CN111009608B - Solid electrolyte memristor and preparation method and application thereof - Google Patents
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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
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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
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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
- H10N70/245—Multistable switching devices, e.g. memristors based on migration or redistribution of ionic species, e.g. anions, vacancies the species being metal cations, e.g. programmable metallization cells
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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
- H10N70/8833—Binary metal oxides, e.g. TaOx
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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
- H10N70/884—Switching materials based on at least one element of group IIIA, IVA or VA, e.g. elemental or compound semiconductors
- H10N70/8845—Carbon or carbides
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Abstract
The invention provides a solid electrolyte memristor, a preparation method and application thereof, wherein the memristor sequentially comprises a substrate serving as a bottom electrode and Ga (gallium) from bottom to top 2 O 3 The C quantum dot layer is 10-100 nm in thickness. The preparation process of the C quantum dot layer comprises the following steps: and (3) dripping the C solution on the substrate to automatically expand the C solution and cover the whole surface of the substrate, and then annealing the substrate at 80-120 ℃ for 10-50 min in the atmospheric environment to obtain the C quantum dot layer. The memristor provided by the invention is added with the C quantum dots and forms the C conductive filament. The device has the advantages of good device performance, realization of the function of simulating bioaugmentation learning, unique structure, good performance and wide application prospect.
Description
Technical Field
The invention relates to the technical field of memristor preparation, in particular to a solid electrolyte memristor, and a preparation method and application thereof.
Background
In recent years, the size of integrated circuit processes has been deep below 20nm, the physical limit of conventional nonvolatile memory devices has been approached, and the development of new generation nonvolatile memories has become a popular field of research by scientists in various countries. Currently, the main types of non-volatile memory are magnetic memory, phase change memory, and memristors. The memristor has the advantages of low power consumption, high reading and writing speed, good data holding capacity, simple manufacture, easy integration and the like, and is a new generation of memory with great application prospect.
The general structure of the memristor is a typical sandwich structure, and comprises an upper electrode, a lower electrode and a material which is arranged between the upper electrode and the lower electrode and can generate memristor phenomenon. Under the action of the externally applied bias voltage, the resistance state of the device can be changed into a high-low resistance state, so that 0 and 1 storage is realized. For memristors, selecting different resistive layer materials can have a large impact on the device, so to speak, the resistive layer materials are the core of the memristor.
Scientific researches show that the material capable of being used as the resistance change layer is various, and four main types exist at present: first, perovskite oxide, many devices based on this material exhibit bipolar storage characteristics, but such materials are difficult to prepare and are not compatible with conventional devices. And secondly, the transition metal oxide and the transition metal binary oxide have the advantages of simple components, low cost, easiness in preparation, compatibility with a CMOS (complementary metal oxide semiconductor) process and the like, and although memristors based on the transition metal binary oxide have a plurality of advantages, the resistance change mechanism is not completely clear, the reliability of the devices is still to be researched, the development and the application of the devices are hindered to a certain extent, and the development prospect of the memristors is not very clear. And thirdly, solid electrolyte, wherein the memristor has a typical sandwich structure and comprises an electrochemical active electrode (Ag, cu and the like), an electrochemical inert electrode (W, pt and the like) and a resistance change functional layer formed by solid electrolyte materials. The memristive property is caused by the formation and fracture of metal conductive filaments caused by the migration of metal cations generated by electrochemical reaction of active metal electrode materials under the action of an electric field. When a proper forward voltage is applied to the active metal electrode, the active metal is subjected to oxidation reaction to become corresponding metal cations, the corresponding metal cations migrate to the inert electrode through the solid electrolyte material under the action of an electric field, electrons are obtained after reaching the surface of the inert electrode, and reduction reaction is performed to generate metal atoms. And metal atoms are deposited on the cathode, metal filaments grow on one side of the inert electrode, and after the filaments grow completely and are connected with the active electrode of the metal, a conductive channel is formed, the memristor is changed from a high-resistance state to a low-resistance state, and the device is conducted. After reverse voltage is applied, electrochemical dissolution phenomenon can occur on the metal conductive filaments, metal forming the conductive channel is oxidized into metal cations and migrates towards the active electrode under the action of an electric field, at the moment, the conductive channel breaks, the memristor is changed from a low resistance state to a high resistance state, and the device is switched to a closed state. The existing solid electrolyte memristor generally has the problems of poor repeatability and non-centralized switching parameters. Fourth, the organic material is simple to make at present, the cost is low, utilize the bistable property of the organic material to make memristor more extensive research. The greatest advantage of organic materials over inorganic materials is the wide variety and wide choice. Although organic materials have many advantages, most organic materials are poor in stability and storage performance, not resistant to high temperature, poor in durability and data memory characteristics, and slow in operation speed of reading, writing, erasing and the like, so that the application of the organic materials in the field of memristor devices is affected to a certain extent.
