Hollandites as a new class of multiferroics

Discovery of new complex oxides that exhibit both magnetic and ferroelectric properties is of great interest for the design of functional magnetoelectrics, in which research is driven by the technologically exciting prospect of controlling charges by magnetic fields and spins by applied voltages, for sensors, 4-state logic, and spintronics. Motivated by the notion of a tool-kit for complex oxide design, we developed a chemical synthesis strategy for single-phase multifunctional lattices. Here, we introduce a new class of multiferroic hollandite Ba-Mn-Ti oxides not apparent in nature. BaMn3Ti4O14.25, designated BMT-134, possesses the signature channel-like hollandite structure, contains Mn4+ and Mn3+ in a 1 : 1 ratio, exhibits an antiferromagnetic phase transition (T-N similar to 120 K) with a weak ferromagnetic ordering at lower temperatures, ferroelectricity, a giant dielectric constant at low frequency and a stable intrinsic dielectric constant of similar to 200 (1-100 MHz). With evidence of correlated antiferromagnetic and ferroelectric order, the findings point to an unexplored family of structures belonging to the hollandite supergroup with multifunctional properties, and high potential for developing new magnetoelectric materials.