Layer-by-Layer Formation of Oligoelectrolyte Multilayers: A Combined Experimental and Computational Study
Layer-by-Layer Formation of Oligoelectrolyte Multilayers: A Combined Experimental and Computational Study
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寡电解质多层的逐层形成：实验和计算相结合的研究
DOI：
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发表时间：
2014
期刊：
影响因子：
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通讯作者：
R. Klitzing
中科院分区：
文献类型：
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作者：
Samantha Micciulla;Pedro A Sánchez;Jens Smiatek;B. Qiao;M. Sega;A. Laschewsky;Christian Holm;R. Klitzing
对于第一次，结合实验制备和结果的全原子模拟的低聚电解质多层膜（OEM）制成的聚（二烯丙基二甲基氯化铵）/聚（苯乙烯磺酸钠盐）（PDADMAC/PSS）。逐层生长进行了浸渍二氧化硅基板在oligolipolysolate解决方案，并通过原子分子动力学模拟与协议，模仿实验过程的组装四层建模。OEM的厚度，表面粗糙度和吸附的oligoliprolyte链从这两种方法获得的量的测量进行了比较。模拟和实验结果之间的一个很好的协议被发现，由于这两种方法的固有限制，一些偏差。然而，从模拟中提取的信息的组合，以支持实验数据的分析，可以克服这样的限制，提高实验结果的解释。另一方面，由较慢的动力学，如不稳定的吸附层与周围环境的平衡后，占主导地位的过程，是遥不可及的模拟建模方法，但它们可以通过监测原位的oligoelectrolyte吸附在组装过程中进行调查。这证明了模拟和实验的协同使用如何将OEM特性的知识提高到分子尺度。
For the first time, the combination of experimental preparation and results of fully atomistic simulations of an oligoelectrolyte multilayer (OEM) made of poly(diallyl dimethyl ammonium chloride)/poly(styrene sulfonate sodium salt) (PDADMAC/PSS) is presented. The layer-by-layer growth was carried out by dipping silica substrates in oligoelectrolyte solutions and was modeled by means of atomistic molecular dynamics simulations with a protocol that mimics the experimental procedure up to the assembly of four layers. Measurements of OEM thickness, surface roughness and amount of adsorbed oligoelectrolyte chains obtained from both approaches are compared. A good agreement between simulated and experimental results was found, with some deviations due to intrinsic limitations of both methods. However, the combination of information extracted from simulations to support the analysis of experimental data can overcome such restrictions and improve the interpretation of experimental results. On the other hand, processes dominated by slower kinetics, such as the destabilization of adsorbed layers upon equilibration with the surrounding environment, are out of reach for the simulation modeling approach, but they can be investigated by monitoring in situ the oligoelectrolyte adsorption during the assembly process. This demonstrates how the synergistic use of simulation and experiments improves the knowledge of OEM properties down to the molecular scale.