CN111009608A - Solid electrolyte memristor and preparation method and application thereof - Google Patents
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- 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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Abstract
The invention provides a solid electrolyte memristor and a preparation method and application thereof, wherein the memristor sequentially comprises a substrate serving as a bottom electrode and Ga from bottom to top2O3The quantum dot structure comprises a conversion layer, a C quantum dot layer and an upper electrode layer, wherein the thickness of the C quantum dot layer is 10-100 nm. The preparation process of the C quantum dot layer comprises the following steps: and dropping the solution C on the substrate to enable the solution C to automatically expand and cover the whole substrate surface, and then annealing the substrate at the temperature of 80-120 ℃ for 10-50 min in an atmospheric environment to obtain the quantum dot layer C. The memristor provided by the invention is added with the C quantum dots, and the C conductive filament is formed. The device has the advantages of good device performance, realization of the function of simulating biological association learning, unique structure, good performance and wide application prospect.
Description
Technical Field
The invention relates to the technical field of memristors, in particular to a solid electrolyte memristor and a preparation method and application thereof.
Background
In recent years, the size of integrated circuit technology has been reduced to below 20nm, the conventional non-volatile memory device has approached the physical limit, and the development of a new generation of non-volatile memory has become a popular field of research for scientists in various countries. Currently, the main types of non-volatile memories are magnetic memories, phase change memories and memristors. The memristor has the advantages of low power consumption, high read-write speed, good data retention capacity, simplicity in manufacturing, easiness in integration and the like, and is a new-generation memory with a great application prospect.
The general structure of the memristor is a typical sandwich structure, and the memristor is provided with an upper electrode, a lower electrode and a material which is arranged between the upper electrode and the lower electrode and can generate a memristive phenomenon. Under the action of an external bias voltage, the resistance state of the device is converted into a high-low resistance state, so that the storage of 0 and 1 is realized. For the memristor, selecting different resistance change layer materials has a great influence on the device, and the resistance change layer materials can be considered as the core of the memristor.
Scientific research shows that the materials capable of serving as the resistance change layer are various, and at present, four main types exist: the perovskite oxide is a perovskite oxide, and a plurality of devices based on the perovskite oxide show bipolar storage characteristics, but the preparation process of the perovskite oxide is difficult and is incompatible with the traditional devices. The second is transition metal oxide, transition metal binary oxide has the advantages of simple components, low cost, easy preparation, compatible manufacture with CMOS process and the like, although the memristor based on the transition metal binary oxide has many advantages, the resistance change mechanism is not completely clear, the reliability of the memristor needs to be researched, the development and the application of the memristor are hindered to a certain extent, and the development prospect of the memristor is not clear. And thirdly, the memristor is provided with 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 a solid electrolyte material. Their memristive properties are caused by the formation and breakage of metal conductive filaments caused by the migration of metal cations generated by electrochemical reactions 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 can generate oxidation reaction to be changed into corresponding metal cations, the metal cations migrate to the inert electrode through the solid electrolyte material under the action of an electric field to obtain electrons after reaching the surface of the inert electrode, and the metal atoms are generated through reduction reaction. Metal atoms are deposited on a cathode, a metal filament grows on one side of an inert electrode, when the filament grows completely and is connected with a metal active electrode, a conductive channel is formed, the memristor is changed from a high-resistance state to a low-resistance state, and a device is conducted. After reverse voltage is applied, the metal conductive filament can generate an electrochemical dissolution phenomenon, metal forming a conductive channel is oxidized into metal cations and migrates to an active electrode under the action of an electric field, at the moment, the conductive channel is broken, the memristor is changed from a low resistance state to a high resistance state, and the device is switched to a closed state. The problems of poor repeatability and non-centralized switching parameters commonly exist in the existing solid electrolyte memristor. And fourthly, the organic material is simple to manufacture and low in cost at present, and the research of manufacturing the memristor by utilizing the bistable characteristic of the organic material is relatively wide. Compared with inorganic materials, organic materials have the greatest advantages of being wide in variety and wide in choice. Although the organic material has many advantages, most of the organic materials have poor stability and storage performance, are not high temperature resistant, have poor durability and data memory characteristics, and have slow operation speeds of reading, writing, erasing and the like, which affects the application of the organic material in the field of memory devices to a certain extent.
Therefore, it is an active topic of research in the industry to further study the memory devices with stable resistance variation, good memory performance, good memory characteristics, good fatigue endurance, and fast operation speed of reading, writing, erasing, etc.
Disclosure of Invention
The invention aims to provide a solid electrolyte memristor, and a preparation method and application thereof, and aims to solve the problems of unstable resistance change, poor storage performance, poor durability and poor data memory characteristics of the conventional memristor.
