CN113380945A - Magnetic heterostructure based on electric field regulation and control and preparation method thereof - Google Patents

Magnetic heterostructure based on electric field regulation and control and preparation method thereof Download PDF

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CN113380945A
CN113380945A CN202110558170.1A CN202110558170A CN113380945A CN 113380945 A CN113380945 A CN 113380945A CN 202110558170 A CN202110558170 A CN 202110558170A CN 113380945 A CN113380945 A CN 113380945A
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thin film
electrode layer
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CN113380945B (en
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金立川
徐嘉鹏
徐鑫锴
张怀武
唐晓莉
向全军
钟智勇
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University of Electronic Science and Technology of China
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Abstract

A magnetic heterostructure based on electric field regulation and a preparation method thereof belong to the field of preparation of magnetoelectric coupling materials and devices. The magnetic heterostructure comprises a substrate, a bottom electrode layer formed on the substrate, a heterojunction formed on the bottom electrode layer, and a top electrode layer formed on the heterojunction; the heterojunction is a magnetic thin film/MXene heterojunction, and the magnetic thin film and the MXene thin film are stacked up and down. The heterostructure realizes the directional movement of hydrogen ions in the magnetic film/MXene heterojunction by applying voltage to the bottom electrode layer and the top electrode layer in the vertical direction, and converts the hydrogen ions into hydrogen atoms to be stored in the MXene film. The magnetic anisotropy of the magnetic film is very sensitive to the concentration of hydrogen atoms adsorbed on the surface, so that the magnetic film can be regulated and controlled by an external voltage, and when the bias voltage is removed, the hydrogen atoms are quickly diffused into the atmosphere, and the magnetism of the film is restored to the original state.

