CN113130744B - Gating device based on aluminum-doped niobium oxide and preparation method thereof - Google Patents
Gating device based on aluminum-doped niobium oxide and preparation method thereof Download PDFInfo
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- 229910000484 niobium oxide Inorganic materials 0.000 title claims abstract description 78
- URLJKFSTXLNXLG-UHFFFAOYSA-N niobium(5+);oxygen(2-) Chemical compound [O-2].[O-2].[O-2].[O-2].[O-2].[Nb+5].[Nb+5] URLJKFSTXLNXLG-UHFFFAOYSA-N 0.000 title claims abstract description 78
- 238000002360 preparation method Methods 0.000 title claims abstract description 12
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- 238000001755 magnetron sputter deposition Methods 0.000 claims description 22
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- 238000006243 chemical reaction Methods 0.000 abstract description 22
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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
- H10N70/011—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
- H10N70/011—Manufacture or treatment of multistable switching devices
- H10N70/021—Formation of switching materials, e.g. deposition of layers
- H10N70/026—Formation of switching materials, e.g. deposition of layers by physical vapor deposition, e.g. sputtering
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Abstract
The invention provides a gating device based on aluminum-doped niobium oxide and a preparation method thereof, wherein the gating device comprises a bottom electrode; the conversion layer is positioned on the surface of one side of the bottom electrode; the top electrode is positioned on the surface of one side of the transition layer, which is far away from the bottom electrode; wherein the material of the transition layer is an aluminum-doped niobium oxide film, the mol percentage of aluminum doping in the transition layer is m, and m is more than or equal to 0.1% and less than 1.5%. According to the gating device based on the aluminum-doped niobium oxide, the transition layer is the aluminum-doped niobium oxide film, the potential barrier of the niobium oxide in a high resistance state is improved through aluminum doping, the resistance in the high resistance state is increased, and compared with a traditional gating tube with the transition layer made of niobium oxide, the gating device based on the aluminum-doped niobium oxide has a higher gating ratio.
Description
Technical Field
The invention relates to the technical field of information storage, in particular to a gating device based on aluminum-doped niobium oxide and a preparation method thereof.
Background
In recent years, with the development of electronic products, the market demand for nonvolatile memories is increasing. In the process of continuously shrinking the size of the device, the technologies of photoetching, etching and the like gradually approach the physical limit, conventional non-volatile memories also face technical bottlenecks in operating voltage, reliability, power consumption, etc.
A novel Resistive Random Access Memory (RRAM) is a new nonvolatile memory device, and has attracted attention due to its excellent characteristics of fast erase/write speed, good endurance, 3D storage potential, and compatibility with CMOS processes. To achieve higher memory density, the minimum feature area (4F) is typically used in RRAM device array integration 2 ) The cross-shaped structure of the steel wire rope is adopted, but an arrayThere is a serious problem of cross-talk in the columns, a phenomenon of misreading of stored information may occur. The method for effectively solving the crosstalk problem at present is mainly to integrate an RRAM unit into additional rectifying elements (such as transistors, diodes and gate tubes) instead of a self-rectifying RRAM and a complementary memory which are prepared by adopting special materials or structures. While transistors are integrated minimum feature area of 8F 2 Process flow the complexity is high; the diodes being adapted only to a unipolar RRAM device; therefore, a gate tube that can satisfy the minimum feature area and can be integrated with a bipolar RRAM device is generally selected as a rectifying element.
The gate tubes reported at present include: an ovonic threshold switching gate (OTS), a mixed electron ion conduction gate (MIEC), a programmable metallization gate (programming), and an insulator metal transition gate (IMT), among others.
The OTS gate tube mainly adopts the mechanism explanation of thermal-induced electron conversion, impact ionization, recombination and the like, and has the advantage of higher on-state current density in a conducting state. But its material system is very complicated and its non-linearity is low.
MIEC conversion generally occurs in materials that conduct both electronic charge and ions. Such gates are usually copper-based, and a conductive path is formed by copper ion movement to achieve a high non-linear ratio. MIECs have very low leakage currents, but the endurance and retention characteristics are greatly affected due to the gradual failure of the device due to the continuous accumulation of copper ions.
The programmable metallization gating device generally adopts active metals (Ag and Cu) as electrodes, and the basic working principle is as follows: upon application of a sufficient threshold voltage, forming a metallic conductive filament; and after the bias voltage is applied and removed, the conductive wire is broken, and the device shows volatile bidirectional threshold transition characteristics. But its endurance is too poor and it requires a low leakage current RRAM for integration.