Therefore, further research on memory devices with stable resistance change, good memory performance, good fatigue resistance and durability, and fast operation speed of reading, writing, erasing and the like is a subject of industry's product search.
Disclosure of Invention
The invention aims to provide a solid electrolyte memristor, and a preparation method and application thereof, so as to solve the problems of unstable resistance change, poor storage performance, poor durability and poor data memory characteristic of the existing memristor.
The invention aims at realizing the following technical scheme: a solid electrolyte memristor comprises a substrate serving as a bottom electrode and Ga from bottom to top 2 O 3 The C quantum dot layer is 10-100 nm in thickness.
The preparation process of the C quantum dot layer comprises the following steps: and (3) dripping the C solution on the substrate to automatically expand the C solution and cover the whole surface of the substrate, and then annealing the substrate at 80-120 ℃ for 10-50 min in the atmospheric environment to obtain the C quantum dot layer.
The preparation process of the solution C comprises the following steps: c is dissolved in toluene according to the mass-volume ratio of 10-30 mg to 1-5 mL, and is uniformly mixed, and then a filter with the mass-volume ratio of 0.01-0.5 mu m is used for filtering, so that the obtained filtrate is the C solution.
The bottom electrode is made of electrochemical inert electrode materials, and the upper electrode layer is made of electrochemical active electrode materials.
The Ga 2 O 3 The thickness of the conversion layer is 3-50 nm, and the thickness of the upper electrode layer is 50-200 nm.
A preparation method of a solid electrolyte memristor comprises the following steps:
(a) Sequentially cleaning substrate as bottom electrode with ultrasonic wave in acetone, alcohol and deionized water, taking out, and using N 2 Blow-drying;
(b) Sputter deposition of Ga on a substrate 2 O 3 A conversion layer;
(c) Dripping the solution C into the deposited Ga 2 O 3 Automatically expanding the C solution on the substrate of the conversion layer and covering the whole surface of the substrate, and then annealing the substrate at 80-120 ℃ for 10-50 min in the atmospheric environment to form a C quantum dot layer on the substrate, wherein the thickness of the C quantum dot layer is controlled to be 10-100 nm;
(d) And sputtering and depositing an upper electrode layer on the C quantum dot layer.
The preparation process of the solution C comprises the following steps: c is dissolved in toluene according to the mass-volume ratio of 10-30 mg to 1-5 mL, and is uniformly mixed, and then a filter with the mass-volume ratio of 0.01-0.5 mu m is used for filtering, so that the obtained filtrate is the C solution.
The bottom electrode is made of electrochemical inert electrode materials, and the upper electrode layer is made of electrochemical active electrode materials.
The Ga 2 O 3 The thickness of the conversion layer is 3-50 nm, and the thickness of the upper electrode layer is 50-200 nm.
