Development and Validation of Versatile Deep Atomistic Potentials for Metal Oxides

Machine learning interatomic potentials powered by neural networks have been shown to readily model a gradient of compositions in metallic systems. However, their application to date on ionic systems tends to focus on specific compositions and oxidation states owing to their more heterogeneous chemical nature. Herein we show that a deep neural network potential (DNP) can model various properties of metal oxides with different oxidation states without additional charge information. We created and validated DNPs for AgxOy, CuxOy MgxOy, PtxOy, and ZnxOy, whereby each system was trained without any limitations on oxidation states. We illustrate how the database can be augmented to enhance the DNP transferability for a new polymorph, surface energies, and thermal expansion. In addition, we show that these potentials can correctly interpolate significant pressure and temperature ranges, exhibit stability over long molecular dynamics simulation time scales, and replicate nonharmonic thermal expansion, consistent with experimental results.

Automated summary

Machine learning with neural networks is effective in modeling various compositions in metallic systems, but its application to ionic systems is limited to specific compositions and oxidation states due to their more complex chemical nature. This study demonstrates that a deep neural network potential (DNP) can accurately model metal oxides with different oxidation states without the need for charge information.