As introduced before, due to the paramagnetic behavior of Mn II+ complexes, standard 1 H-NMR experiments do not provide insightful information on the purity and structural identity. In contrast to the found magnetic moments of the all-nitrogen coordinated compounds, the Evans method measurements on the manganese ß-ketoiminates exhibit unexpected yet interesting results. The values of the magnetic moments determined can be found in the SI. For compounds ßIII and ßIV, magnetic moments of 5.4 μB and 5.5 μB respectively were found. This is in line with the expected magnetic moment of 5.9 μB for the five unpaired electrons, which suggest tetrahedral or octahedral high spin complexes. On the other hand, for compound ßI and ßII, much higher magnetic moments of 6.5 μB and 7.0 μB respectively were determined. Considering theoretical values of the magnetic moment for potential counts of unpaired electrons, leads to 6 unpaired electrons (µcalc = 6.9 μB). While considering possible spin states for mononuclear complexes, 6 unpaired electrons cannot be explained, as for d-elements, only 5 unpaired electrons are possible. But the consideration of other ligand field splitting and the potential formation of dinuclear structures could explain the high magnetic moments. This in turn, would facilitate the establishment of three unpaired electrons per Mn center in low spin configuration in a trigonal bipyramidal ligand field splitting (graphically illustrated in Figure ), which is in contrast to the tetrahedral mononuclear low-spin Mn complexes that commonly result in one unpaired electrons and high spin complexes exhibiting five unpaired electrons. A detailed discussion on the single crystal structures determined helps to verify this presumption.