CN114388691A - Heterojunction material with spin orbit torque effect and preparation method and application thereof - Google Patents
Heterojunction material with spin orbit torque effect and preparation method and application thereof Download PDFInfo
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- AMWRITDGCCNYAT-UHFFFAOYSA-L hydroxy(oxo)manganese;manganese Chemical compound [Mn].O[Mn]=O.O[Mn]=O AMWRITDGCCNYAT-UHFFFAOYSA-L 0.000 claims abstract description 104
- HTXDPTMKBJXEOW-UHFFFAOYSA-N dioxoiridium Chemical compound O=[Ir]=O HTXDPTMKBJXEOW-UHFFFAOYSA-N 0.000 claims abstract description 75
- 229910000457 iridium oxide Inorganic materials 0.000 claims abstract description 63
- 230000005291 magnetic effect Effects 0.000 claims abstract description 30
- 229910003369 La0.67Sr0.33MnO3 Inorganic materials 0.000 claims abstract description 20
- 238000000151 deposition Methods 0.000 claims description 79
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- 229910052784 alkaline earth metal Inorganic materials 0.000 claims description 2
- -1 alkaline earth metal cation Chemical class 0.000 claims description 2
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- 229910001427 strontium ion Inorganic materials 0.000 claims description 2
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- 239000010408 film Substances 0.000 description 12
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- 238000009210 therapy by ultrasound Methods 0.000 description 10
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- 229910002370 SrTiO3 Inorganic materials 0.000 description 4
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- KTUFCUMIWABKDW-UHFFFAOYSA-N oxo(oxolanthaniooxy)lanthanum Chemical compound O=[La]O[La]=O KTUFCUMIWABKDW-UHFFFAOYSA-N 0.000 description 4
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 4
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- 230000005290 antiferromagnetic effect Effects 0.000 description 2
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- FAQYAMRNWDIXMY-UHFFFAOYSA-N trichloroborane Chemical compound ClB(Cl)Cl FAQYAMRNWDIXMY-UHFFFAOYSA-N 0.000 description 1
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Abstract
The invention discloses a heterojunction material with a spin orbit torque effect, a preparation method and application thereof, wherein the heterojunction material comprises a manganese oxide layer and an iridium oxide layer which are sequentially superposed; the manganese oxide layer is La0.67Sr0.33MnO3A layer; the iridium oxide layer is XIrO3A layer; the iridium oxide in the iridium oxide layer is perovskite type oxide; the thickness of the manganese oxide layer is 3 nm-8 nm; of said iridium oxide layerThe thickness is 5 nm-12 nm. The heterojunction material provided by the invention is an iridium oxide-based heterojunction thin film material with a remarkable spin-orbit torque effect. The material achieves the purpose of adjusting the heterojunction spin orbit torque effect by regulating and controlling the magnetic coupling performance of the heterojunction interface, so that the material has wide application potential in the fields of magnetic information storage, nano oscillators and the like.
Description
Technical Field
The invention relates to the technical field of memories, in particular to a heterojunction material with a spin orbit torque effect and a preparation method and application thereof.
Background
Magnetic Random Access Memory (MRAM) is a new type of nonvolatile Memory that uses electron spin current to replace charge current to realize information storage, has the advantages of low power consumption, long service life, non-volatility, extreme temperature resistance, etc., is more compatible with the current Complementary Metal Oxide Semiconductor (CMOS) Semiconductor process, and is a new technical route that is most hopeful to replace Semiconductor transistors at micrometer scale.
The SOT-MRAM uses Spin-orbit Torque (SOT) effect, so that electron Spin current is generated in a direction perpendicular to the thin film due to Spin hall effect and other mechanisms, which can cause magnetic moment reversal of an adjacent magnetic layer in a magnetic tunnel junction, thereby completing the information storage process. The SOT-MRAM has the characteristics of high writing speed and short initial delay, overcomes the limitation of the bandwidth of the current memory chip, and has obvious advantages in the directions of edge calculation, AI and the like. One technical difficulty of the SOT-MRAM device in the related art is how to implement full current regulation and control of the magnetic sequence without an external magnetic field. The exchange bias effect of the interface is an effective form for realizing the switching without an external field by growing the ferromagnetic/antiferromagnetic heterojunction. But the spin-orbit torque effect of the ferromagnetic/antiferromagnetic heterojunction is weak.
Therefore, it is required to develop a heterojunction material having a spin orbit torque effect, which has a significant spin orbit torque effect.
Disclosure of Invention
In order to solve the problems in the prior art, the invention provides a heterojunction material with a spin orbit torque effect, and the heterojunction material has a remarkable spin orbit torque effect.
The invention also provides a preparation method of the heterojunction material with the spin-orbit torque effect.
The invention also provides a magnetic random access memory which is made of the heterojunction material with the spin orbit torque effect.
The invention also provides a nano oscillator which is prepared from the heterojunction material.
A first aspect of the invention provides a heterojunction material with spin-orbit torque effect,
the material comprises a manganese oxide layer and an iridium oxide layer which are sequentially superposed;
the manganese oxide layer is La0.67Sr0.33MnO3A layer;
the iridium oxide layer is XIrO3A layer;
the iridium oxide in the iridium oxide layer is perovskite type oxide;
wherein said XIrO3X in the layer is an alkaline earth metal cation;
the thickness of the manganese oxide layer is 3 nm-8 nm;
the thickness of the iridium oxide layer is 5 nm-12 nm.
