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Ceramic capacitors with ultrahigh power density are crucial in modern electrical applications, especially under high-temperature conditions. However, the relatively low energy density limits their application scope and hinders device miniaturization and integration. In this work, we present a high-entropy BaTiO 3 -based relaxor ceramic with outstanding energy storage properties, achieving a substantial recoverable energy density of 10.9 J/cm 3 and a superior energy efficiency of 93% at applied electric field of 720 kV/cm. Of particular importance is that the studied high-entropy composition exhibits excellent energy storage performance across a wide temperature range of -50 to 260 °C, with variation below 9%, additionally, it demonstrates great cycling reliability at 450 kV/cm and 200 °C up to 10 6 cycles. Electrical and in-situ structural characterizations revealed that the high-entropy engineered local structures are highly stable under varying temperature and electric fields, leading to superior energy storage performance. This study provides a good paradigm of the efficacy of the high-entropy engineering for developing high-performance dielectric capacitors., Competing Interests: Competing interests: The authors declare no competing interests., (© 2025. The Author(s).)

Polymer dielectric materials are widely used in electrical and electronic systems, and there have been increasing demands on their dielectric properties at high temperatures. Incorporating inorganic nanoparticles into polymers is an effective approach to improving their dielectric properties. However, the agglomeration of inorganic nanoparticles and the destabilization of the organic-inorganic interface at high temperatures have limited the development of nanocomposites toward large-scale industrial production. In this work, we synthesize metal-organic cage crosslinked nanocomposites by incorporating self-assembled metal-organic cages with amino reaction sites into the polyetherimide matrix. The in-situ crosslinking by self-assembled metal-organic cages not only achieves a homogeneous distribution of inorganic components, but also constructs robust organic-inorganic interfaces, which avoids the interfacial losses of conventional nanocomposites and improves the breakdown strength at elevated temperatures. Ultimately, the developed nanocomposites exhibit exceptionally high energy densities of 7.53 J cm -3 (150 °C) and 4.55 J cm -3 (200 °C) with charge-discharge efficiency of 90%., Competing Interests: Competing interests: The authors declare no competing interests., (© 2025. The Author(s).)

Thermoelectrics converting heat and electricity directly attract broad attentions. To enhance the thermoelectric figure of merit, zT, one of the key points is to decouple the carrier-phonon transport. Here, we propose an entropy engineering strategy to realize the carrier-phonon decoupling in the typical SrTiO 3 -based perovskite thermoelectrics. By high-entropy design, the lattice thermal conductivity could be reduced nearly to the amorphous limit, 1.25 W m -1 K -1 . Simultaneously, entropy engineering can tune the Ti displacement, improving the weighted mobility to 65 cm 2 V -1 s -1 . Such carrier-phonon decoupling behaviors enable the greatly enhanced μ W /κ L of ~5.2 × 10 3 cm 3 K J -1 V -1 . The measured maximum zT of 0.24 at 488 K and the estimated zT of ~0.8 at 1173 K in (Sr 0.2 Ba 0.2 Ca 0.2 Pb 0.2 La 0.2 )TiO 3 film are among the best of n-type thermoelectric oxides. These results reveal that the entropy engineering may be a promising strategy to decouple the carrier-phonon transport and achieve higher zT in thermoelectrics., (© 2024. The Author(s).)

Relaxor ferroelectrics are highly desired for pulse-power dielectric capacitors, however it has become a bottleneck that substantial enhancements of energy density generally sacrifice energy efficiency under superhigh fields. Here, we demonstrate a novel concept of highly polarizable concentrated dipole glass in delicately-designed high-entropy (Bi 1/3 Ba 1/3 Na 1/3 )(Fe 2/9 Ti 5/9 Nb 2/9 )O 3  ceramic achieved via substitution of multiple heterovalent ferroelectric-active principal cation species on equivalent lattice sites. The atomic-scaled polar heterogeneity of dipoles with different polar vectors between adjacent unit cells enables diffuse reorientation process but disables appreciable growth with electric fields. These unique features cause superior recoverable energy density of ~15.9 J cm -3 and efficiency of ~93.3% in bulk ceramics. We also extend the highly polarizable concentrated dipole glass to the prototype multilayer ceramic capacitor, which exhibits record-breaking recoverable energy density of ~26.3 J cm -3 and efficiency of ~92.4% with excellent temperature and cycle stability. This research presents a distinctive approach for designing high-performance energy-storage dielectric capacitors., (© 2024. The Author(s).)

