Probing Ferroic States in Oxide Thin Films Using Optical Second Harmonic Generation

Forthcoming low-energy consumption oxide electronics rely on the deterministic control of ferroelectric and multiferroic domain states at the nanoscale. In this review, we address the recent progress in the field of investigation of ferroic order in thin films and heterostructures, with a focus on non-invasive optical second harmonic generation (SHG). For more than 50 years, SHG has served as an established technique for probing ferroic order in bulk materials. Here, we will survey the specific new aspects introduced to SHG investigation of ferroelectrics and multiferroics by working with thin film structures. We show how SHG can probe complex ferroic domain patterns non-invasively and even if the lateral domain size is below the optical resolution limit or buried beneath an otherwise impenetrable cap layer. We emphasize the potential of SHG to distinguish contributions from individual (multi-) ferroic films or interfaces buried in a device or multilayer architecture. Special attention is given to monitoring switching events in buried ferroic domain- and domain-wall distributions by SHG, thus opening new avenues towards the determination of the domain dynamics. Another aspect studied by SHG is the role of strain. We will finally show that by integrating SHG into the ongoing thin film deposition process, we can monitor the emergence of ferroic order and properties in situ, while they emerge during growth. Our review closes with an outlook, emphasizing the present underrepresentation of ferroic switching dynamics in the study of ferroic oxide heterostructures.