Quantum mechanical methods like Density Functional Theory (DFT) are used with great success alongside efficient search algorithms for studying kinetics of reactive systems. However, DFT is prohibitively expensive for large scale exploration. Machine Learning (ML) models have turned out to be excellent emulators of small molecule DFT calculations and could possibly replace DFT in such tasks. For kinetics, success relies primarily on the models capability to accurately predict the Potential Energy Surface (PES) around transition-states and Minimal Energy Paths (MEPs). Previously this has not been possible due to scarcity of relevant data in the literature. In this paper we train state of the art equivariant Graph Neural Network (GNN)-based models on around 10.000 elementary reactions from the Transition1x dataset. We apply the models as potentials for the Nudged Elastic Band (NEB) algorithm and achieve a Mean Average Error (MAE) of 0.13+/-0.03 eV on barrier energies on unseen reactions. We compare the results against equivalent models trained on QM9 and ANI1x. We also compare with and outperform Density Functional based Tight Binding (DFTB) on both accuracy and computational resource. The implication is that ML models, given relevant data, are now at a level where they can be applied for downstream tasks in quantum chemistry transcending prediction of simple molecular features.
翻译:磁力功能理论(DFT)等量子机械方法与研究反应系统动能的高效搜索算法一起使用,非常成功。然而,DFT对于大规模探索来说成本极高。机器学习(ML)模型是小分子DFT计算的最佳模拟器,并有可能取代DFT进行此类任务。动能学的成功主要取决于在转型状态和最小能源路径(MEPs)周围准确预测潜在能源表面(PES)的模型能力。以前,由于文献中缺少相关数据,这是不可能的。在本文中,我们用大约10 000个基础模型来培训基于艺术的等离异性图形神经网络(GNNN)的模型。我们将这些模型用作Noddd Elastic Band(NEB)算法的潜力,并实现在视觉反应屏障能量方面的平均误差0.13+/0.03 eV(MAE) 。我们比较了在QM9和ANI1x(GNNN)中培训的类似模型。我们在TFML(S)级的精度模型上,在常规和外的精确度上,可以比较了该模型。