CN108539019A - Metal organic frame floating gate type organic field effect tube memory and preparation method thereof - Google Patents
Metal organic frame floating gate type organic field effect tube memory and preparation method thereof Download PDFInfo
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- CN108539019A CN108539019A CN201810320467.2A CN201810320467A CN108539019A CN 108539019 A CN108539019 A CN 108539019A CN 201810320467 A CN201810320467 A CN 201810320467A CN 108539019 A CN108539019 A CN 108539019A
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- H10K10/00—Organic devices specially adapted for rectifying, amplifying, oscillating or switching; Organic capacitors or resistors having a potential-jump barrier or a surface barrier
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- H—ELECTRICITY
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- H—ELECTRICITY
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Abstract
The present invention provides a kind of metal organic frame floating gate type organic field effect tube memories and preparation method thereof, the metal organic frame floating gate type organic field effect tube memory includes the source-drain electrode being arranged in order from top to bottom, organic semiconductor layer, floating gate layer, gate insulation layer, substrate and the gate electrode being formed on the substrate, the source-drain electrode is arranged in the surface channel region both sides of the organic semiconductor layer, and the floating gate layer is porphyryl metal organic frame nanometer sheet.The present invention carries out charge storage using porphyryl metal organic frame nanometer sheet as floating gate layer, and no write de-lay, quick storage may be implemented in the ability with fast response characteristic and preferable capture charge, and data keep reliability high, and cost of manufacture is cheap.
Description
Technical field
The present invention relates to a kind of memories, and in particular to a kind of metal organic frame floating gate type organic field effect tube is deposited
Reservoir and preparation method thereof belongs to semicon industry memory technology field.
Background technology
Metal-organic framework materials（MOF）It is that coordinate bond self assembly shape is passed through by organic ligand and metal ion or cluster
At periodically ordered organic-inorganic porous hybrid material, show excellent absorption property, optical property, electromagnetism
Property etc. is widely applied with catalytic field in the storage of sensing, biomedicine, optics, gas with detaching at present.But
It is that MOF is still at an early stage in the application of electronic device especially field of semiconductor memory, only Preliminary Applications are in two poles at present
In pipe memory, transistor and ultracapacitor.
Memory be data processing, communication system important component, wherein organic field effect tube store utensil
There is easy processing, high density, low cost, low-power consumption, can be made into large area and flexibility, is suitble to next generation's wearable electronic production
The research focus in industry developing direction and the field.Organic field effect tube is divided into as ferroelectric type, floating gate type, electret type
Three categories type, wherein floating gate type memory have many advantages, such as low-power consumption, low cost, high storage density and be concerned, in information
Electronic field is with a wide range of applications.Floating gate layer（That is charge storage layer）It is the core of organic field effect tube memory
Unit.Currently, can as floating gate layer material it is more, such as：Inorganic matter（Molybdenum disulfide, graphite alkenes etc.）, organic molecule
（C60、[2-（9-（4-（Octyloxy）Phenyl）- 9H- fluorenes -2- bases）Thiophene]3）, polymer（Seven sugar of malt, polyfluorene）Or composite Nano
Material（Gold nanoparticle and graphene oxide）Deng, but above-mentioned material membrane-film preparation process is complicated, it is difficult to realize quick storage.
Invention content
For the disadvantages described above or Improvement requirement of the prior art, the present invention provides a kind of metal organic frame floating gate types to have
Field effect transistors memory and preparation method thereof, the preparation method is simple for process, easy to operate, and process costs reduce, and fits
In batch production, metal organic frame floating gate type organic field effect tube memory data obtained keeps reliability high.
In order to achieve the above object, the present invention uses following technical scheme：
According to an aspect of the invention, there is provided a kind of metal organic frame floating gate type organic field effect tube memory,
Including be arranged in order from top to bottom source-drain electrode, organic semiconductor layer, floating gate layer, gate insulation layer, substrate and be formed in described
Gate electrode on substrate, the source-drain electrode are arranged in the surface channel region both sides of the organic semiconductor layer, the floating boom
Layer is made of porphyryl metal organic frame nanometer sheet.