The IMT gate tube realizes storage by switching between a high-resistance insulation state and a low-resistance metal stateUsually in NbO 2 And VO 2 Metalloid oxides are observed. The transition is driven by voltage or temperature, so that the leakage current is large, but the stability and the tolerance are good, but the gating rate of the gate tube is low.
In view of the defects of the existing gate tube, the problem to be solved by the technical personnel in the field is to provide a gate tube with good tolerance and high gate ratio.
Disclosure of Invention
In view of the above, the present invention provides a gating device based on aluminum-doped niobium oxide and a method for manufacturing the gating device, which solves or at least partially solves the technical defects in the prior art.
In a first aspect, the present invention provides a gating device based on aluminum doped niobium oxide, comprising:
a bottom electrode;
the conversion layer is positioned on one side surface of the bottom electrode;
the top electrode is positioned on the surface of one side, away from the bottom electrode, of the transition layer;
the material of the transition layer is an aluminum-doped niobium oxide film, the mol percentage of aluminum doping in the transition layer is m, and m is more than or equal to 0.1% and less than 1.5%.
On the basis of the above technical solution, preferably, in the gating device based on aluminum-doped niobium oxide, the material of the bottom electrode is one of Pd, ti, pt, W or TiN; the top electrode is made of one of Pt, ti, pd and W.
On the basis of the above technical solution, preferably, in the gating device based on aluminum-doped niobium oxide, the thickness of the transition layer is 10 to 250nm, and the thickness of the top electrode is 30 to 150nm.
In a second aspect, the present invention further provides a method for preparing a gating device based on aluminum-doped niobium oxide, comprising the following steps:
providing a bottom electrode;
preparing a transition layer on the surface of the bottom electrode;
preparing a top electrode on the surface of one side of the transition layer, which is far away from the bottom electrode;
the material of the transition layer is an aluminum-doped niobium oxide film, and the mol percentage m of aluminum doping in the transition layer is more than or equal to 0.1% and less than 1.5%.
On the basis of the above technical solution, preferably, the preparation method of the gating device based on aluminum-doped niobium oxide specifically includes: niobium oxide and aluminum oxide are used as targets, and a magnetron sputtering method is utilized to carry out codeposition to prepare the transition layer, wherein the sputtering power of the niobium oxide target is n, n is more than 50W and less than or equal to 75W, the sputtering power of the aluminum oxide target is 5-30W, and the sputtering time is 10-120 min.
On the basis of the above technical solution, preferably, in the method for manufacturing a gating device based on aluminum-doped niobium oxide, the material of the top electrode is Pt, and the method for manufacturing the top electrode is as follows: and depositing Pt on the surface of the transition layer by using a magnetron sputtering method by taking Pt as a target material to obtain the Pt, namely obtaining the top electrode.
Further preferably, in the preparation method of the gating device based on the aluminum-doped niobium oxide, the pressure of the vacuum chamber of the magnetron sputtering equipment is controlled to be 2 × 10 during magnetron sputtering -1 ～6×10 -1 Pa, temperature of 290-330K, sputtering power of 20-70W and sputtering time of 20-100 min.
Compared with the prior art, the gating device based on the aluminum-doped niobium oxide and the preparation method thereof have the following beneficial effects:
(1) According to the gating device based on the aluminum-doped niobium oxide, the transition layer is the aluminum-doped niobium oxide film, the potential barrier of the niobium oxide in a high resistance state is improved through aluminum doping, the resistance in the high resistance state is increased, compared with a traditional gating tube with a transition layer made of niobium oxide, the gating device has a higher gating ratio, and meanwhile, the voltage consistency is also improved;
(2) According to the gating device based on the aluminum-doped niobium oxide, the thickness of the conversion layer is 10-250 nm, if the conversion layer is too thin (< 10 nm), metal atoms in the top electrode layer are directly injected into the conversion layer, and the conversion layer is easy to break down when an electrical performance test is carried out, so that resistance state conversion cannot be realized; if the transition layer is too thick (> 250 nm), the resistance of the gating device is large, the forming voltage is too large, and the gating device cannot realize resistance state transition.
Drawings
In order to more clearly illustrate the embodiments of the present invention or the technical solutions in the prior art, the drawings used in the description of the embodiments or the prior art will be briefly described below, and it is obvious that the drawings in the following description are only some embodiments of the present invention, and for those skilled in the art, other drawings can be obtained according to these drawings without creative efforts.
