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We perform dielectric and impedance spectrums on the compressively-strained ceramics of multiferroic bismuth ferrite. The subsurface-nanolayer quasipolarons manifest the step-like characteristic of pressure-dependent transient frequency and, furthermore, pressure-dependency fails in the transformation between complex permittivity and electrical impedance, which is well-known in classic dielectric physics, as well as the bulk dipole chain at the end of the dissipation peak.

Ferro-rotational (FR) materials, renowned for their distinctive material functionalities, present challenges in the growth of homo-FR crystals (i.e., single FR domain). This study explores a cost-effective approach to growing homo-FR helimagnetic RbFe(SO 4 ) 2 (RFSO) crystals by lowering the crystal growth temperature below the T FR threshold using the high-pressure hydrothermal method. Through polarized neutron diffraction experiments, it is observed that nearly 86% of RFSO crystals consist of a homo-FR domain. Notably, RFSO displays remarkable stability in the FR phase, with an exceptionally high T FR of ≈573 K. Furthermore, RFSO exhibits a chiral helical magnetic structure with switchable ferroelectric polarization below 4 K. Importantly, external electric fields can induce a single magnetic domain state and manipulate its magnetic chirality. The findings suggest that the search for new FR magnets with outstanding material properties should consider magnetic sulfates as promising candidates., (© 2024 The Author(s). Advanced Science published by Wiley‐VCH GmbH.)

Spin-crossover (SCO) ferroelectrics with dual-function switches have attracted great attention for significant magnetoelectric application prospects. However, the multiferroic crystals with SCO features have rarely been reported. Herein, a molecular multiferroic Fe(II) crystalline complex [Fe II (C 8 -F-pbh) 2 ] (1-F, C 8 -F-pbh = (1Z,N'E)-3-F-4-(octyloxy)-N'-(pyridin-2-ylmethylene)-benzo-hydrazonate) showing the coexistence of ferroelectricity, ferroelasticity, and SCO behavior is presented for the first time. By H/F substitution, the low phase transition temperature (270 K) of the non-fluorinated parent compound is significantly increased to 318 K in 1-F, which exhibits a spatial symmetry breaking 222F2 type ferroelectric phase transition with clear room-temperature ferroelectricity. Besides, 1-F also displays a spin transition between high- and low-spin states, accompanied by the d-orbital breaking within the t 2g 4 e g 2 and t 2g center. Moreover, the 222F2 type ferroelectric phase transition is also a ferroelastic one, verified by the ferroelectric domains reversal and the evolution of ferroelastic domains. To the knowledge, 1-F is the first multiferroic SCO molecular crystal. This unprecedented finding sheds light on the exploration of molecular multistability materials for future smart devices.6 e g ° configuration change of octahedrally coordinated Fe II center. Moreover, the 222F2 type ferroelectric phase transition is also a ferroelastic one, verified by the ferroelectric domains reversal and the evolution of ferroelastic domains. To the knowledge, 1-F is the first multiferroic SCO molecular crystal. This unprecedented finding sheds light on the exploration of molecular multistability materials for future smart devices., (© 2024 Wiley‐VCH GmbH.)

Manipulating spin transport enhances the functionality of electronic devices, allowing them to surpass physical constraints related to speed and power. For this reason, the use of van der Waals multiferroics at the interface of heterostructures offers promising prospects for developing high-performance devices, enabling the electrical control of spin information. Our work focuses primarily on a mechanism for multiferroicity in two-dimensional van der Waals materials that stems from an interplay between antiferromagnetism and the breaking of inversion symmetry in certain bilayers. We provide evidence for spin-electrical couplings that include manipulating van der Waals multiferroic edges via external voltages and the subsequent control of spin transport including for fully multiferroic spin field-effect transistors.

Hexagonal rare-earth iron oxides ( h-R FeO 3 ) exhibit spontaneous magnetization and room-temperature ferroelectricity simultaneously. However, achieving a large magnetoelectric coupling necessitates further exploration. Herein, we report the impact of the magnetic phase transition on the ferroelectric properties of epitaxial h-R FeO 3 ( R = Tb and Ho) films prepared by pulsed laser deposition. The metastable h - R FeO 3 phase is successfully stabilized with high crystallinity and low leakage current due to the ITO buffer layer, making it possible to investigate the ferroelectric properties. The h -TbFeO 3 film exhibits a magnetic-field-induced transition from antiferromagnetic (AFM) to weak ferromagnetic (wFM) phases below 30 K, while also exhibiting ferroelectricity at 300 K. The dielectric constants change with the magnetic phase transition, demonstrating hysteresis in the magnetocapacitance. In contrast, the h -HoFeO 3 film exhibits antiferroelectric-like behavior and an AFM - wFM phase transition. Notably, the h -HoFeO 3 film shows a rapid increase in the remnant polarization during the AFM-wFM phase transition accompanied by an increase in the ferroelectric component. Considering the strong connection between the antiferroelectric behavior in the h-R FeO 3 system and the ferroelectric domain wall motion, this considerable modification of ferroelectric properties during the magnetic phase transition is probably due to the faster movement of the ferroelectric domain walls in the wFM phase induced by the clamping effect. Our findings indicate the effectiveness of magnetic phase transitions in enhancing the magnetoelectric coupling, particularly when utilizing domain wall clamping properties.

Magneto-optical effects (MOE), interfacing the fundamental interplay between magnetism and light, have served as a powerful probe for magnetic order, band topology, and valley index. Here, based on multiferroic and topological bilayer antiferromagnets (AFMs), we propose a layer control of MOE (L-MOE), which is created and annihilated by layer-stacking or an electric field effect. The key character of L-MOE is the sign-reversible response controlled by ferroelectric polarization, the Néel vector, or the electric field direction. Moreover, the sign-reversible L-MOE can be quantized in topologically insulating AFMs. We reveal that the switchable L-MOE originates from the combined contributions of spin-conserving and spin-flip interband transitions in spin-valley splitting AFMs, a phenomenon not observed in conventional AFMs. Our findings bridge the ancient MOE to the emergent realms of layertronics, valleytronics, and multiferroics and may hold immense potential in these fields.

