CN106449973B - A kind of flexibility resistance-variable storing device and preparation method thereof - Google Patents
A kind of flexibility resistance-variable storing device and preparation method thereof Download PDFInfo
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- H10N70/00—Solid-state devices without a potential-jump barrier or surface barrier, and specially adapted for rectifying, amplifying, oscillating or switching
- H10N70/801—Constructional details of multistable switching devices
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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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- C23C—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL
- C23C14/00—Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material
- C23C14/06—Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material characterised by the coating material
- C23C14/0641—Nitrides
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- C23C14/00—Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material
- C23C14/06—Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material characterised by the coating material
- C23C14/08—Oxides
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- C—CHEMISTRY; METALLURGY
- C23—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; CHEMICAL SURFACE TREATMENT; DIFFUSION TREATMENT OF METALLIC MATERIAL; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL; INHIBITING CORROSION OF METALLIC MATERIAL OR INCRUSTATION IN GENERAL
- C23C—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL
- C23C14/00—Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material
- C23C14/06—Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material characterised by the coating material
- C23C14/08—Oxides
- C23C14/083—Oxides of refractory metals or yttrium
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- C—CHEMISTRY; METALLURGY
- C23—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; CHEMICAL SURFACE TREATMENT; DIFFUSION TREATMENT OF METALLIC MATERIAL; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL; INHIBITING CORROSION OF METALLIC MATERIAL OR INCRUSTATION IN GENERAL
- C23C—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL
- 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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- 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 without a potential-jump barrier or surface barrier, 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 without a potential-jump barrier or surface barrier, and specially adapted for rectifying, amplifying, oscillating or switching
- H10N70/011—Manufacture or treatment of multistable switching devices
- H10N70/021—Formation of the switching material, e.g. layer deposition
- H10N70/026—Formation of the switching material, e.g. layer deposition by physical vapor deposition, e.g. sputtering
Abstract
The invention discloses a kind of flexible resistance-variable storing device, structure is from top to bottom successively are as follows: mica flexible substrate, InGaZnO hearth electrode film layer, ZrHfO media coating and TiN top electrode film layer.The preparation method of the resistance-variable storing device is also disclosed: using certain thickness mica material as flexible substrate, InGaZnO hearth electrode film layer, ZrHfO media coating and TiN top electrode film layer being sequentially formed by the method for magnetron sputtering on flexible substrates.Flexibility resistance-variable storing device provided by the invention has the superperformances such as simple structure, substrate novel and unique, small in size, flexible, read-write is fast, high temperature resistant, corrosion-resistant, bending resistance is strong, it is that a kind of storage performance is stable, at low cost, density is high, service speed is fast, low in energy consumption, fatigue resistance is strong, the flexible resistance-variable storing device that has a extensive future, suitable for promoting the use of in electronic equipment of various.
Description
Technical field
The present invention relates to storage equipment and preparation method thereof, specifically a kind of flexible resistance-variable storing device and its preparation side
Method.
Background technique
In recent years with the continuous diminution of electronic equipment volume, handling data capability constantly enhances, volume constantly reduces,
High density, high speed and the resistive of low-power consumption formula memory become the development trend of memory of new generation.
Resistive formula memory (RRAM) is with the non-resistance for leading material under DC Electric Field, between high low resistance state
Realize the next-generation nonvolatile memory on the basis of reversible transformation.Early in 1967, someone had studied Au/SiO/Al structure
Electric resistance changing.Due to the influence of the various factors such as laboratory facilities and demand, someone develops sull resistance within 2000
Transfer characteristic.From structure, it is the resistive that can be changed up and down that resistive formula memory, which is typical " sandwich " structure,
Material.It can be under applying bias voltage effect, and the resistance of device can change between high resistance on earth resistance.Due to
The advantages of RRAM, can just overcome the problems, such as the thinning caused charge leakage of oxidation film in Flash, so future 32nm or less
The RRAM of node will likely replace Flash reservoir.
In recent years, with the continuous development of flexible electronic, flexible electronic device is because of its light portable and has good machine
Tool performance causes people's extensive concern.So under the premise of flexible electronic technology is fast-developing, the flexibility pair of RRAM is realized
It will be had a very important significance in the application for widening RRAM.Currently, having some PET flexibility resistance-variable storing devices in industry
Research report, still, causes its resistive conversion coating that must prepare at low temperature since the heat-resisting quantity of PET flexible substrate is limited
With use, in addition, the flexible RRAM of preparation, which exists, is easy to make its change in resistance bad stability even resistive by repeatedly bending
Performance is lost, but also there is a problem of that flexibility is poor, not flexible, high temperature resistance is limited, corrosion resistance is poor.
