CN109216401B - Two-dimensional flexible magnetic storage array and preparation method thereof - Google Patents
Two-dimensional flexible magnetic storage array and preparation method thereof Download PDFInfo
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- CN109216401B CN109216401B CN201810803231.4A CN201810803231A CN109216401B CN 109216401 B CN109216401 B CN 109216401B CN 201810803231 A CN201810803231 A CN 201810803231A CN 109216401 B CN109216401 B CN 109216401B
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Abstract
The invention discloses a two-dimensional flexible magnetic storage array and a preparation method thereof, wherein the two-dimensional flexible magnetic storage array adopts a sandwich structure, is reasonable in design, grows a vacancy-doped III-VI chalcogenide layer by accurately controlling the temperature, the proportion and the growth time of a growth source so as to achieve the realizability of electrical regulation and control, thereby realizing the storage and recording functions of each magnetic storage unit device and the two-dimensional flexible magnetic storage array, the regulation and control range of the magnetic moment is 0-1 mu B, the two-dimensional flexible magnetic storage array can be used in an air environment or a vacuum environment from low temperature of liquid nitrogen to room temperature, the magnetic storage function is stable, and the two-dimensional flexible magnetic storage array is combined with a flexible substrate, so that the two.
Description
Technical Field
The invention belongs to the technical field of magnetic storage and magnetic recording, and particularly relates to a two-dimensional flexible magnetic storage array and a preparation method thereof.
Background
Since the 90 s of the last century, the electronic information industry has drawn attention. The modern information storage technology not only enables information storage to be high-density, but also enables information storage and quick retrieval to be combined, so that the modern information storage technology becomes the basis of information work development, and has great application value in the fields of industrial automation, embedded computing, network and data storage, important civil life, national defense, and the like. Among them, the magnetic storage technology has many advantages of non-volatility, long service life, low power consumption, radiation resistance, etc. and has become the pillar of modern information storage technology.
With the increasing demand of people for portable intelligent equipment, wearable electronic and biomedical equipment, the breakthrough of the battery energy storage technology of the flexible magnetic storage technology becomes the key for further development of the portable intelligent equipment. The existing magnetic memory chip is greatly limited in application and is often reflected in the influence of the use temperature and environment on the magnetic function, so that the application range of the magnetic memory chip in the application process is small, the functionality is poor, the magnetic memory chip is unstable and the like.
In 2016, the international team firstly transplants the high-performance magnetic storage chip to the surface of a piece of flexible plastic without damaging the performance of the high-performance magnetic storage chip, and the obtained transparent film-shaped flexible intelligent plastic chip has excellent data storage and processing capabilities and is expected to become a key element for the design and development of flexible light equipment. However, the technology mainly adopts methods such as stripping and transferring, which still cannot be separated from the traditional magnetic memory chip preparation method, and has complex process and high cost. While scientists have conducted a number of studies on different memory chips and materials, the way to construct and apply high performance memory chips directly on flexible substrates remains a significant challenge.
Disclosure of Invention
The invention aims to overcome the defects of the prior art, provides a two-dimensional flexible magnetic storage array and a preparation method thereof, and solves the problems of preparation and application of magnetic storage materials in the background technology.
The technical scheme adopted by the invention for solving the technical problems is as follows: the two-dimensional flexible magnetic storage array comprises a flexible substrate and a plurality of magnetic storage unit devices, wherein the magnetic storage unit devices are arrayed on the flexible substrate;
the magnetic storage unit device comprises a first conductive electrode, a sandwich structure and a second conductive electrode which are sequentially stacked from bottom to top; the sandwich structure sequentially comprises a first BN layer/a vacancy-doped III-VI chalcogenide layer/a second BN layer from bottom to top, the chemical formula of the III-VI chalcogenide is MX, wherein M is at least one of Ga and In, X is at least one of S, Se, and the vacancy is an M atom defect In the III-VI chalcogenide; the magnetic memory cell device is applied through a first conductive electrode and a second conductive electrode
The magnetic properties of the vacancy-doped group III-VI chalcogenide layer are adjusted in the presence of nonmagnetic and ferromagnetic semigoldAnd the attributes are converted to realize the magnetic storage function, and the magnetic moment regulation range of the magnetic storage unit device is 0-1 muB.