Further, metal organic frame floating gate type organic field effect tube memory according to the present invention, the porphin
The chemical composition of quinoline Base Metal organic frame nanometer sheet is four（4- carboxyl phenyls）Porphyrin copper, four（4- carboxyl phenyls）Zinc porphyrin or
Four（4- carboxyl phenyls）Porphyrin cadmium.
Further, metal organic frame floating gate type organic field effect tube memory according to the present invention, the porphin
The thickness of quinoline Base Metal organic frame nanometer sheet is 5nm-10nm, and the thickness of the floating gate layer is 40nm-150nm.
Further, metal organic frame floating gate type organic field effect tube memory according to the present invention, the source
The material of drain electrode is metal, and the thickness of the source-drain electrode is 60nm-100nm.
Further, metal organic frame floating gate type organic field effect tube memory according to the present invention, it is described to have
The material of machine semiconductor layer is pentacene or titan bronze, and the thickness of the organic semiconductor layer is 50nm-70nm.
Further, metal organic frame floating gate type organic field effect tube memory according to the present invention, the grid
The material of insulating layer is silica, aluminium oxide, zirconium oxide, polystyrene or polymethyl methacrylate, and the gate insulation
The thickness of layer is 50nm-300nm.
Further, metal organic frame floating gate type organic field effect tube memory according to the present invention, the grid
The material of electrode is highly doped silicon, aluminium, copper, silver, gold, titanium or tantalum.
Further, metal organic frame floating gate type organic field effect tube memory according to the present invention, the lining
The material at bottom is highly doped silicon, glass or polyethylene terephthalate.
According to another aspect of the present invention, above-mentioned metal organic frame floating gate type organic field effect tube storage is provided
The preparation method of device, includes the following steps：
S1）By nitric hydrate salt, four（4- carboxyl phenyls）Porphyrin and lauryl sodium sulfate are dissolved in N,N-dimethylformamide
With the in the mixed solvent of absolute ethyl alcohol, mixed liquor is put into insulating box, is warming up to 60oC-150oC keeps the temperature 6h-24h, gained is sunk
It forms sediment washing, dry to get to porphyryl metal organic frame nanometer sheet；
S2）The nanometer sheet prepared is dispersed in anhydrous alcohols solvent, dispersion liquid is obtained, dispersion liquid is instilled in water,
The film of one layer of porphyryl metal organic frame nanometer sheet formation is obtained in water surface；
S3）The gate insulation layer that thickness is 50nm-300nm is covered on the gate electrode of substrate, cleaning, drying, and by step S2
The film of formation is transferred on gate insulation layer, is then rinsed with deionized water, and the floating gate layer that thickness is 40nm-150nm is made,
It is dried, and vacuum evaporation organic semiconductor layer and source-drain electrode on floating gate layer, obtains metal organic frame floating gate type
Organic field effect tube memory.
Further, the preparation side of metal organic frame floating gate type organic field effect tube memory according to the present invention
Method, nitric hydrate salt, four in step S1（4- carboxyl phenyls）The molal weight of porphyrin and lauryl sodium sulfate ratio is
0.015mmol−0.02mmol：0.03−0.04mmol：0.005mmol.
Further, the preparation side of metal organic frame floating gate type organic field effect tube memory according to the present invention
Method, the total 16ml of mixed solvent in step S1, wherein n,N-Dimethylformamide and the volume ratio of absolute ethyl alcohol are 3:1.
Compared with the prior art, the present invention has the advantages that：
1. the present invention carries out charge storage using porphyryl metal organic frame nanometer sheet as floating gate layer, there is quick response
The ability of characteristic and preferable capture charge, may be implemented no write de-lay, quick storage, and data keep reliability high, are fabricated to
This is cheap.
2. the preparation side of this metal organic frame floating gate type organic field effect tube memory provided by the invention
Method, simple for process, easy to operate, process costs reduce, and are suitable for batch production.
Description of the drawings
Fig. 1 is the structural representation of one embodiment of the invention metal organic frame floating gate type organic field effect tube memory
Figure.
Fig. 2 is the transfer characteristic curve figure of the embodiment of the present invention 1.
