A hafnium oxide-based single magnetoelectric coupling multiferroic material, and a preparation method and use thereof

Abstract

The application relates to the field of multiferroic materials, in particular to a hafnium oxide-based single magnetic-electric coupling multiferroic material and a preparation method and application thereof. The chemical formula of the hafnium oxide-based single magnetic-electric coupling multiferroic material provided by the application is (Co y Fe 1‑y ) z (Hf x Zr 1‑x ) 1‑ z O2, wherein x=0.2-0.4, y=0-0.48, and z=0.15-0.35. The hafnium oxide-based single magnetic-electric coupling multiferroic material provided by the application is simple in preparation, can be prepared by adopting a pulse laser co-deposition method, and is applied to electronic devices, so that more choices can be provided for the preparation of electronic devices.

Description

Technical Field

[0001] This invention relates to the field of multiferroic materials, and more particularly to a hafnium oxide-based single magnetoelectric coupling multiferroic material, its preparation method, and its applications. Background Technology

[0002] Multiferroic materials typically refer to materials containing two or more ferroic order parameters (such as ferroelectricity, ferromagnetism, ferroelasticity, etc.). Researchers have attempted to integrate multiple order parameters into a single device to achieve correlated control. Among these, magnetoelectric coupled multiferroic materials can achieve mutual control of electricity and magnetism; for example, the polarization state can be controlled by a magnetic field. Such materials are novel multifunctional materials with broad application prospects in spintronics, multi-state storage, and electromagnetic sensors.

[0003] Magnetoelectric coupled multiferroic materials are classified into composite and single-phase types. Composite multiferroic materials are obtained by combining ferroelectric and ferromagnetic phases, and typically possess a specific two-phase composite structure. Single-phase multiferroic materials are homogeneous materials with a single chemical composition or phase structure. Currently, there are relatively few types of single-phase multiferroic materials, and their magnetoelectric coupling effect is weak, which cannot meet the requirements of electronic devices. There is an urgent need to develop more types of single-phase multiferroic materials to provide more options for the fabrication of electronic devices. Summary of the Invention

[0004] This invention provides a hafnium oxide-based single magnetoelectric coupled multiferroic material, its preparation method, and its uses. This invention provides a hafnium oxide-based single magnetoelectric coupled multiferroic material with good magnetoelectric coupling performance.

[0005] This invention provides a hafnium oxide-based single magnetoelectric coupled multiferroic material with the chemical formula (Co). y Fe 1-y ) z (Hf x Zr 1-x ) 1-z O2, where x = 0.2 - 0.4, y = 0 - 0.48, z = 0.15 - 0.35.

[0006] Optionally, the X-ray diffraction pattern of the hafnium oxide-based single magnetoelectric coupled multiferroic material has a characteristic peak at 30.2°.

[0007] Optionally, the macroscopic magnetoelectric coupling coefficient of the hafnium oxide-based single magnetoelectric coupled multiferroic material is 1×10⁻⁶. 5 mV·cm -1 ·Oe -1 -4×10 5 mV·cm -1 ·Oe -1 .

[0008] Optionally, the thickness of the hafnium oxide-based single magnetoelectric coupling multiferroic material is 8-12 nm.

[0009] Alternatively, x = 0.3.

[0010] Alternatively, z = 0.17-0.23.

[0011] The present invention also provides a method for preparing the hafnium oxide-based single magnetoelectric coupled multiferroic material as described in any of the foregoing technical solutions, comprising the following steps:

[0012] Using HfO2, ZrO2, and CoFe2O4 / Co3O4 targets as targets, hafnium oxide-based single magnetoelectric coupled multiferroic materials were obtained by alternating deposition on the substrate using pulsed laser co-deposition.

[0013] Optionally, the number of deposition pulses for the HfO2 target in a single growth cycle is 50, the number of deposition pulses for the ZrO2 target is 100, the number of deposition pulses for the CoFe2O4 target is 15-60, and the number of deposition pulses for the Co3O4 target is 15.

[0014] Optionally, the substrate comprises, from bottom to top, a strontium titanate substrate layer and a lanthanum strontium manganese oxide bottom electrode layer, wherein the hafnium oxide-based single magnetoelectric coupled multiferroic material is deposited on the lanthanum strontium manganese oxide bottom electrode layer.