The step (b) is specifically as follows: fixing the substrate on the substrate table of the cavity of the magnetron sputtering equipment, and vacuumizing the cavity to 1×10 -4 ~6×10 -4 Pa, introducing Ar with the flow rate of 20-75 sccm and O with the flow rate of 10-40 sccm into the cavity 2 Adjusting the interface valve to maintain the pressure in the cavity at 1-6 Pa, and opening to control Ga 2 O 3 The radio frequency source for starting the target material adjusts the power of the radio frequency source to be 60-100W so as to lead Ga 2 O 3 Starting a target material, and pre-sputtering for 1-5 min; performing formal sputtering for 5-20 min, and depositing to form Ga on the substrate 2 O 3 A conversion layer.
The step (d) is specifically as follows: placing a mask on a substrate for forming a C quantum dot layer, and vacuumizing a cavity of a magnetron sputtering device to 1X 10 -4 ~4×10 -4 Pa, introducing Ar with the flow of 20-30 sccm into the cavity, adjusting the interface valve to maintain the pressure in the cavity at 1-6 Pa, and opening to control the starting of the upper electrode target materialThe power of the direct current source is adjusted to be 8-11W, so that the upper electrode target material is started, and the sputtering is performed for 4-6 min; and finally, formally sputtering for 6-10 min, and forming an upper electrode layer on the C quantum dot layer.
The application of the solid electrolyte memristor in the preparation of a nerve bionic device.
The memristor prepared by the method optimizes the device performance by using the C quantum dots, and forms a C conductive path (C conductive filament) to influence the resistance state. The memristor is different from the traditional memristor prepared by using oxides, has novel and unique structure, has good resistance change characteristics through performance detection, shows relatively stable resistance change, has relatively large phase difference between a high resistance value and a low resistance value, is not easy to cause misread, has good performance, realizes a simulated biological associative learning function, and has the advantages of more stable storage performance, strong durability and wider application prospect. The preparation method provided by the invention is simple and easy to implement, has good operability and is suitable for large-scale application.
Drawings
FIG. 1 is a schematic diagram of a memristor fabricated in accordance with the present disclosure. In the figure: 1. substrate, 2, ga 2 O 3 The conversion layer, 3, C quantum dot layer, 4, upper electrode layer.
FIG. 2 is a cross-sectional Transmission Electron Microscope (TEM) image of the memristor prepared in example 2, with the presence of conductive filaments being clearly observed.
FIG. 3 is a graph of current-voltage characteristics and switching power curves of a memristor prepared in example 2.
FIG. 4 is an associative learning behavior of a simulated bapulov dog experiment for a memristor prepared in example 2.
Detailed Description
The following examples serve to further illustrate the invention in detail, but are not intended to limit the invention in any way. Unless specifically stated otherwise, the reagents, methods and apparatus employed in the present invention are those conventional in the art.
Example 1
The memristor structure of the invention is shown in fig. 1, and comprises a lining from bottom to topBottom 1, ga 2 O 3 A conversion layer 2, a C quantum dot layer 3 and an upper electrode layer 4. Wherein the substrate 1 may be Pt substrate, ga 2 O 3 The thickness of the conversion layer 2 is 3-50 nm; the thickness of the C quantum dot layer 3 is 10-100 nm; the thickness of the upper electrode layer 4 is 50-200 nm, and the upper electrode layer 4 is a plurality of round electrodes with the diameter of 80-300 mu m which are uniformly distributed on the C quantum dot layer 3.