The purpose of the invention is realized by the following technical scheme: a solid electrolyte memristor sequentially comprises a substrate serving as a bottom electrode and Ga from bottom to top2O3The quantum dot structure comprises a conversion layer, a C quantum dot layer and an upper electrode layer, wherein the thickness of the C quantum dot layer is 10-100 nm.
The preparation process of the C quantum dot layer comprises the following steps: and dropping the solution C on the substrate to enable the solution C to automatically expand and cover the whole substrate surface, and then annealing the substrate at the temperature of 80-120 ℃ for 10-50 min in an atmospheric environment to obtain the quantum dot layer C.
The preparation process of the solution C comprises the following steps: dissolving C in toluene according to the mass-to-volume ratio of 10-30 mg: 1-5 mL, uniformly mixing, and filtering by using a filter of 0.01-0.5 mu m to obtain a filtrate, namely the solution C.
The bottom electrode is made of an electrochemical inert electrode material, and the upper electrode layer is made of an electrochemical active electrode material.
The Ga is2O3The 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) cleaning the substrate as bottom electrode in acetone, alcohol and deionized water successively by ultrasonic wave, taking out, and using N2Drying;
(b) sputter deposition of Ga on a substrate2O3A translation layer;
(c) adding the solution C dropwise into the solution deposited with Ga2O3Automatically expanding the C solution on the substrate of the conversion layer and covering the whole substrate surface, and then annealing the substrate at 80-120 ℃ for 10-50 min in an 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: dissolving C in toluene according to the mass-to-volume ratio of 10-30 mg: 1-5 mL, uniformly mixing, and filtering by using a filter of 0.01-0.5 mu m to obtain a filtrate, namely the solution C.
The bottom electrode is made of an electrochemical inert electrode material, and the upper electrode layer is made of an electrochemical active electrode material.
The Ga is2O3The 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 magnetron sputtering equipment cavity, and vacuumizing the cavity to 1 × 10-4~6×10-4Pa, introducing Ar with the flow rate of 20-75 sccm and O with the flow rate of 10-40 sccm into the cavity2Adjusting the interface valve to maintain the pressure in the cavity at 1-6 Pa, and opening the interface valve to control Ga2O3The power of the radio frequency source is adjusted to be 60-100W so that Ga is generated2O3Glow starting of target material and pre-sputtering 15 min; then formally sputtering for 5-20 min, and depositing Ga on the substrate2O3A translation layer.
The step (d) is specifically as follows: placing a mask plate on the substrate on which the C quantum dot layer is formed, and vacuumizing the cavity of the magnetron sputtering equipment to 1 × 10-4~4×10-4Pa, introducing Ar with the flow rate of 20-30 sccm into the cavity, adjusting an interface valve to maintain the pressure in the cavity at 1-6 Pa, turning on a direct current source for controlling the glow starting of the upper electrode target, adjusting the power of the direct current source to 8-11W, so that the upper electrode target is glowing, and pre-sputtering for 4-6 min; and then formally sputtering for 6-10 min to form an upper electrode layer on the C quantum dot layer.
The solid electrolyte memristor is applied to manufacturing of the nerve bionic device.
The memristor prepared by the invention uses the C quantum dots to optimize the device performance, and forms the C conductive path (C conductive filament) to influence the resistance state. Compared with the traditional memristor device prepared by using oxide, the memristor device is novel and unique in structure, has good resistance change characteristics through performance detection, presents more stable resistance change, has larger difference between a high resistance value and a low resistance value, is not easy to cause misreading, has good performance, realizes the function of simulating biological association learning, and has more stable memory 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 structural diagram of a memristor prepared in the present invention. In the figure: 1. substrate, 2, Ga2O3Conversion layer, 3, C quantum dot layer, 4, upper electrode layer.
Fig. 2 is a cross-sectional Transmission Electron Microscope (TEM) picture of the memristor prepared in example 2, where the presence of conductive filaments is clearly observable.
FIG. 3 is a graph of current-voltage characteristics and a switching power diagram of the memristor prepared in example 2.
Fig. 4 is an associative learning behavior of a simulated baroreceptor dog experiment of memristors prepared in example 2.
Detailed Description
The following examples are intended to illustrate the present invention in further detail, but the present invention is not limited thereto in any way. Reagents, methods and apparatus used in the present invention are conventional in the art unless otherwise indicated.
Example 1
The memristor structure of the invention is shown in figure 1 and sequentially comprises a substrate 1 and Ga from bottom to top2O3 A conversion layer 2, a C quantum dot layer 3, and an upper electrode layer 4. Wherein, the substrate 1 can be Pt substrate, Ga2O3The 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 circular electrodes with the diameter of 80-300 μm uniformly distributed on the C quantum dot layer 3.