[0015] The present invention also provides the use of hafnium oxide-based single magnetoelectric coupled multiferroic material as described in any of the above technical solutions or hafnium oxide-based single magnetoelectric coupled multiferroic material prepared by any of the above technical solutions in electronic devices.

[0016] This invention provides a hafnium oxide-based single magnetoelectric coupled multiferroic material with the chemical formula (Co). y Fe 1-y ) z (Hf x Zr 1-x ) 1-z O2, where x = 0.2-0.4, y = 0-0.48, z = 0.15-0.34. This invention relates to Hf 1-x Zr x By introducing Co and Fe into O2, the resulting material exhibits both room-temperature ferroelectricity and ferromagnetism, demonstrating excellent magnetoelectric coupling.

[0017] Furthermore, the method for preparing hafnium oxide-based single magnetoelectric coupled multiferroic materials provided by this invention is simple and can be prepared by pulsed laser co-deposition.

[0018] The hafnium oxide-based single magnetoelectric coupling multiferroic material provided by this invention can be applied to electronic devices, providing more options for the fabrication of electronic devices. Attached Figure Description

[0019] The above and other objects, features, and advantages of the invention will be apparent from the following description of preferred embodiments illustrating the gist of the invention and its use, and the accompanying drawings, in which:

[0020] Figure 1 The images shown are transmission electron microscope (TEM) images of the cross section of the hafnium oxide-based single magnetoelectric coupled multiferroic material obtained in Example 2, where (a)-(c) are TEM images of the cross section along the [-110] zone axis of the substrate at different magnifications, and (d)-(f) are TEM images of the cross section along the

[001] zone axis of the substrate at different magnifications.

[0021] Figure 2 The images show the XRD patterns of the hafnium oxide-based single magnetoelectric coupled multiferroic materials obtained in Examples 1-4 and the thin film obtained in Comparative Example 1.

[0022] Figure 3 The in-plane and out-of-plane magnetization curves (MH curves) of the materials obtained in Examples 1-4 and Comparative Examples 1-2 are shown, where (a) is the in-plane MH curve of Examples 1-3 and Comparative Example 1, (b) is the out-of-plane MH curve of Examples 1-3 and Comparative Example 1, (c) is the in-plane MH curve of Examples 1, 4 and Comparative Example 2, and (d) is the out-of-plane MH curve of Examples 1, 4 and Comparative Example 2.

[0023] Figure 4 The hysteresis loop test results of the materials obtained in Examples 1, 2 and Comparative Example 1 are shown.

[0024] Figure 5 The hysteresis loop test results of the thin film materials obtained in Examples 1, 4 and Comparative Example 2 are shown.

[0025] Figure 6 The amplitude curve of the material obtained in Example 1 varies with the in-plane magnetic field strength.

[0026] Figure 7 The results of macroscopic magnetoelectric coupling tests are shown, where (a) is a comparison of the PUND transient current test results of the material obtained in Example 1 with and without an applied in-plane magnetic field (3kOe); (b) is a graph showing the change in remanent polarization intensity of the materials obtained in Examples 1, 2, 4 and Comparative Example 2 as a function of the in-plane magnetic field strength; and (c) is a graph showing the change in out-of-plane remanent polarization intensity of the material obtained in Example 1 as a function of the in-plane magnetic field strength [-110]. STO and

[001] STO The graph shows the variation of the magnetic field strength applied to the crystal orientation. (d) is a graph showing the results of magnetic field cycling test on the material obtained in Example 1. Detailed Implementation

[0027] The present invention will be described below through specific embodiments. Those skilled in the art will understand that the specific embodiments described below are for illustrative purposes only and do not limit the scope of the invention in any way. Furthermore, in the following embodiments, unless otherwise specified, the reagents and equipment used are commercially available. If specific processing conditions and methods are not explicitly described in the following embodiments, conditions and methods known in the art can be used for processing.

[0028] This invention provides a hafnium oxide-based single magnetoelectric coupled multiferroic material with the chemical formula (Co). y Fe 1-y ) z (Hf x Zr 1-x ) 1-z O2, where x = 0.2-0.4, y = 0-0.48, z = 0.15-0.35. The material provided by this invention is Co-doped or Co / Fe co-doped Hf. x Zr 1-x O2(HZO) materials, by introducing Co and Fe, introduce room temperature ferromagnetism while maintaining the room temperature ferroelectricity of the material, and at the same time, the material exhibits excellent magnetoelectric coupling.

