Quantum-accurate machine learning potentials for metal-organic frameworks using temperature driven active learning

Abstract

Understanding structural flexibility of metal-organic frameworks (MOFs) via molecular dynamics simulations is crucial to design better MOFs. Density functional theory (DFT) and quantum-chemistry methods provide highly accurate molecular dynamics, but the computational overheads limit their use in long time-dependent simulations. In contrast, classical force fields struggle with the description of coordination bonds. Here we develop a DFT-accurate machine-learning spectral neighbor analysis potentials for two representative MOFs. Their structural and vibrational properties are then studied and tightly compared with available experimental data. Most importantly, we demonstrate an active-learning algorithm, based on mapping the relevant internal coordinates, which drastically reduces the number of training data to be computed at the DFT level. Thus, the workflow presented here appears as an efficient strategy for the study of flexible MOFs with DFT accuracy, but at a fraction of the DFT computational cost.