FIG. 1 is a schematic structural view of a gated device based on aluminum-doped niobium oxide of the present invention;
FIG. 2 is a scanning electron microscope image of an aluminum-doped niobium oxide-based gating device prepared in example 1 of the present invention;
FIG. 3 shows an aluminum-based alloy prepared in example 1 of the present invention an X-ray photoelectron spectrum of the gating device doped with niobium oxide;
FIG. 4 is a graph of device current versus applied voltage during the forming process for devices prepared in example 1 of the present invention and comparative example 1;
fig. 5 is a direct current I-V cycle test chart of the devices obtained in example 1 of the present invention and comparative example 1.
Detailed Description
In the following, the technical solutions in the embodiments of the present invention will be clearly and completely described in conjunction with the embodiments of the present invention, and it is obvious that the described embodiments are only a part of the embodiments of the present invention, and not all of the embodiments. All other embodiments, which can be obtained by a person skilled in the art without any inventive step based on the embodiments of the present invention, are within the scope of the present invention.
As shown in fig. 1, the present invention provides a gating device based on aluminum doped niobium oxide, comprising:
a bottom electrode 1;
the transition layer 2 is positioned on the surface of one side of the bottom electrode 1;
the top electrode 3 is positioned on the surface of one side of the transition layer 2, which is far away from the bottom electrode 1;
wherein, the material of the transition layer 2 is an aluminum-doped niobium oxide film, the mol percentage of aluminum doping in the transition layer 2 is m, and m is more than or equal to 0.1% and less than 1.5%.
It should be noted that the gating device based on aluminum-doped niobium oxide in the embodiment of the present application sequentially includes, from bottom to top, a bottom electrode 1, a transition layer 2, and a top electrode 3, where the material of the transition layer 2 is an aluminum-doped niobium oxide thin film (NbO) x Al), in particular, nb is present in the niobium oxide in the present application 2 O 5 And NbO 2 The molar percentage of aluminum doping in the transition layer 2 is m,0.1% ≦ m < 1.5%, for both oxide forms, it being understood that the molar percentage of aluminum doping is calculated as: is the molar amount of aluminum in the transition layer 2 divided by the sum of the molar amounts of aluminum, oxygen, and niobium. According to the gating device, the transition layer 2 is an aluminum-doped niobium oxide film, the potential barrier of the niobium oxide in a high-resistance state is improved through aluminum doping, the high-resistance state resistance is increased, and the gating device has a higher gating ratio compared with a traditional gating tube with the transition layer being niobium oxide.
Furthermore, in the gating device, the Al concentration in the aluminum-doped niobium oxide film is 0.1-1.5%, and relatively low, and the NbO inside the niobium oxide film 2 Increase of area barrier, but not to Nb 2 O 5 The regional conductive wires play a role in regulation and control; if the Al doping content is further increased, if the Al doping content exceeds 1.5%, can promote Nb in the niobium oxide film 2 O 5 Regional conductive filament stability of (2).
In some embodiments, the material of the bottom electrode 1 is one of Pd, ti, pt, W or TiN; the top electrode 3 is made of Pt, ti or Pd, one kind of W.
In some embodiments, the substrate is further included, the bottom electrode is located on a surface of the substrate, and the substrate may be a silicon substrate.
In some embodiments, the thickness of the transition layer 2 is 10 to 250nm and the thickness of the top electrode 3 is 30 to 150nm. In the embodiment of the application, the conversion layer is prepared by a magnetron sputtering method, the thickness of the conversion layer is changed by changing the deposition time and the sputtering power, if the conversion layer is too thin (< 10 nm), metal atoms in the top electrode layer are directly injected into the conversion layer, and the conversion layer is easy to break down when an electrical performance test is carried out, so that the resistance state conversion cannot be realized; if the transition layer is too thick (> 250 nm), the resistance of the gating device is large, the forming voltage is too large, and the gating device cannot realize resistance state transition.
Based on the same inventive concept, the invention also provides a preparation method of the gating device based on the aluminum-doped niobium oxide, which comprises the following steps:
s1, providing a bottom electrode;
s2, preparing a conversion layer on the surface of the bottom electrode;
s3, preparing a top electrode on the surface of one side of the transition layer away from the bottom electrode;
wherein the material of the transition layer is an aluminum-doped niobium oxide film, and the mol percentage m of aluminum doping in the transition layer is more than or equal to 0.1% and less than 1.5%.
In some embodiments, the method of preparing the transition layer is specifically: taking niobium oxide and aluminum oxide as targets, and co-depositing by a magnetron sputtering method to prepare the transformation layer, wherein the pressure in a vacuum chamber of magnetron sputtering equipment is controlled to be 2 multiplied by 10 during magnetron sputtering -1 ～6×10 -1 Pa, the temperature of 290-330K, the sputtering power of the niobium oxide target material is n, n is more than 50W and less than or equal to 75W, the sputtering power of the aluminum oxide target material is 5-30W, and the sputtering time is 10-120 min. It is obvious that in practice, instead of using a magnetron sputtering method for the preparation of the conversion layer, other methods such as chemical vapor deposition, physical vapor deposition may be used.