According to at least one embodiment of the present invention, the following advantageous effects are provided:
the manganese oxide in the heterojunction material adopts La0.67Sr0.33MnO3(ii) a By making a pair of La0.67Sr0.33MnO3The thickness of the layer is regulated, so that the magnetocrystalline anisotropy energy of the magnetic layer is regulated, a damping-like field induced by heterojunction current is regulated, the interface magnetic coupling state is regulated, and the heterojunction spin-orbit torque effect is finally regulated.
The heterojunction material provided by the invention is an iridium oxide-based heterojunction thin film material with a remarkable spin-orbit torque effect. The material achieves the purpose of adjusting the heterojunction spin orbit torque effect by regulating and controlling the magnetic coupling performance of the heterojunction interface, so that the material has wide application potential in the fields of magnetic information storage, nano oscillators and the like.
Preferably, the manganese oxide layer has a thickness of one of 3nm, 4nm, 5nm, 6nm, 7nm or 8 nm.
The manganese oxide is too thick, so that the spin orbit torque effect is obviously reduced; the manganese oxide is too thin, resulting in discontinuity of the film.
Preferably, the iridium oxide layer has a thickness of one of 5nm, 6nm, 7nm, 8nm, 9nm, 10nm, or 12 nm.
The thickness of the iridium oxide layer is too thick, so that the spin Hall angle of the film is reduced, and the spin current conversion efficiency is reduced; the iridium oxide layer is too thin, which may result in discontinuity of the film.
According to some embodiments of the present invention, a crystal plane of the manganese oxide in the manganese oxide layer is oriented to (001).
According to some embodiments of the invention, the XIrO3X in the layer is at least one of calcium ion or strontium ion.
According to some embodiments of the invention, the XIrO3Layer is CaIrO3Or SrIrO3。
According to some embodiments of the invention, the heterojunction material has a spin-to-torque ratio of 10 to 30.
According to some embodiments of the invention, the heterojunction material has a spin-to-torque ratio of 15 to 30.
According to some embodiments of the invention, the heterojunction material has a spin-to-torque ratio of 20 to 30.
According to some embodiments of the invention, the heterojunction material has a spin-to-torque ratio of 20.
The invention provides a preparation method of the heterojunction material, which comprises the following steps:
and sequentially depositing manganese oxide and iridium oxide on the substrate to form a manganese oxide layer and an iridium oxide layer.
According to at least one embodiment of the present invention, the following advantageous effects are provided:
the preparation method can prepare the heterojunction material with excellent performance only by simple deposition, is simple and easy to implement, and is beneficial to large-scale industrial production.
According to some embodiments of the invention, the substrate is a perovskite-type substrate.
According to some embodiments of the invention, the crystal plane orientation of the perovskite in the perovskite-type substrate is (001).
According to some embodiments of the invention, the perovskite substrate has a unit cell parameter of
According to some embodiments of the invention, the perovskite substrate has a unit cell parameter of
And
one kind of (1).
According to some embodiments of the invention, the perovskite substrate has a lattice mismatch with the heterojunction material of less than 0.8%.
The substrate and the heterojunction material have high lattice parameter matching degree, and the lattice parameter mismatch rate is less than 0.8%.
According to some embodiments of the invention, the perovskite substrate is SrTiO3Substrate, DyScO3Substrate, LaAlO3Substrate, LSAT (LaAlO)3)0.3(Sr2TaAlO6)0.7Substrate, GdScO3 substrate, and NdGaO3One of the substrates.
According to some embodiments of the invention, the SrTiO3The substrate has a cell parameter of
According to some embodiments of the invention, the DyScO3The substrate has a cell parameter of
According to some embodiments of the invention, said LaAlO3The substrate has a cell parameter of
According to some embodiments of the invention, the LSAT substrate has a unit cell parameter of
According to some embodiments of the invention, the GdScO3The substrate has a cell parameter of
According to some embodiments of the invention, the NdGaO3The substrate has a cell parameter of
The crystal quality of the grown heterojunction material film is controlled by controlling the crystal cell parameters and the crystal face orientation of the wafer.
According to some embodiments of the invention, the substrate is pre-treated.
According to some embodiments of the invention, the pre-treatment comprises sonication.
According to some embodiments of the invention, the number of repetitions of the pre-treatment is 1 to 3.
According to some embodiments of the invention, the sonication consists of a first sonication, a second sonication and a third sonication.
According to some embodiments of the invention, the solvent of the first sonication comprises acetone.
According to some embodiments of the invention, the time of the first sonication is between 5min and 10 min.
Preferably, the time of the first sonication is one of 5min, 6min, 7min, 8min, 9min or 10 min.
According to some embodiments of the invention, the solvent of the second sonication comprises isopropanol.
According to some embodiments of the invention, the time of the second sonication is between 5min and 10 min.
Preferably, the time of the second sonication is one of 5min, 6min, 7min, 8min, 9min or 10 min.
According to some embodiments of the invention, the solvent of the third sonication comprises water.
According to some embodiments of the invention, the time of the third sonication is between 3min and 8 min.
