A classical nucleation theory description of active colloid assembly

Abstract

Non-aligning self-propelled particles with purely repulsive excluded volume interactions undergo athermal motility-induced phase separation into a dilute gas and a dense cluster phase. Here, we use enhanced sampling computational methods and analytic theory to examine the kinetics of formation of the dense phase. Despite the intrinsically nonequilibrium nature of the phase transition, we show that the kinetics can be described using an approach analogous to equilibrium classical nucleation theory, governed by an effective free energy of cluster formation with identifiable bulk and surface terms. The theory captures the location of the binodal, nucleation rates as a function of supersaturation, and the cluster size distributions below the binodal, while discrepancies in the metastable region reveal additional physics about the early stages of active crystal formation. The success of the theory shows that a framework similar to equilibrium thermodynamics can be obtained directly from the microdynamics of an active system, and can be used to describe the kinetics of evolution toward nonequilibrium steady states.

12 pages, 9 figures

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Cited by in corpus (45)

• Generalized Thermodynamics of Phase Equilibria in Scalar Active Matter
• Generalized thermodynamics of Motility-Induced Phase Separation: Phase equilibria, Laplace pressure, and change of ensembles
• Entropy production and fluctuation theorems for active matter
• Interrupted Motility Induced Phase Separation in Aligning Active Colloids
• Time-(ir)reversibility in active matter: from micro to macro
• Phase Diagram of Active Brownian Spheres: Crystallization and the Metastability of Motility-Induced Phase Separation
• Activity controls fragility: A Random First Order Transition Theory for an active glass
• Mechanical pressure and momentum conservation in dry active matter
• Phase co-existence in bidimensional passive and active dumbbell systems
• Phase separation and large deviations of lattice active matter
• Steady-state distributions of ideal active Brownian particles under confinement and forcing
• Mechanical Theory of Nonequilibrium Coexistence and Motility-Induced Phase Separation
• Kinetics of motility-induced phase separation and swim pressure
• Interparticle torques suppress motility-induced phase separation for rodlike particles
• Classical Nucleation Theory for Active Fluid Phase Separation
• Active phase separation: new phenomenology from non-equilibrium physics
• Disorder-Induced Long-Ranged Correlations in Scalar Active Matter
• Exact fluctuating hydrodynamics of active lattice gases -- Typical fluctuations
• Predictive local field theory for interacting active Brownian spheres in two spatial dimensions
• Disordered boundaries destroy bulk phase separation in scalar active matter
• Collective dynamics of active Brownian particles in three spatial dimensions: a predictive field theory
• Nonequilibrium phase behaviour from minimization of free power dissipation
• The stability phase diagram of active Brownian particles
• Target search of active agents crossing high energy barriers
• Phase separation of self-propelled ballistic particles
• Anomalous fluctuations in homogeneous fluid phase of active Brownian particles
• Theory of Capillary Tension and Interfacial Dynamics of Motility-Induced Phases
• Similarity of ensembles of trajectories of reversible and irreversible growth processes
• Steady states of active Brownian particles interacting with boundaries
• Response of active Brownian particles to boundary driving
• Bridging the Gap Between Collective Motility and Epithelial-Mesenchymal Transitions through the Active Finite Voronoi Model
• Diffusion Transients in Motility-Induced Phase Separation
• Statistical properties of microphase and bubbly phase-separated active fluids
• Non-equilibrium systems have steady-state distributions and non-steady dynamics
• How does a hyperuniform fluid freeze?
• Evaluation of transition rates from nonequilibrium instantons
• The Mechanics of Nucleation and Growth and the Surface Tensions of Active Matter
• Interfacial and density fluctuations in a lattice model of motility-induced phase separation
• Collective motion of granular matter subjected to swirling excitation
• AMEP: The Active Matter Evaluation Package for Python
• Emergent Gauge Symmetry in Active Brownian Matter
• Phases of active matter in two dimensions
• An Infinite Set of Integral Formulae for Polar, Nematic, and Higher Order Structures at the Interface of Motility-Induced Phase Separation
• Non-equilibrium pathways between cluster morphologies in active phase separation: necking, rupture and cavitation
• Hyperuniformity in active fluids reshapes nucleation and capillary-wave dynamics