Summary of the invention
The object of the present invention is to provide a kind of flexible resistance-variable storing devices and preparation method thereof, are deposited with solving existing flexible resistive
Reservoir is limited there are the heat-resisting quantity of flexible substrate and causes its resistive conversion coating that must make and use at low temperature, is repeatedly curved
The problem of folding existing resistance value transformation bad stability or even change resistance performance forfeiture.
The purpose of the present invention is what is be achieved through the following technical solutions: it is a kind of flexibility resistance-variable storing device, structure from it is lower to
On successively are as follows: mica flexible substrate, InGaZnO hearth electrode film layer, ZrHfO media coating and TiN top electrode film layer.
The ZrHfO media coating with a thickness of 3 ~ 8nm.
The InGaZnO hearth electrode film layer with a thickness of 60 ~ 190nm, preferably 150 ~ 190nm.
The TiN top electrode film layer with a thickness of 40nm ~ 150nm.
The mica flexible substrate with a thickness of 0.01 ~ 0.04mm.
The present invention also provides the preparation methods of flexible resistance-variable storing device, comprising the following steps:
(a) mica flexible substrate is fixed on the intracorporal substrate table of magnetron sputtering apparatus chamber, by InGaZnO target and
ZrHfO target is individually placed on two target platforms, and cavity is evacuated to 1 × 10-4~4×10-4Pa;It is passed through 25 into cavity ~
The Ar of 50sccm, adjustment slide valve make the intracorporal pressure of chamber maintain 0.1 ~ 3Pa, open penetrating for control InGaZnO target build-up of luminance
Frequency source, adjustment RF source power are 180 ~ 220W, 0.2 ~ 1.5Pa of pressure, make InGaZnO target build-up of luminance, 7 ~ 13min of pre-sputtering,
Baffle 17 ~ the 23min of formal sputtering for opening InGaZnO target, in the upper formation InGaZnO bottom electrode film of mica flexible substrate
Layer, obtains mica flexible substrate/InGaZnO hearth electrode film layer composite construction;
(b) baffle for closing InGaZnO target, is evacuated to 1 × 10 again-4~4×10-4Pa is passed through 10 ~ 40sccm O2
With 20 ~ 70sccm Ar, adjusting slide valve makes the intracorporal pressure of chamber maintain 2 ~ 7Pa, opens penetrating for control ZrHfO target build-up of luminance
Frequency source, adjustment RF source power are 50 ~ 100W, 1 ~ 5Pa of pressure;Make ZrHfO target build-up of luminance, 7 ~ 13min of pre-sputtering;It opens
ZrHfO target baffle 28 ~ 33min of formal sputtering, forms ZrHfO in the InGaZnO hearth electrode film layer in mica flexible substrate
Media coating obtains mica flexible substrate/InGaZnO hearth electrode film layer/ZrHfO media coating composite construction;
(c) baffle for closing ZrHfO target, closes radio frequency source, charge valve, slide valve, opens the chamber of magnetron sputtering apparatus
Body places mask plate in the mica flexible substrate for forming InGaZnO hearth electrode film layer and ZrHfO media coating, is fixed to magnetic
On the substrate table for controlling sputtering equipment cavity;Cavity is evacuated to 1 × 10-4~4×10-4Pa is passed through 20 ~ 30sccm into cavity
Ar, so that the intracorporal pressure of chamber is maintained 0.1 ~ 3Pa, open DC source, the power for adjusting DC source is 13 ~ 17W, pressure 0.5 ~
1Pa makes TiN target build-up of luminance, 7 ~ 13min of pre-sputtering;55 ~ 65min of formal sputtering forms the top TiN electricity on ZrHfO media coating
Pole film layer has obtained mica flexible substrate/InGaZnO hearth electrode film layer/ZrHfO media coating/TiN top electrode film layer composite junction
The flexible resistance-variable storing device of structure.
The present invention provides mica flexible substrate described in step (a) in preparation method can cut the side with tape-stripping by knife
Method is thinned to ideal thickness, and preferably with a thickness of 0.01 ~ 0.04mm in the present invention, flexible substrate bendable can be played under the thickness
Bent characteristic.
