The effects of gamma irradiation on the dielectric and piezoelectric responses of Pb[Zr0.52Ti0.48]O3 (PZT) thin film stacks were investigated for structures with conductive oxide (IrO2) and metallic (Pt) top electrodes. The samples showed, generally, degradation of various key dielectric, ferroelectric, and electromechanical responses when exposed to 2.5 Mrad (Si) 60Co gamma radiation. However, the low-field, relative dielectric permittivity, εr, remained largely unaffected by irradiation in samples with both types of electrodes. Samples with Pt top electrodes showed substantial degradation of the remanent polarization and overall piezoelectric response, as well as pinching of the polarization hysteresis curves and creation of multiple peaks in the permittivity-electric field curves post irradiation. The samples with oxide electrodes, however, were largely impervious to the same radiation dose, with less than 5% change in any of the functional characteristics. The results suggest a radiation-induced change in the defect population or defect energy in PZT with metallic top electrodes, which substantially affects motion of internal interfaces such as domain walls. Additionally, the differences observed for stacks with different electrode materials implicate the ferroelectric–electrode interface as either the predominant source of radiation-induced effects (Pt electrodes) or the site of healing for radiation-induced defects (IrO2 electrodes).
This work investigates the role of crystallization layers’ periodicity and thickness on functional response in chemical solution‐deposited lead zirconate titanate thin films, with periodic, alternating Zr and Ti gradients normal to the surface of the film. The films were processed with a range of layer periodicities and similar total film thickness, in order to relate the number of layers and compositional oscillations to structural and functional response changes. Trends of increased extrinsic contributions to the dielectric and ferroelectric responses are observed with increasing layer periodicity, but are counterpointed by simultaneous reduction in intrinsic contributions to the same. Transmission electron microscopy reveals in‐plane crystallographic discontinuity at individual crystallization interfaces. Samples with smaller periodicity, and thus thinner layers, potentially suffer from grain size refinement and subsequent reduction in domain size, thereby limiting extrinsic contributions to the response. The strong compositional oscillations in samples with larger periodicity result in deep fluctuations to the tetragonal side of the phase diagram, potentially reducing intrinsic contributions to the response. Conversely, piezoresponse force microscopy results suggest that large chemical oscillations in samples with larger periodicity also result in closer proximity to the morphotropic phase boundary, as evidenced by local acoustic softening at switching, signaling potential field‐induced phase transitions.
The influence of surface morphology on the local piezoelectric response of highly (100)-textured 0.70PbMg2/3Nb1/3O3-0.30PbTiO3 thin films is studied using piezoresponse force microscopy in band-excitation mode. The local electromechanical response is mostly suppressed in direct proximity of the grain boundaries. However, within 100–200 nm of the grain boundary, the piezoresponse is substantially enhanced, before decaying again within a region at the center of the grain itself. Nested piezoresponse hysteresis curves confirm the influence of topography descriptors on parameters affecting the hysteresis loop shape. The enhancement of the electromechanical response is rationalized through reduced lateral clamping in the grains with deep trenched boundaries, as well as an expected lower energy for complex domain wall structures, due to curved ferroelectric surfaces. The lower piezoresponse at the center of the grain is assigned to the lateral clamping by the surrounding piezoelectric material.
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