Phase Transformations Driving Biaxial Stress Reduction During Wake‐Up of Ferroelectric Hafnium Zirconium Oxide Thin Films

Biaxial stress is identified to play an important role in the polar orthorhombic phase stability in hafnium oxide‐based ferroelectric thin films. However, the stress state during various stages of wake‐up has not yet been quantified. In this work, the stress evolution with field cycling in hafnium zirconium oxide capacitors is evaluated. The remanent polarization of a 20 nm thick hafnium zirconium oxide thin film increases from 9.80 to 15.0 µC cm−2 following 106 field cycles. This increase in remanent polarization is accompanied by a decrease in relative permittivity that indicates that a phase transformation has occurred. The presence of a phase transformation is supported by nano‐Fourier transform infrared spectroscopy measurements and scanning transmission electron microscopy that show an increase in ferroelectric phase content following wake‐up. The stress of individual devices field cycled between pristine and 106 cycles is quantified using the sin2(ψ) technique, and the biaxial stress is observed to decrease from 4.3 ± 0.2 to 3.2 ± 0.3 GPa. The decrease in stress is attributed, in part, to a phase transformation from the antipolar Pbca phase to the ferroelectric Pca21 phase. This work provides new insight into the mechanisms controlling and/or accompanying polarization wake‐up in hafnium oxide‐based ferroelectrics. Biaxial stress in ferroelectric hafnium zirconium oxide capacitors is quantified during electric field cycling. A remanent polarization increases from 9.80 to 15.0 µC cm−2 after 106 cycles is accompanied by a 1 GPa stress decrease. The observed wake‐up and stress reduction is attributed to a phase transformation from the antipolar Pbca phase to the ferroelectric Pca21 phase and ferroelastic switching.