[0029] In some embodiments of the present invention, the X-ray diffraction pattern of the hafnium oxide-based single magnetoelectric coupled multiferroic material has a characteristic peak at 30.2°. In the present invention, a characteristic peak at 30.2° means a characteristic peak is present near 30.2°, for example, 30.2° ± 0.3°.

[0030] In some embodiments of the present invention, the macroscopic magnetoelectric coupling coefficient of the hafnium oxide-based single magnetoelectric coupled multiferroic material is 1×10⁻⁶. 5 mV·cm -1 ·Oe -1 -4×10 5 mV·cm -1 ·Oe -1 .

[0031] In some embodiments of the present invention, the thickness of the hafnium oxide-based single magnetoelectric coupled multiferroic material is 8-12 nm, specifically 8 nm, 9 nm, 10 nm, 11 nm, 12 nm, etc.

[0032] In some embodiments of the present invention, x = 0.2-0.4, specifically 0.2, 0.3, 0.4, etc.; z = 0.15-0.35, preferably 0.17-0.23.

[0033] In some embodiments of the present invention, the hafnium oxide-based single magnetoelectric coupled multiferroic material is in the form of a thin film, located on a substrate comprising, from bottom to top, a strontium titanate (STO) substrate layer and a lanthanum strontium manganese oxide (LSMO) bottom electrode layer.

[0034] In another aspect, the present invention provides a method for preparing the hafnium oxide-based single magnetoelectric coupled multiferroic material as described in any of the above technical solutions, comprising the following steps:

[0035] Using HfO2, ZrO2, and CoFe2O4 / Co3O4 targets as targets, hafnium oxide-based single magnetoelectric coupled multiferroic materials were obtained by alternating deposition on the substrate using pulsed laser co-deposition.

[0036] The hafnium oxide-based single magnetoelectric coupled multiferroic material provided by this invention can be prepared by a relatively mature and widely applicable pulsed laser co-deposition method. The preparation method is simple and easy to implement.

[0037] In some embodiments of the present invention, the deposition pulse number for the HfO2 target in a single growth cycle is 50, the deposition pulse number for the ZrO2 target is 100, the deposition pulse number for the CoFe2O4 target is 15-60, and the deposition pulse number for the Co3O4 target is 15. In this invention, those skilled in the art can adjust the deposition pulse number of the CoFe2O4 target according to the desired amount of Co and Fe co-doping.

[0038] In some embodiments of the present invention, the substrate comprises, from bottom to top, a strontium titanate substrate layer and a lanthanum strontium manganese oxide bottom electrode layer, wherein the hafnium oxide-based single magnetoelectric coupled multiferroic material is deposited on the lanthanum strontium manganese oxide bottom electrode layer; the strontium titanate substrate layer is a single-crystal strontium titanate substrate layer. In some embodiments of the present invention, the thickness of the lanthanum strontium manganese oxide bottom electrode layer is 8-12 nm, for example, 8 nm, 9 nm, 10 nm, 11 nm, 12 nm, etc. Those skilled in the art can adjust the thickness as needed.

[0039] The present invention also provides the use of hafnium oxide-based single magnetoelectric coupled multiferroic material as described in any of the above technical solutions or hafnium oxide-based single magnetoelectric coupled multiferroic material prepared by the preparation method described in any of the above technical solutions in electronic devices.

[0040] In some embodiments of the present invention, the electronic device includes a magnetoelectric sensor, a magnetoelectric memory, a tunable inductor and filter, an energy recovery device, a magnetoelectric sensor, and an in-memory computing logic device.

[0041] The technical solutions of the present invention will be clearly and completely described below with reference to the accompanying drawings and embodiments. The embodiments of this application are only examples, and all other embodiments obtained by those skilled in the art without creative effort are within the scope of protection of the present invention.

[0042] The STO / LSMO substrates used in the embodiments of this invention were all prepared by the following method:

[0043] A 10 nm thick LSMO bottom electrode layer was deposited on an STO single-crystal substrate using pulsed laser deposition (PLD) with LSMO as the target material, resulting in an STO / LSMO substrate. The deposition temperature was 800 °C, the oxygen partial pressure was 100 mTorr, and the laser energy density was 1.5 J / cm². 2 The number of pulses is 2000, and the pulse frequency is 5Hz.