Fig. 3 is the performance diagram that the embodiment of the present invention 1 applies positive negative sense grid voltage memory window.
Fig. 4 is the read-write wiping cycle characteristics curve graph that the embodiment of the present invention 1 applies storage performance after grid voltage.
Fig. 5 is the performance diagram of holding time for the storage performance that the embodiment of the present invention 1 applies grid voltage.
Fig. 6 is that the embodiment of the present invention 2 applies negative sense grid voltage memory window performance diagram.
Fig. 7 is the performance diagram for the negative sense grid voltage memory window that the embodiment of the present invention 2 applies different durations.
Fig. 8 is the performance diagram that the embodiment of the present invention 3 applies negative sense grid voltage memory window.
Specific implementation mode
The present invention is described in further detail with specific embodiment below in conjunction with the accompanying drawings.The embodiment is shown
Example is shown in the accompanying drawings, specific reality of the specific embodiment described in following embodiments of the present invention only as the present invention
Apply the exemplary illustration of mode, it is intended to for explaining the present invention, and be not configured to limitation of the present invention.
Metal organic frame floating gate type organic field effect tube memory as shown in Figure 1 has layer structure, including
Source-drain electrode, organic semiconductor layer, floating gate layer, gate insulation layer, substrate and the gate electrode being arranged in order from top to bottom, wherein grid
Electrode is formed in substrate, and gate insulation layer is covered on gate electrode, and floating gate layer is formed on gate insulation layer, organic partly to lead
Body layer is formed on floating gate layer, and source-drain electrode is arranged in the surface channel region both sides of organic semiconductor layer, wherein floating gate layer
It is made of porphyryl metal organic frame (MOF), including at least one layer of porphyryl metal organic frame nanometer sheet film, the floating boom
The thickness of layer is 40nm-150nm.
The porphyryl metal organic frame nanometer sheet is ultra-thin two-dimension nano material, and single-sheet thickness 5nm-10nm changes
It studies and is divided into four（4- carboxyl phenyls）Porphyrin copper（CuTCPP）, four（4- carboxyl phenyls）Zinc porphyrin（ZnTCPP）Or four（4- carboxyls
Phenyl）Porphyrin cadmium（CdTCPP）, wherein the thickness in monolayer of the porphyryl metal organic frame film thus constituted is 40nm-
50nm。
The thickness of source-drain electrode is 60nm-100nm, and material is selected from metal gold, silver, copper etc., the preparation of the source-drain electrode
Method is magnetron sputtering method, ink-jet printing or vacuum vapour deposition.
The thickness of organic semiconductor layer is 50nm-70nm, and material is pentacene or titan bronze, is preparing metal organic frame
During floating gate type organic field effect tube memory, which is formed a film using thermal vacuum vapour deposition method.
The thickness of gate insulation layer is 50nm-300nm, and material is selected from silica, aluminium oxide, zirconium oxide, polystyrene
Or polymethyl methacrylate.
The material of substrate is highly doped silicon, and as the general material of substrate and gate electrode, highly doped silicon can be integrated with function,
Not only substrate had been made but also had made gate electrode while using.
