Role of 3Y-TZP grain boundaries in glazing and layering.

OBJECTIVES: Monolithic 3 mol% Yttria-stabilized tetragonal zirconia polycrystal or 3Y-TZP exhibits transformation toughening phenomena which is suitable for dental restorations with minimizing the risk of fracture and to decrease reduction of natural tooth. However, the staining/glazing or layering is required to achieve of a match with the optical properties of natural dentition. The hypothesis under examination is that the physical, chemical, and structural aspects of the 3Y-TZP grain boundaries after the staining/glazing or layering. METHODS: The three sintering temperatures of 1400 °C, 1500 °C, and 1600 °C were considered followed by vacuum annealed at 750 °C for 1 min; and air post-annealed at 750 °C for 1 min RESULTS: The initial sintering step in the fabrication of zirconia restorations plays a critical role in the outcomes of the subsequent stages of glazing and layering. SIGNIFICANCE: The current study revealed for first time the advantage of vacuum annealing by the presence of ferroelastic domain switching toughening mechanism.

Promotion of Probabilistic Bit Generation in Mott Devices by Embedded Metal Nanoparticles.

Considerable attention has been drawn to the use of volatile two-terminal devices relying on the Mott transition for the stochastic generation of probabilistic bits (p-bits) in emerging probabilistic computing. To improve randomness and endurance of bit streams provided by these devices, delicate control of the transient evolution of switchable domains is required to enhance stochastic p-bit generation. Herein, it is demonstrated that the randomness of p-bit streams generated via the consecutive pulse inputs of pump-probe protocols can be increased by the deliberate incorporation of metal nanoparticles (NPs), which influence the transient dynamics of the nanoscale metallic phase in VO2 Mott switches. Among the vertically stacked Pt-NP-containing VO2 threshold switches, those with higher Pt NP density show a considerably wider range of p-bit operation (e.g., up to ≈300% increase in ΔVprobe upon going from (Pt NP/VO2)0 to (Pt NP/VO2)11) and can therefore be operated under the conditions of high speed (400 kbit s-1), low power consumption (14 nJ per bit), and high stability (>105 200 bits) for p-bit generation. Thus, the study presents a novel strategy that exploits nanoscale phase control to maximize the generation of nondeterministic information sources for energy-efficient probabilistic computing hardware.

Achieving High Piezoelectric Performance across a Wide Composition Range in Tetragonal (Bi,Na)TiO3-BaTiO3 Films for Micro-electromechanical Systems.

Tetragonal (1-x)(Bi,Na)TiO3-xBaTiO3 films exhibit enhanced piezoelectric properties due to domain switching over a wide composition range. These properties were observed over a significantly wider composition range than the morphotropic phase boundary (MPB), which typically has a limited composition range of 1-2%. The polarization axis was found to be along the in-plane direction for the tetragonal composition range x = 0.06-1.0, attributed to the tensile thermal strain from the substrate during cooling after the film formation. A "two-step increase" in remanent polarization against an applied maximum electric field was observed at the high-field region due to the domain switching, and a very high piezoelectric response (effective d33 value, denoted as d33,f) over 220 pm/V was achieved for a wide composition range of x = 0.2-0.5 with high tetragonality, exceeding previously reported values for bulk ceramics. Moreover, a transverse piezoelectric coefficient, e31,f, of 19 C/m2 measured using a cantilever structure was obtained for a composition range of at least 10 atom % (for both x = 0.2 and 0.3). This value is the highest reported for Pb-free piezoelectric thin films and is comparable to the best data for Pb-based thin films. Reversible domain switching eliminates the need for conventional MPB compositions, allowing an improvement in the piezoelectric properties over a wider composition range. This strategy could provide a guideline for the development of environmentally acceptable lead-free piezoelectric films with composition-insensitive piezoelectric performance to replace Pb-based materials with MPB composition, such as PZT.

Lead-Free Textured Ceramics with Ultrahigh Piezoelectric Properties by Synergistic Design.