The search for novel materials with enhanced characteristics for the advancement of flexible electronic devices and energy harvesting devices is currently a significant concern. Multiferroics are a prominent example of energy conversion materials. The magnetoelectric conversion in a flexible composite based on a piezopolymer layer and a magnetic elastomer layer was investigated. The study focused on investigating the dynamic magnetoelectric effect in various configurations of external alternating and constant homogeneous magnetic fields (L-T and T-T configurations). The T-T geometry exhibited a two orders of magnitude higher coefficient of the magnetoelectric effect compared to the L-T geometry. Mechanisms of structure bending in both geometries were proposed and discussed. A theory was put forward to explain the change in the resonance frequency in a uniform external field. A giant value of frequency tuning in a magnetic field of up to 362% was demonstrated; one of the highest values of the magnetoelectric effect yet recorded in polymer multiferroics was observed, reaching up to 134.3 V/(Oe∙cm).

In our studies, we combined two powdered materials, i.e., ferroelectric triglycine sulfate (TGS) and ferrimagnetic magnetite Fe 3 O 4 , to obtain a magnetoelectric composite. The ferroelectric (E) part, i.e., TGS, was a hybrid organic-inorganic crystal, which we obtained as a pure single crystal from an aqueous solution using a static water evaporation method. The magnetic (M) part of the composite was commercially available magnetite. The samples used for the dielectric and magnetoelectric measurements were cold-pressed and made in the form of a circular tablet. The measuring electrodes were made of silver-based conductive paste and were attached to the sample. We measured the temperature dependencies of selected electrical parameters (e.g., dielectric permittivity, electrical capacity, and loss angle tangent). We used the dynamic lock-in method to check whether magnetoelectric coupling existed between the E and M phases. In this paper, we present the dielectric properties of pure monocrystalline TGS as a reference sample and compare the results for TGS powder, TGS + carbon powder, and TGS + Fe 3 O 4 powder. The magnetoelectric coupling presumably appeared for the composite TGS + 10 wt. % Fe 3 O 4 , as evidenced by the shift in the phase transition temperature in the TGS. Moreover, the theoretical interpretation of the effect is proposed.

Multiferroic composites exhibit remarkable magnetoelectric (ME) characteristics, offering diverse applications. The study investigated samarium (Sm) doped composites, specifically (1 - x )Ba 0.5 Sm 0.5 TiO 3 - x Co 0.5 Sm 0.5 Fe 2 O 4 ( x = 0.0,0.02,0.04,0.06), formed by combining Sm doped BaTiO 3 and CoFe 2 O 4 using the solid-state reaction method. X-ray diffraction analysis revealed a tetragonal structure in Ba 0.5 Sm 0.5 TiO 3 (SmBT) and a cubic spinel secondary phase in Co 0.5 Sm 0.5 Fe 2 O 4 (SmCF), suggesting uniform distribution of grains. The optical bandgap in SmBT and the composite showed a slight decrease (from 3.14 eV to 3.01 eV) with increasing Sm concentration, as observed in optical studies. The dielectric measurements showed that the dielectric constant of SmBT was higher ( ϵ' = 526.3) between 80 Hz and 8 MHz, while the composites had a lower dielectric constant ( ϵ' = 438.4) at lower frequencies and the real part of dielectric was fitted by Havriliak-Negami (H - N) model shows that the dielectric curves exhibit a characteristic dispersion pattern known as the cole-cole mode (grains) also confirmed by cole-cole plot. The response exhibited linearity, adhering to the universal dielectric response model. Ferroelectric behaviour in the underlying material confirms SmBT non-centrosymmetric character and the storage efficiency ( η ) of all composites surpassed 90%, reaching a peak of 94.8% with a ferrite content of 0.02. The versatility of the Sm-doped composites offers opportunities for diverse applications in fields such as electronics, telecommunications, and biomedical devices. Notably, these materials can be utilized in Memory Devices, Actuators, and other relevant applications., (© 2024 IOP Publishing Ltd.)

We report the magnetic-field-assisted electric-field-controlled domain switching of a magnetic single domain in a multiferroic/magnetoelectric Ni nanochevrons/[Pb(Mg 1/3 Nb 2/3 )O 3 ] 0.68 -[PbTiO 3 ] 0.32 (PMN-PT) layered structure. Initially, a magnetic field was applied in the transverse direction across single-domain Ni nanochevrons to transform each of them into a two-domain state. Subsequently, an electric field was applied to the layered structure, exerting the converse magnetoelectric effect to transform/release the two-domain Ni nanochevrons into one of two possible single-domain states. Finally, the experimental results showed that approximately 50% of the single-domain Ni nanochevrons were switched permanently after applying our approach (i.e., the magnetization direction was permanently rotated by 180 degrees). These results mark important advancements for future nanoelectromagnetic systems.

In the search for environmentally friendly materials with a wide range of properties, polymer composites have emerged as a promising alternative due to their multifunctional properties. This study focuses on the synthesis of composite materials consisting of four components: bacterial nanocellulose (BNC) modified with magnetic Fe 3 O 4 , and a mixture of BaTiO 3 (BT) and polyvinylidene fluoride (PVDF). The BT powder was mechanically activated prior to mixing with PVDF. The influence of BT mechanical activation and BNC with magnetic particles on the PVDF matrix was investigated. The obtained composite films' structural characteristics, morphology, and dielectric properties are presented. This research provides insights into the relationship between mechanical activation of the filler and structural and dielectric properties in the PVDF/BT/BNC/Fe 3 O 4 system, creating the way for the development of materials with a wide range of diverse properties that support the concept of green technologies.

In the room-temperature magnetoelectric multiferroic BiFeO 3 , the noncollinear antiferromagnetic state is coupled to the ferroelectric order, opening applications for low-power electric-field-controlled magnetic devices. While several strategies have been explored to simplify the ferroelectric landscape, here we directly stabilize a single-domain ferroelectric and spin cycloid state in epitaxial BiFeO 3 (111) thin films grown on orthorhombic DyScO 3 (011). Comparing them with films grown on SrTiO 3 (111), we identify anisotropic in-plane strain as a powerful handle for tailoring the single antiferromagnetic state. In this single-domain multiferroic state, we establish the thickness limit of the coexisting electric and magnetic orders and directly visualize the suppression of the spin cycloid induced by the magnetoelectric interaction below the ultrathin limit of 1.4 nm. This as-grown single-domain multiferroic configuration in BiFeO 3 thin films opens an avenue both for fundamental investigations and for electrically controlled noncollinear antiferromagnetic spintronics.

