Interfacial dielectric layer as an origin of polarization fatigue in ferroelectric capacitors

Origins of polarization fatigue in ferroelectric capacitors under electric field cycling still remain unclear. Here, we experimentally identify origins of polarization fatigue in ferroelectric PbZr_0.52Ti_0.48O₃ (PZT) thin-film capacitors by investigating their fatigue behaviours and interface structures. The PZT layers are epitaxially grown on SrRuO₃-buffered SrTiO₃ substrates by a pulsed laser deposition (PLD), and the capacitor top-electrodes are various, including SrRuO₃ (SRO) made by in-situ PLD, Pt by in-situ PLD (Pt-inPLD) and ex-situ sputtering (Pt-sputtered). We found that fatigue behaviour of the capacitor is directly related to the top-electrode/PZT interface structure. The Pt-sputtered/PZT/SRO capacitor has a thin defective layer at the top interface and shows early fatigue while the Pt-inPLD/PZT/SRO and SRO/PZT/SRO capacitor have clean top-interfaces and show much more fatigue resistance. The defective dielectric layer at the Pt-sputtered/PZT interface mainly contains carbon contaminants, which form during the capacitor ex-situ fabrication. Removal of this dielectric layer significantly delays the fatigue onset. Our results clearly indicate that dielectric layer at ferroelectric capacitor interfaces is the main origin of polarization fatigue, as previously proposed in the charge injection model.