Dimerization Triggered Magnetoelectric Coupling Effect and Magnetic Anisotropy in Organic Ternary Crystals

Abstract Developing a new universal strategy to design all organic ferromagnets or multiferroics with satisfactory properties always remains challenging. In this work, ternary charge transfer crystals are fabricated to realize organic multiferroic magnetoelectric coupling effect. Through incorporating the third component into binary crystals, a dimerization between neighbor donor and acceptor is induced to form a lattice symmetry breaking, where a nonpolar to polar phase transition is ensuing to lead to a dipolar polarization. Magnetic field can effectively tune the dipolar polarization to present a magnetoelectric coupling effect. Moreover, the introduction of the third component can result in a rearrangement in molecular configuration to modify the electron–phonon interaction. As a result, anisotropic magnetism is observed due to anisotropic electron–phonon coupling in ternary crystals. Overall, this study forecasts that incorporating an appropriate third component is a potential method for designing all organic multiferroics.