Magnetoelectric Composites Research Articles

Hierarchical core-shell transitional metal chalcogenides Co9S8/ CoSe2@C nanocube embedded into porous carbon for tunable and efficient microwave absorption

In the domain of electromagnetic (EM) wave absorbing materials, the selection of suitable components and microstructures is an effective approach for designing the intense coupling of wave impedance and EM dissipation. In this study, we have successfully fabricated a double-carbon modified Co9S8/CoSe2 nanocube, where the core-shell Co9S8/CoSe2@C cube was anchored onto porous carbon (PC). The existence of three-dimensional (3D) porous carbon and the fabrication of Co9S8/CoSe2@C distributed on carbon nanosheets contribute to the improvement of conduction, magnetic losses, and the optimization of impedance matching. Substantial heterogeneous interfaces are generated between Co9S8, CoSe2, carbon shells, and PC, leading to extensive interfacial polarization and facilitating the transformation of EM energy into thermal energy. The abundant defects, S and Se vacancies in carbon component can act as polarization centers, inducing dipolar polarization and thus increasing the electromagnetic wave (EMW) loss. The Co9S8/CoSe2@C@PC exhibits the best microwave absorption properties, with a minimum reflection loss (RLmin) of −64.1 dB at 2.5 mm and an effective absorption bandwidth (EAB) of 6.3 GHz. The High-Frequency Structure Simulator results indicate the RCS values of the samples within the range of -90 °C < θ < 90 °C are lower than -20 dB m2, which can achieve almost full-angle coverage in the actual environment. This research offers inspiration and strategies for the design and synthesis of multi-component magneto-electric composites based on transitional metal chalcogenides.

Features of 2D mapping technique of non-uniform magnetic fields using self-biased magnetoelectric composites based on “bidomain LiNbO3/Ni/Metglas” structures

Magnetoelectric (ME) composites are extensively researched for their ability to detect magnetic fields but are typically characterized by their interactions with homogeneous magnetic fields. However, practical applications often involve non-uniform magnetic fields (NMFs). In this study, we developed and validated a technique for 2D mapping of NMFs using sensor based on ME composite. The primary focus was on mapping the magnetic field generated by a single wire carrying an alternating current (AC). The experimental setup included a “bidomain LiNbO3/Ni/Metglas” ME structure, which demonstrated a ME coefficient of 0.83 V/(cm⋅Oe) without external biasing at 117 Hz. The ME structure was characterized using both quasi-static and dynamic methods, with the mapping performed at a frequency of 232 Hz, chosen to ensure a linear response and minimize resonance effects. Our measurements revealed that the position of maximum magnitude of the ME signal was consistently shifted from the position of the maximum integral magnetic field intensity of the wire. This shift was attributed to the deformation of the ME structure and the redistribution of the magnetic flux along the sample due to the magnetic layers, as confirmed through modeling. Further, the measured 2D mapping of the NMF from the wire closely matched the theoretical distribution, displaying axial symmetry but with a persistent shift of 2–3 mm along the length of the ME structure. These effects were linked to the linear dimensions and clamping methods of the ME structure. Overall, our experimental results closely correlated with theoretical data and the FEM model, demonstrating that ME composites are effective for NMF detection and mapping. Future work will aim to reduce the dimensions of the ME structure using MEMS technology to minimize the observed shift effects in the measurements.

A tunable self-bias effect in rubbery magnetoelectric materials

Magnetoelectric (ME) composites have recently received extensive attention due to their much higher ME coefficients and relatively high operating temperatures compared to single-phase ME materials. However, the ME coefficients of ME composites depend on the external magnetic field, and high ME coefficients usually require the presence of a biased external DC magnetic field. In this work, we propose a hybrid magnetoactive elastomer, which is a rubber matrix embedded with both soft iron particles and hard NdFeB particles. It is found that such a hybrid MAE shows a nonzero piezomagnetic coefficient even as the applied magnetic field approaches zero. Based on this phenomenon, we further propose a soft ME material with a self-bias effect and experimentally demonstrate that the self-bias effect can be tailored by changing the residual magnetization of the hybrid MAE and the charge density of the electret layer. This work successfully demonstrates a new mechanism of the self-bias effect for magnetoelectric materials and introduces a new member to the family of ME materials.

