Strong Magnetoelectric Effect Research Articles

Stoner instability-mediated large magnetoelectric effects in 2D stacking electrides

Strong magnetoelectric effects in single-phase two-dimensional (2D) materials are extremely rare in nature. Here by first-principles calculations, we find a strong magnetoelectric coupling in polar stacking bilayer Hf2S that allows the reversal of net magnetic moments with the reversal of electric dipoles. Further analysis shows that such strong magnetoelectric effects benefit from the Stoner instability of surface Hf atoms triggered by polar stacking. Moreover, an unexpectedly large out-of-plane electric polarization (which is at least two times larger than that of bilayer BN) survives in the material, despite its metallicity. The large electric polarization is ascribed to the delocalized interlayer electrons which generally present in layered electride materials. It is quite interesting that large electric polarization, metallicity and magnetism coexist in one single-phase material. Our findings reveal rich physical phenomena to be explored in 2D stacking multiferroics and suggest an alternative way of searching for strong magnetoelectric materials with ultrathin thickness.

Non-volatile voltage-controlled magnetization in single-phase multiferroic ceramics at room temperature

Single-phase multiferroics (MFs) exhibiting ferroelectricity and ferromagnetism and the strong magnetoelectric (ME) coupling effect at room temperature are seen as key to the development of the next-generation of spintronic devices, multi-state memories, logic devices and sensors. Herein, the single-tetragonal phase (1–x) (Sr0·3Bi0·35Na0·329Li0.021)TiO3-xBiFeO3 (x = 0.2 or 0.4) system was designed to study the intrinsic ME coupling effect at room temperature and high frequencies. The polarization arises from the cooperative displacement of both Fe3+ and Ti4+ relative to the oxygen sublattice in the tetragonally distorted perovskite structure, and the magnetization stems from indirect exchange magnetic interaction between adjacent iron ions. A switchable voltage-controlled magnetization was confirmed by a change of the coercive magnetic field, Hc, and remnant magnetization, Mr, in the x = 0.4 component subjected to an external electric field at room temperature and was possibly attributed to a strain-mediated ME coupling effect. In addition, resonance behaviours of the complex magnetic permeability and complex dielectric permittivity in the GHz band indicate that this ME effect is intrinsic in nature and could broaden the applications of multiferroics to devices operating at microwave frequencies.

A Novel Spinel Ferrite-Hexagonal Ferrite Composite for Enhanced Magneto-Electric Coupling in a Bilayer with PZT.

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.

Optical and magnetoelectric coupling studies of ErCrO3

ErCrO3 samples were synthesized by solid state method. The structure, optical, magnetic, dielectric and low-temperature pyroelectric properties of the system were investigated. X-ray diffraction (XRD) and scanning electron microscopy (SEM) revealed that the sample has an orthorhombic structure with the Pbnm space group, and an average particle size of 641 nm. Optical studies show that the optical band gaps are 2.1 eV and 3.2 eV for the sample. DC and AC magnetization indicate that ErCrO3 undergoes three magnetic phase transitions near TN (Cr3+), TSR, and TN(Er3+). Interestingly, another hump is observed in the range of 50–70 K during the AC magnetization measurements. Dielectric and pyroelectric measurements demonstrate significant anomalies in the dielectric permittivity and pyroelectricity around TN, TSR and the corresponding temperature of the hump. This suggests a close correlation between the dielectric and pyroelectric properties with the magnetic transition. Furthermore, the pyroelectric measurements at low temperatures prove that the magnetic field could regulate the electric polarization, a further proof of the strong magnetoelectric coupling effect in the system. These properties of ErCrO3 make it have significant applications in optoelectronic devices, storage devices, sensors, and so on.

Analysis of optical channel waveguides composed of bianisotropic materials with a strong magnetoelectric effect using a transmission-line formulation

Optical modes in channel waveguides composed of lossy bianisotropic magnetoelectric (ME) materials have been theoretically investigated here. In this study, a semi-analytical method based on the Fourier expansion technique, a well-known transmission-line formulation, is generalized to ME materials in a general case. Using this method, the dispersion diagram, including both phase and attenuation constants, and the field profile of the guided modes in channel waveguides such as rib waveguides are obtained. The presence of ME materials changes the polarization of guided modes in the structure. In all stages of the analysis, the numerical results are calculated and compared with those generated by commercial electromagnetic solvers to verify the computational efficiency and accuracy of the proposed method.

