An Extendible, Graph-Neural-Network-Based Approach for Accurate Force Field Development of Large Flexible Organic Molecules

Abstract: An accurate force field is the key to the success of all molecular mechanics simulations on organic polymers and biomolecules. Accuracy beyond density functional theory is often needed to describe the intermolecular interactions, while most correlated wavefunction (CW) methods are prohibitively expensive for large molecules. Therefore, it posts a great challenge to develop an extendible ab initio force field for large flexible organic molecules at CW level of accuracy. In this work, we face this challenge by combining the physics-driven nonbonding potential with a data-driven subgraph neural network bonding model (named sGNN). Tests on polyethylene glycol polymer chains show that our strategy is highly accurate and robust for molecules of different sizes. Therefore, we can develop the force field from small molecular fragments (with sizes easily accessible to CW methods) and safely transfer it to large polymers, thus opening a new path to the next-generation organic force fields.