Magnetoelectric effect in composites of magnet,metal-cap,and piezoceramic

We report on the magnetoelectric (ME) effect in three-phase magnet-metal-cap-piezoceramic composites of a thickness-polarized Pb(Zr,Ti)O₃ disk bonded between two truncated conical brass caps and two thickness-magnetized NdFeB magnets along the thickness direction. The effect originated from the product of the magnetic attractive–repellent effect in the magnets and the amplified piezoelectric effect in the cap-disk assembly. The composites exhibited a ME voltage coefficient α_V of ∼2.6 mV/Oe in the non-resonance frequency range of 0.1–10 kHz with good voltage-field linearity in the field range of 10^-3–10 Oe, besides an enhanced α_V of 167.4 mV/Oe at a resonance frequency of 14.4 kHz. Compared to conventional two-phase and three-phase magnetostrictive material-contained ME composites, these composites possessed two distinct benefits of higher property-tailorable flexibility and requiring no external dc bias magnetic field to enable an obvious α_V. PACS 77.84.-S; 75.80.+q; 77.84.Dy; 77.65.-j; 85.80.Jm     

铁电/铁磁三相颗粒复合材料的磁电性能计算

采用格林函数方法给出了三相复合材料的磁电系数的解析式，对稀土-铁合金/压电陶瓷/高分子（Terfenol-D/PZT/PVDF）三相颗粒复合材料的磁电系数进行了计算.计算结果给出了复合材料的磁电性能与材料显微结构的关系，包括三相颗粒复合材料的磁电性能随组分、颗粒的长径比、PZT颗粒的电极化方向以及外磁场的变化趋势，可为实验设计提供参考和指导.通过合理设计，三相磁电复合材料的性能可以达到数百mV/A.作为一种新的磁电复合材料，三相颗粒复合材料有望成为一种新型高性能易制备的磁电材料. 关键词： 磁电效应 复合材料 格林函数     

Influence of the stress on magnetoelectric effect in magnetostrictive-PZT bilayers

In this letter, we investigate the influence of the stress on magnetoelectric (ME) effect in a magnetostrictive-PZT bilayer. ME voltage coefficient α*_E = δE / δH, where δE is the induced electric field for an applied alternating current (ac) magnetic field δH, is obtained by solving the stress-related piezoelectric constitutive equation and the conventional magnetostrictive equation with appropriate boundary condition. Based on the free-energy density function of the PZT film in stress state, we get the stress-related piezoelectric charge coefficient ^p d*₃₁ and dielectric permittivity ^pε*₃₃. After taking the cobalt ferrite (CFO) as magnetostrictive phase, it is found that α*_E increases with decreasing 2-d compressive stress for CFO-PZT, which not only is qualitatively consistent with previous experimental measurements, but also provides a possible route to improve the ME effect.      

偏置电压对磁致伸缩/压电层合换能结构磁电性能影响

分析和测试了偏置电压调整时PZT5/Terfenol-D/PZT8层合换能结构磁电性能. 提出了一种磁致伸缩/压电层合磁电换能结构的一阶谐振频率控制方法. 通过改变压电驱动层的直流电压对磁电层合结构的预应变进行改变, 从而调整谐振频率. 分析偏置电压、 应变、 弹性模量、 谐振频率和谐振磁电电压系数之间关系. 分析表明: 在较小应变情况下, 控制电压几乎可以线性调节谐振频率, 而层合结构谐振磁电电压系数几乎与偏置电压无关. 实验研究验证: 理论与实验结果较好吻合. 在-170 V-+170 V的偏置电压时, 谐振频率可以几乎线性调整. 最大频率调整量达到1 kHz, 偏置电压对一阶纵振频率的控制率达到: 2.94 Hz/V. 在偏置磁场为0-225 Oe时, 谐振频率调整量与偏置磁场无关. 偏置磁场会改变谐振磁电电压系数, 在大于178 Oe静态磁场偏置时, 磁电电压系数最大, 达到1.65 V/Oe.     

