CN112820826A - Based on MXene/MoSe2Nonvolatile memory device with/PMMA/MXene structure - Google Patents
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- 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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- 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
- H10N70/023—Formation of switching materials, e.g. deposition of layers by chemical vapor deposition, e.g. MOCVD, ALD
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- H—ELECTRICITY
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- H10N70/00—Solid-state devices having no potential barriers, and specially adapted for rectifying, amplifying, oscillating or switching
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- H10N70/882—Compounds of sulfur, selenium or tellurium, e.g. chalcogenides
- H10N70/8825—Selenides, e.g. GeSe
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Abstract
The invention discloses a film based on MXene/MoSe2The nonvolatile memory device with/PMMA/MXene structure comprises an MXene layer and MoSe layer on a substrate2Layer, PMMA layer and MXene layer. The nonvolatile memory device has good repeatability, low switching threshold and better application prospect; the nonvolatile memory device is based on organic PMMA and inorganic MoSe2The preparation method is simple, the cost is low, and the industrial production can be realized.
Description
Technical Field
The invention belongs to the field of memory devices, and particularly relates to a memory device based on MXene/MoSe2The nonvolatile memory device has a structure of/PMMA/MXene.
Background
With the continuous update and iteration of integrated circuits, and under the influence of moore's law, the original memory device cannot meet the embedded application system developed at a high speed. In order to break through the current dilemma and overcome the defects of the memories on the market, the research on new materials and new structures is the key point of future development. Among emerging memories, a resistance switching memory has attracted attention because of its advantages such as a simple structure, a high memory speed, and a low cost. Compared with a FLASH memory, the resistance switch memory has higher speed and is not easy to lose compared with a DRAM, and a novel storage system is provided for embedded equipment.
Most of the switch storage materials of a typical resistance switch memory are metal oxides, and a metal electrode is respectively arranged on the upper part and the lower part of the switch storage material. Due to the characteristics of ultrathin, flexible and multilayer structure of the two-dimensional material, the two-dimensional material is very suitable for being used in embedded equipment, and the unique electrochemical, physical and mechanical properties of the two-dimensional material provide a new idea for constructing a nonvolatile memory, such as MoS2WS and MoSe2As memory materials for non-volatile memories, and these materials are mainly based on the penetration of metal particles and the migration of intrinsic substances after being fabricated into devices, devices based on two-dimensional materials generally exhibit higher switching speeds, lower threshold voltages, and superior mechanical properties. Meanwhile, if the resistance conversion performance of the two-dimensional material can be further improved by compounding the organic polymer and the electrodeless semiconductor, better storage performance is achieved, and the method has important industrial value.
Disclosure of Invention
Based on the defects of the prior art, the invention provides a film based on MXene/MoSe2The nonvolatile memory device with the structure of/PMMA/MXene is expected to obtain better memory performance on the basis of industrialization.
In order to realize the purpose of the invention, the following technical scheme is adopted:
based on MXene/MoSe2The nonvolatile memory device with the structure of/PMMA/MXene is characterized in that: the nonvolatile memory device is formed by arranging MXene layer and MoSe layer by layer on a substrate2Layer, PMMA layer and an MXene layer. In the nonvolatile memory device of the present invention:
MXene layer: MXene, as one of two-dimensional materials, has excellent conductivity, excellent flexibility which is not possessed by a traditional metal electrode, and is an excellent choice in the preparation of flexible devices or rigid devices. MXene can be used as an electrode and can provide abundant charges for the intermediate storage layer.
MoSe2PMMA layer: MoSe2The MoSe has excellent performance in certain electronic devices and mature and controllable process, and is an excellent choice as an electron transport layer, but does not show any switching behavior when being used as a storage layer of a memory device per se, so that the MoSe has the advantages of high performance, high stability and low cost2Further functionalization with other materials is essential to achieving switching behavior. Compared with the non-volatile memory manufactured by other structures, the switching current of which can only reach one order of magnitude, the MXene/MoSe-based nonvolatile memory manufactured by the invention2MoSe is selected for the nonvolatile memory device with the structure of/PMMA/MXene2The memory material is made of PMMA, the switching current reaches three orders of magnitude, and the larger switching current ratio not only enlarges the reading margin, but also has better noise resistance. In the structure of the invention, the organic matter in the storage layer is more beneficial to the capture and release of charges, the on-off current ratio is increased, and the organic matter is an advantage that the inorganic matter does not have.
Further, the substrate of the nonvolatile memory device can be a flexible substrate or a rigid substrate, so that the nonvolatile memory device is suitable for different application requirements.
Further, the thickness of the MXene layer is 20-50nm, and the MoSe layer2The thickness of the layer is 4-10nm, and the thickness of the PMMA layer is 50-100 nm. The thickness of each layer has a great influence on the performance of the memory device, and the good memory performance can be obtained within the thickness range screened by the invention.
