High-Endurance Magneto-Electronic Switchable Molecular Electronic Crystal.

Electrically switchable magnetic and electronic properties are promising for quantum sensing and information technology. Here, we report an electrically driven magnetic and electronic phase transition in molecular electronic crystal, potassium-7,7,8,8-tetracyanoquinodimethan, with the magneto-electric switching over 105 cycles at room temperature. Electron spin resonance study reveals the cooperative transition between spin and charge degrees of freedom. In addition, the mechanistic spectroscopy studies suggest the charges in an inhomogeneous conductor-insulator mixed state. The findings shown here suggest electrically controlled ordering in strongly correlated molecular crystal leads to dynamic magneto-electric switching, paving the way for developing molecular-based memory and switching devices.

Reversible Switchability of Magnetic Anisotropy and Magnetodielectric Effect Induced by Intermolecular Motion.

Introducing magnetic switchability into artificial molecular machines is fascinating for precise control of magnetism via external stimuli. Herein, a field-induced CoII single-molecule magnet was found to exhibit the reversible switch of Jahn-Teller distortion near room temperature, along with thermal conformational motion of the 18-crown-6 rotor, which pulls the coordinated H2 O to rotate through intermolecular hydrogen bonds and triggers a single-crystal-to-single-crystal phase transition with Twarm =282 K and Tcool =276 K. Interestingly, the molecular magnetic anisotropy probed by single-crystal angular-resolved magnetometry revealed the reorientation of easy axis by 14.6°. Moreover, ON/OFF negative magnetodielectric effects were respectively observed in the high-/low-temperature phase, which manifests the spin-lattice interaction in the high-temperature phase could be stronger, in accompanied by the hydrogen bonding between the rotating 18-crown-6 and the coordinated H2 O.

The Mechanism of the Magnetodielectric Response in a Molecule-Based Trinuclear Iron Cluster Material.

Magnetodielectric response mechanisms are critical for the rational design and synthesis of molecule-based magnetodielectric materials. Herein, the magnetodielectric response was investigated in the molecule-based material [Fe3 O(CH3 COO)6 (py)3 ](py) (1). Its magnetodielectric coefficient (MD) is -2.8 % for phase transition III and -4.1 % for phase transition I. Study of the mechanism of the magnetodielectric response in 1 reveals that its magnetodielectric response at phase transition I is induced by the charge-frustration of the trinuclear iron cluster, while that at phase transition III is attributed to the spin-frustration of the trinuclear iron cluster, providing a new route for the design of magnetodielectric materials.

Miniaturized Multi-Port Microstrip Patch Antenna Using Metamaterial for Passive UHF RFID-Tag Sensor Applications.

In this paper, a miniaturized Ultra High Frequency Radio Frequency Identification (UHF-RFID) tag-based sensor antenna using a magneto- dielectric substrate (MDS) for wireless identification and sensor applications is presented. Two models of RFID tag-based sensors are designed, fabricated and measured. The first model uses two RFID tags; both of the tags are incorporated with two RFID chips. A passive sensor is also integrated in one of the proposed tags to serve as a sensor node, while the other tag is used as a reference node. Based on the difference in the minimum power required to activate the reference and sensor nodes, the sensed data (temperature or humidity) can be determined. The magneto-dielectric substrate layer is placed underneath the patch antenna to reduce the size of the proposed sensor by about 75% compared to a conventional RFID tag-based sensor. The magneto-dielectric layer is thin enough to embed in the planer circuit. To reduce the size of the proposed sensor, a multi-port tag for including the reference and sensor node in one antenna is also presented. The proposed RFID tag-based sensors have several features such as small size, they are completely capable for two objectives at the same time and easy to integrate with a planer circuit.

Magnetic Field Sensing by Exploiting Giant Nonstrain-Mediated Magnetodielectric Response in Epitaxial Composites.

Heteroepitaxial magnetoelectric (ME) composites are promising for the development of a new generation of multifunctional devices, such as sensors, tunable electronics, and energy harvesters. However, challenge remains in realizing practical epitaxial composite materials, mainly due to the interfacial lattice misfit strain between magnetostrictive and piezoelectric phases and strong substrate clamping that reduces the strain-mediated ME coupling. Here, we demonstrate a nonstrain-mediated ME coupling in PbZr0.52Ti0.48O3 (PZT)/La0.67Sr0.33MnO3 (LSMO) heteroepitaxial composites that resolves these challenges, thereby, providing a giant magnetodielectric (MD) response of ∼27% at 310 K. The factors driving the magnitude of the MD response were found to be the magnetoresistance-coupled dielectric dispersion and piezoelectric strain-mediated modulation of magnetic moment. Building upon this giant MD response, we demonstrate a magnetic field sensor architecture exhibiting a high sensitivity of 54.7 pF/T and desirable linearity with respect to the applied external magnetic field. The demonstrated technique provides a new mechanism for detecting magnetic fields based upon the MD effect.

