论文标题
电荷对称破裂的复杂共隔离
Charge symmetry broken complex coacervation
论文作者
论文摘要
液态液相分离已成为化学物理学中的重要范式之一，以及带电的大分子系统的生物物理学。我们阐明了基于电荷调节的平衡相分离机制，即在理想化的宏观系统中由pH控制的质子 - 替代平衡平衡，该系统可以用作简单共核的代理。首先，低密度密度功能的计算揭示了通过离子吸附在相邻宏观上结合的两粒子构型的优势。然后是在Debye-Hückel上解决的二元细胞模型以及完整的非线性Poisson-Boltzmann级别，将电荷对称破坏揭示为诱导低密度相和高密度相之间的相位分离，这是pH的函数。这些结果可以识别为化学相同宏之间的电荷对称性损坏的复杂共凝聚。
Liquid-liquid phase separation has emerged as one of the important paradigms in the chemical physics as well as biophysics of charged macromolecular systems. We elucidate an equilibrium phase separation mechanism based on charge regulation, i.e., protonation-deprotonation equilibria controlled by pH, in an idealized macroion system which can serve as a proxy for simple coacervation. First, a low-density density-functional calculation reveals the dominance of two-particle configurations coupled by ion adsorption on neighboring macroions. Then a binary cell model, solved on the Debye-Hückel as well as the full nonlinear Poisson-Boltzmann level, unveils the charge-symmetry breaking as inducing the phase separation between low- and high-density phases as a function of pH. These results can be identified as a charge symmetry broken complex coacervation between chemically identical macroions.
