Reactive Brownian Dynamics of Chemically Fueled Droplets: Roles of Attraction and Deactivation Modes.

Abstract

The self-assembly of biological membraneless organelles can be mimicked by active droplets resulting from chemically fueled microphase separation. However, how the nonequilibrium, transient structure of these active droplets can be controlled through the physicochemical input parameters is not yet well understood. In our work, a chemically fueled two-state chemical reaction and subsequent droplet growth and decay are modeled with a reactive Brownian dynamics simulation in two spatial dimensions. In our model, particles that are activated via the consumption of fuel become attractive and can accumulate into droplets. A local-density-dependent distinction of the droplet's 'internal' and 'external' particles allows for structural feedback by giving further control over the deactivation process. The simulation shows that the deactivation of only external particles slows down the decay and stabilizes the droplets, whereas the deactivation of only internal particles can lead to a temporary encapsulation of deactivated particles (in nonequilibrium 'core-shell' structures) where the chemically active particles serve as an outer shell. Additionally, the role of hydrophobicity resembled by the attraction energy ε and the dependency of the nonequilibrium droplet formation on the various parameters of the chemical reaction are investigated. For example, a high attraction energy can lead to transient finite-size crystalline droplets, while other parameter choices indicate bimodal droplet size distributions at specific times. Similarities and differences to related experiments are discussed.