The present invention provide preparation method in step (a) the InGaZnO hearth electrode film layer with a thickness of 60 ~ 190nm;It is preferred that
150~190nm。
The present invention provide preparation method in step (b) the ZrHfO media coating with a thickness of 3 ~ 8nm.
The circle that diameter is 60 ~ 300 μm is evenly equipped in preparation method provided by the invention on mask plate described in step (c)
Shape hole.
TiN top electrode film layer described in step (c) includes several is evenly distributed in preparation method provided by the invention
The circular electrode that diameter on ZrHfO media coating is 60 ~ 300 μm;It is with a thickness of 40 ~ 150nm.
InGaZnO target, ZrHfO target and the TiN target used in the present invention belong to commercial goods.
The present invention is by having selected the mica material of suitable thickness as flexible substrate, by the method for magnetron sputtering in cloud
InGaZnO hearth electrode film layer, ZrHfO media coating and TiN top electrode film layer are sequentially formed in female flexible substrate, have been obtained highly dense
The flexible resistance-variable storing device of degree.The present invention has selected high temperature resistant up to 1500 DEG C of mica material as flexible liner in a creative way
Bottom, and the flexible substrate also has the characteristics that rotproofness is strong, toughness is high, small in size, flexible, is applied to various flexibilities
Electronic equipment has positive impetus to industry technology development.Resistance-variable storing device provided by the present invention, shows more
Stable change in resistance, high and low resistance state resistance value distribution is concentrated very much, and differs larger between high resistance and low-resistance value, because
This does not allow that high and low resistance value is easily caused to obscure, and does not allow to easily cause in reading data and misread;By being repeatedly bent its change in resistance
It can control within the fluctuation range of very little, performance is highly stable.In addition, flexibility resistance-variable storing device provided by the invention has
Significant switching effect, and antifatigue test of the memory under high-impedance state and low resistance state is excellent in.
In short, flexibility resistance-variable storing device provided by the invention has structure simple, substrate novel and unique, small in size, pliable
The superperformances such as bent, read-write data are fast, high temperature resistant, corrosion-resistant, bending resistance is strong, are that a kind of storage performance is stable, at low cost, close
The flexible resistance-variable storing device that degree is high, service speed is fast, low in energy consumption, fatigue resistance is strong, has a extensive future, is suitable in various electronics
It is promoted the use of in equipment.
Detailed description of the invention
Fig. 1 is the structural schematic diagram of flexible resistance-variable storing device provided by the present invention.
Fig. 2 is the structural schematic diagram that embodiment 2 prepares magnetron sputtering apparatus used in flexible resistance-variable storing device.
Fig. 3 is the voltage-current characteristic figure of the made flexible resistance-variable storing device of embodiment 2.
Fig. 4 is HRS the and LRS retention performance figure of the made flexible resistance-variable storing device of embodiment 2.
Fig. 5 is the flexural property figure of the made flexible resistance-variable storing device of embodiment 2.
Specific embodiment
Following example is for present invention be described in more detail, but embodiment does not do any type of limit to the present invention
It is fixed.Unless stated otherwise, the present invention uses reagent, method and apparatus is the art conventional reagents, method and apparatus.But
The invention is not limited in any way.
Embodiment 1
It is prepared by the present invention flexibility resistance-variable storing device structure as shown in Figure 1, include the bottom mica flexible substrate 1,
Method in mica flexible substrate 1 through magnetron sputtering grown InGaZnO hearth electrode film layer 2, in InGaZnO bottom electrode film
The ZrHfO media coating 3 grown on layer 2, grown TiN top electrode film layer 4 on ZrHfO media coating 3.
Wherein mica flexible substrate 1 with a thickness of 0.01 ~ 0.04mm, preferably 0.02mm, can pass through in actual use
Knife cuts the methods of adduction tape-stripping and mica sheet is thinned to ideal thickness.
Wherein ZrHfO media coating 3 with a thickness of 3 ~ 8nm, preferably 5nm;InGaZnO hearth electrode film layer 2 with a thickness of
60 ~ 190nm, preferably 150 ~ 190nm, more preferably 170nm;
Wherein TiN top electrode film layer 4 includes the circle that several diameters being evenly distributed on ZrHfO media coating 3 are 200 μm
Shape electrode;It is with a thickness of 40nm ~ 150nm, preferably 40nm.
