Starting with model size 6×6 within GGA, the total magnetic moments (M tot ) of the pyridinic and pyrrolic models are 1.97 µ B and 2.20 µ B , corresponding to the 2S + 1 = 3 intermediate spin configuration. These values result from different orbital occupations, see Figure (a) and (b) for the spin densities. The pyridinic model A is found in an IS3 configuration. Consequently, the shape of the spin density is determined by a combination of both d xz and d z 2 orbitals, see Figure . We note that the local axes used to describe cubic harmonics in the periodic models are rotated by 45°with respect to the crystallographic c-axis compared to those in the molecular models. As a result, the lowest occupied orbital in the periodic model is d x 2 -y 2 , whereas it is d xy in molecular models in the respective reference frame, but note that it is the same orbital. The pyrrolic model B is found in the IS1 configuration, resulting in a spin density shape that contains d xz and d yz contributions. These intermediate spin configurations remain unchanged when employing the GGA+U or PBE0 hybrid functional, as shown in Figures and in the SI.