Lead-free ceramics with superior piezoelectric performance are highly desirable in various electromechanical applications. Unfortunately, it is still challenging to achieve significantly enhanced piezoelectricity without sacrificing the Curie temperature (Tc) in current BaTiO3-based ceramics. To address this issue, a synergistic design strategy of integrating crystallographic texture, multiphase coexistence, and doping engineering is proposed here. Highly [001]c-textured (Ba0.95Ca0.05)(Ti0.92Zr0.06Sn0.02)O3 ceramics are synthesized through Li-related liquid-phase-assisted templated grain growth, with improved grain orientation quality (f of ∼96% and r of ∼0.16) achieved at substantially reduced texture temperatures. Encouragingly, ultrahigh comprehensive piezoelectric properties, i.e., piezoelectric coefficient d33 of ∼820 pC N-1, electrostrain Smax/Emax of ∼2040 pm V-1, and figure of merit d33 × g33 of ∼23.5 × 10-12 m2 N-1, are simultaneously obtained without sacrificing Tc, which are also about 2.3, 2.4, and 4.3 times as high as those of non-textured counterpart, respectively. On the basis of the experiments and theoretical modeling, the outstanding piezoelectric performance is attributed to more effective exploration of property anisotropy and easier polarization rotation/extension, owing to improved grain orientation quality, dissolution of templates into oriented grains, coexisting R + O + T phases, and domain miniaturization. This work provides important guidelines for developing novel ceramics with outstanding piezoelectric properties and can largely expand application fields of textured BaTiO3-based ceramics into high-performance and multilayer electronic devices.

Domain Switching-Based Nonlinear Coupling Response for Giant Magnetostrictive Materials.

This paper proposes a multilevel three-dimensional constitutive model based on a microscopically phenomenological approach from the domain rotation mechanism, which is a fully coupled self-consistent homogenization scheme considering the interactions between elastic-inelastic strain and hysteresis. Considering the interactions among magnetic domains, grains, polycrystalline complexes, and macroscopic phenomenology, we predict the nonlinear magnetostrictive response of Terfenol-D under different types of external force loads and magnetic excitations in various thermal environments involving multi-fields of coupled magnetic, elastic, thermal, and mechanical phenomena. The average values of the mechanical bulk strains for different magnetization states are obtained at the grain scale utilizing Boltzmann functions and a self-consistent homogenization scheme. A Taylor series expansion of the Gibbs function concerning the field variables and an adapted Jiles-Atherton model are used to construct the hysteresis coupled constitutive relations at the macroscopic scale. The results associated with the experiments show that the established model can reasonably predict the magnetostrictive response under different external mixed stimuli. It can provide theoretical guidance for the precise control of nonlinear vibrations and the optimal design of the rotating giant magnetostrictive transducers at both microscopic and macroscopic multiple scales.

Ultralow Tip-Force Driven Sizable-Area Domain Manipulation through Transverse Flexoelectricity.

Deterministic control of ferroelectric domain is critical in the ferroelectric functional electronics. Ferroelectric polarization can be manipulated mechanically with a nano-tip through flexoelectricity. However, it usually occurs in a very localized area in ultrathin films, with possible permanent surface damage caused by a large tip-force. Here it is demonstrated that the deliberate engineering of transverse flexoelectricity offers a powerful tool for improving the mechanical domain switching. Sizable-area domain switching under an ultralow tip-force can be realized in suspended van der Waals ferroelectrics with the surface intact, due to the enhanced transverse flexoelectric field. The film thickness range for domain switching in suspended ferroelectrics is significantly improved by an order of magnitude to hundreds of nanometers, being far beyond the limited range of the substrate-supported ones. The experimental results and phase-field simulations further reveal the crucial role of the transverse flexoelectricity in the domain manipulation. This large-scale mechanical manipulation of ferroelectric domain provides opportunities for the flexoelectricity-based domain controls in emerging low-dimensional ferroelectrics and related devices.