Two-dimensional multiferroic (2D) materials have garnered significant attention due to their potential in high-density, low-power multistate storage and spintronics applications. MXenes, a class of 2D transition metal carbides and nitrides, were first discovered in 2011, and have become the focus of research in various disciplines. Our study, utilizing first-principles calculations, examines the lattice structures, and electronic and magnetic properties of nitride MXenes with intrinsic band gaps, including V 2 NF 2 , V 2 NO 2 , Cr 2 NF 2 , Mo 2 NO 2 , Mo 2 NF 2 , and Mn 2 NO 2 . These nitride MXenes exhibit orbital ordering, and in some cases the orbital ordering induces magnetoelastic coupling or magnetoelectric coupling. Most notably, Cr 2 NF 2 is a ferroelastic material with a spiral magnetic ordered phase, and the spiral magnetization propagation vector is coupled with the direction of ferroelastic strain. The ferroelectric phase can exist as an excited state in V 2 NO 2 , Cr 2 NF 2 , and Mo 2 NF 2 , with their magnetic order being coupled with polar displacements through orbital ordering. Our results also suggest that similar magnetoelectric coupling effects persist in the Janus MXenes V 8 N 4 O 7 F, Cr 8 N 4 F 7 O, and Mo 8 N 4 F 7 O. Remarkably, different phases of Mo 8 N 4 F 7 O, characterized by orbital ordering rearrangements, can be switched by applying external strain or an external electric field. Overall, our theoretical findings suggest that nitride MXenes hold promise as 2D multiferroic materials.

Multiferroics have tremendous potential to revolutionize logic and memory devices through new functionalities and energy efficiencies. To reach their optimal capabilities will require better understanding and enhancement of the ferroic orders and couplings. Herein, we use ϵ-Fe 2 O 3 as a model system with a simplifying single magnetic ion. Using 15, 20, and 30 nm nanoparticles, we identify that a modified and size-dependent Fe-O hybridization changes the spin-orbit coupling and strengthens it via longer octahedra chains. Fe-O hybridization is modified through the incommensurate phase, with a unique two-step rearrangement of the electronic environment through this transition with attraction and then repulsion of electrons around tetrahedral Fe. Interestingly, size effects disappear in the high-temperature phase where the strongest Fe-O hybridization occurs. By manipulating this hybridization, we tune and control the multiferroic properties.

It has long been expected that the coexistence of ferroelectric and ferrovalley polarizations in one magnetic semiconductor could offer the possibility to revolutionize electronic devices. In this study, monolayer and bilayer YI 2 are studied. Monolayer YI 2 is a ferromagnetic semiconductor and exhibits a valley polarization up to 105 meV. All of the present bilayer YI 2 regardless of stacking orders show antiferromagnetic states. Interestingly, the bilayer YI 2 with 3R-type stackings shows not only valley polarization but also unexpected ferroelectric polarization, proving the concurrent ferrovalley and multiferroics behaviors. Moreover, the valley polarization of 3R-type bilayer YI 2 can be reversed by controlling the direction of ferroelectric polarization through an electric field or manipulating the magnetization direction using an external magnetic field. The amazing phenomenon is also demonstrated in 2D van der Waals LaI 2 and GdBr 2 bilayers. A design idea of multifunctional devices is proposed based on the concurrent ferrovalley and multiferroics characteristics.

The layer Hall effect (LHE) is of fundamental and practical importance in condensed-matter physics and material science; however, it was rarely observed and usually based on the paradigms of persistent electric field and sliding ferroelectricity. Here, a new mechanism of LHE is proposed by coupling layer physics with multiferroics using symmetry analysis and a low-energy k·p model. Due to time-reversal symmetry breaking and valley physics, the Bloch electrons on one valley will be subject to a large Berry curvature. This combined with inversion symmetry breaking gives rise to layer-polarized Berry curvature and can force the electrons to deflect in one direction of a given layer, thereby generating the LHE. We demonstrate that the resulting LHE is ferroelectrically controllable and reversible. Using first-principles calculations, this mechanism and predicted phenomena are verified in the multiferroic material of bilayer Co 2 CF 2 . Our finding opens a new direction for LHE and 2D materials research.

Multilayered magnetoelectric materials are of great interest for investigations due to their unique tuneable properties and giant values of magnetoelectric effect. The flexible layered structures consisting of soft components can reveal lower values of the resonant frequency for the dynamic magnetoelectric effect appearing in bending deformation mode. The double-layered structure based on the piezoelectric polymer polyvinylidene fluoride and a magnetoactive elastomer (MAE) with carbonyl iron particles in a cantilever configuration was investigated in this work. The gradient AC magnetic field was applied to the structure, causing the bending of the sample due to the attraction acting on the magnetic component. The resonant enhancement of the magnetoelectric effect was observed. The main resonant frequency for the samples depended on the MAE properties, namely, their thickness and concentration of iron particles, and was 156-163 Hz for a 0.3 mm MAE layer and 50-72 Hz for a 3 mm MAE layer; the resonant frequency depended on bias DC magnetic field as well. The results obtained can extend the application area of these devices for energy harvesting.

Experimental realization of thin films with a significant room-temperature magnetoelectric coupling coefficient, α ME , in the absence of an external DC magnetic field, has been thus far elusive. Here, a large coupling coefficient of 750 ± 30 mV Oe -1 is reported for multiferroic polymer nanocomposites (MPCs) thin-films in the absence of an external DC magnetic field. The MPCs are based on PMMA-grafted cobalt-ferrite nanoparticles uniformly dispersed in the piezoelectric polymer poly(vinylidene fluoride- -1 is reported for multiferroic polymer nanocomposites (MPCs) thin-films in the absence of an external DC magnetic field. The MPCs are based on PMMA-grafted cobalt-ferrite nanoparticles uniformly dispersed in the piezoelectric polymer poly(vinylidene fluoride- co -trifluoroethylene, P(VDF-TrFE). It is shown that nanoparticle agglomeration plays a detrimental role and significantly reduces α ME values in solution-processed thin films, which can be exploited in flexible and printable multiferroic electronic devices for sensing and memory applications.via atom transfer radical polymerization (ATRP) renders the nanoparticle miscible with P(VDF-TRFE) matrix, thus enabling their uniform dispersion in the matrix even in submicrometer thin films. Uniform dispersion yields maximized interfacial interactions between the ferromagnetic nanoparticles and the piezoelectric polymer matrix leading to the experimental demonstration of large α ME values in solution-processed thin films, which can be exploited in flexible and printable multiferroic electronic devices for sensing and memory applications.

