CN106328809A - Volatile and nonvolatile hybrid memory and its preparation method - Google Patents
Volatile and nonvolatile hybrid memory and its preparation method Download PDFInfo
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- CN106328809A CN106328809A CN201610862100.4A CN201610862100A CN106328809A CN 106328809 A CN106328809 A CN 106328809A CN 201610862100 A CN201610862100 A CN 201610862100A CN 106328809 A CN106328809 A CN 106328809A
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- 230000015654 memory Effects 0.000 title claims abstract description 39
- 238000002360 preparation method Methods 0.000 title claims abstract description 27
- 238000003860 storage Methods 0.000 claims abstract description 45
- 238000000034 method Methods 0.000 claims abstract description 30
- 239000000758 substrate Substances 0.000 claims abstract description 19
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical group [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 27
- 229910021389 graphene Inorganic materials 0.000 claims description 19
- 238000002156 mixing Methods 0.000 claims description 18
- 230000008569 process Effects 0.000 claims description 16
- 229920000144 PEDOT:PSS Polymers 0.000 claims description 15
- 239000000243 solution Substances 0.000 claims description 10
- 238000004528 spin coating Methods 0.000 claims description 10
- IAZDPXIOMUYVGZ-UHFFFAOYSA-N Dimethylsulphoxide Chemical compound CS(C)=O IAZDPXIOMUYVGZ-UHFFFAOYSA-N 0.000 claims description 9
- 239000010408 film Substances 0.000 claims description 8
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N silicon dioxide Inorganic materials O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 8
- 239000007921 spray Substances 0.000 claims description 8
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 8
- 239000002322 conducting polymer Substances 0.000 claims description 7
- 229920001940 conductive polymer Polymers 0.000 claims description 7
- CSCPPACGZOOCGX-UHFFFAOYSA-N Acetone Chemical compound CC(C)=O CSCPPACGZOOCGX-UHFFFAOYSA-N 0.000 claims description 6
- 239000008367 deionised water Substances 0.000 claims description 6
- 229910021641 deionized water Inorganic materials 0.000 claims description 6
- 238000005507 spraying Methods 0.000 claims description 6
- 239000007864 aqueous solution Substances 0.000 claims description 5
- 238000004140 cleaning Methods 0.000 claims description 5
- 229910002804 graphite Inorganic materials 0.000 claims description 5
- 239000010439 graphite Substances 0.000 claims description 5
- 239000010409 thin film Substances 0.000 claims description 5
- VEXZGXHMUGYJMC-UHFFFAOYSA-N Hydrochloric acid Chemical compound Cl VEXZGXHMUGYJMC-UHFFFAOYSA-N 0.000 claims description 4
- MHAJPDPJQMAIIY-UHFFFAOYSA-N Hydrogen peroxide Chemical compound OO MHAJPDPJQMAIIY-UHFFFAOYSA-N 0.000 claims description 4
- 229910052799 carbon Inorganic materials 0.000 claims description 4
- 239000007787 solid Substances 0.000 claims description 4
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 3
- 230000005611 electricity Effects 0.000 claims description 3
- 239000007772 electrode material Substances 0.000 claims description 3
- 229910021642 ultra pure water Inorganic materials 0.000 claims description 3
- 239000012498 ultrapure water Substances 0.000 claims description 3
- 238000004506 ultrasonic cleaning Methods 0.000 claims description 3
- 238000001291 vacuum drying Methods 0.000 claims description 3
- 230000008859 change Effects 0.000 claims description 2
- 229960000935 dehydrated alcohol Drugs 0.000 claims description 2
- 239000008187 granular material Substances 0.000 claims description 2
- 239000005457 ice water Substances 0.000 claims description 2
- 239000012528 membrane Substances 0.000 claims description 2
- 238000000059 patterning Methods 0.000 claims description 2
- 239000012286 potassium permanganate Substances 0.000 claims description 2
- 239000010453 quartz Substances 0.000 claims description 2
- 239000004065 semiconductor Substances 0.000 abstract description 7
- 238000011161 development Methods 0.000 abstract description 5
- 238000005516 engineering process Methods 0.000 abstract description 2
- 230000007334 memory performance Effects 0.000 abstract 1
- 238000012360 testing method Methods 0.000 description 7
- 239000000463 material Substances 0.000 description 4
- 230000006870 function Effects 0.000 description 3
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- 238000013461 design Methods 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 238000003756 stirring Methods 0.000 description 2
- 238000009825 accumulation Methods 0.000 description 1
- 150000001336 alkenes Chemical class 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 239000011248 coating agent Substances 0.000 description 1
- 238000000576 coating method Methods 0.000 description 1
- 230000009977 dual effect Effects 0.000 description 1
- 239000012530 fluid Substances 0.000 description 1
- 238000010438 heat treatment Methods 0.000 description 1
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- 229910052757 nitrogen Inorganic materials 0.000 description 1
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- 230000000737 periodic effect Effects 0.000 description 1
