The coupling between ferroelectricity and ferromagnetism in two-dimensional (2D) materials provides a promising pathway for the realization of electric-field-controlled spintronic devices. In this work, we unveil the microscopic mechanism underlying polarization-dependent magnetic anisotropy in the ferroelectric monolayer ${\mathrm{InCrTe}}_3$ through first-principles calculations. The monolayer ${\mathrm{InCrTe}}_3$, composed of five atomic sublayers with a ${\mathrm{Te}}_{\mathrm{I}}$-Cr-${\mathrm{Te}}_{\mathrm{II}}$-In-${\mathrm{Te}}_{\mathrm{III}}$ stacking sequence, exhibits two inequivalent polar states: a metallic $\mathrm{P}\uparrow$ state with tetrahedral Cr-Te coordination and an insulating $\mathrm{P}\downarrow$ state with octahedral coordination. We show that a substantially larger out-of-plane magnetic anisotropy energy (MAE) in the $\mathrm{P}\uparrow$ state arises from structural transformation and electronic reconstruction associated with a polar structural transition. In the metallic $\mathrm{P}\uparrow$ state, the central ${\mathrm{Te}}_{\mathrm{II}}$ atom undergoes a pronounced out-of-plane distortion, driving its $p$ orbitals closer to the Fermi level. The resulting hybridization between ${\mathrm{Te}}_{\mathrm{II}}\text{−}p$ and Cr-$d$ states enhances spin-orbit coupling (SOC), positioning ${\mathrm{Te}}_{\mathrm{II}}$ as a key SOC hotspot responsible for the large out-of-plane MAE. In contrast, in the insulating $\mathrm{P}\downarrow$ state, the more symmetric octahedral crystal field shifts the Te-$p$ states to lower energies, suppressing orbital mixing and reducing the out-of-plane MAE. These findings provide insight into how polar structural changes can modulate SOC-driven magnetic anisotropy through orbital engineering, offering a microscopic design principle for electrically controllable 2D multiferroic and spintronic devices.

Close

PrevNext

View figure in article

• Magnetic anisotropy
• Ferroelectrics
• Monolayer films
• Density functional calculations