Ferroelectric Order Research Articles

Ultrahigh Energy Storage Performance of BiFeO3-BaTiO3 Flexible Film Capacitor with High-Temperature Stability via Defect Design.

Nanoengineering polar oxide films have attracted great attention in energy storage due to their high energy density. However, most of them are deposited on thick and rigid substrates, which is not conducive to the integration of capacitors and applications in flexible electronics. Here, an alternative strategy using van der Waals epitaxial oxide dielectrics on ultra-thin flexible mica substrates is developed and increased the disorder within the system through high laser flux. The introduction of defects can efficiently weaken or destroy the long-range ferroelectric ordering, ultimately leading to the emergence of a large numbers of weak-coupling regions. Such polarization configuration ensures fast polarization response and significantly improves energy storage characteristics. A flexible BiFeO3-BaTiO3 (BF-BT) capacitor exhibits a total energy density of 43.5 J cm-3 and an efficiency of 66.7% and maintains good energy storage performance over a wide temperature range (20-200 °C) and under large bending deformation (bending radii ≈ 2mm). This study provides a feasible approach to improve the energy storage characteristics of dielectric oxide films and paves the way for their practical application in high-energy density capacitors.

Giant overall energy density performances via introducing aliovalent cations in BNT-based ferroelectric ceramics

The strategy of introducing aliovalent cations in the ferroelectric perovskites is the most promising for obtaining excellent overall energy storage density performances, simultaneously with good efficiency and thermal stability in dielectric ceramics for high pulse power technologies. Aliovalent cations could greatly enhance the short-range ferroelectric order (Polar nanoregions, PNRs), and local random field caused by vacancies, mismatch between size, electronic configuration, and other physical and chemical properties of aliovalent cations with the host perovskite. PNRs and local random field make the ceramic relaxor like with excellent overall energy storage density results such as total energy storage density (WT = 10.55 J/cm3, recoverable energy storage density Wrec = 7.82 J/cm3), power density (PD = 197 MW/cm3), current density (CD = 1312 A/cm2), and ultra-fast discharge rate (t = 24 ns) simultaneously with good working efficiency of 74 % by introducing 14 mol% of Bi(Zn1/3Nb2/3) aliovalent cations in the morphotropic phase boundary (MPB) (Bi0.47Na0.47)TiO3–0.06BaTiO3 composition. In addition, the same optimum sample also showed good thermal stability up to 240 °C, with <10–13 % variation in recoverable energy storage density and working efficiency respectively. The reason of excellent overall energy storage density, and their thermal stability in a broad temperature range might be due to short-range ferroelectric order, local random field, relaxor ferroelectric polymorphic phases, highly dense microstructure with small and uniform grains, as well as large band gape. Our study provides a good clue to obtain giant overall energy density results with good working efficiency and thermal stability in relaxor ferroelectric ceramics for high pulse power technology.

Ferroelectric Order Evolution in Freestanding PbTiO3 Films Monitored by Optical Second Harmonic Generation.

The demand for low-dimensional ferroelectric devices is steadily increasing, however, the thick substrates in epitaxial films impede further size miniaturization. Freestanding films offer a potential solution by eliminating substrate constraints. Nevertheless, it remains an ongoing challenge to improve the stability in thin and fragile freestanding films under strain and temperature. In this work, the structure and ferroelectric order of freestanding PbTiO3 (PTO) films are investigated under continuous variation of the strain and temperature using nondestructive optical second harmonic generation (SHG) technique. The findings reveal that there are both out-of-plane and in-plane domains with polarization along out-of-plane and in-plane directions in the orthorhombic-like freestanding PTO films, respectively. In contrast, only out-of-plane domains are observed in the tetragonal epitaxial PTO films. Remarkably, the ferroelectricity of freestanding PTO films is strengthened under small uniaxial tensile strain from 0% up to 1.66% and well-maintained under larger biaxial tensile strain up to 2.76% along the [100] direction and up to 4.46% along the [010] direction. Moreover, a high Curie temperature of 630K is identified in 50nm thick freestanding PTO films by wide-temperature-range SHG. These findings provide valuable understanding for the development of the next-generation electronic nanodevices with flexibility and thermostability.

