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Pyroelectric current and magnetoelectric coupling measurements on polycrystalline samples of the quadruple perovskite (LaMn)MnO give evidence of ferroelectricity driven by the antiferromagnetic ordering of the -site Mn ions at =78 K with record values of remnant electric polarization up to =0.56 C cm. X-ray diffraction measurements indicates an anomalous behavior of the monoclinic angle at , which suggests that lies in the -plane, where the moments are collinear, so we conclude that exchange striction is the mechanism of spin-driven ferroelectricity. Polarization values 3 C cm are expected in single crystals, which would open the avenue towards practical multiferroic applications.

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