Physics - Soft Condensed Matter Publications (50)


Physics - Soft Condensed Matter Publications

Microscopy is the workhorse of the physical and life sciences, producing crisp images of everything from atoms to cells well beyond the capabilities of the human eye. However, the analysis of these images is frequently little better than automated manual marking. Here, we revolutionize the analysis of microscopy images, extracting all the information theoretically contained in a complex microscope image. Read More

We investigate the structure of a dilute mixture of amphiphilic dimers and spherical particles, a model relevant to the problem of encapsulating globular "guest" molecules in a dispersion. Dimers and spheres are taken to be hard particles, with an additional attraction between spheres and the smaller monomers in a dimer. Using Monte Carlo simulation, we document the low-temperature formation of aggregates of guests (clusters) held together by dimers, whose typical size and shape depend on the guest concentration $\chi$. Read More

Results of broadband dielectric spectroscopy and rheological studies of poly(propylene glycol) + SiO${_2}$ nanocomposites are presented. They show that the dynamics in high-concentrated composite is determined by confinement and adsorption effects, resulting from interactions of confined polymers correspond with the host system at the interface between PPG and solid nanoparticles. The evolution of relaxation times follows the clear Vogel-Fulcher-Tammann pattern, what is proved by the supplementary activation energy temperature index analysis. Read More

We present the linear rheological instability triggered by the interplay of the shear rheology and Keplerian differential rotation of incompressible dense granular fluids. Instability sets in granular fluids, where the viscosity parameter grows faster than the square of the local shear rate (strain rate) at constant pressure. Found instability can play a crucial role in the formation of observed structures in planetary rings, as well as promote structure formation in protoplanetary disks dense granular material. Read More

We develop an approach to liquid thermodynamics based on collective modes. We perform extensive molecular dynamics simulations of noble, molecular and metallic liquids and provide the direct evidence that liquid energy and specific heat are well-described by the temperature dependence of the Frenkel (hopping) frequency. The agreement between predicted and calculated thermodynamic properties is seen in the notably wide range of temperature spanning tens of thousands of Kelvin. Read More

Using transfer operator and fundamental measure theories, we examine the structural and thermodynamic properties of hard rectangles confined between two parallel hard walls. The side lengths of the rectangle ($L$ and $D$, $L>D$) and the pore width ($H$) are chosen such that maximum two layers are allowed to form in planar order ($L$ is parallel to the wall), while only one in homeotropic order ($D$ is parallel to the wall). We observe three different structures: (i) a low density fluid phase with parallel alignment to the wall, (ii) an intermediate and high density fluid phase with two layers and planar ordering and (iii) a dense single fluid layer with homeotropic ordering. Read More

Magnetic Particle Imaging (MPI) has been shown to provide remarkable contrast for imaging applications such as angiography, stem cell tracking, and cancer imaging. Recently, there is growing interest in the functional imaging capabilities of MPI, where color MPI techniques have explored separating different nanoparticles, which could potentially be used to distinguish nanoparticles in different states or environments. Viscosity mapping is a promising functional imaging application for MPI, as increased viscosity levels in vivo have been associated with numerous diseases such as hypertension, atherosclerosis, and cancer. Read More

Soft particulate media include a wide range of systems involving athermal dissipative particles both in non-living and biological materials. Characterization of flows of particulate media is of great practical and theoretical importance. A fascinating feature of these systems is the existence of a critical rigidity transition in the dense regime dominated by highly intermittent fluctuations that severely affects the flow properties. Read More

Cholesteric liquid crystals experience geometric frustration when they are confined between surfaces with anchoring conditions that are incompatible with the cholesteric twist. Because of this frustration, they develop complex topological defect structures, which may be helicoids or skyrmions. We develop a theory for these structures, which extends previous theoretical research by deriving exact solutions for helicoids with the assumption of constant azimuth, calculating numerical solutions for helicoids and skyrmions with varying azimuth, and interpreting the results in terms of competition between terms in the free energy. Read More

We investigate the capillary force that applies on a tilted cylinder as a function of its dipping angle i, using a home-built tilting Atomic Force Microscope (AFM) with custom made probes. A micrometric-size rod is glued at the end of an AFM cantilever of known stiffness, whose deflection is measured when the cylindrical probe is dipped in and retracted from reference liquids. We show that a torque correction is necessary to understand the measured deflection. Read More

