CN108428792A - Based on the multistage resistance-variable storing device and preparation method of inorganic perovskite and application - Google Patents
Based on the multistage resistance-variable storing device and preparation method of inorganic perovskite and application Download PDFInfo
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- CN108428792A CN108428792A CN201810297318.9A CN201810297318A CN108428792A CN 108428792 A CN108428792 A CN 108428792A CN 201810297318 A CN201810297318 A CN 201810297318A CN 108428792 A CN108428792 A CN 108428792A
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- 238000002360 preparation method Methods 0.000 title claims abstract description 24
- 230000008859 change Effects 0.000 claims abstract description 37
- 239000000758 substrate Substances 0.000 claims abstract description 8
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 claims description 33
- LYQFWZFBNBDLEO-UHFFFAOYSA-M caesium bromide Chemical compound [Br-].[Cs+] LYQFWZFBNBDLEO-UHFFFAOYSA-M 0.000 claims description 24
- 238000001035 drying Methods 0.000 claims description 5
- 238000000137 annealing Methods 0.000 claims description 4
- JTCFNJXQEFODHE-UHFFFAOYSA-N [Ca].[Ti] Chemical compound [Ca].[Ti] JTCFNJXQEFODHE-UHFFFAOYSA-N 0.000 claims description 2
- 238000010422 painting Methods 0.000 claims 1
- 239000000463 material Substances 0.000 abstract description 8
- 239000010409 thin film Substances 0.000 abstract description 6
- 238000012360 testing method Methods 0.000 abstract description 5
- 239000000243 solution Substances 0.000 description 15
- ZMXDDKWLCZADIW-UHFFFAOYSA-N N,N-dimethylformamide Substances CN(C)C=O ZMXDDKWLCZADIW-UHFFFAOYSA-N 0.000 description 13
- 239000010408 film Substances 0.000 description 6
- 238000000034 method Methods 0.000 description 6
- 239000011521 glass Substances 0.000 description 5
- 238000005265 energy consumption Methods 0.000 description 4
- 230000000694 effects Effects 0.000 description 3
- 238000005286 illumination Methods 0.000 description 3
- 238000004528 spin coating Methods 0.000 description 3
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- 238000000151 deposition Methods 0.000 description 2
- 238000010586 diagram Methods 0.000 description 2
- 238000005516 engineering process Methods 0.000 description 2
- 238000001755 magnetron sputter deposition Methods 0.000 description 2
- 230000003647 oxidation Effects 0.000 description 2
- 238000007254 oxidation reaction Methods 0.000 description 2
- 239000000843 powder Substances 0.000 description 2
- 239000000523 sample Substances 0.000 description 2
- 229910052709 silver Inorganic materials 0.000 description 2
- CBENFWSGALASAD-UHFFFAOYSA-N Ozone Chemical compound [O-][O+]=O CBENFWSGALASAD-UHFFFAOYSA-N 0.000 description 1
- 229910052782 aluminium Inorganic materials 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 239000013068 control sample Substances 0.000 description 1
- 230000007812 deficiency Effects 0.000 description 1
- 230000008021 deposition Effects 0.000 description 1
- ZASWJUOMEGBQCQ-UHFFFAOYSA-L dibromolead Chemical compound Br[Pb]Br ZASWJUOMEGBQCQ-UHFFFAOYSA-L 0.000 description 1
- 230000005611 electricity Effects 0.000 description 1
- 238000001914 filtration Methods 0.000 description 1
- 229910052737 gold Inorganic materials 0.000 description 1
- 238000010438 heat treatment Methods 0.000 description 1
- 230000006872 improvement Effects 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- 230000007334 memory performance Effects 0.000 description 1
- 239000007769 metal material Substances 0.000 description 1
- 239000011259 mixed solution Substances 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 238000011056 performance test Methods 0.000 description 1
- 230000005622 photoelectricity Effects 0.000 description 1
- 239000004810 polytetrafluoroethylene Substances 0.000 description 1
- 229920001343 polytetrafluoroethylene Polymers 0.000 description 1
- 239000011148 porous material Substances 0.000 description 1
- 238000011160 research Methods 0.000 description 1
- 230000002441 reversible effect Effects 0.000 description 1
- 238000007789 sealing Methods 0.000 description 1
- 239000004332 silver Substances 0.000 description 1
- 239000002904 solvent Substances 0.000 description 1
- 238000003756 stirring Methods 0.000 description 1
- 238000002207 thermal evaporation Methods 0.000 description 1
- 230000009466 transformation Effects 0.000 description 1
- 230000007704 transition Effects 0.000 description 1
Classifications
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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
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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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Abstract
The invention discloses based on the multistage resistance-variable storing device and preparation method of inorganic perovskite and application, wherein multistage resistance-variable storing device includes successively from bottom to up：Substrate, transparent hearth electrode, CsPbBr3Perovskite change resistance layer and top electrode.The present invention is by CsPbBr3Perovskite thin film is separately as change resistance layer, due to CsPbBr3Perovskite has good photoelectric characteristic, can change material high-resistance resistors value by absorbing the light of different-waveband so that be based on CsPbBr3There are the multistage resistance-variable storing device of perovskite more resistance states, test to show that its on-off ratio is more than 5000, meet the requirement more than 1000.
