CN112802964A - Memristor with synapse-like long-term plasticity and preparation method thereof - Google Patents
Memristor with synapse-like long-term plasticity and preparation method thereof Download PDFInfo
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- 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
- H10N70/021—Formation of switching materials, e.g. deposition of layers
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- H—ELECTRICITY
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- 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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- H—ELECTRICITY
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- 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
- H10N70/8833—Binary metal oxides, e.g. TaOx
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Abstract
The invention relates to a memristor with synapse-like long-term plasticity, which comprises a substrate, a first resistance change layer, a second resistance change layer and a top electrode layer which are sequentially stacked from bottom to top, wherein the substrate comprises an insulating layer and a bottom electrode layer which are stacked from bottom to top, the first resistance change layer is prepared from aluminum oxide, and the second resistance change layer is prepared from gallium oxide. Compared with a memristor with a single-layer pure metal oxide layer, the memristor obtained by the invention has the advantages of better resistance change effect, low power consumption, low working voltage, absolute value smaller than 1V, and improved tolerance and stability; the preparation is carried out by a pure solution method, the operation is simple and convenient, the cost is low, the investment of equipment and raw materials is less, and the preparation can be used for large-area preparation, so that large-scale industrial application is realized; the simple substance metal or simple substance metal compound material is used as the top electrode layer to replace the traditional oxide material, thereby reducing the cost and optimizing the preparation process; the memristor enables long-term plasticity of synapse-like devices.
Description
Technical Field
The invention relates to a memristor with synapse-like long-term plasticity and a preparation method thereof, and belongs to the technical field of microelectronics.
Background
Memristors (RRAMs), one of the most promising non-volatile memories, have received increasing attention for their superior performance. By applying voltage, the memory is changed back and forth between high and low configurations, data erasing and writing and current channel blocking operations are realized, and the memristor has great research value due to the characteristics of low voltage, high speed and low power consumption. The characteristics of the memristor are very similar to the working mechanism of synapses connecting different neurons in a biological nervous system, so that the memristor is very suitable to be used as a synapse device for constructing a neuromorphic brain chip and further an artificial neural network, the changeable multiple resistance states of the memristor can be used for simulating the function of the synapses in the human brain, and an electronic device with long-term plasticity similar to the synapses in the human brain is developed. However, the bionic synapse device based on the memristor has the problems of high working voltage, large power consumption and small ratio of high resistance to low resistance.
Disclosure of Invention
The invention aims to provide a memristor with synapse-like long-term plasticity, which is small in working voltage, small in power consumption and good in resistance change effect.
In order to achieve the purpose, the invention provides the following technical scheme: the memristor with the synapse-like long-term plasticity comprises a substrate, a first resistance transformation layer, a second resistance transformation layer and a top electrode layer which are sequentially stacked from bottom to top, wherein the substrate comprises an insulation layer and a bottom electrode layer which are stacked from bottom to top, the first resistance transformation layer is made of aluminum oxide, and the second resistance transformation layer is made of gallium oxide.
Further, the top electrode layer comprises a plurality of top electrodes with cylindrical structures, the top electrodes are made of metal silver, metal copper or gold, the thickness of the top electrodes is 20-60nm, and the diameter of the top electrodes is 0.1-0.5 mm.
Further, a protective layer is arranged on the surface, far away from the second resistance change layer, of the top electrode layer, and the protective layer is made of metal aluminum or metal tungsten.
Further, the bottom electrode layer is made of metal platinum or indium tin oxide, and the thickness of the bottom electrode is 50-150 nm.
Further, the insulating layer is a single-layer transparent glass or a three-layer structure, and the three-layer structure is a titanium layer, a silicon dioxide layer and a silicon layer which are sequentially stacked from top to bottom.
The invention also provides a preparation method of the memristor with the synapse-like long-term plasticity, which is used for preparing the memristor with the synapse-like long-term plasticity, and the preparation method comprises the following steps:
s1, providing a substrate, and cleaning and hydrophilically treating the substrate;
s2, preparing a first resistance change layer on the substrate by using an aqueous solution method;
s3, preparing a second resistance-change layer on the first resistance-change layer by using an aqueous solution method;
and S4, preparing a top electrode layer on the second resistance change layer to obtain the memristor with synapse-like long-term plasticity.