With increasing applications for voltage-controlled magnetism, the need to more fully understand magnetoelectric coupling and strain transfer in nanostructured multiferroic composites has also increased. Here, multiferroic nanocomposites were synthesized using block copolymer templating to create mesoporous cobalt ferrite (CFO), followed by partly filling the pores with ferroelectric zirconium-substituted hafnia (HZO) using atomic layer deposition (ALD) to produce a porous multiferroic composite with enhanced mechanical flexibility. Upon electrical poling of the nanocomposite, we observed large changes in the magnetization. These changes partly relaxed upon removing the electric field, suggesting a strain-mediated mechanism. Both the anisotropic strain transfer from HZO to CFO and the strain relaxation after the field was removed were confirmed using high-resolution X-ray diffraction measurements collected during in-situ poling. The in-situ observation of both anisotropic strain transfer and large magnetization changes allows us to directly characterize the strong multiferroic coupling that can occur in flexible, nanostructured composites.

Over recent decades, the scientific community has managed to make great progress in the theoretical investigation and practical characterization of bismuth ferrite thin films. However, there is still much work to be completed in the field of magnetic property analysis. Under a normal operational temperature, the ferroelectric properties of bismuth ferrite could overcome the magnetic properties due to the robustness of ferroelectric alignment. Therefore, investigation of the ferroelectric domain structure is crucial for functionality of any potential devices. This paper reports deposition and analyzation of bismuth ferrite thin films by Piezoresponse Force Microscopy (PFM) and XPS methods, aiming to provide a characterization of deposited thin films. In this paper, thin films of 100 nm thick bismuth ferrite material were prepared by pulsed laser deposition on multilayer substrates Pt/Ti(TiO 2 )/Si. Our main purpose for the PFM investigation in this paper is to determine which magnetic pattern will be observed on Pt/Ti/Si and Pt/TiO 2 /Si multilayer substrates under certain deposition parameters by utilizing the PLD method and using samples of a deposited thickness of 100 nm. It was also important to determine how strong the measured piezoelectric response will be, considering parameters mentioned previously. By establishing a clear understanding of how prepared thin films react on various biases, we have provided a foundation for future research involving the formation of piezoelectric grains, thickness-dependent domain wall formations, and the effect of the substrate topology on the magnetic properties of bismuth ferrite films.

The geometry-dependent magnetoelectric (ME) and exchange bias (EB) effects of the nano ME sensor were investigated. The sensor consisted of the Longitudinal-Transverse (L-T) mode bi-layer bar structure comprising the ferromagnetic (FM) and ferroelectric (FE) materials and the anti-ferromagnetic (AFM) material. The bi-layer ME coefficient was derived from constitutive equations and Newton's second law. The trade-off between peak ME coefficient and optimal thickness ratio was realized. At the frequency × structure length = 0.1 and 1200, minimum and maximum peak ME coefficients of the Terfenol-D/PZT bi-layer were around 1756 and 5617 mV/Oe·cm, respectively, with 0.43 and 0.19 optimal thickness ratios, respectively. Unfortunately, the bi-layer could not distinguish the opposite magnetic field directions due to their similar output voltages. PtMn and Cr 2 O 3 , the AFM, were introduced to produce the EB effect. The simulation results showed the exchange field starting at a minimum PtMn thickness of 6 nm. Nevertheless, Cr 2 O 3 did not induce the exchange field due to its low anisotropy constant. The tri-layer ME sensor consisting of PZT (4.22 nm)/Terfenol-D (18 nm)/PtMn (6 nm) was demonstrated in sensing 2 Tbit/in 2 magnetic bits. The average exchange field of 5100 Oe produced the output voltage difference of 12.96 mV, sufficient for most nanoscale magnetic sensing applications.

After the discovery of bulk photovoltaic effect more than half a century ago, ferro-electrical and magneto-optical experiments have provided insights into various related topics, revealing above bandgap open voltages and non-central symmetrical current mechanisms. However, the nature of the photon-generated carriers responses and their microscopic mechanisms remain unclear. Here, all-inorganic perovskite Bi0.85Gd0.15Fe1-xMnxO3 thin films were prepared by a sol-gel process and the effects of Gd and Mn co-doped bismuth ferrites on their microtopography, grain boundries, multiferroic, and optical properties were studied. We discovered a simple "proof of principle" type new method that by one-step measuring the leakage current, one can demonstrate the value of photo generated current being the sum of ballistic current and shift current, which are combined to form the so-called bulk photovoltaic current, and can be related to the prototype intrinsic properties such as magneto-optical coupling and ferroelectric polarization. This result has significant potential influence on design principles for engineering multiferroic optoelectronic devices and future photovoltaic industry development.

The paper considers how a film of bismuth ferrite BiFeO 3 (BFO) is formed on a polymeric flexible polyimide substrate at low temperature ALD (250 °C). Two samples of BFO/Polyimide with different thicknesses (42 nm, 77 nm) were studied. As the thickness increases, a crystalline BFO phase with magnetic and electrical properties inherent to a multiferroic is observed. An increase in the film thickness promotes clustering. The competition between the magnetic and electrical subsystems creates an anomalous behavior of the magnetization at a temperature of 200 K. This property is probably related to the multiferroic/polymer interface. This paper explores the prerequisites for the low-temperature growth of BFO films on organic materials as promising structural components for flexible and quantum electronics.

This paper will provide a brief overview of the unique multiferroic material Bismuth ferrite (BFO). Considering that Bismuth ferrite is a unique material which possesses both ferroelectric and magnetic properties at room temperature, the uniqueness of Bismuth ferrite material will be discussed. Fundamental properties of the material including electrical and ferromagnetic properties also will be mentioned in this paper. Electrical properties include characterization of basic parameters considering the electrical resistivity and leakage current. Ferromagnetic properties involve the description of magnetic hysteresis characterization. Bismuth ferrite can be fabricated in a different form. The common forms will be mentioned and include powder, thin films and nanostructures. The most popular method of producing thin films based on BFO materials will be described and compared. Finally, the perspectives and potential applications of the material will be highlighted.

