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Mixing-induced anisotropic correlations in molecular crystalline systems: We investigate the structure of mixed thin films composed of pentacene (PEN) and diindenoperylene (DIP) using X-ray reflectivity and grazing incidence X-ray diffraction. For equimolar mixtures we observe vanishing in-plane order coexisting with an excellent out-of-plane order, a yet unreported disordering behavior in binary mixtures of organic semiconductors, which are crystalline in their pure form. One approach to rationalize our findings is to introduce an anisotropic interaction parameter in the framework of a mean field model. By comparing the structural properties with those of other mixed systems, we discuss the effects of sterical compatibility and chemical composition on the mixing behavior, which adds to the general understanding of interactions in molecular mixtures.
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Self-replicating segregation patterns in horizontally vibrated binary mixture of granules: When granular mixtures of different sizes are fluidized, each species spontaneously separates and condenses to form patterns. Although granular segregation has been extensively studied, the inability to directly observe the time evolution of the internal structure hinders the understanding of the mechanism of segregation dynamics driven by surface flow. In this study, we report rich band dynamics, including a self-replicating band, in a horizontally shaken granular mixture in a quasi-two-dimensional container where the granules formed steady surface waves. Direct observation of surface flow and segregated internal structure revealed that coupling among segregation, surface flow, and hysteresis in the fluidity of granules is key to understanding complex band dynamics.
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Quantum Field Theory of Treasury Bonds: The Heath-Jarrow-Morton (HJM) formulation of treasury bonds in terms of forward rates is recast as a problem in path integration. The HJM-model is generalized to the case where all the forward rates are allowed to fluctuate independently. The resulting theory is shown to be a two-dimensional Gaussian quantum field theory. The no arbitrage condition is obtained and a functional integral derivation is given for the price of a futures and an options contract.
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Mechanical equilibrium of aggregates of dielectric spheres: Industrial as well as natural aggregation of fine particles is believed to be associated with electrostatics. Yet like charges repel, so it is unclear how similarly treated particles aggregate. To resolve this apparent contradiction, we analyze conditions necessary to hold aggregates together with electrostatic forces. We find that aggregates of particles charged with the same sign can be held together due to dielectric polarization, we evaluate the effect of aggregate size, and we briefly summarize consequences for practical aggregation.
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Towards the description of water adsorption in slit-like nanochannels with grafted molecular brushes. Density functional theory: We have explored a model for adsorption of water into slit-like nanochannels with two walls chemically modified by grafted polymer layers forming brushes. A version of density functional method is used as theoretical tools. The water-like fluid model adopted from the work of Clark et al. [Mol. Phys., 2006, 104, 3561] adequately reproduces the bulk vapour-liquid coexistence envelope. The polymer layer consists of chain molecules in the framework of pearl-necklace model. Each chain molecule is chemically bonded to the pore walls by a single terminating segment. Our principal focus is in the study of the dependence of polymer layer height on grafting density and in the microscopic structure of the interface between adsorbed fluid and brushes. Thermal response of these properties upon adsorption is investigated in detail. The results are of importance to understand shrinking and swelling of the molecular brushes in the nanochannels.
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Analytical classical density functionals from an equation learning network: We explore the feasibility of using machine learning methods to obtain an analytic form of the classical free energy functional for two model fluids, hard rods and Lennard--Jones, in one dimension . The Equation Learning Network proposed in Ref. 1 is suitably modified to construct free energy densities which are functions of a set of weighted densities and which are built from a small number of basis functions with flexible combination rules. This setup considerably enlarges the functional space used in the machine learning optimization as compared to previous work 2 where the functional is limited to a simple polynomial form. As a result, we find a good approximation for the exact hard rod functional and its direct correlation function. For the Lennard--Jones fluid, we let the network learn (i) the full excess free energy functional and (ii) the excess free energy functional related to interparticle attractions. Both functionals show a good agreement with simulated density profiles for thermodynamic parameters inside and outside the training region.
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Nematic-Isotropic Transition with Quenched Disorder: Nematic elastomers do not show the discontinuous, first-order, phase transition that the Landau-De Gennes mean field theory predicts for a quadrupolar ordering in 3D. We attribute this behavior to the presence of network crosslinks, which act as sources of quenched orientational disorder. We show that the addition of weak random anisotropy results in a singular renormalization of the Landau-De Gennes expression, adding an energy term proportional to the inverse quartic power of order parameter Q. This reduces the first-order discontinuity in Q. For sufficiently high disorder strength the jump disappears altogether and the phase transition becomes continuous, in some ways resembling the supercritical transitions in external field.
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Wetting, roughness and hydrodynamic slip: The hydrodynamic slippage at a solid-liquid interface is currently at the center of our understanding of fluid mechanics. For hundreds of years this science has relied upon no-slip boundary conditions at the solid-liquid interface that has been applied successfully to model many macroscopic experiments, and the state of this interface has played a minor role in determining the flow. However, the problem is not that simple and has been revisited recently. Due to the change in the properties of the interface, such as wettability and roughness, this classical boundary condition could be violated, leading to a hydrodynamic slip. In this chapter, we review recent advances in the understanding and expectations for the hydrodynamic boundary conditions in different situations, by focussing mostly on key papers from past decade. We highlight mostly the impact of hydrophobicity, roughness, and especially their combination on the flow properties. In particular, we show that hydrophobic slippage can be dramatically affected by the presence of roughness, by inducing novel hydrodynamic phenomena, such as giant interfacial slip, superfluidity, mixing, and low hydrodynamic drag. Promising directions for further research are also discussed.
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Role of rotational inertia for collective phenomena in active matter: We investigate the effect of rotational inertia on the collective phenomena of underdamped active systems and show that the increase of the moment of inertia of each particle favors non-equilibrium phase coexistence, known as motility induced phase separation, and counteracts its suppression due to translational inertia. Our conclusion is supported by a non-equilibrium phase diagram (in the plane spanned by rotational inertial time and translational inertial time) whose transition line is understood theoretically through scaling arguments. In addition, rotational inertia increases the correlation length of the spatial velocity correlations in the dense cluster. The fact that rotational inertia enhances collective phenomena, such as motility induced phase separation and spatial velocity correlations, is strongly linked to the increase of rotational persistence. Moreover, large moments of inertia induce non-monotonic temporal (cross) correlations between translational and rotational degrees of freedom truly absent in non-equilibrium systems.
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Oscillatory decay of a two-component Bose-Einstein condensate: We study the decay of a two-component Bose-Einstein condensate with negative effective interaction energy. With a decreasing atom number due to losses, the atom-atom interaction becomes less important and the system undergoes a transition from a bistable Josephson regime to the monostable Rabi regime, displaying oscillations in phase and number. We study the equations of motion and derive an analytical expression for the oscillation amplitude. A quantum trajectory simulation reveals that the classical description fails for low emission rates, as expected from analytical considerations. Observation of the proposed effect will provide evidence for negative effective interaction.
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GCIceNet: A Graph Convolutional Network for Accurate Classification of Water Phases: Understanding phases of water molecules based on local structure is essential for understanding their anomalous properties. However, due to complicated structural motifs formed via hydrogen bonds, conventional order parameters represent the water molecules incompletely. In this paper, we develop a GCIceNet, which automatically generates machine-based order parameters for classifying the phases of the water molecules via supervised and unsupervised learning. Multiple graph convolutional layers in the GCIceNet can learn topological informations of the complex hydrogen bond networks. It shows a substantial improvement of accuracy for predicting the phase of water molecules in the bulk system and the ice/vapor interface system. A relative importance analysis shows that the GCIceNet can capture the structural features of the given system hidden in the input data. Augmented with the vast amount of data provided by molecular dynamics simulations, the GCIceNet is expected to serve as a powerful tool for the fields of glassy liquids and hydration layers around biomolecules.
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Sliding droplets of Xanthan solutions: a joint experimental and numerical study: We have investigated the sliding of droplets made of solutions of Xanthan, a stiff rodlike polysaccharide exhibiting a non-newtonian behavior, notably characterized by a shear-rate dependence of the viscosity. These experimental results are quantitatively compared with those of newtonian fluids (water). The impact of the non-newtonian behavior on the sliding process was shown through the relation between the average dimensionless velocity (i.e. the Capillary number) and the dimensionless volume forces (i.e. the Bond number). To this aim, it is needed to define operative strategies to compute the Capillary number for the shear thinning fluids and compare with the corresponding newtonian case. Results from experiments were complemented with lattice Boltzmann numerical simulations of sliding droplets, aimed to disentangle the influence that non-newtonian flow properties have on the sliding.
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An improved integration scheme for Mode-coupling-theory equations: Within the mode-coupling theory (MCT) of the glass transition, we reconsider the numerical schemes to evaluate the MCT functional. Here we propose nonuniform discretizations of the wave number, in contrast to the standard equidistant grid, in order to decrease the number of grid points without losing accuracy. We discuss in detail how the integration scheme on the new grids has to be modified from standard Riemann integration. We benchmark our approach by solving the MCT equations numerically for mono-disperse hard disks and hard spheres and by computing the critical packing fraction and the nonergodicity parameters. Our results show that significant improvements in performance can be obtained by employing a nonuniform grid.
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On the relaxation dynamics of glass-forming systems: Insights from computer simulations: We discuss the relaxation dynamics of a simple lattice gas model for glass-forming systems and show that with increasing density of particles this dynamics slows down very quickly. By monitoring the trajectory of tagged particles we find that their motion is very heterogeneous in space and time, leading to regions in space in which there is a fast dynamics and others in which it is slow. We determine how the geometric properties of these quickly relaxing regions depend on density and time. Motivated by this heterogeneous hopping dynamics, we use a simple model, a variant of a continuous time random walk, to characterize the relaxation dynamics. In particular we find from this model that for large displacements the self part of the van Hove function shows an exponential tail, in agreement with recent findings from experiments and simulations of glass-forming systems.
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Motion of nanodroplets near edges and wedges: Nanodroplets residing near wedges or edges of solid substrates exhibit a disjoining pressure induced dynamics. Our nanoscale hydrodynamic calculations reveal that non-volatile droplets are attracted or repelled from edges or wedges depending on details of the corresponding laterally varying disjoining pressure generated, e.g., by a possible surface coating.
