Chemical State Detection and Charge Transfer in Complex Oxide Heterostructures via In Situ Auger Electron Spectroscopy

Understanding and controlling the chemical states both in the bulk and at the interfaces of complex oxide thin films is essential for engineering a wide range of electronic, optical, and magnetic functionalities, which arise through emergent phenomena such as two‐dimensional electron gases, interfacial magnetism, and associated phase transitions. Here, we demonstrate the use of in situ Auger Electron Spectroscopy (AES) as a powerful tool for probing oxidation states and dynamic chemical processes during the growth of complex oxide heterostructures. By leveraging the chemical sensitivity of AES to subtle changes in valence electron populations, we show that this technique can distinguish distinct oxidation states in multivalent perovskite manganate and vanadate systems with high fidelity during deposition. Furthermore, we show evidence for dynamic chemical phenomena, specifically charge transfer processes at the polar–nonpolar / interface. Our results establish in situ AES as a powerful diagnostic tool for monitoring and controlling interfacial chemistry during thin film growth, offering a pathway toward the atomic‐scale engineering of chemical states in functional oxide heterostructures.