The ferroelectric properties of hafnium oxide based thin films prepared by chemical solution deposition (CSD) are investigated. In this extensive study, a wealth of strongly different dopants (size and valence) and dopant concentrations is used to induce ferroelectricity in 42 nm thin films. Using the same precursors and preparation conditions for all dopants a good comparability is given. In particular, the dopant size appears to have a crucial impact on the resulting ferroelectric properties. For smaller dopants only a small ferroelectric response is observed whereas for larger dopants the remanent polarization is increased significantly. The crystal phase for varying dopant concentrations and dopant sizes is investigated by grazing incidence X-ray diffractions (GI-XRD). A dominating cubic phase is found for doping concentrations showing the highest remanent polarization. Similar to first CSD studies on Y:HfO 2 , this is reflected in a prominent wake-up behavior, which is attributed to a phase transition from cubic to orthorhombic during field cycling.
Comprehensive imprint measurements on PbZrxTi1−xO3 (PZT) thin films were carried out. Different models, which were proposed in literature to explain imprint in ferroelectric thin films or a similar aging effect (internal bias) in ferroelectric bulk material, are reviewed. Discrepancies between the experimental results obtained on the PZT films in this work and the prediction of the literature models indicate that these models do not describe the dominant imprint mechanism in PZT thin films. Hence, in this work a model is proposed which suggests imprint to be caused by a strong electric field within a thin surface layer in which the ferroelectric polarization is smaller or even absent compared to the bulk of the film. With the proposed imprint model the influence of important experimental parameters like dopant, illumination, and bias dependence can be qualitatively explained.
Ferroelectric and piezoelectric properties of Hf1-xZrxO2 (HZO) and pure ZrO2 films with a layer thickness of up to 390 nm prepared by chemical solution deposition (CSD) are investigated. The piezoelectric properties are measured using a double-beam laser interferometer (DBLI) and piezoresponse force microscopy. It is shown that for 100 nm thick films, the maximum remanent polarization is found for pure ZrO2 and reduces for the increasing hafnium content. A stable remanent polarization of 8 μC/cm2 is observed for ZrO2 film thicknesses between 195 and 390 nm. A piezoelectric coefficient of 10 pm/V is extracted from unipolar DBLI measurements. The observed thickness limitation for atomic layer deposition deposited HZO based ferroelectrics can be overcome by the CSD deposition technique presented in this work. Thick ZrO2 films are promising candidates for energy related applications such as pyroelectric and piezoelectric energy harvesting and electrocaloric cooling as well as for microelectromechanical systems.
The polarization reversal process of tetragonal Pb(Zr,Ti)O 3 thin films has been intensively studied using conventional hysteresis and rectangle pulse measurements. Decreasing the voltage level of the pulses significantly slows down the polarization switching to the range of milliseconds. The switching current response shows a Curie-von Schweidler behavior over a broad time range. The transient current and the frequency dependence of the P -V loops of these films compared to the properties of ferroelectric single crystals show some similarities but also significant differences. The theoretical models of the classical ferroelectric phase transition and especially the conditions of the pulse measurements in single crystals and thin films are discussed. It leads to the conclusion that it is not the domain wall structure and domain wall motion that determine the polarization reversal but dissipative polarization processes which can take place in both ferroelectric and nonferroelectric high-k dielectric thin films.
In this article, the interface screening model is theoretically discussed which explains imprint in ferroelectric thin films caused by a large electric field within a surface layer with deteriorated ferroelectric properties. During aging this field is gradually screened by electronic charges. Different screening mechanisms such as charge injection from the electrodes into the film as well as charge separation within the surface layer are considered by implementing a numerical simulation based on the different screening mechanisms. A comparison between experimental and simulation results is presented. The best agreement between experiment and simulation is obtained for a Frenkel–Poole type charge separation mechanism within the surface layer. The simulation results indicate relatively shallow trap states (0.35 eV) and a surface layer extension of approximately 5 nm.
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