Bipolar and unipolar electrical fatigue in ferroelectric lead zirconate titanate thin films: an experimental comparison study

TL;DR

This study compares bipolar and unipolar electrical fatigue in ferroelectric PZT thin films, revealing that unipolar fatigue is less severe and highlighting the importance of measurement methods and interface effects in polarization degradation.

Contribution

It provides the first experimental comparison of bipolar and unipolar fatigue in PZT thin films and introduces a new method to estimate the degraded interfacial layer thickness.

Findings

Unipolar fatigue is less severe than bipolar fatigue at the same voltage.

Dielectric and hysteresis measurements at higher voltages are more reliable for assessing fatigue.

Polarization fatigue primarily occurs at the interface, not in the bulk material.

Abstract

By performing standard PUND (positive-up-negative-down), hysteresis-loop and dielectric measurements on the ferroelectric lead zirconate titanate (PZT) thin-film capacitors subject to bipolar/unipolar electrical cycling, we show that unipolar fatigue is evident though still less severe than bipolar fatigue conducted at the same voltage. That has been attributed to polarization retention (backswitching) induced by the residual depolarization field between the monopolar pulses where the applied field is lower than the depolarization field, and explained using the LPD-SICI model (LPD-SICI stands for local phase decomposition caused by switching-induced charge injection). The conventional view that switching does not occur during unipolar electrical cycling may need to be corrected. PUND results recorded using the pulses of the same voltage as those for repetitive fatigue cycling are not reliable if the voltage is lower than 2Vc (Vc is the saturated coercive voltage). Dielectric measurements or hysteresis-loop measurements at higher voltages (e.g. 4Vc) are more reliable ways to evaluate the degree of fatigue and could provide more valuable information in such situations. Finally, dielectric results have been used to estimate the effective thickness di of the fatigue-induced degraded (pyrochlorelike) interfacial layer after bipolar/unipolar fatigue, which has not been done so far to our best knowledge. The fact that di is still much less than the film thickness even after the most severe bipolar fatigue strongly suggests that polarization fatigue in ferroelectrics is an interface effect, not a bulk one.