量化长程力对水中晶体成核的相关性

IF 5.5 1区 化学 Q2 CHEMISTRY, PHYSICAL
Renjie Zhao, Ziyue Zou, John D. Weeks* and Pratyush Tiwary*, 
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引用次数: 0

摘要

了解水溶液中的成核过程对于从材料科学到生物物理学等众多领域都具有重要意义。水溶液中由溶剂介导的复杂相互作用阻碍了简单物理图像的发展,无法阐明成核过程中不同相互作用的作用。在这项研究中,我们利用了三种互补技术来厘清短程和长程相互作用在溶剂介导的成核过程中所起的作用。具体来说,我们采用的第一种方法是局部分子场(LMF)理论,对长程库仑静电进行重规范化。其次,我们使用好脾气元动力学来加速受短程相互作用支配的罕见事件。第三,我们采用了基于深度学习的状态预测信息瓶颈方法,来分析由 LMF 处理与好温元动力学耦合得到的成核过程的反应坐标。我们发现,短程相互作用在很大程度上可以捕捉到两步成核机制,而长程相互作用则进一步促进了环境条件下主晶态的稳定性。此外,通过分析 LMF-元动力学联合处理所得到的反应坐标,我们发现了不同时间尺度上的波动,突出了在考虑陨变时长程相互作用的必要性。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Quantifying the Relevance of Long-Range Forces for Crystal Nucleation in Water

Quantifying the Relevance of Long-Range Forces for Crystal Nucleation in Water

Quantifying the Relevance of Long-Range Forces for Crystal Nucleation in Water

Understanding nucleation from aqueous solutions is of fundamental importance in a multitude of fields, ranging from materials science to biophysics. The complex solvent-mediated interactions in aqueous solutions hamper the development of a simple physical picture, elucidating the roles of different interactions in nucleation processes. In this work, we make use of three complementary techniques to disentangle the role played by short- and long-range interactions in solvent-mediated nucleation. Specifically, the first approach we utilize is the local molecular field (LMF) theory to renormalize long-range Coulomb electrostatics. Second, we use well-tempered metadynamics to speed up rare events governed by short-range interactions. Third, the deep learning-based State Predictive Information Bottleneck approach is employed in analyzing the reaction coordinate of the nucleation processes obtained from the LMF treatment coupled with well-tempered metadynamics. We find that the two-step nucleation mechanism can largely be captured by the short-range interactions, while the long-range interactions further contribute to the stability of the primary crystal state under ambient conditions. Furthermore, by analyzing the reaction coordinate obtained from the combined LMF-metadynamics treatment, we discern the fluctuations on different time scales, highlighting the need for long-range interactions when accounting for metastability.

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来源期刊
Journal of Chemical Theory and Computation
Journal of Chemical Theory and Computation 化学-物理:原子、分子和化学物理
CiteScore
9.90
自引率
16.40%
发文量
568
审稿时长
1 months
期刊介绍: The Journal of Chemical Theory and Computation invites new and original contributions with the understanding that, if accepted, they will not be published elsewhere. Papers reporting new theories, methodology, and/or important applications in quantum electronic structure, molecular dynamics, and statistical mechanics are appropriate for submission to this Journal. Specific topics include advances in or applications of ab initio quantum mechanics, density functional theory, design and properties of new materials, surface science, Monte Carlo simulations, solvation models, QM/MM calculations, biomolecular structure prediction, and molecular dynamics in the broadest sense including gas-phase dynamics, ab initio dynamics, biomolecular dynamics, and protein folding. The Journal does not consider papers that are straightforward applications of known methods including DFT and molecular dynamics. The Journal favors submissions that include advances in theory or methodology with applications to compelling problems.
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