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Within a simple model of attractive active Brownian particles, we predict flocking behavior and challenge the widespread idea that alignment interactions are necessary to observe this collective phenomenon. Here, we show that even nonaligning attractive interactions can lead to a flocking state. Monitoring the velocity polarization as the order parameter, we reveal the onset of a first-order transition from a disordered phase, characterized by several small clusters, to a flocking phase, where a single flocking cluster is emerging. The scenario is confirmed by studying the spatial connected correlation function of particle velocities, which reveals scale-free behavior in flocking states and exponential-like decay for nonflocking configurations. Our predictions can be tested in microscopic and macroscopic experiments showing flocking, such as animals, migrating cells, and active colloids.
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The probability per unit time for a thermally activated Brownian particle to escape over a potential well is, in general, well-described by Kramers's theory. Kramers showed that the escape time decreases exponentially with increasing barrier height. The dynamics slow down when the particle is charged and subjected to a Lorentz force due to an external magnetic field. This is evident via a rescaling of the diffusion coefficient entering as a prefactor in the Kramers's escape rate without any impact on the barrier-height-dependent exponent. Here, we show that the barrier height can be effectively changed when the charged particle is subjected to a vortex flow. While the vortex alone does not affect the mean escape time of the particle, when combined with a magnetic field, it effectively pushes the fluctuating particle either radially outside or inside depending on its sign relative to that of the magnetic field. In particular, the effective potential over which the particle escapes can be changed to a flat, a stable, and an unstable potential by tuning the signs and magnitudes of the vortex and the applied magnetic field. Notably, the last case corresponds to enhanced escape dynamics.
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At the triple point of a repulsive screened Coulomb system, a fcc crystal, a bcc crystal, and a fluid phase coexist. At their intersection, these three phases form a liquid groove, the triple junction. Using confocal microscopy, we resolve the triple junction on a single-particle level in a model system of charged PMMA colloids in a nonpolar solvent. The groove is found to be extremely deep and the incommensurate solid-solid interface to be very broad. Thermal fluctuations hence appear to dominate the solid-solid interface. This indicates a very low interfacial energy. The fcc-bcc interfacial energy is quantitatively determined based on Young's equation and, indeed, it is only about 1.3 times higher than the fcc-fluid interfacial energy close to the triple point.
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To gain insight into the fundamental processes determining the motion of macromolecules in polymeric matrices, the dynamical hindrance of polymeric dextran molecules diffusing as probe through a polyacrylamide hydrogel is systematically explored. Three complementary experimental methods combined with Brownian dynamics simulations are used to study a broad range of dextran molecular weights and salt concentrations. While multi-parameter fluorescence image spectroscopy (MFIS) is applied to investigate the local diffusion of single molecules on a microscopic length scale inside the hydrogel, a macroscopic transmission imaging (MTI) fluorescence technique and nuclear magnetic resonance (NMR) are used to study the collective motion of dextrans on the macroscopic scale. These fundamentally different experimental methods, probing different length scales of the system, yield long-time diffusion coefficients for the dextran molecules which agree quantitatively. The measured diffusion coefficients decay markedly with increasing molecular weight of the dextran and fall onto a master curve. The observed trends of the hindrance factors are consistent with Brownian dynamics simulations. The simulations also allow us to estimate the mean pore size for the herein investigated experimental conditions. In addition to the diffusing molecules, MFIS detects temporarily trapped molecules inside the matrix with diffusion times above 10 ms, which is also confirmed by anisotropy analysis. The fraction of bound molecules depends on the ionic strength of the solution and the charge of the dye. Using fluorescence intensity analysis, also MTI confirms the observation of the interaction of dextrans with the hydrogel. Moreover, pixelwise analysis permits to show significant heterogeneity of the gel on the microscopic scale.
