Reversible modulation of critical electric fields for a field-induced ferroelectric effect with field-cycling in ZrO2 thin films†

This study investigates the effects of field-cycling on the critical electric fields (E_t→PO and E_PO→t) of the field-induced ferroelectric (FFE) effect in atomic layer deposited ZrO₂ thin films, focusing on their reversibility and temperature dependence. High-field cycling decreases these critical fields, whereas subsequent lower-field cycling effectively rejuvenates them, challenging the previous report of their irreversibility. Elevated temperature experiments reveal that higher temperature increases the lower limit of E_t→PO reduction, corroborating the thermodynamic predictions of the Landau–Ginzburg–Devonshire (LGD) theory. The rejuvenation effect is also more pronounced at higher temperatures, further corroborating the LGD theory. This study highlights that these reversible transitions between polar and non-polar phases with high- and low-field cycling are a universal phenomenon in fluorite-structured materials, not limited to ferroelectric materials. These findings provide new insights into the field-cycling and temperature-dependent behavior of FFE thin films.