Molecularly Informed Field Theories from Bottom-up Coarse-Graining
Molecularly Informed Field Theories from Bottom-up Coarse-Graining
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DOI：
10.1021/acsmacrolett.1c00013
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发表时间：
2021-04-22
影响因子：
7.015
通讯作者：
Fredrickson, Glenn H.
中科院分区：
文献类型：
--
作者：
Sherck, Nicholas;Shen, Kevin;Fredrickson, Glenn H.
具有介观结构或相共存的聚合物制剂由于不同的时间和长度尺度而难以使用原子粒子显式方法进行模拟，而基于场的模拟的预测能力受到在较粗尺度下指定相互作用的需要的阻碍（例如，卡参数）。为了克服这两个弱点，我们引入了一个自下而上的粗粒化方法，利用全原子分子动力学的分子通知粗糙的场论模型。具体来说，我们使用相对熵粗粒化参数化粒子模型，直接和分析转化为统计场理论。我们证明了这种方法的预测能力，通过复制实验含水聚（环氧乙烷）（PEO）的浊点曲线，没有参数适合实验数据。这种多尺度聚合物模拟的协同方法为重新探索各种聚合物溶液和熔体配方的相行为打开了大门。
Polymer formulations possessing mesostructures or phase coexistence are challenging to simulate using atomistic particle-explicit approaches due to the disparate time and length scales, while the predictive capability of field-based simulations is hampered by the need to specify interactions at a coarser scale (e.g., chi-parameters). To overcome the weaknesses of both, we introduce a bottom-up coarsegraining methodology that leverages all-atom molecular dynamics to molecularly inform coarser field-theoretic models. Specifically, we use relative-entropy coarse-graining to parametrize particle models that are directly and analytically transformable into statistical field theories. We demonstrate the predictive capability of this approach by reproducing experimental aqueous poly(ethylene oxide) (PEO) cloud-point curves with no parameters fit to experimental data. This synergistic approach to multiscale polymer simulations opens the door to de novo exploration of phase behavior across a wide variety of polymer solutions and melt formulations.