Suspensions of purely repulsive but self-propelled Brownian particles might undergo phase separation, a phenomenon that strongly resembles the phase separation of passive particles with attractions. Here we employ computer simulations to study the nucleation kinetics and the microscopic pathway active Brownian disks take in two dimensions when quenched from the homogeneous suspension to propulsion speeds beyond the binodal. We find the same qualitative behavior for the nucleation rate as a function of density as for a passive suspension undergoing liquid-vapor separation, suggesting that the scenario of an effective free energy also extends to the kinetics of phase separation. We study the transition in more detail through a committor analysis and find that transition states are best described by a combination of cluster size and the radial polarization of particles in the cluster.
We propose a stochastic process wherein molecular transport is mediated by asymmetric nucleation of domains on a one-dimensional substrate. Track-driven mechanisms of molecular transport arise in biophysical applications such as Holliday junction positioning and collagenase processivity. In contrast to molecular motors that hydrolyze nucleotide triphosphates and undergo a local molecular conformational change, we show that asymmetric nucleation of hydrolysis waves on a track can also result in directed motion of an attached particle. Asymmetrically cooperative kinetics between ``hydrolyzed'' a…
In this work a phenomenological stochastic differential equation is proposed to model the time evolution of the radius of a pre-critical molecular cluster during nucleation (the classical order parameter). Such a stochastic differential equation constitutes the basis for the calculation of the (nucleation) induction time under Kramers' theory of thermally activated escape processes. Considering the nucleation stage as a Poisson rare-event, analytical expressions for the induction time statistics are deduced for both steady and unsteady conditions, the latter assuming the semiadiabatic limit. T…
Classical nucleation theory (CNT), linking rare nucleation events to the free energy landscape of a growing nucleus, is central to understanding phase-change kinetics in passive fluids. Nucleation in non-equilibrium systems is much harder to describe because there is no free energy, but instead a dynamics-dependent quasi-potential that typically must be found numerically. Here we extend CNT to a class of active phase separating systems governed by a minimal field-theoretic model (Active Model B+). In the small noise and supersaturation limits that CNT assumes, we compute analytically the quasi…
We discuss the interplay between a slow continuous drift of temperature, which induces continuous phase separation, and the non-linear diffusion term in the $ϕ^4$-model for phase separation of a binary mixture. This leads to a bound for the stability of diffusive demixing. It is argued that these findings are not specific to the $ϕ^4$ model, but that they always apply up to slight modifications of the bound. In practice stable diffusive demixing can only be achieved when special precautions are taken in experiments on real mixtures. Therefore, the recent observations on complex dynamical behav…
We propose here a new mechanism of droplet coarsening in phase-separating fluid mixtures. In contrast to the conventional understanding that there are no interactions between droplets in the late stage of spinodal decomposition, we demonstrate the existence of interactions between droplets that is caused by the coupling between diffuse concentration change around droplets. We show the possibility that this mechanism plays an important role in droplet phase separation together with Brownian-coagulation mechanism. We also discuss the coupling between hydrodynamic and diffusion modes, namely, "co…
A theoretical framework is presented for the estimation of nucleation times in systems with Brownian type dynamics. This framework is applied to a prototype system: the two-dimensional Ising model with spin-flip dynamics in an external magnetic field. Direct simulation results for the nucleation times, spanning more than four orders of magnitude, are compared with theoretical predictions. There are no free parameters; all system properties required by the theory are determined by simulations in equilibrium systems. Theoretical and simulation values are found to agree in most cases within 20%.
