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Antiferroelectric and ferroelectric materials are prominent non-linear dielectric materials with significant applications across various fields. To fully understand their electrical properties, it is crucial to accurately discriminate the two phases, especially in compositions with the coexistence of antiferroelectric and ferroelectric phases. In this study, we propose an easy method for differentiating domain structures from phase coexistence based on split outskirt reflections. The proposed method addresses existing limitations in the spatial phase distribution and lays the groundwork for understanding their structure–property relationships. [ABSTRACT FROM AUTHOR]

PbZrO3 has been broadly considered as a prototypical antiferroelectric material for high-power energy storage. A recent theoretical study suggests that the ground state of PbZrO3 is threefold-modulated ferrielectric, which challenges the generally accepted antiferroelectric configuration. However, such a novel ferrielectric phase was predicted only to be accessible at low temperatures. Here, we successfully achieve the room-temperature construction of the strongly competing ferrielectric and antiferroelectric state by strain-mediated phase separation in PbZrO3/SrTiO3 thin film. We demonstrate that the phase separation occurs spontaneously in quasi-periodic stripe-like patterns under a compressive misfit strain and can be tailored by varying the film thickness. The ferrielectric phase strikingly exhibitsa threefold modulation period with a nearly up-up-down configuration, which could be stabilized and manipulated by the formation and evolution of interfacial defects under applied strain. The present results construct a fertile ground for further exploring the physical properties and applications based on the novel ferrielectric phase. There is a desire to know how the threefold ferrielectric coexists with the antiferroelectric phase. Here, the authors realize a threefold-modulated ferrielectric phase regulated by strain-mediated phase separation in PbZrO3 thin film. [ABSTRACT FROM AUTHOR]

Benefitting from the reversible phase transition between antiferroelectric and ferroelectric states, antiferroelectric materials have recently received widespread attentions for energy storage applications. Antiferroelectric configuration with specific antiparallel dipoles has been used to establish antiferroelectric theories and understand its characteristic behaviors. Here, we report that the so-called antiferroelectric (Pb,La)(Zr,Sn,Ti)O3 system is actually ferrielectric in nature. We demonstrate different ferrielectric configurations, which consists of ferroelectric ordering segments with either magnitude or angle modulation of dipoles. The ferrielectric configurations are mainly contributed from the coupling between A-cations and O-anions, and their displacement behavior is dependent largely on the chemical doping. Of particular significance is that the width and net polarization of ferroelectric ordering segments can be tailored by composition, which is linearly related to the key electrical characteristics, including switching field, remanent polarization and dielectric constant. These findings provide opportunities for comprehending structure-property correlation, developing antiferroelectric/ferrielectric theories and designing novel ferroic materials. The large family PbZrO3-based solid solutions are usually considered as antiferroelectric materials with specific antiparallel polarization configuration. Here, the authors demonstrate the PbZrO3-based material has ferrielectric dipoles ordering and configure a clear structure-property relationship. [ABSTRACT FROM AUTHOR]

Abstract: Energy storage materials and their applications have long been areas of intense research interest for both the academic and industry communities. Dielectric capacitors using antiferroelectric materials are capable of displaying higher energy densities as well as higher power/charge release densities by comparison with their ferroelectric and linear dielectric counterparts and therefore have greater potential for practical energy storage applications. Over the past decade, extensive efforts have been devoted to the development of high performance, antiferroelectric, energy storage ceramics and much progress has been achieved. In this review, the current state‐of‐the‐art as regards antiferroelectric ceramic systems, including PbZrO3‐based, AgNbO3‐based, and (Bi,Na)TiO3‐based systems, are comprehensively summarized with regards to their energy storage performance. Strategies are then discussed for the further improvement of the energy storage properties of these antiferroelectric ceramic systems. This is followed by a review of the low temperature sintering techniques and the charge–discharge performance of antiferroelectric ceramics from a practical point of view. The review will be of benefit for researchers in the area as it offers a quick overview of recent progress in the development of various kinds of antiferroelectric ceramics and their properties. It should also stimulate the development of novel antiferroelectric ceramics with high energy storage performance. [ABSTRACT FROM AUTHOR]

