通过分子跃迁控制共存相的组成
Controlling composition of coexisting phases via molecular transitions
摘要：
相分离和不同分子状态之间的转变在活细胞中普遍存在。这种转变可以由局部平衡热力学或由生物燃料控制的主动过程来控制。在热力学平衡和由于燃料的存在而破坏分子转变速率的细致平衡的情况之间，具有分子转变的相分离系统的行为如何不同，这在很大程度上仍未被探索。在这里，我们提出了一个模型的相分离的三元混合物，其中两个组件可以相互转换。在热力学平衡下，我们发现分子转变可以引起较低的溶解温度，从而导致可重入相行为。此外，我们发现一个不连续的热力学相变的液滴相的组成，如果这两个转换分子吸引自己具有类似的相互作用强度。打破详细的平衡的分子过渡导致准不连续的变化，通过改变燃料量为一个更大的范围内的分子间相互作用的液滴组成。我们的研究结果表明，具有分子转变的相分离提供了一种通用的机制，通过液滴组成的不连续开关来控制细胞内和合成冷凝物的性质。
英文摘要：
Phase separation and transitions among different molecular states are ubiquitous in living cells. Such transitions can be governed by local equilibrium thermodynamics or by active processes controlled by biological fuel. It remains largely unexplored how the behavior of phase-separating systems with molecular transitions differs between thermodynamic equilibrium and cases where detailed balance of the molecular transition rates is broken due to the presence of fuel. Here, we present a model of a phase-separating ternary mixture where two components can convert into each other. At thermodynamic equilibrium, we find that molecular transitions can give rise to a lower dissolution temperature and thus reentrant phase behavior. Moreover, we find a discontinuous thermodynamic phase transition in the composition of the droplet phase if both converting molecules attract themselves with similar interaction strength. Breaking detailed-balance of the molecular transition leads to quasi-discontinuous changes in droplet composition by varying the fuel amount for a larger range of inter-molecular interactions. Our findings showcase that phase separation with molecular transitions provides a versatile mechanism to control properties of intra-cellular and synthetic condensates via discontinuous switches in droplet composition.
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