Atomic-resolution Cs-corrected scanning transmission electron microscopy revealed local shifting of two oxygen positions (OI and OII) within the unit cells of a ferroelectric (Hf0.5Zr0.5)O2 thin film. A reversible transition between the polar Pbc21 and antipolar Pbca phases, where the crystal structures of the 180° domain wall of the Pbc21 phase and the unit cell structure of the Pbca phase were identical, was induced by applying appropriate cycling voltages. The critical field strength that determined whether the film would be woken up or fatigued was ~0.8 MV/cm, above or below which wake-up or fatigue was observed, respectively. Repeated cycling with sufficiently high voltages led to development of the interfacial nonpolar P42/nmc phase, which induced fatigue through the depolarizing field effect. The fatigued film could be rejuvenated by applying a slightly higher voltage, indicating that these transitions were reversible. These mechanisms are radically different from those of conventional ferroelectrics.
HfO2‐based ferroelectric materials are promising candidates for next‐generation nonvolatile memories. Since the first report on Si‐doped HfO2 ferroelectric thin film in 2011, it has been confirmed that various dopants can induce ferroelectricity in HfO2‐based films, and the “wake‐up” effect in HfO2 films with different dopants deposited by different processes has been studied extensively. Recent developments in the wake‐up effect of doped HfO2‐based films are presented. Aside from the differences between the various ferroelectric materials and their deposition methods, the electrodes used in a ferroelectric capacitor, which determine the nature of the interface between the electrode and the ferroelectric layer, can strongly influence the characteristics of the wake‐up effect. The rate of variation of the remanent polarization shows certain trends with different dopants. Based on the wake‐up mechanisms, many methods to optimize and control this effect are presented in this letter. Until now, the reported mechanism explanations of the wake‐up effect all aimed at one type of specific dopant or deposition technique, but can't systematically interpret why the root causes might be different with different dopants and deposition processes. There is also a lack of in‐depth research on the effects of interfacial layer with respect to different electrode material.
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