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The growth of quasicrystals, i.e., aperiodic structures with long-range order, seeded from the melt is investigated using a dynamical phase field crystal model. Depending on the thermodynamic conditions, two different growth modes are detected, namely defect-free growth of the stable quasicrystal and a mode dominated by phasonic flips which are incorporated as local defects into the grown structure such that random tilinglike ordering emerges. The latter growth mode is unique to quasicrystals and can be verified in experiments on one-component mesoscopic systems.
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The equilibrium structure and dynamics of a single polymer chain in a thermal solvent is by now well-understood in terms of scaling laws. Here, we consider a polymer in a bacterial bath, i.e., in a solvent consisting of active particles which bring in nonequilibrium fluctuations. Using computer simulations of a self-avoiding polymer chain in two dimensions which is exposed to a dilute bath of active particles, we show that the Flory-scaling exponent is unaffected by the bath activity provided the chain is very long. Conversely, for shorter chains, there is a nontrivial coupling between the bacteria intruding into the chain which may stiffen and expand the chain in a nonuniversal way. As a function of the molecular weight, the swelling first scales faster than described by the Flory exponent, then an unusual plateau-like behaviour is reached and finally a crossover to the universal Flory behaviour is observed. As a function of bacterial activity, the chain end-to-end distance exhibits a pronounced non-monotonicity. Moreover, the mean-square displacement of the center of mass of the chain shows a ballistic behaviour at intermediate times as induced by the active solvent. Our predictions are verifiable in two-dimensional bacterial suspensions and for colloidal model chains exposed to artificial colloidal microswimmers.
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The ionic composition and pair correlations in fluid phases of realistically salt-free charged colloidal sphere suspensions are calculated in the primitive model. We obtain the number densities of all ionic species in suspension, including low-molecular weight microions, and colloidal macroions with acidic surface groups, from a self-consistent solution of a coupled physicochemical set of nonlinear algebraic equations and non-mean-field liquid integral equations. Here, we study suspensions of colloidal spheres with sulfonate or silanol surface groups, suspended in demineralized water that is saturated with carbon dioxide under standard atmosphere. The only input required for our theoretical scheme are the acidic dissociation constants pKa, and effective sphere diameters of all involved ions. Our method allows for an ab initio calculation of colloidal bare and effective charges, at high numerical efficiency.
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Crystallization in a two-dimensional strongly coupled plasma from a rapidly cooled fluid is found to be efficiently blocked by an external magnetic field. Beyond a threshold of the magnetic field strength B, the relaxation time to the equilibrium crystal increases exponentially with B, which is attributed to an impeded conversion of potential to kinetic energy. Our finding is opposed to the standard picture of two-dimensional freezing of one-component systems which does not exhibit a nucleation barrier and opens the way to keep two-dimensional fluids metastable over long times.
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A competition of incommensurate symmetries occurs whenever a system is forced to conform to an ordering that is different from the intrinsically preferred structure of the system itself. As a model system of such a competition, we study the rivalry between the triangular ordering of hard disks and the square symmetry induced by a periodic square substrate. By using density functional theory as well as Monte Carlo computer simulations, we determine the full phase behavior for the case of one particle per minimum. We observe a rhombic preordering structure preceding the hexagonal solid as a direct consequence of the competing symmetries. Furthermore, the square-rhombic transition is reentrant with increasing substrate interaction. Our predictions can be verified in experiments of colloids in laser fields.
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We determine the orientation-resolved interfacial free energy between a body-centered-cubic (bcc) crystal and the coexisting fluid for a many-particle system interacting via a Yukawa pair potential. For two different screening strengths, we compare results from molecular dynamics computer simulations, density functional theory, and a phase-field-crystal approach. Simulations predict an almost orientationally isotropic interfacial free energy of 0.12k(B)T/a(2) (with k(B)T denoting the thermal energy and a the mean interparticle spacing), which is independent of the screening strength. This value is in reasonable agreement with our Ramakrishnan-Yussouff density functional calculations, while a high-order fitted phase-field-crystal approach gives about 2-3 times higher interfacial free energies for the Yukawa system. Both field theory approaches also give a considerable anisotropy of the interfacial free energy. Our result implies that, in the Yukawa system, bcc crystal-fluid free energies are a factor of about 3 smaller than face-centered-cubic crystal-fluid free energies.
