CN109461812B - Aluminum oxide-based RRAM and preparation method thereof - Google Patents
Aluminum oxide-based RRAM and preparation method thereof Download PDFInfo
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- CN109461812B CN109461812B CN201811128573.7A CN201811128573A CN109461812B CN 109461812 B CN109461812 B CN 109461812B CN 201811128573 A CN201811128573 A CN 201811128573A CN 109461812 B CN109461812 B CN 109461812B
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Abstract
An RRAM based on aluminum oxide in the technical field of electronic devices and a preparation method thereof, comprising a substrate, a resistive oxide layer and an upper electrode layer which are stacked from bottom to top; the substrate comprises an insulating layer and a lower electrode layer; the resistive oxide layer is Al 2 O 3 A thin film layer; the upper electrode layer comprises a plurality of upper electrodes arrayed on the resistive oxide layer, and a metal protective layer is arranged on the surface of each upper electrode far away from the resistive oxide layer. The resistive oxide layer is manufactured by adopting a solution method process, the preparation of the RRAM with low cost is realized, the investment on equipment and raw materials is less, and the large-scale industrial application can be realized.
Description
Technical Field
The invention relates to a technology in the field of electronic devices, in particular to an RRAM (Resistive random access memory) based on aluminum oxide and a preparation method thereof.
Background
With the rapid development of digital technology and the wide popularization of portable digital multimedia products, the requirements for mobile storage devices are higher and higher, for example: the memory has the characteristics of high speed, high density, low cost, low power consumption, long service life and the like, and meanwhile, due to the structure of the memory, different memories have more or less advantages, and irreparable technical defects are also exposed. Volatility has received extensive attention and research as one of the weaknesses of dynamic and static memory, where stored information is lost in the event of a power failure and is highly susceptible to electromagnetic interference. The flash memory has technical obstacles such as low recording density and slow reading speed. Therefore, the memory is developed in a direction of faster reading speed and larger storage capacity, and is also developed in a direction of diversification. The research on the non-volatile memory is promising. RRAM is a major candidate for non-volatile memory due to its simple structure and inclusion of CMOS logic compatible process technology. The RRAM is a memory which changes a material between a high-resistance state (HRS) and a low-resistance state (LRS) according to a voltage applied to a Metal Oxide layer (Metal Oxide) to erase/write data, open or block a current flow channel, and can significantly improve durability and data transmission speed by using the property to store information.
The existing RRAM research mainly focuses on the property aspect of the resistive oxide layer, and the traditional resistive oxide layer film can be realized by methods such as sputtering, Chemical Vapor Deposition (CVD), Atomic Layer Deposition (ALD) and the like, but the methods are limited by equipment and high in production cost, and cannot meet the industrial requirement of low cost.
Disclosure of Invention
Aiming at the defects in the prior art, the invention provides an RRAM based on aluminum oxide and a preparation method thereof, which can meet the low-cost industrialization requirement of the RRAM.
The invention is realized by the following technical scheme:
the invention relates to an RRAM (resistive random access memory) based on aluminum oxide, which comprises a substrate, a resistive oxide layer and an upper electrode layer which are stacked from bottom to top;
the substrate comprises an insulating layer and a lower electrode layer;
the resistive oxide layer is Al 2 O 3 A thin film layer;
the upper electrode layer comprises a plurality of upper electrodes arrayed on the resistive oxide layer, and a metal protective layer is arranged on the surface of each upper electrode far away from the resistive oxide layer.
The metal protective layer is a metal aluminum film layer or a metal tungsten film layer.
The upper electrode is a metal nickel film or a metal titanium film, and the thickness of the upper electrode is 50-100 nm.
The lower electrode layer is a metal platinum film layer or a silicon film layer, and the thickness of the lower electrode layer is 50-150 nm.
Preferably, the insulating layer adopts a three-layer structure which is stacked, and comprises a silicon thin film layer, a silicon dioxide thin film layer and a titanium thin film layer which are arranged from bottom to top.