The kinetic separation of repulsive active Brownian particles into a dense and a dilute phase is analyzed using a systematic coarse-graining strategy. We derive an effective Cahn-Hilliard equation on large length and time scales, which implies that the separation process can be mapped onto that of passive particles. A lower density threshold for clustering is found, and using our approach we demonstrate that clustering first proceeds via a hysteretic nucleation scenario and above a higher threshold changes into a spinodal-like instability. Our results are in agreement with particle-resolved co…
As a result of the competition between self-propulsion and excluded volume interactions, purely repulsive self-propelled spherical particles undergo a motility-induced phase separation (MIPS). We carry out a systematic computational study, considering several interaction potentials, systems confined by hard walls or with periodic boundary conditions, and different initial protocols. This approach allows us to identify that, despite its non-equilibrium nature, the equations of state of Active Brownian Particles (ABP) across MIPS verify the characteristic properties of first-order liquid-gas pha…
The phase separation mechanism of a binary liquid mixture off-critically quenched in its miscibility gap is nucleation and growth, its homogeneous phase reaching a metastable equilibrium state. The successive stages of growth of the nucleated droplets are a diffusion-driven free growth, an intermediate regime and a coarsening by reduction of interface (Ostwald ripening or Brownian collisions induced coalescence). We have made light attenuation experiments to investigate the sedimentation in such systems. These results have given us access experimentally to two values predicted theoretically: t…
The transport of active particles may occur in complex environments, in which it emerges from the interplay between the mobility of the active components and the quenched disorder of the environment. Here we explore structural and dynamical properties of Active Brownian Particles (ABPs) in random environments composed of fixed obstacles in three dimensions. We consider different arrangements of the obstacles. In particular, we consider two particular situations corresponding to experimentally realizable settings. Firstly, we model pinning particles in (non--overlapping) random positions and se…
We review how phase-field models contributed to the understanding of various aspects of crystal nucleation including homogeneous and heterogeneous processes, and their role in microstructure evolution. We recall results obtained both by the conventional phase-field approaches that rely on spatially averaged (coarse grained) order parameters in capturing freezing, and by the recently developed phase-field crystal models that work on the molecular scale, while employing time averaged particle densities, and are regarded as simple dynamical density functional theories of classical particles. Besi…
Active Brownian particles (ABPs), when subject to purely repulsive interactions, are known to undergo activity-induced phase separation broadly resembling an equilibrium (attraction-induced) gas-liquid coexistence. Here we present an accurate continuum theory for the dynamics of phase-separating ABPs, derived by direct coarse-graining, capturing leading-order density gradient terms alongside an effective bulk free energy. Such gradient terms do not obey detailed balance; yet we find coarsening dynamics closely resembling that of equilibrium phase separation. Our continuum theory is numerically…
The kinetics of the transformation from the hexagonal packed cylinder (HEX) phase to the face-centered-cubic (FCC) phase was simulated using Brownian Dynamics for an ABA triblock copolymer in a selective solvent for the A block. The kinetics was obtained by instantaneously changing either the temperature of the system or the well-depth of the Lennard-Jones potential. Detailed analysis showed that the transformation occurred via a rippling mechanism. The simulation results indicated that the order-order transformation (OOT) was a nucleation and growth process when the temperature of the system …
The dynamical density functional theory of Marconi and Tarazona [J. Chem. Phys., 110, 8032 (1999)], a theory for the non-equilibrium dynamics of the one-body density profile of a colloidal fluid, is applied to a binary fluid mixture of repulsive Gaussian particles confined in a spherical cavity of variable size. For this model fluid there exists an extremely simple Helmholtz free energy functional that provides a remarkably accurate description of the equilibrium fluid properties. We therefore use this functional to test the assumptions implicit in the dynamical density functional theory, rath…
In contrast with a gas at thermodynamic equilibrium, the mean force exerted on a wall by a gas of active particles usually depends on the confining potential, thereby preventing a proper definition of mechanical pressure. In this paper, we investigate numerically the properties of a gas of underdamped self-propelled dumbbells subject to Brownian noise of increasing intensity, in order to understand how the notion of pressure is recovered as noise progressively masks the effects of self-propulsion and the system approaches thermodynamic equilibrium. The simulations performed for a mobile asymme…
Collections of non-Brownian particles suspended in a viscous fluid and subjected to oscillatory shear at very low Reynolds number have recently been shown to exhibit a remarkable dynamical phase transition separating reversible from irreversible behaviour as the strain amplitude or volume fraction are increased. We present a simple model for this phenomenon, based on which we argue that this transition lies in the universality class of the conserved DP models or, equivalently, the Manna model. This leads to predictions for the scaling behaviour of a large number of experimental observables. No…
Active work measures how far the local self-forcing of active particles translates into real motion. Using Population Monte Carlo methods, we investigate large deviations in the active work for repulsive active Brownian disks. Minimizing the active work generically results in dynamical arrest; in contrast, despite the lack of aligning interactions, trajectories of high active work correspond to a collectively moving, aligned state. We use heuristic and analytic arguments to explain the origin of dynamical phase transitions separating the arrested, typical, and aligned regimes.