Description

Magnetic heterostructure based on electric field regulation and control and preparation method thereof
Technical Field
The invention belongs to the field of preparation of magnetoelectric coupling materials and devices, and particularly relates to a magnetic heterostructure based on electric field regulation and a preparation method thereof.
Background
The magnetic properties of electric field control materials are seen in many material systems, for example, ferromagnetic materials are magnetically tuned by changing the number and density of charge carriers, while multiferroic materials are coupled by electric polarization and magnetization of an applied electric field. In addition, another voltage-controlled magnetic anisotropy effect, which generally occurs in a ferromagnetic metal/metal oxide structure, can be interpreted as an electrochemical reaction of the thin film, that is, the thin film undergoes directional ion migration under the action of an external electric field, and a reversible magnetic transformation is completed during the electrochemical reaction.
However, the reliability and non-volatility of the electronically controlled ion migration need to be enhanced, and although hydrogen ion migration has been achieved for more than 2000 cycles at a faster speed, the power-off storage time of the device can only last for several days, which is not favorable for permanent data storage, and the hydrogen storage material used, heavy metal lead, has a higher hydrogen mobility, but is easy to generate hydrogen injection phenomenon under vacuum or high temperature, and it is expected that finding a hydrogen storage material with better quality in hydrogen ion migration will become a next important challenge.
Disclosure of Invention
In order to solve the technical problems, the invention provides a magnetic heterostructure based on electric field regulation and a preparation method thereof. The magnetic heterostructure based on electric field regulation has the advantages of high magnetic switching speed, large regulation amplitude, extremely low power consumption and high reliability.
The technical scheme adopted by the invention is as follows:
a magnetic heterostructure based on electric field regulation is characterized by comprising a substrate, a bottom electrode layer formed on the substrate, a heterojunction formed on the bottom electrode layer, and a top electrode layer formed on the heterojunction;
the heterojunction is a magnetic thin film/MXene heterojunction, and the magnetic thin film and the MXene thin film are stacked up and down.
Further, the magnetic thin film may be a magnetic insulator thin film, a ferromagnetic alloy thin film, or an antiferromagnetic thin film; wherein the magnetic insulator thin film may be an Yttrium Iron Garnet (YIG), a thulium iron garnet (TmBiIG), a bismuth-doped thulium iron garnet (TmBiIG), a hexagonal ferrite, a spinel ferrite thin film; the ferromagnetic alloy thin film can be permalloy (NiFe), cobalt iron boron (CoFeB) and Heusler alloy; the antiferromagnetic film can be nickel protoxide (NiO), bismuth ferrite (BiFeO)3) And iridium manganese (IrMn) thin films.
Further, the MXene film can be a transition metal carbide film, a nitride film or a carbonitride film; wherein the transition metal carbide thin film may be Ti3C2TX、Ti2CTXEtc.; the transition metal nitride film may be Ti2NTX、Ti3N2TXEtc.; the transition metal carbonitride may be Ti3CNTXT is a functional group, typically O, F, OH, etc., and x is 1, 2, or 3.
Further, the material of the bottom electrode layer and the top electrode layer may be platinum (Pt), gold (Au), tantalum (Ta), copper (Cu), aluminum (Al), Indium Tin Oxide (ITO), or the like.
Further, the substrate is made of Gadolinium Gallium Garnet (GGG), silicon single crystal (Si) and silicon dioxide (SiO)2) Gallium arsenide (GaAs), or gallium nitride (GaN).
Further, the thickness of the magnetic film is 1 nm-10 μm; the thickness of the MXene film is 1 nm-10 μm.
Preferably, the thickness of the bottom electrode layer is 2-10 nm, the thickness of the top electrode layer is 100-400 nm, the thickness of the magnetic film is 200-400 nm, and the thickness of the MXene film is 200-400 nm.
Further, by applying a bias voltage to the top electrode layer (grounding the bottom electrode layer), the electric field strength is made to be in the range of 0.02V/nm to 0.5V/nm.
The invention also provides a preparation method of the magnetic heterostructure based on electric field regulation, which is characterized by comprising the following steps:
step 1, cleaning a substrate, and growing a bottom electrode layer on the substrate;
step 2, growing a magnetic film on the bottom electrode layer obtained in the step 1;
step 3, obtaining a mixed liquid containing two-dimensional MXene by an acid corrosion method;
step 4, growing an MXene film on the magnetic film obtained in the step 2;
and 5, growing a top electrode layer on the composite film structure obtained in the step 4 to finish the preparation of the device.
Preferably, the method for growing the bottom electrode layer and the top electrode layer is magnetron sputtering.
Preferably, the method for growing the magnetic thin film is pulsed laser deposition, liquid phase epitaxy or magnetron sputtering.
Preferably, the method for growing the MXene film is a spraying method, a spin coating method, a vacuum filtration method or a screen printing method.
The invention provides a magnetic heterostructure based on electric field regulation and a preparation method thereof, wherein the heterostructure applies voltage in the vertical direction through a bottom electrode layer and a top electrode layer to realize the directional movement of hydrogen ions in a magnetic film/MXene heterojunction, and converts the hydrogen ions into hydrogen atoms to be stored in the MXene film. The magnetic anisotropy of the magnetic film is very sensitive to the concentration of hydrogen atoms adsorbed on the surface, so that the magnetic film can be regulated and controlled by an external voltage, and when the bias voltage is removed, the hydrogen atoms are quickly diffused into the atmosphere, and the magnetism of the film is restored to the original state.
Due to the adoption of the technical scheme, compared with the prior art, the invention has the beneficial effects that:
1. according to the magnetic heterostructure based on electric field regulation and control, the MXene film is formed by stacking the transition metal oxide, nitride or carbonitride laminations, and the special structure provides a plurality of channels for ion transportation, so that the ion transportation efficiency is improved, and the faster magnetic switching speed is realized;
2. the hydrogen ions have smaller size, and the transportation speed is higher in the magnetic process of the ion regulating material, but the existing hydrogen storage material such as PdH is very unstable in the hydrogen storage process, so that the reliability of the device is greatly influenced. The MXene film can realize stable hydrogen storage, so that the magnetic film/MXene heterojunction has higher reliability;