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We study the collective vibrational excitations of crystals under out-of-equilibrium steady conditions that give rise to entropy production. Their excitation spectrum comprises equilibriumlike phonons of thermal origin and additional collective excitations called entropons because each of them represents a mode of spectral entropy production. Entropons coexist with phonons and dominate them when the system is far from equilibrium while they are negligible in near-equilibrium regimes. The concept of entropons has been recently introduced and verified in a special case of crystals formed by self-propelled particles. Here we show that entropons exist in a broader class of active crystals that are intrinsically out of equilibrium and characterized by the lack of detailed balance. After a general derivation, several explicit examples are discussed, including crystals consisting of particles with alignment interactions and frictional contact forces.
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In many applications, it is important to catch collections of autonomously navigating microbes and man-made microswimmers in a controlled way. Using computer simulation of a two-dimensional system of self-propelled rods we show that a static chevron-shaped wall represents an excellent trapping device for self-motile particles. Its catching efficiency can be controlled by varying the apex angle of the trap which defines the sharpness of the cusp. Upon decreasing the angle we find a sequence of three emergent states: no trapping at wide angles followed by a sharp transition towards complete trapping at medium angles and a crossover to partial trapping at small cusp angles. A generic trapping "phase diagram" maps out the conditions at which the capture of active particles at a given density is rendered optimal.
Asunto(s)
Modelos Teóricos , Movimiento (Física) , Transición de FaseRESUMEN
A combination of fundamental measure density functional theory and Monte Carlo computer simulation is used to determine the orientation-resolved interfacial tension and stiffness for the equilibrium hard-sphere crystal-fluid interface. Microscopic density functional theory is in quantitative agreement with simulations and predicts a tension of 0.66k(B)T/σ(2) with a small anisotropy of about 0.025k(B)T and stiffnesses with, e.g., 0.53k(B)T/σ(2) for the (001) orientation and 1.03k(B)T/σ(2) for the (111) orientation. Here k(B)T is denoting the thermal energy and σ the hard-sphere diameter. We compare our results with existing experimental findings.
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We propose and demonstrate a concept that mimics the magnetization of the heavy dust particles in a complex plasma while leaving the properties of the light species practically unaffected. It makes use of the frictional coupling between a complex plasma and the neutral gas, which allows us to transfer angular momentum from a rotating gas column to a well-controlled rotation of the dust cloud. This induces a Coriolis force that acts exactly as the Lorentz force in a magnetic field. Experimental normal mode measurements for a small dust cluster with four particles show excellent agreement with theoretical predictions for a magnetized plasma.
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Swimming in circles occurs in a variety of situations at low Reynolds number. Here we propose a simple model for a swimmer that undergoes circular motion, generalising the model of a linear swimmer proposed by Najafi and Golestanian (Phys. Rev. E 69, 062901 (2004)). Our model consists of three solid spheres arranged in a triangular configuration, joined by two links of time-dependent length. For small strokes, we discuss the motion of the swimmer as a function of the separation angle between its links. We find that swimmers describe either clockwise or anticlockwise circular motion depending on the tilting angle in a non-trivial manner. The symmetry of the swimmer leads to a quadrupolar decay of the far flow field. We discuss the potential extensions and experimental realisation of our model.