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- 229920006254 polymer film Polymers 0.000 description 1
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- 239000004575 stone Substances 0.000 description 1
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- 238000002834 transmittance Methods 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 without a potential-jump barrier or surface barrier, and specially adapted for rectifying, amplifying, oscillating or switching
- H10N70/20—Multistable switching devices, e.g. memristors
-
- 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
-
- 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
- H10N70/841—Electrodes
-
- 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
Abstract
The invention discloses a volatile and nonvolatile hybrid memory and its preparation method. The multifunctional memory comprises a substrate, a bottom electrode, a storage active layer and a top electrode. The bottom electrode is arranged on the surface of the substrate; the storage active layer is arranged between the crossed bottom electrode and the top electrode. The preparation method comprises the following steps: 1) preparing a bottom electrode through a wet method; 2) preparing a storage active layer on the bottom electrode through a wet method; and 3) preparing a top electrode on the middle layer through a wet method. The volatile and nonvolatile hybrid memory of the invention has a unique volatile and nonvolatile hybrid memory performance, relatively high transparency, fine durability and reliability and all-wet preparation characteristics, blazing a new path for the development of semiconductor science and technology in post-Moore era.
Description
Technical field
The present invention relates to novel semi-conductor technical field, be specifically related to a kind of volatile and nonvolatile mixing memory and
Its preparation method.
Technical background
Along with the arrival in " big data " epoch, magnanimity information occurs in our life, meanwhile these magnanimity letter
The storage of breath becomes a major challenge that Development of storage technology faces, and seeks more large storage capacity, faster read or write speed, more convenient
Use, less expensive cost and higher environmental-protecting performance, become the certainty of memorizer development under current " big data " background
Trend.
Memorizer according to its storage class difference can be divided into volatibility (volatile) store with non-volatile
(non-volatile) storage, wherein volatile storage can lose the data stored after device power-off, and non-volatile
Storage then will not lose the most stored data because of the power-off of device.Volatile storage mainly includes SRAM
(SRAM) with dynamic RAM (DRAM) two class, SRAM needs persistently to power it without refreshing with regard to energy
Keeping its storage state, SRAM has the response speed that is exceedingly fast but its cost is the highest, therefore static with
Machine storage is used for the cache of computer, and dynamic RAM then needs to use dynamic discontinuous voltage or pulse electricity
Stream carries out periodic refresh to maintain the storage state of data to it.Non-volatile memories mainly includes that write-once repeatedly reads
And flash memory (Flash) the most repeatable erasable (Rewritable) two class (WORM).Write-once repeatedly reads the characteristic of memorizer
Ensure that its data stored will not be lost because of unexpected generation or be modified, its be commonly used for achieving significant data or
Radio-frequency (RF) tag field.Flush memory device has a repeatable erasable nonvolatile memory as a kind of, the hardest at computer
Disk storage and flash disk storage are widely applied.
Number of patent application is 201110302115.2, entitled " nonvolatile semiconductor memory member and nonvolatile semiconductor memory member
Manufacture method ", be the patent of Sony corporation of Japan application, it discloses a kind of information that can suppress and cause due to Joule heat
The intensification of accumulation layer, it is possible to the generation of interference phenomenon is read in suppression.But it remains single memory device.
" More Than Moore " storage is the Main way of current research semiconductor science development, and function is many among these
Sample is one of its principal character.Legacy memory focuses primarily upon in the realization of simple function device, during along with " rear mole "
The arriving in generation, traditional simple function memorizer the most increasingly cannot meet the use demand of people, so, design preparation is many
Functional memory becomes a urgent problem in current semiconductor scientific development.
Summary of the invention
The above-mentioned challenge run in view of legacy memory, present invention is primarily targeted at and propose a kind of multi-functional deposit
The mentality of designing of memory device and preparation method.Memorizer prepared by the method can collect volatile and nonvolatile two kinds of storage merits
Can be in one, and memorizer has and can prepare by Whote-wet method, and read false rate is low, and durability is good, high reliability.