Writing-Speed Dependent Thresholds of Ferroelectric Domain Switching in Monolayer α-In2 Se3.

An electrical-biased or mechanical-loaded scanning probe written on the ferroelectric surface can generate programmable domain nanopatterns for ultra-scaled and reconfigurable nanoscale electronics. Fabricating ferroelectric domain patterns by direct-writing as quickly as possible is highly desirable for high response rate devices. Using monolayer α-In2 Se3 ferroelectric with ≈1.2 nm thickness and intrinsic out-of-plane polarization as an example, a writing-speed dependent effect on ferroelectric domain switching is discovered. The results indicate that the threshold voltages and threshold forces for domain switching can be increased from -4.2 to -5 V and from 365 to 1216 nN, respectively, as the writing-speed increases from 2.2 to 10.6 µm s-1 . The writing-speed dependent threshold voltages can be attributed to the nucleations of reoriented ferroelectric domains, in which sufficient time is needed for subsequent domain growth. The writing-speed dependent threshold forces can be attributed to the flexoelectric effect. Furthermore, the electrical-mechanical coupling can be employed to decrease the threshold force, achieving as low as ≈189±41 nN, a value smaller than those of perovskite ferroelectric films. Such findings reveal a critical issue of ferroelectric domain pattern engineering that should be carefully addressed for programmable direct-writing electronics applications.

Facile Control of Ferroelastic Domain Patterns in Multiferroic Thin Films by a Scanning Tip Bias.

BiFeO3, known as the "holy grail of all multiferroics", provides an appealing platform for exploration of multifield coupling physics and design of functional devices. Many fantastic properties of BiFeO3 are regulated by its ferroelastic domain structure. However, a facile programable control on the ferroelastic domain structure in BiFeO3 remains challenging and our understanding on the existing control strategies is also far from complete. This work reports a facile control of ferroelastic domain patterns in BiFeO3 thin films under area scanning poling by exploiting the tip bias as the control parameter. Combining scanning probe microscopy experiments and simulations, we found that BiFeO3 thin films with pristine 71° rhombohedral-phase stripe domains exhibit at least four switching pathways solely by controlling the scanning tip bias. As a result, one can readily write mesoscopic topological defects into the films without the necessity to change the tip motion. The correlation between conductance of the scanned region and the switching pathway is further investigated. Our results extend the current understanding on the domain switching kinetics and the coupled electronic transport properties in BiFeO3 thin films. The facile voltage control of ferroelastic domains should facilitate the development of configurable electronic and spintronic devices.

Formation of Head/Tail-to-Body Charged Domain Walls by Mechanical Stress.

Domain walls (DWs) in ferroelectric materials are interfaces that separate domains with different polarizations. Charged domain walls (CDWs) and neutral domain walls are commonly classified depending on the charge state at the DWs. CDWs are particularly attractive as they are configurable elements, which can enhance field susceptibility and enable functionalities such as conductance control. However, it is difficult to achieve CDWs in practice. Here, we demonstrate that applying mechanical stress is a robust and reproducible approach to generate CDWs. By mechanical compression, CDWs with a head/tail-to-body configuration were introduced in ultrathin BaTiO3, which was revealed by in-situ transmission electron microscopy. Finite element analysis shows strong strain fluctuation in ultrathin BaTiO3 under compressive mechanical stress. Molecular dynamics simulations suggest that the strain fluctuation is a critical factor in forming CDWs. This study provides insight into ferroelectric DWs and opens a pathway to creating CDWs in ferroelectric materials.

Magnetic-Field-Assisted Electric-Field-Induced Domain Switching of a Magnetic Single Domain in a Multiferroic/Magnetoelectric Ni Nanochevron/[Pb(Mg1/3Nb2/3)O3]0.68-[PbTiO3]0.32 (PMN-PT) Layered Structure.