Description
Technical field
The present invention relates to memory technology field more particularly to a kind of multistage resistance-variable storing device based on inorganic perovskite and
Preparation method and application.
Background technology
Resistance-variable storing device is a kind of memory made using electric resistance changing effect, mainly utilizes film material in change resistance layer
The reversible change of resistance is expected to store information.The basic structure of resistance-variable storing device is that the cross of hearth electrode/change resistance layer/top electrode is handed over
Array structure is pitched, i.e. upper/lower electrode is to intersect vertically, in storage medium is clipped in.However, the resistance-variable storing device of current research is more
For traditional second-level storage, that is, stores state and only there was only 0 and 1 two kind, cause the storage density of memory by dramatically
Limitation, while causing memory window value smaller.
Therefore, the prior art is also to be developed.
Invention content
In view of above-mentioned deficiencies of the prior art, the multistage resistance based on inorganic perovskite that the purpose of the present invention is to provide a kind of
Transition storage and preparation method and application, it is intended to which it is smaller to solve existing second-level storage memory window value, and stability is insufficient, no
The problem of easy-regulating.
Technical scheme is as follows：
It is a kind of multistage resistance-variable storing device, include successively from bottom to up：Substrate, transparent hearth electrode, CsPbBr3Perovskite change resistance layer and
Top electrode.
The multistage resistance-variable storing device, wherein the CsPbBr3The thickness of perovskite change resistance layer is 25-45 nm.
The multistage resistance-variable storing device, wherein the CsPbBr3The thickness of perovskite change resistance layer is 30 nm.
A kind of preparation method of multistage resistance-variable storing device as described above, including：
Step A, transparent hearth electrode is made in substrate；
Step B, CsPbBr is made on the transparent hearth electrode3Perovskite change resistance layer；
Step C, in the CsPbBr3Top electrode is made on perovskite change resistance layer, obtains the multistage resistance-variable storing device.
The preparation method of the multistage resistance-variable storing device, wherein in the step B, the CsPbBr3Perovskite resistive
Layer is prepared by following preparation method：
Step B1, PbBr is prepared respectively2DMF solution and CsBr methanol solution；
Step B2, by the PbBr2DMF solution be spin-coated on the transparent hearth electrode, and it is dry；
Step B3, the sample after drying is contained into PbBr2One side immerse 5-15min in the methanol solution of the CsBr, then take
Go out and anneal, forms CsPbBr3Perovskite change resistance layer.
The preparation method of the multistage resistance-variable storing device, wherein in the step B1, the methanol solution of the CsBr
A concentration of 12-18 mg/mL.
The preparation method of the multistage resistance-variable storing device, wherein in the step B2, the speed of spin coating is 3000rpm-
4500rpm。
The preparation method of the multistage resistance-variable storing device, wherein in the step B2, dry condition is：70-80
Dry 25-35 min at DEG C.
The preparation method of the multistage resistance-variable storing device, wherein in the step B3, the condition of annealing is 175-185
Anneal 1-2 h at DEG C.
A kind of multistage resistance-variable storing device as described above, is applied to non-volatile type memorizer field.
Advantageous effect：The present invention provides a kind of multistage resistance-variable storing device as described above, the present invention is by CsPbBr3Calcium titanium
Mine film is separately as change resistance layer, due to CsPbBr3Perovskite has good photoelectric characteristic, can be by absorbing different-waveband
Light change material high-resistance resistors value so that be based on CsPbBr3The multistage resistance-variable storing device of perovskite has more resistance states, surveys
Its bright on-off ratio of taking temperature is more than 5000, meets the requirement more than 1000.
Description of the drawings
Fig. 1 is the structural schematic diagram of the multistage resistance-variable storing device based on inorganic perovskite of the embodiment of the present invention 1.
