Magnetoelectric phenomena are intimately linked to relativistic effects and also require the material to break spatial inversion symmetry and time-reversal invariance. Magnetoelectric coupling can substantially affect light–matter interaction and lead to non-reciprocal light propagation. Here, we confirm on a fully experimental basis, without invoking either symmetry-based or material-specific assumptions, that the optical magnetoelectric effect in materials with non-parallel magnetization (M) and electric polarization (P) generates a trilinear term in the refractive index, δn ∝ k ⋅ (P × M), where k is the propagation vector of light. Its sharp magnetoelectric resonances in the terahertz regime, which are simultaneously electric and magnetic dipole active excitations, make Co₂Mo₃O₈ an ideal compound to demonstrate this fundamental relation via independent variation of M, P, and k. Remarkably, the material shows almost perfect one-way transparency in moderate magnetic fields for one of these magnetoelectric resonances.

Atomically sharp domain walls in ferroelectrics are considered as an ideal platform to realize easy-to-reconfigure nanoelectronic building blocks, created, manipulated and erased by external fields. However, conductive domain walls have been exclusively observed in oxides, where domain wall mobility and conductivity is largely influenced by stoichiometry and defects. Here, we report on giant conductivity of domain walls in the non-oxide ferroelectric GaV₄S₈. We observe conductive domain walls forming in zig-zagging structures, that are composed of head-to-head and tail-to-tail domain wall segments alternating on the nanoscale. Remarkably, both types of segments possess high conductivity, unimaginable in oxide ferroelectrics. These effectively 2D domain walls, dominating the 3D conductance, can be mobilized by magnetic fields, triggering abrupt conductance changes as large as eight orders of magnitude. These unique properties demonstrate that non-oxide ferroelectrics can be the source of novel phenomena beyond the realm of oxide electronics.

Magnetization reversal in ferro- and ferrimagnets is a well-known archetype of non-equilibrium processes, where the volume fractions of the oppositely magnetized domains vary and perfectly compensate each other at the coercive magnetic field. Here, we report on a fundamentally new pathway for magnetization reversal that is mediated by an antiferromagnetic state. Consequently, an atomic-scale compensation of the magnetization is realized at the coercive field, instead of the mesoscopic or macroscopic domain cancellation in canonical reversal processes. We demonstrate this unusual magnetization reversal on the Zn-doped polar magnet Fe₂Mo₃O₈. Hidden behind the conventional ferrimagnetic hysteresis loop, the surprising emergence of the antiferromagnetic phase at the coercive fields is disclosed by a sharp peak in the field-dependence of the electric polarization. In addition, at the magnetization reversal our THz spectroscopy studies reveal the reappearance of the magnon mode that is only present in the pristine antiferromagnetic state. According to our microscopic calculations, this unusual process is governed by the dominant intralayer coupling, strong easy-axis anisotropy and spin fluctuations, which result in a complex interplay between the ferrimagnetic and antiferromagnetic phases. Such antiferro-state-mediated reversal processes offer novel concepts for magnetization control, and may also emerge for other ferroic orders.

Electrical manipulation of antiferromagnetic (AFM) states, a cornerstone of AFM spintronics, is a great challenge, requiring novel material platforms. Here we report the full control over AFM states by voltage pulses in the insulating Co 3 O 4 spinel well below its Néel temperature. We show that the strong linear magnetoelectric effect is fully governed by the orientation of the Néel vector. As a unique feature of Co 3 O 4 , the magnetoelectric energy can easily overcome the weak magnetocrystalline anisotropy; thus, the Néel vector can be manipulated on demand, either rotated smoothly or reversed suddenly, by combined electric and magnetic fields. We achieve the nonvolatile switching within a few tens of nanoseconds between time-reversed AFM states in macroscopic volumes by voltage pulses. These observations render quasicubic antiferromagnets, like Co 3 O 4 , an ideal platform for the ultrafast (picosecond to nanosecond) manipulation of microscopic AFM domains and may pave the way for the realization of AFM spintronic devices.

Electrical manipulation of antiferromagnetic states, a cornerstone of antiferromagnetic spintronics, is a great challenge, requiring novel material platforms. Here we report the full control over antiferromagnetic states by voltage pulses in the insulating Co$_3$O$_4$ spinel. We show that the strong linear magnetoelectric effect emerging in its antiferromagnetic state is fully governed by the orientation of the Néel vector. As a unique feature of Co$_3$O$_4$, the magnetoelectric energy can easily overcome the weak magnetocrystalline anisotropy, thus, the Néel vector can be manipulated on demand, either rotated smoothly or reversed suddenly, by combined electric and magnetic fields. We succeed with switching between antiferromagnetic states of opposite Néel vectors by voltage pulses within a few microsecond in macroscopic volumes. These observations render quasi-cubic antiferromagnets, like Co$_3$O$_4$, an ideal platform for the ultrafast (pico- to nanosecond) manipulation of microscopic antiferromagnetic domains and may pave the way for the realization of antiferromagnetic spintronic devices.