MULTIFERROIC PROPERTIES OF LEAD-FREE MAGNETOELECTRIC COMPOSITES (1-X)BZT/(X)CFO SYNTHESIZED BY ONE-POT MICROWAVE-ASSISTED PECHINI METHOD

MULTIFERROIC PROPERTIES OF LEAD-FREE MAGNETOELECTRIC COMPOSITES (1-X)BZT/(X)CFO SYNTHESIZED BY ONE-POT MICROWAVE-ASSISTED PECHINI METHOD

Multicaloric response tuned by electric field in cylindrical MnAs/PZT magnetoelectric composite

The possibility observation of the electric field controlled multicaloric response through quasi-isostatic compression as a result of the converse piezoelectric effect was demonstrated on the cylindrical type magnetoelectric composite MnAs/PZT. It was shown that an electric voltage of 100 V corresponding to an electric field of E ∼0.3 kV/mm applied to the walls of the piezoelectric component PZT of the MnAs/PZT composite contributes to an increase in the maximum adiabatic temperature change by 0.2 K in the temperature range of the magnetostructural phase transition of MnAs ∼317 K at a magnetic field change of 1.8 T. Numerical analysis using the finite element method has shown that an electric field voltage of 100 V is capable of creating a quasi-isostatic mechanical stress in the region inside a cylindrical PZT tube of ∼3 MPa. Moreover, in the region of weak pressures up to 10 MPa, the contribution to the total adiabatic temperature change from piezo-mechanical compression linearly depends on the electrical voltage that can be used for control by magnetic and caloric properties of multicaloric materials.

Reducing equivalent magnetic noise by electrode design and magnetic annealing in Quartz/Metglas magnetoelectric sensors

Magnetoelectric (ME) composites are promising for the development of high-performance magnetometers due to their high sensitivity, low cost, low power consumption, and small size. Enhancing the ME coefficient while reducing the background noise is an effective method to improve the performance of ME sensors, which remains challenging. In this work, we propose a method to reduce the equivalent magnetic noise by optimizing the electrode design and the magnetic annealing process in magnetoelectric quartz/Metglas composites. Compared with the non-optimized ME composites, the ME coefficient increases by 1.38 times while the background noise decreases by about 0.78 times, resulting in a LoD of 10 fT at resonance. Due to the high ME coefficient and low background noise, the equivalent magnetic noise from 20 kHz to 50 kHz was less than 6.10 pT/Hz1/2. The results show that proper annealing treatment of Metglas is beneficial for improving the soft magnetic properties. Meanwhile, the hollow electrode of quartz can reduce the equivalent capacitance and enhance the quality factor of the piezoelectric layer. This work demonstrates a feasible way to enhance the performance of ME magnetic field sensors.

Wireless driven and self-sensing flexible gripper based on piezoelectric elastomer/high-entropy alloy magnetoelectric composite

The mechanical gripper shows significant importance as an alternative to manual work, but presents certain limitations in its gas or electric power with complex wire connection, presents limited available area and loud working noise, and lacks sensing function for feedback to the environment. In the present work, a novel magnetically driven and self-sensing flexible gripper was prepared based on piezoelectric elastomer and high-entropy alloy composite. The high-entropy alloy is prepared as FeCoNi(AlGa)0.5 to realize high permeability, while the piezoelectric elastomer is synthesized with superior elasticity and low modulus. The incorporation of FeCoNi(AlGa)0.5 into the piezoelectric elastomer exhibits high flexibility, magnetostriction performances and piezoelectric responses, reaching maximum strain of 1534.5 %, maximum magnetostrictive coefficient of 320 ppm and maximum piezoelectric response of 0.28 V/N. Meanwhile, the flexible gripper achieves synchronous wireless driven gripping function with a maximum lifting ratio to dead load over 41.38, and self-sensing function of target physical size with accuracy over 95 %. The flexible gripper shows maximum work power as low as 5 W. Thus, the magnetically driven and self-sensing flexible gripper shows great potential in intelligent industrial equipment.

