Wake-Up in a Hf0.5Zr0.5O2 Film: A Cycle-by-Cycle Emergence of the Remnant Polarization via the Domain Depinning and the Vanishing of the Anomalous Polarization Switching

The mechanism of the remnant polarization (Pr) growth during the first stage of ferroelectric HfO2-based memory cell operation (the wake-up effect) is still unclear. In this work, we reveal the microscopic nature of the Pr growth in functional ferroelectric capacitors based on a polycrystalline 10 nm thick (111) out-of-plane textured Hf0.5Zr0.5O2 film during electric cycling. We observe the cycle-by-cycle evolution of the domain structure with the piezoresponse force microscopy (PFM). During the early stage of the wake-up, three types of domains are found: (i) normal domains (polarization aligned along the applied electric field), (ii) nonswitchable domains with upward and downward polarization, and (iii) domains with anomalous polarization switching (polarization aligned against the applied electric field) that are commonly surrounded by nonswitchable domains. Initially, nonswitchable and “anomalous” domains are 200–300 nm in width, and they occupy ～70% of the capacitor area. During electric field cycling, these domains reduce in area, which is accompanied by the Pr growth. We attribute the domain pinning and the anomalous polarization reversal to the internal bias field of the oxygen vacancies. The local density of the oxygen vacancies decreases during electric cycling, thus producing the reduction of the internal bias field. The correlation of the PFM data with both the results of the structural analysis of fresh and cycled Hf0.5Zr0.5O2 film by transmission electron microscopy and the performance of the ferroelectric capacitor indicates that after the first cycle of the wake-up the Pr growth is not associated with phase transformations, but only with the transformation of the domain structure. The obtained results elucidate the physical mechanism of the emergence of Pr during the wake-up of the ferroelectric HfO2-based memory cell