The preparation method of the nonvolatile memory device comprises the following steps:
firstly, MoSe is grown on a silicon wafer with a silicon oxide layer by a CVD method2A thin film of a material selected from the group consisting of,then in the MoSe2Spin coating PMMA solution on the film and drying to form MoSe on the silicon wafer2a/PMMA composite layer, and then etching with HF to make MoSe2Stripping the/PMMA composite layer from the silicon wafer;
spin coating MXene solution on a substrate and drying to form an MXene layer; then adding MoSe2the/PMMA composite layer is transferred to the MXene layer; coating MXene solution on the PMMA layer in a spinning mode and drying to form another MXene layer;
finally, annealing the device to finish the MXene/MoSe-based device2And preparing a nonvolatile memory device with a/PMMA/MXene structure.
Further, the annealing is annealing at 200 ℃ for 2 hours under argon.
Further, MoSe2The preparation method of the film comprises the following steps: and cleaning the silicon wafer with the silicon oxide layer by using acetone, ethanol and deionized water in sequence, and treating the silicon wafer with ozone for 30 minutes. 0.01g of MoO was taken3The powder was placed in a quartz boat and the wafer was then inverted over the boat. The quartz boat was placed in the heating zone of a tube furnace and 0.5g of selenium powder was placed in front of the heating zone. Introducing argon into the tubular furnace for three times of cleaning to ensure that no oxygen is doped in the reaction process, then keeping the flow of the argon at 95sccm, and heating to 820 ℃ at the heating rate of 15 ℃/min; argon-hydrogen mixed gas with the flow rate of 95sccm (the volume percentage of hydrogen gas is 5 percent), and growing for 15min under heat preservation; after the heat preservation is finished, the cover is opened for rapid cooling, and argon gas of 95sccm is continuously introduced in the cooling process; taking out to obtain MoSe2A film.
Compared with the prior art, the invention has the beneficial effects that:
the nonvolatile memory device has good repeatability, low switching threshold and better application prospect; the nonvolatile memory device is based on organic PMMA and inorganic MoSe2The layer is realized by cooperation, the preparation method is simple, the cost is low, and the industrial production can be realized.
Drawings
FIG. 1 is a schematic diagram of a non-volatile memory device according to the present invention;
FIG. 2 shows the present inventionExample 1 MoSe grown at various temperatures2SEM image of the film, wherein (a) - (c) correspond to growth temperature 750 deg.C, 800 deg.C, 820 deg.C;
fig. 3 is a raman spectrum of the nonvolatile memory device fabricated in example 1 of the present invention;
fig. 4 is a graph of a current-voltage characteristic of a nonvolatile memory device prepared in example 1 of the present invention;
FIG. 5 shows MXene/MoSe as a comparison in accordance with the present invention2Volt-ampere characteristic curve of/MXene device.
Detailed Description
In order to make the aforementioned objects, features and advantages of the present invention comprehensible, embodiments accompanied with figures are described in detail below. The following disclosure is merely exemplary and illustrative of the inventive concept, and those skilled in the art will appreciate that various modifications, additions and substitutions are possible, without departing from the scope and spirit of the invention as disclosed in the accompanying claims.
Example 1
As shown in FIG. 1, this embodiment is based on MXene/MoSe2The non-volatile memory device with/PMMA/MXene structure is formed by arranging MXene layer and MoSe layer on a substrate layer by layer2Layer, PMMA layer and MXene layer. Specifically, in this embodiment, the substrate is made of FTO glass. Wherein the thickness of the two Mxene layers is about 20nm and MoSe2The layer thickness was about 5nm and the PMMA layer thickness was about 100 nm.
The method for manufacturing the nonvolatile memory device of the embodiment is as follows:
step 1, a silicon wafer (23 mm. times.25 mm) having a silicon oxide layer was washed with acetone, ethanol, and deionized water in this order, and then treated with ozone for 30 minutes. 0.01g of MoO was taken3The powder was placed in a quartz boat and the wafer was then inverted over the boat. The quartz boat was placed in the heating zone of a tube furnace and 0.5g of selenium powder was placed in front of the heating zone. Introducing argon into the tubular furnace for three times of cleaning to ensure that no oxygen is doped in the reaction process, and then keeping the flow of the argon at 95sccmAnd heating to 820 ℃ at a heating rate of 15 ℃/min; argon-hydrogen mixed gas with the flow rate of 95sccm (the volume percentage of hydrogen gas is 5 percent), and growing for 15min under heat preservation; after the heat preservation is finished, the cover is opened for rapid cooling, and argon gas of 95sccm is continuously introduced in the cooling process; taking out to obtain MoSe2A film.
