Stabilizing the Ferroelectric Phase of Hf0.5Zr0.5O2 Thin Films by Charge Transfer

Ferroelectric hafnia-based thin films have attracted significant interest due to their compatibility with complementary metal-oxide-semiconductor technology (CMOS). Achieving and stabilizing the metastable ferroelectric phase in these films is crucial for their application in ferroelectric devices. Recent research efforts have concentrated on the stabilization of the ferroelectric phase in hafnia-based films and delving into the mechanisms responsible for this stability. In this study, we experimentally demonstrate that stabilization of the ferroelectric phase in Hf_{0.5}Zr_{0.5}O_{2} (HZO) can be controlled by the interfacial charge transfer and the associated hole doping of HZO. Using the meticulously engineered charge transfer between an La_{1-x}Sr_{x}MnO_{3} buffer layer with variable Sr concentration x and an HZO film, we find the optimal x=0.33 that provides the required hole doping of HZO to most efficiently stabilize its ferroelectric phase. Our theoretical modeling reveals that the competition of the hole distribution between the threefold and fourfold coordinated oxygen sites in HZO controls the enhancement or reduction of the ferroelectric phase. Our findings offer a novel strategy to stabilize the ferroelectric phase of hafnia-based films and provide new insights into the development of ferroelectric devices compatible with CMOS.