We develop a theoretical description of the critical zipping dynamics of a self-folding polymer. We use tension propagation theory and the formalism of the generalized Langevin equation applied to a polymer that contains two complementary parts which can bind to each other. At the critical temperature, the (un)zipping is unbiased and the two strands open and close as a zipper. Read More

Concentration gradients play a critical role in embryogenesis, bacterial locomotion, as well as the motility of active particles. Particles develop concentration profiles around them by dissolution, adsorption, or the reactivity of surface species. These gradients change the surface energy of the particles, driving both their self-propulsion and governing their interactions. Read More

Affiliations: 1Tablestable Ltd., Switzerland, 2Dipartimento di Fisica e Geologia, Universita' di Perugia, Italy, 3Dipartimento di Fisica e Geologia, Universita' di Perugia, Italy, 4CNR-Istituto Officina dei Materiali, Italy, 5CNR-Istituto Officina dei Materiali, Italy, 6Dipartimento di Chimica Biologia e Biotecnologia, Universita' di Perugia, Italy, 7Dipartimento di Chimica Biologia e Biotecnologia, Universita' di Perugia, Italy, 8Dipartimento di Chimica Biologia e Biotecnologia, Universita' di Perugia, Italy, 9Dipartimento di Chimica Biologia e Biotecnologia, Universita' di Perugia, Italy, 10Dipartimento di Chimica Biologia e Biotecnologia, Universita' di Perugia, Italy, 11Dipartimento di Scienze Farmaceutiche-Sez. Microbiologia, Universita' di Perugia, Italy, 12Dipartimento di Scienze Farmaceutiche-Sez. Microbiologia, Universita' di Perugia, Italy, 13Dipartimento di Scienze Farmaceutiche-Sez. Microbiologia, Universita' di Perugia, Italy, 14University of Exeter, School of Physics and Astronomy, UK, 15Tablestable Ltd., Switzerland, 16Dipartimento di Fisica e Geologia, Universita' di Perugia, Italy

Brillouin and Raman scattering spectroscopy are established techniques for the nondestructive contactless and label-free readout of mechanical, chemical and structural properties of condensed matter. Brillouin-Raman investigations currently require separate measurements and a site-matching approach to obtain complementary information from a sample. Here we demonstrate a new concept of fully scanning multimodal micro-spectroscopy for simultaneous detection of Brillouin and Raman light scattering in an exceptionally wide spectral range, from fractions of GHz to hundreds of THz. Read More

We investigate the mechanical response of thin sheets perforated with a square array of mutually orthogonal cuts, which leaves a network of squares connected by small ligaments. Our combined analytical, experimental and numerical results indicate that under uniaxial tension the ligaments buckle out-of-plane, inducing the formation of 3D patterns whose morphology is controlled by the load direction. We also find that by largely stretching the buckled perforated sheets, plastic strains develop in the ligaments. Read More

We introduce a comprehensive numerical framework to generically infer the emergent macroscopic properties of uniaxial nematic and cholesteric phases from that of their microscopic constituent mesogens. This approach, based on the full numerical resolution of the Poniewierski-Stecki equations in the weak chirality limit, may expediently handle a wide range of particle models through the use of Monte-Carlo sampling for all virial-type integrals. Its predictions in terms of equilibrium cholesteric structures are found to be in excellent agreement with previous full-functional descriptions, thereby demonstrating the quantitative validity of the perturbative treatment of chirality for pitch lengths as short as a few dozen particle diameters. Read More

Density-wave fronts in a vibrofluidized wet granular layer undergoing a gas-liquid-like transition are investigated experimentally. The threshold of the instability is governed by the amplitude of the vertical vibrations. Fronts, which are curved into a spiral shape, propagate coherently along the circular rim of the container with leading edges. Read More

Water radiolysis by low-energy carbon projectiles is studied by first-principles molecular dynamics. Carbon projectiles of kinetic energies between 175 eV and 2.8 keV are shot across liquid water. Read More