3. the MXene film can reach 4 wt% of hydrogen storage capacity at room temperature and in the atmospheric environment, which is difficult to reach by other hydrogen storage materials, so that the MXene-based magnetic device can be allowed to operate at normal temperature and normal pressure, and the large coercive force electric field regulation and control of the magnetic device at room temperature is realized.
Drawings
FIG. 1 is a side view of a heterostructure based on electric field regulation provided in the present invention;
fig. 2 is a flow chart of a method for manufacturing a heterostructure based on electric field regulation provided by the present invention.
Detailed Description
The technical solution of the present invention will be described in detail with reference to specific examples. The following examples are only for illustrating the technical solutions of the present invention more clearly, and are not intended to limit the actual scope of the present invention in any way, and the scope of the present invention is not limited thereby.
Example 1
In this embodiment, a heterostructure based on electric field control includes a Gadolinium Gallium Garnet (GGG) single crystal substrate, a bottom electrode layer platinum (Pt) formed on the substrate, and a Yttrium Iron Garnet (YIG) magnetic thin film/MXene (Ti) sequentially formed on the bottom electrode3C2TX) Thin film heterojunction and top electrode layer chromium/gold (Cr/Au).
Applying positive bias voltage on the top electrode layer to ensure that the electric field intensity is more than 0.02V/nm and simultaneously less than 0.5V/nm, water molecules absorbed from air generate hydrolysis reaction on the surface of the electrode, oxygen in the water molecules is diffused to the atmospheric environment, generated hydrogen atoms are stored in the MXene film, the concentration of the hydrogen atoms depends on the magnitude and time of the applied bias voltage, and the magnetic anisotropy of the magnetic film is very sensitive to the concentration of the hydrogen atoms adsorbed on the surface, so the magnetic film can be controlled by external voltage, and the hydrogen atoms are quickly diffused to the atmosphere after the bias voltage is removed, and the magnetism of the film is restored to the original state.
The preparation process flow of the heterostructure based on electric field regulation is shown in fig. 2, and specifically comprises the following steps:
step 1, ultrasonically cleaning a GGG single crystal substrate for 10 minutes by using acetone, alcohol and deionized water in sequence;
step 2, growing a Pt film with the thickness of 2-10 nm on the substrate cleaned in the step 1 by adopting a direct current magnetron sputtering method to serve as a bottom electrode layer;
step 3, depositing a layer of YIG film with the thickness of 200-400 nm on the basis of the step 2 by adopting a pulse laser deposition method, and annealing the film for 4 hours at the temperature of 800 ℃ in the air by using a tubular annealing furnace after deposition;
step 4, under the magnetic stirring, taking 1g of Ti3AlC2Putting the powder into 20ml of HF solution (the concentration is within 15-20%), and reacting for 24-30 h under oil bath at 25-35 ℃ and magnetic stirring;
centrifuging and washing the obtained mixed solution for multiple times, adding deionized water before each washing to enable the total amount of the mixed solution to reach 50ml, setting the relative centrifugal force to be 3000-4000 RCF, washing for 1-5 min until the pH value of the mixed liquid supernatant is about 6, and centrifuging to obtain a precipitate;
re-dispersing the obtained precipitate in deionized water, centrifuging for about 30 minutes at 500RCF for the last time, and taking supernatant containing layered two-dimensional MXene slices for experiment;
step 5, taking the mixed solution obtained in the step 4 as a spraying solution, and growing an MXene film (Ti) with the thickness of 200-400 nm on the magnetic film obtained in the step 3 by adopting a spraying method3C2TX)；
And 6, depositing a Cr/Au composite film with the thickness of 100-400 nm on the composite film structure obtained in the step 5 by adopting a direct-current magnetron sputtering method, wherein the thickness ratio of Cr to Au is 1: 10, a top electrode layer was obtained.
Example 2
In this embodiment, a heterostructure based on electric field control includes a Gadolinium Gallium Garnet (GGG) single crystal substrate, a bottom electrode layer platinum (Pt) formed on the substrate, and a Yttrium Iron Garnet (YIG) magnetic thin film/MXene (Ti) sequentially formed on the bottom electrode2CTX) Thin film heterojunction and top electrode layer chromium/gold (Cr/Au).
The preparation process flow of the heterostructure based on electric field regulation is shown in fig. 2, and specifically comprises the following steps:
step 1, ultrasonically cleaning a GGG single crystal substrate for 10 minutes by using acetone, alcohol and deionized water in sequence;
step 2, growing a Pt film with the thickness of 2-10 nm on the substrate cleaned in the step 1 by adopting a direct current magnetron sputtering method to serve as a bottom electrode layer;
step 3, depositing a layer of YIG film with the thickness of 200-400 nm on the basis of the step 2 by adopting a pulse laser deposition method, and annealing the film for 4 hours at the temperature of 800 ℃ in the air by using a tubular annealing furnace after deposition;
step 4, under the magnetic stirring, taking 1g of Ti2Placing AlC powder in 20ml of HF solution (the concentration is within 15-20%), and reacting for 24-30 h under the conditions of oil bath at 25-35 ℃ and magnetic stirring;
centrifuging and washing the obtained mixed solution for multiple times, adding deionized water before each washing to enable the total amount of the mixed solution to reach 50ml, setting the relative centrifugal force to be 3000-4000 RCF, washing for 1-5 min until the pH value of the mixed liquid supernatant is about 6, and centrifuging to obtain a precipitate;
re-dispersing the obtained precipitate in deionized water, centrifuging for about 30 minutes at 500RCF for the last time, and taking supernatant containing layered two-dimensional MXene slices for experiment;
step 5, taking the mixed solution obtained in the step 4 as a spraying solution, and growing an MXene film (Ti) with the thickness of 200-400 nm on the magnetic film obtained in the step 3 by adopting a spraying method2CTX)；
And 6, depositing a Cr/Au composite film with the thickness of 100-400 nm on the composite film structure obtained in the step 5 by adopting a direct-current magnetron sputtering method, wherein the thickness ratio of Cr to Au is 1: 10, a top electrode layer was obtained.
It should be understood that the above description is only a preferred embodiment of the present invention, and is only for the purpose of illustrating the present invention and is not intended to limit the scope of the present invention. Further, it should also be understood that various alterations, modifications and/or variations can be made to the present invention by those skilled in the art after reading the technical content of the present invention, and all such equivalents fall within the protective scope defined by the claims of the present application.