Fig. 2 be the embodiment of the present invention 1 based on the multistage resistance-variable storing device of inorganic perovskite under different illumination intensity
Electrical testing performance comparison figure.
Fig. 3 is for the embodiment of the present invention 1 based on the multistage resistance-variable storing device of inorganic perovskite in different resistive layer thickness feelings
Electrical testing performance comparison figure under condition.
Specific implementation mode
The present invention provides a kind of based on the multistage resistance-variable storing device and preparation method of inorganic perovskite and application, to make this
The purpose of invention, technical solution and effect are clearer, define, and the present invention is described in more detail below.It should be appreciated that this
The described specific embodiment in place is only used to explain the present invention, is not intended to limit the present invention.
The structural schematic diagram of the multistage resistance-variable storing device of the present invention is as shown in Figure 1, include successively from bottom to up：Substrate 1, thoroughly
Bright hearth electrode 2（Such as ITO or AZO）、CsPbBr3Perovskite change resistance layer 3 and top electrode 4；Specifically, the transparent hearth electrode can
It is made of ITO or AZO, the top electrode can be selected the metal material with good conductivity such as Al, Au or Ag and make, and thickness is about
30 nm。
The present invention is by CsPbBr3Perovskite thin film is separately as change resistance layer, due to CsPbBr3Perovskite has good light
Electrical characteristics can change material high-resistance resistors value so that be based on CsPbBr by absorbing the light of different-waveband3Perovskite
Multistage resistance-variable storing device has more resistance states, and on-off ratio is more than 1000.
Preferably, the CsPbBr3The thickness of perovskite change resistance layer is 25-45 nm.Resistive layer thickness is too thick, opens electricity
Pressure just increases, and device energy consumption increases；Resistive layer thickness is too thin, although cut-in voltage can reduce, power consumption is reduced, and can cause device
Part is unstable（Current -voltage curve is unstable）, storage performance can be influenced.It can guarantee device steady operation in above-mentioned thickness range
And energy consumption is within the acceptable range.
It is further preferred that the CsPbBr3The thickness of perovskite change resistance layer is 30 nm.Under this thickness, work in device
In terms of stability and energy consumption, comprehensive performance is more preferable.
The present invention also provides a kind of preparation methods of multistage resistance-variable storing device as described above, including：
Step A, transparent hearth electrode is made in substrate；
Step B, CsPbBr is made on the transparent hearth electrode3Perovskite change resistance layer；
Step C, in the CsPbBr3Top electrode is made on perovskite change resistance layer, obtains the multistage resistance-variable storing device.
Specifically, transparent conductive film can be plated in substrate, be then etched into electrode, then made CsPbBr3Perovskite
Change resistance layer, a kind of preferred CsPbBr3The preparation method of perovskite change resistance layer, including：
Step B1, PbBr is prepared respectively2DMF solution and CsBr methanol solution；
Step B2, by the PbBr2DMF solution be spin-coated on the transparent hearth electrode, and it is dry；
Step B3, the sample after drying is contained into PbBr2One side immerse 5-15min in the methanol solution of the CsBr, then take
Go out and anneal, forms CsPbBr3Perovskite change resistance layer.
Compared to the material of traditional medium of oxides, need using the methods of magnetron sputtering, plasma oxidation, the present invention
CsPbBr is prepared by using two step solution-deposition methods3For film as change resistance layer, method is simple, is easy to produce in enormous quantities, especially
It is suitble to commercial Application.
Preferably, in the step B1, a concentration of 12-18 mg/mL of the methanol solution of the CsBr.
Preferably, in the step B2, the speed of spin coating is 3000rpm-4500rpm.
Under above-mentioned concentration and spin speed, can thickness as needed be adjusted, be made uniform CsPbBr3Perovskite
Film.
Preferably, in the step B2, dry condition is：Dry 25-35 min at 70-80 DEG C.
Preferably, in the step B3, the condition of annealing is annealing 1-2 h at 180 DEG C.
Under above-mentioned preparation condition, the CsPbBr that uniform, internal stress fully discharges can be made3Perovskite thin film.
The present invention also provides a kind of applications of multistage resistance-variable storing device as described above.The memory of the present invention has more
The performance of grade resistance-variable storing device, memory window value is big, storage performance stability, easy-regulating, has in non-volatile type memorizer field
There is extensive foreground, about CsPbBr3Perovskite thin film has more resistance states, is applied in non-volatile multistage resistance-variable storing device,
There is no relevant reports at present.