Synthesis and physical properties of multiferroic BaDyFeO4

Materials exhibiting magnetoelectric effects have drawn great interest because of their intriguing physical phenomena and potential applications in electronic devices. The magnetoelectric (ME) coupling makes the materials promising for use in multifunctional devices with electric-field-tunable magnetism and magnetic-field-controlled ferroelectricity. Very recently, a strong ME effect has been found in the BaRFeO4 system (R is a rare-earth element), in which the ferroelectricity is driven by the onset of a long-range cycloidal antiferromagnetic order of Fe spins. However, previous studies have shown how complicated the synthesis procedure is to obtain single-phase samples of the materials. In this work, we present a simple and easy fabrication process to synthesise high-quality BaDyFeO4 using the conventional solid-state reaction method. The structural, morphological, and optical properties of the synthesised sample were investigated by means of X-ray diffraction, scanning electron microscopy, and UV-Vis spectroscopy, respectively. The sample was formed from high-quality microparticles. The X-ray diffraction study reveals the single-phase nature of the sample adopting the Pnma orthorhombic structure without any impurity phases. The detailed structural parameters were refined with Rietveld refinement. The sample demonstrates a direct gap semiconducting behaviour. The experimental results of the structural and electronic properties of BaDyFeO4 are complemented by density functional theory (DFT) calculations.

Tuning magnetism by electric field in MnPS3/Sc2CO2 van der Waals heterostructure

Combining a two-dimensional (2D) antiferromagnetic (AFM) material, MnPS3 and a 2D ferroelectric material, Sc2CO2, we propose 2D van der Waals (vdW) heterostructure multiferroics to realize strong magnetoelectric coupling, which is important for designing high-performance magnetoelectric devices. By using first-principles simulations, it is found that the transition from an AFM state to a ferromagnetic (FM) state of a MnPS3 layer could be realized by reversing the polarization direction of a Sc2CO2 layer. We further reveal that such strong magnetoelectric effects originate from the large inter-layer charge transfer due to the competitive interaction between the difference of the interface work functions between MnPS3 and Sc2CO2 and the strong electronegativity of the O atom interface in the Sc2CO2 layer. Our results suggest a feasible scheme for constructing 2D vdW heterostructure multiferroics with very strong inter-layer magnetoelectric coupling effect.

Density Functional Theory Studies on Magnetic Manipulation in NiI2 Layers

Effective manipulation of magnetic states is fundamentally important to modern data storage and electronic devices that underpin the information age. Controlling magnetism via electric fields instead of magnetic fields has long been envisioned as a revolutionary technology to achieve higher energy efficiency and ultimate device miniaturization. The electric field paradigms, however, face major challenges of volatility, high energy cost, and low storage density. In this work, from density functional theory simulations, we developed effective approaches to achieve magnetic control in bilayer NiI2 via electrostatic doping and polarization field of the ferroelectric heterostructure. The interlayer antiferromagnetic (AFM) to ferromagnetic (FM) transition has been observed in bilayer NiI2 when the critical electron doping concentration reaches 0.625% due to the magnetic exchange competition between antiferromagnetic and ferromagnetic couplings. The critical concentration of magnetic transition can be reduced or increased depending on the polarization direction when it is placed on the ferroelectric substrate of Sc2CO2 as a result of polarization-induced interfacial electron transfer. Owing to the antiferromagnetic-to-ferromagnetic (AFM–FM) transition, the reversal of ferroelectric polarization modulates the electronic properties dramatically due to the strong interfacial magnetoelectric effect. The magnetic and electronic manipulation from electrostatic doping and polarization provides feasible approaches for next-generation electronics and spintronics.

Spin-Lattice and Magnetoelectric Couplings Enhanced by Orbital Degrees of Freedom in Polar Multiferroic Semiconductors.