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Effective interaction between star polymers: The distance-resolved effective interaction between two star polymers in a good solvent is calculated by Molecular Dynamics computer simulations. The results are compared with a pair potential proposed recently by Likos et al. [Phys. Rev. Lett. 1998, 80, 4450] which is exponentially decaying for large distances and crosses over, at the corona diameter of the star, to an ultrasoft logarithmic repulsion for small distances. Excellent agreement is found in a broad range of star arm numbers.
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The Föppl-von Kármán equations of elastic plates with initial stress: Initially stressed plates are widely used in modern fabrication techniques, such as additive manufacturing and UV lithography, for their tunable morphology by application of external stimuli. In this work, we propose a formal asymptotic derivation of the F\"{o}ppl-von K\'{a}rm\'{a}n equations for an elastic plate with initial stresses, using the constitutive theory of nonlinear elastic solids with initial stresses under the assumptions of incompressibility and material isotropy. Compared to existing works, our approach allows to determine the morphological transitions of the elastic plate without prescribing the underlying target metric of the unstressed state of the elastic body. We explicitly solve the derived FvK equations in some physical problems of engineering interest, discussing how the initial stress distribution drives the emergence of spontaneous curvatures within the deformed plate. The proposed mathematical framework can be used to tailor shape on demand, with applications in several engineering fields ranging from soft robotics to 4D printing.
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Normal modes analysis of the microscopic dynamics in hard discs: We estimate numerically the normal modes of the free energy in a glass of hard discs. We observe that, near the glass transition or after a rapid quench deep in the glass phase, the density of states (i) is characteristic of a marginally stable structure, in particular it di splays a frequency scale $\omega^*\sim p^{1/2}$, where $p$ is the pressure and (ii) gives a faithful representation of the short-time dyn amics. This brings further evidences that the boson peak near the glass transition corresponds to the relaxation of marginal modes of a we akly-coordinated structure, and implies that the mean square displacement in the glass phase is anomalously large and goes as $< \delta R^2 > \sim p^{-3/2}$, a prediction that we check numerically.
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Local thermal energy as a structural indicator in glasses: Identifying heterogeneous structures in glasses --- such as localized soft spots --- and understanding structure-dynamics relations in these systems remain major scientific challenges. Here we derive an exact expression for the local thermal energy of interacting particles (the mean local potential energy change due to thermal fluctuations) in glassy systems by a systematic low-temperature expansion. We show that the local thermal energy can attain anomalously large values, inversely related to the degree of softness of localized structures in a glass, determined by a coupling between internal stresses --- an intrinsic signature of glassy frustration ---, anharmonicity and low-frequency vibrational modes. These anomalously large values follow a fat-tailed distribution, with a universal exponent related to the recently observed universal $\omega^4$ density of states of quasi-localized low-frequency vibrational modes. When the spatial thermal energy field --- a `softness field' --- is considered, this power-law tail manifests itself by highly localized spots which are significantly softer than their surroundings. These soft spots are shown to be susceptible to plastic rearrangements under external driving forces, having predictive powers that surpass those of the normal-modes-based approach. These results offer a general, system/model-independent, physical-observable-based approach to identify structural properties of quiescent glasses and to relate them to glassy dynamics.
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Symmetry breaking and coarsening of clusters in a prototypical driven granular gas: Granular hydrodynamics predicts symmetry-breaking instability in a two-dimensional (2D) ensemble of nearly elastically colliding smooth hard spheres driven, at zero gravity, by a rapidly vibrating sidewall. Super- and subcritical symmetry-breaking bifurcations of the simple clustered state are identified, and the supercritical bifurcation curve is computed. The cluster dynamics proceed as a coarsening process mediated by the gas phase. Far above the bifurcation point the final steady state, selected by coarsening, represents a single strongly localized densely packed 2D cluster.
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Drop dynamics on Liquid Infused Surfaces: The Role of the Wetting Ridge: We employ a free energy lattice Boltzmann method to study the dynamics of a ternary fluid system consisting of a liquid drop driven by a body force across a regularly textured substrate, infused by a lubricating liquid. We focus on the case of partial wetting lubricants and observe a rich interplay between contact line pinning and viscous dissipation at the lubricant ridge, which become dominant at large and small apparent angles respectively. Our numerical investigations further demonstrate that the relative importance of viscous dissipation at the lubricant ridge depends on the drop to lubricant viscosity ratio, as well as on the shape of the wetting ridge.
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Self-propelled particle in a nonconvex external potential: Persistent limit in one dimension: Equilibrium mapping techniques for nonaligning self-propelled particles have made it possible to predict the density profile of an active ideal gas in a wide variety of external potentials, however they fail when the self-propulsion is very persistent and the potential is nonconvex, which is precisely when the most uniquely active phenomena occur. Here we show how to predict the density profile of a 1D active Ornstein-Uhlenbeck particle in an arbitrary external potential in the persistent limit and discuss the consequences of the potential's nonconvexity on the structure of the solution, including the central role of the potential's inflection points and the nonlocal dependence of the density profile on the potential.
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Impact of boundaries on velocity profiles in bubble rafts: Under conditions of sufficiently slow flow, foams, colloids, granular matter, and various pastes have been observed to exhibit shear localization, i.e. regions of flow coexisting with regions of solid-like behavior. The details of such shear localization can vary depending on the system being studied. A number of the systems of interest are confined so as to be quasi-two dimensional, and an important issue in these systems is the role of the confining boundaries. For foams, three basic systems have been studied with very different boundary conditions: Hele-Shaw cells (bubbles confined between two solid plates); bubble rafts (a single layer of bubbles freely floating on a surface of water); and confined bubble rafts (bubbles confined between the surface of water below and a glass plate on top). Often, it is assumed that the impact of the boundaries is not significant in the ``quasi-static limit'', i.e. when externally imposed rates of strain are sufficiently smaller than internal kinematic relaxation times. In this paper, we directly test this assumption for rates of strain ranging from $10^{-3}$ to $10^{-2} {\rm s^{-1}}$. This corresponds to the quoted quasi-static limit in a number of previous experiments. It is found that the top plate dramatically alters both the velocity profile and the distribution of nonlinear rearrangements, even at these slow rates of strain.
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Generalized Einstein's and Brinkman's solutions for the effective viscosity of nanofluids: In this paper, we derive the closed form analytical solutions for the effective viscosity of the suspensions of solid spheres that take into account the size effects. This result is obtained using the solution for the effective shear modulus of particulate composites developed in the framework of the strain gradient elasticity theory. Assuming incompressibility of matrix and rigid behavior of particles and using a mathematical analogy between the theory of elasticity and the theory of viscous fluids we derive the generalized Einstein's formula for the effective viscosity. Generalized Brinkman's solution for the concentrated suspensions is derived then using differential method. Obtained solutions contain single additional length scale parameter, which can be related to the interactions between base liquid and solid particles in the suspensions. In the case of the large ratio the between diameter of particles and the length scale parameter, developed solutions reduce to the classical solutions, however for the small relative diameter of particles an increase of the effective viscosity is predicted. It is shown that developed models agree well with known experimental data. Solutions for the fibrous suspensions are also derived and validated.
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Emergent Stereoselective Interactions and Self-recognition in Polar Chiral Active Ellipsoids: In many active matter systems, particle trajectories have a well-defined handedness or chirality. Whether such chiral activity can introduce stereoselective interactions between particles is not known. Here we developed a strategy to tune the nature of chiral activity of 3D-printed granular ellipsoids without altering their shape or size. In vertically agitated monolayers of these particles, we observed two types of dimers form depending on the chirality of the pairing monomers. Heterochiral dimers moved collectively as a single achiral active unit, while homochiral ones formed a translationally immobile spinner. In active racemic mixtures, the former was more abundant than the latter indicating stereoselectivity. Through dimer lifetime measurements, we provide compelling evidence for chiral self-recognition in mixtures of particles with different chiral activities. We finally show that changing only the net chirality of a dense active liquid from a racemic mixture to an enantiopure liquid fundamentally alters its nature of collective relaxation.
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Universal origin of boson peak vibrational anomalies in ordered crystals and in amorphous materials: The vibrational spectra of solids, both ordered and amorphous, in the low-energy regime, control the thermal and transport properties of materials, from heat capacity to heat conduction, electron-phonon couplings, conventional superconductivity etc. The old Debye model of vibrational spectra at low energy gives the vibrational density of states (VDOS) as proportional to the frequency squared, but in many materials the spectrum departs from this law which results in a peak upon normalizing the VDOS by frequency squared, which is known as the "boson peak". A description of the VDOS of solids (both crystals and glasses) is presented starting from first principles. Without using any assumptions whatsoever about the existence and nature of "disorder" in the material, it is shown that the boson peak in the VDOS of both ordered crystals and glasses arises naturally from the competition between elastic mode propagation and viscous damping. The theory explains the recent experimental observations of boson peak in perfectly ordered crystals, which cannot be explained based on previous theoretical frameworks. The theory also explains, for the first time, how the vibrational spectrum changes with the atomic density of the solid, and explains recent experimental observations of this effect.
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Effective pair interactions between colloidal particles at a nematic-isotropic interface: The Landau-de Gennes free energy is used to study theoretically the interaction of parallel cylindrical colloidal particles trapped at a nematic-isotropic interface. We find that the effective interaction potential is non-monotonic. The corresponding force-distance curves exhibit jumps and hysteresis upon approach/separation due to the creation/annihilation of topological defects. Minimization results suggest a simple empirical pair potential for the effective colloid-colloid interaction at the interface. We propose that the interface-mediated interaction can play an important role in self-organization and clustering of colloidal particles at such interfaces.
