Molecular Based Magnetic‐Electric Material With Multi‐Property Synergistic Stimulus‐Response

Molecular magnetic‐electric materials have garnered significant attention due to their potential applications in intelligent systems and spintronics. Nevertheless, the realization of such materials remains challenging, requiring rational optimization and regulation of various factors, including the molecular‐level design of structures and the response mechanism to external stimuli. Herein, a binuclear polar single‐molecule magnet was synthesized by incorporating polar croconic acid, which exhibits distinct magnetic hysteresis loops, magnetization relaxation dynamics, near‐room‐temperature pyroelectric currents, and temperature‐dependent optical second‐harmonic generation signals, accompanied by a temperature‐dependent polar to non‐polar crystal structural phase transition (265 K). Furthermore, reversible color changes were observed under X‐ray irradiation, leading to corresponding reversible alterations in UV–vis spectra (298 K), dielectric properties (265–286 K), and magnetization relaxation dynamics. Mechanism investigations revealed that radicals generated by X‐ray irradiation can synergistically manipulate optical, electrical, and magnetic properties. This work presents a unique strategy for the development of magnetic‐electric materials and broadens the horizon for advanced intelligent devices with integrated functionalities.