Tailoring radiation tolerance of HfO2-ZrO2 ferroelectric nanolaminates via layer-thickness engineering

Nanolaminate ferroelectric thin films, particularly HfO 2 -ZrO 2 based systems, are highly valued for their exceptional fatigue resistance. However, their behavior under radiation remains incompletely understood,. The ferroelectric properties of HfO 2 -ZrO 2 nanolaminate films with varying single-layer thicknesses under electron irradiation were systematically investigated in this work. Compared to uniformly doped HZO films, nanolaminates with architectures of (15/15) 5 and (37/37) 2 initially exhibit modestly reduced ferroelectric performance metrics. Under electron irradiation at a fluence rate of 5×10 12 e/cm 2 ·s, uniformly doped HZO films demonstrate continuous degradation across all accumulated fluences tested. In striking contrast, nanolaminate structures reveal a distinct trend: at a fluence of 1×10 14 e/cm 2 , key electrical characteristics (2Pr or DE max ) actually exhibit improvement over their pre-irradiation values,. Combined electrical and structural analyses reveal that this non-monotonic behavior arises from a competition interplay between ferroelectric phase fraction evolution and domain-wall pinning dynamics, both of which undergo transformation with increasing irradiation fluence. The relative dominance of these competing mechanisms is primarily governed by the superlattice architecture, specifically the individual layer thickness and interface density. These findings provide critical design principles: through judicious engineering of layer thickness and total film architecture, HfO 2 -ZrO 2 nanolaminate ferroelectric can be optimized for radiation-resistant applications. This architectural approach offers a pathway to enhanced radiation tolerance, though ultimate performance limits persist at higher fluence regimes. • The irradiation response of HfO₂–ZrO₂ ferroelectric nanolaminates is strongly dependent on individual layer thickness and interface density. • Nanolaminate structures exhibit a non-monotonic evolution of polarization and dielectric response under electron irradiation, in contrast to uniformly doped HZO films. • Remanent polarization is governed by the competition between ferroelectric phase fraction and domain-wall pinning, whose relative importance is structure dependent. • Superlattice engineering provides an effective pathway to extend the irradiation tolerance window of hafnia-based ferroelectrics.