Tuning Nucleation Kinetics via Nonequilibrium Chemical Reactions
Tuning Nucleation Kinetics via Nonequilibrium Chemical Reactions
复制标题
通过非平衡化学反应调节成核动力学
DOI：
10.1103/physrevlett.130.128203
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发表时间：
2023
影响因子：
8.6
通讯作者：
Jacobs, William M.
中科院分区：
文献类型：
--
作者：
Cho, Yongick;Jacobs, William M.
与处于热平衡的流体不同，生命系统中的生物分子混合物可以维持非平衡稳态，其中活性过程修改组成分子的构象状态。尽管在这些系统中的液-液相分离之间的定性相似性，相分离动力学差异的程度仍然不清楚。在这里，我们表明，非均相化学反应可以改变成核动力学的液-液相分离的方式，是与经典的成核理论相一致，但只能通过引入非平衡界面张力合理化。我们确定的条件下，可以加速成核而不改变的能量或过饱和，从而打破了快速成核和强驱动力，这是典型的相分离和自组装在热平衡之间的相关性。
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.