CN108950507B - Memristive switching device based on a-TSC-O ceramic film and preparation method thereof - Google Patents
Memristive switching device based on a-TSC-O ceramic film and preparation method thereof Download PDFInfo
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- C23C14/00—Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material
- C23C14/22—Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material characterised by the process of coating
- C23C14/34—Sputtering
- C23C14/35—Sputtering by application of a magnetic field, e.g. magnetron sputtering
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- C23C14/00—Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material
- C23C14/0021—Reactive sputtering or evaporation
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- C23C14/00—Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material
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Abstract
A memristor switch device based on an a-TSC-O ceramic film and a preparation method thereof belong to the technical field of photoelectric devices. The invention innovatively provides 'a-TSC: O film/a-TiO' on the basis of the structure of the traditional memristive switching devicexThe dielectric layer structure of the film widens the selection range of the dielectric layer material of the memristor switch device. The resistance change performance of the a-TSC and O film can be adjusted in a large range, and the a-TiOxThe film is transparent and can provide an oxygen vacancy electromigration channel, so that the a-TSC and O film has good resistance change performance and can be used as a dielectric layer of a memristive switching device. Meanwhile, the intrinsic a-TSC ceramic film has very good conductivity and near-infrared transmittance, so that the intrinsic a-TSC ceramic film can be used as a top electrode material to construct a near-infrared fully-transparent memristor switching device together with a top electrode formed by a transparent conductive film. In addition, the preparation process of the memristor switch device is simple, low in cost and high in reliability, and large-scale production is facilitated.
Description
Technical Field
The invention belongs to the technical field of photoelectric devices, and particularly relates to a memristor switching device based on an a-TSC-O ceramic film and a preparation method thereof.
Background
Memristors have received considerable attention from researchers as a new class of nonlinear devices. To date, materials such as Ag, Cu, Au, Pt, and W have been used as electrode materials thereof; a-Si, a-SiOxAnd TiO2The medium films are common resistance change layer materials of the memristor switch device. In recent years, researchers at home and abroad have constructed and prepared various memristive switching devices with color-forming and resistance-changing functions based on various electrodes and resistance-changing layer materials, so that the devices becomePet of a generation of storage technology.
Ti3SiC2Is a ternary layered carbide, is a unique MAX phase material containing Si element, has the properties of ceramic and metal, and can be called TSC ceramic material for short. Ti3SiC2The compound structurally belongs to a ceramic material, and embodies the characteristics of high melting point, high yield strength, good oxidation resistance, corrosion resistance and thermal shock resistance of the ceramic material. At the same time, Ti3SiC2The compound is similar to a metal material in electrical, thermal and mechanical properties, and has high thermal conductivity and electrical conductivity, high shear modulus and elastic modulus, low hardness, good machining performance and certain plasticity at high temperature. In addition, since Ti3SiC2The special layered structure makes the material have good self-lubricating property and damage tolerance.
Based on the prior art to Ti3SiC2And because of Ti3SiC2Has the excellent properties of metal and ceramic, and has attractive application prospect in the fields of automobiles, chemical engineering, national defense industry and the like due to good processibility. Ti3SiC2The electric conductivity of the composite material is about two orders of magnitude higher than that of graphite, and the composite material has ultralow friction performance, lower friction factor than that of graphite and good self-lubricating performance, so that the composite material is expected to replace graphite to manufacture the electric brush of a new generation of alternating current motor. Ti3SiC2Has good corrosion resistance, oxidation resistance, ultralow friction and self-lubricating property, and can be used as an electrode material for metal smelting. Ti3SiC2The high-temperature strength, oxidation resistance and thermal shock resistance of the alloy are superior to those of Si3N4The material can be used as an ideal material for turbine blades and stators of aircraft engines. Ti3SiC2The density of (A) is about the same as that of the current Ni-based high-temperature alloy, but the strength is 2 times of that of the current Ni-based high-temperature alloy, and the high-temperature alloy still has very good mechanical properties at the high temperature of 1400 ℃ and is easier to machine, so that the high-temperature alloy can possibly replace the best high-temperature alloy in the current market. Ti3SiC2Good processability and self-lubricating properties of the composition,making it possible to replace the traditional machinable ceramics. Ti3SiC2It is easy to siliconize and carbonize, the siliconization can make the surface hardness reach 12GPa, the carbonize can reach 25GPa, the surface treatment can improve the performance of the material, and the operation is easy and the processing cost is low. As is clear from the above, Ti has hitherto been used3SiC2The development and research of the application mainly focus on high-temperature structural materials, electrode materials, machinable ceramic materials, antifriction component materials and corrosion-resistant protective layers, and no research report on the application of the antifriction component materials in the photoelectric field is found.