The technical solution adopted in the present invention is as follows: volatile and nonvolatile mixing Multifunctional memory, including substrate,
Hearth electrode, storage active layer and top electrode, described hearth electrode is positioned at substrate surface, and described storage active layer is positioned at the end electricity of intersection
Between pole and top electrode.
Substrate is transparency silica glass, and hearth electrode is positioned at transparent Quartz glass surfaces；Hearth electrode with top electrode is
The polymer patterning thin film of PEDOT:PSS；Storage active layer is graphene oxide film.
The preparation method of volatile and nonvolatile mixing Multifunctional memory, comprises the following steps:
(1) on base material, hearth electrode is prepared by wet spray；
(2) preparation activity storage active layer thin film it is spin-coated on described hearth electrode by wet method；
(3) in active intermediate, the top electrode with hearth electrode square crossing is prepared by wet spray.
Step (1) described base material is quartz glass, and the cleaning of substrate uses ultra-pure water, anhydrous alcohol, acetone respectively
Ultrasonic cleaning 15 minutes, then dried up by nitrogen.
Step (1) and step (3) described hearth electrode are PEDOT:PSS conducting polymer aqueous solution with top electrode material, molten
Fluid solid content is the DMSO in 1.2wt%, and solution doped with 4wt%.
Step (1) is 100 DEG C with the heating-up temperature of substrate in step (3) described wet spray, and has sprayed at electrode
Rear continuation heats 1 hour to solidify PEDOT:PSS thin polymer film.
Step (2) described activity intermediate storage layer membrane materials is graphene oxide, and this graphene oxide is by expanded graphite
Prepared by Hummer ' s method.
In step (2) described spin-coating method, spin coating rotating speed is 2000rpm, and spin coating gained graphene oxide film need to be placed in 40
DEG C vacuum drying oven is dried 30min.
Beneficial effect
Technical scheme design memorizer has volatile and nonvolatile dual memory characteristic；And use complete
Wet method prepares memory device, and step is simple；Memorizer possesses the excellent transparency, the volatile and nonvolatile storage prepared
Device light transmittance reaches 60～70%；It has high stability and repeatability, the non-volatile and volatile storage process of memorizer
Switch current ratio respectively up to 104With 102, wherein the durability of non-volatile memory process is up to 104More than Miao, volatibility is deposited
The cycle-index of storage process reaches 103More than secondary.
Accompanying drawing explanation
Fig. 1. Multifunctional memory part structural representation.
Fig. 2. storage volatility and the I-V relation curve of non-volatile memories process.
Fig. 3. memorizer non-volatile memories process durability test curve.
Fig. 4. storage volatility storing process durability test curve.
Detailed description of the invention
In order to be more fully understood that the content of patent of the present invention, further illustrate below by instantiation.But these are real
Executing example and be not limiting as the present invention, those skilled in the art make some nonessential improvement and tune according to the content of foregoing invention
Whole, belong to scope.
As it is shown in figure 1, the structure of volatile and nonvolatile mixing Multifunctional memory includes substrate, hearth electrode, storage
Active layer and top electrode；It is followed successively by substrate, hearth electrode, storage active layer, top electrode from the bottom to top.
Substrate uses quartz glass substrate, and hearth electrode is PEDOT:PSS conducting polymer thin film, and storage active layer is oxidation
Graphene film, top electrode is PEDOT:PSS conducting polymer thin film.
The preparation method of volatile and nonvolatile mixing Multifunctional memory, comprises the following steps:
(1) hearth electrode is prepared by PEDOT:PSS aqueous solution on a quartz substrate by wet spray；
(2) preparation storage active layer it is spin-coated on described hearth electrode by graphite oxide enolate solution by wet method；
(3) on storage active layer, top electrode is prepared by wet spray by PEDOT:PSS aqueous solution.
