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Job Boekhoven

Publications and source records attributed to Job Boekhoven.

4 recordsLinked to original sources

Physical Mechanism of Vacuole Formation in Liquid Droplets

Vacuoles have been observed in liquid droplets across variety of experimental systems, ranging from biomolecular condensates composed of proteins and RNA, to synthetic coacervates formed by charged polymers or synthetic nanostars. These vacuoles are long-lived domains depleted of droplet material, and their formation is puzzling because the associated increase in interfacial area is thermodynamically unfavorable. Using theory, we show that vacuoles form through a generic mechanism: a local spinodal instability within the droplet. We demonstrate this mechanism in several experimentally relevant scenarios, including temperature quenches and droplets coupled to chemical processes occurring either inside or outside the droplet. Using non-equilibrium thermodynamics, we develop a theoretical framework that identifies the physicochemical conditions controlling whether vacuoles form and how big vacuoles can become. Our results suggest molecular designs and chemical pathways that promote vacuolation, enabling multi-compartment formation with engineered functions such as enhanced surface catalysis and compartment fission.

cond-mat.soft

Excitability and oscillations of active droplets

In living cells, cycles of formation and dissolution of liquid droplets can mediate biological functions such as DNA repair. However, the minimal physicochemical prerequisite for such droplet oscillations remains elusive. Here, we present a simple model composed of only two independent chemical components with their diffusive and chemical fluxes governed by non-equilibrium thermodynamics. There is turnover of fuel that maintains a chemical reaction away from equilibrium, leading to active droplets. We find that a single active droplet undergoes a pitchfork-bifurcation in the droplet volume upon increasing the fueling strength. Strikingly, the active droplet becomes excitable upon adding a further chemical reaction. For sufficient fueling, the system undergoes self-sustained oscillations cycling between droplet formation and dissolution. The minimal nature of our model suggests self-sustained active droplets as functional modules for de novo life.

cond-mat.soft

Critical transition between intensive and extensive active droplets

Emulsions ripen with an average droplet size increasing in time. In chemically active emulsions, coarsening can be absent, leading to a non-equilibrium steady state with mono-disperse droplet sizes. By considering a minimal model for phase separation and chemical reactions maintained away from equilibrium, we show that there is a critical transition in the conserved quantity between two classes of chemically active droplets: intensive and extensive ones. Single intensive active droplets reach a stationary size mainly controlled by the reaction-diffusion length scales. Intensive droplets in an emulsion interact only weakly, and the stationary size of a single droplet approximately sets the size of each droplet. On the contrary, the size of a single extensive active droplet scales with the system size, similar to passive phases. In an emulsion of many extensive droplets, their sizes become stationary only due to interactions among them. We discuss how the critical transition between intensive and extensive active droplets affects shape instabilities, including the division of active droplets, paving the way for the observation of successive division events in chemically active emulsions

cond-mat.soft

Formation of liquid shells in active droplet systems

We study a chemically active binary mixture undergoing phase separation and show that under non-equilibrium conditions, stable liquid spherical shells can form via a spinodal instability in the droplet center. A single liquid shell tends to grow until it undergoes a shape instability beyond a critical size. In an active emulsion, many stable and stationary liquid shells can coexist. We discuss conditions under which liquid shells are stable and dominant as compared to regimes where droplets undergo shape instabilities and divide.

cond-mat.soft