In a preferred embodiment of the present invention, the first BN layer and the second BN layer are both 1 to 3 molecular layers thick.
In a preferred embodiment of the present invention, the group III-VI chalcogenide layer has a thickness from a monolayer to less than 100 nm.
In a preferred embodiment of the present invention, the first conductive electrode and the second conductive electrode are made of non-magnetic material, including Au, Ti/Au.
In a preferred embodiment of the present invention, the flexible substrate includes PET and polyimide films.
The invention also provides a preparation method of the two-dimensional flexible magnetic storage array, which comprises the following steps:
1) preparing a first conductive electrode array and a lead on a flexible substrate by adopting an electron beam lithography method;
2) transferring the BN two-dimensional material grown on the copper foil to the surface of a first conductive electrode by adopting a transfer technology, and repeating the transfer process to enable the thickness of the BN two-dimensional material to be 1-3 molecular layers to form a first BN layer;
3) growing a two-dimensional material of III-VI family chalcogenide on the surface of the first BN layer by adopting a molecular beam epitaxy method, wherein the chemical formula of the III-VI family chalcogenide is MX, and M vacancies are formed in situ by controlling the proportion of an M source and an X source in the growth process to form a vacancy-doped III-VI family chalcogenide layer;
4) transferring the BN two-dimensional material grown on the copper foil to the surface of the vacancy-doped III-VI family chalcogenide layer by adopting the transfer technology of the step 2), and repeating the transfer process to ensure that the thickness of the BN two-dimensional material is 1-3 molecular layers to form a second BN layer;
5) preparing a second conductive electrode array and a lead on the surface of the second BN layer by adopting the electron beam photoetching method of step 1);
6) applying the vacancy-doped III-VI chalcogenide layer through the first conductive electrode and the second conductive electrode in a range of
The vertical voltage of (3) to complete the preparation.
In a preferred embodiment of the present invention, In the chemical formula In step 3), M is at least one of Ga and In, X is at least one of S, Se, and the ratio of the M source to the X source is 7-9: 1.
In a preferred embodiment of the present invention, in step 1), the electron beam lithography method comprises the following specific steps: spin-coating PMMA photoresist on a flexible substrate and drying; carrying out mask and electron beam lithography, exposing the PMMA photoresist, developing with a developing solution after exposure, fixing and drying by blowing to obtain a designed electrode pattern; then evaporating the metal of the conductive electrode, stripping the photoresist by acetone after the metal is finished to form a first conductive electrode array, and then welding a lead on the first conductive electrode.
In a preferred embodiment of the present invention, in step 2), the transferring technique specifically comprises the following steps: spin-coating a layer of PMMA on the surface of a large-area BN two-dimensional material grown on a copper foil, and after the PMMA is cured, using FeCl3The copper foil is dissolved by the solution, the PMMA with the BN two-dimensional material is transferred to the surface of the first conductive electrode array, and then the first conductive electrode array is soaked in acetone until the PMMA is dissolved.
In a preferred embodiment of the present invention, step 3), the molecular beam epitaxy comprises the following specific steps: placing the flexible substrate with the first conductive electrode and the first BN layer in a vacuum chamber of a molecular beam epitaxy system, placing a high-purity M, X growth source in the chamber, and using a mechanical pump and a molecular pump to drive the air pressure 10 in the growth chamber-7Heating an M source and an X source to respective evaporation temperatures below torr, wherein the concentration ratio of the M source to the X source is 7-9: 1 to form an M vacancy; the growth process maintains the temperature of the flexible substrate at room temperature.
Compared with the background technology, the technical scheme has the following advantages:
1. the magnetic storage array adopts a sandwich structure and is reasonable in design, vertical voltage is applied to the vacancy-doped III-VI family chalcogenide two-dimensional material through the first conductive electrode and the second conductive electrode, and the magnetism and half-metallic property of the vacancy-doped III-VI family chalcogenide two-dimensional material are regulated and controlled, so that the storage and recording functions of each magnetic storage unit device and the two-dimensional flexible magnetic storage array are realized, the regulation and control range of the magnetic moment is 0-1 mu B, the magnetic storage array can be used in the environment from liquid nitrogen low temperature to room temperature, air environment or vacuum environment, the magnetic storage function is stable, the flexible substrate is combined, the application range is wide, and the applicability is strong.
