Ab Initio Simulation of Liquid Water without Artificial High Temperature,Journal of Chemical Theory and Computation

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Ab Initio Simulation of Liquid Water without Artificial High Temperature
Journal of Chemical Theory and Computation ( IF 5.7 ) Pub Date : 2024-09-02 , DOI: 10.1021/acs.jctc.4c00650
Chenyu Wang ₁ , Wei Tian ₁ , Ke Zhou ₁

Affiliation

Comprehending the structure and dynamics of water is crucial in various fields, such as water desalination, ion separation, electrocatalysis, and biochemical processes. While reported works show that the ab initio molecular dynamics (AIMD) can accurately portray water’s structure, the artificial high temperature (AHT) from 120 to 30 K is needed to mimic the quantum nature of hydrogen-bond network from GGA, metaGGA to hybrid functionals. The AHT proves to be an inadequate approach for systems involving aqueous multiphase mixtures, such as water–solid interfaces and aqueous solutions. This is due to the activation of additional phonons in other phases, which can lead to an overestimation of the dynamics of nearby water molecules. In this work, we find that the regularized SCAN (rSCAN) functional effectively captures both the structure and dynamics of liquid water at ambient conditions without AHT. Moreover, rSCAN closely matches experimental results for the hydration structures of alkali, alkali earth, and halide ions. We anticipate that the versatile and accurate rSCAN functional will emerge as a key tool based on ab initio simulation for investigating chemical processes in aqueous environments.

中文翻译：

无需人工高温的液态水从头开始模拟

了解水的结构和动力学在海水淡化、离子分离、电催化和生化过程等各个领域都至关重要。虽然报道的工作表明从头算分子动力学 (AIMD) 可以准确地描绘水的结构，但需要 120 至 30 K 的人工高温 (AHT) 来模拟从 GGA、metaGGA 到混合泛函的氢键网络的量子性质。事实证明，对于涉及水性多相混合物的系统（例如水-固体界面和水溶液），AHT 方法并不适用。这是由于其他相中额外声子的激活，这可能导致对附近水分子动力学的高估。在这项工作中，我们发现正则化 SCAN (rSCAN) 函数可以在没有 AHT 的情况下有效地捕获环境条件下液态水的结构和动态。此外，rSCAN 与碱金属、碱土金属和卤离子的水合结构的实验结果非常吻合。我们预计，多功能且准确的 rSCAN 功能将成为基于从头模拟研究水环境中化学过程的关键工具。

更新日期：2024-09-02

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