Simulation of Magnetodielectric Effect in Magnetorheological Elastomers.

We present the results of numerical simulation of magnetodielectric effect (MDE) in magnetorheological elastomers (MRE)-the change of effective permittivity of elastomer placed under the external magnetic field. The computer model of effect is based on an assumption about the displacement of magnetic particles inside the elastic matrix under the external magnetic field and the formation of chain-like structures. Such displacement of metallic particles between the planes of capacitor leads to the change of capacity, which can be considered as a change of effective permittivity of elastomer caused by magnetic field (magnetodielectric effect). In the literature, mainly the 2D approach is used to model similar effects. In this paper, we present a new approach of magnetorheological elastomers simulation-a 3D-model of the magnetodielectric effect with ability to simulate systems of 10 5 particles. Within the framework of the model, three types of particle size distributions were simulated, which gives an advantage over previously reported approaches. Lognormal size distribution was shown to give better qualitative match of the modeling and experimental results than monosized type. The developed model resulted in a good qualitative agreement with all experimental data obtained earlier for Fe-based elastomers. The proposed model is useful to study these novel functional materials, analyze the features of magnetodielectric effect and predict the optimal composition of magnetorheological elastomers for further profound experimental study.

Magnetodielectric Response of Soft Magnetoactive Elastomers: Effects of Filler Concentration and Measurement Frequency.

The magnetodielectric response of magnetoactive elastomers (MAEs) in its dependence on filler concentration, magnetic field, and test frequency is studied experimentally. MAEs are synthesized on the basis of a silicone matrix filled with spherical carbonyl iron particles characterized by a mean diameter of 4.5 µm. The concentration of the magnetic filler within composite materials is equal to 70, 75, and 80 mass%. The effective lossless permittivity ε' as well as the dielectric loss tanδ grow significantly when the magnetic field increases. The permittivity increases and the dielectric loss decreases with increasing filler concentration. In the measurement frequency range between 1 kHz and 200 kHz, the frequency hardly affects the values of ε' and tanδ in the absence of a magnetic field. However, both parameters decrease considerably with the growing frequency in a constant magnetic field. The more strongly the magnetic field is applied, the larger the change in permittivity and loss tangent at the same test frequency is observed. An equivalent circuit formulation qualitatively describes the main tendencies of the magnetodielectric response.

Magnetorheological Hybrid Elastomers Based on Silicone Rubber and Magnetorheological Suspensions with Graphene Nanoparticles: Effects of the Magnetic Field on the Relative Dielectric Permittivity and Electric Conductivity.

Hybrid magnetorheological elastomers (hMREs) were manufactured based on silicone rubber, silicone oil, carbonyl iron microparticles, graphene nanoparticles and cotton fabric. Using the hMREs, flat capacitors (FCs) were made. Using the installation described in this paper, the electrical capacitance and the coefficient of dielectric losses of the hMREs were measured as a function of the intensity of the magnetic field superimposed over an alternating electric field. From the data obtained, the electrical conductivity, the relative dielectric permittivity and magnetodielectric effects are determined. It is observed that the obtained quantities are significantly influenced by the intensity of the magnetic field and the amount of graphene used.

Magneto-Dielectric Synergy and Multiscale Hierarchical Structure Design Enable Flexible Multipurpose Microwave Absorption and Infrared Stealth Compatibility.

Developing advanced stealth devices to cope with radar-infrared (IR) fusion detection and diverse application scenarios is increasingly demanded, which faces significant challenges due to conflicting microwave and IR cloaking mechanisms and functional integration limitations. Here, we propose a multiscale hierarchical structure design, integrating wrinkled MXene IR shielding layer and flexible Fe3O4@C/PDMS microwave absorption layer. The top wrinkled MXene layer induces the intensive diffuse reflection effect, shielding IR radiation signals while allowing microwave to pass through. Meanwhile, the permeable microwaves are assimilated into the bottom Fe3O4@C/PDMS layer via strong magneto-electric synergy. Through theoretical and experimental optimization, the assembled stealth devices realize a near-perfect stealth capability in both X-band (8-12 GHz) and long-wave infrared (8-14 µm) wavelength ranges. Specifically, it delivers a radar cross-section reduction of - 20 dB m2, a large apparent temperature modulation range (ΔT = 70 °C), and a low average IR emissivity of 0.35. Additionally, the optimal device demonstrates exceptional curved surface conformability, self-cleaning capability (contact angle ≈ 129°), and abrasion resistance (recovery time ≈ 5 s). This design strategy promotes the development of multispectral stealth technology and reinforces its applicability and durability in complex and hostile environments.

