Activity-Induced Droplet Inversion in Multicomponent Liquid-Liquid Phase Separation.

IF 5.5 1区 化学 Q2 CHEMISTRY, PHYSICAL Journal of Chemical Theory and Computation Pub Date : 2025-04-08 Epub Date: 2025-03-26 DOI:10.1021/acs.jctc.5c00162
Xianyun Jiang, Zhonghuai Hou
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Abstract

Liquid-liquid phase separation (LLPS) is a vital process in forming membrane-free organelles, crucial for cell physiology and recently gaining significant attention. However, the effects of nonequilibrium factors, which are common in real life, on the process of LLPS have not been fully explored. To address this issue, we developed a model for nonequilibrium phase separation involving three components (A, B, and C) by integrating a nonequilibrium term into the chemical potential for active component B. We find significant changes in the morphology and dynamics of nonequilibrium phase-separated droplets compared to their equilibrium counterparts. Remarkably, with a large enough activity, the B-A-C structure (B at the center, surrounded by A, then enveloped by C) under equilibrium conditions may change to a C-A-B structure. Further simulations give a global picture of the system under both active and passive conditions, revealing the shifts of the phase boundaries and unraveling the effect of activity on different droplet structures. We derived an effective free energy for the active LLPS system to provide a qualitative understanding of our observations. Our study presents a basic model for nonequilibrium phase separation processes, providing crucial insights into LLPS alongside intracellular nonequilibrium phenomena.

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多组分液-液分离中活性诱导的液滴反转。
液-液相分离(LLPS)是形成无膜细胞器的重要过程,在细胞生理中起着至关重要的作用,近年来引起了人们的广泛关注。然而,现实生活中常见的非平衡因素对LLPS过程的影响尚未得到充分的探讨。为了解决这个问题,我们通过将一个非平衡项整合到活性组分B的化学势中,开发了一个涉及三组分(a、B和C)的非平衡相分离模型。我们发现,与平衡相分离的液滴相比,非平衡相分离液滴的形态和动力学发生了显著变化。值得注意的是,当活性足够大时,平衡条件下B- a -C结构(B在中心,被a包围,再被C包围)可以转变为C- a -B结构。进一步的模拟给出了系统在主动和被动条件下的全局图像,揭示了相边界的变化,并揭示了活性对不同液滴结构的影响。我们推导了有源LLPS系统的有效自由能,为我们的观察提供了定性的理解。我们的研究提出了一个非平衡相分离过程的基本模型,为LLPS和细胞内非平衡现象提供了重要的见解。
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来源期刊
Journal of Chemical Theory and Computation
Journal of Chemical Theory and Computation 化学-物理:原子、分子和化学物理
CiteScore
9.90
自引率
16.40%
发文量
568
审稿时长
1 months
期刊介绍: The Journal of Chemical Theory and Computation invites new and original contributions with the understanding that, if accepted, they will not be published elsewhere. Papers reporting new theories, methodology, and/or important applications in quantum electronic structure, molecular dynamics, and statistical mechanics are appropriate for submission to this Journal. Specific topics include advances in or applications of ab initio quantum mechanics, density functional theory, design and properties of new materials, surface science, Monte Carlo simulations, solvation models, QM/MM calculations, biomolecular structure prediction, and molecular dynamics in the broadest sense including gas-phase dynamics, ab initio dynamics, biomolecular dynamics, and protein folding. The Journal does not consider papers that are straightforward applications of known methods including DFT and molecular dynamics. The Journal favors submissions that include advances in theory or methodology with applications to compelling problems.
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