Example 2
The specific preparation process of the solid electrolyte memristor is as follows:
(1) The surface of the Pt substrate is firstly dipped with acetone and absolute ethyl alcohol in turn by using a camera to wipe absorbent cotton, small particles such as dust attached to the surface are wiped off, oil stains on the surface are primarily removed, then the Pt substrate is placed in acetone and is cleaned by ultrasonic for 10min, then is placed in alcohol and is cleaned by ultrasonic for 10min, then is taken out by using a clamp and is placed in deionized water and is cleaned by ultrasonic for 5min, and then is taken out by using N 2 Blow-drying;
(2) Preparation of the conversion layer: fixing a Pt substrate on a magnetron sputtering tabletting table by using magnetron sputtering equipment, placing the tabletting table on a substrate table in a cavity, closing the cavity, and vacuumizing the cavity; to the pressure in the cavity is pumped to 5 multiplied by 10 -4 When Pa is less, an air inlet valve is opened, 50sccm Ar and 25sccm O are introduced into the cavity 2 The pressure in the cavity is regulated to maintain the air pressure of the cavity at 3Pa by regulating the opening and closing of the gate valve; turning on the RF source to make Ga 2 O 3 Starting target material, regulating power of radio frequency source to 80W, pre-sputtering for 3min, and final sputtering for 10min to form Ga with thickness of 10nm on the substrate 2 O 3 A conversion layer;
(3) Dissolving 15mg of C in 1mL of toluene, uniformly mixing, and filtering the obtained solution by using a 0.22 mu m filter to obtain a C solution; will be clean and grow with Ga 2 O 3 The substrate of the conversion layer is arranged in the middle of the annealing furnace; sucking the prepared C solution by a disposable needle tube, dripping the C solution at the middle position of a substrate, expanding the solution to the periphery, finally covering the whole surface, and then annealing for 20min in the atmosphere at 80 ℃ to obtain a C quantum dot layer;
(4) Growing a Pd electrode layer: placing a mask plate uniformly distributed with round holes with the diameter of 90 μm on the C quantum dot layer formed in the step (3), placing the mask plate on a substrate table in a cavity, closing the cavity after fixing, and vacuumizing the cavity and an air path to 2×10 -4 About Pa; opening a direct current source for controlling the starting of the Pd target material, adjusting the power of the direct current source to be 10W, enabling the Pd target material to start, and then pre-sputtering for 6min; then formally sputtering for 10min, and finally sputtering in Ga 2 O 3 A Pd electrode layer with a thickness of 60nm is formed on the resistive layer.
The structure of the memristor prepared according to the steps of the implementation can be expressed as Pd/C/Ga 2 O 3 Pt. The cross-sectional view is shown in fig. 2, and a distinct C-conduction path is observed upon application of a voltage.
Embodiment 2 above is any embodiment of the preparation method protected by the present invention, as long as the memristors of the present invention can be obtained within the process parameters described in the claims and the specification, and the prepared memristors have substantially similar performance as the devices prepared in this embodiment.
Example 3 Performance test
1. Switching voltage detection
The current-voltage characteristic curve was determined by applying the scan voltage to the C-filament memristor prepared in example 2, and the result is shown in fig. 3. As can be seen from fig. 3, when the forward scanning voltage is gradually increased from 0V to 1.7V, the device is initially in a high-resistance state (the current is smaller), and when the current is about 1.7V, the resistance state of the device is gradually changed from the high-resistance state to the low-resistance state, and the low-resistance state reaches a stable value along with the increase of the voltage; after the maximum scan voltage is reached, the scan voltage starts to gradually decrease, when the scan voltage continues to decrease to 0V, then negative scan starts to reach the closing voltage when the scan voltage is about-0.1V, the low resistance state gradually changes to the high resistance state, and the device is kept in the high resistance state until the voltage scans back to 0V.
2. Simulating bioassay learning characteristics
The ability of biology to link related things together, i.e., associative learning. These can be represented by the named pavlov condition or classical condition. As can be seen from fig. 4, we define the bell as a neutral stimulus, the food as an unconditional stimulus, and the salivation work as an unconditional response. The training program is that after we shake bell repeatedly, we feed food. After the training process is finished, only bell will cause saliva reaction like feeding food. In this case, the conditional response is salivation caused by bell, and the conditional stimulus is bell. When paired, the "chime" and "food" signals were applied to the C-filament memristor, as shown in fig. 4a and b. The initial resistance state of the C-filament memristor is HRS, the only "diet" would result in a pronounced unconditional response, while the only "Bell" would not cause a response. When a "chime" and "food" pulse are applied to the C-filament memristor simultaneously, the memristor will turn on as shown in FIG. 4C. In this process, two signals will be associated, that is, only the "ringing" signal will result in a significant conditional response. If this operation is repeated, the unconditional reflection will fade away, i.e. associative learning will not occur, similar to pavlov's associative learning.