Example 2
The specific preparation process of the solid electrolyte memristor is as follows:
(1) sequentially dipping absorbent cotton of acetone and absolute ethyl alcohol on the surface of a Pt substrate by using forceps to wipe the surface of the Pt substrate, wiping off small particles such as dust and the like attached to the surface, preliminarily removing oil stains on the surface of the Pt substrate, putting the Pt substrate into acetone to be cleaned for 10min by ultrasonic waves, putting the Pt substrate into alcohol to be cleaned for 10min by ultrasonic waves, taking the Pt substrate out by a clamp to be put into deionized water to be cleaned for 5min by ultrasonic waves, taking the Pt substrate out, and using N2Drying;
(2) preparation of the conversion layer: fixing a Pt substrate on a magnetron sputtering tabletting table by adopting magnetron sputtering equipment, putting the tabletting table on a substrate table in a cavity, fixing, closing the cavity and vacuumizing the cavity; the pressure in the cavity is pumped to 5 multiplied by 10-4When the pressure is lower than Pa, the air inlet valve is opened, and Ar of 50sccm and O of 25sccm are introduced into the cavity2The pressure in the cavity is adjusted to maintain the air pressure of the cavity at 3Pa by adjusting the size of a switch of the gate valve; turning on the radio frequency source to enable Ga2O3Starting the target, adjusting the power of the radio frequency source to 80W, pre-sputtering for 3min, then formally sputtering for 10min to form Ga with the thickness of 10nm on the substrate2O3A translation layer;
(3) mixing 15mg ofDissolving C in 1mL of toluene, mixing uniformly, and filtering the obtained solution by using a 0.22-micrometer filter to obtain a C solution; clean Ga grows on2O3The substrate of the conversion layer is arranged in the middle of the annealing furnace; sucking the prepared C solution by using a disposable needle tube, dripping the solution at the middle position of the substrate, expanding the solution to the periphery, finally covering the whole surface, and then annealing in the atmosphere at the temperature of 80 ℃ for 20min to obtain a C quantum dot layer;
(4) growing a Pd electrode layer: placing a mask plate with uniformly distributed circular holes with the diameter of 90 mu m on the C quantum dot layer formed in the step (3), placing the mask plate on a substrate table in the cavity, closing the cavity after fixing, and vacuumizing the cavity and the air path to 2 x 10-4Pa is about; turning on a direct current source for controlling the starting of the Pd target, adjusting the power of the direct current source to be 10W to enable the Pd target to be capable of starting, and then pre-sputtering for 6 min; then formally sputtering for 10min in Ga2O3A Pd electrode layer with a thickness of 60nm was formed on the resistance change layer.
The structure of the memristor prepared according to the steps of the implementation can be expressed as Pd/C/Ga2O3and/Pt. A cross-sectional view is shown in fig. 2, and a clear C conductive path is observed after applying a voltage.
The above embodiment 2 is any one of the embodiments of the preparation method protected by the present invention, and the memristor of the present invention can be obtained within the process parameter range described in the claims and the specification, and the prepared memristor has substantially similar performance to the device prepared by the present embodiment.
Example 3 Performance testing
1. Switching voltage detection
The current-voltage characteristics of the C filament memristor prepared in example 2 were determined by applying the sweep voltage thereto, and the results are shown in FIG. 3. As can be seen from fig. 3, in the process of gradually increasing the forward scanning voltage from 0V to 1.7V, the device is initially in a high-resistance state (with a small current), and when the forward scanning voltage is about 1.7V, the resistance state of the device gradually changes from the high resistance state to the low resistance state, and as the voltage increases, the low resistance state reaches a stable value; after the maximum scanning voltage is reached, the scanning voltage starts to be gradually reduced, when the scanning voltage is continuously reduced to 0V, then negative scanning is started to be about-0.1V, the closing voltage is reached, the low resistance state is gradually changed into the high resistance state, and the device is kept in the high resistance state until the voltage is scanned back to 0V.
2. Simulating biological associative learning characteristics
Biology's ability to link related things together, i.e. associative learning. These can be expressed in the named pavlov conditions or classical conditions. As can be seen in fig. 4, we defined chime as the neutral stimulus, food as the unconditional stimulus, and salivation as the unconditional response. The training program is that we repeatedly shake the bell and then feed food. After the training process is finished, only the bell will cause saliva reaction like feeding food. In this case, the conditional response is drooling caused by bell, and the conditional stimulus is bell. When paired, the "chime" and "food" signals are applied to the C filament memristors, as shown in fig. 4a and b. The initial resistive state of the C filament memristor is HRS, with the only "food" resulting in a significant unconditional response, and the only "Bell" not causing a response. When the "chime" and "food" pulses are simultaneously applied to the C filament memristor, the memristor will open, as shown in fig. 4C. In this process, two signals will be correlated, that is, only the "ring" signal will result in a significant condition response. If this operation is repeated, the unconditional reflex will fade away, i.e., associative learning will not occur, similar to pavlov's associative learning.