2. The preparation method of the invention grows the vacancy doped III-VI family chalcogenide two-dimensional material by accurately controlling the temperature, the proportion and the growth time of the growth source so as to achieve the realizability of electrical regulation and control and effectively solve the problem of complex manufacturing process of the flexible magnetic storage chip.
Drawings
FIG. 1 is a schematic diagram of a two-dimensional flexible magnetic memory array structure.
FIG. 2 is a schematic diagram of a magnetic memory cell structure.
FIG. 3 is a graph of the electron density states of a 2.8% Ga vacancy doped monolayer GaSe two-dimensional material in example 1, wherein a is 0 and b is 0
c a voltage of
Fig. 4 is a graph of the trend of the magnetic moment of the 2.8% Ga vacancy doped monolayer GaSe two-dimensional material of example 1 with electric field.
Detailed Description
The invention is explained in detail below with reference to the drawings and examples:
example 1
Referring to fig. 1, a two-dimensional flexible magnetic memory array of the present embodiment includes a PET flexible substrate 6 and a plurality of magnetic memory cell devices, where the magnetic memory cell devices are arranged in an array on the flexible substrate 6;
referring to fig. 2, the magnetic memory cell device includes a first conductive electrode 1, a sandwich structure and a second conductive electrode 5 sequentially stacked from bottom to top; the sandwich structure sequentially comprises a first BN layer 2/vacancy doped III-VI chalcogenide layer 3/second BN layer 4 from bottom to top, the chemical formula of the III-VI chalcogenide is MX, M is Ga and X is Se in the embodiment, and the vacancies are Ga atom defects in a monolayer GaSe two-dimensional material; the thicknesses of the first BN layer 2 and the second BN layer 4 are 3 molecular layers, the thickness of a monolayer GaSe two-dimensional material containing Ga atom vacancies is a monolayer, the vacancy concentration is 2.8 percent, and the materials of the first conductive electrode 5 and the second conductive electrode 5 are Au/Ti (70nm/10 nm).
The magnetic memory cell device is applied via a first conductive electrode 1 and a second conductive electrode 5
The magnetic property of the vacancy doped III-VI group chalcogenide layer 3 is adjusted to be converted between nonmagnetic and ferromagnetic half-metallic properties, the magnetic storage function is realized, and the magnetic moment regulation range of the magnetic storage unit device is 0-1 mu B.
The preparation method of the two-dimensional flexible magnetic storage array comprises the following steps:
0) obtaining a clean PET flexible substrate 6 by chemical cleaning (ultrasonic cleaning using acetone, ethanol, deionized water);
1) preparing a first conductive electrode 1 array and a lead on a flexible substrate 6 by adopting an electron beam lithography method;
the method comprises the following specific steps: the electron beam lithography method comprises the following specific steps: coating PMMA photoresist on the flexible substrate 6 in a spinning way and drying; carrying out mask and electron beam lithography, exposing the PMMA photoresist, developing with a developing solution after exposure, fixing and drying by blowing to obtain a designed electrode pattern; then evaporating Au/Ti (70nm/10nm) metal, stripping the photoresist by using acetone after the completion to form a first conductive electrode 1 array, and then welding a lead on the first conductive electrode 1;
2) transferring the BN two-dimensional material grown on the copper foil to the surface of the first conductive electrode 1 by adopting a transfer technology, and repeating the transfer process to enable the thickness of the BN two-dimensional material to be 1-3 molecular layers to form a first BN layer 2;
the method comprises the following specific steps: taking a small piece of large-area monolayer BN two-dimensional material growing on a copper foil, and spin-coating a layer of PMMA on the monolayer BN two-dimensional material; after PMMA is cured, FeCl is used3Solution-bonding copper foilDissolving; transferring PMMA with the BN two-dimensional material to the surface of a first BN two-dimensional material; soaking the sample transferred with the BN two-dimensional material in acetone for a short time to completely dissolve PMMA; 3 molecular layers of BN two-dimensional material were transferred repeatedly. Then soaking the PMMA in acetone until the PMMA is dissolved;
3) growing a two-dimensional material of III-VI family chalcogenide on the surface of the first BN layer 2 by adopting a molecular beam epitaxy method, wherein the chemical formula of the III-VI family chalcogenide is MX, and M vacancies are formed in situ by controlling the proportion of an M source and an X source in the growth process to form a vacancy-doped III-VI family chalcogenide layer 3; in the embodiment, in the chemical formula, M is Ga, X is Se, and the ratio of the M source to the X source is 8: 1;
