Abstract

PbZrO3-based antiferroelectric crystals are of great interest in both fundamental and applied research, not only because of the antiferroelectric feature at room temperature but also because of the existence of a peculiar intermediate state at elevated temperatures. Here, we report a detailed description of domain structure change at the temperature-induced antiferroelectric-to-ferroelectric phase transition. A complex process of different types of domains is revealed to appear at different stages of the phase transition. A hierarchical ferroelastic domain structure forms in the stabilized intermediate state, where the dense domain walls show potential impact on the physical properties of the crystal.

Highlights

  • As the most widely used antiferroelectric (AFE) material, PbZrO3 (PZ) and PZ-related solid solutions have received extensive attention in fundamental studies and applications, such as actuators and energy conversion devices.1,2 the discovery of ferroelectric translational antiphase boundaries in the AFE phase of PZ3 suggests its application as a novel functional entity

  • A compensator was inserted between the sample and the analyzer and was rotated to an arbitrary angle in order to distinguish the ferroelastic domains with orientations perpendicular to each other. (a) At room temperature. (b) At 227 ○C in the IM state upon heating. (c) At 234 ○C in the IM state upon cooling

  • We investigated the domain structures of PbZr0.98Ti0.02O3 single crystals with a room-temperature AFE phase and a higher-temperature intermediate state

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Summary

INTRODUCTION

As the most widely used antiferroelectric (AFE) material, PbZrO3 (PZ) and PZ-related solid solutions (such as Zr-rich PbZr1−xTixO3, PZT, with x ≤ 0.06) have received extensive attention in fundamental studies and applications, such as actuators and energy conversion devices. the discovery of ferroelectric translational antiphase boundaries in the AFE phase of PZ3 suggests its application as a novel functional entity. The mysterious atomic structure in this phase, both at long-range and local scales, has initiated many discussions in recent years Superstructure reflections, such as intensities at the M points and incommensurate points, were observed via various diffraction and scattering experiments, showing the complexity of the intermediate structure. We recently proposed an average structural model with a coexistence of monoclinic Pc and Cm symmetries while in the short range with competitions of multiple modes, namely, at the Γ point, M point, incommensurate point, and Σ point This complicated structure co-existence is denoted as an IM state instead of a single phase. In the past decade, domain walls themselves have been found to exhibit unique properties separately from the domain bulk, such as electronic conductivity and the photovoltaic effect.32,33 These discoveries have aroused increasing interest in further exploring the domain structures of prototypical materials. Optical experiments and dielectric measurements were used for probing the domain structures as well as the domain structural changes through the phase transition

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