高磁导率材料FeCuNbSiB对超磁致伸缩/压电层合材料磁电性能的影响

采用超磁致伸缩材料TbxDy_1-xFe₂(x≈0.3)(Terfenol-D)、压电材料PbZrxTi_1-xO₃(PZT)和高磁导率材料FeCuNbSiB构造了新型的层合结构.由于引入高磁导率材料FeCuNbSiB改变了Terfenol-D的内部磁场分布,并且在磁场作用下,FeCuNbSiB发生形变对Terfenol-D产生应力,增大了Terfeno 关键词： 磁电效应 磁致伸缩材料 压电材料 高磁导率材料     

Structural and electrical characterization of PZT on gold for micromachined piezoelectric membranes

Piezoelectric membranes have been fabricated that incorporate a gold bottom electrode with an adhesion layer of titanium–tungsten (10:90 wt. %). For solution-deposited acetic acid based lead zirconate titanate (HoAc-PZT) with a Zr:Ti ratio of 40:60, the film’s average piezoelectric coefficient, e₃₁, is -5.31 C/m², with a dielectric constant of 814 at 200 Hz, which is similar to values for platinum bottom electrodes. The PZT structure remains columnar on both types of bottom electrodes. Initial fabrication attempts resulted in cracking that initiated in the PZT layer of the structure. X-ray photoelectron spectroscopy was utilized to establish how processing affects diffusion throughout the composite membrane structure. Crack-free membranes were fabricated and tested. This paper discusses the performance properties and piezoelectric fatigue results for these membranes. PACS 77.84.-s; 77.84.Lf     

Enhanced mangnetoelectric voltage in multiferroic particulate Ni0.83Co0.15Cu0.02Fe1.9O4−δ/PbZr0.52Ti0.48O3 composites – dielectric,piezoelectric and magnetic properties

Multiferroic particulate composites of Ni_0.83Co_0.15Cu_0.02Fe_1.9O_4−δ– NCCF and lead zirconate titanate (PZT) were prepared conventional ceramic method. The generic formulae x NCCF + (1−x) PZT where x = 0.1, 0.2, 0.3, 0.4, 0.5 and 0.6 mole fractions. The presence of two phases in multiferroic was confirmed with XRD technique. The dielectric constant and loss tangent were studied as a function of frequency (100 Hz to 1 M Hz) and temperature (30–500 °C). The piezoelectric coefficient d₃₃ were also studied on these particulate composites. The hysteresis behaviour was studied to understand the magnetic properties such as saturation magnetization (Ms) and magnetic moment (μ_B). The static magnetoelectric (ME) voltage coefficient was measured as a function of dc magnetic bias field. A high value of ME output (3151 mV/Oe.cm) was obtained in the composite containing 50% highly magnetostrictive ferrite component NCCF – 50% highly piezoelectric ferroelectric component PZT. These multiferroic particulate composites are used as phase shifters, magnetic sensors, cables etc.     

Electrical conduction and magnetoelectric effect of (x) BaTiO3 + (1−x) Ni0.92Co0.03Cu0.05Fe2O4 composites in ferroelectric rich region

Particulate composites with composition (x)BaTiO₃+(1−x)Ni_0.92Co_0.03Cu_0.05Fe₂O₄ in which x varies as 1, 0.85, 0.70, 0.55 and 0 (in mol%) were prepared by the conventional double sintering ceramic technique. The presence of two phases viz. ferromagnetic (Ni_0.92Co_0.03Cu_0.05Fe₂O₄) and ferroelectric (BaTiO₃) was confirmed by X-ray diffraction analysis. The dc resistivity and thermo-emf measurements were carried out with variation of temperature. The ac conductivity (σ_ac) measurements investigated in the frequency range 100 Hz to 1 MHz conclude that the conduction in these composites is due to small polarons. The variation of dielectric constant and loss tangent with frequency (20 Hz to 1 MHz) was studied. The static magnetoelectric conversion factor, i.e. dc (dE/dH)_H was measured as a function of intensity of applied magnetic field. The changes were observed in electrical properties as well as in magnetoelectric voltage coefficient as the molar ratio of the constituent phases was varied. A maximum value of magnetoelectric conversion factor of 536.06 μV/cm Oe was observed for the composite with 70% BaTiO₃+30% Ni_0.92Co_0.03Cu_0.05Fe₂O₄ at a dc magnetic field of 2.3 K Oe. The maximum magnetoelectric conversion output has been explained in terms of ferrite-ferroelectric content, applied static magnetic field and resistivity.     

