Antiferroelectric Research Articles

Neural morphology perception system based on antiferroelectric AgNbO3 neurons

AbstractBiologically inspired neuromorphic perceptual systems have great potential for efficient processing of multisensory signals from the physical world. Recently, artificial neurons constructed by memristor have been developed with good biological plausibility and density, but the filament‐type memristor is limited by undesirable temporal and spatial variations, high electroforming voltage and limited reproducibility and the Mott insulator type memristor suffer from large driving current. Here, we propose a novel antiferroelectric artificial neuron (AFEAN) based on the intrinsic polarization and depolarization of AgNbO3 (ANO) antiferroelectric (AFE) films to address these challenges. The antiferroelectric memristor exhibits low power consumption (8.99 nW), excellent durability (~105) and high stability. Using such an AFEAN, a spike‐based antiferroelectric neuromorphic perception system (AFENPS) has been designed, which can encode light level and temperature signals into spikes, and further construct a spiking neural network (SNN) (784 × 196 × 10) for optical image classification and thermal imaging classification, achieving 95.34% and 95.76% recognition accuracy on the MNIST dataset, respectively. This work paves the way for the simulation of spiking neurons using antiferroelectric materials and promising a promising method for the development of highly efficient hardware for neuromorphic perception systems.image

Visible-Photo-Assisted Phase Switching of Antiferroelectric-to-Ferroelectric Orders in an I3 --Intercalated 2D Perovskite.

Antiferroelectric (AFE) has emerged as a promising branch of electroactive materials, due to intriguing physical attributes stemming from the electric field-induced antipolar-to-polar phase transformation. However, the requirement of extremely high electric field strength to switch adjacent sublattice polarization poses great challenges for exploiting new molecular AFE system. Although photoirradiation is striking as a noncontact and nondestructive manipulation tool to optimize physical properties, optical control of antiferroelectricity still remains unexplored. Here, by adopting light-sensitive I3 - anion into 2D perovskite family, we design a new I3 --intercalated molecular AFE of (t-ACH)2EA2Pb3I10(I3)0.5 ⋅ ((H3O)(H2O))0.5 (1, t-ACH=trans-4-aminomethyl-1-cyclohexanecarboxylate, EA=ethylammonium). The I3 --intercalating gives an ultra-narrow band gap of 1.65 eV with strong absorption. In term of AFE structure, the anti-parallel alignment of electric dipoles results in a large spontaneous polarization of 4.3 μC/cm2. Strikingly, 1 merely shows AFE behaviour in the dark even under ultrahigh voltage, while the field-induced ferroelectric state can be facilely obtained upon visible illumination. Such unprecedented visible-photo-assisted phase switching ascribes to the incorporation of photoactive I3 - anions that reduces AFE-to-ferroelectric switching barrier. This pioneering work on the photo-assisting transformation of ferroic orders paves a way to develop future photoactive materials with potential applications.

Superior energy storage properties of BiFeO3 doped NaNbO3 antiferroelectric ceramics

NaNbO3 (NN)-based dielectric ceramics for energy storage have garnered significant interest due to their high saturation polarization, low residual polarization, and superior breakdown strength (Eb). However, the low recoverable energy storage density (Wrec) and efficiency (η) significantly limited their practical application. Herein, BiFeO3 (BF) was incorporated into NN to optimize the energy storage performance. The NN-BF ceramics exhibited pronounced antiferroelectric (AFE) relaxor phase, alongside grain size reduction and Eb enhancement, which contributed to a significant increase of Wrec and η. Specially, the optimum Wrec of 4.43 J/cm³ and η of 71.51 % were achieved at the composition of 0.9NN-0.1BF. Besides, stable energy storage performance was maintained over a wide temperature range (20–120 °C). These results highlight the potential of NN-BF relaxor AFE ceramics as promising candidates for high-performance energy storage applications.

Novel Two-Terminal Synapse/Neuron Based on an Antiferroelectric Hafnium Zirconium Oxide Device for Neuromorphic Computing.

