Magnetoelectric coupling of domains, domain walls and vortices in a multiferroic with independent magnetic and electric order.

Magnetically induced ferroelectrics exhibit rigidly coupled magnetic and electric order. The ordering temperatures and spontaneous polarization of these multiferroics are notoriously low, however. Both properties can be much larger if magnetic and ferroelectric order occur independently, but the cost of this independence is that pronounced magnetoelectric interaction is no longer obvious. Using spatially resolved images of domains and density-functional theory, we show that in multiferroics with separately emerging magnetic and ferroelectric order, the microscopic magnetoelectric coupling can be intrinsically strong even though the macroscopic leading-order magnetoelectric effect is forbidden by symmetry. We show, taking hexagonal ErMnO3 as an example, that a strong bulk coupling between the ferroelectric and antiferromagnetic order is realized because the structural distortions that lead to the ferroelectric polarization also break the balance of the competing superexchange contributions. We observe the manifestation of this coupling in uncommon types of topological defects like magnetoelectric domain walls and vortex-like singularities.

Relation between microscopic interactions and macroscopic properties in ferroics.

The driving force in materials to spontaneously form states with magnetic or electric order is of fundamental importance for basic research and device technology. The macroscopic properties and functionalities of these ferroics depend on the size, distribution and morphology of domains; that is, of regions across which such uniform order is maintained1. Typically, extrinsic factors such as strain profiles, grain size or annealing procedures control the size and shape of the domains2-5, whereas intrinsic parameters are often difficult to extract due to the complexity of a processed material. Here, we achieve this separation by building artificial crystals of planar nanomagnets that are coupled by well-defined, tuneable and competing magnetic interactions6-9. Aside from analysing the domain configurations, we uncover fundamental intrinsic correlations between the microscopic interactions establishing magnetically compensated order and the macroscopic manifestations of these interactions in basic physical properties. Experiment and simulations reveal how competing interactions can be exploited to control ferroic hallmark properties such as the size and morphology of domains, topological properties of domain walls or their thermal mobility.