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Reversible field-induced phase transitions define antiferroelectric perovskite oxides and lay the foundation for high-energy storage density materials, required for future green technologies. However, promising new antiferroelectrics are hampered by transition´s irreversibility and low electrical resistivity. Here, we demonstrate an approach to overcome these problems by adjusting the local structure and defect chemistry, delivering NaNbO 3 -based antiferroelectrics with well-defined double polarization loops. The attending reversible phase transition and structural changes at different length scales are probed by in situ high-energy X-ray diffraction, total scattering, transmission electron microcopy, and nuclear magnetic resonance spectroscopy. We show that the energy-storage density of the antiferroelectric compositions can be increased by an order of magnitude, while increasing the chemical disorder transforms the material to a relaxor state with a high energy efficiency of 90%. The results provide guidelines for efficient design of (anti-)ferroelectrics and open the way for the development of new material systems for a sustainable future. Antiferroelectrics are important in emerging energy-storage technologies. Here, the authors present an approach to adjust their local structure and defect chemistry, in order to overcome the current limitations and make them suitable for environmentally-friendly dielectric energy storage.

Piezoelectric single crystals based on the perovskite ferroelectric system (K,Na)NbO 3 have been widely investigated over the past 20 years due to large piezoelectric coefficients, high transition temperatures, low density, and the nontoxic chemical composition. Various crystal growth methods were examined, including high-temperature solution growth, solid-state crystal growth, Bridgman–Stockbarger method, and the floating zone method. Increased understanding of the crystal growth process and post-growth treatments resulted in improved crystal quality and larger sizes. Recently, crystals with high piezoelectric and electromechanical coupling coefficients exceeding 1000 pC/N and 0.90, respectively, were reported. Moreover, their large potential for high-frequency ultrasonic medical imaging was demonstrated. This work provides a review of the development of piezoelectric (K,Na)NbO 3 -based single crystals, including their growth, defect chemistry, domain structures, electromechanical properties, and applications. Approaches for reducing growth defects, controlling point defects, and domain engineering are discussed. The remaining open issues are presented and an outlook on the future is provided.

Here, we introduce phase change mechanisms in lead-free piezoceramics as a strategy to utilize attendant volume change for harvesting large electrostrain. In the newly developed (K,Na)NbO 3 solid-solution at the polymorphic phase boundary we combine atomic mapping of the local polar vector with in situ synchrotron X-ray diffraction and density functional theory to uncover the phase change and interpret its underlying nature. We demonstrate that an electric field-induced phase transition between orthorhombic and tetragonal phases triggers a dramatic volume change and contributes to a huge effective piezoelectric coefficient of 1250 pm V −1 along specific crystallographic directions. The existence of the phase transition is validated by a significant volume change evidenced by the simultaneous recording of macroscopic longitudinal and transverse strain. The principle of using phase transition to promote electrostrain provides broader design flexibility in the development of high-performance piezoelectric materials and opens the door for the discovery of high-performance future functional oxides. Functional oxides with coexisting states of comparable energy typically exhibit extraordinary responses to external stimuli. Here, the authors demonstrate that coexisting phase structures provide large electric field-triggered volume change.

Studies on the piezoelectric materials capable of efficiently outputting high electrostrains at low electric fields are driven by the demand for precise actuation in a wide range of applications. Large electrostrains of piezoceramics in operation require high driving fields, which limits their practical application due to undesirable nonlinearities and high energy consumption. Herein, a strategy is developed to enhance the electrostrains of piezoceramics while maintaining low hysteresis by incorporating lead magnesium niobate relaxors into lead zirconate titanium at the morphotropic phase boundary. An ultrahigh inverse piezoelectric coefficient d 33 * of 1380 pm/V with a reduced hysteresis of 11.5% is achieved under a low electric field of 1 kV/mm, outperforming the major lead-based piezoelectric materials. In situ synchrotron X-ray diffraction and domain wall dynamics characterization with sub-microsecond temporal resolution reveal that the outstanding performances originate from facilitated domain wall movement, which in turn is due to reduced lattice distortion and miniaturized domain structures. These findings not only address the pending challenges of effective actuation under reduced driving conditions but also lay the foundation for a more systematic approach to exploring the origin of large electrostrains. The authors develop an application-oriented low-field actuating piezoceramic via relaxor substitution. Their in situ synchrotron XRD analysis along with domain wall dynamics characterization reveals the mechanisms of outstanding performance.