Preferably, the time of the third ultrasonic treatment is one of 3min, 4min, 5min, 6min, 7min or 8 min.
According to some embodiments of the invention, the deposition is pulsed laser deposition.
According to some embodiments of the invention, the method of depositing manganese oxide is pulsed laser deposition.
According to some embodiments of the invention, the target material during the deposition of the manganese oxide is La0.67Sr0.33MnO3A target material.
According to some embodiments of the invention, the La0.67Sr0.33MnO3The raw material for preparing the target material is La2O3、SrCO3And MnO2。
According to some embodiments of the invention, the La2O3The SrCO3And said MnO2Is 0.335:0.33: 1.
According to some embodiments of the invention, the La0.67Sr0.33MnO3The preparation method of the target material is a spark plasma sintering method.
According to some embodiments of the invention, the laser energy during deposition of the manganese oxide is 1.0J/cm2～1.8J/cm2。
Preferably, the laser energy during the deposition of the manganese oxide is 1.0J/cm2、1.2J/cm2、1.4J/cm2、1.6J/cm2Or 1.8J/cm2One kind of (1).
According to some embodiments of the invention, the temperature during the deposition of the manganese oxide is between 650 ℃ and 750 ℃.
Preferably, the temperature during the deposition of the deposited manganese oxide is one of 650 ℃, 660 ℃, 670 ℃, 680 ℃, 690 ℃, 700 ℃, 710 ℃, 720 ℃, 730 ℃, 740 ℃ or 750 ℃.
When the temperature is too high, the impure phase of the film can be separated out, the risk of diffusion at the interface is increased, and when the temperature is too low, the film cannot form a phase.
According to some embodiments of the invention, the oxygen pressure during the deposition of the manganese oxide is between 0.1mbar and 0.5 mbar.
Preferably, the oxygen pressure during deposition of the manganese oxide is one of 0.1mbar, 0.2mbar, 0.3mbar, 0.4mbar or 0.5 mbar.
According to some embodiments of the invention, the time during the deposition of the manganese oxide is between 1.5min and 4 min.
According to some embodiments of the invention, the iridium oxide deposition process is a pulsed laser deposition process.
According to some embodiments of the present invention, the target material during deposition of the iridium oxide is XIrO3A target material.
According to some embodiments of the invention, the XIrO3The target material comprises an alkaline earth iridium oxide target material.
According to some embodiments of the invention, the XIrO3The target comprises SrIrO3Target or CaIrO3A target material.
According to some embodiments of the invention, the XIrO3The preparation raw material of the target material is XCO3And IrO2。
According to some embodiments of the invention, the XCO3And said IrO2Is 1: 1.
According to some embodiments of the invention, the XIrO3Preparation method of target material and packageThe method comprises the following steps: will said XCO3And said IrO2And (4) carrying out discharge plasma sintering after planetary ball milling to obtain the material.
According to some embodiments of the invention, the SrIrO3The target material is prepared from SrCO3And IrO2。
According to some embodiments of the invention, the SrCO3And said IrO2Is 1: 1.
According to some embodiments of the invention, the SrIrO3The preparation method of the target comprises the following steps: mixing the SrCO3And said IrO2And (4) carrying out discharge plasma sintering after planetary ball milling to obtain the material.
According to some embodiments of the invention, the CaIrO3The raw material for preparing the target material is CaCO3And IrO2。
According to some embodiments of the invention, the CaCO3And said IrO2Is 1: 1.
According to some embodiments of the invention, the CaIrO3The preparation method of the target comprises the following steps: the CaCO is3And said IrO2And (4) carrying out discharge plasma sintering after planetary ball milling to obtain the material.
According to some embodiments of the invention, the laser energy during the deposition of the iridium oxide is 0.8J/cm2～1.6J/cm2。
According to some embodiments of the invention, the temperature during the deposition of the iridium oxide is between 600 ℃ and 700 ℃.
Preferably, the temperature during deposition of the iridium oxide is at least one of 600 ℃, 610 ℃, 620 ℃, 630 ℃, 640 ℃, 650 ℃, 660 ℃, 670 ℃, 680 ℃, 690 ℃ or 700 ℃.
The temperature for depositing the iridium oxide is too high, so that the Ir element is precipitated; the deposition temperature for depositing the iridium oxide layer is too low, which results in poor crystallinity of the film.
According to some embodiments of the invention, the oxygen pressure during the deposition of the iridium oxide is between 0.16mbar and 0.2 mbar.
According to some embodiments of the invention, the oxygen pressure during the deposition of the iridium oxide is one of 0.16bar, 0.17bar, 0.18bar, 0.19bar or 0.20 bar.
According to some embodiments of the invention, the deposition time during the deposition of the iridium oxide is 1min to 4 min.
According to some embodiments of the invention, the SrIrO3The laser energy in the deposition process of (2) is 0.8J/cm2～1.6J/cm2。
According to some embodiments of the invention, the SrIrO3The temperature in the deposition process is 600-700 ℃.
Preferably, the SrIrO3The temperature in the deposition process of (a) is at least one of 600 ℃, 610 ℃, 620 ℃, 630 ℃, 640 ℃, 650 ℃, 660 ℃, 670 ℃, 680 ℃, 690 ℃ or 700 ℃.