Eu 1- x Ba x Ti 1- y M y O 3 (M = Co or Ni) was sintered at 1400 °C under a reduction atmosphere. X-ray photoelectron spectroscopy revealed the mixed valences of Eu 2+ /Eu 3+ and Ti 4+ /Ti 3+ in EuTiO 3 and Eu 0.7 Ba 0.3 TiO 3 , as well as some oxygen vacancies required to keep the charge neutrality. The co-doping of Co 2+ /Ni 2+ in Eu 0.7 Ba 0.3 TiO 3 resulted in the disappearance of oxygen vacancies, as a result of a reduction in Ti 3+ numbers and an increase in Eu 3+ numbers. On the other hand, Ba 2+ doping led to an increased lattice parameter due to its larger ionic size than Eu 2+ , whereas the Co 2+ /Ni 2+ co-doping resulted in smaller lattice parameters because of the combined effects of ionic size and variation in the oxygen-vacancy numbers. Eu 0.7 Ba 0.3 TiO 3 exhibited a clear ferroelectricity, which persisted in the Co 2+ /Ni 2+ co-doped samples until the doping levels of y = 0.05 and 0.10, respectively. Eu 0.7 Ba 0.3 TiO 3 remained to be antiferromagnetic with a reduced transition temperature of 3.1 K, but co-doping of Co 2+ /Ni 2+ turned the samples from antiferromagnetic to ferromagnetic with transition temperatures of 2.98 K and 2.72 K, respectively. The cause for such a transition could not be explained by the larger lattice volume, oxygen vacancies and mixed valences of Eu 2+ /Eu 3+ , which were proposed in previous works. Instead, it was more likely to arise from a large asymmetric distortion of the Eu-O polyhedron introduced by the aliovalent doping, which promotes the admixture of Eu 5d and 4f states.

Our first-principles evidence shows that the two-dimensional (2D) multiferroic VSe 2 /In 2 Se 3 experiences continuous change of electronic structures, i.e. with the change of the ferroelectric (FE) polarization of In 2 Se 3 , the heterostructure can possess type-I, -II, and -III band alignments. When the FE polarization points from In 2 Se 3 to VSe 2 , the heterostructure has a type-III band alignment, and the charge transfer from In 2 Se 3 into VSe 2 induces half-metallicity. With reversal of the FE polarization, the heterostructure enters the type-I band alignment, and the spin-polarized current is turned off. When the In 2 Se 3 is depolarized, the heterostructure has a type-II band alignment. In addition, influence of the FE polarization on magnetism and magnetic anisotropy energy of VSe 2 was also analyzed, through which we reveal the interfacial magnetoelectric coupling effects. Our investigation about VSe 2 /In 2 Se 3 predicts its wide applications in the fields of both 2D spintronics and multiferroics., (© 2022 IOP Publishing Ltd.)

Organic-inorganic hybrid perovskites (OIHPs) have gained tremendous interest for their rich functional properties. However, the coexistence of more than one of ferroelectricity, ferromagnetism and ferroelasticity has been rarely found in OIHPs. Herein, we report a two-dimensional Cr 2+ -based OIHP, [3,3-difluorocyclobutylammonium] 2 CrCl 4 ([DFCBA] 2 CrCl 4 ), which shows both ferroelectricity and ferromagnetism. It undergoes a 4/mmmFm type ferroelectric phase transition at a temperature as high as 387 K and shows multiaxial ferroelectricity with a saturate polarization of 2.1 μC cm -2 . It acts as a soft ferromagnet with a Curie temperature of 32.6 K. This work throws light on the exploration of OIHPs with the coexistence of ferroelectricity and ferromagnetism for applications in future multifunctional smart devices., (© 2022 Wiley-VCH GmbH.)

Cyanido-bridged dimetallic complexes are attracting attention due to their varied structures and properties. However, homochiral cyanido-bridged dimetallic complexes are rare, and making them ferroelectric is a great challenge. Introducing C-F⋅⋅⋅K interactions between the guest chiral cations and the host [KFe(CN) 6 ] 2- framework, gives three-dimensional cyanido-bridged dimetallic multiferroics, [R- and S-3-fluoropyrrolidinium] 2 [KFe(CN) 6 ] (R- and S-3-FPC). The mirror-symmetric vibrational circular dichroism (VCD) signal shows their enantiomeric nature. R- and S-3-FPC crystallize in the same chiral-polar space group P2 1 at 298 K. Piezoresponse force microscopy (PFM), polarizing optical microscopy, and temperature-dependent second-harmonic generation (SHG) measurements show their multiferroic properties (the coexistence of ferroelectricity and ferroelasticity), in line with the Aizu notation of 222F2. R-3-FPC shows excellent ferroelectricity with saturated polarization up to 9.4 μC cm -2 ., (© 2022 Wiley-VCH GmbH.)

Radial vortex-based spin torque nano-oscillators (RV-STNOs) have attracted extensive attention as potential nano microwave signal generators due to their advantages over other topological states, such as their higher oscillation, higher microwave power, and lower power consumption. However, the current driving the oscillation frequency of the STNOs must be limited in a small range of adjustment, which means less data transmission channels. In this paper, a new RV-STNO system is proposed with a multiferroic nanostructure, which consists of an ultrathin magnetic multilayer and a piezoelectric layer. Phase diagrams of oscillation frequency and amplitude with respect to piezostrain and current are obtained through micromagnetic simulation. The results show that the threshold current density of -4000-ppm compressive strain-assisted RV-STNOs is reduced from 2 × 10 9 A/m 2 to 2 × 10 8 A/m 2 , showing one order of magnitude lower than that of conventional current-driven nano-oscillators. Meanwhile, the range of oscillation frequency adjustment is significantly enhanced, and there is an increased amplitude at the low oscillation point. Moreover, a promising digital binary frequency-shift key (BFSK) and binary amplitude-shift key (BASK) modulation technique is proposed under the combined action of current pulse and piezostrain pulse. They can transmit bit signals and show good modulation characteristics with a minimal transient state. These results provide a reference for developing the next generation of spintronic nano-oscillators with a wide frequency range and low power consumption, showing potential for future wireless communication applications.

Thin films of bismuth and iron oxides were obtained by atomic layer deposition (ALD) on the surface of a flexible substrate poly(4,4'-oxydiphenylene-pyromellitimide) (Kapton) at a temperature of 250°C. The layer thickness was 50 nm. The samples were examined by secondary-ion mass spectrometry, and uniform distribution of elements in the film layer was observed. Surface morphology, electrical polarization, and mechanical properties were investigated by atomic force microscope, piezoelectric force microscopy, and force modulation microscopy. The values of current in the near-surface layer varied in the range of ±80 pA when a potential of 5 V was applied. Chemical analysis was performed by X-ray photoelectron spectroscopy, where the formation of Bi 2 O 3 and Fe 2 O 3 phases, as well as intermediate phases in the Bi-Fe-O system, was observed. Magnetic measurements were carried out by a vibrating sample magnetometer that showed a ferromagnetic response. The low-temperature method of functionalization of the Kapton surface with bismuth and iron oxides will make it possible to adapt the Bi-Fe-O system to flexible electronics., (© 2021 Wiley Periodicals LLC.)

