Nanoscale Phase and Orientation Mapping in Multiphase Polycrystalline Hafnium Zirconium Oxide Thin Films Using 4D-STEM and Automated Diffraction Indexing.

Ferroelectric hafnium zirconium oxide (HZO) holds promise for nextgeneration memory and transistors due to its superior scalability and seamless integration with complementary metal-oxide-semiconductor processing. A major challenge in developing this emerging ferroelectric material is the metastable nature of the non-centrosymmetric polar phase responsible for ferroelectricity, resulting in a coexistence of both polar and non-polar phases with uneven grain sizes and random orientations. Due to the structural similarity between the multiple phases and the nanoscale dimensions of the thin film devices, accurate measurement of phase-specific information remains challenging. Here, the application of 4D scanning transmission electron microscopy is demonstrated with automated electron diffraction pattern indexing to analyze multiphase polycrystalline HZO thin films, enabling the characterization of crystallographic phase and orientation across large working areas on the order of hundreds of nanometers. This approach offers a powerful characterization framework to produce a quantitative and statistically robust analysis of the intricate structure of HZO films by uncovering phase composition, polarization axis alignment, and unique phase distribution within the HZO film. This study introduces a novel approach for analyzing ferroelectric HZO, facilitating reliable characterization of process-structure-property relationships imperative to accelerating the growth optimization, performance, and successful implementation of ferroelectric HZO in devices.