Multiferroic behavior and magnetoelectric effect in CoFe2O4/Pb(Zr0.53Ti0.47)O3 thick films

A CoFe₂O₄/Pb(Zr_0.53Ti_0.47)O₃ (CFO/PZT) multiferroic composite thick film assisted by polyvinylpyrrolidone (PVP) was prepared by a hybrid sol–gel processing and spin coating technique. Scanning electronic microscopy indicated a porous microstructure with a thickness of 6.2 μm. Pure PZT perovskite phase observed from x-ray diffraction suggested that the low ratio of CFO particles was deeply buried in the PZT matrix. Ferroelectric and ferromagnetic properties were observed simultaneously at room temperature as well as a lower leakage current compared with a CFO/PZT thin film. The dynamic and static magnetoelectric effects were strongly dependent on the applied DC/AC magnetic field but their values were very low. The results demonstrated the prediction that ferroelectric and ferromagnetic properties can induce a strong magnetoelectric coupling only if a dense microstructure was achieved.     

Low-frequency magnetoelectric effect in a Galfenol-PZT planar composite structure

The forward and inverse magnetoelectric (ME) effects are experimentally studied in a two-layer planar structure containing mechanically coupled Galfenol and PZT plates. The process of production of polycrystalline Galfenol plates and their magnetic and magnetostriction characteristics are described. For the forward ME conversion, the dependences of the amplitude of the voltage generated by the structure on the magnitude and orientation of a dc magnetic field and the frequency and amplitude of a modulating magnetic field are measured. For the inverse ME conversion, the dependences of the amplitude of the change in the magnetic induction of the structure on the dc magnetic field and the frequency of an ac electric field applied to the structure are measured. The efficiencies of the forward and inverse ME conversion are estimated for the case of low-frequency field modulation and under conditions of the resonance excitation of bending and longitudinal mechanical vibrations in the structure.     

Electric field-induced magnetoresistance in spin-valve/piezoelectric multiferroic laminates for low-power spintronics

Electric field-induced magnetic anisotropy has been realized in the spin-valve-based {Ni₈₀Fe₂₀/Cu/Fe₅₀Co₅₀/IrMn}/piezoelectric multiferroic laminates. In this system, electric-field control of magnetization is accomplished by strain mediated magnetoelectric coupling. Practically, the magnetization in the magnetostrictive FeCo layer of the spin-valve structure rotates under an effective compressive stress caused by the inverse piezoelectric effect in external electrical fields. This phenomenon is evidenced by the magnetization and magnetoresistance changes under the electrical field applied across the piezoelectric layer. The result shows great potential for advanced low-power spintronic devices.     

Optimal magnetoelectric coupling performance of Terfenol-D/PZT composites in resonance state under bias magnetic field

Laminated magnetoelectric (ME) composites with various thickness ratios were optimized, fabricated and experimentally investigated in this work. The Terfenal-D/PZT specimens with optimal thickness ratio between the magnetostrictive phase and piezoelectric phase, and two other values were tested for their ME coupling performance. The coupling voltage output increases linearly with the increase of DC bias magnetic field. The ME voltage coefficient increases more than 100 times in the resonance state for the optimal laminate. The DC bias magnetic field affects the ME voltage coefficient significantly, and also has little effect on the resonant frequency. The strength of AC magnetic field also slightly affects the ME voltage coefficient in resonance state, but does not affect the resonant state under which the same DC magnetic field is required. The experimental results can help understand the coupling performance of ME composite under bias magnetic field and prompt the application of ME devices.     

A theory of the inverse magnetoelectric effect in layered magnetostrictive–piezoelectric structures

A theory of the inverse magnetoelectric effect in layered structures has been presented. The theory is based on solving the equations of elastodynamics and electrostatics separately for the magnetostrictive and piezoelectric phases, taking into account the conditions at the interface between the phases. Expressions for the coefficient of inverse magnetoelectric conversion through the parameters characterizing the magnetostrictive and piezoelectric phases have been obtained. Theoretical dependences of the inverse magnetoelectric conversion coefficient on the frequency of the alternating-current electric field for the three-layer PZT–Ni–PZT structure and the two-layer terfenol-D–PZT structure have been calculated. The results of the calculations are in good agreement with the experimental data.     