Embodiment 2
The preparation method of resistance-variable storing device provided by the present invention includes the following steps:
(1) using magnetron sputtering apparatus as indicated with 2, the lower section of the substrate table 7 in cavity 9 is arranged there are two target platform 5,
5 top of target platform is placed with target 6 respectively;Magnetron sputtering apparatus cavity 9 is opened, it will be first with a thickness of the mica flexible substrate of 0.02mm
It is placed on substrate bracket 8 and on the substrate table 7 that is fixed in cavity 9, InGaZnO target and ZrHfO target is individually placed to two
On a target platform 5, cavity 9 is closed after fixing, 2 × 10 are evacuated to cavity 9 and gas circuit-4Pa;By charge valve 11 to cavity
It is inside passed through the Ar of 25sccm, adjustment slide valve 10 makes the pressure in cavity 9 maintain 0.5Pa, opens control InGaZnO target and rises
The radio frequency source of brightness, adjustment RF source power are 200W, pressure 0.5Pa, make InGaZnO target build-up of luminance, pre-sputtering 10min;It splashes in advance
After penetrating, InGaZnO target baffle formal sputtering 20min is opened, forms the first layer with a thickness of 170nm in mica flexible substrate
InGaZnO hearth electrode film layer;
(2) baffle of InGaZnO target is closed, Yao Chongxin is evacuated to 2 × 10-4Pa is passed through by charge valve 11
25sccm O2With 50sccm Ar, the intracorporal pressure of chamber is made to maintain 3Pa, open the radio frequency source of control ZrHfO target build-up of luminance, adjusted
Whole RF source power is 80W, pressure 3Pa;Make ZrHfO target build-up of luminance, pre-sputtering 10min;After pre-sputtering, ZrHfO target is opened
Baffle formal sputtering 30min is formed in the InGaZnO hearth electrode film layer in mica flexible substrate and is situated between with a thickness of the ZrHfO of 5nm
Plasma membrane layer;
(3) baffle for closing ZrHfO target, closes radio frequency source, charge valve 11, slide valve 10, opens magnetron sputtering apparatus
Cavity 9, the mica flexible substrate that will have plated two membranes are taken out, and place mask plate on ZrHfO media coating, on mask plate
The even round hole for being densely covered with diameter and being 200 μm, the size of these round holes is having for memory after electrode film layer is grown
Imitate the size of working region;And substrate table 8 is taken out, and it is completely extremely shinny with sand paper polishing, the waste polished is cleaned with acetone
With the organic matter of surface attachment, with the last wiped clean of alcohol, the substrate bracket 7 substrate table 8 handled well being put into cavity 9
On, cavity 9 is closed after fixing, and the cavity 9 of magnetron sputtering apparatus is evacuated to 2 × 10 by mechanical pump and molecular pump-4Pa、
The Ar of 25sccm is passed through into cavity, adjustment slide valve 10 makes the intracorporal pressure of chamber maintain 0.8Pa, opens DC source, adjustment
Direct current source power is 15W, pressure 0.8Pa, makes TiN target build-up of luminance, pre-sputtering 10min, formal sputtering 60min, in ZrHfO medium
In film layer formed with a thickness of 40 nm TiN top electrode film layer, obtained mica flexible substrate/InGaZnO hearth electrode film layer/
ZrHfO media coating/TiN top electrode film layer composite construction resistance-variable storing device.
Embodiments described above is any one embodiment in the preparation method that the present invention is protected, this field
Those of ordinary skill can be according to claim and range (the mica flexible liner base thickness of technological parameter described in this description
Degree, the chamber vacuum degree of its magnetron sputtering, RF source power, pre-sputtering time and formal sputtering time etc.) in can get this
The claimed flexible resistance-variable storing device of inventive embodiments 1, and prepared flexible resistance-variable storing device with it is manufactured in the present embodiment
Device has substantially similar performance.
3 performance test of embodiment
Scanning voltage by being added in the flexible resistance-variable storing device of the preparation of embodiment 2 measures its current-voltage characteristic curve,
As a result see Fig. 3.As shown in figure 3, applying positive voltage on the TiN electrode of resistive element prepared in example 2, when voltage reaches
When cut-in voltage (Set Voltage), resistive element is transformed into low resistance state (1 → 2) by high-impedance state, with the reduction of scanning voltage
When closing voltage (Reset Voltage) to forward direction, the resistance value of resistive element is switched to high-impedance state (3 → 4) by low resistance state, is applied anti-
When to scanning voltage similarly.