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We investigated driven crystal formation events in thin layers of sedimented colloidal particles under low salt conditions. Using optical microscopy, we observe particles in a thermodynamically stable colloidal fluid to move radially converging towards cation exchange resin fragments acting as seed particles. When the local particle concentration has become sufficiently large, subsequently crystallization occurs. Brownian dynamics simulations of a 2D system of purely repulsive point-like particles exposed to an attractive potential, yield strikingly similar scenarios, and kinetics of accumulation and micro-structure formation. This offers the possibility of flexibly designing and manufacturing thin colloidal crystals at controlled positions and thus to obtain specific micro-structures not accessible by conventional approaches. We further demonstrate that particle motion is correlated with the existence of a gradient in electrolyte concentration due to the release of electrolyte by the seeds.
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We study a Langevin equation describing the stochastic motion of a particle in one dimension with coordinate x, which is simultaneously exposed to a space-dependent friction coefficient γ(x), a confining potential U(x) and nonequilibrium (i.e., active) noise. Specifically, we consider frictions γ(x)=γ_{0}+γ_{1}|x|^{p} and potentials U(x)â|x|^{n} with exponents p=1,2 and n=0,1,2. We provide analytical and numerical results for the particle dynamics for short times and the stationary probability density functions (PDFs) for long times. The short-time behavior displays diffusive and ballistic regimes while the stationary PDFs display unique characteristic features depending on the exponent values (p,n). The PDFs interpolate between Laplacian, Gaussian, and bimodal distributions, whereby a change between these different behaviors can be achieved by a tuning of the friction strengths ratio γ_{0}/γ_{1}. Our model is relevant for molecular motors moving on a one-dimensional track and can also be realized for confined self-propelled colloidal particles.
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Using experiments and combining theory and computer simulations, we show that binary complex plasmas are particularly good model systems to study the kinetics of fluid-fluid demixing at the "atomistic" (individual particle) level. The essential parameters of interparticle interactions in complex plasmas, such as the interaction range(s) and degree of nonadditivity, can be varied significantly, which allows systematic investigations of different demixing regimes. The critical role of competition between long-range and short-range interactions at the initial stage of the spinodal decomposition is discussed.
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Laboratory realizations of two-dimensional (2D) plasma crystals typically involve monodisperse microparticles confined into horizontal monolayers in radio-frequency (rf) plasma sheaths. This gives rise to the so-called plasma wakes beneath the microparticles. The presence of wakes renders the interactions in such systems nonreciprocal, a fact that can lead to a quite different behavior from the one expected for their reciprocal counterparts. Here we examine the buckling of a hexagonal 2D plasma crystal, occurring as the confinement strength is decreased, taking explicitly into account the nonreciprocity of the system via a well-established point-wake model. We observe that for a finite wake charge, the monolayer hexagonal crystal undergoes a transition first to a bilayer hexagonal structure, unrealizable in harmonically confined reciprocal Yukawa systems, and subsequently to a bilayer square structure. Our theoretical results are confirmed by molecular dynamics simulations for experimentally relevant parameters, indicating the potential of their observation in state-of-the-art experiments with 2D complex plasmas.
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The long-standing observations that different amorphous materials exhibit a pronounced enhancement of viscosity and eventually vitrify on compression or cooling continue to fascinate and challenge scientists, on the ground of their physical origin and practical implications. Glass formation is a generic phenomenon, observed in physically quite distinct systems that encompass hard and soft particles. It is believed that a common underlying scenario, namely cage formation, drives dynamical arrest, especially at high concentrations. Here, we identify a novel, asymmetric glassy state in soft colloidal mixtures, which is characterized by strongly anisotropically distorted cages, bearing similarities to those of hard-sphere glasses under shear. The anisotropy is induced by the presence of soft additives. This phenomenon seems to be generic to soft colloids and its origins lie in the penetrability of the constituent particles. The resulting phase diagram for mixtures of soft particles is clearly distinct from that of hard-sphere mixtures and brings forward a rich variety of vitrified states that delineate an ergodic lake in the parameter space spanned by the size ratio between the two components and by the concentration of the additives. Thus, a new route opens for the rational design of soft particles with desired tunable rheological properties.