Orbital-ordering-driven multiferroicity and magnetoelectric coupling in GeV₄S₈.

We report here the discovery of multiferroicity and large magnetoelectric coupling in the type I orbital order system GeV₄S₈. Our study demonstrates that this clustered compound displays a para-ferroelectric transition at 32 K. This transition originates from an orbital ordering which reorganizes the charge within the transition metal clusters. Below the antiferromagnetic transition at 17 K, the application of a magnetic field significantly affects the ferroelectric polarization, revealing thus a large magnetoelectric coupling. Our study suggests that the application of a magnetic field induces a metamagnetic transition which significantly affects the ferroelectric polarization thanks to an exchange striction phenomenon.