CN104821373A - High-performance organic field effect transistor with double-layer modification, and modification method thereof - Google Patents
High-performance organic field effect transistor with double-layer modification, and modification method thereof Download PDFInfo
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- 238000012986 modification Methods 0.000 title abstract description 8
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- 238000002715 modification method Methods 0.000 title abstract 2
- 229920000642 polymer Polymers 0.000 claims abstract description 43
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims abstract description 34
- 239000004065 semiconductor Substances 0.000 claims abstract description 31
- 239000000758 substrate Substances 0.000 claims abstract description 18
- 239000000377 silicon dioxide Substances 0.000 claims abstract description 17
- 229910052710 silicon Inorganic materials 0.000 claims abstract description 12
- 239000010703 silicon Substances 0.000 claims abstract description 12
- 235000012239 silicon dioxide Nutrition 0.000 claims abstract description 12
- ZMANZCXQSJIPKH-UHFFFAOYSA-N Triethylamine Chemical group CCN(CC)CC ZMANZCXQSJIPKH-UHFFFAOYSA-N 0.000 claims description 36
- 229920001665 Poly-4-vinylphenol Polymers 0.000 claims description 35
- 238000004528 spin coating Methods 0.000 claims description 32
- 238000000034 method Methods 0.000 claims description 30
- 229920003229 poly(methyl methacrylate) Polymers 0.000 claims description 28
- 239000004926 polymethyl methacrylate Substances 0.000 claims description 28
- 239000010410 layer Substances 0.000 claims description 27
- XEKOWRVHYACXOJ-UHFFFAOYSA-N Ethyl acetate Chemical compound CCOC(C)=O XEKOWRVHYACXOJ-UHFFFAOYSA-N 0.000 claims description 21
- 238000001704 evaporation Methods 0.000 claims description 19
- 230000008020 evaporation Effects 0.000 claims description 19
- LLHKCFNBLRBOGN-UHFFFAOYSA-N propylene glycol methyl ether acetate Chemical group COCC(C)OC(C)=O LLHKCFNBLRBOGN-UHFFFAOYSA-N 0.000 claims description 17
- 238000007738 vacuum evaporation Methods 0.000 claims description 17
- SLIUAWYAILUBJU-UHFFFAOYSA-N pentacene Chemical compound C1=CC=CC2=CC3=CC4=CC5=CC=CC=C5C=C4C=C3C=C21 SLIUAWYAILUBJU-UHFFFAOYSA-N 0.000 claims description 16
- 230000004888 barrier function Effects 0.000 claims description 15
- 239000013078 crystal Substances 0.000 claims description 14
- XNGIFLGASWRNHJ-UHFFFAOYSA-N phthalic acid Chemical compound OC(=O)C1=CC=CC=C1C(O)=O XNGIFLGASWRNHJ-UHFFFAOYSA-N 0.000 claims description 14
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 claims description 12
- 239000010931 gold Substances 0.000 claims description 12
- 229910052737 gold Inorganic materials 0.000 claims description 12
- 239000003431 cross linking reagent Substances 0.000 claims description 10
- 239000003054 catalyst Substances 0.000 claims description 9
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- 239000013047 polymeric layer Substances 0.000 claims description 8
- 239000004372 Polyvinyl alcohol Substances 0.000 claims description 7
- 150000008064 anhydrides Chemical class 0.000 claims description 7
- 229920002451 polyvinyl alcohol Polymers 0.000 claims description 7
- 239000004793 Polystyrene Substances 0.000 claims description 6
- 229920002223 polystyrene Polymers 0.000 claims description 4
- 125000001731 2-cyanoethyl group Chemical group [H]C([H])(*)C([H])([H])C#N 0.000 claims description 3
- 239000004373 Pullulan Substances 0.000 claims description 3
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- 235000019423 pullulan Nutrition 0.000 claims description 3
- 238000001035 drying Methods 0.000 claims description 2
- JBTWLSYIZRCDFO-UHFFFAOYSA-N ethyl methyl carbonate Chemical compound CCOC(=O)OC JBTWLSYIZRCDFO-UHFFFAOYSA-N 0.000 claims description 2
- 239000000178 monomer Substances 0.000 claims description 2
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- 238000012546 transfer Methods 0.000 description 12
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- CSCPPACGZOOCGX-UHFFFAOYSA-N Acetone Chemical compound CC(C)=O CSCPPACGZOOCGX-UHFFFAOYSA-N 0.000 description 10
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- 229910021641 deionized water Inorganic materials 0.000 description 5
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- UQEAIHBTYFGYIE-UHFFFAOYSA-N hexamethyldisiloxane Chemical compound C[Si](C)(C)O[Si](C)(C)C UQEAIHBTYFGYIE-UHFFFAOYSA-N 0.000 description 2
- 125000004356 hydroxy functional group Chemical group O* 0.000 description 2
- 239000002094 self assembled monolayer Substances 0.000 description 2
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K10/00—Organic devices specially adapted for rectifying, amplifying, oscillating or switching; Organic capacitors or resistors having potential barriers
- H10K10/40—Organic transistors
- H10K10/46—Field-effect transistors, e.g. organic thin-film transistors [OTFT]
- H10K10/462—Insulated gate field-effect transistors [IGFETs]
- H10K10/468—Insulated gate field-effect transistors [IGFETs] characterised by the gate dielectrics
- H10K10/474—Insulated gate field-effect transistors [IGFETs] characterised by the gate dielectrics the gate dielectric comprising a multilayered structure
- H10K10/476—Insulated gate field-effect transistors [IGFETs] characterised by the gate dielectrics the gate dielectric comprising a multilayered structure comprising at least one organic layer and at least one inorganic layer
