2016/03/31 by Gabriel S. Redner, Caleb G. Wagner, Aparna Baskaran +1 · 99 citations
Materials Science · Physics and Astronomy · #Advanced Thermodynamics and Statistical Mechanics #Binodal #Chemical physics #Classical mechanics #Classical nucleation theory #Cluster (spacecraft) #Kinetics #Materials science #Metastability #Micro and Nano Robotics #Non-equilibrium thermodynamics #Nucleation #Phase (matter) #Phase diagram #Phase transition #Physics #Pickering emulsions and particle stabilization #Quantum mechanics #Statistical physics #Supersaturation #Thermodynamics #cond-mat.soft
paper · pdf · doi:10.1103/physrevlett.117.148002
published in Physical Review Letters 117(14), 148002 (American Physical Society) · 12 pages, 9 figures
arxiv created 2016/08/17 · openalex publication_date 2016/09/30 · arxiv updated 2016/10/05 · openalex created_date 2025/10/10 · openalex updated_date 2026/08/06
Nonaligning 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.