CN108470827A - A kind of flexible and transparent transition metal oxide resistance-variable storing device and preparation method thereof - Google Patents
A kind of flexible and transparent transition metal oxide resistance-variable storing device and preparation method thereof Download PDFInfo
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- CN108470827A CN108470827A CN201810178521.4A CN201810178521A CN108470827A CN 108470827 A CN108470827 A CN 108470827A CN 201810178521 A CN201810178521 A CN 201810178521A CN 108470827 A CN108470827 A CN 108470827A
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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
- H10N70/801—Constructional details of multistable switching devices
- H10N70/881—Switching materials
- H10N70/883—Oxides or nitrides
- H10N70/8836—Complex metal oxides, e.g. perovskites, spinels
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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
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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
- H10N70/061—Patterning of the switching material
Abstract
The present invention discloses a kind of flexible and transparent transition metal oxide resistance-variable storing device and preparation method thereof, the stack architecture that the memory is made of flexible substrates, hearth electrode, change resistance layer and top electrode.Wherein, hearth electrode ITO or FTO or ZTO, change resistance layer are double-layer film structure, and material is transiton metal binary oxides HfO2、TiO2Equal materials, top electrode is using inert metals such as Pt, Au, W, Ti.It is an advantage of the invention that：The device array has high light transmittance and excellent bend performance.The present invention has high-k, thermal stability good and broad stopband, simple in structure, it is easily prepared the features such as.The device of the present invention keeps good readwrite performance upon bending, and does not have significant degradation before bending, its light transmittance is more than 94% in the wave-length coverage of 400nm~800nm.Flexible and transparent resistance-variable storing device meets message area flexible electronic device development trend and demand in the present invention.
Description
Technical field
The present invention relates to microelectronics and materials science field, specifically a kind of flexible and transparent transition metal oxide resistance
Transition storage and preparation method thereof.
Background technology
With portable, wearable device rapid development and solar cell, thin film transistor (TFT), sensor, You Jifa
The extensive use of the flexible and transparents electronic device such as optical diode, RFID antenna, there is an urgent need to develop one kind based on soft by people
Property substrate on memory device, realize data processing, store function, the functions such as radio-frequency communication, and can be with other electronic devices
It integrates and is applied to the fields such as flexible integration circuit, Flexible Displays, RFID tag, biomedical devices.Therefore, flexibility is deposited
Reservoir shows wide application prospect and is concerned, it has also become an important development side of Future Information field of storage
To.For flexible storage unit, traditional Si base MOS techniques cannot meet demand flexible, another aspect current main-stream
Non-volatile holographic storage technology be the floating gate type flash memory based on electric charge capture, and with the continuous diminution of size, floating-gate device exists
Operation voltage, power consumption, integrated technique, reliability, circuit design etc. are faced with physics and technical bottleneck.Therefore, this
Just there is an urgent need to develop a kind of novel flexible and transparent memories.For coming by the conversion of high low resistance state under different electric excitations
For the resistance-variable storing device for storing information, the storage that the candidate as next-generation nonvolatile memory is showed is latent
Power substantially exceeds the nonvolatile memories such as ferroelectric memory, magnetic storage, phase transition storage.Flexible resistance-variable storing device in addition to
Have many advantages, such as general resistive memory, also have it is at low cost, can the excellent spy such as low temperature, deflection and large area production
Property.Therefore related scientific research mechanism is caused more and more to pay close attention to about the research of flexible and transparent resistance-variable storing device.At present for soft
For the practical application of property transparent resistance random access memory, it is still faced with many urgent problems to be solved.For example device is counter-bending
Characteristic is to be improved, after bending during the storage performance decaying of device, the erasable of device operation voltage and current it is higher and
The stability and durability of high low resistance state are to be improved etc..In addition, transiton metal binary oxides are resistance-variable storing device research
Popular dielectric layer material, such as HfO2、TiO2、ZrO2、 ZnO、Nb2O5、Al2O3, NiO and CuO etc..These metal oxides all tables
It is now to realize the reversible transition stablized between high-resistance state and low resistance state under the action of powering up pulse excitation signal outside.Therefore
We use the scheme of a double-layer structure, so that device is obtained a lower operation voltage, and obtain good stabilization
Property, consistency and durability.