Enhancement of Microwave Absorption Properties of Crystal‐Engineered Perovskite Oxide Using Cobalt Ferrite

A multiferroic composite that comprises of a non‐ferromagnetic ferroelectric material with a high dielectric constant and a non‐ferroelectric ferromagnetic material with a high magnetostriction is of tremendous interest as microwave absorption material due to its applicability in tunable microwave phase shifters, resonators, filters, absorbers, etc. In the previous work, the solid solution of strontium titanate and sodium bismuth titanate (Sr0.5(Na0.5Bi0.5)0.5TiO3, SNBT50), which is observed to possess a very high dielectric constant at room temperature (Ferroelectrics, Vol 583, 252–263 [2021]), is successfully reported. Thus, in this work, a core–shell magnetoelectric composite is prepared by coating highly ferromagnetic and magnetostrictive cobalt ferrite onto a diamagnetic but strongly ferroelectric SNBT50 to enhance its magnetic properties and to investigate the modification in microwave absorption. Detailed characterization of electric and magnetic parameters in microwave frequency range (1–20 GHz) reports substantial enhancement in the magnetic permeabilities as well as the magnetic loss of the composite system, as opposed to bare SNBT50. This results in improved impedance matching in the system and enhanced microwave absorption, with a minimum reflection loss (RL) of −20.19 dB and an increased effective absorption bandwidth of 4.56 GHz at a mere 2.7 mm absorber length. Consequently, in this investigation, a promising pathway is established for the development of multiferroic composites with favorable magnetoelectric coupling at room temperature that possesses wide absorption bandwidth and suitable RL, making them highly suitable for use in multiferroic‐based microwave components.

AC/DC Magnetic Field Sensing Based on a Piezoelectric Polymer and a Fully Printed Planar Spiral Coil.

Additive manufacturing (AM) is emerging as an eco-friendly method for minimizing waste, as the demand for responsive materials in IoT and Industry 4.0 is on the rise. Magnetoactive composites, which are manufactured through AM, facilitate nonintrusive remote sensing and actuation. Printed magnetoelectric composites are an innovative method that utilizes the synergies between magnetic and electric properties. The study of magnetoelectric effects, including the recently validated piezoinductive effect, demonstrates the generation of electric voltage through external AC and DC magnetic fields. This shift in magnetic sensors, utilizing piezoinductive effect of the piezoelectric polymer poly(vinylidene fluoride), PVDF, eliminates the need for magnetic fillers in printed devices, aligning with sustainability principles, essential for the deployment of IoT and Industry 4.0. The achieved sensitivity surpasses other studies by 100 times, showcasing linear outputs for both applied AC and DC magnetic fields. Additionally, the sensor capitalizes on the linear phase shift of the generated signal with an applied DC magnetic field, an unprecedented effect. Thus, this work introduces a remarkable magnetoactive device with a sensitivity of ST = 95.1 ± 0.9 μV Oe-1 mT-1, a significantly improved performance compared to magnetoelectric devices using polymer composites. As a functional proof of concept of the developed system, a magnetic position sensor has been demonstrated.

