Machine-Learning-Backed Evolutionary Exploration of Ti-rich SrTiO3(110) Surface Reconstructions

The investigation of inhomogeneous surfaces, where various local structures co-exist, is crucial for understanding interfaces of technological interest, yet it presents significant challenges. Here, we study the atomic configurations of the (2 × m) Ti-rich surfaces at (110)-oriented SrTiO3 by bringing together scanning tunneling microscopy and transferable neural-network force fields combined with evolutionary exploration. We leverage an active learning methodology to iteratively extend the training data as needed for different configurations. Training on only small well-known reconstructions we are able to extrapolate to the complicated and diverse overlayers encountered in different regions of the heterogeneous SrTiO3(110)-(2×m) surface. Our machine-learning-backed approach generates several new candidate structures, in good agreement with experiment and verified using density functional theory.