Below by embodiment, the present invention is described in detail.
Embodiment 1
（1）It is cleaned by ultrasonic ito glass, and etches and form ito transparent electrode；Then glass surface is dried up with nitrogen gun, be used in combination true
Empty drying box toasts 30min with 120 DEG C of temperature, then for use with ultraviolet light ozone irradiation 15min.
（2）The CsBr powder of 30mg is dissolved in 2mL methanol, and mixed solution is placed in sealing container and is added
Hot 10min obtains the methanol solution of CsBr.
By the PbBr of 367mg2Dimethylformamide of the powder stirring and dissolving in 1mL（DMF）In solvent, and it is placed on heating
On platform, 5h is heated with 75 DEG C of temperature, the PTFE Materials Filters filtering of 0.22 μm of pore size is then used, obtains PbBr2
Dimethylformamide（DMF）Solution.
（3）By step（1）The preheating glass containing ITO electrode to 75 DEG C, the PbBr that then will prepare2Solution with
The rotating speed of 4000rpm is spin-coated on the electrode surface of glass, spin coating 40s, then dry 30min at a temperature of 75 DEG C.
After drying, glass is contained into PbBr2Face be immersed in 10 min in 50 DEG C of CsBr solution, immediately after at 180 DEG C
Anneal 1.5 h on warm table, forms the CsPbBr of 30nm thickness3Perovskite change resistance layer.
（4）It is 4 × 10 in vacuum degree-4Under conditions of Pa, the silver of 30nm thickness is made by mask in the form of thermal evaporation
Electrode obtains being based on CsPbBr3Multistage resistance-variable storing device.
According to the method described above, CsPbBr is made respectively3Perovskite resistive layer thickness is the control sample of 10 nm and 60 nm.
Performance test
To CsPbBr in embodiment 13Perovskite change resistance layer is that the multistage resistance-variable storing device of 30nm thickness carries out electrical performance testing, such as
Shown in Fig. 2, in different intensities of illumination（L1=0, i.e. no light, L2=0.041, L3=0.069, L4=0.12, L5=0.153 are single
Position is mW/cm2）Under, with the increase of intensity of illumination, apparent variation occurs for the current value of high-impedance state, according to its changing value
Multistage storage may be implemented in multistage variation.
Influence of the resistive layer thickness to the electric property of the multistage resistance-variable storing device of the present invention, as shown in figure 3, resistive thickness
Degree is thicker, and cut-in voltage is bigger, and device energy consumption will increase；Resistive layer thickness is thinner, and cut-in voltage can reduce, and power consumption subtracts
It is few, but if the too thin device that will result in is unstable, corresponding current -voltage curve will be unstable, influences storage performance
Stability.In the multistage resistance-variable storing device of the present invention, CsPbBr3The thickness of perovskite change resistance layer is 25-45 nm（It is preferred that 30
nm）It can get preferable comprehensive performance.
In conclusion the present invention provides a kind of multistage resistance-variable storing device based on inorganic perovskite and preparation method with answer
With, the present invention by CsPbBr3Perovskite thin film is separately as change resistance layer, due to CsPbBr3Perovskite has good photoelectricity special
Property, material high-resistance resistors value can be changed by absorbing the light of different-waveband so that be based on CsPbBr3The multistage of perovskite
There are resistance-variable storing device more resistance states, test to show that its on-off ratio is more than 5000, meet the requirement more than 1000；Compared to traditional oxygen
The material of compound medium is needed using the methods of magnetron sputtering, plasma oxidation, by the present invention in that with two step liquid depositions
Method prepares CsPbBr3For film as change resistance layer, method is simple, is easy to produce in enormous quantities, is particularly suitable for commercial Application；And
CsPbBr3Perovskite thin film applies another discovery that there is multistage resistance-change memory performance to be of the invention in resistance-variable storing device.
It should be understood that the application of the present invention is not limited to the above for those of ordinary skills can
With improvement or transformation based on the above description, all these modifications and variations should all belong to the guarantor of appended claims of the present invention
Protect range.
Claims (10)
1. a kind of multistage resistance-variable storing device, which is characterized in that include successively from bottom to up：Substrate, transparent hearth electrode, CsPbBr3Calcium
Titanium ore change resistance layer and top electrode.
2. multistage resistance-variable storing device according to claim 1, which is characterized in that the CsPbBr3Perovskite change resistance layer
Thickness is 25-45 nm.
