In Situ Observation of Point-Defect-Induced Unit-Cell-WiseEnergy Storage Pathway in Antiferroelectric PbZrO3

Abstract

Phase transition is established to govern electrostatic energy storage for antiferroelectric (AFE)-type dielectric capacitors. However, the source of inducing the phase transition and the pathway of storing the energy remains elusive so far given the ultrafast charging/discharging process under normal working conditions. Here, by slowing down the phase-transition speed using electronbeam irradiation as an external stimulus, the in situ dynamic energy-storage process in AFE PbZrO3 is captured by using atomic-resolution transmission electron microscopy. Specifically, it is found that oxygen-lead-vacancy-induced defect core acts as a seed to initiate the antiferrodistortive-to-ferrodistortive transition in antiparallel-Pb-based structural frames. Associated with polarity evolution of the compressively strained defect core, the ferroelectric (FE)– ferrodistortive state expands bilaterally along the b-axis direction and then develops into charged domain configurations during the energy-storage process, which is further evidenced by observations at the ordinary FE states. With filling the gap of perception, the findings here provide a straightforward approach of unveiling the unit-cell-wise energy storage pathway in chemical defect-engineered dielectric ceramics.