Microscopic Observation of Entangled Multi-Magnetoelectric Coupling Phenomenon

Searching for new functionality in next generation electronic devices is a principal driver of material physics research. Multiferroics simultaneously exhibit electric and magnetic order parameters that may be coupled through magnetoelectric (ME) effects. In single-phase materials the ME effect arises from one of three known mechanisms: inverse Dzyaloshinskii-Moriya (IDM) interaction, spin dependent ligand-metal (p-d) orbital hybridization, and exchange striction. However, the coupling among these mechanisms remains largely unexplored despite envisioned potential capabilities. Here, we present cooperative tuning between both IDM interaction and p-d hybridization that leads to discrete ME states in Ba0.5Sr2.5Co2Fe24O41. In-situ x-ray diffraction exposes the microscopic interplay between these two mechanisms, marked by a unique ME susceptibility upon electric and magnetic fields. The entangled multi-ME coupling phenomenon observed in this room-temperature ME hexaferrite offers a pathway to novel functional control for ME device applications.