We report the magnetic-field-assisted electric-field-controlled domain switching of a magnetic single domain in a multiferroic/magnetoelectric Ni nanochevrons/[Pb(Mg1/3Nb2/3)O3]0.68-[PbTiO3]0.32 (PMN-PT) layered structure. Initially, a magnetic field was applied in the transverse direction across single-domain Ni nanochevrons to transform each of them into a two-domain state. Subsequently, an electric field was applied to the layered structure, exerting the converse magnetoelectric effect to transform/release the two-domain Ni nanochevrons into one of two possible single-domain states. Finally, the experimental results showed that approximately 50% of the single-domain Ni nanochevrons were switched permanently after applying our approach (i.e., the magnetization direction was permanently rotated by 180 degrees). These results mark important advancements for future nanoelectromagnetic systems.

Improved Subthreshold Characteristics by Back-Gate Coupling on Ferroelectric ETSOI FETs.

In this work, extremely thin silicon-on-insulator field effective transistors (ETSOI FETs) are fabricated with an ultra-thin 3 nm ferroelectric (FE) hafnium zirconium oxides (Hf0.5Zr0.5O2) layer. Furthermore, the subthreshold characteristics of the devices with double gate modulation are investigated extensively. Contributing to the advantages of the back-gate voltage coupling effects, the minimum subthreshold swing (SS) value of a 40 nm ETSOI device could be adjusted from the initial 80.8-50 mV/dec, which shows ultra-steep SS characteristics. To illustrate this electrical character, a simple analytical model based on the transient Miller model is demonstrated. This work shows the feasibility of FE ETSOI FET for ultra-low-power applications with dynamic threshold adjustment.

The First Chiro-Inositol Organosilicon Ferroelectric Crystal.

Organosilicons have been used extensively in aerospace, electronics, food, medicine and other fields, due to their low viscosity, hydrophobicity, corrosion resistance, non-toxic, and physiologically inert features. Despite extensive interest, however, organosilicon ferroelectric crystals have never been found. Here, by using the chemical design strategy, we successfully obtained a molecular ferroelectric D-chiro-inositol-SiMe3 with polar P43 symmetry, whose spontaneous polarization can be electrically switchable on thin film. The introduction of organosilicon groups endows the thin films with excellent softness, ductility and flexibility (extremely low hardness of 72.8 MPa and small elastic modulus of 5.04 GPa) that are desirable for biomedical and human-compatible applications. As the first case of organosilicon ferroelectric crystal to date, this work offers a new structural paradigm for molecular ferroelectrics, and highlights their potential for flexible bio-electronic applications.

Fast Operations of Nonvolatile Ferroelectric Domain Wall Memory with Inhibited Space Charge Injection.

The microampere-level domain wall currents in LiNbO3 single crystals have promising applications in nonvolatile ferroelectric domain wall random access memory and logic with high-density integration, ultrafast operation speeds, and almost unlimited switching cycles. For the memory commercialization, the improvements of the reliability and operation speed of the devices are challenging due to the high-field charge injection. The injected charge could compensate the domain-wall boundary charge that screens the domain switching field and reduces the domain wall current. In this work, two kinds of memory nanocells were fabricated on the surfaces of X-cut LiNbO3 single crystals to study the geometry-dependent charge injection. The striped memory cell due to the appearance of the size-driven reconstruction has a smaller coercive field than that of a clamped memory cell without relaxation of the lattice matching stress, which reduces low-frequency charge injection and increases the domain switching speed. At an operating voltage of 5 V, we observed a retention time of more than 1 week and an on/off current ratio of 2 × 104 for a striped-like cell, paving the route to integrate energy-efficient high-density domain wall memory in high reliability.

Dynamics of Anisotropic Oxygen-Ion Migration in Strained Cobaltites.