Orbital degrees of freedom mediating an interaction between spin and lattice were predicted to raise strong magnetoelectric effect, i.e., to realize an efficient coupling between magnetic and ferroelectric orders. However, the effect of orbital fluctuations has been considered only in a few magnetoelectric materials, as orbital-degeneracy driven Jahn-Teller effect rarely couples to polarization. Here, we explore the spin-lattice coupling in multiferroic Swedenborgites with mixed valence and Jahn-Teller active transition metal ions on a stacked triangular and Kagome lattice using infrared and dielectric spectroscopy. On one hand, in CaBaM_{4}O_{7} (M=Co, Fe), we observe a strong magnetic-order-induced shift in the phonon frequencies and a corresponding large change in the dielectric response. Remarkably, as an unusual manifestation of the spin-phonon coupling, the spin fluctuations reduce the phonon lifetime by one order of magnitude at the magnetic phase transitions. On the other hand, lattice vibrations, dielectric response, and electric polarization show no variation at the Néel temperature of CaBaFe_{2}Co_{2}O_{7}, which is built up by orbital singlet ions. Our results provide a showcase for orbital degrees of freedom enhanced magnetoelectric coupling via the example of Swedenborgites.

Investigations of room temperature multiferroic and magneto-electric properties of (1-Φ) PZTFT-Φ CZFMO particulate composites

Multiferroic composites consisting of a single-phase multiferroic [0.6(PbZr0.53Ti0.47O3)-0.4(PbFe0.5Ta0.5)O3] as a matrix and a magnetostrictive phase (Co0.6Zn0.4Fe1.7Mn0.3O4) dispersed in the matrix are fabricated via hybrid synthesis technique. The structure and surface morphology studies using x-ray diffraction and field emission scanning electron microscopy techniques indicate the formation of 3-0 type particulate composites. Coexistence of soft-magnetic behavior and ferroelectric characteristics are confirmed for composites from magnetization vs magnetic field (M–H) and polarization vs electric field (P–E) measurements, respectively. Magneto-dielectric (MD) measurement shows significant changes in the dielectric properties with the application of a magnetic field, indicating the existence of strong MD behavior. The biquadratic nature of magneto-electric (ME) coupling is described by the Landau free energy equation arising from the strain transfer at the interfaces between the constituent phases. The direct magneto-electric voltage coefficient measurement also confirms very strong coupling between ferroelectricity and magnetism and supports the strain-mediated magneto-electric effect in composites. The Φ = 0.3 composite exhibits the maximum ME coefficient of 20.72 mV/cm Oe with MS = 24.62 emu/g, HC = 59.66 Oe, and piezoelectric coefficient value d33 = 19 pC/N. The strong magneto-electric effect along with low dielectric loss at room temperature in these composites suggests their suitability for multifunctional magneto-electric device applications such as magnetic sensors, etc.

Spin-splitting and switchable half-metallicity in a van der Waals multiferroic CuBiP2Se6/GdClBr heterojunction.

Multiferroic van der Waals (vdW) heterojunctions have a strong and nonvolatile magnetoelectric coupling effect, which is of great significance in spintronic devices. The electronic structure and magnetic properties of a GdClBr/CuBiP2Se6 vdW multiferroic heterojunction have been calculated using first-principles methods. Due to the spin-up charge transfer and Zeeman field, the ferroelectric CuBiP2Se6 exhibits spin splitting at the gamma point. It is found that the electronic structure and magnetic properties of the GdClBr/CuBiP2Se6 vdW multiferroic heterojunction have been significantly modulated by the electric polarization of CuBiP2Se6. During the reversal of the ferroelectric polarization of CuBiP2Se6, the ferromagnetic GdClBr monolayer transforms from a semiconductor to a half-metal. Meanwhile, in both upward and downward ferroelectric polarization, the GdClBr/CuBiP2Se6 heterojunction exhibits perpendicular magnetic anisotropy with a Curie temperature of 239 K. As the strain changes from -6% to 6%, the band structure of GdClBr shifts upward, and the band structure of CuBiP2Se6 shifts downward. Compressive strain can increase the Curie temperature of the GdClBr/CuBiP2Se6 heterojunction. The magnetic anisotropy of heterojunctions highly depends on biaxial strain, where the perpendicular (in-plane) magnetic anisotropy increases with the increased compressive (tensile) strain. The vdW multiferroic GdClBr/CuBiP2Se6 heterojunction has potential applications in spintronic devices.

