Coexistence and Coupling of Multiple Charge Orderings and Spin States in Hexagonal Ferrite

The coupling between charge and spin orderings in strongly correlated systems plays a crucial role in fundamental physics and device applications. As a candidate of multiferroic materials, LuFe2O4with a nominal Fe2.5+valence state has the potential for strong charge-spin interactions; however, these interactions have not been fully understood until now. Here, combining complementary characterization methods with theoretical calculations, two types of charge orderings with distinct magnetic properties are revealed. The ground states of LuFe2O4are decided by the parallel/antiparallel coupling of both charge and spin orderings in the adjacent FeO double layers. Whereas the ferroelectric charge ordering remains ferrimagnetic below 230 K, the antiferroelectric ordering undergoes antiferromagnetic-ferrimagnetic-paramagnetic transitions from 2 K to room temperature. This study demonstrates the unique aspects of strong spin-charge coupling within LuFe2O4. Our results shed light on the coexistence and competing nature of orderings in quantum materials.