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Polymer Glass Formation: Role of Activation Free Energy, Configurational Entropy, and Collective Motion: We provide a perspective on polymer glass formation, with an emphasis on models in which the fluid entropy and collective particle motion dominate the theoretical description and data analysis. We first discuss the dynamics of liquids in the high temperature Arrhenius regime, where transition state theory is formally applicable. We then summarize the evolution of the entropy theory from a qualitative framework for organizing and interpreting temperature-dependent viscosity data by Kauzmann to the formulation of a hypothetical `ideal thermodynamic glass transition' by Gibbs and DiMarzio, followed by seminal measurements linking entropy and relaxation by Bestul and Chang and the Adam-Gibbs (AG) model of glass formation rationalizing the observations of Bestul and Chang. These developments laid the groundwork for the generalized entropy theory (GET), which merges an improved lattice model of polymer thermodynamics accounting for molecular structural details and enabling the analytic calculation of the configurational entropy with the AG model, giving rise to a highly predictive model of the segmental structural relaxation time of polymeric glass-forming liquids. The development of the GET has occurred in parallel with the string model of glass formation in which concrete realizations of the cooperatively rearranging regions are identified and quantified for a wide range of polymeric and other glass-forming materials. The string model has shown that many of the assumptions of AG are well supported by simulations, while others are certainly not, giving rise to an entropy theory of glass formation that is largely in accord with the GET. As the GET and string models continue to be refined, these models progressively grow into a more unified framework, and this Perspective reviews the present status of development of this promising approach to the dynamics of polymeric glass-forming liquids.
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Non-Newtonian viscosity of E-coli suspensions: The viscosity of an active suspension of E-Coli bacteria is determined experimentally in the dilute and semi dilute regime using a Y shaped micro-fluidic channel. From the position of the interface between the pure suspending fluid and the suspension, we identify rheo-thickening and rheo-thinning regimes as well as situations at low shear rate where the viscosity of the bacteria suspension can be lower than the viscosity of the suspending fluid. In addition, bacteria concentration and velocity profiles in the bulk are directly measured in the micro-channel.
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Extraterrestrial sink dynamics in granular matter: A loosely packed bed of sand sits precariously on the fence between mechanically stable and flowing states. This has especially strong implications for animals or vehicles needing to navigate sandy environments, which can sink and become stuck in a "dry quicksand" if their weight exceeds the yield stress of this fragile matter. While it is known that the contact stresses in these systems are loaded by gravity, very little is known about the sinking dynamics of objects into loose granular systems under gravitational accelerations different from the Earth's (g). A fundamental understanding of how objects sink in different gravitational environments is not only necessary for successful planetary navigation and engineering, but it can also improve our understanding of celestial impact dynamics and crater geomorphology. Here we perform and explain the first systematic experiments of the sink dynamics of objects into granular media in different gravitational accelerations. By using an accelerating experimental apparatus, we explore gravitational conditions ranging from 0.4g to 1.2g. With the aid of discrete element modeling simulations, we reproduce these results and extend this range to include objects as small as asteroids and as large as Jupiter. Surprisingly, we find that the final sink depth is independent of the gravitational acceleration, an observation with immediate relevance to the design of future extraterrestrial structures land-roving spacecraft. Using a phenomenological equation of motion that includes a gravity-loaded frictional term, we are able to quantitatively explain the experimental and simulation results.
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Holographic interferometry study of the dissolution and diffusion of gypsum in water: We have performed holographic interferometry measurements of the dissolution of the (010) plane of a cleaved gypsum single crystal in pure water. These experiments have provided the value of the dissolution rate constant k of gypsum in water and the value of the interdiffusion coefficient D of its aqueous species in water. D is 1.0 x 10^-9 m2 s^-1, a value close to the theoretical value generally used in dissolution studies. k is 4 x 10^-5 mol m^-2 s^-1. It directly characterizes the microscopic transfer rate at the solid-liquid interface, and is not an averaged value deduced from quantities measured far from the surface as in macroscopic dissolution experiments. It is found to be two times lower than the value obtained from macroscopic experiments.
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Heat Transfer between Graphene and Amorphous SiO2: We study the heat transfer between graphene and amorphous SiO2. We include both the heat transfer from the area of real contact, and between the surfaces in the non-contact region. We consider the radiative heat transfer associated with the evanescent electromagnetic waves which exist outside of all bodies, and the heat transfer by the gas in the non-contact region. We find that the dominant contribution to the heat transfer result from the area of real contact, and the calculated value of the heat transfer coefficient is in good agreement with the value deduced from experimental data.
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Scaling theory for the jamming transition: We propose a scaling ansatz for the elastic energy of a system near the critical jamming transition in terms of three relevant fields: the compressive strain $\Delta \phi$ relative to the critical jammed state, the shear strain $\epsilon$, and the inverse system size $1/N$. We also use $\Delta Z$, the number of contacts relative to the minimum required at jamming, as an underlying control parameter. Our scaling theory predicts new exponents, exponent equalities and scaling collapses for energy, pressure and shear stress that we verify with numerical simulations of jammed packings of soft spheres. It also yields new insight into why the shear and bulk moduli exhibit different scalings; the difference arises because the shear stress vanishes as $1/\sqrt{N}$ while the pressure approaches a constant in the thermodynamic limit. The success of the scaling ansatz implies that the jamming transition exhibits an emergent scale invariance, and that it should be possible to develop a renormalization-group theory for jamming.
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Active Motion of Janus Particle by Self-thermophoresis in Defocused Laser Beam: We study self-propulsion of a half-metal coated colloidal particle under laser irradiation. The motion is caused by self-thermophoresis: i.e. absorption of laser at the metal-coated side of the particle creates local temperature gradient which in turn drives the particle by thermophoresis. To clarify the mechanism, temperature distribution and a thermal slip flow field around a micro-scale Janus particle are measured for the first time. With measured temperature drop across the particle, the speed of self-propulsion is corroborated with the prediction based on accessible parameters. As an application for driving micro-machine, a micro-rotor heat engine is demonstrated.
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Minimal Surfaces, Screw Dislocations and Twist Grain Boundaries: Large twist-angle grain boundaries in layered structures are often described by Scherk's first surface whereas small twist-angle grain boundaries are usually described in terms of an array of screw dislocations. We show that there is no essential distinction between these two descriptions and that, in particular, their comparative energetics depends crucially on the core structure of their screw-dislocation topological defects.
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Phase nucleation in curved space: Nucleation and growth is the dominant relaxation mechanism driving first order phase transitions. In two-dimensional at systems nucleation has been applied to a wide range of problems in physics, chemistry and biology. Here we study nucleation and growth of two-dimensional phases lying on curved surfaces and show that curvature modify both, critical sizes of nuclei and paths towards the equilibrium phase. In curved space nucleation and growth becomes inherently inhomogeneous and critical nuclei form faster on regions of positive Gaussian curvature. Substrates of varying shape display complex energy landscapes with several geometry-induced local minima, where initially propagating nuclei become stabilized and trapped by the underlying curvature.
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Relaxation dynamics of functionalized colloids on attractive substrates: Particle-based simulations are performed to study the post-relaxation dynamics of functionalized (patchy) colloids adsorbed on an attractive substrate. Kinetically arrested structures that depend on the number of adsorbed particles and the strength of the particle-particle and particle-substrate interactions are identified. The radial distribution function is characterized by a sequence of peaks, with relative intensities that depend on the number of adsorbed particles. The first-layer coverage is a non-monotonic function of the number of particles, with an optimal value around one layer of adsorbed particles. The initial relaxation towards these structures is characterized by a fast (exponential) and a slow (power-law) dynamics. The fast relaxation timescale is a linearly increasing function of the number of adsorbed particles in the submonolayer regime, but it saturates for more than one adsorbed layer. The slow dynamics exhibits two characteristic exponents, depending on the surface coverage.
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Effects of strongly selective additives on volume phase transition in gels: We investigate volume phase transition in gels immersed in mixture solvents, on the basis of a three-component Flory-Rehner theory. When the selectivity of the minority solvent component to the polymer network is strong, the gel tends to shrink with an increasing concentration of the additive, regardless of whether it is good or poor. This behavior originates from the difference of the additive concentration between inside and outside the gel. We also found the gap of the gel volume at the transition point can be controlled by adding the strongly selective solutes. By dissolving a strongly poor additive, for instance, the discontinuous volume phase transition can be extinguished. Furthermore, we observed that another volume phase trasition occurs far from the original transition point. These behaviors can be well explained by a simplified theory neglecting the non-linearity of the additive concentration.
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Nanofluidic logic with mechano-ionic memristive switches: While most neuromorphic systems are based on nanoscale electronic devices, nature relies on ions for energy-efficient information processing. Therefore, finding memristive nanofluidic devices is a milestone toward realizing electrolytic computers mimicking the brain down to its basic principles of operation. Here, we present a nanofluidic device designed for circuit scale in-memory processing that combines single-digit nanometric confinement and large entrance asymmetry. Our fabrication process is scalable while the device operates at the second timescale with a conductance ratio in the range 10-60. In-operando optical microscopy unveils the origin of memory, arising from the reversible formation of liquid blisters modulating the device conductance. The combination of features of these mechano-ionic memristive switches permits assembling logic circuits composed of two interactive devices and an ohmic resistor. These results open the way to design multi-component ionic machinery, such as nanofluidic neural networks, and implementing brain-inspired ionic computations.
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Surface patterns in drying films of silica colloidal dispersions: We report an experimental study on the drying of silica colloidal dispersions. Here we focus on a surface instability occurring in a drying paste phase before crack formation which affects the final film quality. Observations at macroscopic and microscopic scales reveal the occurrence of the instability, and the morphology of the film surface. Furthermore, we show that the addition of adsorbing polymers on silica particles can be used to suppress the instability under particular conditions of molecular weight and concentration. We relate this suppression to the increase of the paste elastic modulus.