We present a theoretical study of the statics and dynamics of a partially wetting liquid droplet, of equilibrium contact angle $\theta_{\rm e}$, confined in a solid wedge geometry of opening angle $\beta$. We focus on a mostly non-wetting regime, given by the condition $\theta_{\rm e} - \beta > 90^\circ$, where the droplet forms a liquid barrel -- a closed shape of positive mean curvature. Using a quasi-equilibrium assumption for the shape of the liquid-gas interface, we compute the surface energy landscapes experienced by the liquid upon translations along the symmetry plane of the wedge. Read More

In order to improve our understanding of landing on small bodies and of asteroid evolution, we use our novel drop tower facility to perform low-velocity (2-40 cm s^-1), shallow impact experiments of a 10 cm diameter aluminum sphere into quartz sand in low effective gravities (~0.2-1 m s^-2). Using in situ accelerometers, we measure the acceleration profile during the impacts and determine the peak accelerations, collision durations and maximum penetration depth. Read More

In kinetic theory, a system is usually described by its one-particle distribution function $f(\mathbf{r},\mathbf{v},t)$, such that $f(\mathbf{r},\mathbf{v},t)d\mathbf{r} d\mathbf{v}$ is the fraction of particles with positions and velocities in the intervals $(\mathbf{r}, \mathbf{r}+d\mathbf{r})$ and $(\mathbf{v}, \mathbf{v}+d\mathbf{v})$, respectively. Therein, global stability and the possible existence of an associated Lyapunov function or $H$-theorem are open problems when non-conservative interactions are present, as in granular fluids. Here, we address this issue in the framework of a lattice model for granular-like velocity fields. Read More

Colloidal Laves phases (LPs) of $MgCu_2$ type are promising precursors for diamond structure photonic materials. They have been predicted for hard sphere binary mixtures, but not yet observed. We here report a time resolved static light scattering study on their formation in a binary mixture of buoyant experimental hard sphere approximants (size ratio $\Gamma=0. Read More

We consider possibility of embedding large sheets of polymer piezoelectrics in clothing for sensing and energy harvesting for wearable electronic applications. Power is generated by the crumpling of clothes due to human body movements. From the mechanics of a gently crumpled foil we develop theoretical models and scaling laws for the open circuit voltage and short circuit current and verify via experiments. Read More

Harnessing a model from composite materials science, we show how point-like cusped surface features arise as quasi-particle excitations, termed "ghost fibers", on the surface of a homogeneous soft elastic material. These deformations appear above a critical compressive strain at which ghost fiber dipoles unbind, analogous to vortices in the Kosterlitz-Thouless transition. Finite-length creases can be described in the same framework. Read More

We perform particle resolved experimental studies on the heterogeneous crystallisation process of two component mixtures of hard spheres. The components have a size ratio of 0.39. Read More

Emerging technologies based on liquid crystal (LC) materials increasingly leverage the presence of nanoscale defects, unlike the canonical application of LCs -- LC displays. The inherent nanoscale characteristics of LC defects present both significant opportunities and barriers for the application of this fascinating class of materials. Simulation-based approaches to the study of the effects of confinement and interface anchoring conditions on LC domains has resulted in significant progress over the past decade, where simulations are now able to access experimentally-relevant micron-scales while simultaneously capturing nanoscale defect structures. Read More

We use molecular simulation to study the structural and dynamic properties of glassy nanoclusters formed both through the direct condensation of the vapor below the glass transition temperature, without the presence of a substrate, and \textit{via} the slow supercooling of unsupported liquid nanodroplets. An analysis of local structure using Voronoi polyhedra shows that the energetic stability of the clusters is characterized by a large, increasing fraction of bicapped square antiprism motifs. We also show that nanoclusters with similar inherent structure energies are structurally similar, independent of their history, which suggests the supercooled clusters access the same low energy regions of the potential energy landscape as the vapor condensed clusters despite their different methods of formation. Read More

Determining the solvation free energies of single ions in water is one of the most fundamental problems in physical chemistry and yet many unresolved questions remain. In particular, the ability to decompose the solvation free energy into simple and intuitive contributions will have important implications for coarse grained models of electrolyte solution. Here, we provide rigorous definitions of the various types of single ion solvation free energies based on different simulation protocols. Read More

A large amplitude oscillatory shear (LAOS) is considered in the strain-controlled regime, and the interrelation between the Fourier transform (FT) and the stress decomposition (SD) approaches is established. Several definitions of the generalized storage and loss moduli are examined in a unified conceptual scheme based on the Lissajous--Bowditch plots. An illustrative example of evaluating the generalized moduli from a LAOS flow is given. Read More