In some embodiments, the top electrode can also be prepared by magnetron sputtering, and obviously, in addition to preparing the top electrode by magnetron sputtering, other methods such as chemical vapor deposition and physical vapor deposition can be adopted.
In some embodiments, the top electrode is made of Pt, and Pt is deposited on the surface of the transition layer by using the Pt as a target material through a magnetron sputtering method, so as to obtain the top electrode, wherein the pressure in a vacuum chamber of a magnetron sputtering device is controlled to be 2 × 10 during magnetron sputtering -1 ～6×10 -1 Pa, 290-330K, 20-70W of sputtering power of the Pt target and 20-100 min of sputtering time.
Applying a larger forward forming voltage to the top electrode of the gating device based on the aluminum-doped niobium oxide prepared in the application to initially form a conductive channel, wherein the gating device is changed into a low-resistance state; then a smaller negative voltage is added to break the channel and return to the high-resistance state again; then a smaller forward voltage is applied, and when the applied voltage is greater than a threshold voltage, the gating device is changed from an insulating state with high resistance to a metal state with low resistance; after the applied voltage is removed, the temperature of a phase change region in the transition layer is reduced due to the reduction of joule heat, so that the gating device returns to the high-resistance insulation state from the low-resistance metal state.
The method of fabricating the aluminum doped niobium oxide based gated device of the present application is further illustrated by the following specific examples.
Practice of example 1
The embodiment of the application provides a preparation method of a gating device based on aluminum-doped niobium oxide, the method comprises the following steps:
s1, providing a silicon substrate with a Pt bottom electrode;
s2, installing a niobium oxide target material and an aluminum oxide target material in the magnetron sputtering equipment, introducing argon gas serving as inert gas into a vacuum chamber of the magnetron sputtering equipment, and controlling the system pressure in the vacuum chamber to be 4.1 multiplied by 10 -1 Pa, the temperature is 300K, the sputtering power of the niobium oxide target is 55W, the sputtering power of the aluminum oxide target is 5W, and the sputtering time is 40min, namely, a conversion layer aluminum-doped niobium oxide film is obtained by deposition on the Pt bottom electrode, and after the deposition is finished, the thickness of the aluminum-doped niobium oxide film is about 90nm;
s3, mounting a titanium target in the magnetron sputtering equipment, introducing argon as inert gas into a vacuum chamber of the magnetron sputtering equipment, and controlling the system pressure in the vacuum chamber to be 4.1 multiplied by 10 -1 Pa, the temperature is 300K, titanium is sputtered and deposited on the surface of the conversion layer under the sputtering power of 40W, the sputtering time is 30min, and the titanium is deposited after the deposition is finishedThe thickness of the top electrode is about 50nm.
Comparative example 1
This comparative example provides a niobium oxide gate device having the same structure as example 1 except that the material of the conversion layer is niobium oxide, and the niobium oxide gate device provided by this comparative example has the same manufacturing method as example 1 except that no alumina target is used in S2.
Performance testing
Figure 1 is a schematic structural diagram of a gated device based on aluminum doped niobium oxide in one embodiment of the present application, during testing, a bias voltage is applied to the top electrode while the bottom electrode is grounded.
FIG. 2 is a scanning electron microscope image of a gating device based on aluminum-doped niobium oxide prepared in example 1 of the present application, wherein the top electrode is a titanium metal layer with a thickness of about 70nm; the middle layer is aluminum-doped niobium oxide (NbO in the figure) x Al) with a thickness of about 90nm; the bottom electrode is a metal platinum layer, and the thickness of the bottom electrode is about 210nm; the rest is Ti adhesion layer and SiO 2 A substrate.
FIG. 3 is an X-ray photoelectron spectroscopy (XPS) of a conversion layer in an aluminum-doped niobium oxide-based gating device prepared in example 1 of the present application; the abscissa of each graph in fig. 3 is the binding energy and the ordinate is the response intensity; in the graphs, a, b and c are all base lines, the relative content of different elements can be calculated according to the area of a region enclosed by the base lines and the curves, for example, the mass content of the Nb element in the conversion layer can be calculated according to the ratio of the area of the region enclosed between the base line b and the Nd3d in the graph to the sum of the areas of the base line and the region enclosed by the curves in the 3 graphs in the graph. Calculated in fig. 3, the mole percent of Al element in the switching layer was 1.03%, the mole percent of Nb element was 64.29%, and the mole percent of O element was 34.68%, indicating successful doping of Al into niobium oxide.
