arXiv:2604.13897cs.LGphysics.comp-ph2026-04

构建首个分子晶体机器学习势数据库,支持高精度模拟多晶型行为。

MolCryst-MLIPs: A Machine-Learned Interatomic Potentials Database for Molecular Crystals

  • 基于自动化流程训练9种分子晶体的精细调优机器学习势。
  • 能量和力误差均低于0.15 kJ/mol/atom与0.65 kJ/mol/Å,优于基线模型。
  • 适用于分子晶体多晶型演化与物性模拟,适合材料与药物研发者使用。

我们发布了一个开放的分子晶体(MC)机器学习原子间势(MLIP)数据库,名为MolCryst-MLIPs。首版包含九种分子晶体系统(苯甲酰胺、苯甲酸、香豆素、二取代联苯、异烟酰胺、烟酸、烟酰胺、吡嗪酰胺和间苯二酚)的细调MACE模型,通过自动化机器学习流程(AMLP)开发,该流程将参考数据生成、模型训练与验证整合为可复现且易用的管道。模型从MACE-MH-1基础模型微调而来,所有系统平均能量绝对误差为0.141 kJ/mol/atom,平均力绝对误差为0.648 kJ/mol/Å。在基于DFT标注的多晶型集合上对比三种先进基础模型,仅细调模型能准确解析多晶型能级图。通过分子动力学模拟评估了能量守恒、P2取向序参数及径向分布函数,验证了动态稳定性和结构完整性。发布的模型与数据集构成一个不断增长的经验证的MLIP开放数据库,可直接用于目标化合物在不同热力学条件下的多晶型演化生产级分子动力学模拟。

原文摘要 · Abstract (English)

We present an open Molecular Crystal (MC) database of Machine-Learned Interatomic Potentials (MLIP) called MolCryst-MLIPs. The first release comprises fine-tuned MACE models for nine molecular crystal systems---Benzamide, Benzoic acid, Coumarin, Durene, Isonicotinamide, Nicotinic acid , Niacinamide, Pyrazinamide, and Resorcinol---developed using the Automated Machine Learning Pipeline (AMLP), which streamlines the entire MLIP development workflow, from reference data generation to model training and validation, into a reproducible and user-friendly pipeline. Models are fine-tuned from the MACE-MH-1 foundation model omol head), yielding a mean energy MAE of 0.141 kJ/mol/atom and a mean force MAE of 0.648 kJ/mol/Angstrom across all systems. Benchmarked against three state-of-the-art foundation models on the DFT-labelled polymorph set, only the fine-tuned models resolve the polymorphic energy landscape. Dynamical stability and structural integrity, as assessed through energy conservation, P2 orientational order parameters, and radial distribution functions, are evaluated using molecular dynamics simulations. The released models and datasets constitute a growing open database of validated MLIPs, ready for production MD simulations of molecular crystal polymorphism across the polymorphic landscape of each target compound under different thermodynamic conditions.

机器学习势分子晶体多晶型分子动力学

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