Magnetodielectric Effect in a Triangular Dysprosium Single-Molecule Toroics.

Single-molecule toroics are molecular magnets with vortex distribution of magnetic moments. The coupling between magnetic and electric properties such as the magnetodielectric effect will provide potential applications for them. Herein, the observation of significant magnetodielectric effect in a triangular Dy3 crystal with toroidal magnetic moment and multiple magnetic relaxations is reported. The analysis of magnetic and electric properties implies that the magnetodielectric effect is closely related to the strong spin-lattice coupling, magnetic interactions of Dy3+ ions, as well as molecular packing models.

Magnetodielectric and Rheological Effects in Magnetorheological Suspensions Based on Lard, Gelatin and Carbonyl Iron Microparticles.

This study aims to develop low-cost, eco-friendly, and circular economy-compliant composite materials by creating three types of magnetorheological suspensions (MRSs) utilizing lard, carbonyl iron (CI) microparticles, and varying quantities of gelatin particles (GP). These MRSs serve as dielectric materials in cylindrical cells used to fabricate electric capacitors. The equivalent electrical capacitance (C) of these capacitors is measured under different magnetic flux densities (B≤160 mT) superimposed on a medium-frequency electric field (f = 1 kHz) over a period of 120 s. The results indicate that at high values of B, increasing the GP content to 20 vol.% decreases the capacitance C up to about one order of magnitude compared to MRS without GP. From the measured data, the average values of capacitance Cm are derived, enabling the calculation of relative dielectric permittivities (ϵr') and the dynamic viscosities (η) of the MRSs. It is demonstrated that ϵr' and η can be adjusted by modifying the MRS composition and fine-tuned through the magnetic flux density B. A theoretical model based on the theory of dipolar approximations is used to show that ϵr', η, and the magnetodielectric effect can be coarsely adjusted through the composition of MRSs and finely adjusted through the values B of the magnetic flux density. The ability to fine-tune these properties highlights the versatility of these materials, making them suitable for applications in various industries, including electronics, automotive, and aerospace.

Dynamics of magnetic inhomogeneity in La2CoMnO6 films probed by Raman spectroscopy.

We report the dynamic effects of magnetic inhomogeneity on the temperature evolution of the Raman modes in polycrystalline La2CoMnO6 (LCMO) films. The LCMO films were obtained via chemical solution deposition and annealed at different temperatures, 700, 800 and 900 °C. Temperature-dependent Raman spectroscopic studies uncover anomalous phonon energy behaviors, associated with strong spin-phonon couplings revealed even at ambient conditions. This effect, which is observed to occur well above ferromagnetic ordering temperature is ascribed to short-range Mn4+/Co2+ ferromagnetic clusters. Moreover, our study has shown that spin-phonon coupling strength is governed by competing antiferromagnetic (AFM) and ferromagnetic (FM) interactions. These results significantly enhance the understanding of the complex spin-phonon coupling mechanism to provide insights into magnetic inhomogeneity in systems with two or more magnetic sublattices. These findings suggest the presence of similar effects in other double perovskites within the RE2CoMnO6 (RE = rare earths) family, which exhibit analogous magnetic sublattice and order-disorder defects.

Theoretical Study of the Multiferroic Properties of Pure and Ion-Doped Pb5M3F19, M = Fe, Cr, Al.

In a first theoretical investigation of the multiferroic properties of Pb5Fe3F19 (PFF) and Pb5Cr3F19 (PCF), we analyze their magnetic, ferroelectric, and dielectric characteristics as functions of temperature, magnetic field, and ion doping concentration using a microscopic model and Green's function theory. The temperature-dependent polarization in PFF and PCF shows a distinctive kink at the magnetic Neel temperature TN, which vanishes when an external magnetic field is applied, indicating the multiferroic behavior of these two compounds. Ion doping effectively tunes the properties of PFF and PCF. In PFF, Cr ion doping leads to a decrease in the Neel temperature TN, while Cr and Al ion doping lowers the ferroelectric Curie temperature TC. In the case of PCF, we observe the enhancement of TC by Fe ion doping and the reduction by Al ion doping. The last result coincides well quantitatively with the experimental data. Additionally, the magnetodielectric coefficient of PFF is enhanced with the increasing magnetic field.