Multiferroic topologies are an emerging solution for future low-power magnetic nanoelectronics due to their combined tuneable functionality and mobility. Here, we show that in addition to being magnetoelectric multiferroic at room temperature, thin-film Aurivillius phase Bi 6 Ti x Fe y Mn z O 18 is an ideal material platform for both domain wall and vortex topology-based nanoelectronic devices. Utilizing atomic-resolution electron microscopy, we reveal the presence and structure of 180°-type charged head-to-head and tail-to-tail domain walls passing throughout the thin film. Theoretical calculations confirm the subunit cell cation site preference and charged domain wall energetics for Bi 6 Ti x Fe y Mn z O 18 . Finally, we show that polar vortex-type topologies also form at out-of-phase boundaries of stacking faults when internal strain and electrostatic energy gradients are altered. This study could pave the way for controlled polar vortex topology formation via strain engineering in other multiferroic thin films. Moreover, these results confirm that the subunit cell topological features play an important role in controlling the charge and spin state of Aurivillius phase films and other multiferroic heterostructures.

Neodymium iron borate NdFe 3 (BO 3 ) 4 is an intensively studied multiferroic with high electric polarization values controlled by a magnetic field. It is characterized by a large quadratic magnetoelectric effect, rigidity in the base plane and a rather strong piezoelectric effect. In this work, the atomic structure of (Nd 0.91 Bi 0.09 )Fe 3 (BO 3 ) 4 was studied by single-crystal X-ray diffraction in the temperature range 20-500 K (space group R32, Z = 3). The Bi atoms found in the composition partially substitute the Nd atoms in the 3a position; they entered the structure due to the growth conditions in the presence of Bi 2 Mo 3 O 12 . It was shown that in the temperature range 20-500 K there is no structural phase transition R32→P3 1 21, which occurs in rare-earth iron borates (RE = Eu-Er, Y) with an effective rare-earth cation radius smaller than that of Nd. The temperature dependence of the unit-cell c parameter reveals a slight increase on cooling below 90 K, which is similar to the results obtained previously for iron borates of Gd, Y and Ho. The atomic distances (Nd,Bi)-O, (Nd,Bi)-B, (Nd,Bi)-Fe, Fe-O, Fe-B and Fe-Fe in the iron chains and between chains decrease steadily with decreasing temperature from 500 to 90 K, whereas the B1(3b)-O distance does not change and the average B2(9e)-O distance increases slightly. There is a uniform decrease in the atomic displacement parameters with decreasing temperature, with a more pronounced decrease for the Nd(3a) and O2(9e) atoms. The O2(9e) atoms are characterized by the maximum atomic displacement parameters and the most elongated atomic displacement ellipsoids. The characteristic Debye and Einstein temperatures, and the static component in the atomic displacements were determined for cations using multi-temperature diffraction data. It was shown that the Nd cations have the weakest bonds with the surrounding atoms and the B cations have the strongest.

Electrically controlled magnetism in two-dimensional (2D) multiferroics is highly desirable for both fundamental research and the future development of low-power nanodevices. Herein, inspired by the recently experimentally realized 2D antiferromagnetic MnPSe 3 [ Nat. Nanotechnol. 2021, 16 (7), 782] and guided by a heteromagnetic structural design, we engineer strong magnetoelectric coupling in a hydrogen-intercalated 2D MnPSe 3 bilayer. Hydrogen functionalization breaks the centrosymmetry of bilayer MnPSe 3 , leading to out-of-plane ferroelectricity. Moreover, there is a phase transition from antiferromagnetic semiconductor to ferromagnetic half-metal in the H-bonded MnPSe 3 layer, while the other remains antiferromagnetic and semiconducting. When reversing the electrical polarization, the intercalated H atom can flip between the top and bottom layers with an ultralow switching barrier, which allows one to tune the magnetic order and conductivity of the individual layers via an external electric field. Our results pave a new avenue to realize strong magnetoelectric coupling in single-phase multiferroic material. The ferroelectricity-controlled magnetic phase transition and half-metallicity offer promising applications in nanoscale spintronics such as electrically written and magnetically read memories.

Multiferroic devices have attracted renewed attention in applications of photovoltaic devices for their efficient carrier separation driven by internal polarization, magnetization, and above-bandgap generated photovoltages. In this work, Zn 2 SnO 4 -based multiferroic Bi 6 Fe 1.6 Co 0.2 Ni 0.2 Ti 3 O 18 /Bi 2 FeCrO 6 (BFCNT/BFCO) heterojunction photoelectrodes were fabricated. Structural and optical analyses showed that the bandgap of the spinel Zn 2 SnO 4 is ∼3.1 eV while those of Aurivillius-type BFCNT and double-perovskite BFCO are 1.62 and 1.74 eV, respectively. Under the simulated AM 1.5G illumination, the as-prepared photoelectrodes delivered a photoconversion efficiency (η) of 3.40% with a short-circuit current density ( J sc ), open-circuit voltage ( V , 0.66 V, and 50.4%, respectively. Analyses of adjustment of an applied electric and magnetic field on photovoltaic properties indicated that both magnetization and polarization of multiferroics can effectively tune the built-in electric field and the transport of charge carriers, providing a new idea for the design of future high-performance multiferroic oxide photovoltaic devices.oc ), and fill factor (FF) of 10.3 mA·cm -2 , 0.66 V, and 50.4%, respectively. Analyses of adjustment of an applied electric and magnetic field on photovoltaic properties indicated that both magnetization and polarization of multiferroics can effectively tune the built-in electric field and the transport of charge carriers, providing a new idea for the design of future high-performance multiferroic oxide photovoltaic devices.

The effect of optical pumping and magnetic field on properties of the electronic phase separation regions, which are the multiferroic semiconductor heterostructures in the form of superlattices, have been studied in Eu 0.8 Ce 0.2 Mn 2 O 5 . These superlattices are formed due to self-organization in a dielectric crystal matrix as a result of the competing internal interactions balance and occupy a small crystal volume. The dynamical equilibrium states of superlattices are initially formed during cycling of as-grown samples in a magnetic field. The superlattices in such states are ferromagnetic and electrically neutral. Sets of ferromagnetic resonances were observed from individual layers of superlattices. Their features give rise information on properties of these layers and of a superlattice as a whole. The differences in the parameters of these resonances were due to different distributions of Mn 3+ and Mn 4+ ions in individual superlattices layers. It has been found that optical pumping having different powers allows us to control of multiferroic properties of superlattices layers by changing their magnetic and electric properties. It is shown that, under certain conditions, it is possible to significantly increase the temperatures at which multiferroic heterostructures exist.

