arXiv:2605.24073physics.chem-phcs.LG2026-05

用半经验轨道电荷提升多任务学习,让机器学习势函数更省数据、更准。

Multitask learning with semiempirical orbital charges enables sample-efficient MLIPs

论文配图:Multitask learning with semiempirical orbital charges enables sample-efficient MLIPs
图 1 · 摘自论文原文
  • 用轨道分辨的半经验电荷做多任务学习,提升模型对电子结构的捕捉能力。
  • 训练数据减少5倍,能量误差降低46%,性能超过仅用能量训练的模型。
  • 适合构建复杂化学体系的高效、高精度基础模型,尤其利于金属材料研究。

机器学习势函数(MLIPs)需生成计算成本高昂的大规模训练数据以准确模拟材料与分子。利用多任务学习引入电子结构信息可提升样本效率,但全哈密顿矩阵训练(随原子数平方增长)在大数据集下不可行。本文表明,采用轨道分辨的半经验电荷进行多任务学习显著提升MLIP的样本效率与精度。我们设计了一种专用等变模型,有效预测轨道电荷,误差低于不变基线模型。通过引入计算成本低、线性增长的GFN1-xTB轨道电荷作为训练增强,模型实现能量均方误差降低46%,且仅需五分之一的数据即可达到纯能量模型的性能。此外,该方法优于使用高成本密度泛函理论(DFT)原子电荷训练的模型,能捕捉轨道级电子复杂性,促使网络学习物理合理的隐空间,自发按共享化学特性聚类金属。由于轨道电荷仅用于训练,推理效率不受影响,为复杂化学系统构建精准、高效的基础模型提供可扩展方案。

原文摘要 · Abstract (English)

Machine learning interatomic potentials (MLIPs) require generating computationally expensive, large-scale training datasets to accurately simulate materials and molecules. Incorporating electronic structure information using multitask learning improves sample efficiency, however, training on full Hamiltonian matrices, which scale quadratically with the number of atoms, is intractable for large datasets. In this work, we show that multitask learning utilizing orbitally resolved semiempirical charges significantly improves sample efficiency and accuracy in MLIPs. To efficiently predict orbital charges, we implement a specialized equivariant model, reducing charge prediction error compared to an invariant baseline. By augmenting training with computationally inexpensive GFN1-xTB orbital charges, which scale linearly with the number of atoms, our model achieves a 46\% reduction in energy mean absolute error and requires five times less data to match the performance of energy-only models. Furthermore, our approach outperforms models trained on expensive density functional theory (DFT) atomic charges, capturing orbitally resolved electronic complexity and forcing the network to learn a physically accurate latent space that spontaneously clusters metals by shared chemical properties. Because orbital charges are only required during training, this approach preserves inference efficiency, providing a scalable recipe for developing accurate, data-efficient foundation models for complex chemical systems.

机器学习势函数多任务学习电子结构数据效率

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