Influence of CoFe2O4 content on the multifunctional properties of BiFeO3–CoFe2O4 core-shell nanocomposites

The utilization of magnetoelectric composites, particularly core-shell configurations, enhances their versatile applications in various sectors such as medicine and data storage. Among these composites, the perovskite-spinel combination is distinguished by its significant potential. A series of (1-x) BiFeO3-(x) CoFe2O4 (where x = 0.0, 0.2, 0.5, and 1.0) nano core-shell structures were synthesized using a sol-gel auto-combustion method to explore their multifunctional capabilities. Structural analyses identified peaks corresponding to both perovskite and spinel phases. Field Emission Scanning Electron Microscopy revealed a reduction in average particle size with an increase in CoFe2O4 content.The particle size in the BFO80-CFO20 sample has been reduced from 243 nm to 34 nm. Additionally, Transmission Electron Microscopy images of the BFO80-CFO20 sample highlighted the evolution of core-shell structures. Our findings indicate that higher CFO concentrations significantly affect the dielectric, ferroelectric, and optical properties. The bandgaps of the nanocomposites BFO80-CFO20 and BFO50-CFO50 were estimated to be 1.43 eV and 1.39 eV, respectively. Magnetic analysis showed increases in both saturation magnetization and remanent magnetization with increased CFO content, while the coercive field followed a different trend. The saturation magnetization values for the samples BFO, BFO80-CFO20, BFO50-CFO50, and CFO were calculated as 0.205, 14.612, 28.374, and 74.105 (emugr), respectively. The measured values for the same samples were 0.08, 5.07, 11.34, and 34.01 (emugr), respectively. Further, the electrochemical properties were thoroughly investigated using cyclic voltammetry, linear sweep voltammetry, and electrochemical impedance spectroscopy.

Electromagnetic porous lignocellulosic matrix composites: A green electromagnetic shielding material with high absorption efficient electromagnetic interference

Electromagnetic interference (EMI) shielding materials play a vital role in human society, especially in light of the rapid development of electronic communication equipment. Therefore, it is urgent to develop green, high-efficiency EMI shielding materials. Wood, as a renewable raw material, possesses significant structural advantages in studying EMI materials due to its unique 3D pore structure. Herein, we report magnetoelectric lignocellulosic matrix composites derived from the delignified wood for efficient EMI shielding. The composite was fabricated by in-situ polymerization of PEDOT conductive coating and magnetic Fe3O4 in delignified wood. The conductive 3D pore structure of Fe3O4/PEDOT@wood could effectively cause dielectric loss and multiple internal reflections. Combined with the magnetic loss of Fe3O4, the material exhibited excellent EMI shielding effectiveness (SE), which could be attributed to the synergistic effect of dielectric and magnetic losses. The Fe3O4/PEDOT@wood showed excellent conductivity (103 S/m), good magnetism (26.7 emu/g), the EMI SE up to 59.8 dB, and high SEA/SET ratios of∼84.2 % to 95.7 % at 2 mm in X -band. Moreover, the material exhibited a high compressive strength and tensile strength of 100.8 MPa and 18.1 MPa, respectively. Therefore, this work provided a reference for the preparation of high-efficiency EMI shielding materials.

Multilayered magnetoelectric composites for precise and wide-range current sensing

Multilayered magnetoelectric composites for precise and wide-range current sensing

Resonance behaviour of magnetoelectric (PSLZT multilayer - NZFO) layered composites: A comprehensive theory – Experimental perspective

In recent years, compact antenna and miniaturized power transfer devices are among the interesting applications of magnetoelectric (ME) composites in low frequency (LF) / very low frequency (VLF) range. Here we elucidate, in general, analytical calculations used to understand, the vibrational modes and resonance frequencies of the layered ME composite and; Finite Element Analyses (FEM) with isotropic and anisotropic properties to accurately predict the resonance frequencies pertaining to the axisymmetric and asymmetric mode of vibrations with respect to significant ME response. Further, ME coefficient of the composite with Longitudinal - Transverse (L-T) configuration based on the interface coupling model were utilized to completely study the ME composites. The configuration optimized through the design was in particular corroborated experimentally with a representative PSLZT multilayer on NZFO based ME layered composite system. The PSLZT multilayer on NZFO based ME composite was fabricated by tape casting the constituent thick films and co-sintering process which are further analysed for their ME responses at their resonance frequencies. ME voltage spectrum showed a maximum of 7.74 V/cm.Oe at its axisymmetric resonance mode at 30.6 kHz. Various peaks at different resonance frequencies with respect to axisymmetric and asymmetric modes of vibrations agree well and validates the above modeling studies. Overall, the complete study provides a systematic design guideline for optimizing the ME composite configuration suitable for specific application with required resonance frequency.