Disclosure of Invention
The invention aims to provide a memristor switching device based on a TSC ceramic film and a preparation method thereof. The invention innovatively discovers that the oxidized amorphous TSC ceramic film (a-TSC: O) has good resistance change performance, further discovers that the amorphous TSC ceramic film (a-TSC) has the near-infrared all-transparent characteristic, and constructs the memristor switch device with the near-infrared transparent characteristic on the basis.
In order to achieve the purpose, the technical scheme of the invention is as follows:
the invention provides a memristor switch device based on an a-TSC O ceramic film, which is of a vertical four-layer structure of a bottom electrode, a first resistive layer, a second resistive layer and a top electrode from bottom to top, and is characterized in that: the material of the first resistance-change layer is amorphous titanium oxide, the material of the second resistance-change layer is oxidized amorphous TSC, and the material of the bottom electrode is an ITO film.
Further, the material of the top electrode in the invention is selected from amorphous TSC, metal tungsten (W) or metal gold (Au), and in order to make the whole memristive switching device in the invention have near-infrared transparency, the material of the top electrode is preferably amorphous TSC.
On the basis of the scheme, the range of the near-infrared band is 800 nm-1200 nm.
Furthermore, the thickness of the top electrode is 50 nm-200 nm.
Furthermore, the thickness of the bottom electrode is 100 nm-200 nm.
Furthermore, the first resistance change layer is a film prepared by adopting reactive sputtering based on a PVD system, and the thickness of the first resistance change layer is 30 nm-150 nm.
Furthermore, the second resistance-change layer is a film prepared by adopting reactive sputtering based on a PVD system, and the thickness of the second resistance-change layer is 50 nm-300 nm.
The invention provides a preparation method of a memristor switch device based on an a-TSC-O ceramic film, which is characterized by comprising the following steps of:
step A: preparing a clean and dry ITO glass slide;
and B: depositing an amorphous titanium oxide film on the upper surface of the ITO glass slide to serve as a first resistance change layer;
and C: depositing an oxidized amorphous TSC ceramic film on the upper surface of the first resistance-change layer by using a direct-current reactive sputtering or radio-frequency reactive sputtering method to serve as a second resistance-change layer;
step D: and depositing a top electrode on the upper surface of the second resistance change layer.
Further, the thickness of the ITO film in the ITO glass slide in the step A is 100 nm-200 nm.
Further, in the step B of the invention, the amorphous titanium oxide film can be prepared by adopting direct current reactive sputtering or radio frequency reactive sputtering, and the amorphous titanium oxide film can also be prepared by adopting any suitable film forming mode; the thickness of the amorphous titanium oxide film is 30 nm-150 nm.
Further, the parameters of the dc sputtering film forming process in step C of the present invention are as follows: the working current range is 0.20-0.35A, the working voltage range is 360-475V, the argon pressure is 1.5-5 Pa, and the argon flow is 25-50 sccm; the parameters of the radio frequency sputtering film forming process are as follows: the power of the radio frequency source is 40W-200W, the pressure of argon is 0.5 Pa-2.5 Pa, the flow of argon is 20 sccm-40 sccm, and the heating temperature of the substrate is 25 ℃ to 200 ℃.
Further, the material of the top electrode in step D of the present invention is selected from amorphous TSC, metal tungsten (W) or metal gold (Au).
Furthermore, in the step D of the invention, the top electrode can be prepared by direct current sputtering or magnetron sputtering, and can also be prepared by any suitable film forming mode; the thickness of the top electrode is 50 nm-200 nm.