Dielectric and magnetoelectric properties of BaTiO3–CoMn0.2Fe1.8O4 particulate (0-3) multiferroic composites

Multiferroic properties of (x) CoMn_0.2Fe_1.8O₄–(1-x) BaTiO₃ particulate magnetoelectric (ME) composites with x = 0.1, 0.2, 0.3 M percentage was investigated. The CoMn_0.2Fe_1.8O₄ (CMFO) phase was synthesized by solution combustion route and BaTiO₃ (BT) phase was synthesized by wet chemical method. X-ray diffraction studies revealed the purity of constitute phases; confirmed the manifestation of CMFO and BT within the ME composite structure. The microstructural aspects were observed by using Fe-SEM; revealed the effect of constituent phases on the average grain size of the composites. The temperature dependent dielectric properties for BT exhibited the three anomalies associated to its crystallographic lattice structure change with temperature. Dielectric constant of the composite was found to be decreased with CMFO content. All the composite structures exhibited typical magnetic hysteresis nature at room temperature and showed linear effect on the saturation magnetization of the composite with CMFO content. The ME response was examined at room temperature with an ac magnetic field at 1 kHz, all the composite showed a sharp decreasing behavior of the ME voltage coefficient (α_ME) to an applied dc bias in low field region. The maximum α_ME factor of ～8.51 mV/cm Oe was observed for 10% CMFO–90% BT composition.     

Magnetoelectric effect in laminates of polymer-based pseudo-1–3 (Tb0.3Dy0.7)0.5Pr0.5Fe1.55 composite and?0.3Pb(Mg1/3Nb2/3)O3–0.7PbTiO3 single crystal

We report an extrinsic magnetoelectric effect in composite laminates made by sandwiching one thickness-polarized 0.7Pb(Mg_1/3Nb_2/3)O₃–0.3PbTiO₃ (PMN–PT) piezoelectric single crystal plate between two length-magnetized, polymer-based pseudo-1–3 (Tb_0.3Dy_0.7)_0.5Pr_0.5Fe_1.55 magnetostrictive composite plates. The laminates exhibit large magnetoelectric voltage coefficients (α _V ) of ∼0.17 V/Oe with a flat response for frequencies in excess of 40 kHz and of ∼2.97 V/Oe at the natural resonance frequency of ∼65 kHz. The distinct advantages of the laminates include high magnetic field sensitivity, low Joule heating loss, wide operating bandwidth, and low cost.     

Studies on lead-free multiferroic magnetoelectric composites

Lead-free multiferroic magnetoelectric composites consisting of ferrimagnetic Ni_0.93Co_0.02Mn_0.05Fe_1.95O₄ (NMF) and ferroelectric Na_0.5Bi_0.5TiO₃ (NBT) phases were synthesized by the solid-state sintering method. The presence of constituent phases in composites was confirmed by X-ray diffraction (XRD) and scanning electron microscopy (SEM). A systematic study of dc conductivity as a function of temperature (RT −450 °C) revealed that the conduction is due to small polarons. The effect of constituent phase variation on the dielectric constant and piezoelectric strength (d₃₃) was examined. The composites exhibited typical magnetic hysteresis (M–H) loops at room temperature. Furthermore, magnetoelectric (ME) output was evaluated as a function of applied magnetic field, which is a product property of the constituent phases. The compound 50% NMF–50%NBT is a new lead-free magnetoelectric composite with 155 μV/cm ME output, which may have potential applications.     

2-2型磁电复合薄膜CoFe2O4/Pb(Zr0.53Ti0.47)O3静磁耦合

运用溶胶-凝胶法在Pt/Ti/SiO₂/Si基片上旋涂制备了2-2型CoFe₂O₄/Pb(Zr_0.53Ti_0.47)O₃磁电复合薄膜．制备的磁电薄膜结构为基片/PZT/CFO/PZT*/CFO/PZT,通过改变中间层PZT*溶胶的浓度,改变磁性层间距以及静磁耦合的大小．SEM结果表明,复合薄膜结构致密,呈现出界面清晰平整的多层结构．制备的复合薄膜具有较好的铁电与铁磁性能．实验还研究了静磁耦合对薄膜磁电性能的影响,结果表明,随着复合薄膜磁性层间距的减小,静磁耦合效应的增加,磁电电压系数有逐渐增大的趋势.     

