A Combined Tight Binding with Machine Learning Potential Model for Magnesium Compounds

Abstract: We present a model for magnesium-based systems that combines density functional tight binding (DFTB) with MACE, a machine learning interatomic potential (DFTB+MACE). In this model, the conventional repulsive potential, pair potential, is replaced by a many-body MACE potential. The MACE component of the model is trained on the difference between density functional theory (DFT) energies and forces and the corresponding DFTB values, but neglecting the pair potential contribution. Using this model we performed structural relaxation of MgO-CO2 adsorption systems, molecular dynamics calculations of water clusters and phonon spectrum calculations of stable fcc-MgO and metastable bcc-MgO structures. We compare the performance of our model with a pure MACE model and with DFT. We demonstrate that the DFTB+MACE model achieves improved accuracy relative to DFTB with a pair potential, in many cases with only a moderate increase in computational cost. In addition, it can provide electronic structures that most of the machine learning potentials cannot. The training dataset, originally developed for MACE, may not fully represent all regions of the potential surface we may encounter during simulations. Expanding the dataset for a wider potential surface is expected to further enhance predictive accuracy of DFTB+MACE model. Overall, the resulting DFTB+MACE framework enables simulations at length and time scales beyond the reach of first-principles methods while retaining an explicit description of electronic structures, making it particularly attractive for studying charge-transfer in materials.