In order to compare the influence of the growth temperature on the morphology of the film, the film was also prepared at 750 ℃ and 800 ℃ in this example. FIG. 2 shows the MoSe grown at various temperatures2In the SEM images of the thin films, MoSe was observed in the order of (a) to (c) at growth temperatures of 750 ℃, 800 ℃ and 820 DEG2From discrete single sheet to densification, the obtained thin film is dense and faultless at 820 ℃.
Step 2, MoSe grown in the step 12Placing the film on a spin coater, dripping 100 μ L PMMA solution on the sample, spin-coating at 600rpm for 6s, then spin-coating at 3200rpm for 25s, and baking at 80 deg.C for 1 hr to form MoSe on the silicon wafer2a/PMMA composite layer. Placing the mixture in HF solution for etching for 24 hours to ensure that MoSe is obtained2the/PMMA composite layer was peeled from the silicon wafer and transferred to deionized water for use.
Step 3, placing the cleaned FTO glass on a spin coater, dripping 1000 mu L of Mxene solution on the surface of the FTO glass, spin-coating at 3800rpm for 2min, and then placing on a hot table at 80 ℃ for baking for 10 min to form an MXene layer; then adding MoSe2the/PMMA composite layer is transferred to the MXene layer; finally, spin-coating MXene solution on the PMMA layer according to the same conditions and drying to form another MXene layer;
step 4, annealing the device for 2 hours at 200 ℃ under argon to finish the annealing process based on MXene/MoSe2And preparing a nonvolatile memory device with a/PMMA/MXene structure.
Fig. 3 is a raman spectrum of the nonvolatile memory device prepared in this example, and the successful preparation of the device is further confirmed by comparing and analyzing the respective peaks.
Fig. 4 is a graph showing current-voltage characteristics of the nonvolatile memory device prepared in this example, from which the existence of reversible nonvolatile bistability can be seen and which shows a significant asymmetry. For theIn the positive scanning of the device from 0V to 1V, the current is from 10-5A increases to 10-2And A, the switching threshold voltage is 0.9V. This type of switching process represents a transition from a low conductivity state to a high conductivity state, which can be considered as a process in which the memory is performing a "write". Without the application of a negative bias, the device remains in state 2, and if the applied bias is turned off, the device itself can remain in state 2, clearly indicating the presence of non-volatility of the device. And when the scan bias voltage is below-0.8V, the device reverts to state 1 as seen in the current-voltage plot, at which point the state transition from high to low conductivity can be considered a memory operation that is performing an "erase".
This example also prepared MXene/MoSe2Compared with the device with the MXene structure, namely, compared with the memory device, the PMMA layer is reduced, and the preparation method of the memory device is different from the memory device in that: adding MoSe2After the/PMMA composite layer is transferred to the MXene layer, the MXene layer is firstly placed under argon and annealed at 350 ℃ for 3 hours to remove the PMMA layer, and then the MXene solution on the PMMA layer is coated in a spinning mode. FIG. 5 shows MXene/MoSe2Volt-ampere characteristic graph of/MXene device, it can be seen that the device does not show any nonvolatile memory performance in the scanning from-1V to 1V, so that PMMA organic layer can be considered to be in MoSe2The above trapping and releasing of charge is the main reason for the non-volatile storage performance of the device.
The present invention is not limited to the above exemplary embodiments, and any modifications, equivalent replacements, and improvements made within the spirit and principle of the present invention should be included in the protection scope of the present invention.
Claims (5)
1. Based on MXene/MoSe2The nonvolatile memory device with the structure of/PMMA/MXene is characterized in that: the nonvolatile memory device is formed by arranging MXene layer and MoSe layer by layer on a substrate2Layer, PMMA layer and MXene layer.
2. The non-volatile storage device of claim 1, wherein: the substrate is a flexible substrate or a rigid substrate.
3. The non-volatile storage device of claim 1, wherein: the thickness of the MXene layer is 20-50nm, and the MoSe layer2The thickness of the layer is 4-10nm, and the thickness of the PMMA layer is 50-100 nm.
4. A method of manufacturing a non-volatile memory device according to any one of claims 1 to 3, characterized by:
firstly, MoSe is grown on a silicon wafer with a silicon oxide layer by a CVD method2Thin film on said MoSe2Spin coating PMMA solution on the film and drying to form MoSe on the silicon wafer2a/PMMA composite layer, and then etching with HF to make MoSe2Stripping the/PMMA composite layer from the silicon wafer;
spin coating MXene solution on a substrate and drying to form an MXene layer; then adding MoSe2the/PMMA composite layer is transferred to the MXene layer; coating MXene solution on the PMMA layer in a spinning mode and drying to form another MXene layer;
finally, annealing the device to finish the MXene/MoSe-based device2And preparing a nonvolatile memory device with a/PMMA/MXene structure.
5. The method of claim 4, wherein: the annealing is carried out under argon at 200 ℃ for 2 hours.
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| YINGCHAO YANG等: ""Brittle Fracture of 2D MoSe2"", 《ADVANCED MATERILAS》 * |
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