Anisotropic Magnetoelectric Coupling and Cotton-Mouton Effects in the Organic Magnetic Charge-Transfer Complex Pyrene-F₄ TCNQ

Magnetoelectric coupling is of high current interest because of its potential applications in multiferroic memory devices. Although magnetoelectric coupling has been widely investigated in inorganic materials, such observations in organic materials are extremely rare. Here, we report our discovery that organic charge-transfer (CT) complex pyrene-2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodimethane (pyrene−F₄ TCNQ) can display anisotropic magnetoelectric coupling. Investigation of the crystal structure of pyrene−F₄ TCNQ complex demonstrates that the magnetoelectric coupling coefficient along the π-π interaction direction is much larger than the value along other directions. Furthermore, magnetoelectric coupling and magnetization can be tuned by changing the fluorine content in complexes. Besides, the Cotton−Mouton effect in pyrene−F₄ TCNQ is observed, enabling the control of optomagnetic devices. These results can pave the way for a new method for the future development of organic CT complexes and their applications in perpendicular memory devices and energy-transfer-related multiferroics.