Performance to the volatile and nonvolatile mixing Multifunctional memory using said method to prepare, is analyzed,
As in Figure 2-4:
As in figure 2 it is shown, by the I-V relation curve of storage volatility and non-volatile memories process it will be seen that when execute
When adding negative sense scanning voltage, there is ascendant trend drastically in electric current, shows that, when 0～-3V, first device presents " low-resistance
State ".When we continue to strengthen scanning voltage, significantly declining occurs in electric current, and shows that device is changed into " high resistant by low resistance state
State ".Electric current is by 1.22 × 10-4A is reduced to 1.01 × 10-8A, " write " process of the i.e. memorizer of this process." write " it
After, scanning voltage is during-10V to+10V, and the electric current of memorizer is always held at reduced levels.This process is device
The non-volatile memories process of part, the data now " write " in memorizer can not be modified again, shows that memorizer is pacified in information
Full field has potential using value.But when scanning voltage is reduced to 0V from+10V, electric current is from 1.08 × 10-8A is reduced to
2.69×10-12A, now device presents relative " low resistance state ", and we have found that when scanning voltage increases to-10V again,
Device becomes relatively " high-impedance state " again, when we apply scan round voltage, and the storage performance all-the-time stable of device, table
Reveal typical volatile storage feature.From the point of view of this performance test, the memorizer of the present invention has volatibility and non-volatile
The double characteristic of storage.
As it is shown on figure 3, be memorizer non-volatile memories process durability test curve, when we are to device applying-2V
Pulse test voltage time, it has been found that 104After Miao, " low resistance state " and " high-impedance state " electric current of device substantially remains in same number
Magnitude and do not occur significantly decaying, indicate non-volatile memory process and there is good durability.
As shown in Figure 4, for storage volatility storing process durability test curve, we have carried out 1000 times to device
Loop test, and the electric current of device during 2V is carried out statistical analysis, find that the switch current ratio of device does not occurs substantially to become all the time
Change, indicate volatile storage process and there is good durability.
Further by the detailed elaboration graphene oxide active intermediate of two embodiments and carbon back Multifunctional memory
Part preparation method.
Embodiment 1: the preparation method of graphene oxide active intermediate.
Prepared by graphene oxide: by 2g expanded graphite, 1g NaNO3、6g KMnO4H dense with 46ml2SO4In ice-water bath condition
Stir 30 minutes after lower mixing, be then heated to 35 DEG C and continuously stirred 8 hours.Add the ultra-pure water of 92ml 40 DEG C afterwards, hold
System is also heated to 95 DEG C by continuous stirring, reacts 15 minutes.It is eventually adding deionized water and the 20ml hydrogen peroxide of 280ml 40 DEG C.
Being cooled to room temperature, by 5wt% aqueous hydrochloric acid solution eccentric cleaning 3 times, then this is by deionized water eccentric cleaning 5 times, obtains aoxidizing stone
Ink alkene.
Prepared by graphene oxide intermediate active layer: the graphene oxide water solution of preparation 0.05mg/ml, ultrasonic disperse 1 point
Clock, the very small amount sheet granule during then 3000rpm is centrifuged off solution.During spin-coating film, the rotating speed of spin coating instrument is
2000rpm, spin coating gained graphene oxide film need to be placed in 40 DEG C of vacuum drying ovens and be dried 30 minutes.
Embodiment 2: the preparation method of carbon back Multifunctional memory part
Quartz glass substrate after deionized water, dehydrated alcohol and acetone ultrasonic cleaning, pattern mask version in covering,
Prepare hearth electrode by hot spraying method, electrode material be solid content be the PEDOT:PSS conducting polymer of 1.2wt%, and mix
The miscellaneous DMSO having 4wt%.During spraying, the heating-up temperature of substrate is 100 DEG C, continues the PEDOT:PSS that heating 1 hour is after spraying
Electrode is fully cured.After hearth electrode prepares, prepare graphene oxide active intermediate by spin-coating method, finally by adding thermal jet
Coating prepares top electrode, obtains Multifunctional memory based on material with carbon element, and the performance of device has Semiconductor Parameter Analyzer to test
Obtain.
Claims (9)
- The most volatile and nonvolatile mixing Multifunctional memory, it is characterised in that: described Multifunctional memory includes substrate, the end Electrode, storage active layer and top electrode；Described hearth electrode is positioned at substrate surface, and described storage active layer is positioned at the hearth electrode of intersection And between top electrode.
- Volatile and nonvolatile mixing Multifunctional memory the most according to claim 1, it is characterised in that: electricity of the described end Pole and top electrode are PEDOT:PSS conducting polymer thin film.
- Volatile and nonvolatile mixing Multifunctional memory the most according to claim 1, it is characterised in that: described storage Active layer is graphene oxide film.