Harnessing the Induced Magnetostrictive Effect in Fully Flexible Fiber-Based Magnetoelectric Composites for Improved Stray Magnetic Energy Harvesting

Harnessing the Induced Magnetostrictive Effect in Fully Flexible Fiber-Based Magnetoelectric Composites for Improved Stray Magnetic Energy Harvesting

Designing Multifunctional Multiferroic Composites for Advanced Electronic Applications

This paper presents a novel approach for the fabrication of magnetoelectric composites aimed at enhancing cross-coupling between electrical and magnetic phases for potential applications in intelligent sensors and electronic components. Unlike previous methodologies known for their complexity and expense, our method offers a simple and cost-effective assembly process conducted at room temperature, preserving the original properties of the components and avoiding undesired phases. The composites, composed of PZT fibers, cobalt (CoFe2O4), and a polymeric resin, demonstrate the uniform distribution of PZT-5A fibers within the cobalt matrix, as demonstrated by scanning electron microscopy. Detailed morphological analyses reveal the interface characteristics crucial for determining overall performance. Dielectric measurements indicate stable behaviors, particularly when PZT-5A fibers are properly poled, showcasing potential applications in sensors or medical devices. Furthermore, H-dependence studies illustrate strong magnetoelectric interactions, suggesting promising avenues for enhancing coupling efficiency. Overall, this study lays the basic work for future optimization of composite composition and exploration of its long-term stability, offering valuable insights into the potential applications of magnetoelectric composites in various technological domains.

The Elaborate Design of Multi‐Polarization Effect by Non‐Edge Defect Strategy for Ultra‐Broad Microwave Absorption

AbstractAnion defect engineering is proven to be an efficient approach to reconstruct the electronic configuration of carbon‐based magnetoelectric materials for targeted modulation of electromagnetic (EM) performance. However, traditional mono‐anionic doping suffers from low defect concentration and lacks diverse polarization mechanisms. In this work, multi‐anions (N/S/F) stepwise‐doped carbon/Fe3C magnetoelectric composites are elaborately constructed, wherein the predesigned N defects serve as activated sites for anomalously adopting S anions (Step I) and subsequent F anions (Step II) in non‐marginal areas of the carbon layer. It is found that S prefers to replace pyrrolic N defects while F tends to form dangling bonds with the C site adjacent to the pyridinic N. Intriguingly, besides the inherent polarized resonance of N defect at ≈15 GHz, customized S and F defects induce new polarization resonances at ≈10 GHz and ≈15+ GHz, respectively. Under a typical multi‐polarization effect with the synergetic magnetic response, the carbon/Fe3C composites with N/S/F defects harvest the broadest bandwidth of 8.28 GHz (9.72–18 GHz) at 2.55 mm, covering a wide frequency range almost from X to Ku bands. This work demonstrates the positive impact of localized multi‐defects customization and multi‐polarization effect on expanding microwave absorption bandwidth, providing valuable insights for the advanced design of ultra‐broadband absorbers.

Leveraging the strain transfer at the interface between self-composite CoFe2O4 embedded in pre-sintered Na0.5Bi0.5TiO3 ceramics matrix for the enhancement of magnetoelectric voltage coefficient

Magnetoelectric particulate composite (100-x) NBT- xCFO(sc) (x = 5,15,25,35) were prepared from pre-sintered NBT and self-composite CFO(sc) by solid-state reaction route. XRD, SEM, and Raman studies confirm the biphasic composite formation without diffusion at the interfaces. Unsaturated ferroelectric loops and enhanced ferromagnetic properties are evidenced. ME coefficient value is enhanced to 25.1 mV cm−1 Oe in the N65SC35 composite which is the greatest among the reported values in the literature of NBT-CFO composites. The enhancement is due to the effective strain transfer at the interfaces of the composites. This is explained by a simple dimensionless quantity, degree of interface. This quantity is defined using the interface length of ferroelectric-ferromagnetic phases and the weighted average grain size which corroborates the enhancement of the ME coefficient.