The above embodiments are preferred embodiments of the present invention, but the present invention is not limited to the above embodiments, and any other changes, modifications, substitutions, combinations, and simplifications which do not depart from the spirit and principle of the present invention should be construed as equivalents thereof, and all such changes, modifications, substitutions, combinations, and simplifications are intended to be included in the scope of the present invention.
Claims (10)
1. The solid electrolyte memristor is characterized by sequentially comprising a substrate serving as a bottom electrode and Ga from bottom to top2O3Conversion layer, C quantum dot layer, andand the thickness of the upper electrode layer is 10-100 nm.
2. The solid-state electrolyte memristor according to claim 1, wherein the preparation process of the C quantum dot layer is: and dropping the solution C on the substrate to enable the solution C to automatically expand and cover the whole substrate surface, and then annealing the substrate at the temperature of 80-120 ℃ for 10-50 min in an atmospheric environment to obtain the quantum dot layer C.
3. The solid-state electrolyte memristor according to claim 2, wherein the preparation process of the C solution is: dissolving C in toluene according to the mass-to-volume ratio of 10-30 mg: 1-5 mL, uniformly mixing, and filtering by using a filter of 0.01-0.5 mu m to obtain a filtrate, namely the solution C.
4. The solid-state electrolyte memristor according to claim 1, wherein the bottom electrode is made of an electrochemically inert electrode material, and the top electrode layer is made of an electrochemically active electrode material.
5. The solid-state electrolyte memristor of claim 1, wherein the Ga2O3The thickness of the conversion layer is 3-50 nm, and the thickness of the upper electrode layer is 50-200 nm.
6. A preparation method of a solid electrolyte memristor is characterized by comprising the following steps:
(a) cleaning the substrate as bottom electrode in acetone, alcohol and deionized water successively by ultrasonic wave, taking out, and using N2Drying;
(b) sputter deposition of Ga on a substrate2O3A translation layer;
(c) adding the solution C dropwise into the solution deposited with Ga2O3On the substrate of the conversion layer, the C solution automatically expands and covers the whole substrate surface, and then the substrate is annealed at the temperature of 80-120 ℃ for 10-50 min in the atmospheric environment, so that a C quantum dot layer is formed on the substrate, wherein the C quantum dots are formed on the substrateThe thickness of the layer is controlled to be 10-100 nm;
(d) and sputtering and depositing an upper electrode layer on the C quantum dot layer.
7. The preparation method of the solid electrolyte memristor according to claim 6, wherein the preparation process of the C solution is as follows: dissolving C in toluene according to the mass-to-volume ratio of 10-30 mg: 1-5 mL, uniformly mixing, and filtering by using a filter of 0.01-0.5 mu m to obtain a filtrate, namely the solution C.
8. The method of fabricating a solid-electrolyte memristor according to claim 6, wherein the bottom electrode is made of an electrochemically inert electrode material, and the top electrode layer is made of an electrochemically active electrode material.
9. The method of making a solid electrolyte memristor according to claim 6, wherein the Ga2O3The thickness of the conversion layer is 3-50 nm, and the thickness of the upper electrode layer is 50-200 nm.
10. An application of the solid electrolyte memristor in any one of claims 1 to 5 in manufacturing of a neuro-bionic device.
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Cited By (4)
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|---|---|---|---|---|
| CN111477740A (en) * | 2020-05-14 | 2020-07-31 | 天津理工大学 | Polymer/quantum dot film memristor capable of simulating nerve synapse and preparation method thereof |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN111477740A (en) * | 2020-05-14 | 2020-07-31 | 天津理工大学 | Polymer/quantum dot film memristor capable of simulating nerve synapse and preparation method thereof |
| CN111477740B (en) * | 2020-05-14 | 2023-09-26 | 天津理工大学 | Polymer/quantum dot film memristor capable of simulating nerve synapses and preparation method thereof |
| CN112951988A (en) * | 2021-01-29 | 2021-06-11 | 桂林医学院附属医院 | Tungsten oxide-based memristor embedded with Ti or Al nano island array and preparation method thereof |
| CN113013330A (en) * | 2021-02-26 | 2021-06-22 | 华中科技大学 | Based on ZnS SiO2Bidirectional self-current-limiting memristor and preparation method thereof |
| CN113206195A (en) * | 2021-04-30 | 2021-08-03 | 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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| CN111009608B (en) | 2023-09-22 |
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