Knowledge-Guided Construction of Machine Learning Potentials for Reactive Behavior in Energetic Materials

Abstract

Energetic materials involve multiple interactions, making reliable machine-learning potentials (MLPs) difficult to construct without extensive datasets. Here, we enhance the ability of the neural network interatomic potential (NNAP) to describe molecular systems using sphmulti, a refined spherical-harmonic basis set that combines extra radial basis with element-specific chemical weighting in each radial channel. We further integrate hyperactive learning, farthest-point sampling, and iterative sufficiency criteria with knowledge-guided key events, enabling the NNAP to retain essential information for describing the material system. For 3,3'-diamino-4,4'-azoxyfurazan, the resulting NNAP is trained on only 13,680 configurations yet captures key properties, including the isomerization barrier, pyrolysis activation energy, and shock Hugoniot behavior. NNAP-driven molecular dynamics simulations further reveal that pyrolysis proceeds through furazan-ring opening followed by chain reactions, whereas shock loading induces anisotropic hydrogen transfer driven by interlayer structural deformations. This work enables efficient and reliable MLPs for energetic materials.