Tuning Structure and Magnetism in Large-Scale 2D Ferromagnet Fe$_3$GeTe$_2$ through Ni Doping

Two-dimensional ferromagnets with strong perpendicular magnetic anisotropy exhibit magnetic order down to the monolayer thickness, beneficial for energy-efficient spintronic devices. In this work, molecular beam epitaxy has been employed to realize controlled Ni-doping in Fe$_{3}$GeTe$_{2}$ (FGT) epitaxial films. MBE not only enables a large-scale growth of 2D films, but also allows a precise control over thickness and doping. X-ray diffraction and scanning transmission electron microscopy (STEM) reveal the formation of high-quality epitaxial films of pristine and Ni-doped FGT on graphene via van der Waals (vdW) epitaxy. Integrated differential phase contrast STEM images further provide in-depth information on Ni substitution and intercalation into the vdW gaps. Ni incorporation in doped films results in the shrinking of both in-plane and out-of-plane lattice parameters. Superconducting Quantum Interference Device, Hall, and X-ray magnetic circular dichroism measurements were utilized to probe the ferromagnetic properties of the films. Due to both Ni substitution and intercalation into the vdW gaps for Ni-doped FGT films, we observed a suppression of PMA and a drastic reduction in the Curie temperature down to 50 K. Our density functional theory based calculations of structural and magnetic properties further supports and provide deep insights into the variations of magnetic exchange interaction parameters and atom-projected magnetocrystalline anisotropy energies due to Ni doping to understand the experimental observations.