Controlling magnetism by means of electric fields is a key issue for the future development of low-power spintronics1. Progress has been made in the electrical control of magnetic anisotropy2, domain structure3,4, spin polarization5,6 or critical temperatures7,8. However, the ability to turn on and o robust ferromagnetism at room temperature and above has remained elusive. Here we use ferroelectricity in BaTiO3 crystals to tune the sharp metamagnetic transition temperature of epitaxially grown FeRh films and electrically drive a transition between antiferromagnetic and ferromagnetic order with only a few volts, just above room temperature. The detailed analysis of the data in the light of first-principles calculations indicate that the phenomenon is mediated by both strain and field e ects from the BaTiO3. Our results correspond to a magnetoelectric coupling larger than previous reports by at least one order of magnitude and open new perspectives for the use of ferroelectrics in magnetic storage and spintronics.

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Electric-field control of magnetic order above room temperature

Ferroelectrics are a class of materials that possess a variety of interactions between electrical, mechanical, and thermal properties that have enabled a wealth of functionalities. To realize integrated systems, the integration of these functionalities into semiconductor processes is necessary. To this end, the complexity of well-known ferroelectric materials, e.g., the perovskite class, causes severe issues that limit its applications in integrated systems. The discovery of ferroelectricity in hafnium oxide-based materials brought a renewed interest into this field during the last decade. Very recently, ferroelectricity was also verified in aluminum scandium nitride extending the potential of seeing a wealth of ferroelectric functions in integrated electronics in the future. This paper discusses the prospects of both material systems in various applications.

Next generation ferroelectric materials for semiconductor process integration and their applications

Oxide perovskites have emerged as an important class of materials with important applications in many technological areas, particularly thermocatalysis, electrocatalysis, photocatalysis, and energy storage. However, their implementation faces numerous challenges that are familiar to the chemist and materials scientist. The present work surveys the state-of-the-art by integrating these two viewpoints, focusing on the critical role that defect engineering plays in the design, fabrication, modification, and application of these materials. An extensive review of experimental and simulation studies of the synthesis and performance of oxide perovskites and devices containing these materials is coupled with exposition of the fundamental and applied aspects of defect equilibria. The aim of this approach is to elucidate how these issues can be integrated in order to shed light on the interpretation of the data and what trajectories are suggested by them. This critical examination has revealed a number of areas in which the review can provide a greater understanding. These include considerations of (1) the nature and formation of solid solutions, (2) site filling and stoichiometry, (3) the rationale for the design of defective oxide perovskites, and (4) the complex mechanisms of charge compensation and charge transfer. The review concludes with some proposed strategies to address the challenges in the future development of oxide perovskites and their applications.

Defect engineering of oxide perovskites for catalysis and energy storage: synthesis of chemistry and materials science.

Are lead-free relaxor ferroelectric materials the most promising candidates for energy storage capacitors?

Fatigue-Free Aurivillius Phase Ferroelectric Thin Films with Ultrahigh Energy Storage Performance

Lead-free BaBi4-xPrxTi4O15 (BBPT) relaxor ferroelectric films were prepared by the sol−gel method. A giant recoverable energy storage density of 47.8 J/cm3 and a high efficiency of 66.45% are obtained in BaBi3.9Pr0.1Ti4O15 (BBPT10) films. Specifically, the energy utilization ratio reaches as high as 0.0373. After 1 × 109 cycles, both the energy storage density and the efficiency can still be perfectly maintained. Moreover, BBPT10 capacitors possess outstanding thermal stability of energy storage performance over a wide temperature range of −20 °C to 120 °C. The breakdown strength reaches 1285 kV/cm. Such superb energy storage performances are mainly attributable to strong relaxation behaviors of the layered perovskite structure derived from the lattice distortion and structural transformation. BBPT based films provide a exploring area of lead-free ferroelectric materials widely applicable in energy storage devices.

