Predicting Solid-Liquid Interfacial Free Energy with Realistic Interfacial Density Wave Amplitudes.

IF 5.7 1区化学 Q2 CHEMISTRY, PHYSICAL

Journal of Chemical Theory and Computation Pub Date : 2025-07-22 DOI:10.1021/acs.jctc.5c00656

Ya-Shen Wang,Zun Liang,Yang Yang

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Abstract

This study presents a theoretical framework for predicting the solid-liquid interfacial free energy (γ) of FCC systems using the two-mode Ginzburg-Landau (GL) model, refined with atomistic simulation data to generate more accurate density wave amplitude profiles. The analysis focuses on Lennard-Jones (LJ) systems along the p-T two-phase coexistence boundary. Equilibrium molecular dynamics simulations and the analytical minimization methods are employed to obtain the interfacial density wave amplitude profiles, which serve as inputs for the GL model to predict γ and its anisotropy. The predicted γ values strongly agree with previous benchmark computational studies, with a level of accuracy that surpasses prior predictions using either the GL or phase-field crystal models. The results demonstrate that the current two-mode GL model for FCC solid-liquid interfaces (SLIs) is computationally efficient and quantitatively reliable. It could provide valuable insight into the key factors governing the magnitude and anisotropy of γ and offer theoretical guidance for precisely tuning these properties. To further enhance predictive accuracy, refinements to the variational procedure used in the two-mode SLI free energy functionals are suggested, and potential extensions to the GL model are proposed.

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用实际界面密度波振幅预测固液界面自由能。

本研究提出了一个理论框架，利用双模Ginzburg-Landau （GL）模型预测FCC系统的固液界面自由能（γ），并用原子模拟数据进行了改进，以产生更精确的密度波振幅分布图。重点分析了沿p-T两相共存边界的Lennard-Jones （LJ）体系。利用平衡分子动力学模拟和解析最小化方法获得界面密度波幅分布，作为GL模型预测γ及其各向异性的输入。预测的γ值与先前的基准计算研究非常一致，其精度水平超过了使用GL或相场晶体模型的先前预测。结果表明，现有的FCC固液界面双模GL模型计算效率高，定量可靠。它可以为控制γ的大小和各向异性的关键因素提供有价值的见解，并为精确调整这些性质提供理论指导。为了进一步提高预测精度，对双模SLI自由能泛函中的变分过程进行了改进，并对GL模型提出了潜在的扩展。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

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Theory and Computation invites new and original contributions with the understanding that, if accepted, they will not be published elsewhere.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.