Functionally diverse devices with artificial neuron and synapse properties are critical for neuromorphic systems. We present a two-terminal artificial leaky-integrate-fire (LIF) neuron based on 6 nm Hf0.1Zr0.9O2 (HZO) antiferroelectric (AFE) thin films and develop a synaptic device through work function (WF) engineering. LIF neuron characteristics, including integration, firing, and leakage, are achieved in W/HZO/W devices due to the accumulated polarization and spontaneous depolarization of AFE HZO films. By engineering the top electrode with asymmetric WFs, we found that Au/Ti/HZO/W devices exhibit synaptic weight plasticity, such as paired-pulse facilitation and long-term potentiation/depression, achieving >90% accuracy in digit recognition within constructed artificial neural network systems. These findings suggest that AFE HZO capacitor-based neurons and WF-engineered artificial synapses hold promise for constructing efficient spiking neuron networks and artificial neural networks, thereby advancing neuromorphic computing applications based on emerging AFE HZO devices.

Ultrahigh Energy Storage in (Ag,Sm)(Nb,Ta)O3 Ceramics with a Stable Antiferroelectric Phase, Low Domain-Switching Barriers, and a High Breakdown Strength.

AgNbO3 (AN) antiferroelectrics (AFEs) are regarded as a promising candidate for high-property dielectric capacitors on account of their high maximum polarization, double polarization-electric field (P-E) loop characteristics, and environmental friendliness. However, high remnant polarization (Pr) and large polarization hysteresis loss from room-temperature ferrielectric behavior of AN and low breakdown strength (Eb) cause small recoverable energy density (Wrec) and efficiency (η). To solve these issues, herein, we have designed Sm3+ and Ta5+ co-doped AgNbO3. The addition of Sm3+ and Ta5+ reduces the tolerance factor, polarizability of B-site cations, and domain-switching barriers, enhancing AFE phase stability and decreasing hysteresis loss. Meanwhile, adding Sm3+ and Ta5+ leads to decreased grain sizes, increased band gap, and reduced leakage current, all contributing to increased Eb. As a benefit from the above synergistic effects, a high Wrec of 7.24 J/cm3, η of 72.55%, power density of 173.73 MW/cm3, and quick discharge rate of 18.4 ns, surpassing those of many lead-free ceramics, are obtained in the (Ag0.91Sm0.03)(Nb0.85Ta0.15)O3 ceramic. Finite element simulations for the breakdown path and transmission electron microscopy measurements of domains verify the rationality of the design strategy.

Component design for stabilizing P phase in NaNbO3-based ceramics and the energy storage performance

Antiferroelectric (AFE) ceramic dielectrics are widely recognized for their high potential in high-power pulse equipment applications. Lead-free NaNbO3 (NN) antiferroelectric ceramics have emerged as a prominent research topic in the field of energy storage due to their abundant phase structure, affordability, and moderate bandgap. The metastable ferroelectric Q phase results in a square hysteresis loop for NN at room temperature. However, 0.96NaNbO3-0.04 CaZrO3 (NNCZ) exhibits a typical double hysteresis loop at room temperature with the main crystalline phase being the antiferroelectric P phase, which has poor energy storage performance. In this study, Bi0.5Na0.5TiO3 (BNT) is used to optimize the energy storage performance and stabilize the P phase in NNCZ simultaneously. The dielectric constant and temperature-dependence XRD results that from −100 °C to 350 °C, x = 0.05 undergoes a phase transition from AFE P to AFE R and then to PE S. The solid solution of BNT decreased the sintering temperature of NN-based ceramics and decreased average grain size, thereby facilitating domain size reduction and improving the sample's energy storage efficiency from ∼30 % to ∼60 %, with an effective energy storage density reaching 1.51 J/cm3. The above results demonstrate that enhancing energy storage efficiency can be achieved through component design by reducing average grain size.

Local defect structure design enhanced energy storage performance in lead-free antiferroelectric ceramics

Antiferroelectrics (AFEs) are ideal candidates in dielectric, electromechanical, and electrothermal applications. NaNbO3 (NN), as a lead-free antiferroelectric (AFE) material under extensive investigation, exhibits ferroelectric (FE)-like polarization–electric field (P-E) hysteresis loops, characterized by high remnant polarization and large hysteresis. Herein, the local defect structure design is proposed to achieve high energy storage (ES) density in NN-based AFE ceramics. The pinning effect of defect dipoles and the enhancement of local structural disorder stabilize the AFE phase and reduce hysteresis losses. Consequently, an excellent ES performance of large recoverable energy density (Wrec) of 9.70 J/cm3 and high efficiency (η) of 88.75 % is concurrently obtained in NN-based relaxor AFE ceramics, with outstanding charge–discharge performance (PD∼413.2 MW/cm3, WD∼4.47 J/cm3), which are significantly improved compared to other reported values in lead-free ES ceramics. This indicates that NN-based ceramics are candidates for advanced ES capacitors and provides a feasible modulation approach for the development of new lead-free high-performance dielectric materials.

