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Systematic measurements of the magnetic moment of hexagonal 6H-BaTiO 3  + 0.04 BaO +  x  NiO (0.005 ≤  x  ≤ 0.02) ceramics were performed to study the influence of Ni ions on the magnetic properties. By temperature-dependent measurements of the paramagnetic susceptibility at 90 kOe, the Ni 2+  ion was identified as the majority defect in air-sintered Ni-doped hexagonal barium titanate. Q-band EPR investigations of a 2.0 mol% Ni-doped single crystal revealed three different Ni centers located at Ti sites: first, Ni 3+  ions at Ti sites in intact oxygen octahedra, second, Ni 3+  associated with an oxygen vacancy and third, the presence of Ni 2+  centers leading to a forbidden transition. The Ni 3+ —V O  associate characterized by a vacancy in the face-sharing oxygen plane of the oxygen octahedra can be ruled out. The crystal field parameters of the Ni 2+  defect were estimated by a combined fitting of the paramagnetic susceptibility and the EPR fine structure parameter D to    $$B_{0}^{4}$$  B 0 4 ≈ −17,300 cm −1 ,    $$\left| {B_{0}^{2} } \right|$$  B 0 2 ≈ 2500 cm −1  and    $$B_{3}^{4}$$  B 3 4 ≈ 19,000 cm −1 .

On the incorporation of nickel into hexagonal barium titanate: magnetic properties and electron paramagnetic resonance (EPR)