Significantly enhanced hybrid improper ferroelectricity of Ca3Ti2O7 ceramics by the oxygen vacancy engineering

Ca3Ti2O7 materials with hybrid improper ferroelectricity call tremendous interest due to their great potential in designing novel room-temperature single-phase multiferroics with a strong magnetoelectric coupling effect. However, achieving Ca3Ti2O7-based ceramics with superior room-temperature ferroelectricity remains a crucial challenge. Herein, Ca3Ti2O7 ceramics were prepared by a tartaric acid sol–gel method and sintered in air and oxygen atmospheres, respectively. It was found that the long-time high-temperature sintering in air could lead to the formation of CaTiO3/Ca3Ti2O7/CaTiO3 sandwich structure, and oxygen-enriched sintering could effectively avoid the formation of CaTiO3 phase on the surface. The superior hybrid improper ferroelectricity is attained in Ca3Ti2O7 ceramics sintered in oxygen atmosphere with a higher remnant polarization (3.63 μC/cm2) and lower coercive electric field (72.6 kV/cm) obtained by positive-up and negative-down method, which is better than the ceramic sample sintered in air. The significantly better ferroelectricity is benefited from the synergistic effects of its larger distortion of oxygen octahedron, larger grain size, and lower oxygen vacancy concentration. Due to its low leakage current density, Ca3Ti2O7 ceramics sintered in oxygen atmosphere exhibit the remanent polarization as high as 7.40 μC/cm2 under the conditions of 1 Hz and 200 kV/cm obtained by dynamic hysteresis measurement mode. Furthermore, there are obvious stripe ferroelectric domains, which provide direct evidence for the excellent hybrid improper ferroelectricity of Ca3Ti2O7 ceramics. These findings demonstrate that the oxygen vacancy engineering is an effective strategy to improve hybrid improper ferroelectricity of Ca3Ti2O7 materials.

Modeling of core-shell magneto-electric nanoparticles for biomedical applications: Effect of composition, dimension, and magnetic field features on magnetoelectric response.

The recent development of core-shell nanoparticles which combine strain coupled magnetostrictive and piezoelectric phases, has attracted a lot of attention due to their ability to yield strong magnetoelectric effect even at room temperature, thus making them a promising tool to enable biomedical applications. To fully exploit their potentialities and to adapt their use to in vivo applications, this study analyzes, through a numerical approach, their magnetoelectric behavior, shortly quantified by the magnetoelectric coupling coefficient (αME), thus providing an important milestone for the characterization of the magnetoelectric effect at the nanoscale. In view of recent evidence showing that αME is strongly affected by both the applied magnetic field DC bias and AC frequency, this study implements a nonlinear model, based on magnetic hysteresis, to describe the responses of two different core-shell nanoparticles to various magnetic field excitation stimuli. The proposed model is also used to evaluate to which extent realistic variables such as core diameter and shell thickness affect the electric output. Results prove that αME of 80 nm cobalt ferrite-barium titanate (CFO-BTO) nanoparticles with a 60:40 ratio is equal to about 0.28 V/cm∙Oe corresponding to electric fields up to about 1000 V/cm when a strong DC bias is applied. However, the same electric output can be obtained even in absence of DC field with very low AC fields, by exploiting the hysteretic characteristics of the same composites. The analysis of core and shell dimension is as such to indicate that, to maximize αME, larger core diameter and thinner shell nanoparticles should be preferred. These results, taken together, suggest that it is possible to tune magnetoelectric nanoparticles electric responses by controlling their composition and their size, thus opening the opportunity to adapt their structure on the specific application to pursue.