The invention relates to a preparation process method of the RRAM, which comprises the following steps:
a) cleaning a substrate;
completely immersing the substrate into a beaker containing deionized water, and placing the beaker in a deionized water environment for first ultrasonic cleaning; after the first ultrasonic cleaning, completely immersing the substrate into a beaker containing an acetone solvent, and placing the beaker in a deionized water environment for second ultrasonic cleaning; after the second ultrasonic cleaning, repeatedly washing the substrate with deionized water to clean the acetone solvent and impurities remained on the substrate, completely immersing the substrate into a beaker containing absolute ethyl alcohol, and placing the beaker in a deionized water environment to perform third ultrasonic cleaning; after the third ultrasonic cleaning, washing the substrate with deionized water to remove residual impurities, completely immersing the substrate into a beaker containing the deionized water, and placing the beaker in a deionized water environment to carry out fourth ultrasonic cleaning; after the fourth ultrasonic cleaning, washing the substrate by deionized water and drying by nitrogen;
b) preparing a resistance change oxide layer;
Preparing 1.5-3 mol/L aluminum nitrate solution from aluminum nitrate nonahydrate by using deionized water; dropwise adding the prepared aluminum nitrate solution on the lower electrode layer, and performing spin coating, wherein the spin coating time is not more than 60s, and the rotation speed is 3500-5000 rpm; after the spin coating is finished, annealing until an aluminum nitrate solution is solidified to form a film to obtain a resistance change oxide layer, wherein the annealing temperature is 150-300 ℃, and the annealing time is not more than 1 h;
c) preparing an upper electrode layer;
plating granular upper electrode materials on the resistance change oxide layer by an evaporation coating method to form an upper electrode layer;
d) preparing a protective layer;
and plating a granular metal protective layer material on the surface of each upper electrode, far away from the resistance change oxide layer, in the upper electrode layer by an evaporation coating method to obtain the RRAM based on the aluminum oxide.
Carrying out ultrasonic cleaning and then carrying out surface plasma cleaning on the substrate in a vacuum environment so as to enhance the hydrophilicity of the lower electrode layer and improve the film forming property of the resistive oxide layer; the time of the surface plasma cleaning process lasts at least 35min, and the resistive oxide layer is prepared within 20min after the surface plasma cleaning is finished.
Technical effects
Compared with the prior art, the invention has the following technical effects:
1) The resistive oxide layer is manufactured by adopting a solution method process, so that the preparation of the RRAM with low cost is realized, the investment on equipment and raw materials is less, and the method can be used for preparing a large-area RRAM device and realizing large-scale industrial application;
2) the resistance change effect is good, the voltage required by the SET and RESET processes is small, and the absolute value of the voltage is 1-4V;
3) the simple substance metal material is used for replacing indium oxide or titanium nitride to be used as the upper electrode, so that the cost is further reduced.
Drawings
FIG. 1 is a schematic structural view of example 1;
FIG. 2 is a graph showing the change of resistance change characteristics in the temperature range of 200 to 300 ℃ in example 1;
in the figure: the resistive random access memory comprises a metal protection layer 100, an upper electrode 101, a resistive oxide layer 200, a lower electrode layer 300, a titanium thin film layer 400, a silicon dioxide thin film layer 401 and a silicon thin film layer 402.
Detailed Description
The invention is described in detail below with reference to the drawings and the detailed description.
Example 1
As shown in fig. 1, the embodiment relates to an aluminum oxide-based RRAM, which includes a substrate, a resistive oxide layer 200, and an upper electrode layer stacked from bottom to top, where the upper electrode layer includes a plurality of upper electrodes 101 arrayed on the resistive oxide layer 200, and a metal protection layer 100 is disposed on a surface of the upper electrode 101 away from the resistive oxide layer 200;
The substrate includes an insulating layer and a lower electrode layer 300;
the resistive oxide layer 200 is Al 2 O 3 A thin film layer.
The metal protection layer 100 is a metal aluminum thin film layer.
The upper electrode 101 in the upper electrode layer is a cylindrical metal nickel film, the thickness of the upper electrode is 50-100 nm, the diameter of the upper electrode is 0.1-0.3 mm, and preferably, the thickness of the upper electrode is 70nm, and the diameter of the upper electrode is 0.1 mm;
the lower electrode layer 300 is a platinum film layer, and has a thickness of 50-150 nm, preferably 100 nm.
The insulating layer is of a three-layer structure which is arranged in a stacked mode and comprises a silicon thin film layer 402, a silicon dioxide thin film layer 401 and a titanium thin film layer 400 which are arranged from bottom to top.
