Paramagnetic resonance has been studied on the ions [CrI dip3]+, [V° dip3] and [Ti-I dip3]- in the polycrystalline state and in solution. The spectra arising from the odd isotopes gave g=1.9973 ± 0.0002 and |A| = (21.8 ± 0.5) gauss for Cr53; g= 1.9831 ± 0.0002 and |A| = (83.5 ± 1.0) gauss for V51. The splitting constants of the additional HFS due to ligand N14 nuclei were found to be | AN |= (3.05 ± 0.05) gauss and |AN| = (2.3 ± 0.1) gauss, respectively. For the titanium compound only the resonance due to the even-even isotopes was observed giving g=2.0074 ± 0.0002 . It is shown that the results for [CrI dip3]+ and [V°dip3] are consistent with an A1 ground state with 5.47% and 1.09% 4s-admixture, respectively. Further, it is shown that the results suggest strong σ-bonding between metal 4s and ligand Σ0+ orbitals increasing in the order Ti-, V0, Cr+. Two other possibilities to explain the observed HFS are ruled out.