Irradiation-induced amplification of electric fields at oxide interfaces as revealed by correlative DPC-STEM and DFT

Abstract

Heterointerfaces are ubiquitous in modern devices, found in technologies ranging from microelectronics to structural components for energy applications. Many of these emerging technologies are found in applications such as satellites, batteries, and next generation nuclear reactors, that are subject to harsh environments. In some scenarios, multiple extreme conditions, such as irradiation and corrosion, act on the material simultaneously. Extending the lifetime of these technologies is dependent on a detailed understanding of how their component materials platforms and interfaces respond in extreme environments, where irradiation and corrosion may couple in unique ways, distinct from corrosion under ambient conditions. Oxides, which form readily over metal underlayers, can act as protective coatings; enhancing the robustness of oxide overlayers to protect underlying metal alloys is a potential avenue towards corrosion mitigation. Here we study the impact of irradiation-induced non-equilibrium defects on charge segregation and electric fields at and near multi-phase oxide heterointerfaces. We perform a detailed study of irradiated Fe2O3-Cr2O3 thin film heterostructures using first-principles DFT electronic structure modeling paired with 4D-STEM DPC and EELS techniques to measure nanoscale changes in electric fields. Our results show clear evidence that irradiation drives substantial modulation of interfacial electric fields that can be tailored by controlling the atomistic chemical structure of the oxide interface. We show that irradiation can selectively induce built-in electric fields, thereby altering their direction; this suggests a pathway to engineering protective oxide heterostructure overlayers that can electrically control the spatial distribution of defects, with significant implications for the design of corrosion-resistant materials for extreme environments.