According to some embodiments of the invention, the SrIrO3The oxygen pressure during the deposition process of (2) is 0.16mbar to 0.2 mbar.
According to some embodiments of the invention, the SrIrO3The oxygen pressure during deposition of (a) is one of 0.16bar, 0.17bar, 0.18bar, 0.19bar or 0.20 bar.
According to some embodiments of the invention, the SrIrO3The deposition time in the deposition process is 1min to 4 min.
According to some embodiments of the invention, the CaIrO3The laser energy in the deposition process of (2) is 0.8J/cm2～1.6J/cm2。
According to some embodiments of the invention, the CaIrO3The temperature in the deposition process is 600-700 ℃.
Preferably, said CaIrO3The temperature in the deposition process of (a) is at least one of 600 ℃, 610 ℃, 620 ℃, 630 ℃, 640 ℃, 650 ℃, 660 ℃, 670 ℃, 680 ℃, 690 ℃ or 700 ℃.
According to some embodiments of the invention, the CaIrO3The oxygen pressure during the deposition process of (2) is 0.16mbar to 0.2 mbar.
According to some embodiments of the invention, the CaIrO3The oxygen pressure during deposition of (a) is one of 0.16bar, 0.17bar, 0.18bar, 0.19bar or 0.20 bar.
According to some embodiments of the invention, the CaIrO3The deposition time in the deposition process is 1min to 4 min.
According to some embodiments of the invention, the method of preparing a heterojunction material further comprises annealing after deposition.
The purpose of the anneal is to remove possible oxygen vacancies.
According to some embodiments of the invention, the oxygen pressure of the annealing is between 0.4bar and 0.8 bar.
Preferably, the oxygen pressure of the annealing is one of 0.4bar, 0.5bar, 0.6bar, 0.7bar or 0.8 bar.
According to some embodiments of the invention, the temperature of the annealing is between 600 ℃ and 700 ℃.
Preferably, the annealing temperature is one of 600 ℃, 610 ℃, 620 ℃, 630 ℃, 640 ℃, 650 ℃, 660 ℃, 670 ℃, 680 ℃, 690 ℃ or 700 ℃.
According to some embodiments of the invention, the annealing time is between 0.15h and 0.35 h.
Preferably, the annealing time is one of 0.15h, 0.20h, 0.25h, 0.30h or 0.35 h.
According to some embodiments of the invention, the number of anneals is 2 or 3.
According to some embodiments of the invention, the method of preparing the heterojunction material comprises the steps of:
s1, depositing a manganese oxide layer:
depositing a manganese oxide layer on a substrate by adopting a pulse laser deposition method at the deposition temperature of 650-750 ℃ and the deposition oxygen pressure of 0.1-0.5 mbar;
wherein the laser energy of the pulse laser deposition method is 1.0-1.8J/cm2；
S2, depositing an iridium oxide layer:
depositing an iridium oxide layer on the manganese oxide layer prepared in the step S1 by adopting a pulse laser deposition method at the deposition temperature of 600-700 ℃ and the deposition oxygen pressure of 0.16-0.2 mbar to form the heterojunction material;
wherein the laser energy of the pulse laser deposition method is 0.8J/cm2～1.6J/cm2；
S3, annealing:
annealing for the first time for 20min to 40min at the temperature of 600 ℃ to 700 ℃ and the oxygen pressure of 0.4bar to 0.8bar, and cooling;
annealing again at 600-700 deg.C and oxygen pressure of 0.4-0.8 bar for 20-40 min, and cooling to room temperature.
According to some embodiments of the invention, the room temperature is 20 ℃ to 30 ℃.
The purpose of primary annealing cooling is as follows: cooling at a rate of two hours, i.e. cooling to room temperature
According to some embodiments of the invention, the surface of the heterojunction material is further grown with a protective layer.
According to some embodiments of the invention, the protective layer comprises SrTiO3And (3) a layer.
According to some embodiments of the invention, the method of preparing the protective layer comprises the steps of:
depositing a protective layer on the iridium oxide layer by adopting a pulse laser deposition method at the deposition temperature of 600-700 ℃ and the deposition oxygen pressure of 0.16-0.2 mbar;
wherein the laser energy of the laser deposition method is 1.0J/cm2～1.8J/cm2。
According to some embodiments of the invention, the protective layer deposition temperature should be no higher than the iridium oxide layer deposition temperature.
The third aspect of the present invention provides a magnetic random access memory made of the above-mentioned heterojunction material having the spin-orbit torque effect.
The fourth aspect of the present invention provides a nanooscillator made of the above heterojunction material having spin orbit torque effect.
According to at least one embodiment of the invention, the following beneficial effects are achieved:
the heterojunction material provided by the invention has a strong spin orbit torque effect. By adjusting the thickness of the heterojunction film and the annealing process, the interface magnetic coupling performance can be effectively regulated and controlled, so that the spin orbit torque in the heterojunction can be adjusted. The spin-torque ratio theta of the heterojunction provided by the inventionSTIs 20.
The preparation method provided by the invention is simple and feasible, can be industrially popularized and has a certain application value in the field of information storage.
Drawings
FIG. 1 is a schematic structural diagram of a heterojunction material prepared in embodiments 1-3 of the present invention.
Fig. 2 is a diagram of a 6-terminal hall device prepared by adopting a micro-nano structure processing technology for the heterojunction material prepared in the embodiment of the invention.