Phase transitions in Pb0.96La0.04(Zr0.95Ti0.05)O3 capacitors by in-situ AC-HRTEM

Antiferroelectrics (AFEs) undergo reversible antiferroelectric-ferroelectric (AFE-FE) phase transitions under external electric fields, and show great promise in modern electronic devices. The real-time phase transition behavior of pure PZO has been detected, while the dynamic studies of complex incommensurately modulated structure have never been addressed. Here, with the strong support of in-situ aberration corrected high resolution transmission electron microscopy (AC-HRTEM), the structural evolutionary behaviors in Pb0.96La0.04(Zr0.95Ti0.05)O3 (PLZT) film excited by energetic electron beams is decoded. The AFE-to-FE phase transition occurs via a 90° reorientation and a rapid expansion of domain boundary region at the expense of the initial AFE matrix. At the same time, the modulation periods experience a monotonic increase in the reorientation region. The observation is of certain significance to establish the deep-seated phase transition mechanism, which will facilitate the development of antiferroelectric-based nanoelectronics.

Enhancing comprehensive energy storage properties in Pb-free relaxor AFE/FE system via heterogeneous structure tuning and defect engineering

Multi-phase NaNbO3 (NN) exhibits high adjustability on the ordering of both polarization and oxygen octahedral tilt, becoming a perfect carrier to design heterogeneous structure for boosting comprehensive energy storage properties. To balance the energy storage density and efficiency, the coexistence of the relaxor antiferroelectric (AFE) with high polarization capability and the relaxor ferroelectrics (RFE) with high efficiency is designed in this work by introducing Sr0.7Bi0.2□0.1Ti0.75Ta0.2□0.05O3 (SBTT) into NaNbO3-BiFeO3. As a result, an outstanding capacitive energy density (Wrec) of 12.25 J cm−3 with a high η of 83 % can be achieved in NN-BF-SBTT ceramic, which can be identified as a novel heterogeneous coexisting structure with the crossover of high polarization capability in relaxor AFE and high efficiency in RFE in terms of high-resolution TEM. Furthermore, grain refinement and the dense structure inhibit the leak current, suppress the concentration of oxygen vacancy defects and raise the activation energy (Ea), thus enhancing the EB. These excellent energy storage properties overcome the trade-offs between the two sets of parameters (Wrec-η, ΔP-EB), offering a refreshing strategy for the development of high-performance ceramic capacitors.

Enhancing Short-Range Interactions to Broaden the Temperature Range for Coexistence of Antiferroelectricity and Ferroelasticity.

Antiferroelectric (AFE) materials, characterized by double electric hysteresis loops, can be transformed to the ferroelectric (FE) phase under an external electric field, making them promising candidates for electronic energy storage and solid-state refrigeration. Additionally, the field-induced strain in AFE materials is contingent upon the direction of the electric field, rendering it with a switching characteristic. Although AFE materials have made progress in the field of energy storage and negative electrocaloric effect, the coexistence of AFE and ferroelasticity is still rarely reported. Here, two isomorphic organic-inorganic hybrid perovskites, HDAEPbCl4 and HDAEPbBr4 (HDAE is [2-(hydroxydimethylammonio)ethan-1-aminium]), exhibiting FE-AFE-PE (PE is paraelectric) phase transitions, are presented. Remarkably, the temperature range where AFE and ferroelasticity coexist is significantly broadened from 59.9 K to 115.1 K by strengthening short-range forces via halogen substitution. This discovery extends the family of FE, AFE, and ferroelastic materials, contributing to the development of multifunctional materials and advancing multifunctional material development.

