论文标题
从两个极端的界面氢键动力学重新审视空气水接口的厚度
Revisiting the Thickness of the Air-Water Interface from Two Extremes of Interface Hydrogen Bond Dynamics
论文作者
论文摘要
由于其独特的特性，例如二维氢键（HB）网络（HB）网络，并且与大量水相比，空气水界面在科学的许多方面都起着至关重要的作用。但是，准确地确定界面和大量水的边界，即空气水接口的厚度，仍然挑战实验者。已经开发了各种基于仿真的方法来估计厚度，在大约3--10（Angstrom）的范围内收敛。在这项研究中，我们介绍了一种新的方法，该方法基于密度基于功能理论的分子动力学和深度潜在的分子动力学模拟，以测量空气水接口厚度，并基于先前的研究提供了不同的视角。为了捕获空气水接口中的现实HB动力学，获得了接口HB动力学的两个极端场景：一个低估了接口HB动力学，而另一个则高估了它。令人惊讶的是，我们的结果表明，随着空气水接口的厚度增加到4（Angstrom），界面HB动力学都会收敛。这种收敛点表示了逼真的界面厚度，也通过我们对空气水接口处的OH strave和自由OH动力学的计算来验证。
The air-water interface plays a crucial role in many aspects of science, because of its unique properties, such as a two-dimensional hydrogen bond (HB) network and completely different HB dynamics compared to bulk water. However, accurately determining the boundary of interfacial and bulk water, that is, the thickness of the air-water interface, still challenges experimentalists. Various simulation-based methods have been developed to estimate the thickness, converging on a range of approximately 3--10 (Angstrom). In this study, we introduce a novel approach, grounded in density functional theory-based molecular dynamics and deep potential molecular dynamics simulations, to measure the air-water interface thickness, offering a different perspective based on prior research. To capture realistic HB dynamics in the air-water interface, two extreme scenarios of the interface HB dynamics are obtained: one underestimates the interface HB dynamics, while the other overestimates it. Surprisingly, our results suggest that the interface HB dynamics in both scenarios converges as the thickness of the air-water interface increases to 4 (Angstrom). This convergence point, indicative of the realistic interface thickness, is also validated by our calculation of anisotropic decay of OH stretch and the free OH dynamics at the air-water interface.