Fig. 3 is a relationship between hall resistance and an included angle between an in-plane magnetic field and current in a forward (reverse) current direction of the heterojunction material prepared in example 1 of the present invention.
Fig. 4 shows the variation of the differential hall resistance with the included angle between the in-plane magnetic field and the current under different forward (reverse) currents of the heterojunction material prepared in example 1 of the present invention.
Fig. 5 shows the variation of current-induced vertical equivalent field with current intensity of the heterojunction material prepared in example 1 of the present invention.
Figure 6 is an XRD spectrum diagram of the heterojunction material prepared in example 1 of the present invention.
Reference numerals:
100. a substrate; 101. a manganese oxide layer; 102. an iridium oxide layer; 103. and a protective layer.
Detailed Description
The concept and technical effects of the present invention will be clearly and completely described below in conjunction with the embodiments to fully understand the objects, features and effects of the present invention. It is obvious that the described embodiments are only a part of the embodiments of the present invention, and not all embodiments, and those skilled in the art can obtain other embodiments without inventive effort based on the embodiments of the present invention, and all embodiments are within the protection scope of the present invention.
In the description of the present invention, reference to the description of the terms "one embodiment," "some embodiments," "an illustrative embodiment," "an example," "a specific example," or "some examples," etc., means that a particular feature, structure, material, or characteristic described in connection with the embodiment or example is included in at least one embodiment or example of the present invention. In this specification, the schematic representations of the terms used above do not necessarily refer to the same embodiment or example. Furthermore, the particular features, structures, materials, or characteristics described may be combined in any suitable manner in any one or more embodiments or examples.
Specific examples of the present invention are described in detail below.
Example 1
The embodiment is a preparation method of a heterojunction material with spin-orbit torque effect, which comprises the following steps:
s1, ultrasonic treatment:
SrTiO with one side polished by ultrasonic wave3(001) The single crystal substrate is respectively subjected to ultrasonic treatment in acetone for 10min, isopropanol for 10min and water for 5min, and the ultrasonic treatment process in the step is repeated twice.
S2 deposition of La0.67Sr0.33MnO3Layer (b):
adopting pulse laser deposition method at 700 deg.C under 0.3mbar oxygen pressure, and using La0.67Sr0.33MnO3The distance between the target material and the substrate is 4.5cm and is 1.4J/cm2SrTiO treated at step S1 under laser energy3(001) Depositing La with thickness of 5nm on the substrate for 2.5min0.67Sr0.33MnO3And (3) a layer.
S3 deposition of SrIrO3Layer (b):
adopting a pulsed laser deposition method at the deposition temperature of 650 ℃ and the oxygen pressure of 0.18mbar and using SrIrO3Is a target material. The distance between the target and the substrate is 4.5cm and is 1.2J/cm2Under laser energy, La has been prepared in step S20.67Sr0.33MnO3SrTiO of layer3Depositing SrIrO with the thickness of 8nm on a single crystal substrate for 2min3And (3) a layer.
S4, annealing:
after the deposition is finished, annealing the product prepared in the step S3 in situ for 0.25h at 650 ℃ under the oxygen pressure of 0.6bar, and then cooling to room temperature within 2 h;
and annealing in situ again at 650 ℃ under the oxygen pressure of 0.6bar for 0.25h, and then cooling to room temperature within 2h to complete the growth of the heterojunction material on the substrate.
La in this example0.67Sr0.33MnO3The preparation method of the target material comprises the following steps:
with La2O3、SrCO3And MnO2The powder is prepared by weighing and mixing the La, Sr and Mn according to the element ratio of 0.67:0.33:1, fully grinding and mixing the materials uniformly, and performing spark plasma sintering to obtain the La0.67Sr0.33MnO3Is a target material.
In this embodiment, SrIrO3The preparation method of the target material comprises the following steps:
with SrCO3And IrO2The powder is weighed and proportioned according to the proportion of Sr and Ir elements of 1:1, fully ground and uniformly mixed, and then is subjected to spark plasma sintering to obtain SrIrO3Is a target material.
The structure of the heterojunction material prepared in this example is shown in fig. 1, and comprises a manganese oxide layer 101 (La) in sequence0.67Sr0.33MnO3Layer) and iridium oxide layer 102 (SrIrO)3A layer);
manganese oxide layer 101 (La)0.67Sr0.33MnO3Layers) are grown on the substrate 100; manganese oxide layer 101 (La)0.67Sr0.33MnO3Layer) has a thickness of 5 nm;
iridium oxide layer 102 (SrIrO)3Layer) is grown on the manganese oxide layer 101 (La)0.67Sr0.33MnO3Layer); iridium oxide layer 102 (SrIrO)3Layer) having a thickness of 8 nm; iridium oxide layer 102 (SrIrO)3Layer) of SrIrO3Has a crystal plane orientation of (001);
the surface of the iridium oxide layer 102 is also grown with a protective layer 103.
The preparation method of the protective layer 103 in this embodiment includes the following steps:
adopting a pulsed laser deposition method to prepare SrTiO material at the deposition temperature of 650 ℃ and the oxygen pressure of 0.18mbar3Is a target material. The distance between the target and the substrate is 4.5cm and is 1.2J/cm2Depositing SrTiO with the thickness of 8nm on the substrate annealed in the step S4 for 2min under laser energy3And (3) a layer.