the method comprises the following specific steps: placing the substrate 6 with the first conductive electrode 1 and the first BN layer 2 in a vacuum chamber of a molecular beam epitaxy system, and pumping the pressure of the growth chamber to 10 ℃ by using a mechanical pump-3Below torr, then turn on molecular pump to 10-6Below torr, the titanium pump was turned on to pump the gas pressure to 10-9torr; maintaining the substrate 6 at room temperature, 99.999% of high purity Ga and Se sources were heated to 200 ℃ and 400 ℃ respectively so that the evaporation rates of the Ga and Se sources were 8:1, thereby controlling the concentration ratio of the Ga source to the Se source to be 8: 1; after the growth time is 20min, taking out the sample, and placing the sample in a nitrogen environment to prevent oxidation;
4) transferring the BN two-dimensional material grown on the copper foil to the surface of the vacancy-doped III-VI family chalcogenide layer 3 by adopting the transfer technology of the step 2), and repeating the transfer process to ensure that the thickness of the BN two-dimensional material is 3 molecular layers to form a second BN layer 4;
5) preparing a second conductive electrode 5 array and a lead on the surface of the second BN layer 4 by adopting the electron beam photoetching method of step 1);
6) vertical voltage is applied to the vacancy doped III-VI group chalcogenide layer 3 through the first conductive electrode 1 and the second conductive electrode 5, magnetism of each magnetic storage unit device is controlled, and storage and recording functions of the two-dimensional flexible magnetic storage array are achieved.
The theoretical calculation predicts that the spin polarizability of the 2.8 percent Ga vacancy doped monomolecular layer GaSe two-dimensional material is 100 percent and is shown as semimetallic (As shown in fig. 3 a), with a magnetic moment size of 1 μ B (as shown in fig. 4), when less than
The spin polarizability of the 2.8% Ga vacancy doped monolayer GaSe two-dimensional material was still 100% at a vertical voltage, the magnetic moment was 1 μ B, the display was still magnetic (as shown in fig. 3B), and when more than that applied
The spin polarizability of the 2.8% Ga vacancy doped monolayer GaSe two-dimensional material is rapidly converted into 0% and the magnetic moment is 0 μ B, showing as nonmagnetic (as shown in fig. 3 c), thus proving that the magnetic and semimetallic properties of the vacancy doped III-VI chalcogenide two-dimensional material can be regulated and controlled by precisely controlling the vertical voltage intensity, thereby realizing the storage and recording functions of the magnetic memory cell device and the two-dimensional flexible magnetic memory array.
It will be appreciated by those skilled in the art that the same or similar technical effects as those of the above embodiments can be expected when the technical parameters of the present invention are changed within the following ranges:
the group III-VI chalcogenide has the formula MX, wherein M is at least one of Ga and In, X is at least one of S, Se, and the vacancy is an M atom defect In the group III-VI chalcogenide.
The group III-VI chalcogenide layer 3 has a thickness of a monolayer to less than 100 nm.
The first conductive electrode 1 and the second conductive electrode 5 are made of nonmagnetic materials including Au and Ti/Au.
The flexible substrate 6 comprises PET, polyimide film.
The above description is only a preferred embodiment of the present invention, and therefore should not be taken as limiting the scope of the invention, which is defined by the appended claims and their equivalents.
Claims (10)
1. A two-dimensional flexible magnetic memory array, characterized by: the magnetic memory cell array comprises a flexible substrate and a plurality of magnetic memory cell devices, wherein the magnetic memory cell devices are arrayed on the flexible substrate;
the magnetic storage unit device comprises a first conductive electrode, a sandwich structure and a second conductive electrode which are sequentially stacked from bottom to top; the sandwich structure sequentially comprises a first BN layer/a vacancy-doped III-VI chalcogenide layer/a second BN layer from bottom to top, the chemical formula of the III-VI chalcogenide is MX, wherein M is at least one of Ga and In, X is at least one of S, Se, and the vacancy is an M atom defect In the III-VI chalcogenide; the magnetic memory cell device is applied through a first conductive electrode and a second conductive electrode
The magnetic property of the vacancy doped III-VI family chalcogenide layer is adjusted to be converted between nonmagnetic and ferromagnetic half-metallic properties, the magnetic storage function is realized, and the magnetic moment regulation range of the magnetic storage unit device is 0-1 mu B.
