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A series of morphotropic phase boundary (MPB) compositions of (1–x)Na1/2Bi1/2TiO3‐xBaTiO3 (x = 0.05, 0.055, 0.06, 0.065, 0.07), with and without 0.5 mol% Zn‐doping was synthesized using the solid‐state route. The samples were characterized using X‐ray diffraction, dielectric analysis, and electromechanical measurements (piezoelectric d33 coefficient, coupling factor kp, mechanical quality factor Qm, and internal bias field Ebias). The increase in the ferroelectric‐relaxor transition temperature upon Zn‐doping was accompanied by a shift of the MPB toward the Na1/2Bi1/2TiO3‐rich side of the phase diagram. Higher tetragonal phase fraction and increased tetragonal distortion were noted for Zn‐doped (1 – x)Na1/2Bi1/2TiO3‐xBaTiO3. In addition, ferroelectric hardening and the presence of an internal bias field (Ebias) were observed for all doped compositions. The piezoelectric constant d33 and the coupling coefficient kp decreased by up to ∼30%, while a 4‐ to 6‐fold increase in Qm was observed for the doped compositions. Apart from establishing a structure–property correlation, these results highlight the chemically induced shift of the phase diagram upon doping, which is a crucial factor in material selection for optimal performance and commercialization. [ABSTRACT FROM AUTHOR]

A series of morphotropic phase boundary (MPB) compositions of (1–x)Na1/2Bi1/2TiO3‐xBaTiO3 (x = 0.05, 0.055, 0.06, 0.065, 0.07), with and without 0.5 mol% Zn‐doping was synthesized using the solid‐state route. The samples were characterized using X‐ray diffraction, dielectric analysis, and electromechanical measurements (piezoelectric d33 coefficient, coupling factor kp, mechanical quality factor Qm, and internal bias field Ebias). The increase in the ferroelectric‐relaxor transition temperature upon Zn‐doping was accompanied by a shift of the MPB toward the Na1/2Bi1/2TiO3‐rich side of the phase diagram. Higher tetragonal phase fraction and increased tetragonal distortion were noted for Zn‐doped (1 – x)Na1/2Bi1/2TiO3‐xBaTiO3. In addition, ferroelectric hardening and the presence of an internal bias field (Ebias) were observed for all doped compositions. The piezoelectric constant d33 and the coupling coefficient kp decreased by up to ∼30%, while a 4‐ to 6‐fold increase in Qm was observed for the doped compositions. Apart from establishing a structure–property correlation, these results highlight the chemically induced shift of the phase diagram upon doping, which is a crucial factor in material selection for optimal performance and commercialization. [ABSTRACT FROM AUTHOR]