[0044] Example 1

[0045] A 10 nm hafnium oxide-based single magnetoelectric coupled multiferroic material was prepared on an STO / LSMO substrate by alternating deposition of HfO2, ZrO2, and CoFe2O4 (CFO) targets using pulsed laser co-deposition. The deposition temperature was 850 °C, the oxygen partial pressure was 100 mTorr, and the laser energy density was 1.5 J / cm². 2 In a single growth cycle, the deposition pulse number for the HfO2 target was 50, for the ZrO2 target it was 100, and for the CoFe2O4 target it was 15, with a pulse frequency of 2 Hz. X-ray photoelectron spectroscopy (XPS) was used to analyze the material, revealing its chemical formula to be (Co...). 0.47 Fe 0.53 ) 0.17 (Hf 0.3 Zr 0.7 ) 0.83 O2, denoted as HZO-L.

[0046] Example 2

[0047] Hafnium oxide-based single magnetoelectric coupled multiferroic materials were prepared using the method shown in Example 1, with the only difference being that the deposition pulse number of the CoFe2O4 target was 35. XPS analysis was performed on the material, and its chemical formula was obtained as (Co... 0.48 Fe 0.52 ) 0.23 (Hf 0.3 Zr 0.7 ) 0.77 O2, denoted as HZO-M.

[0048] Example 3

[0049] Hafnium oxide-based single magnetoelectric coupled multiferroic materials were prepared using the method shown in Example 1, with the only difference being that the deposition pulse number of the CoFe2O4 target was 60. XPS analysis was performed on the material, and its chemical formula was obtained as (Co... 0.47 Fe 0.53 ) 0.35 (Hf 0.3 Zr 0.7 ) 0.65 O2, denoted as HZO-H.

[0050] Example 4

[0051] Hafnium oxide-based single magnetoelectric coupled multiferroic materials were prepared using the method described in Example 1, with the only difference being that the CoFe2O4 target was replaced with a Co3O4 target, and the deposition pulse number for the Co3O4 target was 15. XPS analysis was performed on the material, revealing its chemical formula to be Co. 0.17 (Hf 0.3 Zr 0.7 ) 0.83 O2, denoted as HZO-Co.

[0052] Comparative Example 1

[0053] The thin film was prepared using the method of Example 1, except that a CFO target was not used. XPS analysis was performed on the thin film material, and its chemical formula was determined to be Hf. 0.3 Zr 0.7 O2, denoted as undoped-HZO.

[0054] Comparative Example 2

[0055] Thin films were prepared using the method described in Comparative Example 1, with the only difference being that the CFO target was replaced with an Fe3O4 target. XPS analysis was performed on the thin film material, revealing its chemical formula to be Fe3O4. 0.17 (Hf 0.3 Zr 0.7 ) 0.83 O2, denoted as HZO-Fe.

[0056] 1. Microstructure characterization

[0057] The cross-section of the hafnium oxide-based single magnetoelectric coupled multiferroic material obtained in Example 2 was characterized using transmission electron microscopy (TEM), and the results are as follows: Figure 1 As shown, (a)-(c) are TEM images at different magnifications of the cross-section along the [-110] zone axis of the substrate, and (d)-(f) are TEM images at different magnifications of the cross-section along the

[001] zone axis of the substrate. Figure 1As can be seen, the film obtained in Example 2 is a single, continuous film with a smooth and even interface with the LSMO. The materials obtained in other examples also have similar morphologies.

[0058] 2. X-ray diffraction (XRD) characterization

[0059] XRD analysis was performed on the hafnium oxide-based single magnetoelectric coupled multiferroic materials obtained in Examples 1-4 and the thin film obtained in Comparative Example 1. The results are as follows: Figure 2 As shown, Cu-Kα radiation is used, and the characteristic peaks are represented by a 2θ diffraction angle. Figure 2 It can be seen that the hafnium oxide-based single magnetoelectric coupled multiferroic materials obtained in Examples 1-4 and Comparative Example 1 both showed characteristic peaks around 30.2, but the characteristic peaks shifted slightly with the doping amount, indicating that the crystal structure of the hafnium oxide-based single magnetoelectric coupled multiferroic material provided by the present invention will change to a certain extent with the change of doping amount.

