For periodic models, the projector augmented wave (PAW) method implemented in Vienna Ab initio Simulation Package (VASP) was employed. To treat the exchange-correlation functional, we utilized the PBE GGA functional and GGA with on-site Coulomb repulsion U (GGA+U ) to account for localized 3d orbitals accurately. The first Brillouin zone was sampled using a Gamma-centered 4×4×1 k-mesh for structure relaxation, while denser k-mesh values of 21×21×1 (for the 4×4 unit cell), 15×15×1 (for 6×6), and 9×9×1 (for 8×8) were chosen for single-point calculations. The plane-wave basis set size was determined by the energy cutoff of 400 eV (500 eV) for relaxation (single-point calculations). All atomic positions were fully relaxed until the net force became smaller than 0.01 eV/Å. To prevent interactions between layers along the crystallographic c-axis, a 20 Åvacuum layer was introduced in all structures. However, for cases with the axial 2-MeHIm ligand, the vacuum thickness was increased to 30 Å.