By the survey for carrying out the retention performance of high-impedance state and low resistance state to flexible substrate resistive device prepared by embodiment 2
Examination, as a result as shown in figure 4, high-impedance state (order of magnitude is 109) and low resistance state (order of magnitude is 106) it in duration is more than 104Second is for a long time
Retention performance is highly stable under testing, and the ratio of high-impedance state and low resistance state is more than 103A order of magnitude has good resistive characteristic,
It is not susceptible to misread.
By carrying out the test of height configuration after 1000 bendings to flexible substrate resistive device prepared by example 2, as a result
As shown in figure 5, the high-impedance state recorded and low configuration state can be in relatively small variations in the bending by 1000 times
It is kept under range, illustrates that the resistive element has flexible characteristic.This characteristic has extensive in future electronic equipment
Application prospect.
The above embodiment is a preferred embodiment of the present invention, but embodiments of the present invention are not by the embodiment
Limitation, other any changes, modifications, substitutions, combinations, simplifications made without departing from the spirit and principles of the present invention,
It should be equivalent substitute mode, be included within the scope of the present invention.
Claims (2)
1. a kind of flexibility resistance-variable storing device, which is characterized in that its structure is from top to bottom successively are as follows: mica flexible substrate, InGaZnO
Hearth electrode film layer, ZrHfO media coating and TiN top electrode film layer;
The ZrHfO media coating with a thickness of 3 ~ 8nm;
The InGaZnO hearth electrode film layer with a thickness of 60 ~ 190nm;
The TiN top electrode film layer with a thickness of 40nm ~ 150nm;
The mica flexible substrate with a thickness of 0.01 ~ 0.04mm.
2. a kind of preparation method of flexible resistance-variable storing device as described in claim 1, which comprises the following steps:
(a) mica flexible substrate is fixed on the intracorporal substrate table of magnetron sputtering apparatus chamber, by InGaZnO target and ZrHfO
Target is individually placed on two target platforms, and cavity is evacuated to 1 × 10-4~4×10-4Pa;25 ~ 50sccm is passed through into cavity
Ar, adjustment slide valve makes the intracorporal pressure of chamber maintain 0.1 ~ 3Pa, opens the radio frequency source of control InGaZnO target build-up of luminance, adjust
Whole RF source power is 180 ~ 220W, 0.2 ~ 1.5Pa of pressure, makes InGaZnO target build-up of luminance, and 7 ~ 13min of pre-sputtering is opened
Baffle 17 ~ 23min of formal sputtering of InGaZnO target is obtained in the upper formation InGaZnO hearth electrode film layer of mica flexible substrate
To mica flexible substrate/InGaZnO hearth electrode film layer composite construction;
(b) baffle for closing InGaZnO target, is evacuated to 1 × 10 again-4~4×10-4Pa is passed through 10 ~ 40sccm O2With 20
~ 70sccm Ar, adjustment slide valve make the intracorporal pressure of chamber maintain 2 ~ 7Pa, open the radio frequency source of control ZrHfO target build-up of luminance,
Adjustment RF source power is 50 ~ 100W, 1 ~ 5Pa of pressure;Make ZrHfO target build-up of luminance, 7 ~ 13min of pre-sputtering;Open ZrHfO target
Baffle 28 ~ 33min of formal sputtering forms ZrHfO media coating in the InGaZnO hearth electrode film layer in mica flexible substrate,
Obtain mica flexible substrate/InGaZnO hearth electrode film layer/ZrHfO media coating composite construction;
(c) baffle for closing ZrHfO target, closes radio frequency source, charge valve, slide valve, opens the cavity of magnetron sputtering apparatus,
It is formed in InGaZnO hearth electrode film layer and the mica flexible substrate of ZrHfO media coating and places mask plate, be fixed to magnetron sputtering
On the substrate table of equipment cavity;Cavity is evacuated to 1 × 10-4~4×10-4Pa is passed through the Ar of 20 ~ 30sccm into cavity,
So that the intracorporal pressure of chamber is maintained 0.1 ~ 3Pa, opens DC source, the power for adjusting DC source is 13 ~ 17W, 0.5 ~ 1Pa of pressure,
Make TiN target build-up of luminance, 7 ~ 13min of pre-sputtering;55 ~ 65min of formal sputtering forms TiN top electrode film on ZrHfO media coating
Layer, has obtained mica flexible substrate/InGaZnO hearth electrode film layer/ZrHfO media coating/TiN top electrode film layer composite construction
Flexible resistance-variable storing device.
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