The electrical hysteresis behaviors and energy storage performance of Pb0.97La0.02(Zr0.58Sn0.335Ti0.085)O3 antiferroelectric ( AFE) ceramics were studied under the combined effects of electric field and temperature. It was observed that the temperature dependence of recoverable energy density ( Wre) of AFE ceramics depends critically on the applied electric field. While Wre at lower electric fields (<8 kV/mm) shows increasing tendency with increasing temperature from 20°C to 100°C, Wre at higher electric fields (>8 kV/mm) demonstrates decreasing dependence. There exists an appropriate electric field (8 kV/mm) under which the AFE ceramics exhibit nearly temperature-independent Wre (the variation is less than 0.5% per 10°C). The underlying physical principles were also discussed in this study. These results indicate that the temperature dependence of Wre of AFE materials can be tuned through selecting appropriate electric fields and provide an avenue to obtain thermal stable energy storage capacitors, which should be of great interest to modern energy storage community. [ABSTRACT FROM AUTHOR]

Several 0.97PbZrO3–0.03Ba(Mg1/3Nb2/3)O3 (0.97PZ–0.03BMN) ceramics were prepared via the columbite precursor method. Their microstructures and pressure-dependent ferroelectric and depolarization performances were then studied. The X-ray diffraction patterns of ground and fresh samples indicate that a main rhombohedral symmetry crystal structure is present in the bulk and that it sits alongside a trace quantity of an orthorhombic antiferroelectric phase that results from the effect of grinding on the surface. The remanent polarization (Pr) of the 0.97PZ–0.03BMN reached 32.4 μC/cm2 at 4.5 kV/mm and ambient pressure. In an in situ pressure-induced current measurement, more than 91% of the retained Pr of the pre-poled sample was released when the pressure was increased from 194 MPa to 238 MPa. That this pressure-driven depolarization should be attributed to the pressure-induced ferroelectric–antiferroelectric phase transition is supported by the emergence of double P–E loops at high hydrostatic pressures. Moreover, the 0.97PZ-0.03BMN ceramics exhibit no temperature-induced phase transitions and little related polarization loss up to 125 °C, which suggests that Pr has excellent thermal stability. The sharp depolarization behavior at low pressures and excellent temperature stability reveal that our 0.97PZ–0.03BMN ceramics exhibit superior performances in mechanical–electrical energy conversion applications. [ABSTRACT FROM AUTHOR]

The effect of residual stress on energy storage property was investigated for a series of PbZrO3 thin films on SrTiO3 and Si substrates. Compressive or tensile residual stress influences the critical electric field EA for the ferroelectric-to-antiferroelectric phase transition, thus for films with (110)/(101) orientation, energy density W of films on SrTiO3 is 38% larger than films on Si; in contrast, (001)-oriented PbZrO3 films on SrTiO3 show slightly smaller W compared to films on Si. We conclude that the different responses of W to stress are related to the different constrain states in films with different orientations. [ABSTRACT FROM AUTHOR]

It is the behavior of electric-field induced antiferroelectric to ferroelectric (AFE-FE) phase transition that determines the specific application scenario of antiferroelectric materials. Here, we report that the evolution of the atomic displacement ordering from full-ordered to semi-ordered modulation should be responsible for the change in the behavior of the AFE-FE transition from sharp to diffuse. The novel semi-ordered configuration is originated from the competing interaction between long-range displacement modulation and compositional inhomogeneity, which just makes the AFE-FE transition diffuse but maintains the switching field. These results provide atomic-scale understanding for AFE-FE transition and new insights for designing hysteresis-free antiferroelectric materials. [Display omitted] [ABSTRACT FROM AUTHOR]

Recently, the (Pb,La)(Zr,Ti)O 3 antiferroelectric materials with slim-and-slanted double hysteresis loops have been widely drawn in the application of advanced pulsed power capacitors due to its low strain characteristic. In this work, the energy storage properties of (Pb 0.895 La 0.07)(Zr x Ti 1- x)O 3 ceramics with different Zr contents are researched thoroughly because the substitution of Ti4+ by Zr4+ can reduce the tolerance factor t , enhancing the antiferroelectricity. The polarization-electric field hysteresis loops of the PLZT ceramics become slimmer with increasing Zr content. The highest recoverable energy storage density (W re) of 3.38 J/cm3 and ultrahigh energy efficiency (η) of 86.5% are achieved in (Pb 0.895 La 0.07)(Zr 0.9 Ti 0.1)O 3 ceramic. The (Pb 0.895 La 0.07)(Zr 0.9 Ti 0.1)O 3 ceramic also hold fairly thermal stability (relative variation of W re is less than 28% over 30 °C-120 °C), excellent frequency stability (10–1000 Hz) and good fatigue endurance. These results demonstrate that the (Pb 0.895 La 0.07)(Zr 0.9 Ti 0.1)O 3 ceramic can be a desirable material for dielectric energy storage capacitors, especially for pulse power technology. [ABSTRACT FROM AUTHOR]