Polymeric-based dielectric materials hold great potential as energy storage media in electrostatic capacitors. However, the inferior thermal resistance of polymers leads to severely degraded dielectric energy storage capabilities at elevated temperatures, limiting their applications in harsh environments. Here we present a flexible laminated polymer nanocomposite where the polymer component is confined at the nanoscale, achieving improved thermal-mechanical-electrical stability within the resulting nanocomposite. The nanolaminate, consisting of nanoconfined polyetherimide (PEI) polymer sandwiched between solid Al 2 O 3 layers, exhibits a high energy density of 18.9 J/cm 3 with a high energy efficiency of ~ 91% at elevated temperature of 200°C. Our work demonstrates that nanoconfinement of PEI polymer results in reduced diffusion coefficient and constrained thermal dynamics, leading to a remarkable increase of 37°C in glass-transition temperature compared to bulk PEI polymer. The combined effects of nanoconfinement and interfacial trapping within the nanolaminates synergistically contribute to improved electrical breakdown strength and enhanced energy storage performance across temperature range up to 250°C. By utilizing the flexible ultrathin nanolaminate on curved surfaces such as thin metal wires, we introduce an innovative concept that enables the creation of a highly efficient and compact metal-wired capacitor, achieving substantial capacitance despite the minimal device volume., (© 2024. The Author(s).)

Polar metals have recently garnered increasing interest because of their promising functionalities. Here we report the experimental realization of an intrinsic coexisting ferromagnetism, polar distortion and metallicity in quasi-two-dimensional Ca 3 Co 3 O 8 . This material crystallizes with alternating stacking of oxygen tetrahedral CoO 4 monolayers and octahedral CoO 6 bilayers. The ferromagnetic metallic state is confined within the quasi-two-dimensional CoO 6 layers, and the broken inversion symmetry arises simultaneously from the Co displacements. The breaking of both spatial-inversion and time-reversal symmetries, along with their strong coupling, gives rise to an intrinsic magnetochiral anisotropy with exotic magnetic field-free non-reciprocal electrical resistivity. An extraordinarily robust topological Hall effect persists over a broad temperature-magnetic field phase space, arising from dipole-induced Rashba spin-orbit coupling. Our work not only provides a rich platform to explore the coupling between polarity and magnetism in a metallic system, with extensive potential applications, but also defines a novel design strategy to access exotic correlated electronic states., (© 2024. The Author(s), under exclusive licence to Springer Nature Limited.)

Dielectric capacitors offer great potential for advanced electronics due to their high power densities, but their energy density still needs to be further improved. High-entropy strategy has emerged as an effective method for improving energy storage performance, however, discovering new high-entropy systems within a high-dimensional composition space is a daunting challenge for traditional trial-and-error experiments. Here, based on phase-field simulations and limited experimental data, we propose a generative learning approach to accelerate the discovery of high-entropy dielectrics in a practically infinite exploration space of over 10 11 combinations. By encoding-decoding latent space regularities to facilitate data sampling and forward inference, we employ inverse design to screen out the most promising combinations via a ranking strategy. Through only 5 sets of targeted experiments, we successfully obtain a Bi(Mg 0.5 Ti 0.5 )O 3 -based high-entropy dielectric film with a significantly improved energy density of 156 J cm -3 at an electric field of 5104 kV cm -1 , surpassing the pristine film by more than eight-fold. This work introduces an effective and innovative avenue for designing high-entropy dielectrics with drastically reduced experimental cycles, which could be also extended to expedite the design of other multicomponent material systems with desired properties., (© 2024. The Author(s).)