Claims (8)

1. A magnetic heterostructure based on electric field regulation is characterized by comprising a substrate, a bottom electrode layer formed on the substrate, a heterojunction formed on the bottom electrode layer, and a top electrode layer formed on the heterojunction;
the heterojunction is a magnetic thin film/MXene heterojunction, and the magnetic thin film and the MXene thin film are stacked up and down.
2. The electric field regulation-based magnetic heterostructure of claim 1, wherein the magnetic thin film is a magnetic insulator thin film, a ferromagnetic alloy thin film, or an antiferromagnetic thin film.
3. The magnetic heterostructure based on electric field regulation of claim 2, wherein the magnetic insulator thin film is a yttrium iron garnet, a thulium iron garnet, a bismuth-doped thulium iron garnet, a hexaferrite, a spinel ferrite thin film; the ferromagnetic alloy film is permalloy, cobalt-iron-boron and Heusler alloy; the antiferromagnetic film is a nickel protoxide film, a bismuth ferrite film and an iridium manganese film.
4. The magnetic heterostructure based on electric field modulation of claim 1, wherein the MXene thin film is a transition metal carbide thin film, a nitride thin film, or a carbonitride thin film.
5. The electric field regulation-based magnetic heterostructure of claim 4, wherein the transition metal carbide thin film is Ti3C2TX、Ti2CTX(ii) a The transition metal nitride film is Ti2NTX、Ti3N2TX(ii) a The transition metal carbonitride is Ti3CNTX。
6. The magnetic heterostructure based on electric field regulation and control of claim 1, wherein the bottom electrode layer has a thickness of 2 to 10nm, the top electrode layer has a thickness of 100 to 400nm, the magnetic thin film has a thickness of 200 to 400nm, and the MXene thin film has a thickness of 200 to 400 nm.
7. The magnetic heterostructure based on electric field regulation of claim 1, wherein the electric field strength is in the range of 0.02V/nm to 0.5V/nm by applying a bias voltage to the top electrode layer.
8. A preparation method of a magnetic heterostructure based on electric field regulation is characterized by comprising the following steps:
step 1, cleaning a substrate, and growing a bottom electrode layer on the substrate;
step 2, growing a magnetic film on the bottom electrode layer obtained in the step 1;
step 3, obtaining a mixed liquid containing two-dimensional MXene by an acid corrosion method;
step 4, growing an MXene film on the magnetic film obtained in the step 2;
and 5, growing a top electrode layer on the composite film structure obtained in the step 4 to finish the preparation of the device.
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Citations (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN109712769A (en) * 2019-01-30 2019-05-03 郑州大学 A kind of MXene- magnetic metal composite material and preparation method thereof
CN111003686A (en) * 2019-12-06 2020-04-14 北京航空航天大学 Novel room temperature hydrogen storage material and preparation method thereof

Patent Citations (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN109712769A (en) * 2019-01-30 2019-05-03 郑州大学 A kind of MXene- magnetic metal composite material and preparation method thereof
CN111003686A (en) * 2019-12-06 2020-04-14 北京航空航天大学 Novel room temperature hydrogen storage material and preparation method thereof

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