Orientation control of the oxygen vacancy channel (OVC) is highly desirable for tailoring oxygen diffusion as it serves as a fast transport channel in ion conductors, which is widely exploited in solid-state fuel cells, catalysts, and ion-batteries. Direct observation of oxygen-ion hopping toward preferential vacant sites is a key to clarifying migration pathways. Here we report anisotropic oxygen-ion migration mediated by strain in ultrathin cobaltites via in situ thermal activation in atomic-resolved transmission electron microscopy. Oxygen migration pathways are constructed on the basis of the atomic structure during the OVC switching, which is manifested as the vertical-to-horizontal OVC switching under tensile strain but the horizontal-to-diagonal switching under compression. We evaluate the topotactic structural changes to the OVC, determine the crucial role of the tolerance factor for OVC stability, and establish the strain-dependent phase diagram. Our work provides a practical guide for engineering OVC orientation that is applicable to ionic-oxide electronics.

Large Piezoelectric Response in Lead-Free (Bi0.5Na0.5)TiO3-Based Perovskite Thin Films by Ferroelastic Domain Switching: Beyond the Morphotropic Phase Boundary Paradigm.

Strong electromechanical coupling is observed in tetragonal Pb-free 0.7(Bi0.5Na0.5)TiO3-0.3BaTiO3 films, which is far from the morphotropic phase boundary, prepared by pulsed laser deposition on a Si substrate. The tensile strain induced during cooling causes in-plane polarization in an oriented film on a Si substrate, while an epitaxial film grown on a SrTiO3 substrate exhibits out-of-plane polarization. S-E curve analysis reveals that the obtained piezoelectric coefficient for the film on the Si substrate (d33,f ≈ 275 pm/V) is approximately eight times higher than that for the epitaxial film on the SrTiO3 substrate (d33,f ≈ 34 pm/V). In situ X-ray diffraction analysis confirms the occurrence of domain switching under an electric field from in-plane to out-of-plane polarization. An effective piezoelectric stress coefficient, e31,eff, of ∼19 C/m2 is obtained from a Si cantilever sample, which is the highest among the reported values for Pb-free piezoelectric films and is comparable to those for Pb-based films. The significant piezoelectric response produced by domain switching in the Pb-free materials with the composition far from the morphotropic phase boundary will expand future applications due to their both outstanding properties and environmental sustainability.

Rippling Ferroic Phase Transition and Domain Switching In 2D Materials.

Ripples are a class of native structural defects widely existing in 2D materials. They originate from the out-of-plane flexibility of 2D materials introducing spatially evolving electronic structure and friction behavior. However, the effect of ripples on 2D ferroics has not been reported. Here a molecular dynamics study of the effect of ripples on the temperature-induced ferroic phase transition and stress-induced ferroic domain switching in ferroelastic-ferroelectric monolayer GeSe is presented. Ripples stabilize the short-range ferroic orders in the high-temperature phase with stronger ferroicity and longer lifetime, thereby increasing the transition temperature upon cooling. In addition, ripples significantly affect the domain switching upon loading, changing it from a highly correlated process into a ripple-driven localized one where ripples act as source of dynamical random stress. These results reveal the fundamental role of ripples on 2D ferroicity and provide theoretical guidance for ripple engineering of controlled phase transition and domain switching with potential applications in flexible 2D electronics.

Lead-Free BiFeO3-BaTiO3 Ceramics with High Curie Temperature: Fine Compositional Tuning across the Phase Boundary for High Piezoelectric Charge and Strain Coefficients.

BiFeO3-BaTiO3 is a promising high-temperature piezoelectric ceramic that possesses both good electromechanical properties and a Curie temperature (TC). Here, the piezoelectric charge constants (d33) and strain coefficients (d*33) of (1 - x)BiFeO3-xBaTiO3 (BF-xBT; 0.20 ≤ x ≤ 0.50) lead-free piezoelectrics were investigated at room temperature. The results showed a maximum d33 of 225 pC/N in the BF-0.30BT ceramic and a maximum d*33 of 405 pm/V in the BF-0.35BT ceramic, with TCs of 503 and 415 °C, respectively. To better understand the performance enhancement mechanisms, a phase diagram was established using the results of XRD, piezoresponse force microscopy, TEM, and electrical property measurements. The superb d33 of the BF-0.30BT ceramic arose because of its location in the optimum point in the morphotropic phase boundary, low oxygen vacancy (VO··) concentration, and domain heterogeneity. The superior d*33 of the BF-0.35BT ceramic was attributed to a weak relaxor behavior between coexisting macrodomains and polar nanoregions. The presented strategy provides guidelines for designing high-temperature BF-BT ceramics for different applications.

