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Searching for lead-free piezoelectric materials with a large piezoelectricity and excellent thermal stability has been a major concern in both scientific research and practical applications. To understand the mechanism of high piezoelectricity and its temperature-dependent behavior in lead-free materials, we focus here on the tetragonal (K,Na,Li)(Nb,Ta)O3 single crystal and investigate the intrinsic d33* along arbitrary directions as well as its evolution with temperature. The synergistic influence of several factors (narrow tetragonal temperature interval, sharp tetragonal-cubic phase transition, and large PS below TC) leads to a strong anisotropy in the d33* profile, while a high d33* is obtained around θ = 45° over a wide temperature range. This work comprehensively reveals the physical mechanism of piezoelectric anisotropy in lead-free materials, which provides vital information to design high-performance lead-free piezoelectric materials through orientation engineering and lattice manipulation, which is expected to benefit a wide range of piezoelectric materials.

Domain wall motions mainly affect all kinds of properties of ferroelectric materials, such as piezoelectricity, dielectric response, and mechanical loss, and the extrinsic contributions associated with domain wall motions have always been an important issue. In this study, the reversible and irreversible extrinsic contributions to the dielectric properties of [011]C‐oriented 0.27Pb(In1/2Nb1/2)O3‐0.46Pb(Mg1/3Nb2/3)O3‐0.27PbTiO3:Mn single crystals have been extracted by the Rayleigh analysis. We found that in the unpoled samples, the extrinsic contributions of reversible and irreversible domain wall motions to dielectric properties significantly reduced, whereas after poling, only the irreversible extrinsic contribution decreased. The pinning effect in the 2R domain structure is much weaker than that in the 4R domain structure, leading to the low enhancement of Qm and a slight decrease in piezoelectricity caused by acceptor doping in 2R domain structure. This study explores the domain wall dynamics of acceptor‐doped single crystals and mainly guides on further performance optimization in PbTiO3‐based relaxor single crystals.

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