论文标题

在非理想化学反应网络和相分离上

On non-ideal chemical-reaction networks and phase separation

论文作者

Miangolarra, Ander Movilla, Castellana, Michele

论文摘要

化学反应网络(CRN)的大部分理论都是在理想解决极限中发展的,即溶质之间的相互作用可以忽略不计。但是,在生物细胞和软物理学中存在各种现象,似乎偏离了理想的行为。特别惊人的是液态液相分离的情况,这通常是由颗粒间相互作用引起的。在这里,我们在理想CRN的领域重新审视了许多已知结果,并将其推广并使其适应源自给定的自由能的溶质之间的任意相互作用。其中是复杂平衡网络的稳态概率分布和Lyapunov函数的形式,其中所有化学复合物的创建和an灭率均等于CRN中的反应物或产物。最后,我们基于与平衡热力学相似的基本原理的最小化基于这种Lyapunov功能的最小化,为复杂平衡的反应扩散溶液绘制相图,但对于可能在稳态下维持非平衡化学电流的系统。然而,我们发现复杂平衡的网络不足以在稳定状态下创建扩散电流。

Much of the theory on chemical-reaction networks (CRNs) has been developed in the ideal-solution limit, where interactions between the solutes are negligible. However, there is a large variety of phenomena in biological cells and soft-matter physics which appear to deviate from the ideal-solution behaviour. Particularly striking is the case of liquid-liquid phase separation, which is typically caused by inter-particle interactions. Here, we revisit a number of known results in the domain of ideal CRNs, and we generalise and adapt them to arbitrary interactions between the solutes which stem from a given free energy. Among these is the form of the steady-state probability distribution and Lyapunov functions for complex-balanced networks, where the creation and annihilation rates are equal for all chemical complexes which appear as reactants or products in the CRN. Finally, we draw a phase diagram for complex-balanced reaction-diffusion solutions based on the minimisation of such Lyapunov function with a rationale similar to that of equilibrium thermodynamics, but for systems that may sustain non-equilibrium chemical currents at steady state. Nevertheless, we find that complex-balanced networks are not sufficient to create diffusion currents at steady state.

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