Robust Magnetoelectric Effect in the Decorated Graphene/InSe Heterostructure.

The magnetoelectric effect is a fundamental physical phenomenon that synergizes electric and magnetic degrees of freedom to generate distinct material responses like electrically tuned magnetism, which serves as a key foundation of the emerging field of spintronics. Here, we show by first-principles studies that ferroelectric (FE) polarization of an InSe monolayer can modulate the magnetism of an adjacent transition-metal (TM)-decorated graphene layer via a ferroelectrically induced electronic transition. The TM nonbonding -orbital shifts downward and hybridizes with carbon-p states near the Fermi level, suppressing the magnetic moment, under one FE polarization, but on reversed FE polarization this TM -orbital moves upward, restoring the original magnetic moment. This finding of robust magnetoelectric effect in the TM-decorated graphene/InSe heterostructure offers powerful insights and a promising avenue for experimental exploration of ferroelectrically controlled magnetism in two-dimensional (2D) materials.