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K10/00—Organic devices specially adapted for rectifying, amplifying, oscillating or switching; Organic capacitors or resistors having potential barriers
- H10K10/40—Organic transistors
- H10K10/46—Field-effect transistors, e.g. organic thin-film transistors [OTFT]
- H10K10/462—Insulated gate field-effect transistors [IGFETs]
- H10K10/491—Vertical transistors, e.g. vertical carbon nanotube field effect transistors [CNT-FETs]
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K10/00—Organic devices specially adapted for rectifying, amplifying, oscillating or switching; Organic capacitors or resistors having potential barriers
- H10K10/80—Constructional details
- H10K10/82—Electrodes
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Abstract
The invention discloses a high-performance organic field effect transistor with double-layer modification, and a modification method thereof. Two polymers are added between insulation layer-semiconductor layer interfaces for modification. The whole device is successively provided with a source-drain electrode, a semiconductor, a polymer made of a high-dielectric-constant material, a polymer with quite good electric insulation performance, and a silicon substrate whose surface is provided with silicon dioxide of a certain thickness from top to bottom. The dielectric layer of such a structure has quite good insulation performance and also has quite high capacitance at the same time. Through measuring the electric property, the growth morphology of semiconductor particles and the degree of crystallization, it can be determined that the device is a high-performance organic field effect transistor. The high-performance organic field effect transistor has the advantages of having high mobility and a high on-off ratio, also maintaining quite good performance after grid pressure is continuously applied thereto, and also having a quite good stability property in air at the same time.
Description
Technical field
The present invention relates to a kind of organic field effect tube and method of modifying thereof, be specifically related to insulating barrier-interface bilayer and be modified with field effect transistors and method of modifying thereof, device hole mobility can be realized more than 1cm
2/ Vs.
Background technology
Organic field effect tube is lower and can large area produce due to its manufacturing cost, receives increasing concern and deep research in the past few decades.It can be widely used in flexible circuit, electronical display, non-volatile memories and sensor equipment, and therefore, the requirement for its Electronic Performance also improves constantly.This mainly comprises the raising of preparation technology, such as printing, vapour deposition, spin coating etc., and the continuous exploration to material therefor.Research has had been found that some have the small molecule material of high carrier mobility, and the research of many organic field effect tubes is all obtain high mobility based on Small molecular as semiconductor layer.Meanwhile, silicon dioxide is also conventional insulating layer material.Due to its surfaces hydrophilic, be unfavorable for the growth of some semiconductor particles, some defects can be produced.
Existing much about the report of semiconductor-insulator layer individual layer modifying interface at present, as far back as nineteen ninety, the people such as Peng just have studied different polymer and do insulating barrier, propose dielectric constant closely related (X Z Peng, the G Horowitz of mobility and insulating barrier, D Fichou, F Garnier, Appl.Phys.Lett, 1990,57,2013).Afterwards, bibliographical information is also had to modify insulating barrier to reach the summary (W Shao, H L Dong, L Jiang, W P Hu, Chem.Sci, 2011,2,590) improving organic field effect tube electrical properties.Conventional decorative material has polymer poly methyl methacrylate (PMMA), poly-4-Vinyl phenol (PVP), polystyrene (PS), polyvinyl alcohol (PVA), also has self-assembled monolayer decorative material octadecyl trichlorosilane alkane (OTS) and hexamethyldisiloxane (HMDS).OTS, owing to having longer alkyl chain, can form the tunneling barrier of hydroxy functional group at oxide surface, and effectively can regulate the structural arrangement of pentacene thin film as interracial contact layer.Polyvinyl alcohol (PVA), poly-4-Vinyl phenol (PVP) etc. are high dielectric constant material (being high k dielectric again).High k dielectric polymer is often used in flexible organic field effect tube, because it can realize low-voltage, but weak point is that it needs higher annealing temperature, and insulating property (properties) is also more weak.Polystyrene (PS), polymethyl methacrylate (PMMA) etc. are the good polymer of electrical insulating property, these polymer with better insulating properties are also often used in insulating barrier and modify, and this is because they effectively can reduce charge trap between insulating barrier and semiconductor layer improving further electrical insulating property while.Above-mentioned polymer, owing to not having hydroxy functional group, makes surface hydrophobic stronger, and hydrone is difficult to contact its surface thus improve the aerial stability of device, but, along with the raising of insulating properties, the concentration of electric charges between insulating barrier-semiconductor layer interface can reduce, and causes the leakage current of device to become large.