In ferroelectric thin films, the polarization state and the domain configuration define the macroscopic ferroelectric properties such as the switching dynamics. Engineering of the ferroelectric domain configuration during synthesis is in permanent evolution and can be achieved by a range of approaches, extending from epitaxial strain tuning over electrostatic environment control to the influence of interface atomic termination. Exotic polar states are now designed in the technologically relevant ultrathin regime. The promise of energy-efficient devices based on ultrathin ferroelectric films depends on the ability to create, probe, and manipulate polar states in ever more complex epitaxial architectures. Because most ferroelectric oxides exhibit ferroelectricity during the epitaxial deposition process, the direct access to the polarization emergence and its evolution during the growth process, beyond the realm of existing structural in situ diagnostic tools, is becoming of paramount importance. We review the recent progress in the field of monitoring polar states with an emphasis on the non-invasive probes allowing investigations of polarization during the thin film growth of ferroelectric oxides. A particular importance is given to optical second harmonic generation in situ . The ability to determine the net polarization and domain configuration of ultrathin films and multilayers during the growth of multilayers brings new insights towards a better understanding of the physics of ultrathin ferroelectrics and further control of ferroelectric-based heterostructures for devices., (© 2021 IOP Publishing Ltd.)

Magnetic structure of the Co ions in monoclinic Co 3 TeO 6 in the antiferroelectric state at 16 K has been determined by neutron powder together with single-crystal diffractions. The indices of the magnetic reflections that appear at the incommensurate positions were determined by diffractions from a single crystal, which allow to uniquely identify the magnetic modulation vector. There are two crystallographically distinct Co layers. Magnetic incommensurability appears in the Co spins in the layers comprising zig-zag chains, with a magnetic modulation vector of (0.357, 0.103, 0.121) at 3 K but changes to (0.4439, 0, 0.137) at 16 K, while the Co ions in the honeycomb webs form a collinear antiferromagnetic structure. Thermal reduction rate of the Co moments in the honeycomb webs was found to be much smaller than those in the zigzag chains. Shifting of large amounts of electronic charge into the Co─O bonds in the honeycomb webs on warming is used to understand the behavior.

The antiferroelectric (AFE) phase, in which nonpolar and polar states are switchable by an electric field, is a recent discovery in promising multiferroics of hexagonal rare-earth manganites (ferrites), h - R Mn(Fe)O 3 . However, this phase has so far only been observed at 60-160 K, which restricts key investigations into the microstructures and magnetoelectric behaviors. Herein, we report the successful expansion of the AFE temperature range (10-300 K) by preparing h -DyFeO 3 films through epitaxial stabilization. Room-temperature scanning transmission electron microscopy reveals that the AFE phase originates from a nanomosaic structure comprising AFE P 3̅ c 1 and ferroelectric P 6 3 cm domains with small domain sizes of 1-10 nm. The nanomosaic structure is stabilized by a low c / a ratio derived from the large ionic radius of Dy 3+ . Furthermore, weak ferromagnetism and magnetocapacitance behaviors are observed. Below 10 K, the film exhibits an M-shaped magnetocapacitance versus magnetic field curve, indicating unusual magnetoelectric coupling in the AFE phase.

Recently, CuO has been proposed as a potential multiferroic material with high transition temperature. Competing models based on spin current and ionic displacements are invoked to explain ferroelectricity in CuO. The theoretical model based on ionic displacement predicted very small displacement (∼10 -5 Å) along the b axis. Experimentally detecting displacements of such a small amplitude in a particular direction is extremely challenging. Through our detailed angle resolved polarized Raman spectroscopy study on single crystal of CuO, we have validated the theoretical study and provided direct evidence of displacement along the b axis. Our study provides important contribution in the high temperature multiferroic compounds and showed for the first time, the use of the polarized Raman scattering in detecting ionic displacements at the femtometer scale., (© 2021 IOP Publishing Ltd.)

The composite material filled with nano-sized BaTiO3 and Fe3O4 was designed and studied. The aluminium phosphate ceramics was used as a matrix. The XRD analysis demonstrates only the crystalline structure of the fillers used. The thermogravimetric analysis proves the thermal stability of the composites up to 950 K. The Maxwell-Wagner relaxation was observed in the dielectric spectra of the investigated composites. The dielectric spectroscopy proves the close contact between the nanoparticles with the different ferroic ordering. The phosphate-based composites have been proved to be a prospective candidate for the multiphase multiferroic materials design and development.

Electric-field-driven spintronic devices are considered promising candidates for beyond CMOS logic and memory applications thanks to their potential for ultralow energy switching and nonvolatility. In this work, we have developed a comprehensive modeling framework to understand the fundamental physics of the switching mechanisms of the antiferromagnet/ferromagnet heterojunction by taking BiFeO 3 /CoFe heterojunctions as an example. The models are calibrated with experimental results and demonstrate that the switching of the ferromagnet in the antiferromagnet/ferromagnet heterojunction is caused by the rotation of the Neel vector in the antiferromagnet and is not driven by the unidirectional exchange bias at the interface as was previously speculated. Additionally, we demonstrate that the fundamental limit of the switching time of the ferromagnet is in the subnanosecond regime. The geometric dependence and the thermal stability of the antiferromagnet/ferromagnet heterojunction are also explored. Our simulation results provide the critical metrics for designing magnetoelectric devices.

Magnetoelectric (ME) materials composed of magnetostrictive and piezoelectric phases have been the subject of decades of research due to their versatility and unique capability to couple the magnetic and electric properties of the matter. While these materials are often studied from a fundamental point of view, the 4.0 revolution (automation of traditional manufacturing and industrial practices, using modern smart technology) and the Internet of Things (IoT) context allows the perfect conditions for this type of materials being effectively/finally implemented in a variety of advanced applications. This review starts in the era of Rontgen and Curie and ends up in the present day, highlighting challenges/directions for the time to come. The main materials, configurations, ME coefficients, and processing techniques are reported., Competing Interests: The authors declare no conflict of interest.

Ferroelectric-paraelectric superlattices show emerging new states, such as polar vortices, through the interplay and different energy scales of various thermodynamic constraints. By introducing magnetic coupling at BiFeO 3 -La 0.7 Sr 0.3 MnO 3 interfaces epitaxially grown on SrTiO 3 substrate, we find, for the first time in thin films, a sub-nanometer thick lamella-like BiFeO 3 . The emergent phase is characterized by an arrangement of a two unit cell thick lamella-like structure featuring antiparallel polarization, resulting an antiferroelectric-like structure typically associated with a morphotropic phase transition. The antipolar phase is embedded within a nominal R 3 c structure and is independent of the BiFeO 3 thickness (4-30 unit cells). Moreover, the superlattice structure with the morphotropic phase demonstrates azimuth-independent second harmonic generation responses, indicating a change of overall symmetry mediated by a delicate spatial distribution of the emergent phase. This work enriches the understanding of a metastable state manipulated by thermodynamic constraints by lattice strain and magnetic coupling.