Ferroelectric materials have important applications in transduction, data storage, and nonlinear optics. Inorganic ferroelectrics such as lead zirconate titanate possess large polarization, though they are rigid and brittle. Ferroelectric polymers are light weight and flexible, yet their polarization is low, bottlenecked at 10 μC cm -2 . Here we show poly(vinylidene fluoride) nanocomposite with only 0.94% of self-nucleated CH 3 NH 3 PbBr 3 nanocrystals exhibits anomalously large polarization (~19.6 μC cm -2 ) while retaining superior stretchability and photoluminance, resulting in unprecedented electromechanical figures of merit among ferroelectrics. Comprehensive analysis suggests the enhancement is accomplished via delicate defect engineering, with field-induced Frenkel pairs in halide perovskite stabilized by the poled ferroelectric polymer through interfacial coupling. The strategy is general, working in poly(vinylidene fluoride-co-hexafluoropropylene) as well, and the nanocomposite is stable. The study thus presents a solution for overcoming the electromechanical dilemma of ferroelectrics while enabling additional optic-activity, ideal for multifunctional flexible electronics applications., (© 2024. The Author(s).)

Owing to their excellent discharged energy density over a broad temperature range, polymer nanocomposites offer immense potential as dielectric materials in advanced electrical and electronic systems, such as intelligent electric vehicles, smart grids and renewable energy generation. In recent years, various nanoscale approaches have been developed to induce appreciable enhancement in discharged energy density. In this Review, we discuss the state-of-the-art polymer nanocomposites with improved energy density from three key aspects: dipole activity, breakdown resistance and heat tolerance. We also describe the physical properties of polymer nanocomposite interfaces, showing how the electrical, mechanical and thermal characteristics impact energy storage performances and how they are interrelated. Further, we discuss multi-level nanotechnologies including monomer design, crosslinking, polymer blending, nanofiller incorporation and multilayer fabrication. We conclude by presenting the current challenges and future opportunities in this field., (© 2024. Springer Nature Limited.)

Electric field-induced second harmonic generation allows electrically controlling nonlinear light-matter interactions crucial for emerging integrated photonics applications. Despite its wide presence in materials, the figures-of-merit of electric field-induced second harmonic generation are yet to be elevated to enable novel device functionalities. Here, we show that the polar skyrmions, a topological phase spontaneously formed in PbTiO 3 /SrTiO 3 ferroelectric superlattices, exhibit a high comprehensive electric field-induced second harmonic generation performance. The second-order nonlinear susceptibility and modulation depth, measured under non-resonant 800 nm excitation, reach ~54.2 pm V -1 and ~664% V -1 , respectively, and high response bandwidth (higher than 10 MHz), wide operating temperature range (up to ~400 K) and good fatigue resistance (>10 10 cycles) are also demonstrated. Through combined in-situ experiments and phase-field simulations, we establish the microscopic links between the exotic polarization configuration and field-induced transition paths of the skyrmions and their electric field-induced second harmonic generation response. Our study not only presents a highly competitive thin-film material ready for constructing on-chip devices, but opens up new avenues of utilizing topological polar structures in the fields of photonics and optoelectronics., (© 2024. The Author(s).)

Topology created by quasi-continuous spatial variations of a local polarization direction represents an exotic state of matter, but field-driven manipulation has been hitherto limited to creation and destruction. Here we report that relatively small electric or mechanical fields can drive the non-volatile rotation of polar spirals in discretized microregions of the relaxor ferroelectric polymer poly(vinylidene fluoride-ran-trifluoroethylene). These polar spirals arise from the asymmetric Coulomb interaction between vertically aligned helical polymer chains, and can be rotated in-plane through various angles with robust retention. Given also that our manipulation of topological order can be detected via infrared absorption, our work suggests a new direction for the application of complex materials., (© 2024. The Author(s).)

