Predicting surfactant phase behavior with a molecularly informed field theory
Predicting surfactant phase behavior with a molecularly informed field theory
复制标题
用分子信息场理论预测表面活性剂相行为
DOI：
10.1016/j.jcis.2023.01.015
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发表时间：
2023
影响因子：
9.9
通讯作者：
Fredrickson, Glenn H.
中科院分区：
文献类型：
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作者：
Shen, Kevin;Nguyen, My;Sherck, Nicholas;Yoo, Brian;Köhler, Stephan;Speros, Joshua;Delaney, Kris T.;Shell, M. Scott;Fredrickson, Glenn H.
假设表面活性剂和自组装的计算研究是具有挑战性的，因为1）模型需要反映化学特定的相互作用，2）自组装结构很难与传统的分子动力学平衡。我们建议克服这些挑战与多尺度模拟方法，其中相对熵最小化转移化学详细信息从全原子（AA）模拟粗粒度（CG）模型，可以使用场论方法模拟。场论模拟不受扩散等固有物理时间尺度的限制，并且允许通过自由能量最小化实现严格的平衡。这种方法应该使研究的属性是很难获得基于粒子的simulation.Simulation工作我们应用此工作流程十二烷基硫酸钠。为了确保化学保真度，我们提出了一个AA力场校准界面张力实验。我们产生CG模型从AA模拟轨迹，并表明，基于粒子和场理论的CG模型的模拟再现AA模拟和实验measurement.FindingsThe工作流捕捉复杂的平衡的相互作用，最终描述的一个原子模型的多组分系统。由此产生的CG模型可以研究复杂的3D相位，如双重或交替的陀螺，并再现盐对聚集数和形状转变等属性的影响。
HypothesisThe computational study of surfactants and self-assembly is challenging because 1) models need to reflect chemistry-specific interactions, and 2) self-assembled structures are difficult to equilibrate with conventional molecular dynamics. We propose to overcome these challenges with a multiscale simulation approach where relative entropy minimization transfers chemically-detailed information from all-atom (AA) simulations to coarse-grained (CG) models that can be simulated using field-theoretic methods. Field-theoretic simulations are not limited by intrinsic physical time scales like diffusion and allow for rigorous equilibrationviafree energy minimization. This approach should enable the study of properties that are difficult to obtain by particle-based simulations.Simulation WorkWe apply this workflow to sodium dodecylsulfate. To ensure chemical fidelity we present an AA force field calibrated against interfacial tension experiments. We generate CG models from AA simulation trajectories and show that particle-based and field-theoretic simulations of the CG model reproduce AA simulations and experimental measurements.FindingsThe workflow captures the complex balance of interactions in a multicomponent system ultimately described by an atomistic model. The resulting CG models can study complex 3D phases like double or alternating gyroids, and reproduce salt effects on properties like aggregation number and shape transitions.