Enhanced magnetic property and magnetodielectric coupling effect in multiferroic Gd2BaCuO5 via Zn2+ doping

The multiferroics with remarkable magnetoelectric (ME) coupling and technological application have drawn significant attention. Here, we report a chemical doping tunable effect on the magnetic, ferroelectric, and dielectric properties in type-II multiferroic Gd2BaCuO5. The magnetic measurement results show that a long-range antiferromagnetic ordering forms at the Néel temperature (TN1) of ∼12.1 K, and a second magnetization anomaly occurs at a lock-in transition temperature (TN2) of ∼6.4 K. Sharp peaks in the pyroelectric and dielectric curves are observed at the magnetic transition temperatures, indicating intrinsic coupling between magnetic and ferroelectric orderings. The doping of Zn2+ results in a gradual enhancement of magnetization due to the increase of uncompensated spins, and large magnetodielectric (MD) coupling parameter up to ∼7.65 % is obtained in Gd2BaCu0.7Zn0.3O5 because of strong spin-phonon coupling. The ferroelectric property is weakened in Zn2+ doped samples, suggesting the critical role of the 4f-3d magnetic interactions in determining the ME coupling effect. Moreover, an effective manipulation of electric field on magnetization is observed in Gd2BaCuO5. This work helps understand the importance of 4f-3d magnetic interactions in inducing ferroelectricity and explore the ME and MD coupling effects with multiple magnetic orderings.

Structurally Regulated Design Strategy of Bi0.5Na0.5TiO3-Based Ceramics for High Energy-Storage Performance at a Low Electric Field.

Dielectric ceramic capacitors are prospective energy-storage devices for pulsed-power systems owing to their ultrafast charge-discharge speed. However, low energy-storage density makes them difficult to commercialize for high-pulse-power technology applications. Herein, we presented a structurally regulated design strategy to disrupt a long-range ferroelectric order, refined grains, and eventually achieve excellent comprehensive energy-storage performance in (1 - x) (0.7Bi0.5Na0.5TiO3-0.3SrTiO3)-x Sm(Zn2/3Nb1/3)O3 eco-friendly ceramics. A large Wrec of ∼7.43 ± 0.05 J/cm3 and a high η of ∼85 ± 0.5% of 0.96 (0.7Bi0.5Na0.5TiO3-0.3SrTiO3)-0.04 Sm(Zn2/3Nb1/3)O3 were obtained at a low electric field of 290 kV cm-1 with good energy-storage temperature (25-120 °C), frequency (1-100 Hz) stability, and charge-discharge properties (PD ∼ 74 ± 1 MW/cm3 and τ0.9 ∼ 159 ± 2 ns). This strategy inspires rational structurally regulated designs and aims to promote the development of eco-friendly 0.7Bi0.5Na0.5TiO3-based ceramics with excellent energy-storage characteristics.

Intrinsic-strain-induced ferroelectric order and ultrafine nanodomains in SrTiO3

Nano ferroelectrics holds the potential application promise in information storage, electro-mechanical transformation, and novel catalysts but encounters a huge challenge of size limitation and manufacture complexity on the creation of long-range ferroelectric ordering. Herein, as an incipient ferroelectric, nanosized SrTiO3 was indued with polarized ordering at room temperature from the nonpolar cubic structure, driven by the intrinsic three-dimensional (3D) tensile strain. The ferroelectric behavior can be confirmed by piezoelectric force microscopy and the ferroelectric TO1 soft mode was verified with the temperature stability to 500 K. Its structural origin comes from the off-center shift of Ti atom to oxygen octahedron and forms the ultrafine head-to-tail connected 90° nanodomains about 2 to 3 nm, resulting in an overall spontaneous polarization toward the short edges of nanoparticles. According to the density functional theory calculations and phase-field simulations, the 3D strain-related dipole displacement transformed from [001] to [111] and segmentation effect on the ferroelectric domain were further proved. The topological ferroelectric order induced by intrinsic 3D tensile strain shows a unique approach to get over the nanosized limitation in nanodevices and construct the strong strain-polarization coupling, paving the way for the design of high-performance and free-assembled ferroelectric devices.

