Orbital-ordering driven simultaneous tunability of magnetism and electric polarization in strained monolayer VCl3

Two-dimensional (2D) van der Waals magnetic materials have demonstrated promising and versatile electronic and magnetic properties in the 2D limit, indicating a considerable potential to advance spintronic applications. Theoretical predictions thus far have not ascertained whether monolayer VCl3 is a ferromagnetic (FM) or anti-FM monolayer; this also remains to be experimentally verified. This study entailed a theoretical investigation of the influence of potential factors, including C3 symmetry breaking, orbital ordering, epitaxial strain, and charge doping, on the magnetic ground state. Utilizing first-principles calculations, we predicted a collinear Type-III FM ground state in monolayer VCl3 with a broken C3 symmetry, wherein only the former two of three t 2gorbitals (a 1g, e π g2, and e π g1) are occupied. The atomic layer thickness and bond angles of monolayer VCl3 undergo abrupt changes driven by an orbital ordering switch, resulting in concomitant structural and magnetic phase transitions. Introducing doping to the underlying Cl atoms of monolayer VCl3 without C3 symmetry simultaneously induces in- and out-of-plane polarizations. This can achieve a multiferroic phase transition if combined with the discovered adjustments of magnetic ground state and polarization magnitude under strain. The establishment of an orbital-ordering driven regulatory mechanism can facilitate deeper exploration and comprehension of magnetic properties of strongly correlated systems in monolayer VCl3.