Chubak Iurii, Likos Christos N, Egorov Sergei A
Faculty of Physics, University of Vienna, Boltzmanngasse 5, A-1090 Vienna, Austria.
Sorbonne Université CNRS, Physico-Chimie des Électrolytes et Nanosystèmes Interfaciaux, F-75005 Paris, France.
J Phys Chem B. 2021 May 13;125(18):4910-4923. doi: 10.1021/acs.jpcb.1c01953. Epub 2021 May 3.
We apply a hierarchy of multiscale modeling approaches to investigate the structure of ring polymer solutions under planar confinement. In particular, we employ both monomer-resolved (MR-DFT) and a coarse-grained (CG-DFT) density functional theories for fully flexible ring polymers, with the former based on a flexible tangent hard-sphere model and the latter based on an effective soft-colloid representation, to elucidate the ring polymer organization within slits of variable width in different concentration regimes. The predicted monomer and polymer center-of-mass densities in confinement, as well as the surface tension at the solution-wall interface, are compared to explicit molecular dynamics (MD) simulations. The approaches yield quantitative (MR-DFT) or semiquantitative (CG-DFT) agreement with MD. In addition, we provide a systematic comparison between confined linear and ring polymer solutions. When compared to their linear counterparts, the rings are found to feature a higher propensity to structure in confinement that translates into a distinct shape of the depletion potentials between two walls immersed into a polymer solution. The depletion potentials that we extract from CG-DFT and MR-DFT are in semiquantitative agreement with each other. Overall, we find consistency among all approaches as regards the shapes, trends, and qualitative characteristics of density profiles and depletion potentials induced on hard walls by linear and cyclic polymers.
我们应用多层次的多尺度建模方法来研究平面受限条件下环形聚合物溶液的结构。具体而言,对于完全柔性的环形聚合物,我们采用了单体分辨(MR-DFT)和粗粒化(CG-DFT)密度泛函理论,前者基于柔性切线硬球模型,后者基于有效的软胶体表示,以阐明不同浓度区域中不同宽度狭缝内的环形聚合物排列。将受限条件下预测的单体和聚合物质心密度以及溶液-壁界面处的表面张力与显式分子动力学(MD)模拟结果进行比较。这些方法与MD模拟结果在定量(MR-DFT)或半定量(CG-DFT)上达成一致。此外,我们对受限的线性和环形聚合物溶液进行了系统比较。与线性聚合物相比,发现环形聚合物在受限条件下具有更高的结构化倾向,这转化为浸入聚合物溶液中的两壁之间耗尽势的独特形状。我们从CG-DFT和MR-DFT中提取的耗尽势彼此半定量一致。总体而言,我们发现在所有方法中,线性和环状聚合物在硬壁上引起的密度分布和耗尽势的形状、趋势和定性特征方面具有一致性。