• a way of external pressure to enhance energy storage properties of AgNbO 3 ceramics. • An η of 56% and W rec of 1.3 J/cm3 has been achieved in AgNbO 3 ceramics under 400 MPa. • Hydrostatic pressure results in an enhancement in η and W rec by 47% and 23%, respectively. Despite its low energy storage efficiency (∼46%), silver niobate (AgNbO 3) is considered as a promising lead-free antiferroelectric material due to its environmental advantages. Herein, we demonstrate that the energy storage efficiency of AgNbO 3 ceramics can be enhanced by applying hydrostatic pressure. The results reveal that the hydrostatic pressure contributed to the decline of remanent polarization (P r) and the switching hysteresis Δ E. In addition, the externally applied pressure improved the reverse switching field (E A). This indicates an enhanced antiferroelectricity, benefiting the enhancement of energy storage properties of AgNbO 3 ceramics. Under the pressure of 400 MPa, the as-prepared AgNbO 3 ceramics exhibited an energy storage efficiency (η) of 56% and a recoverable energy storage density (W rec) of 1.3 J/cm3 under the electric field of 13 kV/mm, corresponding to an enhancement of 47% and 30%, respectively. [ABSTRACT FROM AUTHOR]

Abstract Bulk ceramics with high recoverable energy density (W re) and energy efficiency (η) play a critical role in the development of pulsed power systems for miniaturization and lightweight. The orthorhombic phase (Pb,La)(Zr,Ti)O 3 -based antiferroelectric (AFE) ceramics have been regarded as one of the most promising candidates for pulsed power system applications due to their relatively high energy storage density and efficiency. However, the main drawback of orthorhombic phase (Pb,La)(Zr,Ti)O 3 -based AFE ceramics is relatively low dielectric breakdown strengthen (DBS), which has always restricted the improvement of energy storage density. In this study, an effectively method to increase DBS by the introduction of Mn has been proposed. The relative density of orthorhombic phase (Pb 0.91 La 0.06)(Zr 0.96 Ti 0.04)O 3 (PLZT) ceramics was improved by Mn-doping. And the introduction of Mn can decrease the tolerance factor (t) of PLZT ceramics because the radius of Mn2+ is larger than that of B-site Zr4+/Ti4+, and thus enhancing antiferroelectricity. Meanwhile, the effects of Mn-doping on the phase structure, microstructure and dielectric properties of PLZT ceramics have been studied thoroughly in this study. It is found that the highest W re of 7.65 J/cm3 is obtained at 1.0 mol% Mn-doped PLZT ceramic, which is obviously larger than that of undoped PLZT ceramic (5.71 J/cm3). These results suggest that the Mn-doped PLZT ceramics are potential energy storage materials in pulsed power systems. Highlights • Enhanced the dielectric breakdown strengthen of pure antiferroelectric ceramics by Mn-doping. • Obtained a high recoverable energy density of 7.65 J/cm3 and relatively high η of 87% in Mn-doped antiferroelectric ceramics. • Better understanding of the mechanism on energy storage properties of Mn-doped antiferroelectric ceramics. [ABSTRACT FROM AUTHOR]

Antiferroelectric Pb 0.97 La 0.02 (Zr 0.33 Sn 0.55 Ti 0.12 )O 3 @SiO 2 (with 5% mole of SiO 2 ) particles were synthesized by a citric acid sol-gel method. Transmission electron microscopy(TEM) results illustrated the formation of core–shell nanostructures with controllable shell thicknesses about 3–5 nm. X-ray diffraction(XRD) patterns displayed that a stable perovskite phase was preserved and no other crystallization peaks were discovered from the shell component. Scanning electron microscopy(SEM) and Energy Dispersive Spectrometer(EDS) investigations confirmed that core-shell structures were inherited from particles to ceramics after sintering. As a result, through the coating process, the breakdown strength of the ceramic increases by 95% from 12.2 kV/mm to 23.8 kV/mm and the recoverable energy density was greatly enhanced from 1.76 J/cm 3 to 2.68 J/cm 3 . These results demonstrate a promising reaction method to enhance breakdown strength in antiferroelectrics for energy storage capacitor applications. [ABSTRACT FROM AUTHOR]

