of one another, replicable ad infinitum without introducing any overlap. This makes these hard concave particles, in spite of being infinitesimally thin, most densely pack with a finite number density. This raises the question as to what are these densest packings and what is the number density that they achieve. Supported by Monte Carlo numerical simulations, this work shows that one can analytically construct compact closed circular groups of hard major circular arcs in which a specific, θ -dependent, number of them (anti-)clockwise intertwine. These compact closed circular groups then arrange on a triangular lattice. These analytically constructed densest-known packings are compared to corresponding results of Monte Carlo numerical simulations to assess whether they can spontaneously turn up.

Suspensions of motile active particles with space dependent activity form characteristic polarization and density patterns. Recent single-particle studies for planar activity landscapes identified several quantities associated with emergent density-polarization patterns, including swim pressure, that are solely determined by bulk variables and thus constitute state functions. We show that for radially symmetric activity steps these variables depend on the curvature of the active-passive interface. In the specific case of total polarization and swim pressure, we generalize this result for arbitrary radially symmetric activity landscapes. Our exact as well as approximate analytical results agree with exact numerical calculations. We expect qualitatively the same results to hold for arbitrarily curved activity landscapes.

Considering the rheology of two-dimensional soft suspensions above the jamming density, we derive a tensorial constitutive model from the microscopic particle dynamics. Starting from the equation governing the N -particle distribution, we derive an evolution equation for the stress tensor. This evolution equation is not closed, as it involves the pair and three-particle correlation functions. To close this equation, we first employ the standard Kirkwood closure relation to express the three-particle correlation function in terms of the pair correlation function. Then we use a simple and physically motivated parametrization of the pair correlation function to obtain a closed evolution equation for the stress tensor. The latter is naturally expressed as separate evolution equations for the pressure and for the deviatoric part of the stress tensor. These evolution equations provide us with a non-linear tensorial constitutive model describing the rheological response of a jammed soft suspension to an arbitrary uniform deformation. One of the advantages of this microscopically-rooted description is that the coefficients appearing in the constitutive model are known in terms of packing fraction and microscopic parameters.

In moderately coupled Yukawa fluids, longitudinal mode dispersion is determined by the competition between kinetic and potential effects. In a recent paper [Khrapak and Couëdel, Phys. Rev. E 102, 033207 (2020)], a semi-phenomenological dispersion relation was constructed by the ad-hoc addition of the Bohm-Gross kinetic term to the generalized instantaneous excess bulk modulus, which showed very good agreement with simulations. In this paper, a nearly identical dispersion relation is derived in a rigorous manner based on a dielectric formulation with static local field corrections. At moderate coupling, this formalism is revealed to be more accurate than other successful theoretical approaches.

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.

The dielectric nature of polar liquids underpins much of their ability to act as useful solvents, but its description is complicated by the long-ranged nature of dipolar interactions. This is particularly pronounced under the periodic boundary conditions commonly used in molecular simulations. In this article, the dielectric properties of a water model whose intermolecular electrostatic interactions are entirely short-ranged are investigated. This is done within the framework of local molecular field theory (LMFT), which provides a well controlled mean-field treatment of long-ranged electrostatics. This short-ranged model gives a remarkably good performance on a number of counts, and its apparent shortcomings are readily accounted for. These results not only lend support to LMFT as an approach for understanding solvation behavior, but are relevant to those developing interaction potentials based on local descriptions of liquid structure.