Ferroelectric crystals have emerged as promising candidates for exotic optoelectronic platforms. However, the wide bandgaps of transparent ferroelectric crystals restrict their ultraviolet optical activity, hindering broadband photoelectric conversion. Herein, a hierarchical defect engineering strategy is proposed for ferroelectric oxides to achieve full-spectrum optical absorption and boost broadband self-powered photodetection. Based on the transparent calcium barium niobate crystal, red Ce:CSBN is designed through the cooperative isovalent substitution of Sr 2+ and aliovalent substitution of Ce 3+ . Furthermore, a black Ce:CSBN crystal is fabricated via thermal reduction, which demonstrated ultra-broadband absorption from the ultraviolet to the mid-infrared range. This extended absorption capability is attributed to the judiciously modulated oxygen vacancies. Consequently, self-powered photodetection is realized in the 250–5000 nm range with a high responsivity of >1 mA/W, representing the widest responsive range among all-known ferroelectric detectors. More impressively, a reversible red-black transition is achieved by controlling oxygen vacancy concentration. The authors propose a hierarchical defect engineering strategy for ferroelectric oxides to achieve full-spectrum optical absorption and boost broadband self-powered photodetection, realizing self-powered photodetection in the 250–5000 nm range with a responsivity of >1 mA/W.

Piezoelectric materials are capable of converting between mechanical and electrical energy, and are suitable for sensing, actuating and energy harvesting. While most conventional piezoelectric materials are brittle solids, flexible piezoelectric materials (FPM) retain functionality even under bending and stretching conditions. This characteristic has garnered increasing attention in recent years, particularly for wearable devices, where the ability to adapt to dynamic human movements is essential. In addition, wearable devices also demand excellent conformability, durability, and adaptability to miniaturization. FPM emerge as a promising solution that meet all these requirements. This review thus aims to offer a comprehensive summary of recent advances in the field of FPM, including piezoelectric polymers, composites, and inorganic flexible films. We introduce and categorize the specific features of these materials and highlight their emerging applications in electronic devices, and comment on the prospect of FPM as well as their potential challenges.

Re-poling of unexpected partially depoled piezoelectric materials conventionally needs to be first fully depoled through annealing above their Curie temperature to revive piezoelectric performances. Here, we investigated de-poling and re-poling of Pb(In 1/2 Nb 1/2 )O 3 -Pb(Mg 1/3 Nb 2/3 )O 3 -PbTiO 3 single crystals under electric fields at room temperature. We found that alternating current electric fields with amplitudes near the coercive field at low frequencies (<10 Hz) can be employed to successfully depolarize poled crystals at room temperature. We also demonstrated a reversible polarization switching process with a relaxor-PbTiO 3 single crystal ultrasound transducer without device performance degradations. This experimental observation is supported by phase-field simulation, showing that alternating current electric fields can readily induce de-poling at room temperature, while direct current electric fields induce a transient depoled state only within an uncontrollable short period of time. The findings suggest new strategies for unprecedented in-device tailoring of the polarization states of ferroelectric materials. The authors find that alternating current electric fields with amplitudes near the coercive field at low frequencies (<10 Hz) can be employed to depolarize poled relaxor-PbTiO 3 single crystals at room temperature, without conventional heat treatment.

The functionality of ferroelectrics is often constrained by their Curie temperature, above which depolarization occurs. Lithium (Li) is the only experimentally known substitute that can increase the Curie temperature in ferroelectric niobate-based perovskites, yet the mechanism remains unresolved. Here, the unique phenomenon in Li-substituted KNbO 3 is investigated using first-principles density functional theory. Theoretical calculations show that Li substitution at the A-site of perovskite introduces compressive chemical pressure, reducing Nb–O hybridization and associated ferroelectric instability. However, the large off-center displacement of the Li cation compensates for this reduction and further enhances the soft polar mode, thereby raising the Curie temperature. In addition, the stability of the tetragonal phase over the orthorhombic phase is predicted upon Li substitution, which reasonably explains the experimental observation of a decreased orthorhombic-to-tetragonal phase transition temperature. Finally, a metastable anti-phase polar state in which the Li cation displaces oppositely to the Nb cation is revealed, which could also contribute to the variation of phase transition temperatures. These findings provide critical insights into the atomic-scale mechanisms governing Curie temperature enhancement in ferroelectrics and pave the way for designing advanced ferroelectric materials with improved thermal stability and functional performance.

Polarization switching in lead-free (K 0.40 Na 0.60 )NbO 3 (KNN) single crystals was studied by switching spectroscopy piezoresponse force microscopy (SS-PFM). Acquisition of multiple hysteresis loops on a closely spaced square grid enables polarization switching parameters to be mapped in real space. Piezoresponse amplitude and phase hysteresis loops show collective symmetric/asymmetric characteristics, affording information regarding the switching behavior of different domains. As such, the out-of-plane polarization states of the domains, including amplitudes and phases can be determined. Our results could contribute to a further understanding of the relationships between polarization switching and polarization vectors at the nanoscale, and provide a feasible method to correlate the polarization hysteresis loops in a domain under an electric field with the polarization vector states.

Pore characteristics of pavement concrete with nano-particles (TiO2 or SiO2) are experimentally studied and compared with that of plain pavement concrete. The test results indicate that the addition of nano-particles improves the pore structure of concrete. The refined extent of pore structure of concretes increase with decreasing content of nano-particles. The pore structure of concrete with nano-TiO2 is better than that of concrete with the same content of nano-SiO2.