CN111969108A - Flexible substrate-based copper metaaluminate memristor and preparation method - Google Patents
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- 229910052802 copper Inorganic materials 0.000 title claims abstract description 65
- 239000010949 copper Substances 0.000 title claims abstract description 65
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 title claims abstract description 62
- 239000000758 substrate Substances 0.000 title claims abstract description 48
- 238000002360 preparation method Methods 0.000 title claims abstract description 10
- 230000008859 change Effects 0.000 claims abstract description 39
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 claims abstract description 14
- AMGQUBHHOARCQH-UHFFFAOYSA-N indium;oxotin Chemical compound [In].[Sn]=O AMGQUBHHOARCQH-UHFFFAOYSA-N 0.000 claims abstract description 14
- 229910052709 silver Inorganic materials 0.000 claims abstract description 14
- 239000004332 silver Substances 0.000 claims abstract description 14
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 claims description 24
- 229920002120 photoresistant polymer Polymers 0.000 claims description 24
- 238000004544 sputter deposition Methods 0.000 claims description 24
- 238000000034 method Methods 0.000 claims description 21
- -1 polyethylene naphthalate Polymers 0.000 claims description 21
- 229910052786 argon Inorganic materials 0.000 claims description 12
- 238000000151 deposition Methods 0.000 claims description 12
- 238000001035 drying Methods 0.000 claims description 10
- 229920003207 poly(ethylene-2,6-naphthalate) Polymers 0.000 claims description 10
- 239000011112 polyethylene naphthalate Substances 0.000 claims description 10
- 238000001259 photo etching Methods 0.000 claims description 9
- CSCPPACGZOOCGX-UHFFFAOYSA-N Acetone Chemical compound CC(C)=O CSCPPACGZOOCGX-UHFFFAOYSA-N 0.000 claims description 8
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 8
- 239000001301 oxygen Substances 0.000 claims description 8
- 229910052760 oxygen Inorganic materials 0.000 claims description 8
- 229920000139 polyethylene terephthalate Polymers 0.000 claims description 8
- 239000005020 polyethylene terephthalate Substances 0.000 claims description 8
- 230000008569 process Effects 0.000 claims description 8
- 238000004140 cleaning Methods 0.000 claims description 6
- 239000002184 metal Substances 0.000 claims description 6
- 229910052751 metal Inorganic materials 0.000 claims description 6
- 239000000919 ceramic Substances 0.000 claims description 4
- 239000011248 coating agent Substances 0.000 claims description 4
- 238000000576 coating method Methods 0.000 claims description 4
- 238000001816 cooling Methods 0.000 claims description 4
- 239000008367 deionised water Substances 0.000 claims description 4
- 229910021641 deionized water Inorganic materials 0.000 claims description 4
- 238000005137 deposition process Methods 0.000 claims description 4
- 239000007789 gas Substances 0.000 claims description 4
- 239000003292 glue Substances 0.000 claims description 4
- 238000010438 heat treatment Methods 0.000 claims description 4
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 4
- 239000013077 target material Substances 0.000 claims description 3
- 238000004528 spin coating Methods 0.000 claims description 2
- 239000000463 material Substances 0.000 abstract description 14
- 229920000642 polymer Polymers 0.000 abstract description 2
- 239000010408 film Substances 0.000 description 33
- 239000004065 semiconductor Substances 0.000 description 5
- 239000012212 insulator Substances 0.000 description 2
- 230000004048 modification Effects 0.000 description 2
- 238000012986 modification Methods 0.000 description 2
- 238000005406 washing Methods 0.000 description 2
- 239000002202 Polyethylene glycol Substances 0.000 description 1
- 230000009471 action Effects 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 239000003990 capacitor Substances 0.000 description 1
- 238000007385 chemical modification Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 230000005684 electric field Effects 0.000 description 1
- 239000007772 electrode material Substances 0.000 description 1
- 239000011521 glass Substances 0.000 description 1
- 229910021645 metal ion Inorganic materials 0.000 description 1
- 230000005693 optoelectronics Effects 0.000 description 1
- 238000000206 photolithography Methods 0.000 description 1
- 229920001223 polyethylene glycol Polymers 0.000 description 1
- 229910052710 silicon Inorganic materials 0.000 description 1
- 239000010703 silicon Substances 0.000 description 1
- 238000003860 storage Methods 0.000 description 1
- KKEYFWRCBNTPAC-UHFFFAOYSA-L terephthalate(2-) Chemical compound [O-]C(=O)C1=CC=C(C([O-])=O)C=C1 KKEYFWRCBNTPAC-UHFFFAOYSA-L 0.000 description 1
- 239000010409 thin film Substances 0.000 description 1
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10N—ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10N70/00—Solid-state devices having no potential barriers, and specially adapted for rectifying, amplifying, oscillating or switching
- H10N70/801—Constructional details of multistable switching devices
- H10N70/881—Switching materials
- H10N70/883—Oxides or nitrides
- H10N70/8836—Complex metal oxides, e.g. perovskites, spinels
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10N—ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10N70/00—Solid-state devices having no potential barriers, and specially adapted for rectifying, amplifying, oscillating or switching
