论文标题
通过不同方案的广泛的AB始于从头开始模拟，过量质子和氢氧化物在水中的准确扩散系数
Accurate diffusion coefficients of the excess proton and hydroxide in water via extensive ab initio simulations with different schemes
论文作者
论文摘要
[本文只能下载供个人使用。任何其他用途都需要事先获得作者和AIP发布的许可。本文发表在《化学物理学杂志》，157，024504（2022）中，可以在以下网址找到：https：//doi.org/10.1063/5.0093958] 尽管具有简单的分子公式，但在水的硅描述中获得精确的远非直接。它的许多非常奇特的特性非常难以捉摸，尤其是对以合理的计算成本进行溶剂化质子和氢氧化物的扩散系数的良好估计一直是迄今为止尚未解决的挑战。在这里，我在这里提出了几个异常长期的MD模拟的广泛结果，该模拟使用了出生的不同组合 - oppenheimer和2 $^\ MATHRM {nd} $ - 生成car-parinello md传播方法与不同的合奏（NVE和NVT）和恒温器，这些方法与这些方法相同，这表明了这些方法的功能，这些方法与rpbe的效果相同，这是一个功能，该方法与RP-d-D 3相互作用，而RP-d-d 3的功能是rp-d的功能。在溶剂化的h $ _3 $ o $^+$和OH $^ - $ ions中，以及对中性水的几种特性（例如液体的结构及其扩散和剪切粘度系数）的非常准确的描述。此外，我证明了$ d_ \ mathrm {h_3o^+} $和$ d_ \ mathrm {oh^ - } $的估计极大地取决于模拟长度，这对于以数百个picoseconds的顺序到达时标而是必要的，以获得可靠的结果。
[ This article may be downloaded for personal use only. Any other use requires prior permission of the author and AIP Publishing. This article appeared in The Journal of Chemical Physics, 157, 024504 (2022) and may be found at: https://doi.org/10.1063/5.0093958 ] Despite its simple molecular formula, obtaining an accurate in silico description of water is far from straightforward. Many of its very peculiar properties are quite elusive, and in particular obtaining good estimations of the diffusion coefficients of the solvated proton and hydroxide at a reasonable computational cost has been an unsolved challenge until now. Here I present extensive results of several unusually long ab initio MD simulations employing different combinations of the Born--Oppenheimer and 2$^\mathrm{nd}$-generation Car--Parrinello MD propagation methods with different ensembles (NVE and NVT) and thermostats, which show that these methods together with the RPBE-D3 functional provide a very accurate estimation of the diffusion coefficients of the solvated H$_3$O$^+$ and OH$^-$ ions, together with an extremely accurate description of several properties of neutral water (such as the structure of the liquid and its diffusion and shear viscosity coefficients). In addition, I show that the estimations of $D_\mathrm{H_3O^+}$ and $D_\mathrm{OH^-}$ depend dramatically on the simulation length, being necessary to reach timescales in the order of hundreds of picoseconds to obtain reliable results.