The memristive switching device is built on an oxidized amorphous TSC (a-TSC: O) ceramic material, has good resistance change performance, namely the resistance performance of an a-TSC: O film can be continuously adjusted by controlling the oxidation degree of the a-TSC: O, and amorphous titanium oxide (a-TiO) is adoptedx) The material, the a-TSC and the O material are jointly used as a double-resistance-change layer of a memristive switching device, and the a-TiOxAn oxygen vacancy transfer channel can be provided. The specific working principle is as follows: when a forward voltage is applied between the top and bottom electrodes of the device (electrical modulation), oxygen ions in the O film, which is the second resistance change layer, migrate under the action of an electric field and even migrate to TiO, which is the first resistance change layerxIn the thin film, the distribution of oxygen ions in the memristor resistance change layer is recombined; the ITO slide can also provide oxygen ions to promote migration to TiO when a reverse voltage is applied between the top and bottom electrodes of the device (electrical modulation)xOxygen ions in the film return to the a-TSC-O film under the action of an electric field, so that the distribution of the oxygen ions in the resistance change layer of the memristor can be recombined again, and nonlinear continuous change of the resistance is realized. Based on the principle, the invention constructs and obtains the ITO glass sheet and the alpha-TiOxO' double resistance change layer and top electrode, and further using the a-TSC ceramic film as the top electrode and the ITO glass as the conductive transparent substrate, the memristive switching device with the whole near-infrared full-transparent characteristic can be constructed.
Compared with the prior art, the invention has the beneficial effects that:
the invention innovatively provides a dielectric layer structure (namely a resistance change layer) based on an a-TSC ceramic material on the basis of the traditional memristive switching device structure, and widens the selection range of the material of the dielectric layer of the memristive switching device. The resistance change performance of the a-TSC and O film can be adjusted in a large range, and the a-TiOxThe film is transparent and can provide an oxygen vacancy (namely an oxygen hole) electromigration channel, so that the a-TSC/O film has good resistance change performance and can be used as a dielectric layer of a memristive switching device. Furthermore, the a-TSC ceramic film has very good conductivity and near infrared transmittanceThe near-infrared all-transparent memristor can be used as a top electrode material to jointly construct a near-infrared all-transparent memristor switching device with a top electrode formed by a transparent conductive film. In addition, the preparation process of the memristor switch device is simple, low in cost and high in reliability, and large-scale production is facilitated.
Drawings
Fig. 1 is a schematic structural diagram of a memristive switching device according to specific embodiment 1 of the present invention, where 1 is an ITO glass slide, and 2 is a-TiOxThe film 3 is a-TSC-O film, and the film 4 is a-TSC film.
Fig. 2 is a transmittance-wavelength diagram of an a-TSC ceramic thin film in a memristive switch provided in embodiment 1 of the present invention.
Detailed Description
In order to make the objects, technical solutions and advantages of the present invention more apparent, the present invention will be described in detail below with reference to the following embodiments, and with reference to the accompanying drawings:
example 1:
this embodiment provides a memristive switching device, as shown in fig. 1, whose structure is, from bottom to top, "ITO slide 1, a-TiOx Film 2, a-TSC, O film 3, a-TSC film 4 'vertical four-layer structure' a-TiOxThe double-layer structure of the film 2/a-TSC and the O film 3 serves as a double-resistance layer (namely a dielectric layer of a memristive switching device).
The embodiment provides a preparation method of the memristor switch device, and the preparation process comprises the following steps:
step A: preparing an ITO glass slide 1 as a transparent substrate with a bottom electrode, and cleaning and drying the ITO glass slide according to a standard process;
and B: depositing an a-TiOx film 2 on an ITO glass substrate 1 as a first resistance-change layer by using a titanium target as a raw material target material and oxygen and argon as working gases through reactive radio frequency sputtering;
and C: by using Ti3SiC2Using polycrystalline powder as a raw material target material, using oxygen and argon as working gases, and depositing a-TSC on the a-TiOx film 2 by reactive radio frequency sputtering, wherein the O film 3 is used as a second resistance change layer; the present embodiment is based on a PVD system, and specifically operates as follows:
c1: preparing a target material:
mixing Ti3SiC2Adding the powder into deionized water, and uniformly stirring to obtain Ti3SiC2Dispersing the Ti in a solvent, and then adding Ti3SiC2Putting the dispersion liquid into an aluminum tray with the diameter of 90mm and the thickness of 3-4 mm, then putting the aluminum tray into a vacuum drying oven at 120 ℃ for drying for 24 hours, taking out the aluminum tray, and preparing a direct-current sputtering target material based on the operation, wherein the target material is required to be vacuumized and sealed when not used;
c2: sample loading:
opening a cavity of the PVD system, and putting the target and the substrate into vacuum sputtering coating equipment;
c3: vacuumizing and sputtering:
