An Unconventional Transient Phase with Cycloidal Order of Polarization in Energy‐Storage Antiferroelectric PbZrO3

Xian‐Kui Wei,Rafal E Dunin‐Borkowski,Hong‐Chu Du,Krystian Roleder,Chun‐Lin Jia,Joachim Mayer

doi:10.1002/adma.201907208

Abstract

Antiferroelectric-based dielectric capacitors are receiving tremendous attention for their outstanding energy-storage performance and extraordinary flexibility in collecting pulsed powers. Nevertheless, the in situ atomic-scale structural-evolution pathway, inherently coupling to the energy storage process, has not been elucidated for the ultimate mechanistic understanding so far. Here, time- and atomic-resolution structural phase evolution in antiferroelectric PbZrO3 during storage of energy from the electron-beam illumination is reported. By employing state-of-the-art negative-spherical-aberration imaging technique, the quantitative transmission electron microscopy study presented herein clarifies that the hierarchical evolution of polar oxygen octahedra associated with the unit-cell volume change and polarization rotation accounts for the stepwise antiferroelectric-to-ferroelectric phase transition. In particular, an unconventional ferroelectric category-the ferrodistortive phase characteristic of a unique cycloidal polarization order-is established during the dynamic structure investigation. Through clarifying the atomic-scale phase transformation pathway, findings of this work unveil a new territory to explore novel ferrodistortive phases in energy-storage materials with the nonpolar-to-polar phase transitions.

Highlights

Citation style: Wei Xian-Kui, Jia Chun-Lin, Du Hong-Chu, Roleder Krystian, Mayer Joachim, Dunin-Borkowski Rafal E. (2020)
With adoption of different design strategies, e.g., polymorphic nanodomain,[3] chemical doping[4] and structure sandwiching,[5] the recoverable energy density has been improved from ≈5 to over 150 J cm−3 during storage of energy from the electron-beam illumination is reported
Among the dielectrics, employing state-of-the-art negative-spherical-aberration imaging technique, the antiferroelectric-based capacitors serve as an quantitative transmission electron microscopy study presented clarifies that the hierarchical evolution of polar oxygen octahedra associated with the unit-cell volume change and polarization rotation accounts for the stepwise antiferroelectric-to-ferroelectric phase transition

Summary

Introduction

Citation style: Wei Xian-Kui, Jia Chun-Lin, Du Hong-Chu, Roleder Krystian, Mayer Joachim, Dunin-Borkowski Rafal E. (2020). Our time- and atomic-resolution TEM study provides a novel insight to understand the phase-transition pathway in PbZrO3-based energy-storage materials.

Results

Conclusion