Invention content
The object of the present invention is to be based on above-mentioned background technology, a kind of flexible and transparent transition metal oxide resistive is provided and is deposited
Reservoir and preparation method thereof, the preparation method can be prepared and easy to operate, of low cost at room temperature, and device of the present invention is in difference
Under the test condition of bending curvature, which keeps good readwrite performance upon bending, with bending before do not have significant degradation,
Its light transmittance is more than 94% in the wave-length coverage of 400nm~800nm.
It is made of flexible substrate, hearth electrode, change resistance layer and top electrode the invention is realized in this way sequentially consisting of
Stack architecture；The flexible substrate is polyethylene naphthalate, and the hearth electrode is tin indium oxide (ITO), thick
Degree is 50~300nm, and change resistance layer is the double-deck transiton metal binary oxides membrane structure, and bilayer oxide thickness range is 10
~50nm；Top electrode thickness is 100~300nm.
Further, heretofore described hearth electrode is tin indium oxide (ITO) or fluorine mixes tin oxide (FTO) or is
Zinc mixes tin oxide (ZTO) or is the conductive metallic compounds such as titanium nitride (TiN).
Further, heretofore described resistive layer material is HfO2、TiO2、ZrO2、ZnO、Ta2O5, levels are this respectively
The various combination of a little materials.
Further, heretofore described top electrode is made of the conductive metals magnetron sputtering such as Pt, Au, W, Ti, Cu, Ag,
Or atomic layer deposition is made.
A kind of preparation method of flexible and transparent transition metal oxide resistance-variable storing device of the present invention, is as follows：
1. flexible substrate of the selection with hearth electrode, is used in combination ultrasonic cleaning；
2. the insulating tape of 4mm wide is sticked in long side side in the above-mentioned flexible substrate for having hearth electrode, as reserved electrode,
To test pressing；
3. by being placed on target platform as the target of lower layer's change resistance layer, then change resistance layer, magnetic are prepared using magnetron sputtering technique
Control sputtering vacuum degree is less than 10-4Pa, underlayer temperature are room temperature, operating pressure is 0.3~0.8 Pa, sputtering power is 50~80W,
Sputtering thickness is 10~50nm；
4. by being placed on target platform as the target of upper layer change resistance layer, then change resistance layer, magnetic are prepared using magnetron sputtering technique
Control sputtering vacuum degree is less than 10-4Pa, underlayer temperature are room temperature, operating pressure is 0.3~0.8 Pa, sputtering power is 50~80W,
Sputtering thickness is 10~50nm；
5. a good sample pair made above carries out photoetching treatment, by being dried after gluing, front baking, exposure, exposure, naked exposure,
Development, the technological process dried afterwards obtain the top electrode pattern of 100 μm of diameter.
6. by being placed on target platform as the target material of top electrode, magnetron sputtering technique is utilized on good sample made above
Or atomic layer deposition prepares top electrode, magnetron sputtered vacuum degree is less than 10-4Pa, underlayer temperature are room temperature, operating pressure be 0.3~
0.8Pa, sputtering power are 50~100W.
7. ultrasound 30s or so removes extra photoresist in the power of 40W by the sample prepared, insulating cement is removed
Band makes hearth electrode expose, and to be tested, so far prepared by product to complete.
Film characterization and device detection
The flexible and transparent resistance-variable storing device prepared is subjected to light transmittance test, test equipment is UV, visible light near-infrared point
Light photometer (MPC-3100), is tested in the wave-length coverage of 400nm~800nm.
The flexible and transparent resistance-variable storing device prepared is subjected to electrology characteristic test, test equipment is Agilent B1500 half
Conductor parameter analyzer.
The advantage of the invention is that:The flexible and transparent resistance-variable storing device can be prepared at room temperature, method is simple, at low cost
It is honest and clean, and the present invention shows preferable consistency, stability and durability in the test of differently curved curvature, upon bending
With preferable readwrite performance, while the device has good translucency, it is saturating in the wave-length coverage of 400nm~800nm
Light rate be more than 94%, therefore in the present invention flexible and transparent resistance-variable storing device meet message area flexible electronic device development trend and
Demand has preferable development potentiality and application value.