Dielectric and Magnetoelectric Properties of TGS-Magnetite Composite.

In our studies, we combined two powdered materials, i.e., ferroelectric triglycine sulfate (TGS) and ferrimagnetic magnetite Fe3O4, 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 + Fe3O4 powder. The magnetoelectric coupling presumably appeared for the composite TGS + 10 wt. % Fe3O4, as evidenced by the shift in the phase transition temperature in the TGS. Moreover, the theoretical interpretation of the effect is proposed.

Performance analysis of acoustically actuated magnetoelectric antennas via equivalent circuit method

Acoustically actuated magnetoelectric (ME) antennas based on resonant magnetoelectric coupling within ferromagnetic/piezoelectric ME laminated composites have recently been considered as a promising solution for antenna miniaturization. However, its radiation performance has been theoretically overestimated, since the negative effects on performances due to the magnetization saturation and the nonlinear mechanical behavior that occur from high-field driving have not been paid enough attention. This work presents a unique equivalent-circuit-based numerical method to analyze the near-field resonance radiation performances of ME antennas driven by high electric fields. In this method, we establish an equivalent circuit of the converse magnetoelectric effect for a ME laminated composite to describe the operating principle of acoustically actuated electromagnetic radiation. The equivalent parameters related to resonance characteristics are determined by fitting the circuit model to the data from frequency response measurements of the near-field magnetic flux density. The validity of the model is verified by comparing the theoretical predictions with the experimental results, in the view of the volume fraction dependence of the mechanical resonance-related radiation characteristics of the fabricated ME composites. Based on the proposed model, the influence of driving voltage amplitude on near-field radiation performances is further analyzed by experimental fitting to the model, and the potential limiting factors of ME antennas are discussed according to the driving-amplitude dependence of parameters obtained from the fit. This work provides an effective and engineering-friendly approach to predict the evolution of ME antenna performances, leading a way to improve the performance limit for resonant magnetoelectric coupling.

Enhanced piezoelectricity of P(VDF-TrFE) by BN nanosheets doping and leading to high performance laminated magnetoelectric composites

With the development trend of miniaturization, lightweight and portability of electronic equipment, piezoelectric devices have been widely applied to transducers, sensors and energy harvesters. Piezoelectric polymers, like poly(vinylidene fluoride-trifluoroethylene) (P(VDF-TrFE)), possess the advantages of light weight, good flexibility, and simple preparation methods. However, P(VDF-TrFE) films is not entirely composed of piezoelectric phase (β phase), so increasing the content of β-phase is very important for the piezoelectric property of P(VDF-TrFE) films. Doping nanomaterials with unique properties has been proved to be a feasible way to increase the content of β-phase. In this paper, hexagonal boron nitride (h-BN) nanosheets, a kind of 2-dimensional van der Waals materials with wide bandgap, as filler were doping into poly(vinylidene fluoride-trifluoroethylene) (P(VDF-TrFE)) piezoelectric films by solution casting method. The composite films as designed, in which h-BN nanosheets were uniformly dispersed in P(VDF-TrFE), achieved higher contents of piezoelectric phase (β phase). Compared with pure P(VDF-TrFE) films, the optimal P(VDF-TrFE)/BN piezoelectric film achieved a much higher piezoelectric coefficient (d33) (∼42 pC/N), also leading to a higher piezoelectric voltage output than that of pure P(VDF-TrFE). By laminating the P(VDF-TrFE)/BN films as designed with FeSiB Metglas, high magnetoelectric voltage coefficients under zero and low DC magnetic bias were achieved. In summary, this paper presents a feasible and potential method for improving PVDF piezoelectricity, which has been successfully applied in high performance magnetoelectric devices.