Example 2
The embodiment is a preparation method of a heterojunction material with spin-orbit torque effect, which comprises the following steps:
s1, ultrasonic treatment:
SrTiO with one side polished by ultrasonic wave3(001) The single crystal substrate is respectively subjected to ultrasonic treatment in acetone for 10min, isopropanol for 10min and water for 5min, and the ultrasonic treatment process in the step is repeated twice.
S2 deposition of La0.67Sr0.33MnO3Layer (b):
adopting pulse laser deposition method at 700 deg.C under 0.3mbar oxygen pressure, and using La0.67Sr0.33MnO3The distance between the target material and the substrate is 4.5cm and is 1.4J/cm2SrTiO treated at step S1 under laser energy3(001) Depositing La with thickness of 8nm on the substrate for 4min0.67Sr0.33MnO3And (3) a layer.
S3 deposition of SrIrO3Layer (b):
adopting a pulsed laser deposition method at the deposition temperature of 650 ℃ and the oxygen pressure of 0.18mbar and using SrIrO3Is a target material. The distance between the target and the substrate is 4.5cm and is 1.2J/cm2Under laser energy, La has been prepared in step S20.67Sr0.33MnO3SrTiO of layer3Depositing SrIrO with the thickness of 8nm on a single crystal substrate for 2min3And (3) a layer.
S4, annealing:
after the deposition is finished, annealing the product prepared in the step S3 in situ for 0.25h at 650 ℃ under the oxygen pressure of 0.6bar, and then cooling to room temperature within 2 h;
and annealing in situ again at 650 ℃ under the oxygen pressure of 0.6bar for 0.25h, and then cooling to room temperature within 2h to complete the growth of the heterojunction material on the substrate.
La in this example0.67Sr0.33MnO3The preparation method of the target material comprises the following steps:
with La2O3、SrCO3And MnO2The powder is prepared by weighing and mixing the La, Sr and Mn according to the element ratio of 0.67:0.33:1, fully grinding and mixing the materials uniformly, and performing spark plasma sintering to obtain the La0.67Sr0.33MnO3Is a target material.
In this embodiment, SrIrO3The preparation method of the target material comprises the following steps:
with SrCO3And IrO2The powder is weighed and proportioned according to the proportion of Sr and Ir elements of 1:1, fully ground and uniformly mixed, and then is subjected to spark plasma sintering to obtain SrIrO3Is a target material.
The structure of the heterojunction material prepared in this example is shown in fig. 1, and comprises a manganese oxide layer 101 (La) in sequence0.67Sr0.33MnO3Layer) and iridium oxide layer 102 (SrIrO)3A layer);
manganese oxide layer 101 (La)0.67Sr0.33MnO3Layers) are grown on the substrate 100; manganese oxide layer 101 (La)0.67Sr0.33MnO3Layer) having a thickness of 8 nm;
iridium oxide layer 102 (SrIrO)3Layer) is grown on the manganese oxide layer 101 (La)0.67Sr0.33MnO3Layer); iridium oxide layer 102 (SrIrO)3Layer) having a thickness of 8 nm; iridium oxide layer 102 (SrIrO)3Layer) of SrIrO3Has a crystal plane orientation of (001);
the surface of the iridium oxide layer 102 is also grown with a protective layer 103.
The preparation method of the protective layer 103 in this embodiment includes the following steps:
adopting a pulsed laser deposition method to prepare SrTiO material at the deposition temperature of 650 ℃ and the oxygen pressure of 0.18mbar3Is a target material. Target material andthe distance between the substrates was 4.5cm at 1.2J/cm2Depositing SrTiO with the thickness of 8nm on the substrate annealed in the step S4 for 2min under laser energy3And (3) a layer.
Example 3
The embodiment is a preparation method of a heterojunction material with spin-orbit torque effect, which comprises the following steps:
s1, ultrasonic treatment:
SrTiO with one side polished by ultrasonic wave3(001) The single crystal substrate is respectively subjected to ultrasonic treatment in acetone for 10min, isopropanol for 10min and water for 5min, and the ultrasonic treatment process in the step is repeated twice.
S2 deposition of La0.67Sr0.33MnO3Layer (b):
adopting pulse laser deposition method at 700 deg.C under 0.3mbar oxygen pressure, and using La0.67Sr0.33MnO3The distance between the target material and the substrate is 4.5cm and is 1.4J/cm2SrTiO treated at step S1 under laser energy3(001) Depositing La with thickness of 10nm on the substrate for 5min0.67Sr0.33MnO3And (3) a layer.
S3 deposition of SrIrO3Layer (b):
adopting a pulsed laser deposition method at the deposition temperature of 650 ℃ and the oxygen pressure of 0.18mbar and using SrIrO3Is a target material. The distance between the target and the substrate is 4.5cm and is 1.2J/cm2Under laser energy, La has been prepared in step S20.67Sr0.33MnO3SrTiO of layer3Depositing SrIrO with the thickness of 8nm on a single crystal substrate for 2min3And (3) a layer.