2. A two-dimensional flexible magnetic memory array according to claim 1, wherein: the thickness of the first BN layer and the thickness of the second BN layer are both 1-3 molecular layers.
3. A two-dimensional flexible magnetic memory array according to claim 1, wherein: the group III-VI chalcogenide layer has a thickness from a monolayer to less than 100 nm.
4. A two-dimensional flexible magnetic memory array according to claim 1, wherein: the first conductive electrode and the second conductive electrode are made of nonmagnetic materials including Au and Ti/Au.
5. A two-dimensional flexible magnetic memory array according to claim 1, wherein: the flexible substrate comprises PET and polyimide films.
6. A method of fabricating a two-dimensional flexible magnetic memory array as claimed in any of claims 1 to 5, comprising the steps of:
1) preparing a first conductive electrode array and a lead on a flexible substrate by adopting an electron beam lithography method;
2) transferring the BN two-dimensional material grown on the copper foil to the surface of a first conductive electrode by adopting a transfer technology, and repeating the transfer process to enable the thickness of the BN two-dimensional material to be 1-3 molecular layers to form a first BN layer;
3) growing a two-dimensional material of III-VI family chalcogenide on the surface of the first BN layer by adopting a molecular beam epitaxy method, wherein the chemical formula of the III-VI family chalcogenide is MX, and M vacancies are formed in situ by controlling the proportion of an M source and an X source in the growth process to form a vacancy-doped III-VI family chalcogenide layer;
4) transferring the BN two-dimensional material grown on the copper foil to the surface of the vacancy-doped III-VI family chalcogenide layer by adopting the transfer technology of the step 2), and repeating the transfer process to ensure that the thickness of the BN two-dimensional material is 1-3 molecular layers to form a second BN layer;
5) preparing a second conductive electrode array and a lead on the surface of the second BN layer by adopting the electron beam photoetching method of step 1);
6) applying the vacancy-doped III-VI chalcogenide layer through the first conductive electrode and the second conductive electrode in a range of
The vertical voltage of (3) to complete the preparation.
7. The method of claim 6, wherein: in the chemical formula In the step 3), M is at least one of Ga and In, X is at least one of S, Se, and the ratio of the M source to the X source is 7-9: 1.
8. The method of claim 6, wherein: in step 1), the electron beam lithography method specifically comprises the following steps: spin-coating PMMA photoresist on a flexible substrate and drying; carrying out mask and electron beam lithography, exposing the PMMA photoresist, developing with a developing solution after exposure, fixing and drying by blowing to obtain a designed electrode pattern; then evaporating the metal of the conductive electrode, stripping the photoresist by acetone after the metal is finished to form a first conductive electrode array, and then welding a lead on the first conductive electrode.
9. The method of claim 6, wherein: in the step 2), the transfer technology comprises the following specific steps: spin-coating a layer of PMMA on the surface of a large-area BN two-dimensional material grown on a copper foil, and after the PMMA is cured, using FeCl3The copper foil is dissolved by the solution, the PMMA with the BN two-dimensional material is transferred to the surface of the first conductive electrode array, and then the first conductive electrode array is soaked in acetone until the PMMA is dissolved.
10. The method of claim 6, wherein: step 3), the molecular beam epitaxy comprises the following specific steps: placing the flexible substrate with the first conductive electrode and the first BN layer in a vacuum chamber of a molecular beam epitaxy system, placing a high-purity M, X growth source in the chamber, and using a mechanical pump and a molecular pump to drive the air pressure 10 in the growth chamber-7Heating an M source and an X source to respective evaporation temperatures below torr, wherein the concentration ratio of the M source to the X source is 7-9: 1 to form an M vacancy; the growth process maintains the temperature of the flexible substrate at room temperature.
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