Constructing Accurate and Efficient General-Purpose Atomistic Machine Learning Model with Transferable Accuracy for Quantum Chemistry
Yicheng Chen, Wenjie Yan, Zhanfeng Wang, Jianming Wu, Xin Xu
Abstract
Density functional theory (DFT) has been a cornerstone in computational science, providing powerful insights into structure-property relationships for molecules and materials through first-principles quantum-mechanical (QM) calculations. However, the advent of atomistic machine learning (ML) is reshaping the landscape by enabling large-scale dynamics simulations and high-throughput screening at DFT-equivalent accuracy with drastically reduced computational cost. Yet, the development of general-purpose atomistic ML models as surrogates for QM calculations faces several challenges, particularly in terms of model capacity, data efficiency, and transferability across chemically diverse systems. This work introduces a novel extension of the polarizable atom interaction neural network (namely, XPaiNN) to address these challenges. Two distinct training strategies have been employed, one direct-learning and the other Δ-ML on top of a semiempirical QM method. These methodologies have been implemented within the same framework, allowing for a detailed comparison of their results. The XPaiNN models, in particular the one using Δ-ML, not only demonstrate competitive performance on standard benchmarks, but also demonstrate the effectiveness against other ML models and QM methods on comprehensive downstream tasks, including noncovalent interactions, reaction energetics, barrier heights, geometry optimization and reaction thermodynamics, etc. This work represents a significant step forward in the pursuit of accurate and efficient atomistic ML models of general-purpose, capable of handling complex chemical systems with transferable accuracy.