- H10N70/011—Manufacture or treatment of multistable switching devices
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10N—ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10N70/00—Solid-state devices having no potential barriers, and specially adapted for rectifying, amplifying, oscillating or switching
- H10N70/20—Multistable switching devices, e.g. memristors
- H10N70/24—Multistable switching devices, e.g. memristors based on migration or redistribution of ionic species, e.g. anions, vacancies
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10N—ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10N70/00—Solid-state devices having no potential barriers, and specially adapted for rectifying, amplifying, oscillating or switching
- H10N70/801—Constructional details of multistable switching devices
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Abstract
The invention provides a flexible substrate-based copper metaaluminate memristor, which is sequentially provided with an upper electrode, a resistance change layer, a lower electrode and a vertical four-layer structure of a flexible substrate from top to bottom; the upper electrode of the memristor is a copper film or a silver film; the resistance change layer of the memristor is a copper metaaluminate film; the lower electrode is an indium tin oxide transparent conductive film; the flexible memristor based on the copper metaaluminate film is simple in preparation process and low in cost, and can obtain good resistance change characteristics on the polymer flexible substrate. The memristor widens the material system of the memristor resistance change layer, and is expected to be applied to the fields of flexible devices and wearable electronic devices.
Description
Technical Field
The invention belongs to the field of semiconductor optoelectronic devices, and particularly relates to a copper metaaluminate memristor based on a flexible substrate and a preparation method thereof.
Background
The memristor is used as a fourth basic circuit element after a resistor, a capacitor and an inductor, has the characteristics of simple device structure, high working speed, low power consumption and the like, and has important application prospects in the fields of information storage, logic operation, neuromorphic chips and the like. The memristor has an electrode/resistance change layer/electrode sandwich structure, and the resistance change property of the memristor is closely related to an electrode material and a resistance change material. The resistance change characteristic presented by the memristor to some extent determines the application field of the memristor. In order to meet different application scenarios, researchers have adopted various methods to obtain different resistive switching characteristics. The method is an effective method for changing the resistance change characteristics of the memristor by selecting different resistance change layer materials. Researchers have conducted a lot of studies on different resistive materials, and the resistive materials include various types, insulators, semiconductors, and the like. Research shows that when the insulator material, the intrinsic semiconductor material and the n-type semiconductor material are respectively adopted as the memristor resistance change layers, the memristor shows different resistance change characteristics, and therefore the memristor is suitable for different application scenes.
The substrate adopted by the memristor has influence on the application scene. In recent years, with the development of wearable electronics, researchers have been focusing on electronic devices using flexible materials as substrates. For the memristor, when the substrate is changed from a traditional rigid substrate of silicon, glass and the like to a flexible substrate, the memristor performance faces a great challenge. Among the many resistance change materials studied so far, only a small part of the materials can have good resistance change characteristics in the case of a flexible substrate.
The copper metaaluminate film is a P-type semiconductor material. In 1997, Kawazoe et al prepared this P-type direct bandgap transparent oxide film with delafossite structure for the first time based on the valence band Chemical Modification (CMVB) theory. The successful preparation of copper metaaluminate provides new possibility for realizing fully transparent memristors. More importantly, the copper metaaluminate has a unique delafossite structure, so that the memristor taking the copper metaaluminate as a resistance change layer is expected to show good memristive performance on a flexible substrate. However, there are few reports of copper metaaluminate memristors based on flexible substrates to date.
Disclosure of Invention
In order to achieve the purpose, the technical scheme of the invention is as follows:
a copper metaaluminate memristor based on a flexible substrate is provided with a vertical four-layer structure of an upper electrode 4, a resistance change layer 3, a lower electrode 2 and the flexible substrate 1 from top to bottom in sequence; the upper electrode 4 of the memristor is a copper film or a silver film; the resistance change layer 3 of the memristor is a copper metaaluminate film; the lower electrode 2 is an indium tin oxide transparent conductive film; the flexible substrate 1 of the memristor is made of polyethylene naphthalate or polyethylene terephthalate.
