Abstract The spin Hamiltonian parameters (SHPs) of Cu2+‐doped halo‐glasses PbX2–PbO–B2O3 (X = F and Br) are investigated by means of the perturbation method where the impact of the halides and the local structure of the dopants, that is, the [CuO6]10− clusters suffering the tetragonal elongation distortions, is involved. By comparing with the obtained results of the 3d1 system (VO2+), Cu2+ and V4+ are complementary state, which show opposite distortions. Furthermore, the d‐d transition bands and the sign of anisotropy g factors also show whole opposite concentration variation trends with similar fluctuations due to the increase of non‐bridging oxygen (NBO). The values of the optical basicity Λth referring to the Pauling electronegativity, whose influence on E1 and g factors are also discussed. The above correlations would be beneficial to analyze and predict the properties of analogous borate glasses and ceramics when doped with different transition metal ions.
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