Improvement of leakage, magnetic and magnetodielectric properties in cobalt doped gallium ferrite.

Gallium ferrite (GFO) is a magnetoelectric (ME) material, capturing growing attention due to its strong ME coupling at room temperature. However, the application of the material in practical use is hindered due to its high leakage. In this work, the effects of cobalt (Co) substitution at the iron (Fe) sites of GaFe1-xCoxO3(0.0 ⩽x⩽ 0.1) polycrystals on the structure, electric and magnetic properties are investigated in detail. 5 at. wt.% substitution (x= 0.05) with cobalt ions achieves a reduction in leakage current density by four orders of magnitude due to reduced hopping between Fe3+and Fe2+ions and suppression of the oxygen vacancy formation. This is supported by higher dielectric constant and lower dielectric loss, as well as a significant difference between grain and grain boundary resistances. Two-phase-like magnetic behavior in magnetic hysteresis loop with enhanced magnetization and two magnetic transition temperatures are observed in the doped samples. All samples exhibited an increase in the magnetodielectric factor, indicating enhanced coupling between magnetic and electrical parameters. By concurrently increasing dielectric, magnetic, and coupling between them, this study describes a viable technique for lowering the most significant impediment to GFO's usage as a ME device.

Magnetodielectric Properties of Ordered Microstructured Polydimethylsiloxane-Based Magnetorheological Elastomer with Fe3O4@rGO Nanoparticles.

Magnetodielectric properties of prepared ordered microstructured polydimethylsiloxane-based magnetorheological elastomer with the Fe3O4@rGO (Fe3O4@rGO/PDMS-MRE) were investigated to expand the application of magnetorheological elastomer (MRE) in magnetic sensing fields by improving the magnetodielectric effect. Five types of Fe3O4@rGO electromagnetic biphasic composite particles were synthesized by the solvothermal method, and their characterization and magnetic properties were also tested. Microstructurally ordered Fe3O4@rGO/PDMS-MRE samples with different Fe3O4@rGO concentrations were obtained through the magnetic field orientation technique, an experimental platform for magnetodielectric properties was built, and the relative permittivity of the samples was tested under magnetic flux density from 0 to 500 mT. The results show when the ratio of modified Fe3O4 to GO reaches 10:1, the Fe3O4@rGO composite particles exhibit uniform distribution with a flaky structure and strong magnetic properties and have the best bonding effect of composite particles. The relative permittivity of Fe3O4@rGO/PDMS-MRE increases with the rise of Fe3O4@rGO concentration and applied magnetic flux density. The relative permittivity of Fe3O4@rGO/PDMS-MRE with Fe3O4@rGO concentration of 60 wt% reaches 12.934 under the action of 500 mT magnetic flux density, and the magnetodielectric effect is as high as 92.4%. A reasonable mechanism for improving the magnetodielectric effect of ordered microstructured Fe3O4@rGO/PDMS-MRE is proposed.

Large magnetodielectric coupling in the vicinity of metamagnetic transition in 6H-perovskite Ba3GdRu2O9.

The 6H-perovskites Ba3RRu2O9(R = rare earth element) demonstrate the magnetodielectric (MD) coupling as a manifestation of 4d-4fmagnetic interactions. Here, a detailed study of the structural, magnetic, heat capacity, and MD properties of the 6H-perovskite Ba3GdRu2O9is reported. The signature of long-range antiferromagnetic (AFM) ordering ∼14.8 K (TN) is evident from the magnetization and heat capacity studies. TheTNshifts towards the lower temperature side, apart from splitting in two with the application of the magnetic field. Field-dependent magnetization at 2 K shows three metamagnetic transitions with the opening of small hysteresis in different regions. A new transition atT1emerges after the onset of the first metamagnetic transition. Complex magnetic behavior is observed in different magnetic field regions whereas these field regions themselves vary with the temperature. Dielectric response recorded at zero and 80 kOe field exhibits the development of MD coupling well aboveTN. The MD coupling (∼4.5% at 10 K) is enhanced by 25% as compared to the Dy counterpart. Effect of complex magnetic behavior is also conveyed in the MD results where the maximum value of MD coupling is observed in the vicinity of 10 K (onset ofT1) and near the second metamagnetic transition. Our investigation suggests that both Gd and Ru moments align simultaneously atTN. Short-range magnetic ordering is possibly responsible for MD coupling aboveTN.

