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In Situ Reversible Ionic Control for Nonvolatile Magnetic Phases in a Donor/Acceptor Metal-Organic Framework

ABSTRACT

Reversible magnetic control by electrical means, which is highly desired from the viewpoint of fundamentals and technological applications such as data storage devices, has been a challenging topic. In this study, the authors demonstrate in situ magnetic phase switching between the ferrimagnetic and paramagnetic states of an electron-donor/-acceptor metal-organic framework (D/A-MOF) using band-filling control mediated by the Li+-ion migration that accompanies redox reactions, i.e., “magneto-ionic control”. By taking advantage of the rechargeability of lithium-ion battery systems, in which Li+-ions and electrons are simultaneously inserted into/extracted from a cathode material, the reversible control of nonvolatile magnetic phases in a D/A-MOF has been achieved. This result demonstrates that the combination of a redox-active MOF with porous flexibility and ion-migration capability enables the creation of new pathways toward magneto-electric coupling devices in the field of ionics.