In situ X-ray diffraction evidence of field-induced transitions in a PbHfO3 single crystal

Antiferroelectric (AFE) materials are interesting due to recent discoveries of new prospective applications, although the mechanisms of the phase transitions that are at the heart of these applications remain incompletely understood. This work is devoted to the study of a single crystal of a model AFE, lead hafnate, by X-ray diffraction with in situ application of an electric field to trigger the transition to a polar phase. Two consecutive experiments were carried out on a 35 µm thick plate with [110] surface normal orientation over a field range from 0 to 330 kV cm−1 and back. A sharp drop in the intensity of R- and Σ-type reflections around 225 kV cm−1 was registered, with almost complete disappearance after 250 kV cm−1. This is compatible with a field-induced phase transition from the AFE to the R3m polar phase, which was suggested earlier on the basis of non-diffraction characterizations. X-ray diffraction reveals that the AFE domains with displacements parallel to the field direction react much more smoothly to the field, gradually reducing the AFE order at very small fields instead of holding it almost constant up to the critical field value, which is naturally expected. This expectation is fulfilled for domains with other orientations, but only for the first switching cycle; in the second switching cycle the AFE order already shows a notable decrease at subcritical fields. It is suggested that these observations could be linked with the antiphase domain wall population being affected by the field, which is consistent with the observation of diffuse rods between the Γ and Σ points. Another remarkable observation is the much smoother recovery of the AFE phase compared with its sharp disappearance at the critical field.

PYN-based antiferroelectric ceramics with superior energy storage performance within an ultra-wide temperature range

Antiferroelectric (AFE) ceramics are known for their rich field-induced phase transitions, which mainly contribute to their superior energy storage performance. However, the phase transitions instability caused by high temperature often limits its application scenarios. Developing AFE ceramics with high energy storage properties and wide application temperature ranges is challenging. Here, considering the B-site ordering characteristics of Pb(Yb0.5Nb0.5)O3, we propose a simple approach for introducing A-site distortion and adjusting B-site ordering to confront these challenges. In our Fe3+/Sr2+co-doping system, we realized an ultra-wide temperature range of 25–200 °C, within which the recoverable storage density was considerable: 8.48–13.39 J cm−3. In this interval, the discharge energy density could reach 6.15–9.67J cm−3, and the discharge current density and discharge power density were 755.09–1667.36 A cm−2 and 207.65–500.21 MW cm−3, respectively. The obtained high-temperature energy storage performance was superior to that of existing energy storage ceramics or polymer films. The introduction of A-site distortion improves the stability of AFE phase, the decrease in B-site ordering suppresses the remanent polarization and delays change in structural symmetry with temperature. This study forms a basis for further applications of dielectric capacitors and signifies the development of wide-temperature-range energy storage devices.

Unveiling a giant electrocaloric effect at low electric fields through continuous phase transition design

The reported electrocaloric (EC) effect in ferroelectrics is poised for application in the next generation of solid-state refrigeration technology, exhibiting substantial developmental potential. This study introduces a novel and efficient EC effect strategy in (1–x)Pb(Lu1/2Nb1/2)O3-xPbTiO3 (PLN-xPT) ceramics for low electric-field-driven devices. Phase-field simulations provide fundamental insights into thermally induced continuous phase transitions, guiding subsequent experimental investigations. A comprehensive composition/temperature-driven phase evolution diagram is constructed, elucidating the sequential transformation from ferroelectric (FE) to antiferroelectric (AFE) and finally to paraelectric (PE) phases for x=0.10−0.18 components. Direct measurements of EC performance highlight x=0.16 as an outstanding performer, exhibiting remarkable properties, including an adiabatic temperature change (ΔT) of 3.03 ​K, EC strength (ΔT/ΔE) of 0.08 ​K ​cm kV−1, and a temperature span (Tspan) of 31 ​°C. The superior EC effect performance is attributed to the temperature-induced FE to AFE transition at low electric fields and diffusion phase transition behavior contributing to the wide Tspan. This work provides valuable insights into developing high-performance EC effect across broad temperature ranges through the strategic design of continuous phase transitions, offering a simplified and economical approach for advancing ecofriendly and efficient solid-state cooling technologies.

Boosting room-temperature electrocaloric performance in B-site complex antiferroelectrics: A synergistic design approach

As an emerging eco-friendly solid-state refrigeration technology boasting high energy conversion efficiency, there is a pressing demand for ferroelectrics exhibiting significant electrocaloric effect (ECE) at room temperature (RT) for refrigeration applications. In this study, guided by phase-field simulation, we explore the potential of B-site complex Pb[Mg(1–x)ZnxW]1/2O3 (PMZW100x) antiferroelectrics (AFE) to deliver promising symmetric positive and negative ECE near ambient temperature. The first-order AFE-paraelectric (PE) phase transition occurring around 50 °C induces a substantial change in heat quantity and yields prominent ECE upon electric excitation. Maxwell characterization reveals a potential combination of positive and negative ECE, showcasing significant advantages in cooling capacity. Given the technical limitations of existing direct methods for testing under elevated electric fields, low-field ECE is validated using the heat flux approach to ensure the legitimacy of results. Direct measurements demonstrate a high positive ΔT value of 2.76 K at 52 °C and a negative ΔT of –2.91 K at 44 °C (under 140 kV cm–1), surpassing traditional PbZrO3 bulk materials. The coexistence of substantial positive and negative ΔT near RT in PMZW100x offers a new avenue for developing highly efficient solid-state cooling devices.