The performance of the aluminum-doped niobium oxide-based gating device prepared in example 1 of the present application and the niobium oxide-based gating device prepared in comparative example 1 was tested using an agilent B1500A semiconductor parameter analyzer. During testing, voltage is applied to the titanium top electrode, and the platinum bottom electrode is grounded.
The relationship between the device current and the applied voltage in the formining process of the devices prepared in example 1 and comparative example 1 was tested by setting the scan voltage of 0V-10V by the Agilent B1500A test software, i.e. the current was 101 points when the voltage was scanned from 0V to 10V, and the results are shown in FIG. 4, in which Ti/NbO in FIG. 4 x Pt represents the niobium oxide gated device prepared in comparative example 1, ti/NbO x Al/Pt represents the gating device based on aluminum-doped niobium oxide prepared in example 1.
As can be seen from fig. 4, when a forward forming voltage of 0 to 10V is applied, the niobium oxide gating device obtained in comparative example 1 completes the forming process at 4V, and reaches a set limiting current of 1mA; the gating device based on aluminum-doped niobium oxide obtained in example 1 completes the forming process at 9.3V, and reaches the set limiting current of 1mA.
A scanning voltage of-1.5V to 1.5V is set in Agilent B1500A testing software, direct current I-V cyclic test graphs of the gating devices obtained in the embodiment 1 and the comparative example 1 are respectively tested, one cycle of the scanning voltage is divided into 4 parts, the scanning voltage is firstly scanned from 0V to 1.5V, then scanned from 1.5V to 0V, then scanned from 0V to-1.5V, and finally scanned from-1.5V to 0V, namely one cycle is completed, the scanning step number of each part is 101, namely the current is taken as 101 points when the voltage is scanned from 0V to 5V, and the result is shown in FIG. 5.
As can be seen from FIG. 5, the niobium oxide gating device in comparative example 1 has a minimum current, i.e., a high resistance state current, reaching a level of 100 μ A, a maximum current, i.e., a low resistance state current, of 1mA, and a gating ratio of 36; the minimum current, namely the high-resistance state current, of the gating device based on the aluminum-doped niobium oxide in the embodiment 1 is close to the level of 10 muA, the maximum current, namely the low-resistance state current, is 1mA, and the gating ratio of the device is 88. Therefore, the gating device with the aluminum-doped niobium oxide has a higher gating ratio than that of a gating device with niobium oxide, and the gating ratio can be optimized by adding aluminum into niobium oxide. Meanwhile, as can be seen from fig. 5, the voltage distribution of the gating device of aluminum-doped niobium oxide is more concentrated, and the gating device has better voltage consistency.
The above description is only for the purpose of illustrating the preferred embodiments of the present invention and is not to be construed as limiting the invention, and any modifications, equivalents, improvements and the like that fall within the spirit and principle of the present invention are intended to be included therein.
Claims (5)
1. A preparation method of a gating device based on aluminum-doped niobium oxide is characterized by comprising the following steps:
providing a bottom electrode;
preparing a transition layer on the surface of the bottom electrode;
preparing a top electrode on the surface of one side of the transition layer, which is far away from the bottom electrode;
the material of the transition layer is an aluminum-doped niobium oxide film, and the molar percentage of aluminum doping in the transition layer is 1.03%;
the preparation method of the transition layer comprises the following specific steps: niobium oxide and aluminum oxide are used as targets, and a magnetron sputtering method is utilized to carry out codeposition to prepare the transition layer, wherein the sputtering power of the niobium oxide target is n, n is more than 50W and less than or equal to 75W, the sputtering power of the aluminum oxide target is 5-30W, and the sputtering time is 10-120 min.
2. The method of claim 1, wherein the bottom electrode is made of one of Pd, ti, pt, W or TiN; the top electrode is made of one of Pt, ti, pd and W.
3. The method of claim 1, wherein the thickness of the transition layer is between 10nm and 250nm and the thickness of the top electrode is between 30 nm and 150nm.
4. The method of making a gating device based on aluminum-doped niobium oxide as claimed in claim 2, wherein the material of the top electrode is Pt and the method of making the top electrode is: and depositing Pt on the surface of the transition layer by using a magnetron sputtering method by taking Pt as a target material to obtain the Pt, namely obtaining the top electrode.
5. The method of claim 4, wherein magnetron sputtering is performed while controlling a pressure in a vacuum chamber of a magnetron sputtering apparatus to be 2 x 10 -1 ～6×10 -1 Pa, temperature of 290-330K, sputtering power of 20-70W and sputtering time of 20-100 min.
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