Abstract
Magnetically induced ferroelectric polarization in rare-earth RMn2O5 manganites is believed to originate from the symmetric exchange striction associated with a specific antiferromagnetic phase in the low temperature (T) region and would be irrelevant with electropoling in the high-T paramagnetic-paraelectric phase region. In this work, we demonstrate that low-T pyroelectric polarization of GdMn2O5 single crystals along the b axis in the antiferromagnetic phase exhibits remarkable dependence on the electropoling history imposed in the high-T paramagnetic-paraelectric phase. In particular, the high-T electropoling results in a reversal of ferroelectric polarization in the low-T region, which can be flopped back by the electropoling being sustained in the low-T ferroelectric region. The existence of an electrically polarizable magnetic cluster state in the high-T paramagnetic-paraelectric region is proposed based on a combination of experimental observations and first-principles calculations. An intrinsic correlation between the low-T antiferromagnetic ordering and the high-T polarizable state is discussed. The present experiments unveil the emergent phenomena on multiferroicity of RMn2O5 and suggest an alternative scenario for electrocontrol of magnetism. Published under license by AIP Publishing.