3. multistage resistance-variable storing device according to claim 2, which is characterized in that the CsPbBr3Perovskite change resistance layer
Thickness is 30 nm.
4. a kind of preparation method of multistage resistance-variable storing device as described in any one of claims 1-3, which is characterized in that including：
Step A, transparent hearth electrode is made in substrate；
Step B, CsPbBr is made on the transparent hearth electrode3Perovskite change resistance layer；
Step C, in the CsPbBr3Top electrode is made on perovskite change resistance layer, obtains the multistage resistance-variable storing device.
5. the preparation method of multistage resistance-variable storing device according to claim 4, which is characterized in that described in the step B
CsPbBr3Perovskite change resistance layer is prepared by following preparation method：
Step B1, PbBr is prepared respectively2DMF solution and CsBr methanol solution；
Step B2, by the PbBr2DMF solution be spin-coated on the transparent hearth electrode, and it is dry；
Step B3, the sample after drying is contained into PbBr2One side immerse 5-15min in the methanol solution of the CsBr, then take out
And anneal, form CsPbBr3Perovskite change resistance layer.
6. the preparation method of multistage resistance-variable storing device according to claim 5, which is characterized in that in the step B1, institute
State a concentration of 12-18 mg/mL of the methanol solution of CsBr.
7. the preparation method of multistage resistance-variable storing device according to claim 5, which is characterized in that in the step B2, rotation
The speed of painting is 3000rpm-4500rpm.
8. the preparation method of multistage resistance-variable storing device according to claim 5, which is characterized in that in the step B2, do
Dry condition is：Dry 25-35 min at 70-80 DEG C.
9. the preparation method of multistage resistance-variable storing device according to claim 5, which is characterized in that in the step B3, move back
The condition of fire is annealing 1-2 h at 175-185 DEG C.
10. a kind of multistage resistance-variable storing device as described in any one of claims 1-3, which is characterized in that deposited applied to non-volatile
Reservoir field.
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Cited By (5)
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| CN109755391A (en) * | 2018-12-28 | 2019-05-14 | 大连理工大学 | A kind of threshold switching device and preparation method thereof based on organic inorganic hybridization perovskite |
| CN110379921A (en) * | 2019-07-25 | 2019-10-25 | 陕西科技大学 | A kind of flexible multi-state resistive memory and one step solwution method preparation method based on full-inorganic perovskite thin film |
| CN110660912A (en) * | 2019-09-19 | 2020-01-07 | 深圳第三代半导体研究院 | Preparation method of flexible resistive random access memory device based on perovskite |
| CN110707212A (en) * | 2019-08-31 | 2020-01-17 | 郑州大学 | Application of PVAm modified OHP film, polymer perovskite RRAM device and preparation method thereof |
| CN110931634A (en) * | 2018-08-31 | 2020-03-27 | 清华大学 | Resistive device and preparation method and design method thereof |
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| CN108539012A (en) * | 2018-02-28 | 2018-09-14 | 湖北大学 | A kind of full-inorganic perovskite resistance-variable storing device and preparation method thereof |
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Cited By (8)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN110931634A (en) * | 2018-08-31 | 2020-03-27 | 清华大学 | Resistive device and preparation method and design method thereof |
| CN110931634B (en) * | 2018-08-31 | 2022-05-31 | 清华大学 | Resistive device and preparation method and design method thereof |
| CN109755391A (en) * | 2018-12-28 | 2019-05-14 | 大连理工大学 | A kind of threshold switching device and preparation method thereof based on organic inorganic hybridization perovskite |
| CN110379921A (en) * | 2019-07-25 | 2019-10-25 | 陕西科技大学 | A kind of flexible multi-state resistive memory and one step solwution method preparation method based on full-inorganic perovskite thin film |
| CN110379921B (en) * | 2019-07-25 | 2023-03-24 | 陕西科技大学 | Flexible multi-state resistive random access memory based on all-inorganic perovskite thin film and one-step solution method preparation method thereof |
| CN110707212A (en) * | 2019-08-31 | 2020-01-17 | 郑州大学 | Application of PVAm modified OHP film, polymer perovskite RRAM device and preparation method thereof |
| CN110707212B (en) * | 2019-08-31 | 2022-07-26 | 郑州大学 | Application of PVAm modified OHP film, polymer perovskite RRAM device and preparation method thereof |
| CN110660912A (en) * | 2019-09-19 | 2020-01-07 | 深圳第三代半导体研究院 | Preparation method of flexible resistive random access memory device based on perovskite |
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