Polymer nanocomposites with nanoparticles dispersed in polymer matrices have attracted extensive attention due to their significantly improved overall performance, in which the nanoparticle-polymer interface plays a key role. Understanding the structures and properties of the interfacial region, however, remains a major challenge for polymer nanocomposites. Here, we directly observe the presence of two interfacial polymer layers around a nanoparticle in polar polymers, i.e., an inner bound polar layer (~10 nm thick) with aligned dipoles and an outer polar layer (over 100 nm thick) with randomly orientated dipoles. Our results reveal that the impacts of the local nanoparticle surface potential and interparticle distance on molecular dipoles induce interfacial polymer layers with different polar molecular conformations from the bulk polymer. The bilayer interfacial features lead to an exceptional enhancement in polarity-related properties of polymer nanocomposites at ultralow nanoparticle loadings. By maximizing the contribution of inner bound polar layer via a nanolamination design, we achieve an ultrahigh dielectric energy storage density of 86 J/cm 3 , far superior to state-of-the-art polymers and nanocomposites., (© 2023. Springer Nature Limited.)

Solomon rings, upholding the symbol of wisdom with profound historical roots, were widely used as decorations in ancient architecture and clothing. However, it was only recently discovered that such topological structures can be formed by self-organization in biological/chemical molecules, liquid crystals, etc. Here, we report the observation of polar Solomon rings in a ferroelectric nanocrystal, which consist of two intertwined vortices and are mathematically equivalent to a [Formula: see text] link in topology. By combining piezoresponse force microscopy observations and phase-field simulations, we demonstrate the reversible switching between polar Solomon rings and vertex textures by an electric field. The two types of topological polar textures exhibit distinct absorption of terahertz infrared waves, which can be exploited in infrared displays with a nanoscale resolution. Our study establishes, both experimentally and computationally, the existence and electrical manipulation of polar Solomon rings, a new form of topological polar structures that may provide a simple way for fast, robust, and high-resolution optoelectronic devices., (© 2023. The Author(s).)

Thermoelectric materials can realize direct conversion between heat and electricity, showing excellent potential for waste heat recovery. Cu 2 Se is a typical superionic conductor thermoelectric material having extraordinary ZT values, but its superionic feature causes poor service stability and low mobility. Here, we reported a fast preparation method of self-propagating high-temperature synthesis to realize in situ compositing of BiCuSeO and Cu 2 Se to optimize the service stability. Additionally, using the interface design by introducing graphene in these composites, the carrier mobility could be obviously enhanced, and the strong phonon scatterings could lead to lower lattice thermal conductivity. Ultimately, the Cu 2 Se-BiCuSeO-graphene composites presented excellent thermoelectric properties with a ZT max value of ~2.82 at 1000 K and a ZT ave value of ~1.73 from 473 K to 1000 K. This work provides a facile and effective strategy to largely improve the performance of Cu 2 Se-based thermoelectric materials, which could be further adopted in other thermoelectric systems., (© 2023. The Author(s).)

Space-charge layers are frequently believed responsible for the large resistance of different interfaces in all-solid-state Li batteries. However, such propositions are based on the presumed existence of a Li-deficient space-charge layer with insufficient charge carriers, instead of a comprehensive investigation on the atomic configuration and its ion transport behavior. Consequently, the real influence of space-charge layers remains elusive. Here, we clarify the role of space-charge layers in Li 0.33 La 0.56 TiO 3 , a prototype solid electrolyte with large grain-boundary resistance, through a combined experimental and computational study at the atomic scale. In contrast to previous speculations, we do not observe the Li-deficient space-charge layers commonly believed to result in large resistance. Instead, the actual space-charge layers are Li-excess; accommodating the additional Li + at the 3c interstitials, such space-charge layers allow for rather efficient ion transport. With the space-charge layers excluded from the potential bottlenecks, we identify the Li-depleted grain-boundary cores as the major cause for the large grain-boundary resistance in Li 0.33 La 0.56 TiO 3 ., (© 2023. The Author(s).)