But most report is all the method for modifying adopting individual layer, applies the advantage of decorative material, but the inferior position problem of unresolved decorative material.Therefore, the report of the breakthrough being reached organic field effect tube electrical properties by modifying interface is seldom had.Also no longer only mobility is embodied in the performance requirement of organic field effect tube, also comprises the stability in air, subthreshold value skew, bias effect etc.Although also there is article (the Y M Sun on bibliographical information double-deck modification silicon dioxide insulating layer surface before, X F Lu, S W Lin, J Kettle, S G Yeates, A M Song, Org.Electron, 2010,11,351), above-mentioned article bilayer modifies the combination adopting polymer and self-assembled monolayer, and this kind of combination does not effectively improve the mobility of device.Do not reach the problem of organic field effect tube electrical properties to solve modifying interface, the present invention adopts two layers of polymers to modify, and obtain the device that can increase substantially electrology characteristic, device hole mobility is more than 1cm
2/ Vs.
Summary of the invention
In order to play polymer-modified advantage, solve polymer-modified weak point simultaneously, prepare the organic field effect tube having breakthrough at electrology characteristics such as mobility, stability, subthreshold value skew, bias effects, the invention provides a kind of high-performance organic field effect transistor and method of modifying thereof of bilayer modification.Adopt ELECTRODE WITH BILAYER POLYMERIC thing to modify certain thickness silica surface, promote that upper strata semiconductor particle better grows, improve the electrical properties of organic field effect tube, comprise stability in mobility, air, subthreshold value skew, bias effect.
Object of the present invention is achieved through the following technical solutions.
The high-performance organic field effect transistor that a kind of bilayer is modified, comprise source-drain electrode, semiconductor layer, insulating barrier, described insulating barrier is silica/silicon substrate, has high k dielectric polymeric layer and high-insulativity polymeric layer from top to bottom successively between described semiconductor layer and silica/silicon substrate.
Preferably, in described high k dielectric polymeric layer, high k dielectric polymer is selected from polyvinyl alcohol, poly-4-Vinyl phenol, cyanoethyl pullulan.
Preferably, in described high-insulativity polymeric layer, high-insulativity polymer is selected from polystyrene, polymethyl methacrylate.
Preferably, described high-insulativity polymer and high k dielectric polymer are spun on described insulating barrier successively.
The method of modifying of above-mentioned organic field effect tube, comprises the steps:
(1) configure high-insulativity polymer solution, high-insulativity polymer, is dissolved in ethyl acetate, concentration 10-60mg/ml;
(2) the crosslinked high k dielectric polymer solution of configuration: adopt anhydrides compound to make crosslinking agent, select high-dissolvability to contain ester solvent, select the organic base based on this polymer monomer to make catalyst, be configured to the solution that concentration is 10-30mg/ml;
(3) select surface to have the heavily doped silicon of 40-60nm silicon dioxide as substrate, clean up substrate post-drying;
(4) at the high-insulativity polymer solution that clean substrate surface spin-coating step (1) configures, thickness is 180-300nm; Then spin coating is thereon cross-linked high k dielectric polymer solution, and thickness is 60-80nm;
(5) slice, thin piece complete for spin coating is put into baking oven to dry, cool afterwards;
(6) vacuum evaporation semi-conducting material and source-drain electrode on decorative layer.
Preferably, described in step (1), high-insulativity polymer solution is polymethyl methacrylate solution.
Preferably, high k dielectric polymer solution described in step (2) is crosslinked poly-4-Vinyl phenol solution.
Preferably, crosslinking agent described in step (2) is 4,4'-(hexafluoroisopropylidenyl) two anhydride phthalic acid, and described solvent is 1-Methoxy-2-propyl acetate, and described catalyst is triethylamine.
Preferably, step (4) described spin coating high-insulativity polymer solution, rotating speed is 3000-5000 rev/min, rotates 55-65 second; Described spin coating high k dielectric polymer solution, rotating speed is 1500-2500 rev/min, rotates 35-45s.
Preferably, the described vacuum evaporation semi-conducting material of step (6) is pentacene, and evaporation rate is
vacuum degree control is 6 × 10
-4pa-10
-5pa, adopts crystal oscillator to control thickness at 40-70nm.The described vacuum evaporation source-drain electrode of step (6) is gold, and evaporation rate is
vacuum degree control is 6 × 10
-4pa-10
-5pa, adopts crystal oscillator to control thickness at 15-40nm.