S4, annealing:
after the deposition is finished, annealing the product prepared in the step S3 in situ for 0.25h at 650 ℃ under the oxygen pressure of 0.6bar, and then cooling to room temperature within 2 h;
and annealing in situ again at 650 ℃ under the oxygen pressure of 0.6bar for 0.25h, and then cooling to room temperature within 2h to complete the growth of the heterojunction material on the substrate.
La in this example0.67Sr0.33MnO3The preparation method of the target material comprises the following steps:
with La2O3、SrCO3And MnO2The powder is prepared by weighing and mixing the La, Sr and Mn according to the element ratio of 0.67:0.33:1, fully grinding and mixing the materials uniformly, and performing spark plasma sintering to obtain the La0.67Sr0.33MnO3Is a target material.
In this embodiment, SrIrO3The preparation method of the target material comprises the following steps:
with SrCO3And IrO2The powder is weighed and proportioned according to the proportion of Sr and Ir elements of 1:1, fully ground and uniformly mixed, and then is subjected to spark plasma sintering to obtain SrIrO3Is a target material.
The structure of the heterojunction material prepared in this example is shown in fig. 1, and comprises a manganese oxide layer 101 (La) in sequence0.67Sr0.33MnO3Layer) and iridium oxide layer 102 (SrIrO)3A layer);
manganese oxide layer 101 (La)0.67Sr0.33MnO3Layers) are grown on the substrate 100; manganese oxide layer 101 (La)0.67Sr0.33MnO3Layer) has a thickness of 10 nm;
iridium oxide layer 102 (SrIrO)3Layer) is grown on the manganese oxide layer 101 (La)0.67Sr0.33MnO3Layer); iridium oxide layer 102 (SrIrO)3Layer) having a thickness of 8 nm; iridium oxide layer 102 (SrIrO)3Layer) of SrIrO3Has a crystal plane orientation of (001);
the surface of the iridium oxide layer 102 is also grown with a protective layer 103.
The preparation method of the protective layer 103 in this embodiment includes the following steps:
adopting a pulsed laser deposition method to prepare SrTiO material at the deposition temperature of 650 ℃ and the oxygen pressure of 0.18mbar3Is a target material. The distance between the target and the substrate is 4.5cm and is 1.2J/cm2Depositing SrTiO with the thickness of 8nm on the substrate annealed in the step S4 for 2min under laser energy3And (3) a layer.
Test example
Preparing a Hall device:
and spin-coating the grown film with positive ultraviolet photoresist at the rotation speed of 4000 rpm for 60s, and baking at 100 ℃ for 1 min.
By adopting an ultraviolet exposure process, a Hall pattern with the length of 40 mu m and the width of 10 mu m is obtained by exposure and development, and the development time is 40 s. Using a reactive ion etching process (Cl)2+BCl3) And etching the part which is not protected by the photoresist for 2min, and removing the heterojunction material outside the pattern to obtain a Hall bar (Hallbar) pattern of the heterojunction material.
And (3) spin-coating the obtained heterojunction Hall bar with positive ultraviolet photoresist at the rotation speed of 4000r/min for 60s, and baking at 100 ℃ for 1min after the spin-coating is finished. And (3) adopting an ultraviolet exposure process, and carrying out exposure and development to obtain the extraction electrode part connected with the Hall pattern, wherein the development time is 40 s.
And (3) evaporating a Cr (10nm)/Au (60nm) metal electrode on the thin film by using a thermal evaporation process, and finally obtaining a 6-end Hall device shown in figure 2 by using a lift off process, wherein the 6-end Hall device is used for representing the spin-orbit torque effect in the heterojunction material.
The spin-orbit torque performance characterization of the heterojunction material obtained in the embodiment 1 is performed under the condition of a low-temperature strong magnetic field, and the change of the in-plane hall resistance along with the in-plane included angle between the current and the magnetic field direction under the condition that the current in the opposite direction (+/-500 muA) is applied under the magnetic fields of 1.6K and 5T is shown in fig. 3. La0.67Sr0.33MnO3/SrIrO3The Hall resistance of the heterojunction film is periodically changed along with the change of an included angle between a magnetic field and a current direction, when currents in different directions are loaded, the Hall resistance is obviously different from the current direction along with the angle change curve, and the phenomena clearly show that the current-induced damping-like effective field in the heterojunction material is influenced by the spin orbit torque generated by the currents, so that the overturning behavior of the magnetic moment under the magnetic field is influenced, and the phenomenon that the stronger current-induced spin orbit torque effect exists on a heterojunction interface is proved.
FIG. 4 shows the Hall resistance along with the surface under different forward (reverse) currents of the heterojunction material prepared in example 1 of the inventionThe change relationship of the included angle between the magnetic field and the current can be seen from the graph, and the differential Hall resistance induced by the current is increased along with the increase of the current intensity
And also gradually becomes larger.
Fig. 5 shows the variation of the current-induced vertical equivalent field of the heterojunction material prepared in this example 1 with the current and the current intensity, and the generated equivalent field increases with the increase of the current. The resulting spin torque ratio θSTIs 20, which is much larger than Pt/NiFe (theta) in the related artST＝0.08)、Ta/CoFeB(θST0.15) equiheavy metal/ferromagnetic heterojunction.
