arXiv:2603.25373cs.LG2026-03

让机器学习势能模型感知能量曲率,更准预测实验现象。

Hessian-informed machine learning interatomic potential towards bridging theory and experiments

  • 引入海森矩阵监督训练,提升模型对能量曲面局部曲率的感知能力。
  • 提出高效训练协议HINT,减少99%以上昂贵的海森标签需求。
  • 适用于数据稀少、强非简谐体系,可精准预测相变与超导温度。

分子与材料的势能面局部曲率对从第一性原理预测某些实验可观测物至关重要,但对复杂体系仍难以实现。本文提出一种海森矩阵感知的机器学习原子间势能模型(Hi-MLIP),可靠捕捉曲率信息,从而准确分析相关热力学与动力学现象。为使海森监督实用化,开发了高效训练协议HINT,实现海森标签需求降低2至4个数量级。HINT融合海森预训练、构型采样、课程学习与随机投影海森损失等关键技术。在HINT支持下,Hi-MLIP显著提升过渡态搜索性能,并在数据稀缺场景中使吉布斯自由能预测接近化学精度。该框架还可准确处理强非简谐氢化物,重现声子重整化与超导临界温度,与实验高度吻合,同时规避了非简谐计算的计算瓶颈。结果表明,该方法为提升机器学习势能模型的曲率感知能力提供了可行路径,广泛连接模拟与实验观测。

原文摘要 · Abstract (English)

Local curvature of potential energy surfaces is critical for predicting certain experimental observables of molecules and materials from first principles, yet it remains far beyond reach for complex systems. In this work, we introduce a Hessian-informed Machine Learning Interatomic Potential (Hi-MLIP) that captures such curvature reliably, thereby enabling accurate analysis of associated thermodynamic and kinetic phenomena. To make Hessian supervision practically viable, we develop a highly efficient training protocol, termed Hessian INformed Training (HINT), achieving two to four orders of magnitude reduction for the requirement of expensive Hessian labels. HINT integrates critical techniques, including Hessian pre-training, configuration sampling, curriculum learning and stochastic projection Hessian loss. Enabled by HINT, Hi-MLIP significantly improves transition-state search and brings Gibbs free-energy predictions close to chemical accuracy especially in data-scarce regimes. Our framework also enables accurate treatment of strongly anharmonic hydrides, reproducing phonon renormalization and superconducting critical temperatures in close agreement with experiment while bypassing the computational bottleneck of anharmonic calculations. These results establish a practical route to enhancing curvature awareness of machine learning interatomic potentials, bridging simulation and experimental observables across a wide range of systems.

机器学习势能海森矩阵非简谐超导

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