论文标题
通过非平衡化学反应调整成核动力学
Tuning nucleation kinetics via nonequilibrium chemical reactions
论文作者
论文摘要
与热平衡处的流体不同，活系统中的生物分子混合物可以维持非平衡的稳态，在这种状态下，主动过程会改变组成分子的构象状态。尽管在这些系统中液 - 液相分离之间的质性相似性，但相分开动力学的不同程度尚不清楚。在这里，我们表明，不均匀的化学反应可以以与经典成核理论一致的方式改变液态 - 液相分离的成核动力学，但只能通过引入非质量室间张力来合理化。我们确定可以加速成核的条件，而不会改变能量或过饱和，从而破坏了快速成核和强驱动力之间的相关性，这是相位分离和在热平衡下自我组装的典型特征。
Unlike fluids at thermal equilibrium, biomolecular mixtures in living systems can sustain nonequilibrium steady states, in which active processes modify the conformational states of the constituent molecules. Despite qualitative similarities between liquid--liquid phase separation in these systems, the extent to which the phase-separation kinetics differ remains unclear. Here we show that inhomogeneous chemical reactions can alter the nucleation kinetics of liquid--liquid phase separation in a manner that is consistent with classical nucleation theory, but can only be rationalized by introducing a nonequilibrium interfacial tension. We identify conditions under which nucleation can be accelerated without changing the energetics or supersaturation, thus breaking the correlation between fast nucleation and strong driving forces that is typical of phase separation and self-assembly at thermal equilibrium.
