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Composites of ferromagnetic and ferroelectric phases are of interest for studies on mechanical strain-mediated coupling between the two phases and for a variety of applications in sensors, energy harvesting, and high-frequency devices. Nanocomposites are of particular importance since their surface area-to-volume ratio, a key factor that determines the strength of magneto-electric (ME) coupling, is much higher than for bulk or thin-film composites. Core–shell nano- and microcomposites of the ferroic phases are the preferred structures, since they are free of any clamping due to substrates that are present in nanobilayers or nanopillars on a substrate. This review concerns recent efforts on ME coupling in coaxial fibers of spinel or hexagonal ferrites for the magnetic phase and PZT or barium titanate for the ferroelectric phase. Several recent studies on the synthesis and ME measurements of fibers with nickel ferrite, nickel zinc ferrite, or cobalt ferrite for the spinel ferrite and M-, Y-, and W-types for the hexagonal ferrites were considered. Fibers synthesized by electrospinning were found to be free of impurity phases and had uniform core and shell structures. Piezo force microscopy (PFM) and scanning microwave microscopy (SMM) measurements of strengths of direct and converse ME effects on individual fibers showed evidence for strong coupling. Results of low-frequency ME voltage coefficient and magneto-dielectric effects on 2D and 3D films of the fibers assembled in a magnetic field, however, were indicative of ME couplings that were weaker than in bulk or thick-film composites. A strong ME interaction was only evident from data on magnetic field-induced variations in the remnant ferroelectric polarization in the discs of the fibers. Follow-up efforts aimed at further enhancement in the strengths of ME coupling in core–shell composites are also discussed in this review. 

This report is on Co and Ti substituted M-type barium and strontium hexagonal ferrites that are reported to be single phase multiferroics due to a transition from Neel type ferrimagnetic order to a spiral spin structure that is accompanied by a ferroelectric polarization in an applied magnetic field. The focus here is the nature of magnetoelectric (ME) interactions in the bilayers of ferroelectric PZT and Co and Ti substituted BaM and SrM. The ME coupling in the ferrite-PZT bilayers arise due to the transfer of magnetostriction-induced mechanical deformation in a magnetic field in the ferrite resulting in an induced electric field in PZT. Polycrystalline Co and Ti doped ferrites, Ba (CoTi)x Fe12−2xO19, (BCTx), and Sr (CoTi)x Fe12−2xO19 (SCTx) (x = 0–4) were found to be free of impurity phases for all x-values except for SCTx, which had a small amount of α-Fe2O3 in the X-ray diffraction patterns for x ≤ 2.0. The magnetostriction for the ferrites increased with applied filed H to a maximum value of around 2 to 6 ppm for H~5 kOe. BCTx/SCTx samples showed ferromagnetic resonance (FMR) for x = 1.5–2.0, and the estimated anisotropy field was on the order of 5 kOe. The magnetization increased with the amount of Co and Ti doping, and it decreased rapidly with x for x > 1.0. Measurements of ME coupling strengths were conducted on the bilayers of BCTx/SCTx platelets bonded to PZT. The bilayer was subjected to an AC and DC magnetic field H, and the magnetoelectric voltage coefficient (MEVC) was measured as a function of H and frequency of the AC field. For BCTx-PZT, the maximum value of MEVC at low frequency was ~5 mV/cm Oe, and a 40-fold increase at electromechanical resonance (EMR). SCTx–PZT composites also showed a similar behavior with the highest MEVC value of ~14 mV/cm Oe at low frequencies and ~200 mV/cm Oe at EMR. All the bilayers showed ME coupling for zero magnetic bias due to the magnetocrystalline anisotropy field in the ferrite that provided a built-in bias field. 