closing the chamber of the PVD system, and automatically vacuumizing to 5.5 multiplied by 10-4Pa, closing the pumping speed valve, setting the argon gas flow rate to be 25sccm, setting the current to be 0.3A, starting the target, sputtering after pre-sputtering, and controlling the thickness of the a-TSC film by adjusting the sputtering time, wherein the sputtering time is 7 minutes in the embodiment;
step D: by using Ti3SiC2The method comprises the following steps of using polycrystalline powder as a raw material target material, using argon gas as working gas, depositing an intrinsic a-TSC thin film 4 on an a-TSC: O thin film 3 as a top electrode through radio frequency sputtering, and specifically operating as follows:
d1: preparing a target material:
selecting Ti prepared in the step C13SiC2Opening a cavity of the PVD system, and putting the target and the substrate into vacuum sputtering coating equipment;
d2: sample loading:
opening a cavity of the PVD system, and putting the target and the substrate into vacuum sputtering coating equipment;
d3: vacuumizing and sputtering:
closing the PVD chamber, and automatically vacuumizing to 5.5 × 10-4Pa, closing the pumping speed valve, setting the argon gas flow rate to be 20sccm, setting the current to be 0.3A, starting the target, sputtering after pre-sputtering, and controlling the thickness of the a-TSC film by adjusting the sputtering time, wherein the sputtering time is 3 minutes in the embodiment;
when the a-TSC film is prepared, a quartz substrate and a K9 glass substrate are selected to prepare the a-TSC film under the same process conditions, the transmittance of the a-TSC film prepared on the basis of the quartz substrate and the K9 glass substrate is tested, and the test result is shown in figure 2. As can be seen from FIG. 2, the Ti of the present invention3SiC2The transmittance of the ceramic film in the spectral range of 800-2200 nm is not less than 80%, and the ceramic film has the characteristic of full transparency in a near-infrared band.
The basic working principle of the memristor switching device is as follows: when a forward voltage is applied between the top and bottom electrodes of the device (electrical modulation), oxygen ions in the O film 3 of the a-TSC as the second resistive layer migrate under the action of the electric field and even move to the TiO as the first resistive layerxIn the thin film 2, the distribution of oxygen ions in the memristor resistance changing layer is recombined; the ITO glass slide 1 can also be supplied with oxygen ions to promote migration to TiO when a reverse voltage is applied between the top and bottom electrodes of the device (electrical modulation)xOxygen ions in the film 2 return to the a-TSC-O film 3 under the action of an electric field, so that the distribution of the oxygen ions in the resistance change layer of the memristor can be recombined again, and nonlinear continuous change of the resistance is realized.
Example 2:
the embodiment provides a preparation method of a memristor switching device, and the preparation process comprises the following steps:
step A: preparing a K9 glass substrate as a transparent substrate, and cleaning and drying the transparent substrate according to a standard process; then depositing an ITO film on the substrate as a bottom electrode;
and B: depositing an a-TiOx film on the ITO film by reactive radio frequency sputtering to serve as a first resistance change layer by adopting a titanium target as a raw material target material and oxygen and argon as working gases;
and C: by using Ti3SiC2The polycrystalline powder is used as a raw material target material, oxygen and argon are used as working gases, a-TSC is deposited on the a-TiOx film through reactive radio frequency sputtering, and the O film is used as a second resistance change layer, and the method specifically comprises the following steps:
c1: preparing a target material:
mixing Ti3SiC2Adding the powder into deionized water, and uniformly stirring to obtain Ti3SiC2Dispersing the Ti in a solvent, and then adding Ti3SiC2Putting the dispersion liquid into an aluminum tray with the diameter of 90mm and the thickness of 3-4 mm, then putting the aluminum tray into a vacuum drying oven at 120 ℃ for drying for 24 hours, taking out the aluminum tray, and preparing a direct-current sputtering target material based on the operation, wherein the target material is required to be vacuumized and sealed when not used;
c2: sample loading:
opening the cavity, and putting the target and the substrate into vacuum sputtering coating equipment;
c3: vacuumizing and sputtering:
the cavity is closed, and the automatic vacuum pumping reaches 5.5 multiplied by 10-4Pa, closing the pumping speed valve, setting the argon gas flow rate to be 30sccm, setting the current to be 0.5A, starting the target, sputtering after pre-sputtering, and controlling the thickness of the a-TSC film by adjusting the sputtering time, wherein the sputtering time is 7 minutes in the embodiment;
step D: an Au target is used as a raw material target material, argon is used as a working gas, a metal Au film is deposited on the a-TSC: O film through radio frequency sputtering to be used as a top electrode, and the specific operation is as follows:
the difference between this embodiment and embodiment 1 is that the transparency of the device in the near infrared light is reduced as a whole because the top electrode and the bottom electrode have low transmittance for the near infrared light, while embodiment 1 uses the a-TSC ceramic film as the top electrode and the ITO glass sheet as the conductive transparent substrate to make the device have the specific transparency in the near infrared light. Therefore, when the memristive switching device is used in a near-infrared band field, appropriate top electrode and bottom electrode materials should be selected according to actual needs.
