Exploring Complex Reaction Networks Using Neural Network-Based Molecular Dynamics Simulation.

Abstract

Ab initio molecular dynamics (AIMD) is an established method for revealing the reactive dynamics of complex systems. However, the high computational cost of AIMD restricts the explorable length and time scales. Here, we develop a fundamentally different approach using molecular dynamics simulations powered by a neural network potential to investigate complex reaction networks. This potential is trained via a workflow combining AIMD and interactive molecular dynamics in virtual reality to accelerate the sampling of rare reactive processes. A panoramic visualization of the complex reaction networks for decomposition of a novel high explosive (ICM-102) is achieved without any predefined reaction coordinates. The study leads to the discovery of new pathways that would be difficult to uncover if established methods were employed. These results highlight the power of neural network-based molecular dynamics simulations in exploring complex reaction mechanisms under extreme conditions at the ab initio level, pushing the limit of theoretical and computational chemistry toward the realism and fidelity of experiments.