Thin shells are characterized by a high cost of stretching compared to bending. As a result isometries of the midsurface of a shell play a crucial role in their mechanics. In turn, curves with zero normal curvature play a critical role in determining the number and behavior of isometries. Read More

One emerging approach for the fabrication of complex architectures on the nanoscale is to utilize particles customized to intrinsically self-assemble into a desired structure. Inverse methods of statistical mechanics have proven particularly effective for the discovery of interparticle interactions suitable for this aim. Here, we review one such recently introduced inverse design strategy [Lindquist et al. Read More

The reaction ensemble and the constant pH method are well-known chemical equilibrium approaches to simulate protonation and deprotonation reactions in classical molecular dynamics and Monte Carlo simulations. In this article, we show similarity between both methods {under certain conditions}. We perform molecular dynamics simulations of a weak polyelectrolyte in order to compare the titration curves obtained by both approaches. Read More

We present new method for studying the equilibrium properties of interacting fluids in an arbitrary external filed. The method is valid in any dimension and it yields an exact results in one dimension. Using this approach, we derive a recurrence relation for the pair distribution function of a three dimensional in-homogeneous fluids, constitute of spherical molecules with arbitrary nearest neighbour interaction that extends to two molecules diameter. Read More

The cage effect is generally invoked when discussing the delay in the decay of time correlation functions of dense fluids. In an attempt to examine the role of caging more closely we consider the spread of the displacement distributions of Brownian particles. These distributions are necessarily biased by the presence of neighbouring particles. Read More

Ionic solutions are often regarded as fully dissociated ions dispersed in a polar solvent. While this picture holds for dilute solutions, at higher ionic concentrations, oppositely charged ions can associate into dimers, referred to as Bjerrum pairs. We consider the formation of such pairs within the nonlinear Poisson-Boltzmann framework, and investigate their effects on bulk and interfacial properties of electrolytes. Read More

We use molecular dynamic simulations to investigate the relation between the presence of packing defects in a glass-former and the spontaneous cooperative motions called dynamic heterogeneity. For that purpose we use a simple diatomic glass-former and add a small number of larger or smaller diatomic probes. The diluted probes modify locally the packing, inducing structural defects in the liquid, while we find that the number of defects is small enough not to disturb the average structure. Read More

We provide a minimal model for an active nematic film in contact with both a solid substrate and a passive isotropic fluid, and explore its dynamics in one and two dimensions using a combination of hybrid Lattice Boltzmann simulations and analytical calculations. By imposing nematic anchoring at the substrate while active flows induce a preferred alignment at the interface ("active anchoring"), we demonstrate that directed fluid flow spontaneously emerges in cases where the two anchoring types are opposing. In one dimension, our model reduces to an analogue of a loaded elastic column. Read More

Magnetic skyrmions are nanoscale windings of the spin configuration that hold great promise for technology due to their topology-related properties and extremely reduced sizes. After the recent observation at room temperature of sub-100 nm skyrmions stabilized by interfacial chiral interaction in magnetic multilayers, several pending questions remain to be solved, notably about the means to nucleate individual compact skyrmions or the exact nature of their motion. In this study, a method leading to the formation of magnetic skyrmions in a micrometer-sized nanotrack using homogeneous current injection is evidenced. Read More

Core-level spectra of liquids can be difficult to interpret due to the presence of a range of local environments. We present computational methods for investigating core-level spectra based on the idea that both local structural parameters and the X-ray spectra behave as functions of the local atomic configuration around the absorbing site. We identify correlations between structural parameters and spectral intensities in defined regions of interest, using the oxygen K-edge excitation spectrum of liquid water as a test case. Read More

The interaction of solidification fronts with objects such as particles, droplets, cells, or bubbles is a phenomenon with many natural and technological occurrences. For an object facing the front, it may yield various fates, from trapping to rejection, with large implications regarding the solidification pattern. However, whereas most situations involve multiple particles interacting with each other and the front, attention has focused almost exclusively on the interaction of a single, isolated object with the front. Read More

