Quantitative Understanding of Liquid Dynamics at Interfaces from a Free-Energy Landscape Perspective,Physical Review Letters

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Quantitative Understanding of Liquid Dynamics at Interfaces from a Free-Energy Landscape Perspective
Physical Review Letters ( IF 8.1 ) Pub Date : 2024-09-04 , DOI: 10.1103/physrevlett.133.106201
Simon Hefner ₁ , Robin Horstmann ₁ , Sebastian Kloth ₁ , Michael Vogel ₁

Affiliation

On the basis of molecular dynamics simulations of water and ethanol in nanopores, we devise a methodology to determine the free-energy landscape (FEL) imposed by an interface on an adjoining liquid directly from the particle trajectories. The methodology merely uses the statistical mechanical relation between occupancy and energy and, hence, is particularly suitable in complex situations, e.g., for disordered or rough atomistic interfaces and molecular liquids, as encountered in many biological, geological, and technological situations. Moreover, we show that the thus-obtained FEL enables a quantitative understanding of interface effects on liquid dynamics. Specifically, by determining the local minima and barriers of the FEL and using an Arrhenius-like relation, we reproduce the very strong spatial variation of the structural relaxation time of water and ethanol across nanopores over a broad temperature range. We anticipate that the proposed FEL approach is transferable to various other liquids and interfaces.

中文翻译：

从自由能景观的角度定量理解界面处的液体动力学

基于纳米孔中水和乙醇的分子动力学模拟，我们设计了一种直接从粒子轨迹确定相邻液体界面所施加的自由能景观（FEL）的方法。该方法仅使用占用率和能量之间的统计力学关系，因此特别适合复杂情况，例如，对于许多生物、地质和技术情况中遇到的无序或粗糙原子界面和分子液体。此外，我们还表明，由此获得的 FEL 能够定量理解界面对液体动力学的影响。具体来说，通过确定 FEL 的局部最小值和势垒并使用类阿累尼乌斯关系，我们重现了水和乙醇在宽温度范围内跨纳米孔的结构弛豫时间的非常强的空间变化。我们预计所提出的 FEL 方法可以转移到各种其他液体和界面。

更新日期：2024-09-05

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