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Higher-order moment theories for dilute granular gases of smooth hard-spheres: Grad's method of moments is employed to develop higher-order Grad's moment equations---up to first 26-moments---for granular gases within the framework of the (inelastic) Boltzmann equation. The homogeneous cooling state of a freely cooling granular gas is investigated with the Grad's 26-moment equations in a semi-linearized setting and it is shown that the granular temperature in the homogeneous cooling state still decays according to Haff's law while the other higher-order moments decay on a faster time scale. The constitutive relations for stress and heat flux (the Navier--Stokes and Fourier relations) are obtained by performing a Chapman--Enskog-like expansion on the Grad's 26-moment equations and compared with those existing in the literature. The linear stability of the homogeneous cooling state is analyzed through the Grad's 26-moment system and various sub-systems by decomposing them into longitudinal and transverse systems. It is found that one eigenmode in both longitudinal and transverse systems in case of inelastic gases is unstable. By comparing the eigenmodes from various theories, it is established that the 13-moment eigenmode theory predicts that the unstable eigenmode remains unstable for all wavenumbers below a certain coefficient of restitution while any other higher-order moment theory shows that this mode becomes stable above some critical wavenumber for all values of coefficient of restitution. In particular, the Grad's 26-moment theory leads to a smooth profile for the critical wavenumber in contrast to the other considered theories. Furthermore, the critical system size obtained through the Grad 26-moment and existing theories are also in excellent agreement.
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Coordinated Stress-Structure Self-Organization in Granular Packing: It is accepted that stress and structure self-organize cooperatively during quasi-static dynamics of granular systems, but the consequences of this self-organization are not fully understood. Such an understanding is essential because local structural properties of the settled material are then correlated with the local stress, which calls into question existing linear theories of stress transmission in granular media. A method to quantify the local stress-structure correlations is necessary for addressing this issue and we present here such a method for planar systems. We then use it to analyze numerically several different systems, compressed quasi-statically by two different procedures. We define cells, cell orders, cell orientations, and cell stresses and report the following. 1. The mean ratio of cell principal stresses decreases with cell order and increases with friction. 2. The ratio distributions collapse onto a single curve under a simple scaling, for all packing protocols and friction coefficients. 3. Cells orient along the local stress major principal axes. 4. A simple first-principles model explains the correlations between the local cell and stress principal axis orientations. Our results quantify the cooperative stress-structure self-organization and provide a way to relate quantitatively the stress-structure coupling to different process parameters and particle characteristics. Significantly, the strong stress-structure correlation, driven by structural re-organization upon application of external stress, suggests that current stress theories of granular matter need to be revisited.
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Bogoliubov approach to superfluidity of atoms in an optical lattice: We use the Bogoliubov theory of atoms in an optical lattice to study the approach to the Mott-insulator transition. We derive an explicit expression for the superfluid density based on the rigidity of the system under phase variations. This enables us to explore the connection between the quantum depletion of the condensate and the quasi-momentum distribution on the one hand and the superfluid fraction on the other. The approach to the insulator phase may be characterized through the filling of the band by quantum depletion, which should be directly observable via the matter wave interference patterns. We complement these findings by self-consistent Hartree-Fock-Bogoliubov-Popov calculations for one-dimensional lattices including the effects of a parabolic trapping potential.
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Stability and interactions of nanocolloids at fluid interfaces: effects of capillary waves and line tensions: We analyze the effective potential for nanoparticles trapped at a fluid interface within a simple model which incorporates surface and line tensions as well as a thermal average over interface fluctuations (capillary waves). For a single colloid, a reduced steepness of the potential well hindering movements out of the interface plane compared to rigid interface models is observed, and an instability of the capillary wave partition sum in case of negative line tensions is pointed out. For two colloids, averaging over the capillary waves leads to an effective Casimir--type interaction which is long--ranged, power-like in the inverse distance but whose power sensitively depends on possible restrictions of the colloid degress of freedom. A nonzero line tension leads to changes in the magnitude but not in the functional form of the effective potential asymptotics.
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Reversible magnetomechanical collapse: virtual touching and detachment of rigid inclusions in a soft elastic matrix: Soft elastic composite materials containing particulate rigid inclusions in a soft elastic matrix are candidates for developing soft actuators or tunable damping devices. The possibility to reversibly drive the rigid inclusions within such a composite together to a close-to-touching state by an external stimulus would offer important benefits. Then, a significant tuning of the mechanical properties could be achieved due to the resulting mechanical hardening. For a long time, it has been argued whether a virtual touching of the embedded magnetic particles with subsequent detachment can actually be observed in real materials, and if so, whether the process is reversible. Here, we present experimental results that demonstrate this phenomenon in reality. Our system consists of two paramagnetic nickel particles embedded at finite initial distance in a soft elastic polymeric gel matrix. Magnetization in an external magnetic field tunes the magnetic attraction between the particles and drives the process. We quantify the scenario by different theoretical tools, i.e., explicit analytical calculations in the framework of linear elasticity theory, a projection onto simplified dipole-spring models, as well as detailed finite-element simulations. From these different approaches, we conclude that in our case the cycle of virtual touching and detachment shows hysteretic behavior due to the mutual magnetization between the paramagnetic particles. Our results are important for the design and construction of reversibly tunable mechanical damping devices. Moreover, our projection on dipole-spring models allows the formal connection of our description to various related systems, e.g., magnetosome filaments in magnetotactic bacteria.
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Scaling regimes for wormlike chains confined to cylindrical surfaces under tension: We compute the free energy of confinement ${\cal{F}}$ for a wormlike chain (WLC), with persistence length $l_p$, that is confined to the surface of a cylinder of radius $R$ under an external tension $f$ using a mean field variational approach. For long chains, we analytically determine the behavior of the chain in a variety of regimes, which are demarcated by the interplay of $l_p$, the Odijk deflection length ($l_d=(R^2l_p)^{1/3}$), and the Pincus length ($l_f = {k_BT}/{f}$, with $k_BT$ being the thermal energy). The theory accurately reproduces the Odijk scaling for strongly confined chains at $f=0$, with ${\cal{F}}\sim Ll_p^{-1/3}R^{-2/3}$. For moderate values of $f$, the Odijk scaling is discernible only when ${l_p}\gg R$ for strongly confined chains. Confinement does not significantly alter the scaling of the mean extension for sufficiently high tension. The theory is used to estimate unwrapping forces for DNA from nucleosomes.
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Improved general-purpose five-point model for water: TIP5P/2018: A new five point potential for liquid water, TIP5P/2018, is presented along with the techniques used to derive its charges from ab initio per-molecule electrostatic potentials in the liquid phase using the split charge equilibration (SQE) of Nistor et al. [J. Chem. Phys. 125, 094108 (2006)]. By taking the density and diffusion dependence on temperature as target properties, significant improvements to the behavior of isothermal compressibility were achieved along with improvements to other thermodynamic and rotational properties. While exhibiting a dipole moment close to ab initio values, TIP5P/2018 suffers from a too small quadrupole moment due to the charge assignment procedure and results in an overestimation of the dielectric constant.
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Analysis of the shape of x-ray diffraction peaks originating from the hexatic phase of liquid crystal films: X-ray diffraction studies of the bond-orientational order in the hexatic-B phase of 75OBC and 3(10)OBC compounds are presented. The temperature evolution of an angular profile of a single diffraction peak is analyzed. Close to the hexatic-B-smectic-A transition these profiles can be approximated by the Gaussian function. At lower temperatures in the hexatic-B phase the profiles are better fitted by the Voigt function. Theoretical analysis of the width of diffraction peaks in three-dimentional (3D) hexatics is performed on the basis of the effective Hamiltonian introduced by Aharony and Kardar. Theoretical estimations are in good agreement with the results of x-ray experiments.
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Microscopic Description of Entanglements in Polyethylene Networks and Melts: Strong, Weak, Pairwise, and Collective Attributes: We present atomistic molecular dynamics simulations of two Polyethylene systems where all entanglements are trapped: a perfect network, and a melt with grafted chain ends. We examine microscopically at what level topological constraints can be considered as a collective entanglement effect, as in tube model theories, or as certain pairwise uncrossability interactions, as in slip-link models. A pairwise parameter, which varies between these limiting cases, shows that, for the systems studied, the character of the entanglement environment is more pairwise than collective. We employ a novel methodology, which analyzes entanglement constraints into a complete set of pairwise interactions, similar to slip links. Entanglement confinement is assembled by a plethora of links, with a spectrum of confinement strengths, from strong to weak. The strength of interactions is quantified through a link `persistence', which is the fraction of time for which the links are active. By weighting links according to their strength, we show that confinement is imposed mainly by the strong ones, and that the weak, trapped, uncrossability interactions cannot contribute to the low frequency modulus of an elastomer, or the plateau modulus of a melt. A self-consistent scheme for mapping topological constraints to specific, strong binary links, according to a given entanglement density, is proposed and validated. Our results demonstrate that slip links can be viewed as the strongest pairwise interactions of a collective entanglement environment. The methodology developed provides a basis for bridging the gap between atomistic simulations and mesoscopic slip link models.
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Mechanics of invagination and folding: hybridized instabilities when one soft tissue grows on another: We address the folding induced by differential growth in soft layered solids via an elementary model that consists of a soft growing neo-Hookean elastic layer adhered to a deep elastic substrate. As the layer/substrate modulus ratio is varied from above unity towards zero we find a first transition from supercritical smooth folding followed by cusping of the valleys to direct subcritical cusped folding, then another to supercritical cusped folding. Beyond threshold the high amplitude fold spacing converges to about four layer thicknesses for many modulus ratios. In three dimensions the instability gives rise to a wide variety of morphologies, including almost degenerate zigzag and triple-junction patterns that can coexist when the layer and substrate are of comparable softness. Our study unifies these results providing understanding for the complex and diverse fold morphologies found in biology, including the zigzag precursors to intestinal villi, and disordered zigzags and triple-junctions in mammalian cortex.
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Creation of a monopole in a spinor condensate: We propose a method to create a monopole structure in a spin-1 spinor condensate by applying the basic methods used to create vortices and solitons experimentally in single-component condensates. We show, however, that by using a two-component structure for a monopole, we can simplify our proposed experimental approach and apply it also to ferromagnetic spinor condensates. We also discuss the observation and dynamics of such a monopole structure, and note that the dynamics of the two-component monopole differs from the dynamics of the three-component monopole.
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Snapping Mechanical Metamaterials under Tension: We present a monolithic mechanical metamaterial comprising a periodic arrangement of snapping units with tunable tensile behavior. Under tension, the metamaterial undergoes a large extension caused by sequential snap-through instabilities, and exhibits a pattern switch from an undeformed wavy-shape to a diamond configuration. By means of experiments performed on 3D printed prototypes, numerical simulations and theoretical modeling, we demonstrate how the snapping architecture can be tuned to generate a range of nonlinear mechanical responses including monotonic, S-shaped, plateau and non-monotonic snap-through behavior. This work contributes to the development of design strategies that allow programming nonlinear mechanical responses in solids.
