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HfO2-based ferroelectrics show tremendous potential for applications in computing technologies, but questions remain as to what dictates the stabilization of the desired phase. Here, it is demonstrated that the substrate the film is grown on is more influential than factors such as thickness, defect content, and strain. The presence of different possible polymorphs of Hf0.5Zr0.5O2 are observed to vary widely for different substrate materials—with La0.67Sr0.33MnO3, (LaAlO3)0.3(Sr2AlTaO6)0.7, and Al2O3 being (more) optimal for stabilizing the ferroelectric-orthorhombic phase. This substrate effect is found to be more influential than any changes observed from varying the film thickness (7.5–60 nm), deposition environment (oxygen vs argon), and annealing temperature (400–600 °C) in vacuum (10−5 Torr). X-ray diffraction and scanning transmission electron microscopy verify the phases present, and capacitor-based studies reveal ferroelectric behavior (or lack thereof) consistent with the phases observed. First-principles calculations suggest that forming oxygen vacancies in Hf0.5Zr0.5O2 lowers its work function, driving electrons away and helping to stabilize the ferroelectric phase. Substrates with a high work function (e.g., La0.67Sr0.33MnO3) facilitate this electron transfer but must also have sufficient ion conductivity to support oxygen-vacancy formation in Hf0.5Zr0.5O2. Together, these observations help clarify key factors essential to the stabilization of HfO2-based ferroelectrics. 

Abstract Over the last 30 years, the study of ferroelectric oxides has been revolutionized by the implementation of epitaxial‐thin‐film‐based studies, which have driven many advances in the understanding of ferroelectric physics and the realization of novel polar structures and functionalities. New questions have motivated the development of advanced synthesis, characterization, and simulations of epitaxial thin films and, in turn, have provided new insights and applications across the micro‐, meso‐, and macroscopic length scales. This review traces the evolution of ferroelectric thin‐film research through the early days developing understanding of the roles of size and strain on ferroelectrics to the present day, where such understanding is used to create complex hierarchical domain structures, novel polar topologies, and controlled chemical and defect profiles. The extension of epitaxial techniques, coupled with advances in high‐throughput simulations, now stands to accelerate the discovery and study of new ferroelectric materials. Coming hand‐in‐hand with these new materials is new understanding and control of ferroelectric functionalities. Today, researchers are actively working to apply these lessons in a number of applications, including novel memory and logic architectures, as well as a host of energy conversion devices. 

Abstract Thermoelectric generators are an environmentally friendly and reliable solid‐state energy conversion technology. Flexible and low‐cost thermoelectric generators are especially suited to power flexible electronics and sensors using body heat or other ambient heat sources. Bismuth telluride (Bi₂Te₃) based thermoelectric materials exhibit their best performance near room temperature making them an ideal candidate to power wearable electronics and sensors using body heat. In this report, Bi₂Te₃thin films are deposited on a flexible polyimide substrate using low‐cost and scalable manufacturing methods. The synthesized Bi₂Te₃nanocrystals have a thickness of 35 ± 15 nm and a lateral dimension of 692 ± 186 nm. Thin films fabricated from these nanocrystals exhibit a peak power factor of 0.35 mW m⁻¹·K⁻²at 433 K, which is among the highest reported values for flexible thermoelectric films. In order to evaluate the flexibility of the thin films, static and dynamic bending tests are performed while monitoring the change in electrical resistivity. After 1000 bending cycles over a 50 mm radius of curvature, the change in electrical resistance of the film is 23%. Using Bi₂Te₃solutions, the ability to print thermoelectric thin films with an aerosol jet printer is demonstrated, highlighting the potential of additive manufacturing techniques for fabricating flexible thermoelectric generators.