Description of the drawings
Fig. 1 is the structure chart of device of the present invention；
Fig. 2 is the light transmittance test of the present invention；
Fig. 3 is the present invention current-voltage cyclic curve front and back in bending；
Fig. 4 is the high low resistance state distribution of the present invention 100 cycles of dc sweeps under differently curved radius；
Specific implementation mode
The present invention is described in further details with reference to embodiment.
A kind of flexible and transparent transition metal oxide resistance-variable storing device, the memory are by flexible substrates, hearth electrode, resistance
The stack architecture of change layer and top electrode composition, change resistance layer is double-layer film structure, using transiton metal binary oxides hafnium oxide
And titanium oxide, the above change resistance layer matching way, only it is used for illustrating the present invention, and be not used to limit the scope of the invention.
Wherein use Pt as top electrode material, the shape of top electrode is round, a diameter of 100 μm, thickness 150nm；
Using polyethylene naphthalate as flexible substrate, it is pros to be used as hearth electrode material, shape using tin indium oxide (ITO)
Shape is device cell, and its side length is 2cm, thickness 200nm；Using double layered transition metal oxide as resistive layer material, under
Layer oxide thickness is 15nm, and upper layer oxide thickness is 10nm.
Embodiment 1：
1, it prepares shape to be square, the length of side is the flexible substrate of 2cm；
2, the insulating tape of 4mm wide is sticked in side in the above-mentioned flexible substrate with hearth electrode, as reserved electrode, with
Just pressing is tested；
3, it will be placed on target platform as the titanium oxide target of change resistance layer lower layer, then radiofrequency magnetron sputtering technology utilized to prepare
Lower layer's change resistance layer, magnetron sputtered vacuum degree are less than 10-4Pa, underlayer temperature are room temperature, operating pressure 0.45Pa, sputtering power are
60W, sputtering time 15 minutes；
4, it will be placed on target platform as the hafnium oxide target on change resistance layer upper layer, then radiofrequency magnetron sputtering technology utilized to prepare
Upper layer change resistance layer, magnetron sputtered vacuum degree are less than 10-4Pa, underlayer temperature are room temperature, operating pressure 0.45Pa, sputtering power are
60W, sputtering time 10 minutes；
5, photoetching treatment is carried out to good sample made above, by being dried after gluing, front baking, exposure, exposure, naked exposure,
Development, the technological process dried afterwards obtain the top electrode pattern of 100 μm of diameter.
6, it will be placed on target platform as the platinum target of top electrode, magnetically controlled DC sputtering utilized on good sample made above
Technology prepares top electrode, and magnetron sputtered vacuum degree is less than 10-4Pa, underlayer temperature are room temperature, operating pressure 0.5Pa, sputtering work(
Rate is 100W, sputtering time 2 minutes.
7, by the sample prepared, ultrasound 30s or so removes extra photoresist in the power of 40W, removes insulating cement
Band makes hearth electrode expose, to be tested.
The present embodiment light transmittance is 94% or more.See Fig. 2
The flexible and transparent transition metal oxide resistance-variable storing device prepared is subjected to I-V tests.The test of device be
It is carried out on Agilent B1500A Semiconductor Parameter Analyzer test platforms, a probe is pressed in the surfaces hearth electrode ITO, then
Another probe is pressed in platinum top electrode surface.Filament is formed (Forming) process and is tested using Agilent B1500A first
Software set scanning voltage is 0V~10V, and limitation electric current is 1mA, and Forming voltages are about 2V；Then Agilent is utilized
B1500A test softwares set the scanning voltage of -2.3 V~+2.3V, and using current limiting measures, current limit 3mA prevents device
It is breakdown.Scanning voltage, which works one to recycle, is divided into four parts, is first scanned from 0V to+2.3V, then scanned to 0V, so from+2.3V
It scans to -2.3V from 0V, is finally scanned from -2.3V to 0V afterwards, that is, complete a cycle, it is 101 that each section, which scans step number, i.e.,
Voltage scans to electric current when+2.3V from 0V and takes 101 points.Bend performance test under differently curved curvature is to put device
Onto the mold of differently curved radius, pressing test is carried out, is continuously recycled under dc sweeps voltage 100 times, then reads electricity
The high low resistance of device obtains the high low resistance state distribution of device when pressure is -0.2V.
