Abstract The influence of donor and acceptor co-doping on structure and dielectric properties of (Ba 1− x Nd x )(Ti 1− y Fe y )O 3 (BNTF) ( x = 0.05, y = 0.01–0.07; and x = 0–0.08, y = 0.05) ceramics was investigated with X-ray diffraction (XRD), scanning electron microscopy (SEM), electron paramagnetic resonance (EPR), Raman spectroscopy, and dielectric measurements. When x y , two types of Nd 3+ –Fe 3+ and Fe 3+ – V O –Fe 3+ defect complexes formed and could not coexist, leading to the mixed phases of cubic and hexagonal. A single-phase ceramic with a cubic or tetragonal structure formed for x ⩾ y and the dielectric-peak temperature ( T m ) in BNTF with x = 0.05 decreased linearly with increasing y at a rate of −5 °C/mol% Fe ions. A high-k Y5V behavior can be realized at x = y = 0.05 (i.e., C-N5F5). The same concentrations of Nd 3+ and Fe 3+ formed Nd 3+ –Fe 3+ complexes, which could effectively suppress the dielectric loss and silence the 840 cm −1 band called “Raman charge effect” associated with Nd 3+ donors. C-N5F5 exhibited a cubic structure, medium-sized grains (3.3 μm), low dielectric loss ( e RT ′ = 6790). Defect chemistry associated with structure evolution is discussed.
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