Phase separation in fluids with many interacting components
Phase separation in fluids with many interacting components
复制标题
具有许多相互作用组分的流体中的相分离
DOI：
10.1073/pnas.2108551118
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发表时间：
2021
期刊：
影响因子：
--
通讯作者：
Brenner, Michael P.
中科院分区：
文献类型：
--
作者：
Shrinivas, Krishna;Brenner, Michael P.
自然系统中的流体（如细胞的细胞质）通常包含数千种分子种类，这些分子种类被组织成多个共存相，从而实现多样化和特定的功能。众多分子物种之间的相互作用如何编码不同的涌现阶段尚不清楚。在这里，我们利用随机矩阵理论和统计物理学的方法来描述具有许多物质的流体混合物的涌现相行为，这些物质的相互作用是从基础分布中随机得出的。通过数值模拟和稳定性分析，我们表明这些混合物表现出阶段性相分离动力学，并具有稳态下具有不同组成的多个共存相的特征。随机矩阵理论预测共存相的数量，并通过不同组件数量和相互作用参数的模拟进行验证。令人惊讶的是，该模型预测了从动力学考虑得出的相数上限，该上限远低于吉布斯相规则的限制，吉布斯相规则是从平衡热力学约束中获得的。我们设计了对组件数量和共存相之间的线性或非单调缩放关系进行编码的系综，并通过模拟和理论进行验证。最后，受生物系统中相似情况的启发，我们表明，通过化学反应进行组分的非平衡周转可以在不改变总体流体成分的情况下调节稳态共存相的数量。总之，我们的研究提供了一个模型框架，描述了具有许多相互作用成分的液体混合物的新兴动态和稳态相行为。
Fluids in natural systems, like the cytoplasm of a cell, often contain thousands of molecular species that are organized into multiple coexisting phases that enable diverse and specific functions. How interactions between numerous molecular species encode for various emergent phases is not well understood. Here, we leverage approaches from random-matrix theory and statistical physics to describe the emergent phase behavior of fluid mixtures with many species whose interactions are drawn randomly from an underlying distribution. Through numerical simulation and stability analyses, we show that these mixtures exhibit staged phase-separation kinetics and are characterized by multiple coexisting phases at steady state with distinct compositions. Random-matrix theory predicts the number of coexisting phases, validated by simulations with diverse component numbers and interaction parameters. Surprisingly, this model predicts an upper bound on the number of phases, derived from dynamical considerations, that is much lower than the limit from the Gibbs phase rule, which is obtained from equilibrium thermodynamic constraints. We design ensembles that encode either linear or nonmonotonic scaling relationships between the number of components and coexisting phases, which we validate through simulation and theory. Finally, inspired by parallels in biological systems, we show that including nonequilibrium turnover of components through chemical reactions can tunably modulate the number of coexisting phases at steady state without changing overall fluid composition. Together, our study provides a model framework that describes the emergent dynamical and steady-state phase behavior of liquid-like mixtures with many interacting constituents.
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DOI：
10.1098/rsif.2021.0255
发表时间：
2021-06
期刊：
Journal of the Royal Society, Interface
影响因子：
--
作者：
Kirschbaum J;Zwicker D
通讯作者：
Zwicker D
影响因子：
21.8
作者：
Simon JR;Carroll NJ;Rubinstein M;Chilkoti A;López GP
通讯作者：
López GP
影响因子：
8.6
作者：
Sollich, P;Cates, ME
通讯作者：
Cates, ME
影响因子：
3.4
作者：
Jacobs, William M.;Frenkel, Daan
通讯作者：
Frenkel, Daan
影响因子：
4
作者：
Fei, Jingyi;Jadaliha, Mahdieh;Ha, Taekjip
通讯作者：
Ha, Taekjip