Further, the first resistance change layer is prepared by the following specific steps: preparing an alumina precursor solution at the temperature of 20-30 ℃, standing for 5-10min at room temperature, and dripping the alumina precursor solution on the substrate; spin coating in air at 2000-; annealing at a temperature of 250-350 ℃.
Further, the second resistance change layer is prepared by the following specific steps: preparing a gallium oxide precursor solution at the temperature of 20-30 ℃, standing for 5-10min at the room temperature, and dripping the gallium oxide precursor solution on the first resistance change layer; spin coating in air at 2000-; annealing at a temperature of 250-350 ℃.
Further, a protective layer is arranged on the surface, far away from the second resistance change layer, of the top electrode layer, and the top electrode layer and the protective layer are prepared through an evaporation coating method.
Further, before the second resistance change layer is prepared on the first resistance change layer, the preparation method further comprises the step of carrying out hydrophilic treatment on the first resistance change layer.
The invention has the beneficial effects that:
1) compared with a memristor with a single-layer pure metal oxide layer, the memristor obtained by the invention has the advantages of better resistance change effect, low power consumption, low working voltage, absolute value smaller than 1V, and improved tolerance and stability;
2) the preparation is carried out by a pure solution method, the operation is simple and convenient, the cost is low, the investment of equipment and raw materials is less, and the preparation can be used for large-area preparation, so that large-scale industrial application is realized;
3) the simple substance metal or simple substance metal compound material is used as the top electrode layer to replace the traditional oxide material, thereby reducing the cost and optimizing the preparation process;
4) the memristor enables long-term plasticity of synapse-like devices.
The foregoing description is only an overview of the technical solutions of the present invention, and in order to make the technical solutions of the present invention more clearly understood and to implement them in accordance with the contents of the description, the following detailed description is given with reference to the preferred embodiments of the present invention and the accompanying drawings.
Drawings
FIG. 1 is a schematic diagram of a memristor with synapse-like long-term plasticity according to an embodiment of the present disclosure;
FIG. 2 is a diagram of the resistance change characteristic of the memristor with synapse-like long-term plasticity shown in FIG. 1 within an annealing range of 200-300 ℃;
FIG. 3 is a long-term plasticity test diagram of memristors with synapse-like long-term plasticity shown in FIG. 1.
Detailed Description
The technical solutions of the present invention will be described clearly and completely with reference to the accompanying drawings, and it should be understood that the described embodiments are some, but not all embodiments of the present invention. All other embodiments, which can be derived by a person skilled in the art from the embodiments given herein without making any creative effort, shall fall within the protection scope of the present invention.
In addition, the technical features involved in the different embodiments of the present invention described below may be combined with each other as long as they do not conflict with each other.
Referring to fig. 1, a memristor with synapse-like long-term plasticity according to an embodiment of the present invention includes a substrate, a first resistance-change layer 201, a second resistance-change layer 200, and a top electrode layer 101 stacked in sequence from bottom to top, where the substrate includes an insulating layer 301 and a bottom electrode layer 300 stacked from bottom to top, the first resistance-change layer 201 is made of aluminum oxide, and the second resistance-change layer 200 is made of gallium oxide, but the first resistance-change layer 201 and the second resistance-change layer 200 may also be made of other metal oxides, and are not limited in particular.
The top electrode layer 101 includes a plurality of top electrodes having a cylindrical structure, the top electrodes may be arranged at equal intervals, the top electrodes are made of silver, copper or gold, but not limited thereto, the top electrodes may also be made of other conductive materials, which are not specifically listed here, the top electrodes have a thickness of 20-60nm and a diameter of 0.1-0.5 mm. In this example, the top electrode was made of metallic silver, with a thickness of 40nm and a diameter of 0.1 mm. The simple substance metal or simple substance metal compound material is used as the top electrode layer 101, so that the traditional oxide material is replaced, the cost is reduced, and the preparation process is optimized.