Manipulating the insulator-metal transition in strongly correlated materials has attracted a broad range of research activity due to its promising applications in, for example, memories, electrochromic windows and optical modulators 1,2 . Electric-field-controlled hydrogenation using ionic liquids 3-6 and solid electrolytes 7-9 is a useful strategy to obtain the insulator-metal transition with corresponding electron filling, but faces technical challenges for miniaturization due to the complicated device architecture. Here we demonstrate reversible electric-field control of nanoscale hydrogenation into VO 2 with a tunable insulator-metal transition using a scanning probe. The Pt-coated probe serves as an efficient catalyst to split hydrogen molecules, while the positive-biased voltage accelerates hydrogen ions between the tip and sample surface to facilitate their incorporation, leading to non-volatile transformation from insulating VO 2 into conducting H x VO 2 . Remarkably, a negative-biased voltage triggers dehydrogenation to restore the insulating VO 2 . This work demonstrates a local and reversible electric-field-controlled insulator-metal transition through hydrogen evolution and presents a versatile pathway to exploit multiple functional devices at the nanoscale., (© 2022. The Author(s), under exclusive licence to Springer Nature Limited.)

The operation of lithium-ion batteries involves electron removal from and filling into the redox orbitals of cathode materials, experimentally probing the orbital electron population thus is highly desirable to resolve the redox processes and charge compensation mechanism. Here, we combine quantitative convergent-beam electron diffraction with high-energy synchrotron powder X-ray diffraction to quantify the orbital populations of Co and O in the archetypal cathode material LiCoO 2 . The results indicate that removing Li ions from LiCoO 2 decreases Co t 2g orbital population, and the intensified covalency of Co-O bond upon delithiation enables charge transfer from O 2p orbital to Co e g orbital, leading to increased Co e g orbital population and oxygen oxidation. Theoretical calculations verify these experimental findings, which not only provide an intuitive picture of the redox reaction process in real space, but also offer a guidance for designing high-capacity electrodes by mediating the covalency of the TM-O interactions., (© 2022. The Author(s).)

Electrostatic dielectric capacitors are essential components in advanced electronic and electrical power systems due to their ultrafast charging/discharging speed and high power density. A major challenge, however, is how to improve their energy densities to effectuate the next-generation applications that demand miniaturization and integration. Here, we report a high-entropy stabilized Bi 2 Ti 2 O 7 -based dielectric film that exhibits an energy density as high as 182 J cm -3 with an efficiency of 78% at an electric field of 6.35 MV cm -1 . Our results reveal that regulating the atomic configurational entropy introduces favourable and stable microstructural features, including lattice distorted nano-crystalline grains and a disordered amorphous-like phase, which enhances the breakdown strength and reduces the polarization switching hysteresis, thus synergistically contributing to the energy storage performance. This high-entropy approach is expected to be widely applicable for the development of high-performance dielectrics., (© 2022. The Author(s), under exclusive licence to Springer Nature Limited.)

The electronic conductivities of ferroelectric domain walls have been extensively explored over the past decade for potential nanoelectronic applications. However, the realization of logic devices based on ferroelectric domain walls requires reliable and flexible control of the domain-wall configuration and conduction path. Here, we demonstrate electric-field-controlled stable and repeatable on-and-off switching of conductive domain walls within topologically confined vertex domains naturally formed in self-assembled ferroelectric nano-islands. Using a combination of piezoresponse force microscopy, conductive atomic force microscopy, and phase-field simulations, we show that on-off switching is accomplished through reversible transformations between charged and neutral domain walls via electric-field-controlled domain-wall reconfiguration. By analogy to logic processing, we propose programmable logic gates (such as NOT, OR, AND and their derivatives) and logic circuits (such as fan-out) based on reconfigurable conductive domain walls. Our work might provide a potentially viable platform for programmable all-electric logic based on a ferroelectric domain-wall network with low energy consumption., (© 2022. The Author(s).)