Comparative performance of fluorite-structured materials for nanosupercapacitor applications

Over the last fifteen years, ferroelectric (FE) and antiferroelectric (AFE) ultra-thin films based on fluorite-structured materials have drawn significant attention for a wide variety of applications requiring high integration density. AFE ZrO2, in particular, holds significant promise for nanosupercapacitors, owing to its potential for high energy storage density (ESD) and high efficiency (η). This work assesses the potential of high-performance Hf1−xZrxO2 thin films encapsulated by TiN electrodes that show linear dielectric (LD), FE, and AFE behavior. A wake-up effect is observed for AFE ZrO2, a phenomenon barely reported for pure zirconium oxide and AFE materials in general, correlated with the disappearance of the pinched hysteresis loop commonly observed for Zr-doped HfO2 thin films. ESD and η are compared for FE, AFE, and LD samples at the same electrical field (3.5 MV/cm). As expected, ESD is higher for the FE sample (95 J/cm3), but η is ridiculously small (≈55%) because of the opening of the FE hysteresis curve, inducing high loss. Conversely, LD samples exhibit the highest efficiency (nearly 100%), at the expense of a lower ESD. AFE ZrO2 thin film strikes a balance between FE and LD behavior, showing reduced losses compared to the FE sample but an ESD as high as 52 J/cm3 at 3.5 MV/cm. This value can be further increased up to 84 J/cm3 at a higher electrical field (4.0 MV/cm), with an η of 75%, among the highest values reported for fluorite-structured materials, offering promising perspectives for future optimization.

Significant enhancement of ferroelectric performance in lead-free NaNbO3 ceramics

The comparable free energy between antiferroelectric (AFE) and ferroelectric (FE) phases in NaNbO3 (NN) leads to unstable ferroelectricity, restricting future applications for energy storage devices. In this work, lead-free NN ceramics based on different sintering aids have been rigorously synthesized and the microstructural, dielectric, and ferroelectric properties of this system have been thoroughly examined. It is found that a tiny amount of sintering aids effectively lowers the sintering temperature and manipulates the grain growth, as well as plays an essential role in the stability of FE phase in NN ceramics. The tunable ferroelectricity is observed in NN: CuO as sintering aids results in a hardening effect, whereas MnO2 addition promotes softening behavior. More interestingly, introducing 1 wt% MnO2 as sintering aids results in strong ferroelectricity with high polarization (Pm) of 84.6 μC/cm2 stabilized by a stimulated electric field (Ef) as low as 60 kV/cm. This is significantly better than other NN-based ceramics (Pm is smaller than 40 μC/cm2 and Ef is higher than 90 kV/cm in the NN-based systems reported earlier). Our findings demonstrate the potential of sintering aids in tailoring the ferroelectric performance of lead-free NN ceramics, offering insights into the development of environmentally friendly ferroelectric materials.

Revealing the phase transition scenario in antiferroelectric thin films by x-ray diffuse scattering

There is no consensus among researchers regarding how phase transitions occur in antiferroelectric (AFE) epitaxial heterostructures, in particular, in heterostructures based on model AFE lead zirconate. The questions about the number of phase transitions in such films and by what mechanism they occur remain controversial. This paper presents a look at the phase transition scenario in two types of epitaxial heterostructures: PbZrO3/Ba[La–Sn]O3/MgO (001) thin films with thicknesses from 25 to 1000 nm and PbZrO3/SrRuO3/SrTiO3 (001) thin film 100 nm thick using the diffuse x-ray scattering in the grazing incidence setup. We register the characteristic butterfly-shaped diffuse scattering (DS) intensity distribution in the HK pseudocubic planes, which corresponds to the anisotropic ferroelectric soft mode. No incommensurate soft mode was observed in the cuts of reciprocal space parallel to the film surface by diffuse scattering. We reproduce the shape of DS distribution at different temperatures by the model based on the dielectric stiffness and the electric polarization correlation tensor in the cubic approximation. Such modeling allows not only to characterize the DS parameters from the challengingly low signal-to-background data set, but also to extract experimentally the sensitivity of the materials with respect to inhomogeneous polarization. While the observed temperature evolution of DS is consistent with the dielectric measurements, the correlation between the DS and the phase transition sequence observed by superstructure reflections is yet to be understood better.