[0060] 3. Ferromagnetic characterization

[0061] The in-plane and out-of-plane magnetization curves (MH curves) of the materials obtained in Examples 1-4 and Comparative Examples 1-2 were measured at room temperature using a vibrating sample magnetometer (VSM). The results are as follows: Figure 3 As shown, where M is the magnetization intensity and H is the applied magnetic field intensity, (a) is the in-plane MH curve for Examples 1-3 and Comparative Example 1, (b) is the out-of-plane MH curve for Examples 1-3 and Comparative Example 1, (c) is the in-plane MH curve for Examples 1, 4 and Comparative Example 2, and (d) is the out-of-plane MH curve for Examples 1, 4 and Comparative Example 2. Figure 3 It can be seen that for HZO thin films, almost no magnetization signal can be detected in either aspect, while the thin film materials obtained in Examples 1-4 and Comparative Example 2 all showed magnetization signals. Furthermore, when Co and Fe are co-doped, the saturation magnetization increases with the increase of the Co and Fe ratio, indicating that Co doping alone or co-doping with Fe imparts room temperature ferromagnetism to the material.

[0062] 4. Ferroelectricity characterization

[0063] The materials obtained in Examples 1, 2, and Comparative Example 1 were fabricated into metal-ferroelectric layer-metal (MFM) two-terminal devices, and hysteresis loop tests were performed using the Positive-Up-Negative-Down (PUND) method. The results are as follows: Figure 4 As shown. By Figure 4 It can be seen that as the Co / Fe doping concentration increases, the remanent polarization intensity of the material decreases significantly.

[0064] The hysteresis loop tests of the thin film materials obtained in Examples 1, 4 and Comparative Example 2 using the PUND method were as follows: Figure 5 As shown. By Figure 5 It can be seen that Fe and Co-doped HZO films have remanent polarization and coercive field similar to those of Co / Fe co-doped films.

[0065] 5. Characterization of magnetoelectric coupling performance

[0066] (1) Microscopic magnetoelectric coupling test

[0067] In-situ analysis of the piezoelectric response of the material obtained in Example 1 under a magnetic field was performed using piezoelectric microscopy (SS-PFM). The results are as follows: Figure 6 As shown. By Figure 6 It can be seen that the amplitude of the piezoelectric response increases significantly with the increase of the in-plane magnetic field strength. This indicates that the magnetic field strength applied in the in-plane direction has a significant enhancing effect on the ferroelectric polarization intensity in the out-of-plane direction of HZO-L, and the material exhibits obvious magnetoelectric coupling behavior. The magnetoelectric coupling coefficient (α) of HZO-L was calculated. 31 The value is 1.37 × 10 5 mV·cm -1 ·Oe -1 .

[0068] (2) Macroscopic magnetoelectric coupling test

[0069] The material obtained in Example 1 was subjected to PUND transient current testing with and without an applied in-plane magnetic field (3 kOe). Figure 7 As shown in (a) in the figure, by Figure 7 As shown in (a), the current intensity under the first positive and negative pulses is contributed by both polarization reversal current and leakage current, while the current intensity under the second pulse signal is entirely contributed by leakage current. The difference between the two over time integrals is the current intensity contributed by polarization reversal, which is an important reference for the magnitude of ferropolarization. The transient current test results show that under the influence of the in-plane magnetic field, the total current inside the sample increases significantly under both positive and negative pulse signals, while the intensity of the current contributed by leakage current remains almost unchanged. This indicates that, on a macroscopic scale, the in-plane magnetic field intensity can cause an enhancement effect on the out-of-plane ferropolarization intensity, a phenomenon consistent with the amplitude results measured in microscopic SS-PFM.

[0070] The changes in remanent polarization intensity (ΔPr) of the materials obtained in Examples 1, 2, 4 and Comparative Example 2 under different in-plane magnetic fields (H) were tested at room temperature. Figure 7 As shown in (b) in the figure), by Figure 7 As shown in (b), within the magnetic field range of 0-3 kOe, the changes in remanent polarization intensity of HZO-L, HZO-M, and HZO-Co all exhibit a monotonically increasing trend with increasing magnetic field strength, demonstrating a significant magnetoelectric coupling effect at the macroscopic scale. However, almost no magnetoelectric coupling effect is observed in HZO-Fe. The calculated α value of HZO-L at the macroscopic scale...31 Approximately 1×10 5 mV·cm -1 ·Oe -1 The results are roughly equivalent to those obtained by SS-PFM, while HZO-M, with a higher doping concentration, α 31 The value is even higher, reaching 3×10 5 mV·cm -1 ·Oe -1 α of HZO-Co 31 The value is 4×10 5 mV·cm -1 ·Oe -1 This indicates that Co-doped and Co / Fe co-doped materials exhibit significant room-temperature magnetoelectric coupling effects.