The top electrode layer 101 is provided with a protection layer 100 on a surface far away from the second resistance change layer 200 to improve the service life of the memristor. The protection layer 100 is made of metal aluminum or metal tungsten, but is not limited thereto, and the protection layer 100 may be made of other materials. In this embodiment, the protection layer 100 is made of aluminum metal.
The bottom electrode layer 300 is made of conductive materials such as platinum or indium tin oxide, and the thickness of the bottom electrode is 50-150 nm. In this embodiment, the bottom electrode layer 300 is made of indium tin oxide and has a thickness of 100 nm.
The insulating layer 301 is a single-layer transparent glass or a three-layer structure, in which the three-layer structure is a titanium layer, a silicon dioxide layer, and a silicon layer stacked in sequence from top to bottom. The material of the insulating layer 301 is not particularly limited, and other materials may be used, which are not listed here, and the insulating layer 301 may be selected as appropriate according to actual needs. In this embodiment, the insulating layer 301 and the bottom electrode layer 300 are integrally formed as a substrate, and the substrate is prepared in advance and can be used as it is, but may be obtained by preparing the bottom electrode layer 300 on the insulating layer 301 by a method such as an evaporation coating method.
The invention also provides a preparation method of the memristor with the synapse-like long-term plasticity, which is used for preparing the memristor with the synapse-like long-term plasticity, and the preparation method comprises the following steps:
s1, providing a substrate, and cleaning and hydrophilically treating the substrate;
s2, preparing a first resistance change layer on the substrate by using an aqueous solution method;
s3, preparing a second resistance-change layer on the first resistance-change layer by using an aqueous solution method;
and S4, preparing a top electrode layer on the second resistance change layer to obtain the memristor with synapse-like long-term plasticity.
Before the second resistance-change layer is prepared on the first resistance-change layer, the preparation method further comprises the step of carrying out hydrophilic treatment on the first resistance-change layer, so that the bonding strength of the first resistance-change layer and the second resistance-change layer is enhanced.
The specific preparation steps of the first resistance change layer are as follows: preparing an alumina precursor solution at the temperature of 20-30 ℃, standing for 5-10min at room temperature, and dripping the alumina precursor solution on a substrate; spin coating in air at 2000-; annealing at a temperature of 250-350 ℃.
The second resistance-change layer is prepared by the following specific steps: preparing a gallium oxide precursor solution at the temperature of 20-30 ℃, standing for 5-10min at room temperature, and dripping the gallium oxide precursor solution on the first resistance change layer; spin coating in air at 2000-; annealing at a temperature of 250-350 ℃.
And the protective layer arranged on the surface of the top electrode layer far away from the second resistance change layer and the top electrode layer are both prepared by adopting an evaporation coating method.
The preparation method is a solution method, has the characteristics of environmental protection, low temperature, less investment on equipment and raw materials, and large-area preparation, realizes large-scale industrial application, and has the advantages of simple and efficient preparation and low preparation cost due to the lower temperature in the preparation process.
The following is a detailed description of the method for preparing a memristor with synapse-like long-term plasticity.
Step one, cleaning and hydrophilically treating a substrate
Completely immersing the substrate into a beaker containing absolute ethyl alcohol, and placing the beaker in a deionized water environment for ultrasonic cleaning for 25 min; washing the substrate with deionized water to remove residual ethanol impurities; then completely immersing the substrate into a beaker containing acetone, and placing the beaker in a deionized water environment for ultrasonic cleaning again for 25 min; then completely immersing the substrate into a beaker containing deionized water, and placing the beaker in a deionized water environment for ultrasonic cleaning for 25 min; finally, the substrate is rinsed with deionized water and blown dry with nitrogen, thereby completing the cleaning of the substrate.
And (3) putting the substrate subjected to ultrasonic cleaning and drying treatment into a vacuum cavity of a surface plasma cleaning machine, performing surface plasma cleaning to enhance the hydrophilicity of the bottom electrode layer, wherein the time of the surface plasma cleaning process lasts for 45 min. The hydrophilic treatment is to change the hydrophilicity of the surface of the bottom electrode layer.