Multiferroic materials endowed with both dielectric and magnetic orders, are ideal candidates for a wide range of applications. In this work, we reported two phase transitions of MnI 2 at 3.45 K and 4 K by systemically measuring the magnetic-field and temperature-dependent magnetization of the MnI 2 thin flakes. Furthermore, we observed similar temperature and field-dependent behaviours for the magnetic susceptibility of MnI 2 and electronic capacitance of the Ag/MnI 2 /Ag devices below 3.5 K. Considering the related theory work, we discussed the relationship between the antiferromagnetic and ferroelectric orders in MnI 2 . Our work reveals the in-plane magnetic and electric properties of MnI 2 materials, which might be helpful for the further investigation and application of MnI 2 multiferroics in the future., (© 2020 IOP Publishing Ltd.)

Nanocrystalline La 0.9 A 0.1 MnO 3 (where A is Li, Na, K) powders were synthesized by a combustion method. The powders used to prepare nanoceramics were fabricated via a high-temperature sintering method. The structure and morphology of all compounds were characterized by X-ray powder diffraction (XRD) and scanning electron microscopy (SEM). It was found that the size of the crystallites depended on the type of alkali ions used. The high-pressure sintering method kept the nanosized character of the grains in the ceramics, which had a significant impact on their physical properties. Magnetization studies were performed for both powder and ceramic samples in order to check the impact of the alkali ion dopants as well as the sintering pressure on the magnetization of the compounds. It was found that, by using different dopants, it was possible to strongly change the magnetic characteristics of the manganites.

Magnetic sensors are mandatory in a broad range of applications nowadays, being the increasing interest on such sensors mainly driven by the growing demand of materials required by Industry 4.0 and the Internet of Things concept. Optimized power consumption, reliability, flexibility, versatility, lightweight and low-temperature fabrication are some of the technological requirements in which the scientific community is focusing efforts. Aiming to positively respond to those challenges, this work reports magnetic proximity sensors based on magnetoelectric (ME) polyvinylidene fluoride (PVDF)/Metglas composites and an excitation-printed coil. The proposed magnetic proximity sensor shows a maximum resonant ME coefficient (α) of 50.2 Vcm -1 Oe -1 , an AC linear response (R 2 = 0.997) and a maximum voltage output of 362 mV, which suggests suitability for proximity-sensing applications in the areas of aerospace, automotive, positioning, machine safety, recreation and advertising panels, among others.

The operation mechanism of giant magnetoresistance (GMR) sensors relies on the linear response of the magnetization direction to an external magnetic field. Since the magnetic anisotropy of ferromagnetic layers can be manipulated by a strain-mediated magnetoelectric coupling effect, we propose a tunable GMR magnetic field sensor design that allows for voltage tuning of the linear range and sensitivity. A spin valve structure Ru/CoFe/Cu/CoFe/IrMn/Ru is grown on a PMN-PT (011) substrate, and the magnetization directions of ferromagnetic layers can be controlled by an electric field. An adjustable linear magnetoresistance is therefore induced. Based on the magnetoelectric coupling effect and spin valve, we prepared tunable GMR magnetic field sensors with bridge structures. The linear sensing range of a DC magnetic field is enhanced 6 times by applying an electric field of 14 kV/cm. The electrically tunable GMR sensor fulfills the requirements to work at different magnetic field ranges in the same configuration, therefore exhibiting great potential for applications in the Internet of things.

Laser fragmentation of colloidal submicron-sized bismuth ferrite particles was performed by irradiating a liquid jet to synthesize bismuth ferrite nanoparticles. This treatment achieved a size reduction from 450 nm to below 10 nm. A circular and an elliptical fluid jet were compared to control the energy distribution within the fluid jet and thereby the product size distribution and educt decomposition. The resulting colloids were analysed via UV-VIS, XRD and TEM. All methods were used to gain information on size distribution, material morphology and composition. It was found that using an elliptical liquid jet during the laser fragmentation leads to a slightly smaller and narrower size distribution of the resulting product compared to the circular jet.

The magnetoelectric properties of exchange-coupled Ni/CoFeB-based composite multiferroic microstructures are investigated. The strength and sign of the magnetoelastic effect are found to be strongly correlated with the ratio between the thicknesses of two magnetostrictive materials. In cases where the thickness ratio deviates significantly from one, the magnetoelastic behavior of the multiferroic microstructures is dominated by the thicker layer, which contributes more strongly to the observed magnetoelastic effect. More symmetric structures with a thickness ratio equal to one show an emergent interfacial behavior which cannot be accounted for simply by summing up the magnetoelastic effects occurring in the two constituent layers. This aspect is clearly visible in the case of ultrathin bilayers, where the exchange coupling drastically affects the magnetic behavior of the Ni layer, making the Ni/CoFeB bilayer a promising next-generation synthetic magnetic system entirely. This study demonstrates the richness and high tunability of composite multiferroic systems based on coupled magnetic bilayers compared to their single magnetic layer counterparts. Furthermore, because of the compatibility of CoFeB with present magnetic tunnel junction-based spintronic technologies, the reported findings are expected to be of great interest for the development of ultralow-power magnetoelectric memory devices.

We demonstrate a flexible nonvolatile multilevel memory and artificial synaptic devices based on the Cu/P(VDF-TrFE)/Ni memtranstor which exhibits pronounced nonlinear magnetoelectric effects at room temperature. The states of the magnetoelectric voltage coefficient α E of the memtranstor are used to encode binary information. By applying selective electric-field pulses, the states of α E can be switched repeatedly among 2 n states ( n = 1, 2, 3) in a zero dc bias magnetic field. In addition, the magnetoelectric coefficient is used to act as synaptic weight, and the induced magnetoelectric voltage V ME is regarded as postsynaptic potentials (excitatory or inhibitory). The artificial synaptic devices based on the Cu/P(VDF-TrFE)/Ni memtranstor display the long-term potentiation (depression) and spiking-time-dependent plasticity behaviors. The advantages of a simple structure, flexibility, multilevel, and self-biasing make the Cu/P(VDF-TrFE)/Ni organic memtranstor a promising candidate for applications in nonvolatile memory as well as artificial synaptic devices with low energy consumption.