Preferably, the resistance change layer 3 of the memristor is obtained by radio frequency sputtering, and the thickness is 50 nm-300 nm.
Preferably, the upper electrode 4 of the memristor is a copper thin film.
Preferably, the bottom electrode 2 is an ITO bottom electrode with a thickness of 100-200 nm.
The invention also provides a preparation method of the copper metaaluminate memristor based on the flexible substrate, which comprises the following process steps:
(1) preparing polyethylene naphthalate or polyethylene terephthalate as a flexible substrate, and carrying out cleaning and drying treatment;
(2) depositing indium tin oxide on a polyethylene naphthalate or polyethylene terephthalate flexible substrate by a direct current sputtering method by adopting an indium tin oxide target material as a lower electrode 2, wherein the thickness is 100-200 nm;
(3) the method comprises the steps of depositing a copper metaaluminate film serving as a resistance change layer 3 by using a copper metaaluminate ceramic target through a radio frequency sputtering method, wherein in the film deposition process, a substrate is not heated, and the background vacuum of a sputtering chamber is 5 multiplied by 10-5Pa, working gas is oxygen and argon, the flow of the argon is 60SCCM, and the flow ratio of the oxygen to the argon is 1: 20, the sputtering power is less than 100W;
(4) covering a photoresist pattern on the copper metaaluminate film by adopting a photoetching process and combining a mask pattern to form a top electrode window;
(5) depositing a copper or silver film with the thickness of 50-100 nm on the resistance change layer 3 by adopting a metal copper or silver target through a direct current sputtering method;
(6) the photoresist is removed using an acetone solution, and the copper or silver upper electrode 4 is obtained.
Preferably, the photolithography process of step (4) includes the steps of:
the first step is as follows: heating the sample for 1min at the temperature of 100-150 ℃;
the second step is that: uniformly coating photoresist on the surface of the copper metaaluminate film, and performing spin coating by adopting a rotary spin coater;
the third step: after the glue is homogenized, repeating the first step;
the fourth step: on the basis of the third step, the photoresist on the surface of the copper metaaluminate film is exposed by combining a photoetching mask plate;
the fifth step: after exposure is finished, heating the sample for 3min at the temperature of 110-120 ℃;
and a sixth step: after cooling, placing the sample in a developing solution for developing;
the seventh step: and cleaning the residual photoresist by using deionized water and drying the photoresist to obtain an electrode window.
The basic working principle of the invention is as follows: when a forward voltage is applied between the upper electrode 4 and the lower electrode 2 of the device (electrical modulation), the metal in the upper electrode 4 is oxidized, and formed metal ions migrate under the action of an electric field and move into the resistive layer 3, so that the memristor forms a metal conductive filament in the resistive layer; when a reverse voltage is applied between the upper electrode 4 and the lower electrode 2 of the device (electrical modulation), a metal conductive filament formed in the resistive layer 3 of the memristor is broken, so that the resistive function of the memristor is realized.
The invention has the beneficial effects that: the flexible memristor based on the copper metaaluminate film is simple in preparation process and low in cost, and can obtain good resistance change characteristics on a polymer flexible substrate. Therefore, the memristor widens the material system of the memristor resistance change layer, and is expected to be applied to the fields of flexible devices and wearable electronic devices.
Drawings
Fig. 1 is a schematic structural view of the present invention.
The notations in the figure are respectively: 1-flexible substrate, 2-lower electrode, 3-resistance change layer and 4-upper electrode.
Detailed Description
The embodiments of the present invention are described below with reference to specific embodiments, and other advantages and effects of the present invention will be easily understood by those skilled in the art from the disclosure of the present specification. The invention is capable of other and different embodiments and of being practiced or of being carried out in various ways, and its several details are capable of modification in various respects, all without departing from the spirit and scope of the present invention.
Example 1
The embodiment provides a flexible substrate-based copper metaaluminate memristor, which is sequentially provided with an upper electrode 4, a resistance change layer 3, a lower electrode 2 and a vertical four-layer structure of a flexible substrate 1 from top to bottom; the upper electrode 4 of the memristor is a copper film; the resistance change layer 3 of the memristor is a copper metaaluminate film; the lower electrode 2 is an indium tin oxide transparent conductive film; the flexible substrate 1 of the memristor is polyethylene naphthalate.
The resistance change layer 3 of the memristor is obtained by radio frequency sputtering, and the thickness is 50 nm-300 nm.