Measurement result is shown in Fig. 3, Fig. 4.
Claims (4)
1. a kind of flexible and transparent transition metal oxide resistance-variable storing device, successively by flexible substrate, hearth electrode, change resistance layer and top electricity
The stack architecture of pole composition；It is characterized in that, the flexible substrate is polymer poly (ethylene naphthalate), or poly- pair
Ethylene terephthalate or polyimides, the hearth electrode are that tin indium oxide (ITO) or fluorine mix tin oxide
(FTO) zinc mixes tin oxide (ZTO) or titanium nitride (TiN) conductive metallic compound, and thickness is 50~300nm；
The change resistance layer is the double-deck transiton metal binary oxides membrane structure, and thickness range is 10~50nm；The top electrode is
Platinum (Pt), or golden (Au), tungsten (W), titanium (Ti), silver-colored (Ag), copper (Cu), thickness are 100~300nm.
2. a kind of flexible and transparent transition metal oxide resistance-variable storing device according to claim 1, it is characterised in that described
Resistive layer material is HfO2、TiO2、ZnO、ZrO2、Ta2O5, levels are the various combination of these materials respectively.
3. a kind of flexible and transparent transition metal oxide resistance-variable storing device according to claim 1, it is characterised in that
Its light transmittance is more than 94% in the wave-length coverage of 400nm~800nm.
4. a kind of preparation method of flexible and transparent transition metal oxide resistance-variable storing device, it is characterised in that be as follows：
1) flexible substrate of the selection with hearth electrode, is used in combination ultrasonic cleaning；
2) insulating tape of 4mm wide is sticked in long side side in the above-mentioned flexible substrate for having hearth electrode, as reserved electrode, so as to
Test pressing；
3) it will be placed on target platform as the target of lower layer's change resistance layer, then prepare change resistance layer using magnetron sputtering technique, magnetic control splashes
It penetrates vacuum degree and is less than 10-4Pa, underlayer temperature are room temperature, operating pressure is 0.3~0.8Pa, sputtering power is 50~80W, sputtering
Thickness is 10~50nm；
4) it will be placed on target platform as the target of upper layer change resistance layer, then prepare change resistance layer using magnetron sputtering technique, magnetic control splashes
It penetrates vacuum degree and is less than 10-4Pa, underlayer temperature are room temperature, operating pressure is 0.3~0.8Pa, sputtering power is 50~80W, sputtering
Thickness is 10~50nm；
5) photoetching treatment is carried out to good sample made above, by drying, naked exposure, developing after gluing, front baking, exposure, exposure,
The technological process dried afterwards obtains the top electrode pattern of 100 μm of diameter；
6) it will be placed on target platform as the target of top electrode, magnetron sputtering technique or atom utilized on good sample made above
Layer deposition prepares top electrode, and magnetron sputtered vacuum degree is less than 10-4Pa, underlayer temperature are room temperature, operating pressure be 0.3~0.8Pa,
Sputtering power is 50~100W.
7) by the sample prepared, ultrasound 30s or so removes extra photoresist in the power of 40W, and removing insulating tape makes bottom
Electrode exposes, and to be tested, so far prepared by product to complete.