This report is on experiments and theory on the process of optically stimulated electron population density redistribution in Si-substituted yttrium-iron garnet single crystals at 77 K. It was determined that a photo-induced uniaxial anisotropy field arose in the YIG:Si sample in response to illumination by quasi-linearly polarized laser (λ = 808 nm) leading to redistribution of Fe2+ ions among the nonequivalent octahedral sites. The photo-induced field was measured by variation of ferromagnetic resonance (FMR) frequencies in the X-band. The measured FMR frequency shift demonstrated a pronounced dependence on the polarization vector orientation with respect to crystallographic axes, in accordance with the theory discussed here. The frequency shift dependence on light intensity (for optimal polarization orientation) was found to be nearly linear, at least within the output intensity range of the optical source. The maximum frequency shift was −130 MHz for 75 mW applied optical power. A similar phenomenon was also observed at room temperature but was attributed to the sample heating by the incident light. The results presented here demonstrate the potential of the phenomenon for application in the development of ferrite signal processing devices with dual tuning by both magnetic field and optical irradiation. 

This report is on magneto-electric (ME) interactions in bulk composites with coaxial fibers of nickel–zinc ferrite and PZT. The core–shell fibers of PZT and Ni1−xZnxFe2O4 (NZFO) with x = 0–0.5 were made by electrospinning. Both kinds of fibers, either with ferrite or PZT core and with diameters in the range of 1–3 μm were made. Electron and scanning probe microscopy images indicated well-formed fibers with uniform core and shell structures and defect-free interface. X-ray diffraction data for the fibers annealed at 700–900 °C did not show any impurity phases. Magnetization, magnetostriction, ferromagnetic resonance, and polarization P versus electric field E measurements confirmed the ferroic nature of the fibers. For ME measurements, the fibers were pressed into disks and rectangular platelets and then annealed at 900–1000 °C for densification. The strengths of strain-mediated ME coupling were measured by the H-induced changes in remnant polarization Pr and by low-frequency ME voltage coefficient (MEVC). The fractional change in Pr under H increased in magnitude, from +3% for disks of NFO–PZT to −82% for NZFO (x = 0.3)-PZT, and a further increase in x resulted in a decrease to a value of −3% for x = 0.5. The low-frequency MEVC measured in disks of the core–shell fibers ranged from 6 mV/cm Oe to 37 mV/cm Oe. The fractional changes in Pr and the MEVC values were an order of magnitude higher than for bulk samples containing mixed fibers with a random distribution of NZFO and PZT. The bulk composites with coaxial fibers have the potential for use as magnetic field sensors and in energy-harvesting applications. 

In the present work, we have synthesized rare-earth ion modified Bi4−xRExTi2Fe0.7Co0.3O12−δ (RE = Dy, Sm, La) multiferroic compounds by the conventional solid-state route. Analysis of X-ray diffraction by Rietveld refinement confirmed the formation of a polycrystalline orthorhombic phase. The morphological features revealed a non-uniform, randomly oriented, plate-like grain structure. The peaks evident in the Raman spectra closely corresponded to those of orthorhombic Aurivillius phases. Dielectric studies and impedance measurements were carried out. Asymmetric complex impedance spectra suggested the relaxation of charge carriers belonging to the non-Debye type and controlled by a thermally activated process. Temperature-dependent AC conductivity data showed a change of slope in the vicinity of the phase transition temperature of both magnetic and electrical coupling natures. Based on the universal law and its exponent nature, one can suppose that the conduction process is governed by a small polaron hopping mechanism but significant distortion of TiO6 octahedral. The doping of the A-sites with rare-earth element ions and changes in the concentrations of Fe and Co ions located on the B-sites manifested themselves in saturated magnetic hysteresis loops, indicating competitive interactions between ferroelectric and canted antiferromagnetic spins. The magnetic order in the samples is attributed to pair-wise interactions between adjacent Fe3+–O–Fe3+, Co2+/3+–O–Co3+/2+, and Co2+/3+–O–Fe3+ ions or Dzyaloshinskii–Moriya interactions among magnetic ions in the adjacent sub-lattices. As a result, enhanced magnetoelectric coefficients of 42.4 mV/cm-Oe, 30.3 mV/cm-Oe, and 21.6 mV/cm-Oe for Bi4−xDyxTi2Fe0.7Co0.3O12−δ (DBTFC), Bi4−xLaxTi2Fe0.7Co0.3O12−δ (LBTFC), and Bi4−xSmxTi2Fe0.7Co0.3O12−δ (SBTFC), respectively, have been obtained at lower magnetic fields (<3 kOe). The strong coupling of the Aurivillius compounds observed in this study is beneficial to future multiferroic applications. 