Realization of 2D multiferroic with strong magnetoelectric coupling by intercalation: a first-principles high-throughput prediction

The discovery of novel two-dimensional (2D) multiferroic materials is attractive due to their potential for the realization of information storage and logic devices. Although many approaches have been explored to simultaneously introduce ferromagnetic (FM) and ferroelectric (FE) orders into a 2D material, the resulting systems are often plagued by weak magnetoelectric (ME) coupling or limited room-temperature stability. Here, we present a superlattice strategy to construct non-centrosymmetric AM2X4 multiferroic monolayers, i.e., intercalating transition metal ions (A) into the tetragonal-like vacancies of transition metal dichalcogenide bilayers (MX2). Starting from 960 intercalated AM2X4 compounds, our high-throughput calculations have identified 21 multiferroics with robust magnetic order, large FE polarization, low transition barrier, high FE/FM transition temperature, and strong ME coupling. According to the origin of magnetism, we have classified them into twelve type-a, seven type-b, and two type-c multiferroics, which exhibit different ME coupling behavior. During the switching of polarization, the reversal of skyrmions chirality, the transition of the magnetic ground state from FM to antiferromagnetic, and the changes in spin-polarized electron distribution were observed in type-a, type-b, and type-c 2D multiferroic materials, respectively. These results substantially expand the family of 2D ferroic materials and pave an avenue for designing and implementing nonvolatile logic and memory devices.

A molecular perspective on the emergence of long-range polar order from an isotropic fluid

The ferroelectric nematic phase (NF) has quickly become the most studied system in liquid crystal research. In this work, we investigate the origin of such polar structure by studying a compound for which the NF phase directly follows the isotropic liquid phase on cooling, making it a particularly interesting system. Our experimental results evidence the presence of polar correlations already in the high-temperature phase, in which ferroelectric order can be induced under a sufficiently strong electric field. In the NF phase, molecular dynamics and polar correlations are investigated through detailed dynamic dielectric measurements, while second harmonic generation experiments evidence a large value of the main coefficient of the second order dielectric susceptibility tensor. Lastly, experimentally determined parameters are employed for calculations based on a recently proposed theoretical model for the stability of the NF phase. The obtained results suggest that the parallel alignment of dipoles is driven by a subtle interplay between electrostatic and excluded volume interactions.

Ferroelectric Order in the Chiral Coordination Polymers [Ln2(L*)2(ox)2(H2O)2] with Ln=Gd3+ or Dy3+, L*=((S, S)‐1,3‐bis(1‐Carboxylethyl)imidazolium and Ox=Oxalate.

AbstractWe evidence the ferroelectricity of two isostructural magnetic coordination networks obtained from a chiral imidazolium dicarboxylate salt ((S, S)‐1,3‐bis(1‐carboxylethyl)imidazolium or [HL*]) and Gd3+ or Dy3+ ions in presence of oxalic acid (H2ox). The two compounds exhibit a chiral structure P1 and ferroelectric properties. The crystallographic study shows that the Dy based‐compound is isostructural to the Gd analog. The non‐centrosymmetry of the two samples was further checked by means of nonlinear optical spectroscopy. The room temperature ferroelectric character of the compounds has been investigated through by an original method, derived from that used for thin films, made possible by preparing the sample as thin slices of resin containing inclusions of the coordination compounds.

Noncollinear Electric Dipoles in a Polar Chiral Phase of CsSnBr3 Perovskite.