Magnons can transfer information in metals and insulators without Joule heating, and therefore are promising for low-power computation. The on-chip magnonics however suffers from high losses due to limited magnon decay length. In metallic thin films, it is typically on the tens of micrometre length scale. Here, we demonstrate an ultra-long magnon decay length of up to one millimetre in multiferroic/ferromagnetic BiFeO 3 (BFO)/La 0.67 Sr 0.33 MnO 3 (LSMO) heterostructures at room temperature. This decay length is attributed to a magnon-phonon hybridization and is more than two orders of magnitude longer than that of bare metallic LSMO. The long-distance modes have high group velocities of 2.5 km s -1 as detected by time-resolved Brillouin light scattering. Numerical simulations suggest that magnetoelastic coupling via the BFO/LSMO interface hybridizes phonons in BFO with magnons in LSMO to form magnon-polarons. Our results provide a solution to the long-standing issue on magnon decay lengths in metallic magnets and advance the bourgeoning field of hybrid magnonics., (© 2021. The Author(s).)

Strongly correlated oxides with a broken symmetry could exhibit various phase transitions, such as superconductivity, magnetism and ferroelectricity. Construction of superlattices using these materials is effective to design crystal symmetries at atomic scale for emergent orderings and phases. Here, antiferromagnetic Ruddlesden-Popper Sr 2 IrO 4 and perovskite paraelectric (ferroelectric) SrTiO 3 (BaTiO 3 ) are selected to epitaxially fabricate superlattices for symmetry engineering. An emergent magnetoelectric phase transition is achieved in Sr 2 IrO 4 /SrTiO 3 superlattices with artificially designed ferroelectricity, where an observable interfacial Dzyaloshinskii-Moriya interaction driven by non-equivalent interface is considered as the microscopic origin. By further increasing the polarization namely interfacial Dzyaloshinskii-Moriya interaction via replacing SrTiO 3 with BaTiO 3 , the transition temperature can be enhanced from 46 K to 203 K, accompanying a pronounced magnetoelectric coefficient of ~495 mV/cm·Oe. This interfacial engineering of Dzyaloshinskii-Moriya interaction provides a strategy to design quantum phases and orderings in correlated electron systems., (© 2021. The Author(s).)

In order to fully understand the lithium-ion transport mechanism in solid electrolytes for batteries, not only the periodic lattice but also the non-periodic features that disrupt the ideal periodicity must be comprehensively studied. At present only a limited number of non-periodic features such as point defects and grain boundaries are considered in mechanistic studies. Here, we discover an additional type of non-periodic feature that significantly influences ionic transport; this feature is termed a "single-atom-layer trap" (SALT). In a prototype solid electrolyte Li 0.33 La 0.56 TiO 3 , the single-atom-layer defects that form closed loops, i.e., SALTs, are found ubiquitous by atomic-resolution electron microscopy. According to ab initio calculations, these defect loops prevent large volumes of materials from participating in ionic transport, and thus severely degrade the total conductivity. This discovery points out the urgency of thoroughly investigating different types of non-periodic features, and motivates similar studies for other solid electrolytes.