Preferably, the gross thickness after two layers of polymers spin coating is complete controls at 200-380nm, and the thickness of semiconductor layer is 40-70nm, and source-drain electrode is 15-40nm.
The present invention utilizes effective combination of the polymer of high k dielectric (as PVAC polyvinylalcohol, poly-4-Vinyl phenol PVP, cyanoethyl pullulan CYPEL etc.) and the good polymer of electrical insulating property (as polystyrene PS, polymetylmethacrylate etc.) advantage, the high-performance organic field effect transistor that preparation double focusing compound is modified, angularly verifies from mobility, operating voltage, device stability.Utilize atomic force microscope images (AFM), X-ray diffraction (XRD), and the different characterization method such as surface energy being calculated insulating barrier by the Liquid contact angle measured on insulating barrier is comprehensively analyzed, finally have found the best collocation concentration and the device architecture of two kinds of different insulative layers.Choose suitable solvent extremely important, the polymer simultaneously had also needs to be cross-linked, and adopts different crosslinking agents, different concentration, different prepare environment and all can obtain different electrical properties.It is lower that we often understand alternative costs, and solubility better and the material that can not react with any one deck of device makes solvent, simultaneously preferably can comparatively stable existence in atmosphere.
Present invention employs ELECTRODE WITH BILAYER POLYMERIC thing and modify silicon dioxide (SiO
2) (structure as shown in Figure 1), mobility, compared with unmodified, improves 2 times, reaches 1cm
2/ more than Vs, and the organic field effect tube of preparation also can possess higher stability in atmosphere, and in addition, it does not almost return stagnant phenomenon.And carry out analyzing from the aspect such as AFM, XRD and contact angle and also can obtain certification further.
First the solution of two kinds of modified polymers is configured.Then spin coating two kinds of solution successively on cleaned substrate, the thickness of the spin-coated layer of survey is about 200-380 nanometer.Vacuum evaporation semiconductor layer and source-drain electrode on decorative layer, be prepared into complete device subsequently.
The described organic field effect tube modified based on ELECTRODE WITH BILAYER POLYMERIC thing, adopt Agilent B1500 test analytical instrument to test, can obtain higher ON state current, the mobility calculated is at 1cm
2/ more than Vs.By the transfer curve that test data is drawn, as shown in Figure 2, with curve of output, as shown in Figure 3.Compared with the 300nm silicon dioxide that this and OTS modify, there is the thickness of close dielectric layer, but carrier mobility is but doubled, and relative to the surface of unmodified, mobility and on-off ratio all improve a lot.
The described organic field effect tube modified based on ELECTRODE WITH BILAYER POLYMERIC thing, except having higher mobility, does not also significantly return stagnant phenomenon, and as shown in Figure 4, this illustrates that the defect of semiconductive thin film is little, can not catch charge carrier when applying grid voltage.This characteristic can also reflect from bias effect characteristic pattern, as shown in Figure 5, can find out, based on device of the present invention, there is higher electrical stability, after being continuously applied-30V the grid voltage of 60s, 1200s, 2400s, mobility has the trend of increase, as shown in Figure 6.Except electricity is stable, the present invention also confirms in atmosphere also can comparatively stable existence, Fig. 7-Fig. 9 illustrates three important performance characteristic (mobility, on-off ratio and threshold voltage) the change schematic diagram between seven weeks, can find out that the present invention still can keep certain field effect after seven weeks in atmosphere, mobility only have dropped an order of magnitude, still maintains 0.5cm
2/ more than Vs.
The described organic field effect tube modified based on ELECTRODE WITH BILAYER POLYMERIC thing, why can obtain higher electrical properties, be the growth of semiconductor, this can observe from the atomic force microscope images of the p-type semiconductor of 10nm semiconductor-insulator bed boundary and draw, as shown in Figure 10 at all.Particle granules larger after modification can reduce particle edges concentration, contributes to the transmission of charge carrier.The p-type semiconductor that insulating barrier of the present invention grows grows according to island and stratiform hybrid mode, and the particle in this case between interface can closely be connected with substrate, improves the quality of conducting channel.
The described organic field effect tube modified based on ELECTRODE WITH BILAYER POLYMERIC thing, by X-ray diffraction analysis figure, the degree of crystallinity can observing its p-type is also greatly improved compared with before modification, as shown in figure 11, directly can cause the lifting of device performance.
The modifying interface method of high-performance organic field effect transistor of the present invention, effectively can improve surface of insulating layer, improves the interface quality of semiconductor-insulator layer, contributes to the growth of upper strata semiconductor particle, reduces defect, improves the efficiency of transmission of charge carrier.And the raising of electrical properties is not only embodied in transfer, curve of output, also have subthreshold value drift, bias effect, echo effect etc., in atmosphere also can stable existence.The high-performance of device prepared by the present invention is determined from microcosmic by the graphical analysis of atomic force microscope and X-ray diffraction analysis.