Polar and chiral crystal symmetries confer a variety of potentially useful functionalities upon solids by coupling otherwise noninteracting mechanical, electronic, optical, and magnetic degrees of freedom. We describe two phases of the 3D perovskite, CsSnBr3, which emerge below 85 K due to the formation of Sn(II) lone pairs and their interaction with extant octahedral tilts. Phase II (77 K < T < 85 K, space group P21/m) exhibits ferroaxial order driven by a noncollinear pattern of lone pair-driven distortions within the plane normal to the unique octahedral tilt axis, preserving the inversion symmetry observed at higher temperatures. Phase I (T < 77 K, space group P21) additionally exhibits ferroelectric order due to distortions along the unique tilt axis, breaking both inversion and mirror symmetries. This polar and chiral phase exhibits second harmonic generation from the bulk and pronounced electrostriction and negative thermal expansion along the polar axis (Q22 ≈ 1.1 m4 C-2; αb = -7.8 × 10-5 K-1) through the onset of polarization. The structures of phases I and II were predicted by recursively following harmonic phonon instabilities to generate a tree of candidate structures and subsequently corroborated by synchrotron X-ray powder diffraction and polarized Raman and 81Br nuclear quadrupole resonance spectroscopies. Preliminary attempts to suppress unintentional hole doping to allow for ferroelectric switching are described. Together, the polar symmetry, small band gap, large spin-orbit splitting of Sn 5p orbitals, and predicted strain sensitivity of the symmetry-breaking distortions suggest bulk samples and epitaxial films of CsSnBr3 or its neighboring solid solutions as candidates for bulk Rashba effects.

Colossal Ferroelectric Photovoltaic Effect in Inequivalent Double-Perovskite Bi2FeMnO6 Thin Films.

Double perovskite films have been extensively studied for ferroelectric order, ferromagnetic order, and photovoltaic effects. The customized ion combinations and ordered ionic arrangements provide unique opportunities for bandgap engineering. Here, a synergistic strategy to induce chemical strain and charge compensation through inequivalent element substitution is proposed. A-site substitution of the barium ion is used to modify the chemical valence and defect density of the two B-site elements in Bi2FeMnO6 double perovskite epitaxial thin films. We dramatically increased the ferroelectric photovoltaic effect to ∼135.67 μA/cm2 from 30.62 μA/cm2, which is the highest in ferroelectric thin films with a thickness of less than 100 nm under white-light LED irradiation. More importantly, the ferroelectric polarization can effectively improve the photovoltaic efficiency of more than 5 times. High-resolution HAADF-STEM, synchrotron-based X-ray diffraction and absorption spectroscopy, and DFT calculations collectively demonstrate that inequivalent ion plays a dual role of chemical strain (+1.92 and -1.04 GPa) and charge balance, thereby introducing lattice distortion effects. The reduction of the oxygen vacancy density and the competing Jahn-Teller distortion of the oxygen octahedron are the main phenomena of the change in electron-orbital hybridization, which also leads to enhanced ferroelectric polarization values and optical absorption. The inequivalent strategy can be extended to other double perovskite systems and applied to other functional materials, such as photocatalysis for efficient defect control.

Flexoelectric Engineering of Bulk Photovoltaic Photodetector.

The bulk photovoltaic effect (BPVE) offers an interesting approach to generate a steady photocurrent in a single-phase material under homogeneous illumination, and it has been extensively investigated in ferroelectrics exhibiting spontaneous polarization that breaks inversion symmetry. Flexoelectricity breaks inversion symmetry via a strain gradient in the otherwise nonpolar materials, enabling manipulation of ferroelectric order without an electric field. Combining these two effects, we demonstrate active mechanical control of BPVE in suspended 2-dimensional CuInP2S6 (CIPS) that is ferroelectric yet sensitive to electric field, which enables practical photodetection with an order of magnitude enhancement in performance. The suspended CIPS exhibits a 20-fold increase in photocurrent, which can be continuously modulated by either mechanical force or light polarization. The flexoelectrically engineered photodetection device, activated by air pressure and without any optimization, possesses a responsivity of 2.45 × 10-2 A/W and a detectivity of 1.73 × 1011 jones, which are superior to those of ferroelectric-based photodetection and comparable to those of the commercial Si photodiode.

