Unveiling hidden ferrimagnetism and giant magnetoelectricity in polar magnet Fe₂Mo₃O₈

Magnetoelectric (ME) effect is recognized for its utility for low-power electronic devices. Largest ME coefficients are often associated with phase transitions in which ferroelectricity is induced by magnetic order. Unfortunately, in these systems, large ME response is revealed only upon elaborate poling procedures. These procedures may become unnecessary in single-polar-domain crystals of polar magnets. Here we report giant ME effects in a polar magnet Fe₂Mo₃O₈ at temperatures as high as 60 K. Polarization jumps of 0.3 μC/cm², and repeated mutual control of ferroelectric and magnetic moments with differential ME coefficients on the order of 10⁴ ps/m are achieved. Importantly, no electric or magnetic poling is needed, as necessary for applications. The sign of the ME coefficients can be switched by changing the applied "bias" magnetic field. The observed effects are associated with a hidden ferrimagnetic order unveiled by application of a magnetic field.