FIG. 6 is an XRD pattern of a heterojunction material obtained in example 1 of the present invention (LSMO in the figure represents: La)0.67Sr0.33MnO3(ii) a SIO represents: SrIrO3(ii) a STO stands for: SrTiO3) (PDF card LSMO: 00-050-; and SIO: 01-76-0221); from the figures it follows that: the crystal plane orientation of LSMO in the heterojunction material prepared in example 1 of the present invention is (002); the crystal plane of SIO is oriented to (002).
Further, the XRD absorption intensity of the single-crystal epitaxial thin film is viewed in log coordinates (logarithmic coordinates) because: the thin film sample is thin, the signal intensity is weaker than that of the bulk material, and the satellite peak appearing on the XRD spectrum of the invention well explains the epitaxial orientation of the monocrystalline film (LSMO/STO film) prepared by the invention.
From the above test results, it can be seen that: the heterojunction material prepared in the embodiment of the invention has the advantages of low lattice mismatch rate, good crystal symmetry and low oxygen vacancy concentration.
The transition metal oxide (iridium oxide) heterojunction interface has strong interaction among charge, spin, orbit and lattice freedom, so that the heterojunction interface shows a plurality of peculiar physical properties and has unique advantages in the design of materials with exchange bias and spin-orbit torque. In addition, 5d iridium-based transition metal oxide (iridium oxide) having strong spin-orbit coupling energy provides considerable spin current to the heterojunction interface. Moreover, the heterojunction with a clear interface has higher requirements on growth materials, and the all-perovskite oxide has natural advantages in the growth of the heterojunction interface, has high lattice matching degree and is convenient to form a better interface structure. Therefore, the invention realizes the spin orbit torque effect in the all-perovskite oxide heterojunction by regulating and controlling the magnetic coupling performance of the interface.
In summary, the manganese oxide in the heterojunction material of the invention adopts La0.67Sr0.33MnO3(ii) a By making a pair of La0.67Sr0.33MnO3The thickness of the layer is regulated, so that the magnetocrystalline anisotropy energy of the magnetic layer is regulated, a damping-like field induced by heterojunction current is regulated, the interface magnetic coupling state is regulated, and the heterojunction spin-orbit torque effect is finally regulated. The heterojunction material provided by the invention is an iridium oxide-based heterojunction thin film material with a remarkable spin-orbit torque effect. The material achieves the purpose of adjusting the heterojunction spin orbit torque effect by regulating and controlling the magnetic coupling performance of the heterojunction interface, so that the material has wide application potential in the fields of magnetic information storage, nano oscillators and the like.
While the embodiments of the present invention have been described in detail with reference to the specific embodiments, the present invention is not limited to the embodiments, and various changes can be made without departing from the spirit of the present invention within the knowledge of those skilled in the art. Furthermore, the embodiments of the present invention and the features of the embodiments may be combined with each other without conflict.
Claims (10)
1. A heterojunction material having a spin-orbit torque effect, characterized by: the material comprises a manganese oxide layer and an iridium oxide layer which are sequentially superposed;
the manganese oxide layer is La0.67Sr0.33MnO3A layer;
the iridium oxide layer is XIrO3A layer;
the iridium oxide in the iridium oxide layer is perovskite type oxide;
wherein said XIrO3In the layerX is an alkaline earth metal cation;
the thickness of the manganese oxide layer is 3 nm-8 nm;
the thickness of the iridium oxide layer is 5 nm-12 nm.
2. The heterojunction material with spin-orbit torque effect of claim 1, wherein: the thickness of the manganese oxide layer is 3 nm-8 nm; preferably, the iridium oxide layer has a thickness of 5nm to 12 nm.
3. The heterojunction material with spin-orbit torque effect of claim 1, wherein: the crystal plane orientation of the manganese oxide in the manganese oxide layer is (001).
4. The heterojunction material with spin-orbit torque effect of claim 1, wherein: the XIrO3X in the layer is at least one of calcium ion or strontium ion.
5. A method for preparing a heterojunction material with spin-orbit torque effect as claimed in any of claims 1 to 4, characterized in that:
and sequentially depositing manganese oxide and iridium oxide on the substrate to form a manganese oxide layer and an iridium oxide layer.
6. The method of claim 5, wherein: the substrate is a perovskite substrate; preferably, the perovskite substrate has a unit cell parameter of
7. The method of claim 5, wherein: the deposition is pulsed laser deposition; preferably, the laser energy during the deposition of the manganese oxide is 1.0J/cm2～1.8J/cm2(ii) a Preferably, the temperature during the deposition of the manganese oxide is650-750 ℃; preferably, the oxygen pressure in the deposition process of the manganese oxide is 0.1 mbar-0.5 mbar; preferably, the time during the deposition of the manganese oxide is 1.5min to 4 min.
8. The method of claim 7, wherein: the laser energy in the deposition process of the iridium oxide is 0.8J/cm2～1.6J/cm2(ii) a Preferably, the temperature in the deposition process of the iridium oxide is 600-700 ℃; preferably, the oxygen pressure in the deposition process of the iridium oxide is 0.16 mbar-0.2 mbar; preferably, the time in the deposition process of the iridium oxide is 1min to 4 min.
9. Magnetic random access memory, characterized in that it comprises a heterojunction material with spin-orbit torque effect according to any of claims 1 to 4.
10. Nanooscillator comprising a heterojunction material with spin-orbit torque effect as claimed in any of claims 1 to 4.
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