While the present invention has been described in detail and with reference to the drawings, the foregoing embodiments are illustrative rather than restrictive, and the present invention is not limited to the foregoing embodiments. Many variations of the invention can be made by one of ordinary skill in the art in light of the teachings herein without departing from the spirit and scope of the invention as defined by the appended claims.
Claims (10)
1. A memristive switching device based on an a-TSC O ceramic film is of a vertical four-layer structure of 'bottom electrode/first resistance change layer/second resistance change layer/top electrode' from bottom to top, and is characterized in that: the first resistance-change layer is an amorphous titanium oxide film, the second resistance-change layer is an oxidized amorphous TSC film, and the bottom electrode is an ITO film.
2. The memristive switching device based on the a-TSC O ceramic thin film is characterized in that the first resistance change layer is a thin film prepared by reactive sputtering based on a PVD system, and the thickness of the thin film is 30 nm-150 nm.
3. The memristive switching device based on the a-TSC O ceramic thin film is characterized in that the second resistance change layer is a thin film prepared by reactive sputtering based on a PVD system, and the thickness of the thin film is 50 nm-300 nm.
4. The a-TSC O ceramic thin film-based memristive switching device according to claim 1, wherein the material of the top electrode is selected from intrinsic amorphous TSC, metal tungsten or metal gold.
5. The memristive switching device based on the a-TSC: O ceramic thin film is characterized in that the thickness of the top electrode is 50 nm-200 nm.
6. The memristive switching device based on the a-TSC: O ceramic thin film according to claim 1, wherein the thickness of the bottom electrode is 100 nm-200 nm.
7. A preparation method of a memristor switching device based on a-TSC O ceramic film is characterized by comprising the following steps:
step A: preparing a clean and dry ITO glass slide;
and B: depositing an amorphous titanium oxide film on the upper surface of the ITO glass slide to serve as a first resistance change layer;
and C: depositing an oxidized amorphous TSC ceramic film on the upper surface of the first resistance-change layer by using a direct-current reactive sputtering or radio-frequency reactive sputtering method to serve as a second resistance-change layer;
step D: and depositing a top electrode on the upper surface of the second resistance change layer.
8. The method for preparing the memristive switching device based on the a-TSC O ceramic film is characterized in that in the step B, the amorphous titanium oxide film is prepared by adopting direct-current reactive sputtering or radio-frequency reactive sputtering; the thickness of the amorphous titanium oxide film is 30 nm-150 nm.
9. The method for preparing the memristive switching device based on the a-TSC O ceramic thin film according to claim 7, wherein the parameters of the direct current sputtering film forming process in the step C are as follows: the working current range is 0.20-0.35A, the working voltage range is 360-475V, the argon pressure is 1.5-5 Pa, and the argon flow is 25-50 sccm; the parameters of the radio frequency sputtering film forming process are as follows: the power of the radio frequency source is 40W-200W, the pressure of argon is 0.5 Pa-2.5 Pa, the flow of argon is 20 sccm-40 sccm, and the heating temperature of the substrate is 25 ℃ to 200 ℃.
10. The method for preparing a memristive switching device based on an a-TSC: O ceramic thin film as claimed in claim 7, wherein the material of the top electrode in the step D is selected from intrinsic amorphous TSC, metal tungsten or metal gold, and the thickness of the top electrode is 50nm to 200 nm.
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