Data-efficient iterative training of Gaussian approximation potentials: Application to surface structure determination of rutile IrO2 and RuO2

J Timmermann and YHY Lee and CG Staacke and JT Margraf and C Scheurer and K Reuter, JOURNAL OF CHEMICAL PHYSICS, 155, 244107 (2021).

DOI: 10.1063/5.0071249

Machine-learning interatomic potentials, such as Gaussian Approximation Potentials (GAPs), constitute a powerful class of surrogate models to computationally involved first-principles calculations. At a similar predictive quality but significantly reduced cost, they could leverage otherwise barely tractable extensive sampling as in global surface structure determination (SSD). This efficiency is jeopardized though, if an a priori unknown structural and chemical search space as in SSD requires an excessive number of first-principles data for the GAP training. To this end, we present a general and data-efficient iterative training protocol that blends the creation of new training data with the actual surface exploration process. Demonstrating this protocol with the SSD of low-index facets of rutile IrO2 and RuO2, the involved simulated annealing on the basis of the refining GAP identifies a number of unknown terminations even in the restricted sub-space of (1 x 1) surface unit cells. Particularly in an O-poor environment, some of these, then metal-rich terminations, are thermodynamically most stable and are reminiscent of complexions as discussed for complex ceramic materials.

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