Theory of Microphase Separation in Concentrated Solutions of Sequence-Specific Charged Heteropolymers
Theory of Microphase Separation in Concentrated Solutions of Sequence-Specific Charged Heteropolymers
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DOI：
10.1021/acs.macromol.2c00008
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发表时间：
2022-06
期刊：
影响因子：
5.5
通讯作者：
Siao-Fong Li;M. Muthukumar
中科院分区：
文献类型：
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作者：
Siao-Fong Li;M. Muthukumar
我们提出了一个具有特定化学序列的带电柔性杂聚物浓多组分溶液相行为的一般理论。使用场理论的形式主义，我们占了序列特异性，静电和货车的所有组成物种之间的相互作用，和拓扑结构的相关性在系统中的所有杂聚物链。我们的亥姆霍兹自由能的系统的一般表达式是在各种组件的密度分布方面，是一个明确的功能的杂聚物，聚合物浓度，盐浓度，各种单体和溶剂之间的化学失配的序列特异性，和温度。我们说明了我们的一般理论的背景下，内在无序的蛋白质的自组装考虑解决方案的序列特异性带电中性杂聚物。对于所考虑的杂聚物，该系统表现出微相分离。有序-无序过渡的边界和相对稳定性的典型的微相分离的形态（层状，圆柱形，球形）的弱偏析极限作为序列，聚合物浓度，化学失配参数，和盐浓度的函数。提出了杂聚物序列与形态图之间的唯一映射。推导出的一般理论具有广泛的适用性，在解决序列效应的热力学行为的任何多组分系统包含灵活的杂聚物。
We present a general theory of the phase behavior of concentrated multicomponent solutions of charged flexible heteropolymers with specific chemical sequences. Using a field theoretic formalism, we have accounted for sequence specificity, electrostatic and van der Waals interactions among all constituent species, and topological correlations among all heteropolymer chains in the system. Our general expression for the Helmholtz free energy of the system is in terms of density profiles of the various components and is an explicit function of the sequence specificity of the heteropolymers, polymer concentration, salt concentration, chemical mismatch among the various monomers and solvent, and temperature. We illustrate our general theory in the context of the self-assembly of intrinsically disordered proteins by considering solutions of sequence-specific charged-neutral heteropolymers. For the heteropolymers under consideration, the system exhibits microphase separation. The boundaries of order–disorder transition and the relative stabilities of the canonical microphase-separated morphologies (lamellar, cylindrical, and spherical) are presented in the weak segregation limit as functions of sequence, polymer concentration, chemical mismatch parameters, and salt concentration. Unique mapping between heteropolymer sequence and morphology diagram is presented. The derived general theory is of broad applicability in addressing sequence effects on the thermodynamic behavior of any multicomponent system containing flexible heteropolymers.