Spin waves may constitute key components of low-power spintronic devices. Antiferromagnetic-type spin waves are innately high-speed, stable and dual-polarized. So far, it has remained challenging to excite and manipulate antiferromagnetic-type propagating spin waves. Here, we investigate spin waves in periodic 100-nm-wide stripe domains with alternating upward and downward magnetization in La 0.67 Sr 0.33 MnO 3 thin films. In addition to ordinary low-frequency modes, a high-frequency mode around 10 GHz is observed and propagates along the stripe domains with a spin-wave dispersion different from the low-frequency mode. Based on a theoretical model that considers two oppositely oriented coupled domains, this high-frequency mode is accounted for as an effective antiferromagnetic spin-wave mode. The spin waves exhibit group velocities of 2.6 km s -1 and propagate even at zero magnetic bias field. An electric current pulse with a density of only 10 5  A cm -2 can controllably modify the orientation of the stripe domains, which opens up perspectives for reconfigurable magnonic devices.

BiCuSeO oxyselenides are promising thermoelectric materials, yet further thermoelectric figure of merit ZT improvement is largely limited by the inferior electrical transport properties. The established literature on these materials shows only one power factor maximum upon carrier concentration optimization, which is typical for most thermoelectric semiconductors. Surprisingly, we found three power factor maxima when doping Bi with Pb. Based on our first-principles calculations, numerical modeling, and experimental investigation, we attribute the three maxima to the Fermi energy optimization, band convergence, and compositing effect due to in situ formed PbSe precipitates. Consequently, three ZT peaks of 0.9, 1.1, and 1.3 at 873 K are achieved for 4, 10, and 14 at.% Pb-doped samples, respectively, revealing the significance of complex electronic structure and multiple roles of Pb in BiCuSeO. The results establish an accurate band structure characterization for BiCuSeO and identify the role of band convergence and nanoprecipitation as the driving mechanism for high ZT.

Understanding the breakdown mechanisms of polymer-based dielectrics is critical to achieving high-density energy storage. Here a comprehensive phase-field model is developed to investigate the electric, thermal, and mechanical effects in the breakdown process of polymer-based dielectrics. High-throughput simulations are performed for the P(VDF-HFP)-based nanocomposites filled with nanoparticles of different properties. Machine learning is conducted on the database from the high-throughput simulations to produce an analytical expression for the breakdown strength, which is verified by targeted experimental measurements and can be used to semiquantitatively predict the breakdown strength of the P(VDF-HFP)-based nanocomposites. The present work provides fundamental insights to the breakdown mechanisms of polymer nanocomposite dielectrics and establishes a powerful theoretical framework of materials design for optimizing their breakdown strength and thus maximizing their energy storage by screening suitable nanofillers. It can potentially be extended to optimize the performances of other types of materials such as thermoelectrics and solid electrolytes.

Charged domain walls in ferroelectrics exhibit a quasi-two-dimensional conduction path coupled to the surrounding polarization. They have been proposed for use as non-volatile memory with non-destructive operation and ultralow energy consumption. Yet the evolution of domain walls during polarization switching makes it challenging to control their location and conductance precisely, a prerequisite for controlled read-write schemes and for integration in scalable memory devices. Here, we explore and reversibly switch the polarization of square BiFeO 3 nanoislands in a self-assembled array. Each island confines cross-shaped, charged domain walls in a centre-type domain. Electrostatic and geometric boundary conditions induce two stable domain configurations: centre-convergent and centre-divergent. We switch the polarization deterministically back and forth between these two states, which alters the domain wall conductance by three orders of magnitude, while the position of the domain wall remains static because of its confinement within the BiFeO 3 islands.

Ferroelectrics, which generate a switchable electric field across the solid-liquid interface, may provide a platform to control chemical reactions (physical properties) using physical fields (chemical stimuli). However, it is challenging to in-situ control such polarization-induced interfacial chemical structure and electric field. Here, we report that construction of chemical bonds at the surface of ferroelectric BiFeO 3 in aqueous solution leads to a reversible bulk polarization switching. Combining piezoresponse (electrostatic) force microscopy, X-ray photoelectron spectroscopy, scanning transmission electron microscopy, first-principles calculations and phase-field simulations, we discover that the reversible polarization switching is ascribed to the sufficient formation of polarization-selective chemical bonds at its surface, which decreases the interfacial chemical energy. Therefore, the bulk electrostatic energy can be effectively tuned by H + /OH - concentration. This water-induced ferroelectric switching allows us to construct large-scale type-printing of polarization using green energy and opens up new opportunities for sensing, high-efficient catalysis, and data storage.