Electronic structure orientation as a map of in-plane antiferroelectricity in β'-In2Se3.

Antiferroelectric (AFE) materials are excellent candidates for sensors, capacitors, and data storage due to their electrical switchability and high-energy storage capacity. However, imaging the nanoscale landscape of AFE domains is notoriously inaccessible, which has hindered development and intentional tuning of AFE materials. Here, we demonstrate that polarization-dependent photoemission electron microscopy can resolve the arrangement and orientation of in-plane AFE domains on the nanoscale, despite the absence of a net lattice polarization. Through direct determination of electronic transition orientations and analysis of domain boundary constraints, we establish that antiferroelectricity in β'-In2Se3 is a robust property from the scale of tens of nanometers to tens of micrometers. Ultimately, the method for imaging AFE domain organization presented here opens the door to investigations of the influence of domain formation and orientation on charge transport and dynamics.

Antiferroelectric Ceramics for Energy-Efficient Capacitors by Theory-Guided Discovery.

Antiferroelectric ceramics, via the electric-field-induced antiferroelectric (AFE)-ferroelectric (FE) phase transitions, show great promise for high-energy-density capacitors. Yet, currently, only 70-80% energy release is found during a charge-discharge cycle. Here, for PbZrO3-based oxides, geometric nonlinear theory of martensitic phase transitions is applied (first used to guide supercompatible shape-memory alloys) to predict the reversibility of the AFE-FE transition by using density-functional theory to assess AFE/FE interfacial lattice-mismatch strain that assures ultralow electric hysteresis and extended fatigue lifetime. A good correlation of mismatch strain with electric hysteresis, hence, with energy efficiency of AFE capacitors is observed. Guided by theory, high-throughput material search is conducted and AFE compositions with a near-perfect charge-discharge energy efficiency (98.2%), i.e., near-zero hysteresis are discovered. And the fatigue life of the capacitor reaches 79.5 million charge-discharge cycles, a factor of 80 enhancement over AFE ceramics with large electric hysteresis.

Regulating the switching electric field and energy-storage performance in antiferroelectric ceramics via heterogeneous laminated engineering

Antiferroelectric (AFE) ceramics with near-zero remanent polarization originating from unique electric field-induced antiferroelectric-ferroelectric phase transition are of great importance for the application in the energy-storage devices. However, achieving the most widely optimized switching electric field and energy-storage performance of antiferroelectric ceramics has predominantly relied on A/B-site ion doping strategies, often accomplished through a series of experimental and analytical works. In this context, we propose a novel strategy of heterogeneous laminated engineering as a substitute for A/B-site ion doping. This approach allows for a more intuitive regulation of the switching electric field and energy-storage performance in antiferroelectric ceramics without the need for complicated workload. Namely, the ferroelectric Pb0.99(Nb0.9Ta0.1)0.2(Zr0.9Sn0.1)0.8O3 (PNTZS) and antiferroelectric (Pb0.875La0.05Sr0.05) (Zr0.7Sn0.3)O3 (PLSZS) were layer-by-layer laminated using a tape-casting technique. All heterogeneous laminated ceramics exhibit antiferroelectric characteristics, and the magnitude of the switching electric field can be controlled by regulating the ratio between PNTZS and PLSZS. Furthermore, the finite element simulation revealed differences in the local electric fields between PNTZS and PLSZS in heterogeneous laminated ceramics, resulting in a win-win situation for both polarization and the breakdown strength. A large recoverable energy density of 11.2 J cm−3 with ultrahigh energy efficiency of 94.2 % can be obtained under 56 kV mm−1. Moreover, the energy storage performance shows no obvious deterioration in a broad frequency range (1–100 Hz) and temperature range (25–120 °C). Particularly, the outstanding discharge properties with a large discharge energy density of 7.1 J cm−3 and a high power density of 263.7 MW cm−3 show great potential for energy-storage applications. To conclude, a new strategy is opened up herein for designing antiferroelectric energy storage materials, showing the great application potential in the pulse power devices.