Accompanying drawing explanation
Fig. 1 is the bottom gate top contact organic field effect tube structural representation prepared based on modifying interface method;
Fig. 2 is the transfer characteristic curve of the organic field effect tube test that embodiment 1 is prepared based on modifying interface method;
Fig. 3 is the output characteristic curve of the organic field effect tube test that embodiment 1 is prepared based on modifying interface method;
Fig. 4 is the snapback of the organic field effect tube test that embodiment 1 is prepared based on modifying interface method;
Fig. 5 is the bias effect curve of the organic field effect tube test that embodiment 1 is prepared based on modifying interface method;
Fig. 6 is that embodiment 1 applies the mobility after 60s, 1200s and 2400s and threshold voltage variation figure based on organic field effect tube prepared by modifying interface method;
Fig. 7 is embodiment 1 places in seven weeks processes in atmosphere mobility change figure based on organic field effect tube prepared by modifying interface method;
Fig. 8 is embodiment 1 places in seven weeks processes in atmosphere on-off ratio variation diagram based on organic field effect tube prepared by modifying interface method;
Fig. 9 is embodiment 1 places in seven weeks processes in atmosphere threshold voltage variation figure based on organic field effect tube prepared by modifying interface method;
In Figure 10, a figure is the atomic force microscope images of the p-type semiconductor of the 10nm of growth on unmodified interface, and b figure is the atomic force microscope images that embodiment 1 grows in the p-type semiconductor of modifying the 10nm on interface;
Figure 11 be embodiment 1 grow modification interface on contrast with the X-ray diffraction image of the p-type semiconductor of the 50nm on unmodified interface;
Figure 12 is the transfer characteristic curve of the organic field effect tube test that embodiment 2 is prepared based on modifying interface method;
Figure 13 is the transfer characteristic curve of the organic field effect tube test that embodiment 3 is prepared based on modifying interface method;
Figure 14 is the transfer characteristic curve of the organic field effect tube test that embodiment 4 is prepared based on modifying interface method;
Figure 15 is the transfer characteristic curve of the organic field effect tube test that embodiment 5 is prepared based on modifying interface method.
Embodiment
Below by specific embodiment, be described in detail the present invention is based on bottom gate top contact organic field effect tube preparation method prepared by modifying interface method.
Embodiment 1
(1) crosslinked poly-4-Vinyl phenol (PVP) solution of configuration and polymethyl methacrylate (PMMA) solution.PMMA solution is 30mg/ml, is dissolved in ethyl acetate; Cross-linked pvp adopts 4,4'-(hexafluoroisopropylidenyl) two anhydride phthalic acid (HDA) as crosslinking agent, and PVP and HDA mass ratio is 10:1, HDA be 6mg, PVP is 60mg; 2ml 1-Methoxy-2-propyl acetate (PGMEA) is adopted to make solvent; Triethylamine makees catalyst, is configured to the catalytic solution of 3 μ l/ml (triethylamine/PGMEA) concentration, uses the above-mentioned catalytic solution of 1ml; Finally be configured to the solution that PVP concentration is 20mg/ml;
(2) the heavily doped silicon of 50nm silicon dioxide is had on surface to dry with the baking oven that acetone, ethanol, each ultrasonic cleaning of deionized water put into 120 DEG C after 10 minutes successively;
(3) at clean substrate surface (SiO
2face) two kinds of solution configuring of spin-coating step (1).First spin coating PMMA solution, rotating speed is 4000 revs/min, and rotate 60 seconds, THICKNESS CONTROL is at 180-300nm.Then spin coating cross-linked pvp solution thereon, rotating speed is 2000 revs/min, and rotate 40s, THICKNESS CONTROL is at 60-80nm;
(4) baking oven slice, thin piece complete for spin coating being put into 100 DEG C is dried 2 hours, takes out cooling 1 hours subsequently;
(5) vacuum evaporation pentacene, evaporation rate is
vacuum degree control is 6 × 10
-4below pa, adopts crystal oscillator to control thickness at about 50nm;
(6) add mask plate, vacuum evaporation gold electrode, the evaporation environment of gold electrode is the same with pentacene, and evaporation rate is
crystal oscillator is adopted to control thickness at about 20nm.The channel width of mask plate is 2000 μm, and length is 100 μm.
The electrical properties prepared is measured by Agilent B1500 semiconductor analysis instrument, and the transfer characteristic curve be depicted as is as shown in Fig. 2, and mobility reaches 1.271cm
2/ Vs, on-off ratio reaches 10
5, threshold voltage is within-10V.In addition, do not find that there is through flyback and significantly return stagnant phenomenon, as shown in Figure 4, this illustrates that the trap between interface is little.After grid voltage by applying certain hour, mobility does not only reduce, and also presents the trend of rising, and as shown in Figure 6, this has fully demonstrated the electrical stability of this invention.Place in atmosphere after seven weeks, mobility still maintains 0.5cm
2/ more than Vs, as shown in Figure 7, the present invention shows the stability in good air.Atomic force microscope images (AFM) figure (as Figure 10) of the pentacene before and after being modified by investigation and comparison and X-ray diffraction image (XRD) analysis chart (as Figure 11), the pentacene particle can observing growth after modifying is larger, and grow according to the hybrid mode of island and stratiform, improve tight type and the order of interparticle arrangement, the degree of crystallinity simultaneously scheming also can to find out pentacene by XRD also relatively unmodified had raising, contribute to the transmission of charge carrier.
