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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.more » « less
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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.more » « less
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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.more » « less
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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.more » « less
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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.more » « less
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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.more » « less
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Abstract This work is on the design, fabrication and characterization of a hexagonal ferrite band-pass filter that can be tuned either with a magnetic field or an electric field. The filter operation is based on a straight-edge Y-type hexagonal ferrite resonator symmetrically coupled to the input and output microstrip transmission lines. The Zn2Yfilter demonstrated magnetic field tunability in the 8–12 GHz frequency range by applying an in-plane bias magnetic fieldH0provided by a built-in permanent magnet. The insertion loss and 3 dB bandwidth within this band were 8.6 ± 0.4 dB and 350 ± 40 MHz, respectively. The electric fieldEtunability of the pass-band of the device was facilitated by the nonlinear magnetoelectric effect (NLME) in the ferrite. TheE-tuning of the center frequency of the filter by (1150 ± 90) MHz was obtained for an input DC electric power of 200 mW. With efforts directed at a significant reduction in the insertion loss, the compact and power efficient magnetic and electric field tunable Zn2Y band-pass filter has the potential for use in novel reconfigurable RF/microwave devices and communication systems.more » « less
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Abstract This work focuses on the nature of magnetic anisotropy in 2.5–16 micron thick films of nickel ferrite (NFO) grown by liquid phase epitaxy (LPE). The technique, ideal for rapid growth of epitaxial oxide films, was utilized for films on (100) and (110) substrates of magnesium gallate (MGO). The motivation was to investigate the dependence of the growth induced anisotropy field on film thickness since submicron films of NFO were reported to show a very high anisotropy. The films grown at 850–875 C and subsequently annealed at 1000 C were found to be epitaxial, with the out-of-plane lattice constant showing unanticipated decrease with increasing film thickness and the estimated in-plane lattice constant increasing with the film thickness. The uniaxial anisotropy field H σ , estimated from X-ray diffraction data, ranged from 2.8–7.7 kOe with the films on (100) MGO having a higher H σ value than for the films on (110) MGO. Ferromagnetic resonance (FMR) measurements for in-plane and out-of-plane static magnetic field were utilized to determine both the magnetocrystalline the anisotropy field H 4 and the uniaxial anisotropy field H a . Values of H 4 range from −0.24 to −0.86 kOe. The uniaxial anisotropy field H a was an order of magnitude smaller than H σ and it decreased with increasing film thickness for NFO films on (100) MGO, but H a increased with film thickness for films on (110) MGO substrates. These observations indicate that the origin of the induced anisotropy could be attributed to several factors including (i) strain due to mismatch in the film-substrate lattice constants, (ii) possible variations in the bond lengths and bond angles in NFO during the growth process, and (iii) the strain arising from mismatch in the thermal expansion coefficients of the film and the substrate due to the high growth and annealing temperatures involved in the LPE technique. The LPE films of NFO on MGO substrates studied in this work are of interest for use in high frequency devices.more » « less