Dipole-dipole interactions and the origin of ferroelectric ordering in polar nematics

ABSTRACT A molecular origin of the ferroelectric ordering in the nematic phase is considered in detail considering a model based on electrostatic interaction between permanent molecular dipoles modulated by the anisotropic molecular shape. It is shown that a contribution to the total free energy of the long-range tail of the dipole-dipole interaction potential defines the total electrostatic energy of the system which depends on the sample shape and on the boundary conditions. This contribution may strongly affect the transition into the ferroelectric phase. However, the dipole-dipole interaction itself can hardly be responsible for the ferroelectric ordering in nematic liquid crystals for any reasonable values of the molecular dipole. A more promising model which combines dipole-dipole interaction and short-range orientational-translational correlations is also considered.

Revealing the three-dimensional arrangement of polar topology in nanoparticles

In the early 2000s, low dimensional ferroelectric systems were predicted to have topologically nontrivial polar structures, such as vortices or skyrmions, depending on mechanical or electrical boundary conditions. A few variants of these structures have been experimentally observed in thin film model systems, where they are engineered by balancing electrostatic charge and elastic distortion energies. However, the measurement and classification of topological textures for general ferroelectric nanostructures have remained elusive, as it requires mapping the local polarization at the atomic scale in three dimensions. Here we unveil topological polar structures in ferroelectric BaTiO3 nanoparticles via atomic electron tomography, which enables us to reconstruct the full three-dimensional arrangement of cation atoms at an individual atom level. Our three-dimensional polarization maps reveal clear topological orderings, along with evidence of size-dependent topological transitions from a single vortex structure to multiple vortices, consistent with theoretical predictions. The discovery of the predicted topological polar ordering in nanoscale ferroelectrics, independent of epitaxial strain, widens the research perspective and offers potential for practical applications utilizing contact-free switchable toroidal moments.

A design approach to obtaining highly polar liquid crystal dimers

ABSTRACT The synthesis and characterisation of 10 members of the [4[(E)-[4-[4-[ω-(4-cyanophenyl)phenoxy]alkyloxy]-3-nitrophenyl]methylideneamino]phenyl] 2,4-dimethoxybenzoates is reported in which the number of methylene units in the flexible spacer is increased from three to twelve. The mesogenic units are based on cyanobiphenyl and 3-nitrobenzylideneaniline benzoate and linked by the spacer such that their dipoles are parallel giving rise to a large longitudinal dipole moment. All 10 members of the series show a nematic phase, and the nematic-isotropic transition temperatures, TNI, and associated entropy changes show a strong dependence on the length and parity of the spacer. This behaviour is attributed to the average shapes of the molecules and their flexibility. The heptyl member was further characterised using dielectric spectroscopy revealing a high value of dielectric permittivity reflecting the large dipole moment of the molecules and possibly indicating local short-range ferroelectric order. The synthesis and characterisation of two members of the [4[(E)-[4-[4-[3-(ω-cyanophenyl)phenoxy]alkyloxy]-4-nitrophenyl]methylideneamino]phenyl] 2,4-dimethoxybenzoates are also described for which the difference in shape between odd and even members is reduced. Both dimers are exclusively nematogenic and the difference between TNI for the odd and even member is smaller reflecting the more similar molecular shapes. The potential for developing dimers that exhibit the ferroelectric nematic phase is discussed.