The bottom electrode 2 is an ITO bottom electrode with a thickness of 100-200 nm.
The embodiment also provides a preparation method of the copper metaaluminate memristor based on the flexible substrate, which comprises the following process steps:
(1) preparing polyethylene naphthalate serving as a flexible substrate, and carrying out cleaning and drying treatment;
(2) depositing indium tin oxide on a polyethylene naphthalate flexible substrate by a direct current sputtering method by using an indium tin oxide target as a lower electrode 2, wherein the thickness is 100-200 nm;
(3) the method comprises the steps of depositing a copper metaaluminate film serving as a resistance change layer 3 by using a copper metaaluminate ceramic target through a radio frequency sputtering method, wherein in the film deposition process, a substrate is not heated, and the background vacuum of a sputtering chamber is 5 multiplied by 10-5Pa, working gas is oxygen and argon, the flow of the argon is 60SCCM, and the flow ratio of the oxygen to the argon is 1: 20, the sputtering power is less than 100W;
(4) covering a photoresist pattern on the copper metaaluminate film by adopting a photoetching process and combining a mask pattern to form a top electrode window; the photoetching process of the step (4) comprises the following steps:
the first step is as follows: drying the sample prepared in the step (3) for 1min at 150 ℃;
the second step is that: coating photoresist on the surface of the copper metaaluminate film of the sample, and homogenizing the photoresist for 35s at 3500rpm by using a rotary homogenizer;
the third step: after the glue is homogenized, drying the sample for 3min at 150 ℃;
the fourth step: exposing the photoresist on the surface of the copper metaaluminate film by combining a mask plate for 21 s;
the fifth step: after exposure, the sample was dried at 120 ℃ for 3 min;
and a sixth step: after cooling, the sample is placed in a developing solution for development;
the seventh step: washing the residual photoresist by deionized water to obtain an electrode window;
(5) depositing a copper film with the thickness of 50-100 nm on the resistance change layer 3 by adopting a metal copper target through a direct current sputtering method;
(6) the photoresist was removed using an acetone solution, and the upper electrode 4 of copper was obtained.
Example 2
The embodiment provides a flexible substrate-based copper metaaluminate memristor, which is sequentially provided with an upper electrode 4, a resistance change layer 3, a lower electrode 2 and a vertical four-layer structure of a flexible substrate 1 from top to bottom; the upper electrode 4 of the memristor is a copper film or a silver film; the resistance change layer 3 of the memristor is a copper metaaluminate film; the lower electrode 2 is an indium tin oxide transparent conductive film; the flexible substrate 1 of the memristor is a polyethylene terephthalate material.
The resistance change layer 3 of the memristor is obtained by radio frequency sputtering, and the thickness is 50 nm-300 nm.
The upper electrode 4 of the memristor is a copper film.
The bottom electrode 2 is an ITO bottom electrode with a thickness of 100-200 nm.
The embodiment also provides a preparation method of the copper metaaluminate memristor based on the flexible substrate, which comprises the following process steps:
(1) preparing polyethylene glycol terephthalate as a flexible substrate, and carrying out cleaning and drying treatment;
(2) depositing indium tin oxide on a polyethylene naphthalate or polyethylene terephthalate flexible substrate by a direct current sputtering method by adopting an indium tin oxide target material as a lower electrode 2, wherein the thickness is 100-200 nm;
(3) the method comprises the steps of depositing a copper metaaluminate film serving as a resistance change layer 3 by using a copper metaaluminate ceramic target through a radio frequency sputtering method, wherein in the film deposition process, a substrate is not heated, and the background vacuum of a sputtering chamber is 5 multiplied by 10-5Pa, working gas is oxygen and argon, the flow of the argon is 60SCCM, and the flow ratio of the oxygen to the argon is 1: 20, the sputtering power is less than 100W;
(4) covering a photoresist pattern on the copper metaaluminate film by adopting a photoetching process and combining a mask pattern to form a top electrode window; the photoetching process of the step (4) comprises the following steps:
the first step is as follows: drying the sample prepared in the step (3) for 1min at 150 ℃;
the second step is that: coating photoresist on the surface of the copper metaaluminate film of the sample, and homogenizing the photoresist for 35s at 3500rpm by using a rotary homogenizer;
the third step: after the glue is homogenized, drying the sample for 3min at 150 ℃;
the fourth step: exposing the photoresist on the surface of the copper metaaluminate film by combining a mask plate for 21 s;
the fifth step: after exposure, the sample was dried at 120 ℃ for 3 min;
and a sixth step: after cooling, the sample is placed in a developing solution for development;
the seventh step: washing the residual photoresist by deionized water to obtain an electrode window;
(5) depositing a silver film with the thickness of 50-100 nm on the resistance change layer 3 by adopting a silver target through a direct current sputtering method;
(6) the photoresist was removed using an acetone solution, and the upper electrode 4 of silver was obtained.
