Differentiable Optimization for the Prediction of Ground State Structures (DOGSS)

Ground state or relaxed inorganic structures are the starting point for most computational materials science or surface science analyses. Many of these structure relaxations represent systematic changes to the structure, but there are currently no general methods to improve the initial structure guess based on past calculations. Here we present a method to directly predict the ground state configuration using differentiable optimization and graph neural networks to learn the properties of a simple harmonic force field that approximates the ground state structure and properties. We demonstrate this flexible open source tool for improving the initial configurations for large datasets of inorganic multicomponent surface relaxations across 32 elements and the relaxation of adsorbates (H and CO) on these surfaces. Using these improved initial configurations reduces the expensive adsorbate-covered surface relaxations by approximately 50% and is complementary to other approaches to accelerate the relaxation process.