The present invention provides a kind of above-mentioned preparation sides of metal organic frame floating gate type organic field effect tube memory
Method includes the following steps：
a）By the four of 0.005 mmol（4- carboxyl phenyls）Porphyrin is dissolved in the N,N-dimethylformamide and absolute ethyl alcohol of 4ml
The volume ratio of in the mixed solvent, wherein n,N-Dimethylformamide and absolute ethyl alcohol is 3:1；
b）The lauryl sodium sulfate of the Gerhardite of 0.015mmol-0.02mmol and 0.03mmol-0.04mmol is existed
It is dissolved in the n,N-Dimethylformamide of 12ml and the in the mixed solvent of absolute ethyl alcohol, wherein N, N- bis- under magnetic stirrer stirring
Methylformamide and the volume ratio of absolute ethyl alcohol are 3:1, continue to stir and be added dropwise mixed liquor made from step a, until solution
It stirs evenly, rotating speed is 600 r/min -1200r/min；
c）The mixed liquor of step b is put into insulating box, is warming up to 80oC keeps the temperature 8h, takes out, and the sediment in reaction solution is carried out
Centrifugation is dried, obtains porphyryl metal organic frame nanometer sheet；
d）Above-mentioned freshly prepared porphyryl metal organic frame nanometer sheet is dispersed in anhydrous alcohols, through ultrasound or is shaken
It shakes, so that it is uniformly mixed, form the dispersion liquid of a concentration of 1-5 mg/ml；
e）Appropriate amount of deionized water is taken, and draws dispersion liquid prepared by a little step d and instills in water, can be formed in water surface one layer thin
Film；
f）Substrate is chosen as substrate, and forms gate electrode over the substrate, and is the gate insulation layer of 50nm-300nm by thickness
It is covered on the gate electrode, is then cleaned and dried；
g）The step e films formed are transferred on the substrate of step f, are then rinsed with deionized water, it is 40nm- that thickness, which is made,
The floating gate layer of 150 nm is dried, and vacuum evaporation organic semiconductor layer and source-drain electrode on floating gate layer, obtains metal
Organic frame floating gate type organic field effect tube memory.
Further, the anhydrous alcohols solvent in step d is methanol, ethyl alcohol or other alcohols solvents.
Further, the film forming transfer process in step g is in air
Embodiment 1
A kind of preparation method of metal organic frame floating gate type organic field effect tube memory, includes the following steps：
S1）Configuration concentration is the four of 1mg/ml-5mg/ml（4- carboxyl phenyls）Porphyrin copper（CuTCPP）Nanometer sheet dispersion liquid, and point
It dissipates in ethyl alcohol；
S2）Appropriate amount of deionized water is taken, and the dispersion liquid prepared in step 1 is drawn a little and is instilled in water, water surface is made to be formed
Thin film；
S3）It chooses heavily doped silicon and makes substrate as substrate and gate electrode simultaneously, and cover the titanium dioxide of 300nm over the substrate
Then gate insulation layer is respectively cleaned by ultrasonic 10min, supersonic frequency 100KHz with acetone, ethyl alcohol, deionized water successively, then uses
High pure nitrogen dries up substrate surface liquid to ensure substrate surface cleaning, is put into 120 lateroIt is dried in the baking oven of C；
S4）Substrate after step S3 drying is subjected to UV ozone and handles 5min；
S5）The step S2 films formed are transferred to step S4 UV ozones treated substrate, are then rinsed with deionized water,
The floating gate layer that thickness is 40nm-50nm is made, nitrogen be used in combination that processing is dried, is subsequently placed in 80 DEG C of -120 DEG C of items in glove box
It is dry under part；
S6）The floating gate layer film surface vacuum evaporation pentacene organic semiconductor layer made from step S5, evaporation rate be 1/
S, vacuum degree are 5 × 10-4Pa is hereinafter, it is about 55nm to obtain pentacene organic semiconductor layer thickness；In the organic semiconductor layer table
Face carries out patterned process plus mask plate, and vacuum evaporation gold is as source-drain electrode, 1/s of evaporation rate, the source-drain electrode
Thickness be 60 nm-80 nm；
The channel width of aforementioned mask plate is 2000 μm, and length is 100 μm.
Metal organic frame floating gate type organic field effect tube memory made from preparation method using embodiment 1,
Its electric property is characterized by 4200 semiconductor analysis instrument of Keithley, the transfer curve that data processing is depicted as shown in Fig. 2,
Mobility reaches 0.1cm2/ Vs, on-off ratio is up to 104。
Fig. 3 is positive negative sense storage characteristics transfer curve figure, it can be seen from the figure that the write-in window of device is big, and is write
The angle of incidence can be written in 0.02s compared with big window, show that the memory has good response characteristic.
Write-in-reading-erasing-reading performance data also indicates that the memory has preferable repeatedly erasable ability in Fig. 4,
After the erasable cycle of some cycles, the erasable window of device does not change substantially.
Fig. 5 indicates the data holding ability of the memory, as can be seen from the figure passes through after 10000s, storage switch ratio
10 or more are remained in, illustrates that the memory reliability of memory is higher.