Multiferroic and Magnetodielectric Effects in Multiferroic Pr2FeAlO6 Double Perovskite.

Single-phase multiferroics that allow the coexistence of ferroelectric and magnetic ordering above room temperature are highly desirable, and offer a fundamental platform for novel functionality. In this work, a double perovskite multiferroic Pr2FeAlO6 ceramic is prepared using a sol-gel process followed by a quenching treatment. The well-crystallized and purified Pr2FeAlO6 in trigonal structure with space group R3c is confirmed. A combination of the ferroelectric (2Pr = 0.84 µC/cm2, Ec = 7.78 kV/cm at an applied electric field of 20 kV/cm) and magnetic (2Mr = 433 memu/g, Hc = 3.3 kOe at an applied magnetic field of 1.0 T) hysteresis loops reveals the room-temperature multiferroic properties. Further, the magnetoelectric effect is observed from the measurements of magnetically induced dielectric response and polarization. The present results suggest a new complex oxide candidate for room-temperature multiferroic applications.

Structure driven magnetic correlations and magnetodielectric coupling in 6H-perovskite Ba3DyRu2O9.

The 6H-perovskites Ba3(R/M)Ru2O9(R= rare Earth,M= transition metal) exhibit complex magnetism and have been extensively studied recently for their magnetodielectric (MD) properties. Here, we present a detailed study of structural, magnetic, thermodynamic and MD properties of a 6H-perovskite Ba3DyRu2O9. This compound is found to undergo long range antiferromagnetic ordering below ∼5.8 K (TN), along with the presence of metamagnetic transition at low temperatures. The heat capacity shows two additional anomalies at ∼28 K (T1) and ∼33 K (T2), besides the anomaly atTN. Signature of these anomalies is also visible in the derivative of magnetization curve. The dielectric response also shows weak anomalies aroundT1andT2at zero field whereas anomaly atT2gets suppressed at 80 kOe. The observed MD coupling of ∼2%-4% at 80 kOe field below ∼30 K temperature range, is among the highest values observed for the compounds of this family. Low temperature crystal structures of the compound show sharp distortion of Ru2O9octahedra nearT2. Our study points toward the emergence of structurally driven spin correlations of Ru moments resulting in the observed MD coupling in this compound.

Inorganic-Organic Hybrid Molecular Materials: From Multiferroic to Magnetoelectric.

Inorganic-organic hybrid molecular multiferroic and magnetoelectric materials, similar to multiferroic oxide compounds, have recently attracted increasing attention because they exhibit diverse architectures, a flexible framework, fascinating physics, and potential magnetoelectric functionalities in novel multifunctional devices such as energy transformation devices, sensors, and information storage systems. Herein, the classification of multiferroicity and magnetoelectricity is briefly outlined and then the recent advances in the multiferroicity and magnetoelectricity of inorganic-organic hybrid molecular materials, particularly magnetoelectricity and the relevant magnetoelectric mechanisms and their categories are summarized. In addition, a personal perspective and an outlook are provided.

Dielectric Spectroscopy of Hybrid Magnetoactive Elastomers.

Dielectric properties of two series of magnetoactive elastomers (MAEs) based on a soft silicone matrix containing 35 vol% of magnetic particles were studied experimentally in a wide temperature range. In the first series, a hybrid filler representing a mixture of magnetically hard NdFeB particles of irregular shape and an average size of 50 µm and magnetically soft carbonyl iron (CI) of 4.5 µm in diameter was used for MAE fabrication. MAEs of the second series contained only NdFeB particles. The presence of magnetically hard NdFeB filler made it possible to passively control MAE dielectric response by magnetizing the samples. It was shown that although the hopping mechanism of MAEs conductivity did not change upon magnetization, a significant component of DC conductivity appeared in the magnetized MAEs presumably due to denser clustering of interacting particles resulting in decreasing interparticle distances. The transition from a non-conducting to a conducting state was more pronounced for hybrid MAEs containing both NdFeB and Fe particles with a tenfold size mismatch. Hybrid MAEs also demonstrated a considerable increase in the real part of the complex relative permittivity upon magnetization and its asymmetric behavior in external magnetic fields of various directions. The effects of magnetic filler composition and magnetization field on the dielectric properties of MAEs are important for practical applications of MAEs as elements with a tunable dielectric response.