Embodiment 2
(1) crosslinked poly-4-Vinyl phenol (PVP) solution of configuration and polymethyl methacrylate (PMMA) solution.PMMA solution is 20mg/ml, is dissolved in ethyl acetate; Cross-linked pvp adopts 4,4'-(hexafluoroisopropylidenyl) two anhydride phthalic acid (HDA) as crosslinking agent, and PVP and HDA mass ratio is 10:1, HDA be 6mg, PVP is 60mg; 2ml 1-Methoxy-2-propyl acetate (PGMEA) is adopted to make solvent; Triethylamine makees catalyst, is configured to the catalytic solution of 3 μ l/ml (triethylamine/PGMEA) concentration, uses the above-mentioned catalytic solution of 1ml; Finally be configured to the solution that PVP concentration is 20mg/ml;
(2) the heavily doped silicon of 50nm silicon dioxide is had on surface to dry with the baking oven that acetone, ethanol, each ultrasonic cleaning of deionized water put into 120 DEG C after 10 minutes successively;
(3) at clean substrate surface (SiO
2face) two kinds of solution configuring of spin coating.First spin coating PMMA solution, rotating speed is 4000 revs/min, and rotate 60 seconds, THICKNESS CONTROL is at 180-300nm.Then spin coating cross-linked pvp solution thereon, rotating speed is 2000 revs/min, and rotate 40s, THICKNESS CONTROL is at 60-80nm;
(4) baking oven slice, thin piece complete for spin coating being put into 100 DEG C is dried 2 hours, takes out cooling 1 hours subsequently;
(5) vacuum evaporation pentacene, evaporation rate is
vacuum degree control is 6 × 10
-4below pa, adopts crystal oscillator to control thickness at about 50nm;
(6) add mask plate, vacuum evaporation gold electrode, the evaporation environment of gold electrode is the same with pentacene, and evaporation rate is
crystal oscillator is adopted to control thickness at about 20nm.The channel width of mask plate is 2000 μm, and length is 100 μm.
The electrical properties prepared is measured by Agilent B1500 semiconductor analysis instrument, and as shown in figure 12, mobility reaches 0.892cm to the transfer characteristic curve be depicted as
2/ Vs, on-off ratio reaches 10
5, threshold voltage is that-14.67V possesses higher electrology characteristic equally.
Embodiment 3
(1) crosslinked poly-4-Vinyl phenol (PVP) solution of configuration and polymethyl methacrylate (PMMA) solution.PMMA solution is 50mg/ml, is dissolved in ethyl acetate; Cross-linked pvp adopts 4,4'-(hexafluoroisopropylidenyl) two anhydride phthalic acid (HDA) as crosslinking agent, and PVP and HDA mass ratio is 10:1, HDA be 6mg, PVP is 60mg; 2ml 1-Methoxy-2-propyl acetate (PGMEA) is adopted to make solvent; Triethylamine makees catalyst, is configured to the catalytic solution of 3 μ l/ml (triethylamine/PGMEA) concentration, uses the above-mentioned catalytic solution of 1ml; Finally be configured to the solution that PVP concentration is 20mg/ml;
(2) the heavily doped silicon of 50nm silicon dioxide is had on surface to dry with the baking oven that acetone, ethanol, each ultrasonic cleaning of deionized water put into 120 DEG C after 10 minutes successively;
(3) at clean substrate surface (SiO
2face) two kinds of solution configuring of spin coating.First spin coating PMMA solution, rotating speed is 4000 revs/min, and rotate 60 seconds, THICKNESS CONTROL is at 180-300nm.Then spin coating cross-linked pvp solution thereon, rotating speed is 2000 revs/min, and rotate 40s, THICKNESS CONTROL is at 60-80nm;
(4) baking oven slice, thin piece complete for spin coating being put into 100 DEG C is dried 2 hours, takes out cooling 1 hours subsequently;
(5) vacuum evaporation pentacene, evaporation rate is
vacuum degree control is 6 × 10
-4below pa, adopts crystal oscillator to control thickness at about 50nm;
(6) add mask plate, vacuum evaporation gold electrode, the evaporation environment of gold electrode is the same with pentacene, and evaporation rate is
crystal oscillator is adopted to control thickness at about 20nm.The channel width of mask plate is 2000 μm, and length is 100 μm.