Step two, preparing a first resistance change layer
Preparing an alumina precursor solution at the temperature of 25 ℃, specifically: placing 9.3536g of aluminum nitrate powder with the purity of 99.99% in a beaker, adding 10ml of deionized water into the beaker to prepare 2.5M of alumina precursor solution, and uniformly stirring until the solution is clarified to obtain the alumina precursor solution; standing for 10min at room temperature, dripping the prepared alumina precursor solution on the bottom electrode layer through a syringe with the aperture of 0.22 μm and a PES (polyether sulfone) filter tip within 30min after finishing surface plasma cleaning, and spin-coating in air at the speed of 4000rpm for 40 s; and after the spin coating is finished, annealing for 1h on a heating plate at 250 ℃, and solidifying the alumina precursor solution on the bottom electrode layer to form a film to obtain the first resistance change layer.
Step three, hydrophilic treatment of the first resistance change layer
And (3) placing the substrate with the first resistance-change layer into a vacuum chamber of a surface plasma cleaning machine, and performing surface plasma cleaning, wherein the time of the surface plasma cleaning process lasts for 45min, so that the first resistance-change layer is hydrophilic.
Step four, preparing a second resistance change layer
Preparing a gallium oxide precursor solution at the temperature of 25 ℃, specifically: putting 6.8742g of gallium nitrate powder with the purity of 99.99% in a beaker, adding 10ml of deionized water into the beaker to prepare 2.5M gallium oxide precursor solution, and uniformly stirring until the solution is clarified to obtain the gallium oxide precursor solution; standing for 10min at room temperature, dripping the prepared gallium oxide precursor solution on the first resistance change layer through an injector with an aperture of 0.22 μm and a PES (polyether sulfone) filter tip within 30min after finishing surface plasma cleaning, and spin-coating in air at the speed of 4000rpm for 40 s; and after the spin coating is finished, placing the substrate on a heating plate at 250 ℃ for annealing for 0.5h, and solidifying the gallium oxide precursor solution on the first resistance change layer to form a film so as to obtain a second resistance change layer.
Step five, preparing a top electrode layer
And placing the granular metal material Ag in a crucible of a thermal evaporation coating machine, covering a mask plate with the aperture of 0.1mm on the surface of the second resistance change layer, downwards placing the mask plate on a suction plate in a cavity of the coating machine, closing the cavity to perform thermal evaporation coating operation, and coating the metal material Ag on the second resistance change layer to form a top electrode layer.
Step six, preparing a protective layer
Placing granular metal material Al in a crucible of a thermal evaporation coating machine, covering a mask plate with the aperture of 0.1mm on a top electrode layer, placing the mask plate downwards on a suction plate in a cavity of the coating machine, closing the cavity to perform thermal evaporation coating operation, and coating a metal Al protective layer on the surface of the top electrode layer to obtain the memristor device.
Referring to fig. 2, a resistance change effect test is performed on the memristor prepared in the embodiment, a horizontal coordinate point 0 is taken as a boundary, a positive axis is a SET (SET) process, a negative axis is a RESET (RESET) process, voltage bias absolute values of the devices are below 1V, the device working voltage is low, energy consumption is low, the resistance change effect is kept within a certain range, a gradual change phenomenon with a certain probability occurs in the RESET process, and the tolerance and the stability of the device are also improved. The ratio of high to low resistance in fig. 2 (greater than 20000) is significantly larger than that of the prior art memristor, and the storage data capacity is increased.
Referring to fig. 3, a synapse-like long-term plasticity test is performed on the memristor prepared in this embodiment, where the abscissa is the number of pulse excitations, the ordinate is the conductance of the device, the pulse amplitudes are all below 1V, the first 100 pulses are continuous positive pulses of 0.5V/10ms, and the last 100 pulses are continuous negative pulses of 0.5V/10ms, and the test result shows the multi-level conductance, i.e., the multi-level resistance state, which proves that the device has the synapse-like long-term plasticity of the device. And the linearity degree of data in the synaptic performance of the device is good, which means that the device can be more suitable for an ANN (artificial neural netwok) algorithm.
