论文标题
深入了解Fe $ _3 $ o $ _4 $（001）的界面和通过多尺度分子动力学模拟的水叠加仪
Insight into the interface between Fe$_3$O$_4$(001) surface and water overlayers through multiscale molecular dynamics simulations
论文作者
论文摘要
在这项工作中，我们通过组合几种理论方法（从混合功能方法（HSE06）到密度功能功能紧密结合（DFTB）到分子力学（MM），我们研究了Fe $ _3 $ o $ $ _4 $（001）表面/水接口。首先，我们评估了DFTB方法的准确性，以正确复制HSE06的结构细节和能量学以及可用的实验数据，以吸附孤立的水，二聚体，三聚体等，直至水单层。其次，我们构建了两种可能的构造的第二个和第三个叠层器，并使用DFTB进行分子动力学模拟，监视水取向，H键网络以及有序的水结构形成。为了使我们的型号更加现实，然后我们在Fe $ _3 $ o $ $ _4 $（001）的表面平板模型的顶部建造了一个12 nm厚的水多层，我们通过MM Molecular Dynamics进行了调查。水层的结构是通过对这种大型MM模型的长MM-MD运行的原子位置的分析所揭示的，可扩展到约6-7Å，并与对水的三层模型观察到的原子位置相比。但是，由于对模型参数化的Fe-oH2距离的描述不佳，MM和DFTB MD模拟显示出一些差异。
In this work we investigate the Fe$_3$O$_4$(001) surface/water interface by combining several theoretical approaches, ranging from a hybrid functional method (HSE06) to density-functional tight-binding (DFTB) to molecular mechanics (MM). First, we assess the accuracy of the DFTB method to reproduce correctly HSE06 results on structural details and energetics and available experimental data for the adsorption of isolated water, dimers, trimers, etc. up to a water monolayer. Secondly, we build two possible configurations of a second and a third overlayer and perform molecular dynamics simulations with DFTB, monitoring the water orientation, the H-bond network, and ordered water structures formation. To make our models more realistic, we then build a 12-nm thick water multilayer on top of the Fe$_3$O$_4$(001) surface slab model, which we investigate through MM molecular dynamics. The water layers structuring, revealed by the analysis of the atomic positions from a long MM-MD run for this large MM model, extends up to about 6-7 Å and nicely compares with that observed for a water trilayer model. However, MM and DFTB MD simulations show some discrepancy due to the poor description of the Fe--OH2 distance in MM that calls for further work in the parametrization of the model.
