Reaction-Driven Diffusiophoresis of Liquid Condensates: Potential Mechanisms for Intracellular Organization.

The cellular environment, characterized by its intricate composition and spatial organization, hosts a variety of organelles, ranging from membrane-bound ones to membraneless structures that are formed through liquid-liquid phase separation. Cells show precise control over the position of such condensates. We demonstrate that organelle movement in external concentration gradients, diffusiophoresis, is distinct from the one of colloids because fluxes can remain finite inside the liquid-phase droplets and movement of the latter arises from incompressibility. Within cellular domains diffusiophoresis naturally arises from biochemical reactions that are driven by a chemical fuel and produce waste. Simulations and analytical arguments within a minimal model of reaction-driven phase separation reveal that the directed movement stems from two contributions: Fuel and waste are refilled or extracted at the boundary, resulting in concentration gradients, which (i) induce product fluxes via incompressibility and (ii) result in an asymmetric forward reaction in the droplet's surroundings (as well as asymmetric backward reaction inside the droplet), thereby shifting the droplet's position. We show that the former contribution dominates and sets the direction of the movement, toward or away from fuel source and waste sink, depending on the product molecules' affinity toward fuel and waste, respectively. The mechanism thus provides a simple means to organize condensates with different composition. Particle-based simulations and systems with more complex reaction cycles corroborate the robustness and universality of this mechanism.

Reaction-driven assembly: controlling changes in membrane topology by reaction cycles.

Chemical reaction cycles are prototypical examples how to drive systems out of equilibrium and introduce novel, life-like properties into soft-matter systems. We report simulations of amphiphilic molecules in aqueous solution. The molecule's head group is permanently hydrophilic, whereas the reaction cycle switches the molecule's tail from hydrophilic (precursor) to hydrophobic (amphiphile) and vice versa. The reaction cycle leads to an arrest in coalescence and results in uniform vesicle sizes that can be controlled by the reaction rate. Using a continuum description and particle-based simulation, we study the scaling of the vesicle size with the reaction rate. The chemically active vesicles are inflated by precursor, imparting tension onto the membrane and, for specific parameters, stabilize pores.