In summary, 1) compared with a memristor with a single-layer pure metal oxide layer, the memristor obtained by the method has the advantages of better resistance change effect, low power consumption, low working voltage, absolute value smaller than 1V, and improved tolerance and stability;
2) the preparation is carried out by a pure solution method, the operation is simple and convenient, the cost is low, the investment of equipment and raw materials is less, and the preparation can be used for large-area preparation, so that large-scale industrial application is realized;
3) the simple substance metal or simple substance metal compound material is used as the top electrode layer to replace the traditional oxide material, thereby reducing the cost and optimizing the preparation process;
4) the memristor enables long-term plasticity of synapse-like devices.
The technical features of the embodiments described above may be arbitrarily combined, and for the sake of brevity, all possible combinations of the technical features in the embodiments described above are not described, but should be considered as being within the scope of the present specification as long as there is no contradiction between the combinations of the technical features.
The above-mentioned embodiments only express several embodiments of the present invention, and the description thereof is more specific and detailed, but not construed as limiting the scope of the invention. It should be noted that, for a person skilled in the art, several variations and modifications can be made without departing from the inventive concept, which falls within the scope of the present invention. Therefore, the protection scope of the present patent shall be subject to the appended claims.
Claims (10)
1. The memristor with the synapse-like long-term plasticity is characterized by comprising a substrate, a first resistance change layer, a second resistance change layer and a top electrode layer which are sequentially stacked from bottom to top, wherein the substrate comprises an insulating layer and a bottom electrode layer which are stacked from bottom to top, the first resistance change layer is made of aluminum oxide, and the second resistance change layer is made of gallium oxide.
2. The memristor with synapse-like long-term plasticity according to claim 1, wherein the top electrode layer comprises a plurality of top electrodes with cylindrical structures, the top electrodes are made of metallic silver, metallic copper or gold, and the top electrodes have a thickness of 20-60nm and a diameter of 0.1-0.5 mm.
3. The memristor with synapse-like long-term plasticity, according to claim 1, wherein the top electrode layer is provided with a protective layer on a surface far from the second resistance change layer, the protective layer being made of metallic aluminum or metallic tungsten.
4. The memristor with synapse-like long-term plasticity of claim 1, wherein the bottom electrode layer is made of platinum metal or indium tin oxide, and the thickness of the bottom electrode is 50-150 nm.
5. The memristor with synapse-like long-term plasticity according to claim 1, wherein the insulating layer is a single-layer transparent glass or a three-layer structure, and the three-layer structure is a titanium layer, a silicon dioxide layer and a silicon layer which are sequentially stacked from top to bottom.
6. A method for preparing a memristor with synapse-like long-term plasticity, the method being used for preparing the memristor with synapse-like long-term plasticity according to any one of claims 1-5, the method comprising:
s1, providing a substrate, and cleaning and hydrophilically treating the substrate;
s2, preparing a first resistance change layer on the substrate by using an aqueous solution method;
s3, preparing a second resistance-change layer on the first resistance-change layer by using an aqueous solution method;
and S4, preparing a top electrode layer on the second resistance change layer to obtain the memristor with synapse-like long-term plasticity.
7. The method of fabricating a memristor with synapse-like long-term plasticity as claimed in claim 6, wherein the first resistive layer is fabricated by the following steps: preparing an alumina precursor solution at the temperature of 20-30 ℃, standing for 5-10min at room temperature, and dripping the alumina precursor solution on the substrate; spin coating in air at 2000-; annealing at a temperature of 250-350 ℃.
8. The method of fabricating a memristor with synapse-like long-term plasticity as claimed in claim 6, wherein the second resistive layer is fabricated by the following steps: preparing a gallium oxide precursor solution at the temperature of 20-30 ℃, standing for 5-10min at the room temperature, and dripping the gallium oxide precursor solution on the first resistance change layer; spin coating in air at 2000-; annealing at a temperature of 250-350 ℃.
9. The method of claim 6, wherein the top electrode layer has a protective layer disposed on a surface thereof remote from the second resistive layer, and the top electrode layer and the protective layer are formed by evaporation coating.
10. The method of fabricating a memristor with synaptic long-term plasticity according to claim 6, wherein before fabricating a second resistive layer on the first resistive layer, the method further comprises performing hydrophilic treatment on the first resistive layer.
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