The magnetoelectric effect (ME) is an important strain mediated-phenomenon in a ferromagnetic-piezoelectric composite for a variety of sensors and signal processing devices. A bias magnetic field, in general, is essential to realize a strong ME coupling in most composites. Magnetic phases with (i) high magnetostriction for strong piezomagnetic coupling and (ii) large anisotropy field that acts as a built-in bias field are preferred so that miniature, ME composite-based devices can operate without the need for an external magnetic field. We are able to realize such a magnetic phase with a composite of (i) barium hexaferrite (BaM) with high magnetocrystalline anisotropy field and (ii) nickel ferrite (NFO) with high magnetostriction. The BNx composites, with (100 − x) wt.% of BaM and x wt.% NFO, for x = 0–100, were prepared. X-ray diffraction analysis shows that the composites did not contain any impurity phases. Scanning electron microscopy images revealed that, with an increase in NFO content, hexagonal BaM grains become prominent, leading to a large anisotropy field. The room temperature saturation magnetization showed a general increase with increasing BaM content in the composites. NFO rich composites with x ≥ 60 were found to have a large magnetostriction value of around −23 ppm, comparable to pure NFO. The anisotropy field HA of the composites, determined from magnetization and ferromagnetic resonance (FMR) measurements, increased with increasing NFO content and reached a maximum of 7.77 kOe for x = 75. The BNx composite was cut into rectangular platelets and bonded with PZT to form the bilayers. ME voltage coefficient (MEVC) measurements at low frequencies and at mechanical resonance showed strong coupling at zero bias for samples with x ≥ 33. This large in-plane HA acted as a built-in field for strong ME effects under zero external bias in the bilayers. The highest zero-bias MEVC of ~22 mV/cm Oe was obtained for BN75-PZT bilayers wherein BN75 also has the highest HA. The Bilayer of BN95-PZT showed a maximum MEVC ~992 mV/cm Oe at electromechanical resonance at 59 kHz. The use of hexaferrite–spinel ferrite composite to achieve strong zero-bias ME coupling in bilayers with PZT is significant for applications related to energy harvesting, sensors, and high frequency devices. 

Abstract The nature of nonlinear magnetoelectric (NLME) effect has been investigated at room-temperature in a single-crystal Zn substituted nickel ferrite. Tuning of the frequency of magnetostatic surface wave (MSSW) modes under an applied pulsed DC electric field/current has been utilized to probe the effect. The frequencies of the modes at 8–20 GHz were found to decrease by ~ 400 MHz for an applied DC powerPof ~ 100 mW and the frequency shift was the same for all of the MSSW modes and linearly proportional toP. A model is proposed for the effect and the NLME phenomenon was interpreted in terms of a reduction in the saturation magnetization due to the DC current. The decrease of magnetization with applied electric power, estimated from data on mode frequency versusP, was − 2.50 G/mW. The frequency tuning efficiency of the MSSW modes due to NLME effects in the ferrite resonator was found to be 4.1 MHz/mW which is an order of magnitude higher than the shift reported for M-type strontium and barium hexaferrite resonators investigated earlier. The spinel ferrite resonator discussed here has the potential for miniature, electric field tunable, planar microwave devices for the 8–20 GHz frequency range. 