Embodiment 2
A kind of preparation method of metal organic frame floating gate type organic field effect tube memory, wherein step S1-S6 with
The corresponding steps of above-described embodiment a are identical, and transfer is repeated in step S5 twice, are co-deposited three layers of CuTCPP nanometer sheet films,
Obtained floating boom layer thickness is 120 nm-150 nm.
In the technical solution of the present embodiment, heavily doped silicon is as substrate and gate electrode；The silica of one layer of 300nm is made
For gate insulation layer；Floating gate layer is by three layer four（4- carboxyl phenyls）Porphyrin-copper（CuTCPP）The film layer that nanometer sheet is formed is constituted, and is floated
Grid layer thickness is 120nm-150 nm；The pentacene of one layer of 50nm-70nm thickness is deposited above floating gate layer as organic semiconductor layer；
Again in its conducting channel both sides evaporation metal gold as source-drain electrode, alcohols solvent is ethyl alcohol.
Metal organic frame floating gate type organic field effect tube memory made from preparation method using embodiment 2,
Fig. 6 is the memory negative sense storage characteristics transfer curve figure, and Fig. 7 is memory negative sense storage characteristics under the different write times
Curve graph, it can be seen from the figure that the write-in window of device is big, and the write time is in 0.02s and the memory window in 1s
Quite, and write-in window is larger, shows the ability that the memory has quickly write-in response characteristic and preferable capture charge.
Embodiment 3
A kind of preparation method of metal organic frame floating gate type organic field effect tube memory, wherein step S1-S6 with
The corresponding steps of above-described embodiment a are identical, using phthalocyanine bronze as organic semiconductor layer in only step S6.
In the technical solution of the present embodiment, heavily doped silicon is as substrate and gate electrode；The silica of one layer of 300nm is made
For gate insulation layer；Floating gate layer is by one layer four（4- carboxyl phenyls）Porphyrin-copper（CuTCPP）The film layer that nanometer sheet is formed is constituted, thick
Degree is 120nm-150nm；The phthalocyanine bronze of one layer of 50nm-70nm thickness is deposited above floating gate layer as organic semiconductor layer；Again at it
For conducting channel both sides evaporation metal gold as source-drain electrode, alcohols solvent is ethyl alcohol.
Metal organic frame floating gate type organic field effect tube memory made from preparation method using embodiment 3,
Fig. 8 is the memory negative sense storage characteristics transfer curve figure, larger deposit also occurs in the case where 0.02s is written in negative sense 50V
Window is stored up, the ability that memory has fast response characteristic and preferable capture charge is embodied.
In conclusion metal organic frame floating gate type organic field effect tube memory provided by the invention, using porphin
Quinoline Base Metal organic frame nanometer sheet carries out charge storage as floating gate layer, and no write de-lay, quick storage may be implemented, and has fast
The ability of fast response characteristic and preferable capture charge, while data keep reliability height, storage stability good, it is of low cost；
In addition, a kind of preparation method of metal organic frame floating gate type organic field effect tube memory provided by the invention, technique
Simply, easy to operate, process costs reduce, and are suitable for batch production.
It should be noted that above-described embodiment is that the present invention will be described rather than limits the invention, and
Those skilled in the art can design alternative embodiment without departing from the scope of the appended claims.In claim
In, word "comprising" does not exclude the presence of data or step not listed in the claims.
Claims (11)
1. a kind of metal organic frame floating gate type organic field effect tube memory, including the source and drain that is arranged in order from top to bottom
Electrode, organic semiconductor layer, floating gate layer, gate insulation layer, substrate and the gate electrode being formed on the substrate, the source-drain electrode
It is arranged in the surface channel region both sides of the organic semiconductor layer, it is characterised in that：The floating gate layer is had by porphyrin Base Metal
Machine frame nanometer sheet forms.
2. metal organic frame floating gate type organic field effect tube memory according to claim 1, it is characterised in that：
The chemical composition of the porphyryl metal organic frame nanometer sheet is four（4- carboxyl phenyls）Porphyrin copper, four（4- carboxyl phenyls）Porphin
Quinoline zinc or four（4- carboxyl phenyls）Porphyrin cadmium.
