Unveiling the stacking-dependent electronic properties of the 2D ultrathin rare-earth metalloxenes family LnX₂ (Ln = Eu, Gd, Dy; X = Ge, Si)

Studies of electronic effects in reduced dimensionality have become a frontier in nanoscience due to the exotic and highly tunable character of quantum phenomena. Recently, a new class of 2D ultrathin LnX(2) metalloxenes composed of a triangular lattice of lanthanide ions (Ln) coupled with 2D-Xenes of silicene or germanene (X-2) was introduced and studied with a particular focus on magnetic and transport properties. However, the electronic properties of metalloxenes and their effective functionalization remain mainly unexplored. Here, using a number of experimental and theoretical techniques, we trace the evolution of the electronic properties and magnetic ground state of metalloxenes triggered by external perturbations. We demonstrate that the band structure of LnX(2) films can be uniquely modified by controlling the Xenes stacking, thickness, varying the rare-earth and host elements, and applying an external electric field. Our findings suggest new pathways to manipulate the electronic properties of 2D rare-earth magnets that can be adjusted for spintronics applications.