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Insights into DNA-mediated interparticle interactions from a coarse-grained model: DNA-functionalized particles have great potential for the design of complex self-assembled materials. The major hurdle in realizing crystal structures from DNA-functionalized particles is expected to be kinetic barriers that trap the system in metastable amorphous states. Therefore, it is vital to explore the molecular details of particle assembly processes in order to understand the underlying mechanisms. Molecular simulations based on coarse-grained models can provide a convenient route to explore these details. Most of the currently available coarse-grained models of DNA-functionalized particles ignore key chemical and structural details of DNA behavior. These models therefore are limited in scope for studying experimental phenomena. In this paper, we present a new coarse-grained model of DNA-functionalized particles which incorporates some of the desired features of DNA behavior. The coarse-grained DNA model used here provides explicit DNA representation (at the nucleotide level) and complementary interactions between Watson-Crick base pairs, which lead to the formation of single-stranded hairpin and double-stranded DNA. Aggregation between multiple complementary strands is also prevented in our model. We study interactions between two DNA- functionalized particles as a function of DNA grafting density, lengths of the hybridizing and non-hybridizing parts of DNA, and temperature. The calculated free energies as a function of pair distance between particles qualitatively resemble experimental measurements of DNA-mediated pair interactions.
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Salt-induced reentrant stability of polyion-decorated particles with tunable surface charge density: The electrostatic complexation between DOTAP-DOPC unilamellar liposomes and an oppositely charged polyelectrolyte (NaPA) has been investigated in a wide range of the liposome surface charge density. We systematically characterized the "reentrant condensation" and the charge inversion of polyelectrolyte-decorated liposomes by means of dynamic light scattering and electrophoresis. We explored the stability of this model polyelectrolyte/colloid system by fixing each time the charge of the bare liposomes and by changing two independent control parameters of the suspensions: the polyelectrolyte/colloid charge ratio and the ionic strength of the aqueous suspending medium. The progressive addition of neutral DOPC lipid within the liposome membrane gave rise to a new intriguing phenomenon: the stability diagram of the suspensions showed a novel reentrance due to the crossing of the desorption threshold of the polyelectrolyte. Indeed, at fixed charge density of the bare DOTAP/DOPC liposomes and for a wide range of polyion concentrations, we showed that the simple electrolyte addition first (low salt regime) destabilizes the suspensions because of the enhanced screening of the residual repulsion between the complexes, and then (high salt regime) determines the onset of a new stable phase, originated by the absence of polyelectrolyte adsorption on the particle surfaces. We show that the observed phenomenology can be rationalized within the Velegol-Thwar model for heterogeneously charged particles and that the polyelectrolyte desorption fits well the predictions of the adsorption theory of Winkler and Cherstvy. Our findings unambiguously support the picture of the reentrant condensation as driven by the correlated adsorption of the polyelectrolyte chains on the particle surface, providing interesting insights into possible mechanisms for tailoring complex colloids via salt-induced effects.
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Topological vortex formation in a Bose-Einstein condensate: Vortices were imprinted in a Bose-Einstein condensate using topological phases. Sodium condensates held in a Ioffe-Pritchard magnetic trap were transformed from a non-rotating state to one with quantized circulation by adiabatically inverting the magnetic bias field along the trap axis. Using surface wave spectroscopy, the axial angular momentum per particle of the vortex states was found to be consistent with $2\hbar$ or $4\hbar$, depending on the hyperfine state of the condensate.
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Mutual diffusion of inclusions in freely-suspended smectic liquid crystal films: We study experimentally and theoretically the hydrodynamic interaction of pairs of circular inclusions in two-dimensional, fluid smectic membranes suspended in air. By analyzing their Brownian motion, we find that the radial mutual mobilities of identical inclusions are independent of their size but that the angular coupling becomes strongly size-dependent when their radius exceeds a characteristic hydrodynamic length. The observed dependence of the mutual mobilities on inclusion size is described well for arbitrary separations by a model that generalizes the Levine/MacKintosh theory of point-force response functions and uses a boundary-element approach to calculate the mobility matrix.
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Transient deformation of a droplet near a microfluidic constriction : a quantitative analysis: We report on experiments that consist in deforming a collection of monodisperse droplets produced by a microfluidic chip through a flow-focusing device. We show that a proper numerical modelling of the flow is necessary to access the stress applied by the latter on the droplet along its trajectory through the chip. This crucial step enables the full integration of the differential equation governing the dynamical deformation, and consequently the robust measurement of the interfacial tension by fitting the experiments with the calculated deformation. Our study thus demonstrates the feasibility of quantitative in-situ rheology in microfluidic flows involving e.g. droplets, capsules or cells.
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How do ionic superdiscs self-assemble in nanopores?: Discotic ionic liquid crystals (DILCs) consist of self-assembled superdiscs of cations and anions that spontaneously stack in linear columns with high one-dimensional ionic and electronic charge mobility, making them prominent model systems for functional soft matter. Unfortunately, a homogeneous alignment of DILCs on the macroscale is often not achievable, which significantly limits their applicability. Infiltration into nanoporous solid scaffolds can in principle overcome this drawback. However, due to the extreme experimental challenges to scrutinise liquid crystalline order in extreme spatial confinement, little is known about the structures of DILCs in nanopores. Here, we present temperature-dependent high-resolution optical birefringence measurement and 3D reciprocal space mapping based on synchrotron-based X-ray scattering to investigate the thermotropic phase behaviour of dopamine-based ionic liquid crystals confined in cylindrical channels of 180~nm diameter in macroscopic anodic aluminum oxide (AAO) membranes. As a function of the membranes' hydrophilicity and thus the molecular anchoring to the pore walls (edge-on or face-on) and the variation of the hydrophilic-hydrophobic balance between the aromatic cores and the alkyl side chain motifs of the superdiscs by tailored chemical synthesis, we find a particularly rich phase behaviour, which is not present in the bulk state. It is governed by a complex interplay of liquid crystalline elastic energies (bending and splay deformations), polar interactions and pure geometric confinement, and includes textural transitions between radial and axial alignment of the columns with respect to the long nanochannel axis.
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Motion of nanodroplets near chemical heterogeneities: We investigate the dynamics of nanoscale droplets in the vicinity of chemical steps which separate parts of a substrate with different wettabilities. Due to long-ranged dispersion forces, nanodroplets positioned on one side of the step perceive the different character of the other side even at some distances from the step, leading to a dynamic response. The direction of the ensuing motion of such droplets does not only depend on the difference between the equilibrium contact angles on these two parts but in particular on the difference between the corresponding Hamaker constants. Therefore the motion is not necessarily directed towards the more wettable side and can also be different from that of droplets which span the step.
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Sedimentation of active colloidal suspensions: In this paper, we investigate experimentally the non-equilibrium steady state of an active colloidal suspension under gravity field. The active particles are made of chemically powered colloids, showing self propulsion in the presence of an added fuel, here hydrogen peroxide. The active suspension is studied in a dedicated microfluidic device, made of permeable gel microstructures. Both the microdynamics of individual colloids and the global stationary state of the suspension under gravity - density profiles, number fluctuations - are measured with optical microscopy. This allows to connect the sedimentation length to the individual self-propelled dynamics, suggesting that in the present dilute regime the active colloids behave as 'hot' particles. Our work is a first step in the experimental exploration of the out-of-equilibrium properties of artificial active systems.
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Metastability of lipid necks via geometric triality: "Necks" are features of lipid membranes characterized by an uniquley large curvature, functioning as bridges between different compartments. These features are ubiquitous in the life-cycle of the cell and instrumental in processes such as division, extracellular vesicles uptake and cargo transport between organelles, but also in life-threatening conditions, as in the endocytosis of viruses and phages. Yet, the very existence of lipid necks challenges our understanding of membranes biophysics: their curvature, often orders of magnitude larger than elsewhere, is energetically prohibitive, even with the arsenal of molecular machineries and signalling pathways that cells have at their disposal. Using a geometric triality, namely a correspondence between three different classes of geometric objects, here we demonstrate that lipid necks are in fact metastable, thus can exist for finite, but potentially long times even in the absence of stabilizing mechanisms. This framework allows us to explicitly calculate the forces a corpuscle must overcome in order to penetrate cellular membranes, thus paving the way for a predictive theory of endo/exo-cytic processes.
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Drag coefficient of a liquid domain in a two-dimensional membrane: Using a hydrodynamic theory that incorporates a momentum decay mechanism, we calculate the drag coefficient of a circular liquid domain of finite viscosity moving in a two-dimensional membrane. We derive an analytical expression for the drag coefficient which covers the whole range of domain sizes. Several limiting expressions are discussed. The obtained drag coefficient decreases as the domain viscosity becomes smaller with respect to the outer membrane viscosity. This is because the flow induced in the domain acts to transport the fluid in the surrounding matrix more efficiently.
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Depletion-induced crystallization of anisotropic triblock colloids: The intricate interplay between colloidal particle shape and precisely engineered interaction potentials has paved the way for the discovery of unprecedented crystal structures in both two and three dimensions. Here, we make use of anisotropic triblock colloidal particles composed of two distinct materials. The resulting surface charge heterogeneity can be exploited to generate regioselective depletion interactions and directional bonding. Using extensive molecular dynamics simulations and a dimensionality reduction analysis approach, we map out state diagrams for the self-assembly of such colloids as a function of their aspect ratio and packing fraction for varying depletant sizes in a quasi two-dimensional set-up. We observe the formation of a wide variety of crystal structures such as a herringbone, brick-wall, tilted brick-wall, and (tilted) ladder-like structures. More specifically, we determine the optimal parameters to enhance crystallization, and investigate the nucleation process. Additionally, we explore the potential of using crystal monolayers as templates for deposition, thereby creating complex three-dimensional structures that hold promise for future applications.