3. metal organic frame floating gate type organic field effect tube memory according to claim 2, it is characterised in that：
The thickness of the porphyryl metal organic frame nanometer sheet is 5nm-10nm, and the thickness of the floating gate layer is 40nm-150nm.
4. metal organic frame floating gate type organic field effect tube memory according to claim 1, it is characterised in that：
The material of the source-drain electrode is metal, and the thickness of the source-drain electrode is 60nm-100nm.
5. metal organic frame floating gate type organic field effect tube memory according to claim 1, it is characterised in that：
The material of the organic semiconductor layer is pentacene or phthalein cyanogen copper, and the thickness of the organic semiconductor layer is 50nm-70nm.
6. metal organic frame floating gate type organic field effect tube memory according to claim 1, it is characterised in that：
The material of the gate insulation layer is silica, aluminium oxide, zirconium oxide, polystyrene or polymethyl methacrylate, and described
The thickness of gate insulation layer is 50nm-300nm.
7. metal organic frame floating gate type organic field effect tube memory according to claim 1, it is characterised in that：
The material of the gate electrode is highly doped silicon, aluminium, copper, silver, gold, titanium or tantalum.
8. metal organic frame floating gate type organic field effect tube memory according to claim 1, it is characterised in that：
The material of the substrate is highly doped silicon, glass or polyethylene terephthalate.
9. the preparation method of metal organic frame floating gate type organic field effect tube memory according to claim 1,
It is characterized in that, method includes the following steps：
S1）By nitric hydrate salt, four（4- carboxyl phenyls）Porphyrin and lauryl sodium sulfate are dissolved in N,N-dimethylformamide
With the in the mixed solvent of absolute ethyl alcohol, mixed liquor is put into insulating box, is warming up to 60oC-150oC keeps the temperature 6h-24h, gained is sunk
It forms sediment washing, dry to get to porphyryl metal organic frame nanometer sheet；
S2）The porphyryl metal organic frame nanometer sheet prepared is dispersed in anhydrous alcohols solvent, is obtained a concentration of
Dispersion liquid is instilled in water, i.e., obtains one layer of porphyryl metal organic frame in water surface and receive by the dispersion liquid of 1mg/ml-5mg/ml
The film that rice piece is formed；
S3）The gate insulation layer that thickness is 50nm-300nm is covered on the gate electrode of substrate, cleaning, drying, and by step S2
The film of formation is transferred on gate insulation layer, is then rinsed with deionized water, and the floating gate layer that thickness is 40nm-150nm is made,
It is dried, and vacuum evaporation organic semiconductor layer and source-drain electrode on floating gate layer, obtains metal organic frame floating gate type
Organic field effect tube memory.
10. the preparation method of metal organic frame floating gate type organic field effect tube memory according to claim 9,
It is characterized in that：Nitric hydrate salt, four in step S1（4- carboxyl phenyls）The molal weight of porphyrin and lauryl sodium sulfate ratio
For 0.015mmol 0.02mmol：0.03−0.04mmol：0.005mmol.
11. the preparation method of metal organic frame floating gate type organic field effect tube memory according to claim 9,
It is characterized in that：The total 16ml of mixed solvent in step S1, wherein n,N-Dimethylformamide and the volume ratio of absolute ethyl alcohol are 3:
1。
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| CN110964052B (en) * | 2019-12-23 | 2022-08-05 | 南京和颂材料科技有限公司 | Storage property of organic functional material containing terminal aldehyde group |
| JP7359793B2 (en) | 2020-04-21 | 2023-10-11 | トヨタ自動車株式会社 | Field effect transistor, gas sensor, and manufacturing method thereof |
| CN111696856A (en) * | 2020-06-29 | 2020-09-22 | 济南大学 | Full-covalent-bond graphene field effect transistor and construction method thereof |
| CN111696856B (en) * | 2020-06-29 | 2022-08-23 | 济南大学 | Full-covalent-bond graphene field effect transistor and construction method thereof |
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| CN116390607B (en) * | 2023-03-17 | 2023-10-20 | 天津大学 | Method for improving photoelectric performance of transistor |
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Application publication date: 20180914 |