Adding an axial 2-MeHIm ligand to the pyridinic models maintains an intermediate spin state, see Figure . Consequently, the isomer shift is converged within the uncertainty range at all model sizes, and the quadrupole splitting is converged at model size 4, probably due to its symmetry dependence and the asymmetry of size 2 and 3. No true high spin state is energetically accessible at any model size. The experimentally observed iron(II) high spin signals can thus not be explained with this pyridinic model, as is supported by Ni, Gallenkamp et al. This can be explained with the structure of the A-2-MeHIm complex, where the iron is strictly in plane with the carbon environment, destabilizing high spin states . The axial ligand is thus not sufficient to significantly alter the ligand field and stabilize the highest lying d-orbital.