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Structural Relaxation Time and Dynamic Shear Modulus of Glassy Graphene: We theoretically investigate glass transition behaviors of the glassy graphene in a wide range of temperature, where this amorphous graphene is described as a hard-sphere fluid. The dynamic arrest of a particle is assumingly caused by interactions with its nearest neighbors and surrounding fluid particles. The assumption allows us to analyze roles of local and collective particle mobility. We calculate the temperature dependence of structural relaxation time and dynamic shear modulus, the dynamic fragility, and the glass transition temperature. In addition, correlations between these physical quantities are comprehensively discussed. Our theoretical calculations agree quantitatively well with recent simulations and Dyre's shoving model.
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Control and ultrasonic actuation of a gas-liquid interface in a microfluidic chip: This article describes the design and manufacturing of a microfluidic chip, allowing for the actuation of a gas-liquid interface and of the neighboring fluid. A first way to control the interface motion is to apply a pressure difference across it. In this case, the efficiency of three different micro-geometries at anchoring the interface is compared. Also, the critical pressures needed to move the interface are measured and compared to theoretical result. A second way to control the interface motion is by ultrasonic excitation. When the excitation is weak, the interface exhibits traveling waves, which follow a dispersion equation. At stronger ultrasonic levels, standing waves appear on the interface, with frequencies that are half integer multiple of the excitation frequency. An associated microstreaming flow field observed in the vicinity of the interface is characterized. The meniscus and associated streaming flow have the potential to transport particles and mix reagents.
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Knotting and weak knotting in confined, open random walks using virtual knots: We probe the character of knotting in open, confined polymers, assigning knot types to open curves by identifying their projections as virtual knots. In this sense, virtual knots are transitional, lying in between classical knot types, which are useful to classify the ambiguous nature of knotting in open curves. Modelling confined polymers using both lattice walks and ideal chains, we find an ensemble of random, tangled open curves whose knotting is not dominated by any single knot type, a behaviour we call weakly knotted. We compare cubically confined lattice walks and spherically confined ideal chains, finding the weak knotting probability in both families is quite similar and growing with length, despite the overall knotting probability being quite different. In contrast, the probability of weak knotting in unconfined walks is small at all lengths investigated. For spherically confined ideal chains, weak knotting is strongly correlated with the degree of confinement but is almost entirely independent of length. For ideal chains confined to tubes and slits, weak knotting is correlated with an adjusted degree of confinement, again with length having negligible effect.
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A surface force apparatus for nanorheology under large shear strain: We describe a surface force apparatus designed to probe the rheology of a nanoconfined medium under large shear amplitudes (up to 500 $\mu$m). The instrument can be operated in closed-loop, controlling either the applied normal load or the thickness of the medium during shear experiments. Feedback control allows to greatly extend the range of confinement/shear strain attainable with the surface force apparatus. The performances of the instrument are illustrated using hexadecane as the confined medium.
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UV-Manipulation of Order and Macroscopic Shape in Nematic Elastomers: A range of monodomain nematic liquid crystal elastomers containing differing proportions of photo-isomerisable mesogenic moieties, which turn from a rod-like to a kinked shape upon ultraviolet (UV) irradiation, was studied. Depending on the proportion and positional role of the photo-sensitive groups in the crosslinked polymer network, different types and magnitudes of response were found. The principle consequence of such photo-isomerisation is the destabilisation of the nematic phase, whose order parameter depends on temperature in a near-critical fashion. Accordingly, the effect of UV-irradiation is dramatically enhanced near the critical temperature, with the associated reduction in the nematic order parameter manifesting as a change in the macroscopic shape of the elastomer samples, producing a large uniaxial contraction. Theoretical analysis of this phenomenon gives a good quantitative agreement with experiment.
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Topology in non-linear mechanical systems: Many advancements have been made in the field of topological mechanics. The majority of the works, however, concerns the topological invariant in a linear theory. We, in this work, present a generic prescription of defining topological indices which accommodates non-linear effects in mechanical systems without taking any approximation. Invoking the tools of differential geometry, a Z-valued quantity in terms of the Poincare-Hopf index, that features the topological invariant of non-linear zero modes (ZMs), is predicted. We further identify one type of topologically protected solitons that are robust to disorders. Our prescription constitutes a new direction of searching for novel topologically protected non-linear ZMs in the future.
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Localized fluidization in granular materials: Theoretical and numerical study: We present analytical and numerical results on localized fluidization within a granular layer subjected to a local injection of fluid. As the injection rate increases the three different regimes previously reported in the literature are recovered: homogeneous expansion of the bed, fluidized cavity in which fluidization starts developing above the injection area, and finally the chimney of fluidized grains when the fluidization zone reaches the free surface. The analytical approach is at the continuum scale, based on Darcy's law and Therzaghi's effective stress principle. It provides a good description of the phenomenon as long as the porosity of the granular assembly remains relatively homogeneous, i.e. for small injection rates. The numerical approach is at the particle scale based on the coupled DEM-PFV method. It tackles the more heterogeneous situations which occur at larger injection rates. The results from both methods are in qualitative agreement with data published independently. A more quantitative agreement is achieved by the numerical model. A direct link is evidenced between the occurrence of the different regimes of fluidization and the injection aperture. While narrow apertures let the three different regimes be distinguished clearly, larger apertures tend to produce a single homogeneous fluidization regime. In the former case, it is found that the transition between the cavity regime and the chimney regime for an increasing injection rate coincides with a peak in the evolution of inlet pressure. Finally, the occurrence of the different regimes is defined in terms of the normalized flux and aperture.
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Continuous rotation of achiral nematic liquid crystal droplets driven by heat flux: Suspended droplets of cholesteric (chiral nematic) liquid crystals spontaneously rotate in the presence of a heat flux due to a temperature gradient, a phenomenon known as Lehmann effect. So far, it is not clear whether this effect is due to the chirality of the phase and the molecules or only to the chirality of the director field. Here, we report the continuous rotation in a temperature gradient of nematic droplets of a lyotropic chromonic liquid crystal featuring a twisted bipolar configuration. The achiral nature of the molecular components leads to a random handedness of the spontaneous twist, resulting in the coexistence of droplets rotating in the two senses, with speeds proportional to the temperature gradient and inversely proportional to the droplet radius. This result shows that a macroscopic twist of the director field is sufficient to induce a rotation of the droplets, and that the phase and the molecules do not need to be chiral. This suggests that one can also explain the Lehmann rotation in cholesteric liquid crystals without introducing the Leslie thermomechanical coupling -- only present in chiral mesophases. An explanation based on the Akopyan and Zeldovich theory of thermomechanical effects in nematics is proposed and discussed.
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Entanglement and weak interaction driven mobility of small molecules in polymer networks: Diffusive transport of small molecules within the internal structures of biological and synthetic material systems is complex because the crowded environment presents chemical and physical barriers to mobility. We explored this mobility using a synthetic experimental system of small dye molecules diffusing within a polymer network at short time scales. We find that the diffusion of inert molecules is inhibited by the presence of the polymers. Counter-intuitively, small, hydrophobic molecules display smaller reduction in mobility and also able to diffuse faster through the system by leveraging crowding specific parameters. We explained this phenomenon by developing a de novo model and using these results, we hypothesized that non-specific hydrophobic interactions between the molecules and polymer chains could localize the molecules into compartments of overlapped and entangled chains where they experience microviscosity, rather than macroviscosity. We introduced a characteristic interaction time parameter to quantitatively explain experimental results in the light of frictional effects and molecular interactions. Our model is in good agreement with the experimental results and allowed us to classify molecules into two different mobility categories solely based on interaction. By changing the surface group, polymer molecular weight, and by adding salt to the medium, we could further modulate the mobility and mean square displacements of interacting molecules. Our work has implications in understanding intracellular diffusive transport in microtubule networks and other systems with macromolecular crowding and could lead to transport enhancement in synthetic polymer systems.
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Structure factor and thermodynamics of rigid dendrimers in solution: The ''polymer reference interaction site model'' (PRISM) integral equation theory is used to determine the structure factor of rigid dendrimers in solution. The theory is quite successful in reproducing experimental structure factors for various dendrimer concentrations. In addition, the structure factor at vanishing scattering vector is calculated via the compressibility equation using scaled particle theory and fundamental measure theory. The results as predicted by both theories are systematically smaller than the experimental and PRISM data for platelike dendrimers.
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Modeling growing confluent tissues using a lattice Boltzmann method: interface stability and fluctuations: Tissue growth underpins a wide array of biological and developmental processes, and numerical modeling of growing systems has been shown to be a useful tool for understanding these processes. However, the phenomena that can be captured are often limited by the size of systems that can be modeled. Here, we address this limitation by introducing a Lattice-Boltzmann method (LBM) for a growing system that is able to efficiently model hydrodynamic length-scales. The model incorporates a novel approach to describing the growing front of a tissue, which we use to investigate the dynamics of the interface of growing model tissues. We find that the interface grows with scaling in agreement with the Kardar-Parisi-Zhang (KPZ) universality class when growth in the system is bulk driven. Interestingly, we also find the emergence of a previously unreported hydrodynamic instability when proliferation is restricted to the tissue edge. We then develop an analytical theory to show that the instability arises due to a coupling between the number of cells actively proliferating and the position of the interface.
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Pentagon deposits unpack under gentle tapping: We present results from simulations of regular pentagons arranged in a rectangular die. The particles are subjected to vertical tapping. We study the behavior of the packing fraction, number of contacts and arch distributions as a function of the tapping amplitude. Pentagons show peculiar features as compared with disks. As a general rule, pentagons tend to form less arches than disks. Nevertheless, as the tapping amplitude is decreased, the typical size of the pentagon arches grows significantly. As a consequence, a pentagon packing reduces its packing fraction when tapped gently in contrast with the behavior found in rounded particle deposits.