The electrical properties prepared is measured by Agilent B1500 semiconductor analysis instrument, and as shown in figure 13, mobility reaches 0.931cm to the transfer characteristic curve be depicted as
2/ Vs, on-off ratio reaches 10
5, threshold voltage is that-22.43V possesses higher electrology characteristic equally.
Embodiment 4
(1) crosslinked poly-4-Vinyl phenol (PVP) solution of configuration and polymethyl methacrylate (PMMA) solution.PMMA solution is 30mg/ml, is dissolved in ethyl acetate; Cross-linked pvp adopts 4,4'-(hexafluoroisopropylidenyl) two anhydride phthalic acid (HDA) as crosslinking agent, and PVP and HDA mass ratio is 10:1, HDA be 3mg, PVP is 30mg; 2ml 1-Methoxy-2-propyl acetate (PGMEA) is adopted to make solvent; Triethylamine makees catalyst, is configured to the catalytic solution of 3 μ l/ml (triethylamine/PGMEA) concentration, uses the above-mentioned catalytic solution of 1ml; Finally be configured to the solution that PVP concentration is 10mg/ml.
(2) the heavily doped silicon of 50nm silicon dioxide is had on surface to dry with the baking oven that acetone, ethanol, each ultrasonic cleaning of deionized water put into 120 DEG C after 10 minutes successively;
(3) at clean substrate surface (SiO
2face) two kinds of solution configuring of spin coating.First spin coating PMMA solution, rotating speed is 4000 revs/min, and rotate 60 seconds, THICKNESS CONTROL is at 180-300nm.Then spin coating cross-linked pvp solution thereon, rotating speed is 2000 revs/min, and rotate 40s, THICKNESS CONTROL is at 60-80nm;
(4) baking oven slice, thin piece complete for spin coating being put into 100 DEG C is dried 2 hours, takes out cooling 1 hours subsequently;
(5) vacuum evaporation pentacene, evaporation rate is
vacuum degree control is 6 × 10
-4below pa, adopts crystal oscillator to control thickness at about 50nm;
(6) add mask plate, vacuum evaporation gold electrode, the evaporation environment of gold electrode is the same with pentacene, and evaporation rate is
crystal oscillator is adopted to control thickness at about 20nm.The channel width of mask plate is 2000 μm, and length is 100 μm.
The electrical properties prepared is measured by Agilent B1500 semiconductor analysis instrument, and the transfer characteristic curve be depicted as is as shown in Figure 14, and mobility reaches 1.253cm
2/ Vs, on-off ratio is close to 10
7, threshold voltage is-13.34V, possesses higher electrology characteristic equally.
Embodiment 5
(1) crosslinked poly-4-Vinyl phenol (PVP) solution of configuration and polymethyl methacrylate (PMMA) solution.PMMA solution is 30mg/ml, is dissolved in ethyl acetate; Cross-linked pvp adopts 4,4'-(hexafluoroisopropylidenyl) two anhydride phthalic acid (HDA) as crosslinking agent, and PVP and HDA mass ratio is 10:1, HDA be 9mg, PVP is 90mg; Adopt 2ml 1-Methoxy-2-propyl acetate (PGMEA) to make solvent, triethylamine makees catalyst, is configured to the catalytic solution of 3 μ l/ml (triethylamine/PGMEA) concentration, uses the above-mentioned catalytic solution of 1ml; Finally be configured to the solution that PVP concentration is 30mg/ml;
(2) the heavily doped silicon of 50nm silicon dioxide is had on surface to dry with the baking oven that acetone, ethanol, each ultrasonic cleaning of deionized water put into 120 DEG C after 10 minutes successively;
(3) at clean substrate surface (SiO
2face) two kinds of solution configuring of spin coating.First spin coating PMMA solution, rotating speed is 4000 revs/min, and rotate 60 seconds, THICKNESS CONTROL is at 180-300nm.Then spin coating cross-linked pvp solution thereon, rotating speed is 2000 revs/min, and rotate 40s, THICKNESS CONTROL is at 60-80nm;
(4) baking oven slice, thin piece complete for spin coating being put into 100 DEG C is dried 2 hours, takes out cooling 1 hours subsequently;
(5) vacuum evaporation pentacene, evaporation rate is
vacuum degree control is 6 × 10
-4below pa, adopts crystal oscillator to control thickness at about 50nm;
(6) add mask plate, vacuum evaporation gold electrode, the evaporation environment of gold electrode is the same with pentacene, and evaporation rate is
crystal oscillator is adopted to control thickness at about 20nm.The channel width of mask plate is 2000 μm, and length is 100 μm.
The electrical properties prepared is measured by Agilent B1500 semiconductor analysis instrument, and as shown in figure 15, mobility is up to 1.644cm for the transfer characteristic curve be depicted as
2/ Vs, on-off ratio is 10
5, threshold voltage is-9.67V, possesses higher electrology characteristic equally.