The embodiments described above are preferred embodiments of the present invention, but the embodiments of the present invention are not limited to the embodiments described above, and any other changes, modifications, substitutions, combinations, and simplifications that do not depart from the spirit and principles of the present invention should be made in the equivalent manner, and are included in the scope of the present invention.
Claims (6)
1. A solid electrolyte memristor is characterized by sequentially comprising a substrate serving as a bottom electrode and Ga from bottom to top 2 O 3 The C quantum dot layer is 10-100 nm in thickness;
the preparation process of the C quantum dot layer comprises the following steps: dropping the C solution on the substrate to automatically expand the C solution and cover the whole surface of the substrate, and then annealing the substrate at 80-120 ℃ for 10-50 min in the atmospheric environment to obtain a C quantum dot layer;
the preparation process of the solution C comprises the following steps: c is dissolved in toluene according to the mass-volume ratio of 10-30 mg to 1-5 mL, uniformly mixed, and then filtered by a filter with the thickness of 0.01-0.5 mu m, and the obtained filtrate is the solution C;
the bottom electrode is made of electrochemical inert electrode materials, and the upper electrode layer is made of electrochemical active electrode materials;
the Ga 2 O 3 The thickness of the conversion layer is 3-50 nm, and the thickness of the upper electrode layer is 50-200 nm;
the C quantum dots form C conductive filaments to affect the resistive state.
2. The preparation method of the solid electrolyte memristor is characterized by comprising the following steps of:
(a) Sequentially cleaning substrate as bottom electrode with ultrasonic wave in acetone, alcohol and deionized water, taking out, and using N 2 Blow-drying;
(b) Sputter deposition of Ga on a substrate 2 O 3 A conversion layer;
(c) Dripping the solution C into the deposited Ga 2 O 3 Automatically expanding the C solution on the substrate of the conversion layer and covering the whole surface of the substrate, and then annealing the substrate at 80-120 ℃ for 10-50 min in the atmospheric environment to form a C quantum dot layer on the substrate, wherein the thickness of the C quantum dot layer is controlled to be 10-100 nm;
(d) Sputtering and depositing an upper electrode layer on the C quantum dot layer;
the C quantum dots form C conductive filaments to affect the resistive state.
3. The method for preparing a solid electrolyte memristor according to claim 2, wherein the preparation process of the C solution is: c is dissolved in toluene according to the mass-volume ratio of 10-30 mg to 1-5 mL, and is uniformly mixed, and then a filter with the mass-volume ratio of 0.01-0.5 mu m is used for filtering, so that the obtained filtrate is the C solution.
4. The method of claim 2, wherein the bottom electrode is made of an electrochemically inert electrode material and the upper electrode layer is made of an electrochemically active electrode material.
5. The method of manufacturing a solid state electrolyte memristor of claim 2, wherein the Ga 2 O 3 The thickness of the conversion layer is 3-50 nm, and the thickness of the upper electrode layer is 50-200 nm.
6. Use of the solid-state electrolyte memristor of claim 1 in the fabrication of a neuromorphic device.
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| CN113013330B (en) * | 2021-02-26 | 2023-05-02 | 华中科技大学 | ZnS-SiO-based material 2 Bidirectional self-limiting memristor and preparation method thereof |
| CN113206195B (en) * | 2021-04-30 | 2022-09-20 | 华中科技大学 | Memristor for regulating and controlling positioning of conductive filament based on quantum dots and preparation method of memristor |
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