- The preparation method of volatile and nonvolatile mixing Multifunctional memory the most according to claim 1, including as follows Step:(1) hearth electrode is prepared by PEDOT:PSS aqueous solution on a quartz substrate by wet spray；(2) preparation storage active layer it is spin-coated on described hearth electrode by graphite oxide enolate solution by wet method；(3) on storage active layer, top electrode is prepared by wet spray by PEDOT:PSS aqueous solution.
- The preparation method of volatile and nonvolatile mixing Multifunctional memory the most according to claim 4, its feature exists In: described step (1) and the hearth electrode in step (3) they are cross one another patterning PEDOT:PSS conducting polymer with top electrode Thing membrane electrode.
- The preparation method of volatile and nonvolatile mixing Multifunctional memory the most according to claim 5, its feature exists In: the preparation process of described hearth electrode is as follows:A. quartz glass substrate is after deionized water, dehydrated alcohol and acetone ultrasonic cleaning, pattern mask version in covering；B. prepare hearth electrode by hot spraying method, electrode material be solid content be the PEDOT:PSS conducting polymer of 1.2wt% Thing, and doped with the DMSO of 4wt%；C. during spraying, the heating-up temperature of substrate is 100 DEG C, continues to heat the PEDOT:PSS electrode 1 hour being the most solid after spraying Change.
- The preparation method of volatile and nonvolatile mixing Multifunctional memory the most according to claim 5, its feature exists In: the preparation process of described top electrode is as follows: after prepared by hearth electrode, graphene oxide storage active layer, finally by adding Hot spray process prepares top electrode at storage active layer.
- The preparation method of volatile and nonvolatile mixing Multifunctional memory the most according to claim 4, its feature exists In: graphene oxide preparation process is as follows:A. by 2g expanded graphite, 1g NaNO3、6g KMnO4H dense with 46ml2SO430 points are stirred after mixing under the conditions of ice-water bath Clock, is then heated to 35 DEG C and continuously stirred 8 hours；B. the ultra-pure water of 92ml 40 DEG C is added, continuously stirred and system is heated to 95 DEG C, react 15 minutes；C. add deionized water and the 20ml hydrogen peroxide of 280ml 40 DEG C, be cooled to room temperature；D. use 5wt% aqueous hydrochloric acid solution eccentric cleaning 3 times, then this uses deionized water eccentric cleaning 5 times, obtains graphene oxide.
- The preparation method of volatile and nonvolatile mixing Multifunctional memory the most according to claim 4, its feature exists In: graphene oxide intermediate active layer preparation process is as follows:A. the graphene oxide water solution of 0.05mg/ml, ultrasonic disperse 1 minute are prepared；B.3000rpm the very small amount sheet granule being centrifuged off in solution；C. spin-coating film, the rotating speed of spin coating instrument is 2000rpm, and spin coating gained graphene oxide film need to be placed in 40 DEG C of vacuum drying Case is dried 30 minutes.
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| CN108447989A (en) * | 2018-02-28 | 2018-08-24 | 武汉工程大学 | Single polymer layer electrical storage based on electrical bistable property and its manufacturing method |
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|---|---|---|---|---|
| CN101083300A (en) * | 2006-06-02 | 2007-12-05 | 三星电子株式会社 | Organic memory devices including organic material and fullerene layers and related methods |
| CN101599530A (en) * | 2009-06-24 | 2009-12-09 | 中国科学院宁波材料技术与工程研究所 | Memory cell of a kind of resistive random access memory (RRAM) and preparation method thereof |
| CN105914047A (en) * | 2016-04-14 | 2016-08-31 | 南京邮电大学 | Flexible transparent thin-film electrode and manufacturing method thereof |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN101083300A (en) * | 2006-06-02 | 2007-12-05 | 三星电子株式会社 | Organic memory devices including organic material and fullerene layers and related methods |
| CN101599530A (en) * | 2009-06-24 | 2009-12-09 | 中国科学院宁波材料技术与工程研究所 | Memory cell of a kind of resistive random access memory (RRAM) and preparation method thereof |
| CN105914047A (en) * | 2016-04-14 | 2016-08-31 | 南京邮电大学 | Flexible transparent thin-film electrode and manufacturing method thereof |
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| CN108447989A (en) * | 2018-02-28 | 2018-08-24 | 武汉工程大学 | Single polymer layer electrical storage based on electrical bistable property and its manufacturing method |
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