Abstract

The discovery of ultrahigh piezoelectricity in relaxor-ferroelectric solid solution single crystals is a breakthrough in ferroelectric materials. A key signature of relaxor-ferroelectric solid solutions is the existence of polar nanoregions, a nanoscale inhomogeneity, that coexist with normal ferroelectric domains. Despite two decades of extensive studies, the contribution of polar nanoregions to the underlying piezoelectric properties of relaxor ferroelectrics has yet to be established. Here we quantitatively characterize the contribution of polar nanoregions to the dielectric/piezoelectric responses of relaxor-ferroelectric crystals using a combination of cryogenic experiments and phase-field simulations. The contribution of polar nanoregions to the room-temperature dielectric and piezoelectric properties is in the range of 50–80%. A mesoscale mechanism is proposed to reveal the origin of the high piezoelectricity in relaxor ferroelectrics, where the polar nanoregions aligned in a ferroelectric matrix can facilitate polarization rotation. This mechanism emphasizes the critical role of local structure on the macroscopic properties of ferroelectric materials.

Highlights

  • The discovery of ultrahigh piezoelectricity in relaxor-ferroelectric solid solution single crystals is a breakthrough in ferroelectric materials

  • It should be noted that the large longitudinal piezoelectric properties in domain-engineered relaxor–PT crystals originate from the high shear piezoelectric response in the corresponding single-domain state28–30

  • To demonstrate the generality of our results and the proposed mechanism, we investigated three different types of phases with all of them single-domain crystals: (1) rhombohedral [111]-poled PMN–0.28PT; (2) orthorhombic [011]-poled PMN–0.32PT; and (3) tetragonal [001]-poled PZN–0.15PT crystals

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Summary

Introduction

The discovery of ultrahigh piezoelectricity in relaxor-ferroelectric solid solution single crystals is a breakthrough in ferroelectric materials. A mesoscale mechanism is proposed to reveal the origin of the high piezoelectricity in relaxor ferroelectrics, where the polar nanoregions aligned in a ferroelectric matrix can facilitate polarization rotation. This mechanism emphasizes the critical role of local structure on the macroscopic properties of ferroelectric materials. The corresponding mechanisms include ‘electric field-induced phase transition’6, ‘ease of polarization rotation via a monoclinic phase’13,14, ‘giant electromechanical response as a critical phenomenon’15, ‘adaptive domain structure’ and so on These mechanisms fail to explain why relaxor-ferroelectric solid solutions exhibit significantly higher piezoelectricity when compared with nonrelaxor-based MPB ferroelectrics, for example, crystals (500–1,000 pC N À 1 for x around 0.5). For example, PMN, are characterized by cation disorder on the nanoscale, Loss factor

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