Energy-Efficient Ferroelectric Domain Wall Memory with Controlled Domain Switching Dynamics.

High readout domain-wall currents in LiNbO3 single-crystal nanodevices are attractive because of their application in a ferroelectric domain wall random access memory (DWRAM) to drive a fast memory circuit. However, the wall current at a small read voltage would increase nonlinearly at a much higher write voltage, which could cause high energy consumption. Here, we resolved this problem by controlling the two-step domain forward growth within a ferroelectric mesa-like cell that was formed at the surface of an X-cut LiNbO3 single crystal. The mesa-like cell contacts two side Pt/Ni electrodes that extend over the cell surface by 90 nm for the generation of an in-plane inhomogeneous electric field. The domain forward growth processes at first in the formation of an inclined charged 180° domain to span the in-plane electrode gap under a write voltage of 5 V in a large readout wall current, and then, the domain expands fully throughout the entire cell in the formation of a neutral 180° wall to reduce the wall current by 10 times at a higher write voltage of 6 V. Meantime, the domain below the mesa-like cell in an opposite orientation is unchanged to serve as the reference. A higher wall current at a lower read voltage and a lower wall current at a higher write voltage can satisfy both requirements of low energy consumption and fast operation speeds for the DWRAM.

Beyond Substrates: Strain Engineering of Ferroelectric Membranes.

Strain engineering in perovskite oxides provides for dramatic control over material structure, phase, and properties, but is restricted by the discrete strain states produced by available high-quality substrates. Here, using the ferroelectric BaTiO3 , production of precisely strain-engineered, substrate-released nanoscale membranes is demonstrated via an epitaxial lift-off process that allows the high crystalline quality of films grown on substrates to be replicated. In turn, fine structural tuning is achieved using interlayer stress in symmetric trilayer oxide-metal/ferroelectric/oxide-metal structures fabricated from the released membranes. In devices integrated on silicon, the interlayer stress provides deterministic control of ordering temperature (from 75 to 425 °C) and releasing the substrate clamping is shown to dramatically impact ferroelectric switching and domain dynamics (including reducing coercive fields to <10 kV cm-1 and improving switching times to <5 ns for a 20 µm diameter capacitor in a 100-nm-thick film). In devices integrated on flexible polymers, enhanced room-temperature dielectric permittivity with large mechanical tunability (a 90% change upon ±0.1% strain application) is demonstrated. This approach paves the way toward the fabrication of ultrafast CMOS-compatible ferroelectric memories and ultrasensitive flexible nanosensor devices, and it may also be leveraged for the stabilization of novel phases and functionalities not achievable via direct epitaxial growth.

Reproducible Ultrathin Ferroelectric Domain Switching for High-Performance Neuromorphic Computing.

Neuromorphic computing consisting of artificial synapses and neural network algorithms provides a promising approach for overcoming the inherent limitations of current computing architecture. Developments in electronic devices that can accurately mimic the synaptic plasticity of biological synapses, have promoted the research boom of neuromorphic computing. It is reported that robust ferroelectric tunnel junctions can be employed to design high-performance electronic synapses. These devices show an excellent memristor function with many reproducible states (≈200) through gradual ferroelectric domain switching. Both short- and long-term plasticity can be emulated by finely tuning the applied pulse parameters in the electronic synapse. The analog conductance switching exhibits high linearity and symmetry with small switching variations. A simulated artificial neural network with supervised learning built from these synaptic devices exhibited high classification accuracy (96.4%) for the Mixed National Institute of Standards and Technology (MNIST) handwritten recognition data set.