Claims (10)
1. the double-deck high-performance organic field effect transistor modified, comprise source-drain electrode, semiconductor layer, insulating barrier, described insulating barrier is silica/silicon substrate, it is characterized in that having high k dielectric polymeric layer and high-insulativity polymeric layer from top to bottom successively between described semiconductor layer and silica/silicon substrate.
2. organic field effect tube according to claim 1, is characterized in that, in described high k dielectric polymeric layer, high k dielectric polymer is selected from polyvinyl alcohol, poly-4-Vinyl phenol, cyanoethyl pullulan.
3. organic field effect tube according to claim 1, is characterized in that, in described high-insulativity polymeric layer, high-insulativity polymer is selected from polystyrene, polymethyl methacrylate.
4. organic field effect tube according to claim 1, is characterized in that, described high-insulativity polymer and high k dielectric polymer are spun on described insulating barrier successively.
5. a method of modifying for the arbitrary organic field effect tube of claim 1-4, is characterized in that, comprise the steps:
(1) configure high-insulativity polymer solution, high-insulativity polymer, is dissolved in ethyl acetate, concentration 10-60mg/ml;
(2) the crosslinked high k dielectric polymer solution of configuration: adopt anhydrides compound to make crosslinking agent, select high-dissolvability to contain ester solvent, select the organic base based on this polymer monomer to make catalyst, be configured to the solution that concentration is 10-30mg/ml;
(3) select surface to have the heavily doped silicon of 40-60nm silicon dioxide as substrate, clean up substrate post-drying;
(4) at the high-insulativity polymer solution that clean substrate surface spin-coating step (1) configures, thickness is 180-300nm; Then spin coating is thereon cross-linked high k dielectric polymer solution, and thickness is 60-80nm;
(5) slice, thin piece complete for spin coating is put into baking oven to dry, cool afterwards;
(6) vacuum evaporation semi-conducting material and source-drain electrode on decorative layer.
6. the method for modifying of organic field effect tube according to claim 5, it is characterized in that, described in step (1), high-insulativity polymer solution is polymethyl methacrylate solution.
7. the method for modifying of organic field effect tube according to claim 5, is characterized in that, high k dielectric polymer solution described in step (2) is the poly-4-Vinyl phenol solution of connection.
8. the method for modifying of organic field effect tube according to claim 5, it is characterized in that, described crosslinking agent is 4,4'-(hexafluoroisopropylidenyl) two anhydride phthalic acid, and described solvent is 1-Methoxy-2-propyl acetate, and described catalyst is triethylamine.
9. the method for modifying of organic field effect tube according to claim 5, it is characterized in that, the described vacuum evaporation semi-conducting material of step (6) is pentacene, and evaporation rate is
vacuum degree control is 6 × 10
-4pa-10
-5pa, adopts crystal oscillator to control thickness at 40-70nm; The described vacuum evaporation source-drain electrode of step (6) is gold, and evaporation rate is
vacuum degree control is 6 × 10
-4pa-10
-5pa, adopts crystal oscillator to control thickness at 15-40nm.
10. the method for modifying of organic field effect tube according to claim 5, it is characterized in that: the gross thickness after two layers of polymers spin coating is complete controls at 200-380nm, the thickness of semiconductor layer is 40-70nm, and source-drain electrode is 15-40nm.
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| CN106876585A (en) * | 2017-01-19 | 2017-06-20 | 南京邮电大学 | A kind of method that organic field effect tube mobility is improved by short annealing |
| CN106981573A (en) * | 2017-03-20 | 2017-07-25 | 南京邮电大学 | A kind of organic field effect tube memory from barrier layer structure and preparation method thereof |
| CN109638158A (en) * | 2018-11-28 | 2019-04-16 | 中南大学 | A kind of flexible organic film transistor and preparation method thereof |
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| CN105336860A (en) * | 2015-11-09 | 2016-02-17 | 南京邮电大学 | Flexible low-voltage organic field effect transistor and manufacturing method thereof |
| CN105591029A (en) * | 2016-03-24 | 2016-05-18 | 华南师范大学 | Organic non-volatile memory device based on high K materials and preparation method thereof |
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| CN106981573A (en) * | 2017-03-20 | 2017-07-25 | 南京邮电大学 | A kind of organic field effect tube memory from barrier layer structure and preparation method thereof |
| CN106981573B (en) * | 2017-03-20 | 2019-06-21 | 南京邮电大学 | A kind of organic field effect tube memory and preparation method thereof from barrier layer structure |
| CN109638158A (en) * | 2018-11-28 | 2019-04-16 | 中南大学 | A kind of flexible organic film transistor and preparation method thereof |
| CN109638158B (en) * | 2018-11-28 | 2020-10-23 | 中南大学 | Flexible organic thin film transistor and preparation method thereof |
| CN112652718A (en) * | 2020-12-11 | 2021-04-13 | 华南理工大学 | Method for improving mobility of all-organic thin film transistor device |
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