Excellent energy storage properties and multi-scale regulation mechanism of Sr(Zr0.5Ti0.5)O3-(Na0.5Bi0.5)0.94Ba0.06TiO3 ceramics

With the rapid advancement of energy storage technologies, dielectric capacitor materials with the outstanding recoverable energy density and power density have garnered significant attention from researchers in the past decades. In this study, (1-x) (Na0.5Bi0.5)0.94Ba0.06TiO3-xSr(Zr0.5Ti0.5)O3 ceramics were prepared via a solid-state reaction method, and the impact of composition on their structure, energy storage performance and stability were investigated. The results revealed that the introduction of Sr(Zr0.5Ti0.5)O3 induced the ferroelectric-relaxor transformation of (Na0.5Bi0.5)0.94Ba0.06TiO3 ceramics, leading to the destruction of the long-range ferroelectric order and the formation of polar nanoregions. In addition, the 0.7(Na0.5Bi0.5)0.94Ba0.06TiO3–0.3Sr(Zr0.5Ti0.5)O3 ceramic exhibited the optimal comprehensive energy storage performance: its recoverable energy storage Wrec attained 8.19 J/cm3 at 650 kV/cm, while the energy storage efficiency η was 85.6 %. Meanwhile, it displayed exceptionally high power density (315.7 MW/cm3) and charge-discharge rate (t0.9 = 50.4 ns). Moreover, this ceramic demonstrated the impressive energy storage performance, in particular, good temperature stability across a wide range of temperatures (20–140 °C), frequency stability (1–200 Hz), and fatigue resistance (1–106 cycles). Finite element analysis showed an enhancement in the breakdown field strength of the ceramics was attributed to the reduction in grain size. First-principles calculations revealed that the band gap increased after adding Sr and Zr elements, and the interactions between the states of O 2p and Ti 3d, Zr 3d, Bi 6p may serve as the microscopic origin of electron energy level polarization and enhanced dielectric performance. Thus, the ceramics have great potential for the application in high-power pulsed electronic systems.

Kapitza Stabilization of Quantum Critical Order

Dynamical perturbations modify the states of classical systems in surprising ways and give rise to important applications in science and technology. For example, Floquet engineering exploits the possibility of band formation in the frequency domain when a strong, periodic variation is imposed on parameters such as spring constants. We describe here Kapitza engineering, where a drive field oscillating at a frequency much higher than the characteristic frequencies for the linear response of a system changes the potential energy surface so much that maxima found at equilibrium become local minima, in precise analogy to the celebrated Kapitza pendulum where the unstable inverted configuration, with the mass above rather than below the fulcrum, actually becomes stable. Our starting point is a quantum field theory of the Ginzburg-Devonshire type, suitable for many condensed matter systems, including particularly ferroelectrics and quantum paralectrics. We show that an off-resonance oscillatory electric field generated by a laser-driven terahertz source can induce ferroelectric order in the quantum-critical limit. Heating effects are estimated to be manageable using pulsed radiation; “hidden” radiation-induced order can persist to low temperatures without further pumping due to stabilization by strain. We estimate the Ginzburg-Devonshire free-energy coefficients in SrTiO3 using density-functional theory and the stochastic self-consistent harmonic approximation accelerated by a machine-learned force field. Although we find that SrTiO3 is not an optimal choice for Kapitza stabilization, we show that scanning for further candidate materials can be performed at the computationally convenient density-functional theory level. We suggest second harmonic generation, soft-mode spectroscopy, and x-ray diffraction experiments to characterize the induced order. Published by the American Physical Society 2024

Enhanced structural, magnetodielectric, and multiferroic response in Fe and Co Co-doped Barium strontium titanate ceramics

