Abstract
The unique properties of ferroelectric materials enable a plethora of applications, which are hindered by the phenomenon known as ferroelectric fatigue that leads to the degradation of ferroelectric properties with polarization cycling. Multiple microscopic models explaining fatigue have been suggested; however, the chemical origins remain poorly understood. Here, we utilize multimodal chemical imaging that combines atomic force microscopy with time-of-flight secondary mass spectrometry to explore the chemical phenomena associated with fatigue in PbZr0.2Ti0.8O3 (PZT) thin films. Investigations reveal that the degradation of ferroelectric properties is correlated with a local chemical change and migration of electrode ions into the PZT structure. Density functional theory simulations support the experimental results and demonstrate stable doping of the thin surface PZT layer with copper ions, leading to a decrease in the spontaneous polarization. Overall, the performed research allows for the observation and understanding of the chemical phenomena associated with polarization cycling and their effects on ferroelectric functionality.
Highlights
The unique properties of ferroelectric materials enable a plethora of applications, which are hindered by the phenomenon known as ferroelectric fatigue that leads to the degradation of ferroelectric properties with polarization cycling
The chemical aspects of fatigue are still poorly understood with studies mostly limited to electron microscopy research, which do not allow for examination of the connection between material functional response and local chemical signatures in-situ[19,28,29,30]
This approach combines different complimentary imaging techniques, like atomic force microscopy (AFM), in order to provide information about functional material responses and mass spectrometry chemical imaging to allow for the precise mapping of the chemical composition of the surface and in the bulk
Summary
The unique properties of ferroelectric materials enable a plethora of applications, which are hindered by the phenomenon known as ferroelectric fatigue that leads to the degradation of ferroelectric properties with polarization cycling. We utilize multimodal chemical imaging that combines atomic force microscopy with time-offlight secondary mass spectrometry to explore the chemical phenomena associated with fatigue in PbZr0.2Ti0.8O3 (PZT) thin films. We utilize multimodal chemical imaging that combines AFM with ToF-SIMS to study the chemical phenomena associated with fatigue in ferroelectric thin films. Subsequent 3D chemical imaging indicates that this behavior is correlated with the quasi-doping of the film due to the introduction of copper ions into a few nanometerthick layer of PZT These results are consistent with DFT calculations showing a corresponding decrease in the spontaneous polarization with increasing Cu doping concentration. The explored chemical phenomena are important for understanding the fundamental properties of ferroelectric materials and their practical applications
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