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PECVD and PEALD on polymer substrates (Part II): Understanding and tuning of barrier and membrane properties of thin films: This feature article presents insights concerning the correlation of PECVD and PEALD thin film structures with their barrier or membrane properties. While in principle similar precursor gases and processes can be applied, the adjustment of deposition parameters for different polymer substrates can lead to either an effective diffusion barrier or selective permeabilities. In both cases the understanding of the film growth and the analysis of the pore size distribution and the pore surface chemistry is of utmost importance for the understanding of the related transport properties of small molecules. In this regard the article presents both concepts of thin film engineering and analytical as well as theoretical approaches leading to a comprehensive description of the state of the art in this field. Moreover, based on the presented correlation of film structure and molecular transport properties perspectives of future relevant research in this area is presented.
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Spin-lattice NMR relaxation by anomalous translational diffusion: A model-free theoretical framework for a phenomenological description of spin-lattice relaxation by anomalous translational diffusion in inhomogeneous systems based on the fractional diffusion equation is developed. The dependence of the spin-lattice relaxation time on the size of the pores in porous glass Vycor is experimentally obtained and found to agree well with our theoretical predictions. We obtain nonmonotonic behavior of the translational spin-lattice relaxation rate constant (it passes through a maximum) with the variation of the parameter referring to the extent of inhomogeneity of the system.
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Geometric and Topological Entropies of Sphere Packing: We present a statistical mechanical description of randomly packed spherical particles, where the average coordination number is treated as a macroscopic thermodynamic variable. The overall packing entropy is shown to have two contributions: geometric, reflecting statistical weights of individual configurations, and topological, which corresponds to the number of topologically distinct states. Both of them are computed in the thermodynamic limit for isostatic packings in 2D and 3D, and the result is further expanded to the case of "floppy" particle clusters. The theory is directly applicable to sticky colloids, and in addition, generalizes concepts of granular and glassy configurational entropies for the case of non-jammed systems.
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Physical processes causing the formation of penitentes: Snow penitentes form in sublimation conditions by differential ablation. Here we investigate the physical processes at the initial stage of penitente growth and perform the linear stability analysis of a flat surface submitted to the solar heat flux. We show that these patterns do not simply result from the self-illumination of the surface --a scale-free process-- but are primarily controlled by vapor diffusion and heat conduction. The wavelength at which snow penitentes emerge is derived and discussed. We found that it is controlled by aerodynamic mixing of vapor above the ice surface.
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Partitioning of energy in highly polydisperse granular gases: A highly polydisperse granular gas is modeled by a continuous distribution of particle sizes, a, giving rise to a corresponding continuous temperature profile, T(a), which we compute approximately, generalizing previous results for binary or multicomponent mixtures. If the system is driven, it evolves towards a stationary temperature profile, which is discussed for several driving mechanisms in dependence on the variance of the size distribution. For a uniform distribution of sizes, the stationary temperature profile is nonuniform with either hot small particles (constant force driving) or hot large particles (constant velocity or constant energy driving). Polydispersity always gives rise to non-Gaussian velocity distributions. Depending on the driving mechanism the tails can be either overpopulated or underpopulated as compared to the molecular gas. The deviations are mainly due to small particles. In the case of free cooling the decay rate depends continuously on particle size, while all partial temperatures decay according to Haff's law. The analytical results are supported by event driven simulations for a large, but discrete number of species.
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Self-assembly of binary solutions to complex structures: Self-assembly in natural and synthetic molecular systems can create complex aggregates or materials whose properties and functionality rises from their internal structure and molecular arrangement. The key microscopic features that control such assemblies remain poorly understood, nevertheless. Using classical density functional theory we demonstrate how the intrinsic length scales and their interplay in terms of interspecies molecular interactions can be used to tune soft matter self-assembly. We apply our strategy to two different soft binary mixtures to create guidelines for tuning intermolecular interactions that lead to transitions from fully miscible, liquid-like uniform state to formation of simple and core-shell aggregates, and mixed aggregate structures. Furthermore, we demonstrate how the interspecies interactions and system composition can be used to control concentration gradients of component species within these assemblies. The insight generated by this work contributes towards understanding and controlling soft multi-component self-assembly systems. Additionally, our results aid in understanding complex biological assemblies and their function and provide tools to engineer molecular interactions in order to control polymeric and protein-based materials, pharmaceutical formulations, and nanoparticle assemblies.
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On the Granular Stress-Geometry Equation: Using discrete calculus, we derive the missing stress-geometry equation for rigid granular materials in two dimensions, in the mean-field approximation. We show that (i) the equation imposes that the voids cannot carry stress, (ii) stress transmission is generically elliptic and has a quantitative relation to anisotropic elasticity, and (iii) the packing fabric plays an essential role.
cond-mat_soft
Spontaneous stable rotation of flocking flexible active matter: In nature, active matter, such as worms or dogs, tend to spontaneously form a stable rotational cluster when they flock to the same food source on an unregulated and unconfined surface. {In this paper we present an $n$-node flexible active matter model to study the collective motion due to the flocking of individual agents on a two-dimensional surface, and confirm that there exists a spontaneous stable cluster rotation synchronizing with a chirality produced by the alignment of their bodies under the impetus of the active force.} A prefactor of 1.86 is obtained for the linear relationship between normalized angular velocity and chirality. The angular velocity of such a rotation is found to be dependent on the individual flexibility, the number of nodes in each individual, and the magnitude of the active force. The conclusions well explain the spontaneous stable rotation of clusters that exists in many flexible active matter, like worms or {dogs}, when they flock to the same single source.
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An Ising model for the thermal and dynamic properties of supercooled liquids and the glass transition: We describe the behavior of an Ising model with orthogonal dynamics, where changes in energy and changes in alignment never occur during the same Monte Carlo (MC) step. This orthogonal Ising model (OIM) allows conservation of energy and conservation of momentum to proceed independently, on their own preferred time scales. MC simulations of the OIM mimic more than twenty distinctive characteristics that are commonly found above and below the glass temperature, Tg. Examples include a specific heat that has hysteresis around Tg, out-of-phase loss that exhibits primary and secondary peaks, super-Arrhenius T dependence for the alpha response time, and fragilities that increase with increasing system size (N). Mean-field theory for energy fluctuations in the OIM yields a novel expression for the super-Arrhenius divergence. Because this divergence is reminiscent of the Vogel-Fulcher-Tammann (VFT) law squared, we call it the VFT2 law. A modified Stickel plot, which linearizes the VFT2 law, gives qualitatively consistent agreement with measurements of primary response (from the literature) on five glass-forming liquids. Such agreement with the OIM suggests that several basic features govern supercooled liquids. The freezing of a liquid into a glass involves an underlying 2nd-order transition that is broadened by finite-size effects. The VFT2 law comes from energy fluctuations that enhance the pathways through an entropy bottleneck, not activation over an energy barrier. Primary response times vary exponentially with inverse N, consistent with the distribution of relaxation times deduced from measurements. System sizes found via the T dependence of the primary response are similar to sizes of independently relaxing regions measured by nuclear magnetic resonance for simple-molecule glass-forming liquids. The OIM provides a broad foundation for more-detailed models of liquid-glass behavior.
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Entropically Driven Helix Formation: The helix is a ubiquitous motif for biopolymers. We propose a heuristic, entropically based model that predicts helix formation in a system of hard spheres and semiflexible tubes. We find that the entropy of the spheres is maximized when short stretches of the tube form a helix with a geometry close to that found in natural helices. Our model could be directly tested with wormlike micelles as the tubes, and the effect could be used to self-assemble supramolecular helices.
cond-mat_soft
How to make and trap a pseudo-vesicle with a micropipette: We present a simple method to produce giant lipid pseudo-vesicles (vesicles with an oily cap on the top), trapped in an agarose gel. The method can be implemented using only a regular micropipette and relies on the formation of a water/oil/water double droplet in liquid agarose. We characterize the produced vesicle with fluorescence imaging and establish the presence and integrity of the lipid bilayer by the successful insertion of {\alpha}-Hemolysin transmembrane proteins. Finally, we show that the vesicle can be easily mechanically deformed, non-intrusively, by indenting the surface of the gel.
cond-mat_soft
Nucleation-induced transition to collective motion in active systems: While the existence of polar ordered states in active systems is well established, the dynamics of the self-assembly processes are still elusive. We study a lattice gas model of self-propelled elongated particles interacting through excluded volume and alignment interactions, which shows a phase transition from an isotropic to a polar ordered state. By analyzing the ordering process we find that the transition is driven by the formation of a critical nucleation cluster and a subsequent coarsening process. Moreover, the time to establish a polar ordered state shows a power-law divergence.
cond-mat_soft
A multi-species exchange model for fully fluctuating polymer field theory simulations: Field-theoretic models have been used extensively to study the phase behavior of inhomogeneous polymer melts and solutions, both in self-consistent mean-field calculations and in numerical simulations of the full theory capturing composition fluctuations. The models commonly used can be grouped into two categories, namely {\it species} models and {\it exchange} models. Species models involve integrations of functionals that explicitly depend on fields originating both from species density operators and their conjugate chemical potential fields. In contrast, exchange models retain only linear combinations of the chemical potential fields. In the two-component case, development of exchange models has been instrumental in enabling stable complex Langevin (CL) simulations of the full complex-valued theory. No comparable stable CL approach has yet been established for field theories of the species type. Here we introduce an extension of the exchange model to an arbitrary number of components, namely the multi-species exchange (MSE) model, which greatly expands the classes of soft material systems that can accessed by the complex Langevin simulation technique. We demonstrate the stability and accuracy of the MSE-CL sampling approach using numerical simulations of triblock and tetrablock terpolymer melts, and tetrablock quaterpolymer melts. This method should enable studies of a wide range of fluctuation phenomena in multiblock/multi-species polymer blends and composites.
