Synergistic Integration of Physical Embedding and Machine Learning Enabling Precise and Reliable Force Field.

Machine-learning force fields have achieved significant strides in accurately reproducing the potential energy surface with quantum chemical accuracy. However, this approach still faces several challenges, e.g., extrapolating to uncharted chemical spaces, interpreting long-range electrostatics, and mapping complex macroscopic properties. To address these issues, we advocate for a synergistic integration of physical principles and machine learning techniques within the framework of a physically informed neural network (PINN). This approach involves incorporating physical knowledge into the parameters of the neural network, coupled with an efficient global optimizer, the Tabu-Adam algorithm, proposed in this work to augment optimization under strict physical constraint. We choose the AMOEBA+ force field as the physics-based model for embedding and then train and test it using the diethylene glycol dimethyl ether (DEGDME) data set as a case study. The results reveal a breakthrough in constructing a precise and noise-robust machine learning force field. Utilizing two training sets with hundreds of samples, our model exhibits remarkable generalization and density functional theory (DFT) accuracy in describing molecular interactions and enables a precise prediction of the macroscopic properties such as the diffusion coefficient with minimal cost. This work provides valuable insight into establishing a fundamental framework of the PINN force field.