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Perovskite developments in the Pb(Zn1/3Ta2/3)O3–PbTiO3 system were explored. Formation yields and lattice parameters of the perovskite were determined from X‐ray diffractometry results. Weak‐field low‐frequency dielectric properties of the system ceramics were investigated, followed by microstructure examination. Perovskite started to develop in Pb(Zn1/3Ta2/3)O3 after the introduction of 30 mol% PbTiO3, whereas complete stabilization was accomplished at 60% substitution. Dielectric relaxation behavior was not substantial across the entire composition range, whereas phase transition modes changed from diffuse to sharp with increased PbTiO3 fraction.

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