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Two-dimensional (2D) multiferroics exhibit cross-control capacity betweenmagnetic and electric responses in reduced spatial domain, making them wellsuited for next-generation nanoscale devices; however, progress has been slowin developing materials with required characteristic properties. Here weidentify by first-principles calculations robust 2D multiferroic behaviors indecorated Fe2O3 monolayer, showcasing N@Fe2O3 as a prototypical case, whereferroelectricity and ferromagnetism stem from the same origin, namely Fed-orbit splitting induced by the Jahn-Teller distortion and associated crystalfield changes. The resulting ferromagnetic and ferroelectric polarization canbe effectively reversed and regulated by applied electric field or strain,offering efficient functionality. These findings establish strong materialsphenomena and elucidate underlying physics mechanism in a family of truly 2Dmultiferroics that are highly promising for advanced device applications.

Multiferroic Decorated Fe2O3 Monolayer Predicted from First Principles