Correlation between spin–phonon coupling and magneto-electric effects in CoFe2O4/PMN-PT nanocomposite: Raman spectroscopy and XMCD study

We have investigated strain-induced spin lattice coupling in the CoFe2O4/0.65Pb (Mg1/3Nb2/3)O3–0.35PbTiO3(PMN-PT) composite system, evident by temperature-dependent Raman spectroscopy and magnetization measurements. The strain interactions lead to magneto-electric coupling, and the measured magneto-electric voltage coefficient is 40 mV/cm−1Oe−1 for the CoFe2O4/PMN-PT composite samples. X-ray magnetic circular dichroism (XMCD) analysis establishes modified spin structure in the electrically poled CoFe2O4/PMN-PT composite, further validating the coupling between magnetic and electric ordering in the composite. The magneto-electric coupling coefficient α vs dc magnetic field curves revealed hysteretic behavior and enhanced α values after electric poling, which originates from the strain-induced modifications in the magnetic structure of composite in the electrically poled samples. These findings suggest that the existence of spin lattice coupling may lead to the mechanism of strong magneto-electric effects via strain interactions in CoFe2O4/PMN-PT composite.

Direct evidence of mutual control of ferroelectric polarization and magnetization in Y-type hexaferrite BaSrCo2Fe12-Al O22 ceramics

Hexaferrites that exhibit the intrinsic and strong magnetoelectric (ME) coupling effect have been considered the most promising candidate for single-phase multiferroics. Currently, the strong ME coupling effect in this system was widely reported in single crystal form, while it is rare in polycrystalline one. In this work, Y-type hexaferrite BaSrCo2Fe12-xAlxO22 (x = 0.0, 0.3, 0.6 and 0.9) ceramics were manufactured with conventional solid-state reaction. Their magnetic, dielectric, and ME coupling properties were systematically surveyed. It was revealed that Al doping could result in a high magnetic transition temperature of ~ 345 K for x = 0.9. Also, the ferroelectric polarization and abnormal magnetodielectric properties were significantly enhanced which could be maintained down to 200 K. Most interestingly, the sample x = 0.9 displayed strong direct and converse ME coefficients of ~ 400 ps/m and ~ 900 ps/m at 150 K, respectively. Therefore, these results reveal that Al doping can broaden our understanding of the Y-type hexaferrite in room-temperature multiferroics.

Giant anomalous charge-spin conversion at Co/Pb(Mg1/3Nb2/3)O3–Pb0.7Ti0.3O3 interfaces

An efficient out-of-plane anti-damping spin–orbit torque (SOT) is in great demand for high-density spintronic devices with perpendicular magnetic anisotropy. Despite its importance, direct realization of such SOT in a single magnetic layer is scarce and has remained challenging. Here, we present experimental evidence uncovering unconventional out-of-plane anti-damping torques in the Co film deposited on the ferroelectric Pb(Mg1/3Nb2/3)O3–Pb0.7Ti0.3O3 (PMN–PT) substrate. We show via spin-torque ferromagnetic resonance that both Rashba- and unconventional-type SOT give rise to a high-efficient charge-to-spin conversion. The strong magnetoelectric effect at the Co/PMN-PT interface allows further directly electric-field control of the conversion.

Improper multiferroiclike transition in a metal

Magnetic frustration in insulators often induces cooperative atomic displacements to form a polar structure with long-range ordered electric dipoles, commonly known as improper multiferroics. In metals, such a multiferroic phenomenon is not expected to occur because free carriers tend to screen internal electrostatic forces, eliminating long-range ordered electric dipoles. To date, intrinsic multiferroiclike metals have rarely been reported. Here we present a spin-frustration-induced long-range antiparallel ordering of electric dipoles in metallic CrN with an unusual antiferromagnetic ground state. Two equivalent magnetic structures are also iden- tified and linked to two distinct antiparallel polar orders. Such a scenario is analogous to that of conventional improper multiferroics with a magnetic origin of polar transition. The order parameter of structural distortion is linearly coupled to the magnetic order due to a strong magnetoelectric effect. The multiferroiclike metal is in striking contrast to insulating multiferroics, offering an extraordinary archetype for probing new underlying physics and exploring unusual properties for practical applications.