[0071] The material obtained in Example 1 was tested along the in-plane [-110]. STO and

[001] STO The effect of applying a magnetic field to the crystal orientation on the change in the external remanent polarization (e.g.) Figure 7 As shown in (c) in the figure, by Figure 7 As shown in (c), the above coupling effect is independent of the direction of the applied in-plane magnetic field.

[0072] The material obtained in Example 1 was subjected to magnetic field cyclic testing (e.g. Figure 7 As shown in (d) in the figure, it can be seen that during the repeated cycles of the magnetic field in the range of 0-3k Oe, the out-of-plane ferroelectric remanent polarization intensity also exhibits a reversible cyclic change, indicating that the above-mentioned magnetoelectric coupling effect has good cyclicity and repeatability at room temperature.

[0073] In summary, the hafnium oxide-based single magnetoelectric coupling multiferroic material provided by this invention has a good magnetoelectric coupling effect and can be applied to electronic devices such as magnetoelectric sensors, magnetoelectric memories, tunable inductors and filters, energy recovery devices, magnetoelectric sensors and in-memory computing logic devices.

[0074] Although preferred embodiments of the invention have been shown and described, it is conceivable that those skilled in the art can devise various modifications to the invention within the spirit and scope of the appended claims.

Claims

1. A hafnium oxide-based single magnetoelectric coupling multiferroic material, with the chemical formula (Co... y Fe 1-y ) z (Hf x Zr 1-x ) 1-z O2, where x = 0.2-0.4, y = 0.47-0.48 or 1, z = 0.15-0.

35.

2. The hafnium oxide-based single magnetoelectric coupled multiferroic material according to claim 1, characterized in that, The X-ray diffraction pattern of the hafnium oxide-based single magnetoelectric coupled multiferroic material has a characteristic peak at 30.2°.

3. The hafnium oxide-based single magnetoelectric coupled multiferroic material according to claim 1, characterized in that, The macroscopic magnetoelectric coupling coefficient of the hafnium oxide-based monomagnetically coupled multiferroic material is 1×10⁻⁶. 5 mV·cm -1 ·Oe -1 -4×10 5 mV·cm -1 ·Oe -1 .

4. The hafnium oxide-based single magnetoelectric coupled multiferroic material according to claim 1, characterized in that, The thickness of the hafnium oxide-based single magnetoelectric coupling multiferroic material is 8-12 nm.

5. The hafnium oxide-based single magnetoelectric coupled multiferroic material according to claim 1, characterized in that, x＝0.3。 6. The hafnium oxide-based single magnetoelectric coupled multiferroic material according to claim 1, characterized in that, z＝0.17-0.23。 7. A method for preparing a hafnium oxide-based single magnetoelectric coupled multiferroic material according to any one of claims 1-6, comprising the following steps: Using HfO2, ZrO2 and CoFe2O4 / Co3O4 targets as targets, hafnium oxide-based single magnetoelectric coupled multiferroic materials were obtained by alternating deposition on the substrate using pulsed laser co-deposition. The deposition conditions were as follows: deposition temperature 850℃, oxygen partial pressure 100 mTorr, and laser energy density 1.5 J / cm³. 2 The pulse frequency is 2Hz; The deposition pulse number for HfO2 target in a single growth cycle is 50, for ZrO2 target it is 100, for CoFe2O4 target it is 15-60, and for Co3O4 target it is 15.

8. The preparation method according to claim 7, characterized in that, The substrate comprises, from bottom to top, a strontium titanate substrate layer and a lanthanum strontium manganese oxide bottom electrode layer, wherein the hafnium oxide-based single magnetoelectric coupled multiferroic material is deposited on the lanthanum strontium manganese oxide bottom electrode layer.

9. Use of the hafnium oxide-based single magnetoelectric coupled multiferroic material according to any one of claims 1-6 or the hafnium oxide-based single magnetoelectric coupled multiferroic material prepared by the preparation method according to any one of claims 7-8 in electronic devices.

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