Lead-free antiferroelectric materials can be used in environmental-friendly energy applications and are receiving tremendous attention owing to their high energy-storage density, which is achieved through a phase transition between antiferroelectric and ferroelectric state. Here, by slowing down the antiferroelectric-ferroelectric transition via controllable beam irradiation in a transmission electron microscope, we demonstrate that such a transition in NaNbO 3 undergoes by means of forming a buffer-area (about 40–150 nm wide) at the on-going transition front. The spatial buffer-area approximately maintains its shape during moving and are characterized to be the antiferroelectric phase but exhibits a gradual variation of lattice spacing along the [010] proceeding direction of phase transition. With help of such buffer-area, the overall stress or barrier between the two phases could be considerably reduced compared to the direct change between the two structures. Therefore, our findings provide new insights for understanding the dynamical energy-storage process in antiferroelectric materials. [Display omitted] [ABSTRACT FROM AUTHOR]

The composition dependent dielectric, ferroelectric and energy storage properties of tetragonal lead lanthanum zirconate stannate titanate (PLZST) antiferroelectric ceramics were systematically studied in this paper. Two sets of simple linear scaling relations were established for the forward switching field E AFE-FE , the backward switching field E FE-AFE and recoverable energy density W re . As Zr content increases (Ti fixed), E AFE-FE , E FE-AFE , W re decreases linearly, while the stored energy density W st declines first and then increases. In addition, decreasing Ti content (Zr fixed) leads to linear increments in all of E AFE-FE , E FE-AFE , W re and W st . These results not only reveal the superiority of PLZST with lower Zr and lower Ti contents for energy storage capacitors, but also provide a fast way to design PLZST ceramics with specific energy storage properties. Our work may also be very helpful for better understanding the mechanism of phase transition behaviors of antiferroelectric materials. [ABSTRACT FROM AUTHOR]

In this study, we investigated the scaling behavior of dynamic hysteresis with frequency f and electric field E in epitaxial PbZrO 3 antiferroelectric film on (111)-oriented SrTiO 3 substrate. The scaling relation for the saturated hysteresis loops takes the form of hysteresis area ∝ f 0.03 ( E − 499) 0.20 at relatively low testing f . However, when frequency exceeds 30 Hz, the shows stronger dependence on f while remains basically unchanged relation with E , leading to a form of ∝ f 0.10 ( E − 499) 0.20 . The scaling behavior is modeled as occurring in a viscous medium where several forces, such as viscous and restoring forces, act on the phase transition process. [ABSTRACT FROM AUTHOR]

• E-field controlled magnetism in an AFE-based YIG/PLZST heterostructure shows potentials for creating device functionalities. • A large CME coefficient (11.6 × 10−8 s/m) is obtained at 0 Oe. • E-field tuning of susceptibility variation can reach 33% at a low magnetic field of 10 Oe. The magnetoelectric properties of a laminated heterostructure consisting of ferromagnetic yttrium iron garnet (YIG) film and antiferroelectric (Pb 0.97 La 0.02) (Zr 0.6 Sn 0.3 Ti 0.1)O 3 (PLZST) ceramic is, for the first time, reported in this work. The electric-field-controlled susceptibility, a shift of the coercive magnetic field and magnetization variations are demonstrated in YIG/PLZST multiferroic heterostructure. A large variation of the relative magnetic susceptibility is observed, practically 33% at a low magnetic field of 10 Oe. A sharp reduction of magnetization occurs at the antiferroelectric-ferroelectic phase transition field of PLZST ceramic. Thus the converse magnetoelectric coefficient peaks at the switching field and the maximum can reach 11.6 × 10−8 s/m without bias magnetic field. These features indicate that antiferroelectric materials can also be alternative candidates to combine with ferromagnetic materials for magnetoelectric tunable devices. [ABSTRACT FROM AUTHOR]

• Obtained the PLZST ceramics with "slanted" shape of P-E loops by modifying Sn content. • Obtained a high recoverable energy density of 1.42 J/cm3 and high η of 90% in PLZST30/60/10. • Better understanding of the mechanism on energy storage properties of PLZST ceramics. Both high energy density and high energy efficiency are indispensable as considering antiferroelectric materials for pulse power capacitor applications. However, the electrical hysteresis will inevitably limit the energy efficiency reported in previous literatures. In this work, lead lanthanum zirconate stannate titanate (PLZST) antiferroelectrics with both high energy density and high energy efficiency was presented. It is found that PLZST antiferroelectric ceramics with high Sn content not only exhibit enhanced antiferroelectricity, but also demonstrate higher energy efficiency. As Sn content increases, grain size decreases and the electric hysteresis values reduces. The high energy density of 1.28 J/cm3 and ultrahigh energy efficiency of 91% was obtained for PLZST30/60/10. The results will not only enrich our understanding of PLZST antiferroelectric materials but also offers new approach to developing high performance antiferroelectric for energy storage based applications. [ABSTRACT FROM AUTHOR]