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Abstract Structural domains and domain walls, inherent in single crystalline perovskite oxides, can significantly influence the properties of the material and therefore must be considered as a vital part of the design of the epitaxial oxide thin films. We employ 4D-STEM combined with machine learning (ML) to comprehensively characterize domain structures at both high spatial resolution and over a significant spatial extent. Using orthorhombic LaFeO₃as a model system, we explore the application of unsupervised and supervised ML in domain mapping, which demonstrates robustness against experiment uncertainties. The results reveal the consequential formation of multiple domains due to the structural degeneracy when LaFeO₃film is grown on cubic SrTiO₃. In situ annealing of the film shows the mechanism of domain coarsening that potentially links to phase transition of LaFeO₃at high temperatures. Moreover, synthesis of LaFeO₃on DyScO₃illustrates that a less symmetric orthorhombic substrate inhibits the formation of domain walls, thereby contributing to the mitigation of structural degeneracy. High fidelity of our approach also highlights the potential for the domain mapping of other complicated materials and thin films. 

Abstract In the burgeoning field of spintronics, antiferromagnetic materials (AFMs) are attracting significant attention for their potential to enable ultra‐fast, energy‐efficient devices. Thin films of AFMs are particularly promising for practical applications due to their compatibility with spin‐orbit torque (SOT) mechanisms. However, studying these thin films presents challenges, primarily due to the weak signals they produce and the rapid dynamics driven by SOT, that are too fast for conventional electric transport or microwave techniques to capture. The time‐resolved magneto‐optical Kerr effect (TR‐MOKE) has been a successful tool for probing antiferromagnetic dynamics in bulk materials, thanks to its sub‐picosecond (sub‐ps) time resolution. Yet, its application to nanometer‐scale thin films has been limited by the difficulty of detecting weak signals in such small volumes. In this study, the first successful observation of antiferromagnetic dynamics are presented in nanometer‐thick orthoferrite films using the pump‐probe technique to detect TR‐MOKE signal. This paper report an exceptionally low damping constant of 1.5 × 10⁻⁴and confirms the AFM magnonic nature of these dynamics through angular‐dependent measurements. Furthermore, it is observed that electrical currents can potentially modulate these dynamics via SOT. The findings lay the groundwork for developing tunable, energy‐efficient spintronic devices, paving the way for advancements in next‐generation spintronic applications.