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Unexpected type-II multiferroic phase in GdMnO3 under high magnetic fields

Perovskite manganites with small A-site ions, as the first and canonical branch of type-II multiferroics, are ideal systems to exhibit magnetism-induced ferroelectricity. Despite their established magnetoelectric phase diagrams under low magnetic fields, here an unidentified phase with a large magnetism-induced polarization (up to 1500 μC/m2) is revealed in GdMnO3 under high magnetic fields up to 60 T. Based on multiprobe experiments, a complete phase diagram is constructed with successive polar-nonpolar-polar-nonpolar transitions. Such a nonmonotonic evolution is well mimicked by model simulation, while the spin-lattice coupling is the key ingredient for the reentrant ferroelectric phase.