The embodiment relates to a preparation process method of the RRAM, which comprises the following steps:
a) cleaning the substrate;
completely immersing the substrate into a beaker containing deionized water, and placing the beaker in a deionized water environment for ultrasonic cleaning for 10min for the first time;
after the first ultrasonic cleaning, completely immersing the substrate into a beaker containing an acetone solvent, and placing the beaker in a deionized water environment for carrying out second ultrasonic cleaning for 10 min;
after the second ultrasonic cleaning, repeatedly washing the substrate with deionized water, cleaning residual acetone solvent and impurities on the substrate, continuously and completely immersing the substrate into a beaker containing absolute ethyl alcohol, and placing the beaker in a deionized water environment for the third ultrasonic cleaning for 10 min;
After the third ultrasonic cleaning, the substrate is fished out and properly washed by deionized water, the substrate is continuously and completely immersed into a beaker containing the deionized water, and the beaker is placed in a deionized water environment for ultrasonic cleaning for 10min for the fourth time;
after the fourth ultrasonic cleaning, washing the substrate by deionized water and drying by nitrogen;
placing the substrate subjected to the ultrasonic cleaning treatment and dried into a vacuum chamber of a surface plasma cleaning machine, and performing surface plasma cleaning to enhance the hydrophilicity of the lower electrode layer 300; the time of the surface plasma cleaning process lasts for 50 min;
b) preparing a resistive oxide layer 200;
preparing 1.5-3 mol/L aluminum nitrate solution from aluminum nitrate nonahydrate by using deionized water at room temperature (25 ℃); preferably, 18.75g of aluminum nitrate nonahydrate with the purity of 99.99 percent is placed in a beaker, 20ml of deionized water is added into the beaker to prepare 2.5mol/L of aluminum nitrate solution, the solution is stirred at a constant speed until the solution is clear, and then the solution is kept stand for 10 min;
within 20min after the surface plasma cleaning is finished, dropwise adding the prepared aluminum nitrate solution on the lower electrode layer 300 through an injector with the aperture of 0.45 mu m and a PES filter tip, and spin-coating for 45s at the rotating speed of 3500-4500 rpm; after the spin coating is finished, placing the electrode on a heating plate at the temperature of 150-300 ℃ for annealing for 1h, and solidifying an aluminum nitrate solution on the lower electrode layer 300 to form a film to obtain a resistance change oxide layer 200;
c) Preparing an upper electrode 101;
placing granular metal material nickel in a crucible of an electron beam evaporation coating machine, covering a mask plate with the aperture of 0.1mm on the resistive oxide layer 200, downwards placing the mask plate on a suction plate in a cavity of the coating machine, closing the cavity to perform evaporation coating operation, and plating the metal material nickel on the resistive oxide layer 200 to form a semi-finished product with an upper electrode 101;
d) preparing a metal protection layer 100;
after the upper electrode 101 is manufactured, granular metal material aluminum is placed in a crucible of an electron beam evaporation coating machine, a mask plate with the aperture of 0.1mm is covered on the upper electrode 101, the mask plate is downwards placed on a suction plate in a coating machine cavity, the cavity is closed to carry out secondary evaporation coating operation, and a metal aluminum protective layer 100 is formed on the upper electrode 101 in a coating mode.
As shown in fig. 2, which is a resistance change test result of the RRAM device of this embodiment, the abscissa 0 point is used as a boundary, the negative axis is a RESET (RESET) process, the positive axis is a SET (SET) process, voltage bias absolute values are all below 4V, resistance changes are all kept in a certain range, and a gradual change phenomenon occurs with a certain probability in the RESET process.
It is to be emphasized that: the above embodiments are only preferred embodiments of the present invention, and are not intended to limit the present invention in any way, and all simple modifications, equivalent changes and modifications made to the above embodiments according to the technical spirit of the present invention are within the scope of the technical solution of the present invention.