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Optical responses through dilute anisotropic composites: Numerical calculations via Green's-function formalism: We investigate the linear and nonlinear optical responses of dilute anisotropic networks using the Green's-function formalism (GFF)[Gu Y et al. 1999 Phys. Rev. B 59 12847]. For the different applied fields, numerical calculations indicate that a large third order nonlinear enhancement and a broad infrared absorption arise from the geometric anisotropy. It is also shown the overlap and separation between the absorption peak and nonlinear enhancement peak when the applied field is parallel, perpendicular to the anisotropy respectively. In terms of the inverse participation ratios (IPR) with q=2 and spectral distribution of optical responses, the results can be understood.
cond-mat_soft
Ordering transitions of weakly anisotropic hard rods in narrow slit-like pores: The effect of strong confinement on the positional and orientational ordering is examined in a system of hard rectangular rods with length L and diameter D (L>D) using the Parsons-Lee modification of the second virial density functional theory. The rods are nonmesogenic (L/D<3)and confined between two parallel hard walls, where the width of the pore (H) is chosen in such a way that both planar (particle's long axis parallel to the walls) and homeotropic (particle's long axis perpendicular to the walls) orderings are possible and a maximum of two layers are allowed to form in the pore. In the extreme confinement limit of ,where only one layer structures appear, we observe a structural transition from a planar to a homeotropic fluid layer with increasing density, which becomes sharper as L->H. In wider pores (2D<H<3D) planar order with two layers, homeotropic order, and even combined bilayer structures (one layer is homeotropic, while the other is planar) can be stabilized at high densities. Moreover, first order phase transitions can be seen between different structures. One of them emerges between a monolayer and a bilayer with planar orders at relatively low packing fractions.
cond-mat_soft
Actuation performances of anisotropic gels: We investigated the actuation performances of anisotropic gels driven by mechanical and chemical stimuli, in terms of both deformation processes and stroke--curves, and distinguished between the fast response of gels before diffusion starts and the asymptotic response attained at the steady state. We also showed as the range of forces that an anisotropic hydrogel can exert when constrained is especially wide;indeed, changing fiber orientation allows to induce shear as well as transversely isotropic extensions.
cond-mat_soft
Membrane stress and torque induced by Frank's nematic textures: A geometric perspective using surface-based constraints: An elastic membrane with embedded nematic molecules is considered as a model of anisotropic fluid membrane with internal ordering. By considering the geometric coupling between director field and membrane curvature, the nematic texture is shown to induce anisotropic stresses additional to Canham-Helfrich elasticity. Building upon differential geometry, analytical expressions are found for the membrane stress and torque induced by splaying, twisting and bending of the nematic director as described by the Frank energy of liquid crystals. The forces induced by prototypical nematic textures are visualized on the sphere and on cylindrical surfaces.
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Hierarchical microphase separation in non-conserved active mixtures: Non-equilibrium phase separating systems with reactions can break time-reversal symmetry (TRS) in two distinct ways. Firstly, the conservative and non-conservative sectors of the dynamics can be governed by incompatible free energies; when both sectors are present, this is the leading-order TRS violation, captured in its simplest form by 'Model AB'. Second, the diffusive dynamics can break TRS in its own right. This happens only at higher order in the gradient expansion (but is the leading behaviour without reactions present) and is captured by 'Active Model B+' (AMB+). Each of the two mechanisms can lead to microphase separation, by quite different routes. Here we introduce Model AB+, for which both mechanisms are simultaneously present, and show that for slow reaction rates the system can undergo a new type of hierarchical microphase separation, whereby a continuous phase of fluid 1 contains large droplets of fluid 2 within which small droplets of fluid 1 are continuously created and then absorbed into the surrounding fluid-1 phase. In this state of 'bubbly microphase separation' the small-scale 1-in-2 droplets arise by the conservative diffusive dynamics with the larger scale 2-in-1 structure governed by the nonconservative reactions.
cond-mat_soft
2D to 3D transition in soap films demonstrated by microrheology: We follow the diffusive motion of colloidal particles of diameter $d$ in soap films of varying thickness $h$ with fluorescence microscopy. Diffusion constants are obtained both from one- and two-particle microrheological measurements of particle motion in these films. These diffusion constants are related to the surface viscosity of the interfaces comprising the soap films, by means of the Trapeznikov approximation [A. A. Trapeznikov, \emph{PICSA} (1957)] and Saffman's equation for diffusion in a 2D fluid. Unphysical values of the surface viscosity are found for thick soap films ($h/d > 7$), indicating a transition from 2D to 3D behavior.
cond-mat_soft
Stopping and reversing sound via dynamic dispersion tuning in a phononic metamaterial: Slowing down, stopping, and reversing a signal is a core functionality for information processing. Here, we show that this functionality can be realized by tuning the dispersion of a periodic system through a dispersionless, or flat, band. Specifically, we propose a phononic metamaterial based on plate resonators, in which the phonon band dispersion can be modified from an acoustic-like to an optical character by modulating a uniform prestress. The switch is enabled by the change in sign of an effective coupling between fundamental modes, which generically leads to a nearly dispersion-free band at the transition point. We demonstrate how adiabatic tuning of the band dispersion can immobilize and reverse the propagation of a sound pulse in simulations of a one-dimensional resonator chain. Our study relies on the basic principles of thin-plate elasticity independently of any specific material, making our results applicable across varied length scales and experimental platforms. More broadly, our approach could be metamaterials and electronic heterostructures.
cond-mat_soft
Exceptional Anti-Icing Performance of Self-Impregnating Slippery Surfaces: A heat exchange interface at subzero temperature in a water vapor environment, exhibits high probability of frost formation due to freezing condensation, a factor that markedly decreases the heat transfer efficacy due to the considerable thermal resistance of ice. Here we report a novel strategy to delay ice nucleation on these types of solid-water vapor interfaces. With a process-driven mechanism, a self-generated liquid intervening layer immiscible to water, is deposited on a textured superhydrophobic surface and acts as a barrier between the water vapor and the solid substrate. This liquid layer imparts remarkable slippery conditions resulting in high mobility of condensing water droplets. A large increase of the ensuing ice coverage time is shown compared to the cases of standard smooth hydrophilic or textured superhydrophobic surfaces. During deicing of these self-impregnating surfaces we show an impressive tendency of ice fragments to skate expediting defrosting. Robustness of such surfaces is also demonstrated by operating them under subcooling for at least 490hr without a marked degradation. This is attributed to the presence of the liquid intervening layer, which protects the substrate from hydrolyzation enhancing longevity and sustaining heat transfer efficiency.
cond-mat_soft
Surface sulci in squeezed soft solids: The squeezing of soft solids, the constrained growth of biological tissues, and the swelling of soft elastic solids such as gels can generate large compressive stresses at their surfaces. This causes the otherwise smooth surface of such a solid to becomes unstable when its stress exceeds a critical value. Previous analyses of the surface instability have assumed two-dimensional plane-strain conditions, but in experiments isotropic stresses often lead to complex three-dimensional sulcification patterns. Here we show how such diverse morphologies arise by numerically modeling the lateral compression of a rigidly clamped elastic layer. For incompressible solids, close to the instability threshold, sulci appear as I-shaped lines aligned orthogonally with their neighbors; at higher compressions they are Y-shaped and prefer a hexagonal arrangement. In contrast, highly compressible solids when squeezed show only one sulcified phase characterized by a hexagonal sulcus network.
cond-mat_soft
Asymptotic Analysis of Diffuse-Layer Effects on Time-Dependent Interfacial Kinetics: We investigate the subtle effects of diffuse charge on interfacial kinetics by solving the governing equations for ion transport (Nernst-Planck) with realistic boundary conditions representing reaction kinetics (Butler-Volmer) and compact-layer capacitance (Stern) in the asymptotic limit $\epsilon = \lambda_D/L \to 0$, where $\lambda_D$ is the Debye screening length and $L$ is the distance between the working and counter electrodes. Using the methods of singular perturbation theory, we derive the leading-order steady-state response to a nonzero applied current in the case of the oxidation of a neutral species into cations, without any supporting electrolyte. In certain parameter regimes, the theory predicts a reaction-limited current smaller than the classical diffusion-limited current. We also analyze the impedance of the electrochemical cell when a small AC current modulation is added to an applied DC current. At sufficiently high AC frequencies, the Maxwell displacement current is found to exceed the Faradaic conduction current, and experimentally observed ``negative impedances'' (out of phase AC voltage responses) are predicted close to the reaction-limited current. Overall, we demonstrate that the dynamics of diffuse charge plays a fundamental role in nonequilibrium surface reactions when the transport of one of the reacting species is coupled to the total interfacial reponse of the compact and diffuse layers.
cond-mat_soft
Bistability in a self-assembling system confined by elastic walls. Exact results in a one-dimensional lattice model: The impact of confinement on self-assembly of particles interacting with short-range attraction and long-range repulsion (SALR) potential is studied for thermodynamic states corresponding to local ordering of clusters or layers in the bulk. Exact and asymptotic expressions for the local density and for the effective potential between the confining surfaces are obtained for a one-dimensional lattice model introduced in [J. P\k{e}kalski et al. $J. Chem. Phys.$ ${\bf 140}$, 144903 (2013)].The simple asymptotic formulas are shown to be in good quantitative agreement with exact results for slits containing at least 5 layers. We observe that the incommensurability of the system size and the average distance between the clusters or layers in the bulk leads to structural deformations that are different for different values of the chemical potential $\mu$. The change of the type of defects is reflected in the dependence of density on $\mu$ that has a shape characteristic for phase transitions. Our results may help to avoid misinterpretation of the change of the type of defects as a phase transition in simulations of inhomogeneous systems. Finally, we show that a system confined by soft elastic walls may exhibit bistability such that two system sizes that differ approximately by the average distance between the clusters or layers are almost equally probable. This may happen when the equilibrium separation between the soft boundaries of an empty slit corresponds to the largest stress in the confined self-assembling system.
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Time resolved viscoelastic properties during structural arrest and aging of a colloidal glass: Evolution of the energy landscape during physical aging of glassy materials can be understood from the frequency and strain dependence of the shear modulus but the non-stationary nature of these systems frustrates investigation of their instantaneous underlying properties. Using a series of time dependent measurements we systematically reconstruct the frequency and strain dependence as a function of age for a repulsive colloidal glass undergoing structural arrest. In this manner, we are able to unambiguously observe the structural relaxation time, which increases exponentially with sample age at short times. The yield stress varies logarithmically with time in the arrested state, consistent with recent simulation results, whereas the yield strain is nearly constant in this regime. Strikingly, the frequency dependence at fixed times can be rescaled onto a master curve, implying a simple connection between the aging of the system and the change in the frequency dependent modulus.
cond-mat_soft