In this note we introduce a hierarchy of phase spaces for static friction, which give a graphical way to systematically quantify the directional dependence in static friction via subregions of the phase spaces. We experimentally plot these subregions to obtain phenomenological descriptions for static friction in various examples where the macroscopic shape of the object affects the frictional response. The phase spaces have the universal property that for any experiment in which a given object is put on a substrate fashioned from a chosen material with a specified nature of contact, the frictional behavior can be read off from a uniquely determined classifying map on the control space of the experiment which takes values in the appropriate phase space. Read More

The mechanical deformability of single cells is an important indicator for various diseases such as cancer, blood diseases and inflammation. Lab-on-a-chip devices allow to separate such cells from healthy cells using hydrodynamic forces. We perform hydrodynamic simulations based on the lattice-Boltzmann method and study the behavior of an elastic capsule in a microfluidic channel flow in the inertial regime. Read More

The interaction between thin structures and incompressible Newtonian fluids is ubiquitous both in nature and in industrial applications. In this paper we present an isogeometric formulation of such problems which exploits a boundary integral formulation of Stokes equations to model the surrounding flow, and a non linear Kirchhoff-Love shell theory to model the elastic behaviour of the structure. We propose three different coupling strategies: a monolithic, fully implicit coupling, a staggered, elasticity driven coupling, and a novel semi-implicit coupling, where the effect of the surrounding flow is incorporated in the non-linear terms of the solid solver through its damping characteristics. Read More

Contact angle is an essential characteristic in wetting, capillarity and moving contact line; however, although contact angle phenomena are effectively simulated, an accurate and real-time measurement for this characteristic has not been well studied in computational fluid dynamics, especially in dynamic environments. Here, we design a geometry-based mesoscopic scheme to onthesport measure the contact angle in the lattice Boltzmann method. The computational results without gravity effect are in excellent agreement with the benchmarks from the spherical cap method. Read More

Inspired by the synchronized beating of cilia, we show that the collective dynamics of hair-like fibers in a meniscus during fast drainage enables their self-organization into multiple topologies including complex shape inversions. By draining liquid from triangular-base hair bundles, we demonstrate their transformations into concave hexagons, rounded triangles, circles and inverted triangles. These topologically distinct shapes are quenched collective mode shapes of the beating hair each corresponding to specific drainage rates of the liquid, and cyclic shape re-transformations can be simply stimulated by repeated immersion and drainage. Read More

We formulate and solve the equations governing the dynamics of a microscopic artificial swimmer composed of a head and of a tail made of a thin film of permanent magnetic material. This is a variant of the model swimmer proposed by Dreyfus et al. in 2005, whose tail is a filament obtained from the assembly of super-paramagnetic beads. Read More

Chemotaxis, a basic and universal phenomenon among living organisms, directly controls the transport kinetics of active fluids such as swarming bacteria, but has not been considered when utilizing passive tracer to probe the nonequilibrium properties of such fluids. Here we present the first theoretical investigation of the diffusion dynamics of a chemoattractant-coated tracer in bacterial suspension, by developing a molecular dynamics model of bacterial chemotaxis. We demonstrate that the non-Gaussian statistics of full-coated tracer arises from the noises exerted by bacteria, which is athermal and exponentially correlated. Read More

Superhydrophobic surfaces (SHSs) have the potential to achieve large drag reduction for internal and external flow applications. However, experiments have shown inconsistent results, with many studies reporting significantly reduced performance. Recently, it has been proposed that surfactants, ubiquitous in flow applications, could be responsible, by creating adverse Marangoni stresses. Read More

It is commonly considered that the frustration between the curvature energy and the chain stretching energy plays an important role in the formation of lyotropic liquid crystals in bicontinuous cubic phases. Theoretic and numeric calculations were performed for two extreme cases: Parallel surfaces eliminate the variance of the chain length; constant mean curvature surfaces eliminate the variance of the mean curvature. We have implemented a model with Brakke's Surface Evolver which allows a competition between the two variances. Read More

The assembly of banana-shaped rodlike proteins on membranes, and the associated membrane shape transformations, are investigated by analytical theory and coarse-grained simulations. The membrane-mediated interactions between two banana-shaped inclusions are derived theoretically using a point-like formalism, both for zero surface tension and for finite surface tension. On a larger scale, the interactions between assemblies of such rodlike inclusions are determined analytically. Read More