Pyroelectric current and field-dependent specific heat measurements on polycrystalline samples of the quadruple perovskite (LaMn3)Mn4O12 give evidence of ferroelectricity driven by the canted antiferromagnetic ordering of the B-site Mn3+ ions at TN,B=78 K with record large remnant electric polarization up to 0.56 μC cm−2. X-ray diffraction measurements indicate an anomalous behavior of the monoclinic β angle at TN,B, which suggests that the polarization lies in the ac-plane, where the moments are collinear, and that symmetric exchange striction is the mechanism of spin-driven ferroelectricity. Polarization values up to ∼3–6 μC cm−2 are expected in single crystals or epitaxial films, which would enable the development of practical multiferroic applications.

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