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Hexagonal perovskite 15R-BaMnO2.99 with a ratio of cubic to hexagonal layersof 1/5 in the unit cell is an antiferromagnetic insulator that orders at aN\'eel temperature TN = 220 K. Here we report structural, magnetic, dielectricand thermal properties of single crystal BaMnO2.99 and its derivativesBaMn0.97Li0.03O3 and Ba0.97K0.03MnO3. The central findings of this work are:(1) these materials possess a usually large, high-temperature magnetoelectriceffect that amplifies the dielectric constant by more than an order ofmagnitude near their respective N\'eel temperature; (2) Li and K doping canreadily vary the ratio of cubic to hexagonal layers and cause drastic changesin dielectric and magnetic properties; in particular, a mere 3% Li substitutionfor Mn significantly weakens the magnetic anisotropy and relaxes the lattice;consequently, the dielectric constant for both the a- and c-axis sharply risesto 2500 near the N\'eel temperature. This lattice softening is also accompaniedby weak polarization. These findings provide a new paradigm for developingnovel, high-temperature magnetoelectric materials that may eventuallycontribute to technology.

Giant Magnetoelectric Effect in Antiferromagnetic BaMnO3-\delta and Its Derivatives