基于能量转换原理的磁电层合材料低频磁电响应分析

提出了一种基于能量转换原理的磁致伸缩/压电层合材料低频磁电响应模型,并对不同层合结构的磁电响应特性进行了对比研究.该模型假定层合材料层间能量传递通过层间剪切力来实现,利用应力函数法分析了磁致伸缩层和压电层的应力与应变,求出了磁致伸缩层的应变能和存储磁场能以及压电层的应变能和电场能;利用Hamilton最小能量原理求出了层间剪切力的大小,获得了开路状态下层合材料的低频磁电响应模型.发现磁电电压系数与磁致伸缩材料的磁导率、泊松比、磁机耦合系数以及压电材料的泊松比、机电耦合系数等有关,并对这些参数的影响进行了分析.同时对两层和三层结构的层合材料磁电特性进行了对比研究,发现层合结构不同则获得的磁电系数公式不同,用相应的公式计算得到的误差才会最小.研究结果表明,本文的理论误差小于6.5%,与其他方法相比,本文的理论模型能更好地描述磁电层合材料的低频磁电响应特性.     

Investigation of magnetostrictive/piezoelectric multilayer composite with a giant zero-biased magnetoelectric effect

In this paper, we investigate the resonance magnetoelectric (ME) effect in the middle supported multilayer composites consisting of high-permeability Fe-based nanocrystalline soft magnetic alloy Fe_73.5Cu₁Nb₃Si_13.5B₉ (FeCuNbSiB), Nickel (Ni), and piezoelectric Pb(Zr_1?x Ti _x )O₃ (PZT). The coupling effect between positive magnetostrictive FeCuNbSiB and negative magnetostrictive Ni results in the build-in magnetic bias due to their different magnetic permeability and coercivity. As a result, a giant resonance ME voltage coefficient (α _ME,r ) at zero DC magnetic bias field (H _dc) and multi-peaks of α _ME,r for FeCuNbSiB/Ni/PZT/Ni/FeCuNbSiB composite are observed. The experimental results show that the giant zero-biased α _ME,r strongly depends on the thickness of FeCuNbSiB ribbon. The maximum zero-biased α _ME,r is up to 86 V/cm?Oe for FeCuNbSiB/Ni/PZT/Ni/FeCuNbSiB with four-layer FeCuNbSiB ribbons, which is ～500 times higher than that of the previously reported NKNLS-NZF/Ni/NKNLS-NZF trilayer composite. Compared with the peak α _ME,r and the optimum H _dc of Ni/PZT/Ni composite, the largest peak α _ME,r of FeCuNbSiB/Ni/PZT/Ni/FeCuNbSiB composite with four-layer FeCuNbSiB ribbons increases ～185 %, and the optimum H _dc decreases ～300 Oe, respectively. Based on the nonlinear magnetostrictive constitutive relation and the magnetoelectric equivalent circuit, a theoretical model of α _ME,r versus H _dc is built under free boundary conditions. Calculated zero-biased α _ME,r and α _ME,r versus H _dc are in good agreement with the experimental data. This laminate composite shows promising applications for high-sensitivity power-free magnetic field sensors, zero-biased ME transducers and small-size energy harvesters.     

磁致伸缩/压电层叠复合材料磁电效应分析

采用有限元分析软件COMSOL5.0建立了三维悬臂梁模型,分析了磁致伸缩/压电/磁致伸缩叠层复合材料的磁电系数α_(ME),并就几何参数对复合结构磁电系数的影响进行了优化分析.首先,利用稳态求解器研究了磁电层状复合结构内部的应力、应变、位移以及电势分布情况,利用瞬态求解分析了磁电复合结构各变量动态分布规律;其次,应用小信号频域分析研究了该结构的谐振频率以及在不同偏置磁场对输出电压的影响,结果表明,随着直流偏置磁场的增加,输出电压逐渐减小.改变复合材料不同层的厚度,分析了磁电层与压电层厚度比t_m/t_p对磁电系数的影响,结果表明,随着厚度比增加,α_(ME)逐渐增大,其增加速率逐渐减小;最后,分析了磁电系数α_(ME)随复合结构面积、长宽比的变化情况.分析表明,α_(ME)随磁电复合结构面积的增加逐渐增加,其增加速率逐渐减小;当磁电复合结构面积恒定时,其磁电系数随长宽比L/W增加表现出先增加后减小的趋势,存在最优值.