We demonstrate indirect electric-field control of ferromagnetic resonance (FMR) in devices that integrate the low-loss, molecule-based, room-temperature ferrimagnet vanadium tetracyanoethylene (V[TCNE]x∼2) mechanically coupled to PMN-PT piezoelectric transducers. Upon straining the V[TCNE]x films, the FMR frequency is tuned by more than 6 times the resonant linewidth with no change in Gilbert damping for samples with α = 6.5 × 10−5. We show this tuning effect is due to a strain-dependent magnetic anisotropy in the films and find the magnetoelastic coefficient |λs| ∼ (1–4.4) ppm, backed by theoretical predictions from density-functional theory calculations and magnetoelastic theory. Noting the rapidly expanding application space for strain-tuned FMR, we define a new metric for magnetostrictive materials, magnetostrictive agility, given by the ratio of the magnetoelastic coefficient to the FMR linewidth. This agility allows for a direct comparison between magnetostrictive materials in terms of their comparative efficacy for magnetoelectric applications requiring ultra-low loss magnetic resonance modulated by strain. With this metric, we show V[TCNE]x is competitive with other magnetostrictive materials, including YIG and Terfenol-D. This combination of ultra-narrow linewidth and magnetostriction, in a system that can be directly integrated into functional devices without requiring heterogeneous integration in a thin film geometry, promises unprecedented functionality for electric-field tuned microwave devices ranging from low-power, compact filters and circulators to emerging applications in quantum information science and technology. 

In this work, we have prepared intergrowth of multiferroic compounds namely Bi4RTi3Fe0.7Co0.3O15-Bi3RTi2Fe0.7Co0.3O12−δ (BRTFCO15-BRTFCO12) (rare earth (R) = Dy, Sm, La) by solid-state reaction method. From the X-ray diffraction Rietveld refinement, the structure of the intergrowths was found to be orthorhombic in which satisfactory fittings establish the existence of three-layered (space group: b 2 c b) and four-layered compounds (space group: A21am). Analysis of magnetic measurements confirmed a larger magnetization for theSm-modified intergrowth compound (BSTFCO15-BSTFCO12) compared to Dy- and La-doped ones. The emergence of higher magnetic properties can be due to distortion in the unit cell when some Bi3+ ions are replaced with the Sm3+, bonding of Fe3+-O-Co3+ as well as a possible mixture of FexCoy-type nanoparticles that are formed generally in the synthesis of intergrowths. The changes in the magnetic state of the Aurivillius intergrowths have been reflected in the magnetoelectric (ME) coupling: higher ME coefficient (~30 mV/Cm-Oe) at lower magnetic fields and is constant up to 3 kOe. The results were corroborated by Raman spectroscopy and variation of temperature with magnetization data. The results revealed that the RE-modified intergrowth route is an effective preparative method for higher-layer Aurivillius multiferroic ceramics. 

Here, we discuss a model for the quasi-static magnetoelectric (ME) interaction in three-layer composites consisting of a single piezoelectric (PE) layer and two magnetostrictive (MS) layers with positive and negative magnetostriction. Two types of layer arrangements are considered: Type 1: a sandwich structure with the PE layer between the two MS layers and Type 2: the two MS layers form the adjacent layers. Expressions for the ME response are obtained using the system of equations of elasto- and electrostatics for the PE and MS phases. The contributions from longitudinal and bending vibrations to the net ME response are considered. The theory is applied for trilayers consisting of lead zirconate titanate (PZT), nickel for negative magnetostriction, and Metglas for positive magnetostriction. Estimates of the dependence of the strength of the ME response on the thickness of the three layers are provided. It is shown that the asymmetric three-layer structures of both types lead to an increase in the strength of ME interactions by almost an order of magnitude compared to a two-layer piezoelectric-magnetostrictive structure. The model predicts a much stronger ME response in Type 2 structures than in Type 1. The theory discussed here is of importance for designing composites for applications such as magnetic field sensors, gyrators, and energy harvesters.