High energy storage performances in lead-free BaBi3.9Pr0.1Ti4O15 relaxor ferroelectric films

The inevitable defect carriers in dielectric capacitors are generally considered to depress the polarization and breakdown strength, which decreases energy storage performances. Distinctive from the traditional aims of reducing defects as much as possible, this work designs (FeTi' - Vo••)• and (FeTi″ - Vo••) defect dipoles by oxygen vacancy defect engineering in acceptor doped Sr2Bi4Ti(5-x)FexO18 layered perovskite films with n-type leakage conductance. It is shown that oxygen vacancies effectively capture electrons (carriers) in n-type dielectrics to enhance the breakdown strength. Meanwhile, defect dipoles provide a driving field for depolarization to engineer the generation energy of domains and the domain wall energy, which effectively lowers the residual polarization Pr but not at the expense of the maximum polarization Pmax as relaxor ferroelectric regulations. Such defect engineering effectively breaks through the limitation, in which the energy storage density suffers from the trade-off relationship between polarization and breakdown strength. The Sr2Bi4Ti4.92Fe0.08O18 film with the proper oxygen vacancy content achieves a high energy density of 110.5 J/cm3 and efficiency of 70.0% at a high breakdown strength of 3915 kV/cm. This work explores an alternative way for breakthroughs possible in the intrinsic trade-off relationship to regulate dielectric energy storage by defect engineering.

Capturing Carriers and Driving Depolarization by Defect Engineering for Dielectric Energy Storage.

BaLaxBi4−xTi4O15 relaxor ferroelectric films with multilayered perovskite structure were prepared by the sol-gel method. Structural tunability is realized by layer selection engineering for La doping, which consequently regulates the energy storage performances. As x ≤ 0.2, Bi3+ is substituted by La3+ at perovskite-like layers, which increases the disorder degree of A-site cations and depresses the defects, it results in a high energy storage density of 44.7 J/cm3 and an energy storage efficiency of 60.1% in BaLa0.2Bi3.8Ti4O15 films under an applied electric field of 1667 kV/cm. While continuing to increase x, La3+ tends to enter (Bi2O2)2+ high resistance layers, which decreases the insulating properties and results in the reduction of the energy storage density. Moreover, good fatigue resistance after 108 polar switching and excellent thermal stability from −30 to 150 °C for energy storage performances are obtained by layer selection for La doping. This layer selection engineering for rare-earth doping provides an approach to regulate the energy storage performances in multilayered perovskite relaxor ferroelectric films.

Energy storage performances regulated by layer selection engineering for doping in multi-layered perovskite relaxor ferroelectric films

Ultrahigh energy storage performances derived from the relaxation behaviors and inhibition of the grain growth in La doped Bi5Ti3FeO15 films

Based on semiconductor characteristics under a high electric field for dielectric films, PNP-type heterostructural films composed of P-type Na0.5Bi3.25La1.25Ti4O15 (P-NBLT) and N-type BaBi3.4Pr0.6Ti4O15 (N-BBPT) layers with the same Aurivillius layered perovskite structure are designed to regulate the energy storage performances by depletion region engineering. An ultra-high recoverable energy storage density of 159.7 J cm−3 and a high storage efficiency of 70% are obtained in such PNP-type heterostructural films, which are attributed to the regulation of depletion region engineering highly sensitive to the applied electric field. The widths of depletion regions increase with the applied electric field due to the recombination and motion of the majority carriers to induce a high resistance state in depletion regions, which greatly improves the insulation characteristics and the breakdown electric field. Meanwhile, the designed PNP-type heterostructural films also exhibit good stability in terms of temperature, frequency and anti-fatigue, which provides an alternative way to improve the breakdown electric field and realize ultrahigh energy storage performances by depletion region engineering.

Ultra-high energy storage performances regulated by depletion region engineering sensitive to the electric field in PNP-type relaxor ferroelectric heterostructural films

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