Enhanced dielectric, ferroelectric, and ferromagnetic properties of 0.7Bi1−xTmxFeO3–0.3BaTiO3 ceramics by Tm-induced structural modification

In this study, Tm-doped 0.7Bi1−xTmxFeO3–0.3BaTiO3 (x = 0–0.05) ceramics have been fabricated using traditional solid-phase reactions and their structural, morphological, and dielectric as well as multiferroic properties are investigated. X-ray diffraction and Rietveld refinement indicated the formation of a Tm-modulated morphotropic phase boundary (MPB) from the rhombohedral (R3c) and tetragonal (P4mm) phases to a single P4mm phase for Tm content of x = 0.02–0.03. Tm occupation of lattice sites is strongly suggested at both the A and B sites in the ABO3-type perovskite structure, which is supported by the obtained Raman spectra, the calculated tolerance factor, and dielectric relaxation characteristics. With the Tm-induced aforementioned–structural modification, the dielectric constant, remnant polarization (Pr), and remnant magnetization (Mr) values indicate that the dielectric and multiferroic properties are greatly improved. The obtained maximum remnant polarization (2Pr = 35.28 μC/cm2) and remnant magnetization (2Mr = 0.56 emu/g) are approximately two and seven times larger, respectively, than those of the sample without Tm substitution (x = 0). With increasing the Tm content, the remnant polarization, and the remnant magnetization exhibit almost the same trends in variation, indicating the possible existence of a relatively strong magnetoelectric coupling effect. Our study may provide a substitution strategy (structural modification by substituting the same element into two different lattice sites) to efficiently enhance the dielectric and multiferroic properties of BiFeO3–BaTiO3-based ceramics.

Strain-Induced Magnetoelectric Coupling in Fe3O4/BaTiO3 Nanopillar Composites.

Magnetoelectric coupling properties are limited to the substrate clamping effect in traditional ferroelectric/ferromagnetic heterostructures. Here, Fe3O4/BaTiO3 nanopillar composites are successfully constructed. The well-ordered BaTiO3 nanopillar arrays are prepared through template-assisted pulsed laser deposition. The Fe3O4 layer is coated on BaTiO3 nanopillar arrays by atomic layer deposition. The nanopillar arrays and heterostructure are confirmed by scanning electron microscopy and transmission electron microscopy. A large thermally driven magnetoelectric coupling coefficient of 395 Oe °C-1 near the phase transition of BaTiO3 (orthorhombic to rhombohedral) is obtained, indicating a strong strain-induced magnetoelectric coupling effect. The enhanced magnetoelectric coupling effect originated from the reduced substrate clamping effect and increased the interface area in nanopillar structures. This work opens a door toward cutting-edge potential applications in spintronic devices.

Observation of Anomalously Large Magnetoelectric Coupling in the Hexagonal Z‐Type Ferrite Films

AbstractAlthough the bulk hexaferrites are known to exhibit strong magnetoelectric (ME) effects near room temperature, the same effects are not realized in a thin film form. Herein, the growth of nearly epitaxial Co2Z‐type hexaferrite Ba0.3Sr2.7Co2Fe24O41 (BSCFO) thin films on a SrTiO3 (111) substrate by a chemical solution deposition method is reported. The reciprocal space mapping on the annealed BSCFO films reveals broadening along the qx directions in the (0014) and (0018) peaks, indicating that the oxygen planes belonging to the off‐centered octahedra have randomly distributed out‐of‐plane tilt to indicate significant disorder in the crystallographic orientation. Quantitative investigations reveal that both ME susceptibility and modulated electric polarization (ΔP) by magnetic field up to 370 K in the BSCFO films are always larger than those of the Co2Z‐type single crystal by ≈2–15 times and further increase upon having enhanced qx broadening in the (0014) and (0018) peaks. As the off‐centered octahedral sites can be a primary source of ΔP as predicted by the p–d hybridization mechanism, these results indicate that effective off‐centering could be further enhanced by the orientational disorder. This study identifies the potential of applying the ME hexaferrite films for multifunctional devices.