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Magnetic phase transition induced ferroelectric polarization in BaFeF4 with room temperature weak ferromagnetism

BaMF4 (M=Fe, Co, Ni and Mn) family are typical multiferroic materials, having antiferromagnetism at around liquid nitrogen temperature. In this work, polycrystalline BaFeF4 has been prepared by solid state reaction. The slight deficiency of Fe leads to the coexistence of valence states of +2 and +3, facilitating the electrons to hop between the neighboring Fe2+ and Fe3+ ions through the middle F- ion, leading to the strong double exchange interaction with weak ferromagnetism above room temperature. A bifurcation at about 170 K between the zero-field-cooled and field-cooled temperature dependent magnetization curves indicates the onset of 2-dimensional antiferromagnetism, which is completed at about 125 K with the sudden drop of magnetization. Despite the fact of type-I multiferroic, its magnetoelectricity can be evidenced by the pyroelectric current, which shows a peak starting at about 170 K and finishing at about 125 K. The saturated ferroelectric polarization change of around 34 μC/m2 is observed, which is switchable by the reversed poling electric field and decreases to about 30 μC/m2 under a magnetic field of 90 kOe. This magnetoelectricity can be qualitatively reproduced by first-principles calculations. Our results represent substantial progress to search for high-temperature multiferroics in ferroelectric fluorides.