Direct Observation of Magnetic‐Ion Off‐Centering‐Induced Ferroelectricity in Multiferroic Manganite Pr(Sr_0.1Ca_0.9)₂Mn₂O₇

Ferroelectricity in multiferroic Pr(Sr0.1Ca0.9)2Mn2O7 is found to originate from the off-centering of Mn ions. This polar displacement is energetically stabilized by the cooperative interplay of lattice deformation induced by orbital ordering and oxygen octahedral tilting. This mechanism implies that magnetism and ferroelectricity arise from the same magnetic ions, providing direct evidence for the magnetic-ion off-centering-driven ferroelectricity. As a service to our authors and readers, this journal provides supporting information supplied by the authors. Such materials are peer reviewed and may be re-organized for online delivery, but are not copy-edited or typeset. Technical support issues arising from supporting information (other than missing files) should be addressed to the authors. Please note: The publisher is not responsible for the content or functionality of any supporting information supplied by the authors. Any queries (other than missing content) should be directed to the corresponding author for the article.