Cho Yongick, Jacobs William M
Department of Chemistry, Princeton University, Princeton, New Jersey 08544, USA.
J Chem Phys. 2023 Oct 21;159(15). doi: 10.1063/5.0166824.
Chemically driven fluids can demix to form condensed droplets that exhibit phase behaviors not observed at equilibrium. In particular, nonequilibrium interfacial properties can emerge when the chemical reactions are driven differentially between the interior and exterior of the phase-separated droplets. Here, we use a minimal model to study changes in the interfacial tension between coexisting phases away from equilibrium. Simulations of both droplet nucleation and interface roughness indicate that the nonequilibrium interfacial tension can either be increased or decreased relative to its equilibrium value, depending on whether the driven chemical reactions are accelerated or decelerated within the droplets. Finally, we show that these observations can be understood using a predictive theory based on an effective thermodynamic equilibrium.
化学驱动的流体可以发生相分离,形成凝聚液滴,这些液滴表现出在平衡状态下未观察到的相行为。特别是,当相分离液滴的内部和外部之间的化学反应以不同方式驱动时,非平衡界面性质可能会出现。在这里,我们使用一个极简模型来研究远离平衡的共存相之间的界面张力变化。液滴成核和界面粗糙度的模拟表明,非平衡界面张力相对于其平衡值可以增加或降低,这取决于液滴内驱动的化学反应是加速还是减速。最后,我们表明,使用基于有效热力学平衡的预测理论可以理解这些观察结果。