论文标题
神经网络 - 神经网络可以快速找到反应路径
NeuralNEB -- Neural Networks can find Reaction Paths Fast
论文作者
论文摘要
量子力学方法(如密度功能理论(DFT))与有效的搜索算法相同,用于研究反应性系统的动力学。但是,对于大规模探索,DFT非常昂贵。机器学习(ML)模型已成为小分子DFT计算的出色模拟器,并且可以在此类任务中取代DFT。对于动力学,成功主要依赖于模型能力来准确预测过渡态和最小能量路径(MEP)周围的势能表面(PES)。以前,由于文献中相关数据的稀缺,这是不可能的。在本文中,我们训练来自Transition1x数据集的大约10.000个基本反应的基于Art Equivariant图形神经网络(GNN)的模型。我们将模型应用于屏障的平均平均误差(MAE)为0.13 +/- 0.03 eV的平均平均误差(MAE)在未见反应的屏障能量上,平均平均误差(MAE)为0.13 +/- 0.03 eV。我们将结果与在QM9和ANI1X训练的同等模型进行比较。我们还将与精度和计算资源的基于密度的紧密结合(DFTB)进行比较。这意味着,鉴于相关数据的ML模型现在处于可以用于超越简单分子特征预测量子化学预测的下游任务的水平。
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.