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| CN109461814A (en) * | 2018-10-09 | 2019-03-12 | 河北大学 | A kind of memristor based on zinc oxide and preparation method thereof and preparing the application in the bionical device of nerve synapse |
| CN109473547A (en) * | 2018-10-29 | 2019-03-15 | 江苏师范大学 | Bionical device of a kind of flexibility cynapse and preparation method thereof |
| CN109585651A (en) * | 2018-12-17 | 2019-04-05 | 湖北大学 | A kind of flexible double threshold value gating tube device and preparation method thereof |
| CN109638154A (en) * | 2018-12-17 | 2019-04-16 | 湖北大学 | A kind of flexible gating tube device and preparation method thereof based on hafnium titanyl laminated film |
| CN110176538A (en) * | 2019-05-28 | 2019-08-27 | 湖北大学 | One kind being based on two dimension Ti3C2Transparent flexible resistance-variable storing device of-MXene thin-film material and preparation method thereof |
| CN110265547A (en) * | 2019-06-13 | 2019-09-20 | 复旦大学 | A kind of preparation method of the flexible 3D memory based on COMS backend process |
| CN110473962A (en) * | 2019-07-17 | 2019-11-19 | 深圳大学 | A kind of degradable resistance-variable storing device and preparation method thereof |
| CN110911559A (en) * | 2019-11-08 | 2020-03-24 | 华中科技大学 | Analog HfOx/HfOyHomogeneous junction memristor and regulation and control method thereof |
| CN111739974A (en) * | 2020-06-04 | 2020-10-02 | 中国科学院宁波材料技术与工程研究所 | Bionic optical pain sensor and application thereof |
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Cited By (15)
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| CN109461814A (en) * | 2018-10-09 | 2019-03-12 | 河北大学 | A kind of memristor based on zinc oxide and preparation method thereof and preparing the application in the bionical device of nerve synapse |
| CN109461814B (en) * | 2018-10-09 | 2023-03-24 | 河北大学 | Memristor based on zinc oxide, preparation method of memristor and application of memristor in preparation of neurosynaptic biomimetic device |
| CN109473547B (en) * | 2018-10-29 | 2022-03-15 | 江苏师范大学 | Flexible synapse bionic device and preparation method thereof |
| CN109473547A (en) * | 2018-10-29 | 2019-03-15 | 江苏师范大学 | Bionical device of a kind of flexibility cynapse and preparation method thereof |
| CN109585651A (en) * | 2018-12-17 | 2019-04-05 | 湖北大学 | A kind of flexible double threshold value gating tube device and preparation method thereof |
| CN109638154A (en) * | 2018-12-17 | 2019-04-16 | 湖北大学 | A kind of flexible gating tube device and preparation method thereof based on hafnium titanyl laminated film |
| CN109585651B (en) * | 2018-12-17 | 2024-02-06 | 湖北大学 | Flexible double-layer threshold value gate tube device and preparation method thereof |
| CN109638154B (en) * | 2018-12-17 | 2023-02-28 | 湖北大学 | Flexible gate tube device based on hafnium-titanium-oxygen composite film and preparation method thereof |
| CN110176538A (en) * | 2019-05-28 | 2019-08-27 | 湖北大学 | One kind being based on two dimension Ti3C2Transparent flexible resistance-variable storing device of-MXene thin-film material and preparation method thereof |
| CN110265547A (en) * | 2019-06-13 | 2019-09-20 | 复旦大学 | A kind of preparation method of the flexible 3D memory based on COMS backend process |
| CN110473962A (en) * | 2019-07-17 | 2019-11-19 | 深圳大学 | A kind of degradable resistance-variable storing device and preparation method thereof |
| CN110911559B (en) * | 2019-11-08 | 2021-10-15 | 华中科技大学 | Analog HfOx/HfOyHomogeneous junction memristor and regulation and control method thereof |
| CN110911559A (en) * | 2019-11-08 | 2020-03-24 | 华中科技大学 | Analog HfOx/HfOyHomogeneous junction memristor and regulation and control method thereof |
| CN111739974A (en) * | 2020-06-04 | 2020-10-02 | 中国科学院宁波材料技术与工程研究所 | Bionic optical pain sensor and application thereof |
| CN111739974B (en) * | 2020-06-04 | 2023-08-25 | 中国科学院宁波材料技术与工程研究所 | Bionic optical pain sensor and application thereof |
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Inventor after: Ye Cong Inventor after: Liu Yanxin Inventor after: Zhang Rulin Inventor after: He Pin Inventor after: Wei Xiaodi Inventor after: Xia Qing Inventor after: Zhang Li Inventor before: Ye Cong Inventor before: Zhang Rulin Inventor before: He Pin Inventor before: Wei Xiaodi Inventor before: Xia Qing Inventor before: Zhang Li |
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Application publication date: 20180831 |