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Abstract The dielectric gap between the scanning probe microscopy (SPM) tip and the surface of a ferroelectric using conductive atomic force microscopy and piezoresponse force microscopy (PFM) is investigated. While the gap functions as a dielectric layer, it also allows tunneling current to inject charges into the ferroelectric when a critical loading force between 10–20 µN is applied to a tip with a radius of 25 nm under a bias voltage of 0.5 V. It is observed that the permittivity of the dielectric gap determines the coercive voltage measured by the piezoresponse hysteresis loop. While such studies done in air often produce coercive voltages much larger than those studied for the same materials in capacitor‐based studies, the use of high permittivity media such as water (ɛ_r= 79) or silicone oil (ɛ_r= 2.1‐2.8) produces coercive fields that more closely match those measured in conventional capacitor‐based polarization hysteresis loop measurements. Furthermore, using water as a dielectric medium in PFM imaging enhances the accuracy in extracting the amplitude and phase data from periodically poled lithium niobate crystals. These findings provide insight into the nanoscale phenomena of polarization switching instigated by the SPM tip and provide a pathway to improved quantitative studies. 

Abstract The development of next‐generation in‐memory and neuromorphic computing can be realized with memory transistors based on 2D ferroelectric semiconductors. Among these, In₂Se₃is the interesting since it possesses ferroelectricity in 2D quintuple layers. Synthesis of large amounts of In₂Se₃crystals with the desired phase, however, has not been previously achieved. Here, the gram‐scale synthesis of α‐In₂Se₃crystals using a flash‐within‐flash Joule heating method is demonstrated. This approach allows the synthesis of single‐phase α‐In₂Se₃crystals regardless of the conductance of precursors in the inner tube and enables the synthesis of gram‐scale quantities of α‐In₂Se₃crystals. Then, α‐In₂Se₃flakes are fabricated and used as a 2D ferroelectric semiconductor FET artificial synaptic device platform. By modulating the degree of polarization in α‐In₂Se₃flakes according to the gate electrical pulses, these devices exhibit distinct essential synaptic behaviors. Their synaptic performance shows excellent and robust reliability under repeated electrical pulses. Finally, it is demonstrated that the synaptic devices achieve an estimated learning accuracy of up to ≈87% for Modified National Institute of Standards and Technology patterns in a single‐layer neural network system. 

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. 

Voltage-tunable capacitors (varactors) are key components in microwave circuits. Tunable dielectric varactors can outperform competing technologies but typically suffer from high dielectric loss. Ruddlesden–Popper dielectric thin films can, by contrast, offer low microwave loss. Unfortunately, their crystallographic symmetry is usually not compatible with an out-of-plane parallel-plate varactor design, which can minimize size and maximize the electric field in the tunable dielectric compared with an in-plane device design. Here we show that a low-loss and tunable Ruddlesden–Popper dielectric thin film that is compatible with the parallel-plate varactor design can be created by breaking this crystallographic symmetry. We study films that are similar to the widely studied tunable microwave dielectric Ba0.45Sr0.55TiO3 but have a Ba0.45Sr0.55O rock-salt layer for every n-perovskite unit cells. The film with n = 8 exhibit an optimum combination of tunability and loss, with a material quality factor of around 200 and a relative tunability of 51% at an applied electric field of 250 kV cm−1, which results in a dielectric tuning figure of merit of 100 at 10 GHz. 

Abstract The pursuit of smaller, energy‐efficient devices drives the exploration of electromechanically active thin films (<1 µm) to enable micro‐ and nano‐electromechanical systems. While the electromechanical response of such films is limited by substrate‐induced mechanical clamping, large electromechanical responses in antiferroelectric and multilayer thin‐film heterostructures have garnered interest. Here, multilayer thin‐film heterostructures based on antiferroelectric PbHfO₃and ferroelectric PbHf_1‐xTi_xO₃overcome substrate clamping to produce electromechanical strains >4.5%. By varying the chemistry of the PbHf_1‐xTi_xO₃layer (x = 0.3‐0.6) it is possible to alter the threshold field for the antiferroelectric‐to‐ferroelectric phase transition, reducing the field required to induce the onset of large electromechanical response. Furthermore, varying the interface density (from 0.008 to 3.1 nm⁻¹) enhances the electrical‐breakdown field by >450%. Attaining the electromechanical strains does not necessitate creating a new material with unprecedented piezoelectric coefficients, but developing heterostructures capable of withstanding large fields, thus addressing traditional limitations of thin‐film piezoelectrics. 

Abstract Highly responsive, voltage‐tunable dielectrics are essential for microwave‐telecommunication electronics. Ferroelectric/relaxor materials have been leading candidates for such functionality and have exhibited agile dielectric responses. Here, it is demonstrated that relaxor materials developed from antiferroelectrics can achieve both ultrahigh dielectric response and tunability. The system, based on alloying the archetypal antiferroelectric PbZrO₃with the dielectric BaZrO₃, exhibits a more complex phase evolution than that in traditional relaxors and is characterized by an unconventional multi‐phase competition between antiferroelectric, ferroelectric, and paraelectric order. This interplay of phases can greatly enhance the local heterogeneities and results in relaxor characteristics while preserving considerable polarizability. Upon studying Pb_1‐xBa_xZrO₃forx= 0‐0.45, Pb_0.65Ba_0.35ZrO₃is found to provide for exceptional dielectric tunability under low bias fields (≈81% at 200 kV cm⁻¹and ≈91% at 500 kV cm⁻¹) at 10 kHz, outcompeting most traditional relaxor ferroelectric films. This high tunability is sustained in the radio‐frequency range, resulting in a high commutation quality factor (>2000 at 1 GHz). This work highlights the phase evolution from antiferroelectrics (with lower, “positive” dielectric tunability) to relaxors (with higher, “negative” tunability), underscoring a promising approach to develop relaxors with enhanced functional capabilities and new possibilities.