Department of Chemistry and The James Franck Institute, University of Chicago, Chicago, Illinois 60637, USA.
J Chem Phys. 2019 Mar 7;150(9):094708. doi: 10.1063/1.5042251.
Interfaces in phase-separated driven liquids are one example of how energy input at the single-particle level changes the long-length-scale material properties of nonequilibrium systems. Here, we measure interfacial fluctuations in simulations of two liquids driven by time-dependent forces, one with repulsive interactions and one with attractive interactions. The time-dependent forces lead to currents along the interface, which can modify the scaling of interface height fluctuations with respect to predictions from capillary wave theory (CWT). We therefore characterize the whole spectrum of fluctuations to determine whether CWT applies. In the system with repulsive interactions, we find that the interface fluctuations are well-described by CWT at one amplitude of the driving forces but not at others. In the system with attractive interactions, they obey CWT for all amplitudes of driving, allowing us to extract an effective surface tension. The surface tension increases linearly over two orders of magnitude of the driving forces, more than doubling its equilibrium value. Our results show how the interfaces of nonequilibrium liquids with time-dependent forces are modified by energy input.
分相驱动液体中的界面是能量在单粒子水平上输入如何改变非平衡系统长程材料性质的一个例子。在这里,我们在模拟两种由时变力驱动的液体时测量界面波动,一种液体具有排斥相互作用,另一种液体具有吸引力。时变力沿界面产生电流,这会改变界面高度波动与毛细波理论(CWT)预测的标度关系。因此,我们对整个波动谱进行了特征化,以确定 CWT 是否适用。在具有排斥相互作用的系统中,我们发现界面波动在驱动力的一个振幅下很好地符合 CWT,但在其他振幅下则不符合。在具有吸引力相互作用的系统中,它们在所有驱动力振幅下都符合 CWT,从而使我们能够提取出有效表面张力。表面张力在驱动力的两个数量级上呈线性增长,比平衡值增加了一倍以上。我们的结果表明,具有时变力的非平衡液体的界面如何被能量输入所改变。