The foregoing embodiments are merely illustrative of the principles and utilities of the present invention and are not intended to limit the invention. Any person skilled in the art can modify or change the above-mentioned embodiments without departing from the spirit and scope of the present invention. Accordingly, it is intended that all equivalent modifications or changes which can be made by those skilled in the art without departing from the spirit and technical spirit of the present invention be covered by the claims of the present invention.
Claims (6)
1. The utility model provides a copper metaaluminate memristor based on flexible substrate which characterized in that:
the memristor is sequentially provided with an upper electrode (4), a resistance change layer (3), a lower electrode (2) and a vertical four-layer structure of a flexible substrate (1) from top to bottom; the upper electrode (4) of the memristor is a copper film or a silver film; the resistance change layer (3) of the memristor is a copper metaaluminate film; the lower electrode (2) is an indium tin oxide transparent conductive film; the flexible substrate (1) of the memristor is made of polyethylene naphthalate or polyethylene terephthalate.
2. The flexible substrate-based copper aluminate memristor according to claim 1, wherein: the resistance change layer (3) of the memristor is obtained by radio frequency sputtering, and the thickness is 50 nm-300 nm.
3. The flexible substrate-based copper aluminate memristor according to claim 1, wherein: the upper electrode (4) of the memristor is a copper film or a silver film.
4. The flexible substrate-based copper aluminate memristor according to claim 1, wherein: the lower electrode (2) is an indium tin oxide bottom electrode with a thickness of 100-200 nm.
5. The preparation method of the flexible substrate-based copper metaaluminate memristor is characterized by comprising the following process steps of:
(1) preparing polyethylene naphthalate or polyethylene terephthalate as a flexible substrate, and carrying out cleaning and drying treatment;
(2) depositing indium tin oxide on a polyethylene naphthalate or polyethylene terephthalate flexible substrate by a direct current sputtering method by adopting an indium tin oxide target material as a lower electrode (2), wherein the thickness is 100-200 nm;
(3) the method comprises the steps of adopting a copper metaaluminate ceramic target, depositing a copper metaaluminate film as a resistance change layer (3) by a radio frequency sputtering method, wherein in the film deposition process, a substrate is not heated, and the background vacuum of a sputtering chamber is 5 multiplied by 10-5Pa, working gas is oxygen and argon, the flow of the argon is 60SCCM, and the flow ratio of the oxygen to the argon is 1: 20, the sputtering power is less than 100W;
(4) covering a photoresist pattern on the copper metaaluminate film by adopting a photoetching process and combining a mask pattern to form a top electrode window;
(5) depositing a copper or silver film with the thickness of 50-100 nm on the resistance change layer (3) by adopting a metal copper or silver target through a direct current sputtering method;
(6) the photoresist is removed by using an acetone solution to obtain a copper or silver upper electrode (4).
6. The method for preparing the flexible substrate-based copper metaaluminate memristor according to claim 5, wherein the method comprises the following steps: the photoetching process of the step (4) comprises the following steps:
the first step is as follows: heating the sample for 1min at the temperature of 100-150 ℃;
the second step is that: uniformly coating photoresist on the surface of the copper metaaluminate film, and performing spin coating by adopting a rotary spin coater;
the third step: after the glue is homogenized, repeating the first step;
the fourth step: on the basis of the third step, the photoresist on the surface of the copper metaaluminate film is exposed by combining a photoetching mask plate;
the fifth step: after exposure is finished, heating the sample for 3min at the temperature of 110-120 ℃;
and a sixth step: after cooling, placing the sample in a developing solution for developing;
the seventh step: and cleaning the residual photoresist by using deionized water and drying the photoresist to obtain an electrode window.
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CN112750951A (en) * | 2020-12-28 | 2021-05-04 | 山东科技大学 | Flexible memristor based on organic solution and preparation method |
CN112750951B (en) * | 2020-12-28 | 2023-01-10 | 山东科技大学 | Flexible memristor based on organic solution and preparation method |
CN113224236A (en) * | 2021-05-11 | 2021-08-06 | 山东大学 | Transparent double-layer-structure memristor and preparation method thereof |
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