Two-Dimensional Organic–Inorganic Room-Temperature Multiferroics

Organic-inorganic multiferroics are promising for the next generation of electronic devices. To date, dozens of organic-inorganic multiferroics have been reported; however, most of them show a magnetic Curie temperature much lower than room temperature, which drastically hampers their application. Here, by performing first-principles calculations and building effective model Hamiltonians, we reveal a molecular orbital-mediated magnetic coupling mechanism in two-dimensional Cr(pyz)₂ (pyz = pyrazine) and the role that the valence state of the molecule plays in determining the magnetic coupling type between metal ions. Based on these, we demonstrate that a two-dimensional organic-inorganic room-temperature multiferroic, Cr(h-fpyz)₂ (h-fpyz = half-fluoropyrazine), can be rationally designed by introducing ferroelectricity in Cr(pyz)₂ while keeping the valence state of the molecule unchanged. Our work not only reveals the origin of magnetic coupling in 2D organic-inorganic systems but also provides a way to design room-temperature multiferroic materials rationally.