In this paper, the ambient temperature multiferroic effect resulting from the incorporation of transition metal ions (Fe3+ and Co2+) in lead-free BST [ Ba0.7Sr0.3(Fex/2Cox/2)Ti1−xO3;x=0,0.01,0.03,0.05,0.07 ] ceramics synthesized via the solid-state reaction (SSR) procedure has been thoroughly analyzed. The investigation consistently scrutinized the effects of augmenting transition metal co-doping on the structural, ferroelectric, dielectric, magnetic, and magnetodielectric characteristics. The x-ray diffraction (XRD) patterns for all ceramic compositions demonstrated the formation of a monophasic (P4mm) crystalline structure. The Raman analysis evidenced the presence of various modes, which are associated with the occurrence of the single-phase and provide strong corroboration for the x-ray diffraction observations. Scanning electron micrographs reveals that the inclusion of transition metal ions results in the diminution of grain size. The frequency-dependent dielectric characteristics were represented over the frequency range of 1 kHz to 1 MHz. The P-E hysteresis curves demonstrate a consistent reduction in the values of Ps and Pr, whereas, the M-H curve reveals the enhancement in magnetic properties with increased doping. The magnetodielectric analysis confirmed the interplay between the ferroelectric and ferromagnetic ordering. The BST-1CF sample exhibited the highest MC % value of 5.30% along with the magnetoelectric coupling coefficient ‘γ’ of −6.01×10−1(memu/g)−2, making it a favorable entrant for the advancement of innovative non-volatile multiferroic memory gadgets.

Innovative Design of BNKT-xSLZT Ceramics: Maximizing the Polarization Difference for Enhanced Energy Storage.

Lead-free relaxor ferroelectric ceramics with outstanding energy-storage (ES) density (Wrec) and high ES efficiency (η) are crucial for advanced pulse-power capacitors. This study introduces a strategic approach to maximizing the polarization difference (ΔP) by inducing a transition from the ferroelectric phase to the ergodic relaxor (ER) phase. By employing this strategy, a series of ceramics, (1 - x)(Bi0.5Na0.4K0.1)TiO3-x(Sr0.85La0.1)(Zr0.5Ti0.5)O3 (BNKT-xSLZT), with varying SLZT content (x = 0.05, 0.10, 0.15, and 0.20), were designed. The addition of SLZT enhances cationic disorder, induces vacancies at A sites, and disrupts long-range ferroelectric order, facilitating the formation of polar nanoregions and enhancing relaxor ferroelectric behavior. Furthermore, a viscous polymer process (VPP) technology is employed to optimize the ceramics' structure, aiming to increase the breakdown strength (Eb) and enhance ΔP. Ultimately, enhanced ES performance is demonstrated in BNKT-0.15SLZTVPP, achieving a remarkable Wrec of 6.85 J/cm3 and η of 84% under 470 kV/cm. This composition demonstrates excellent stability with minimal variations in Wrec (3.0%) and η (4.4%) over the temperature range of 20-110 °C. Additionally, BNKT-0.15SLZTVPP exhibits exceptional pulse charge-discharge properties, featuring a high discharge density of 3.72 J/cm3, a large power density of 164.2 MW/cm3, and a short discharge time (t0.9) of 193 ns under 300 kV/cm. The study validates the practicality of BNKT-0.15SLZTVPP for pulse capacitors and underscores the potential to enhance ES performance through A-site donor doping and VPP technology. This work provides a comprehensive understanding of the interplay among composition, structure, and ES properties in lead-free relaxor dielectric ceramics, laying the groundwork for innovative advancements in the field.

Switching the spin cycloid in BiFeO3 with an electric field

Bismuth ferrite (BiFeO3) is a multiferroic material that exhibits both ferroelectricity and canted antiferromagnetism at room temperature, making it a unique candidate in the development of electric-field controllable magnetic devices. The magnetic moments in BiFeO3 are arranged into a spin cycloid, resulting in unique magnetic properties which are tied to the ferroelectric order. Previous understanding of this coupling has relied on average, mesoscale measurements. Using nitrogen vacancy-based diamond magnetometry, we observe the magnetic spin cycloid structure of BiFeO3 in real space. This structure is magnetoelectrically coupled through symmetry to the ferroelectric polarization and this relationship is maintained through electric field switching. Through a combination of in-plane and out-of-plane electrical switching, coupled with ab initio studies, we have discovered that the epitaxy from the substrate imposes a magnetoelastic anisotropy on the spin cycloid, which establishes preferred cycloid propagation directions. The energy landscape of the cycloid is shaped by both the ferroelectric degree of freedom and strain-induced anisotropy, restricting the spin spiral propagation vector to changes to specific switching events.