Cross-Linking and Charging Molecular Magnetoelectronics.

Magnetoelectrics are witnessing an ever-growing success toward the voltage-controlled magnetism derived from inorganic materials. However, these inorganic materials have predominantly focused on the ferroelectromagnetism at solid-to-solid interfaces and suffered several drawbacks, including the interface-sensitive coupling mediators, high-power electric field, and limited chemical tunability. Here, we report a promising design strategy to shift the paradigm of next-generation molecular magnetoelectrics, which relies on the integration between molecular magnetism and electric conductivity though an in situ cross-linking strategy. Following this approach, we demonstrate a versatile and efficient synthesis of flexible molecular-based magnetoelectronics by cross-linking of magnetic coordination networks that incorporate conducting chain building blocks. The as-grown compounds feature an improved critical temperature up to 337 K and a room-temperature magnetism control of low-power electric field. It is envisaged that the cross-linking of molecular interfaces is a feasible method to couple and modulate magnetism and electron conducting systems.