arXiv:2512.03974physics.comp-phcs.LG2025-12被引 3

用热力学理论修正机器学习势的相变温度,让模拟更贴近实验。

Refining Machine Learning Potentials through Thermodynamic Theory of Phase Transitions

  • 通过可微轨迹重加权,直接优化相变自由能差以校准相图
  • 对钛的相图修正至实验值误差在0.1开以内,液态扩散系数也提升
  • 不依赖具体模型,适用于多组分及固-固/固-液相变

基础机器学习势可突破经典力场在精度与迁移性上的局限,通过分子动力学模拟提供材料行为的微观洞察,显著加速材料设计与发现。然而,参考数据覆盖不足且系统性偏差影响模型预测质量,常导致相变温度预测误差达数百开。为此,本文提出一种自上而下的微调策略,直接将错误预测的相变温度校准至实验值。该方法基于可微轨迹重加权算法,最小化不同相在实验目标压强和温度下的自由能差。我们在高达5 GPa压力范围内的纯钛相图上验证了该方法,使计算结果与实验值匹配误差小于0.1开,并改善了液态扩散常数。该方法具备模型无关性,适用于含固-固、固-液相变的多组分体系,且兼容对其他实验性质的自上而下训练。因此,该方法可作为构建高精度应用特定及基础型机器学习势的关键步骤。

原文摘要 · Abstract (English)

Foundational Machine Learning Potentials can resolve the accuracy and transferability limitations of classical force fields. They enable microscopic insights into material behavior through Molecular Dynamics simulations, which can crucially expedite material design and discovery. However, insufficiently broad and systematically biased reference data affect the predictive quality of the learned models. Often, these models exhibit significant deviations from experimentally observed phase transition temperatures, in the order of several hundred kelvins. Thus, fine-tuning is necessary to achieve adequate accuracy in many practical problems. This work proposes a fine-tuning strategy via top-down learning, directly correcting the wrongly predicted transition temperatures to match the experimental reference data. Our approach leverages the Differentiable Trajectory Reweighting algorithm to minimize the free energy differences between phases at the experimental target pressures and temperatures. We demonstrate that our approach can accurately correct the phase diagram of pure Titanium in a pressure range of up to 5 GPa, matching the experimental reference within tenths of kelvins and improving the liquid-state diffusion constant. Our approach is model-agnostic, applicable to multi-component systems with solid-solid and solid-liquid transitions, and compliant with top-down training on other experimental properties. Therefore, our approach can serve as an essential step towards highly accurate application-specific and foundational machine learning potentials.

机器学习势相变模拟热力学材料模拟

Thank you to arXiv for use of its open access interoperability. PaperDance 不是 arXiv 官方产品;中文卡片由大模型生成,请以原文为准。