Developing high-performance film dielectrics for capacitive energy storage has been a great challenge for modern electrical devices. Despite good results obtained in lead titanate-based dielectrics, lead-free alternatives are strongly desirable due to environmental concerns. Here we demonstrate that giant energy densities of ~70 J cm -3 , together with high efficiency as well as excellent cycling and thermal stability, can be achieved in lead-free bismuth ferrite-strontium titanate solid-solution films through domain engineering. It is revealed that the incorporation of strontium titanate transforms the ferroelectric micro-domains of bismuth ferrite into highly-dynamic polar nano-regions, resulting in a ferroelectric to relaxor-ferroelectric transition with concurrently improved energy density and efficiency. Additionally, the introduction of strontium titanate greatly improves the electrical insulation and breakdown strength of the films by suppressing the formation of oxygen vacancies. This work opens up a feasible and propagable route, i.e., domain engineering, to systematically develop new lead-free dielectrics for energy storage.

Oxygen ion transport is the key issue in redox processes. Visualizing the process of oxygen ion migration with atomic resolution is highly desirable for designing novel devices such as oxidation catalysts, oxygen permeation membranes, and solid oxide fuel cells. Here we show the process of electrically induced oxygen migration and subsequent reconstructive structural transformation in a SrCoO 2.5-σ film by scanning transmission electron microscopy. We find that the extraction of oxygen from every second SrO layer occurs gradually under an electrical bias; beyond a critical voltage, the brownmillerite units collapse abruptly and evolve into a periodic nano-twined phase with a high c/a ratio and distorted tetrahedra. Our results show that oxygen vacancy rows are not only natural oxygen diffusion channels, but also preferred sites for the induced oxygen vacancies. These direct experimental results of oxygen migration may provide a common mechanism for the electrically induced structural evolution of oxides.Information on how oxygen ions transport is crucial to understanding field-induced phase transformations in materials. Here, Zhang et al. directly image atomic-scale oxygen migration and the subsequent structural reconstruction in a SrCoO 2.5-σ film in the presence of an electric field.

A controllable ferroelastic switching in ferroelectric/multiferroic oxides is highly desirable due to the non-volatile strain and possible coupling between lattice and other order parameter in heterostructures. However, a substrate clamping usually inhibits their elastic deformation in thin films without micro/nano-patterned structure so that the integration of the non-volatile strain with thin film devices is challenging. Here, we report that reversible in-plane elastic switching with a non-volatile strain of approximately 0.4% can be achieved in layered-perovskite Bi2WO6 thin films, where the ferroelectric polarization rotates by 90° within four in-plane preferred orientations. Phase-field simulation indicates that the energy barrier of ferroelastic switching in orthorhombic Bi2WO6 film is ten times lower than the one in PbTiO3 films, revealing the origin of the switching with negligible substrate constraint. The reversible control of the in-plane strain in this layered-perovskite thin film demonstrates a new pathway to integrate mechanical deformation with nanoscale electronic and/or magnetoelectronic applications.

The main bottlenecks limiting the practical applications of current magnetoresistive random access memory (MRAM) technology are its low storage density and high writing energy consumption. Although a number of proposals have been reported for voltage-controlled memory device in recent years, none of them simultaneously satisfy the important device attributes: high storage capacity, low power consumption and room temperature operation. Here we present, using phase-field simulations, a simple and new pathway towards high-performance MRAMs that display significant improvements over existing MRAM technologies or proposed concepts. The proposed nanoscale MRAM device simultaneously exhibits ultrahigh storage capacity of up to 88 Gb inch(-2), ultralow power dissipation as low as 0.16 fJ per bit and room temperature high-speed operation below 10 ns.