We develop a theory of fluctuations for Brownian systems with weak long-range interactions. For these systems, there exists a critical point separating a homogeneous phase from an inhomogeneous phase. Starting from the stochastic Smoluchowski equation governing the evolution of the fluctuating density field, we determine the expression of the correlation function of the density fluctuations around a spatially homogeneous equilibrium distribution. In the stable regime, we find that the temporal correlation function of the Fourier components of the density fluctuations decays exponentially rapid…
We present a study on the dynamics of a system consisting of a pair of hardcore particles diffusing with different rates. We solved the drift-diffusion equation for this model in the case when one particle, labeled F, drifts and diffuses slowly towards the second particle, labeled M. The displacements of particle M exhibits a crossover from diffusion to drift at a characteristic time which depends on the rate constants. We show that the positional fluctuation of M exhibits an intermediate crossover regime of subdiffusion separating initial and asymptotic diffusive behavior; this is in agreemen…
We study a biologically motivated model of overdamped, autochemotactic Brownian agents with concentration-dependent chemotactic sensitivity. The agents in our model move stochastically and produce a chemical ligand at their current position. The ligand concentration obeys a reaction-diffusion equation and acts as a chemoattractant for the agents, which bias their motion towards higher concentrations of the dynamically altered chemical field. We explore the impact of concentration-dependent response to chemoattractant gradients on large-scale pattern formation, by deriving a coarse-grained macr…
Scaling and Condensation of Dry Active Matter Around Circular Obstacles
Faculdade de Física, Universidade Federal do Pará（帕拉联邦大学物理学院）；MMML Lab, Department of Physics, University of Latvia（拉脱维亚大学物理系）；Departamento de Física, Universidade Federal do Ceará（塞阿拉联邦大学物理系）
Via hydrodynamics preserving molecular dynamics simulations we study growth phenomena in a phase separating symmetric binary mixture model. We quench high-temperature homogeneous configurations to state points inside the miscibility gap, for various mixture compositions. For compositions around the symmetric or critical value we capture the rapid linear viscous hydrodynamic growth due to advective transport of material through tube-like interconnected domains. The focus of the work, however, is on compositions close to any of the branches of the coexistence curve. In this case, the growth in t…
We investigate kinetic pathways of the DNA melting transition using variable-range versions of the Poland-Scheraga (PS) and Peyrard-Dauxois-Bishop (PDB) models of DNA. In the PS model, we construct a phi^4-field theory to calculate the critical droplet profile, the initial growth modes, and the exponent characterizing the divergence of the susceptibility near the spinodal. In the PDB model, we use a mean field analysis to calculate susceptibility exponent. We compare these theoretical results with Monte Carlo and Brownian dynamic simulations on the PS and PDB models, respectively. We find that…
Spontaneous liquid-liquid phase separation is commonly understood in terms of phenomenological mean-field theories. These theories correctly predict the structural features of the fluid at sufficiently long time scales and wavelengths. However, these conditions are not met in various examples in biology and materials science where the mixture is slowly destabilised, and phase separation takes place close to the critical point. Using kinetic Monte Carlo and molecular dynamics simulations of a binary surface fluid under these conditions, we show that the characteristic length scale of the emergi…
We present a nanoparticle size-separation device based on a nanofluidic rocking Brownian motor. It features a ratchet-shaped electrostatic particle potential with increasing barrier heights along the particle transport direction. The sharp drop of the particle current with barrier height is exploited to separate a particle suspension into multiple sub-populations. By solving the Fokker--Planck equation, we show that the physics of the separation mechanism is governed by the energy landscape under forward tilt of the ratchet. For a given device geometry and sorting duration, the applied force i…
We discuss the notion of nonequilibrium chemical potential in gases of non-interacting active particles filling two compartments separated by a potential energy barrier. Different types of active particles are considered: run-and-tumble particles, active Brownian particles, and active Brownian particles with a stochastic reorientation along an external field. After recalling some analytical results for run-and-rumble particles in one dimension, we focus on the two-dimensional case and obtain a perturbative expression of the density profile in the limit of a fast reorientation dynamics, for the…
