arXiv:2509.26397physics.chem-phcs.LG2025-09被引 2

大模型在量子化学中失效,仅靠扩大规模无法学好基本物理规律。

Are neural scaling laws leading quantum chemistry astray?

  • 用不同规模模型和数据训练,但只用稳定结构会失败
  • 只有加入拉伸压缩构型才能勉强预测氢分子能量曲线
  • 连两个裸质子的排斥曲线都预测错,暴露基础物理理解缺失

神经网络缩放定律正推动机器学习领域不断训练更大规模的基础模型,承诺在跨任务中实现高精度与可迁移表征。我们在量子化学中验证这一假设:通过扩大模型容量和训练数据量,基于量子化学计算结果进行训练。以中性H₂分子的键解离能预测为泛化任务,评估模型表现。结果发现,无论数据集大小或模型容量如何,仅在稳定构型上训练的模型均无法定性地再现H₂的能量曲线。只有显式包含压缩与拉伸几何构型时,预测结果才大致接近真实形状。然而,即使在最大、最多样化的含解离双原子数据集上训练的最大基础模型,仍对简单双原子分子表现出严重错误。最显著的是,这些模型无法复现两个裸质子间的简单排斥能量曲线,暴露出其未能学习电子结构理论中的基本库仑定律。这表明,单纯依赖缩放无法构建可靠的量子化学模型。

原文摘要 · Abstract (English)

Neural scaling laws are driving the machine learning community toward training ever-larger foundation models across domains, assuring high accuracy and transferable representations for extrapolative tasks. We test this promise in quantum chemistry by scaling model capacity and training data from quantum chemical calculations. As a generalization task, we evaluate the resulting models' predictions of the bond dissociation energy of neutral H$_2$, the simplest possible molecule. We find that, regardless of dataset size or model capacity, models trained only on stable structures fail dramatically to even qualitatively reproduce the H$_2$ energy curve. Only when compressed and stretched geometries are explicitly included in training do the predictions roughly resemble the correct shape. Nonetheless, the largest foundation models trained on the largest and most diverse datasets containing dissociating diatomics exhibit serious failures on simple diatomic molecules. Most strikingly, they cannot reproduce the trivial repulsive energy curve of two bare protons, revealing their failure to learn the basic Coulomb's law involved in electronic structure theory. These results suggest that scaling alone is insufficient for building reliable quantum chemical models.

量子化学大模型失效缩放定律

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