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文章背景与核心概要

传统的计算材料发现很大程度上依赖于基态能量，因为计算决定固态相稳定性的自由能需要复杂的系综平均。本文引入了热力学原子间势（TIP），这是一种将标准原子间势扩展为热力学一致的吉布斯自由能模型的创新方法。

通过使用 TIP[UMA]（基于通用势 UMA 实现）并利用自动微分技术处理温度和压力的响应，该方法成功计算了晶体状态方程，定位了相变（包括动态稳定相），并通过微调模拟了合金的溶解度极限和混溶间隙。最终，TIP 使自由能的获取变得像势能一样简便，为高通量、有限温材料发现铺平了道路。

Universal Thermodynamic Interatomic Potential for Crystalline Materials

arXiv: 2608.14502 [cond-mat.mtrl-sci]
Submitted: August 14, 2026
Authors: Juno Nam, Bowen Deng, Xiaochen Du, Luis Barroso-Luque, Benjamin Kurt Miller, Rafael Gómez-Bombarelli

📌 Summary

Traditional computational materials discovery relies heavily on ground-state energies because calculating free energies—which dictate solid-state phase stability—requires complex ensemble averages. This paper introduces the thermodynamic interatomic potential (TIP), a novel approach that extends standard interatomic potentials into thermodynamically consistent Gibbs free energy models.

Using TIP[UMA] (implemented via the universal potential UMA) and automatic differentiation for temperature and pressure responses, the method successfully computes crystal equations of state, locates phase transitions (including dynamically stabilized phases), and models alloy solubility limits and miscibility gaps through fine-tuning. Ultimately, TIP makes free energy as accessible as potential energy, paving the way for high-throughput, finite-temperature materials discovery.

传统计算材料发现严重依赖于基态能量，因为计算决定固态相稳定性的自由能需要复杂的系综平均。本文引入了热力学原子间势（TIP），这是一种将标准原子间势扩展为热力学一致的吉布斯自由能模型的创新方法。

通过使用 TIP[UMA]（通过通用势 UMA 实现）以及用于温度和压力响应的自动微分，该方法成功计算了晶体状态方程，定位了相变（包括动态稳定相），并通过微调模拟了合金的溶解度极限和混溶间隙。最终，TIP 使自由能的获取变得像势能一样简便，为高通量、有限温材料发现铺平了道路。

Abstract

Free energies govern solid-state phase stability, yet computational materials discovery still relies largely on ground-state energies because free energy calculations require ensemble averages. We introduce the thermodynamic interatomic potential (TIP), which extends an interatomic potential from its static energy to a thermodynamically consistent Gibbs free energy model, with thermodynamic responses following from temperature and pressure by automatic differentiation. We implement TIP[UMA] using the universal potential UMA, train it on free energies from quasi-harmonic to molecular dynamics fidelity, and calibrate it to higher-resolution calculations or experiment. From a single evaluation, it returns the equation of state of a crystal and locates phase transitions among competing branches, including dynamically stabilized phases. Fine-tuning extends the model to alloy solubility limits and miscibility gaps. TIP makes the free energy as accessible as the potential energy, opening finite-temperature phase stability to high-throughput discovery.

自由能控制着固态相稳定性，然而计算材料发现仍然很大程度上依赖于基态能量，因为自由能计算需要系综平均。我们引入了热力学原子间势（TIP），它将原子间势从静态能量扩展为热力学一致的吉布斯自由能模型，其热力学响应通过自动微分由温度和压力得出。我们使用通用势 UMA 实现了 TIP[UMA]，根据从准谐波到分子动力学精度的自由能对其进行训练，并针对更高分辨率的计算或实验对其进行校准。通过单次评估，它就能返回晶体的状态方程，并定位竞争分支之间的相变（包括动态稳定相）。微调将该模型扩展到了合金溶解度极限和混溶间隙。TIP 使自由能像势能一样易于获取，为有限温相稳定性的高通量发现打开了大门。

Article Metadata

  • Primary Subject: Materials Science (cond-mat.mtrl-sci)
  • Secondary Subjects: Statistical Mechanics (cond-mat.stat-mech), Artificial Intelligence (cs.AI), Machine Learning (cs.LG), Chemical Physics (physics.chem-ph)
  • DOI: 10.48550/arXiv.2608.14502
  • 主要学科： 材料科学 (cond-mat.mtrl-sci)
  • 次要学科： 统计力学 (cond-mat.stat-mech)、人工智能 (cs.AI)、机器学习 (cs.LG)、化学物理 (physics.chem-ph)
  • DOI： 10.48550/arXiv.2608.14502

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