Claims (10)
1. A method for preparing RRAM, characterized by comprising:
a) cleaning the substrate;
completely immersing the substrate into a beaker containing deionized water, and placing the beaker in a deionized water environment for carrying out first ultrasonic cleaning; after the first ultrasonic cleaning, completely immersing the substrate into a beaker containing an acetone solvent, and placing the beaker in a deionized water environment for second ultrasonic cleaning; after the second ultrasonic cleaning, repeatedly washing the substrate with deionized water to clean the acetone solvent and impurities remained on the substrate, completely immersing the substrate into a beaker containing absolute ethyl alcohol, and placing the beaker in a deionized water environment to perform third ultrasonic cleaning; after the third ultrasonic cleaning, washing the substrate with deionized water to remove residual impurities, completely immersing the substrate into a beaker containing the deionized water, and placing the beaker in a deionized water environment to carry out fourth ultrasonic cleaning; after the fourth ultrasonic cleaning, washing the substrate by deionized water and drying by nitrogen;
b) preparing a resistance change oxide layer;
preparing 1.5-3 mol/L aluminum nitrate solution from aluminum nitrate nonahydrate by using deionized water; dropwise adding the prepared aluminum nitrate solution on the lower electrode layer, and performing spin coating, wherein the spin coating time is not more than 60s, and the rotation speed is 3500-5000 rpm; after the spin coating is finished, annealing until an aluminum nitrate solution is solidified to form a film to obtain a resistance change oxide layer, wherein the annealing temperature is 150-300 ℃, and the annealing time is not more than 1 h;
c) Preparing an upper electrode layer;
plating granular upper electrode materials on the resistance change oxide layer by an evaporation coating method to form an upper electrode layer;
d) preparing a protective layer;
and plating a granular metal protective layer material on the surface of each upper electrode, far away from the resistance change oxide layer, in the upper electrode layer by an evaporation coating method to obtain the RRAM based on the aluminum oxide.
2. The method for preparing the RRAM of claim 1, wherein the substrate is subjected to surface plasma cleaning in a vacuum environment after ultrasonic cleaning to enhance the hydrophilicity of the lower electrode layer and improve the film forming property of the resistive oxide layer; the time of the surface plasma cleaning process lasts at least 35min, and the resistive oxide layer is prepared within 20min after the surface plasma cleaning is finished.
3. The method for preparing the RRAM of claim 1, wherein the aluminum nitrate solution is prepared at 20 ℃ to 30 ℃, stirred at a constant speed to be clear, and then kept standing for 5-10 min after stirring, wherein the purity of the aluminum nitrate nonahydrate solute is 99.99%.
4. A method of making a RRAM as claimed in claim 3, wherein the aluminium nitrate solution is applied dropwise to the lower electrode layer by means of a 0.45 μm pore size PES filter tip syringe.
5. The method of claim 1, wherein the evaporation coating process comprises placing the granular upper electrode layer material or the metal protective layer material in a crucible, covering the resistive oxide layer with a mask plate having a hole diameter of 0.1-0.3 mm, and performing evaporation coating in an electron beam evaporation coater.
6. An aluminum oxide-based RRAM prepared by the method according to any one of claims 1 to 5, comprising a substrate, a resistance change oxide layer, and an upper electrode layer stacked from bottom to top;
the substrate comprises an insulating layer and a lower electrode layer;
the resistive oxide layer is Al 2 O 3 Film(s)A layer;
the upper electrode layer comprises a plurality of upper electrodes arrayed on the resistive oxide layer, and a metal protective layer is arranged on the surface of each upper electrode far away from the resistive oxide layer.
7. The aluminum oxide-based RRAM of claim 6, wherein the metal protection layer is a metallic aluminum thin film layer or a metallic tungsten thin film layer.
8. The aluminum oxide-based RRAM of claim 6, wherein the upper electrode is a cylindrical metallic nickel film or a metallic titanium film having a thickness of 50 to 100nm and a diameter of 0.1 to 0.3 mm.
9. The aluminum oxide-based RRAM of claim 6, wherein the lower electrode layer is a metal platinum thin film layer or a silicon thin film layer having a thickness of 50 to 150 nm.
10. The aluminum oxide-based RRAM of claim 6, wherein the insulating layer is a three-layer structure including a titanium thin film layer/a silicon dioxide thin film layer/a silicon thin film layer arranged from top to bottom.
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| CN110299448A (en) * | 2019-06-26 | 2019-10-01 | 西交利物浦大学 | A kind of the resistive formula random access memory and preparation method of blended metal oxide |
| CN110828663A (en) * | 2019-10-31 | 2020-02-21 | 西交利物浦大学 | Lanthanum oxide-based RRAM and preparation method thereof |
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