CN101442105B - Organic field effect transistor and special source/drain electrode and preparation method thereof - Google Patents
Organic field effect transistor and special source/drain electrode and preparation method thereof Download PDFInfo
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- CN101442105B CN101442105B CN2007101778142A CN200710177814A CN101442105B CN 101442105 B CN101442105 B CN 101442105B CN 2007101778142 A CN2007101778142 A CN 2007101778142A CN 200710177814 A CN200710177814 A CN 200710177814A CN 101442105 B CN101442105 B CN 101442105B
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Abstract
The invention discloses an organic field effect transistor (FET), as well as a special source-drain electrode and a preparation method thereof. The organic FET with an electrode structure comprises agate electrode, a dielectric layer, an organic semiconductor layer, a source electrode and a drain electrode, wherein the source electrode and the drain electrode are patterned Graphene electrodes. The method for preparing the patterned Graphene electrodes comprises the following steps: 1) a metal film is deposited on a substrate and is patterned; and 2) the substrate on which the patterned metalfilm is deposited is placed in a chemical vapor deposition system, and chemical vapor Graphene deposition is performed on the surface of a patterned metal electrode material, so as to obtain the patterned Graphene electrodes, wherein a carbon source used in chemical vapor deposition is methanol, ethanol, propanol, pentanol, benzene, toluene, xylene, methane and the like.
Description
Technical field
The present invention relates to a kind of organic field effect tube and preparation method thereof, particularly relate to a kind of Graphene electrodes with patterning as organic field effect tube of the lower electrode arrangement of source-drain electrode and preparation method thereof, and the Graphene electrodes of this patterning and preparation method.
Background technology
Organic field effect tube (organic field effect transistors (OFETs)) is by regulating a kind of active device that grid voltage comes size of current between the Controlling Source drain electrode, whole transistor is by gate electrode 1, dielectric layer 2, organic semiconductor layer 3, source electrode 4 and drain electrode 5 constitute, its structure can be divided into by source-drain electrode position difference: upper electrode arrangement and lower electrode arrangement, its structural representation is respectively shown in Fig. 1 a and Fig. 1 b, in upper electrode arrangement, source electrode 4 and drain electrode 5 are located on the organic semiconductor layer 3, are not connected with dielectric layer 2 that (Fig. 1 a); And in lower electrode arrangement, source electrode 4 and drain electrode 5 are arranged between organic semiconductor layer 3 and the dielectric layer 2, all are connected (Fig. 1 b) with dielectric layer 2 with organic semiconductor layer 3.Wherein lower electrode arrangement can be compatible mutually with the photoetching technique of maturation, and is relatively poor but metal electrode contacts with organic semi-conductor.
(Tsumura, A. since the invention eighties in last century organic field effect tube; Koezuka, H.; Ando, T.Appl.Phys.Lett.1986,49,1210), organic field effect tube is owing to show that in flexibility the potential application foreground of aspects such as organic integration circuit has caused people's broad research interest.Compare with the inorganic field effect transistor, organic field effect tube has himself distinct advantages, comprises that mainly its preparation technology is simple, with low cost, in light weight, pliability is good etc.In recent years, organic field effect tube had all been obtained significant progress in the each side such as exploitation of material (organic semiconducting materials, electrode material, insulating layer material), device performance and its application.At present, reached and amorphous silicon device performance compare favourably degree (Nelson, S.F. based on the main performance index (mobility and on-off ratio) of organic semi-conductor field-effect transistor; Lin, Y.Y.; Gundlach, D.J.; Jackson, T.N.Appl.Phys.Lett.1998,72,1854), this makes organic field effect tube possess to move towards the fundamental of using.
Reduce cost is to promote the effective way that organic field effect tube moves towards application, therefore, the electrode of the organic insulator of the organic semiconducting materials of developing low-cost and organic semiconductor thin-film preparation technology, developing low-cost and developing low-cost is to study focus at present.With the organic field effect tube electrode is example, for the source-drain electrode of expensive gold as organic field effect tube generally adopted in the effective injection (particularly P type organic field effect tube) that guarantees charge carrier, and cheap copper and the silver-colored performance that can reduce organic field effect tube as electrode of cost.
Graphite is the stable existence form of carbon, so it has a wide range of applications in all many-sides.In recent years, Graphene (one deck or which floor two-dimentional graphite) is as the nova of Condensed Matter Physics and material science, and its relevant research has caused people's extensive concern.By the end of so far, mainly concentrate on the research of basic aspect about the research of this aspect, and the research of application facet is about to cause people's attention.In addition, the growth of Graphene and patterning also are one of its subject matter of facing now, and graphite division, epitaxial growth and graphite oxidation are the effective ways that obtain Graphene at present, ((a) Novoselov, K.S.; Geim, A.K.; Morozov, S.V.; Jiang, D.; Zhang, Y.; Dubonos, S.V.; Grigorieva, I.V.; Firsov, A.A.Science 2004,306,666. (b) Evans, J.W., Th iel, P.A.; Bartelt, M.C.Sur.Sci.Rep.2006,61,1. (c) McAllister, M.J., Li, J.; Adamson, D.H.; Schniepp, H.C.; Abdala, A.A.; Liu, J.; Herrera-Alonso, M.; Milius, D.L.; Car, R.; Prud ' homme, R.K.; Aksay, I.A.Chem.Mater.2007,19,4396.), but these methods are difficult to realize the patterning of Graphene.
Summary of the invention
The purpose of this invention is to provide a kind of patterned Graphene electrodes and preparation method thereof.
The present invention prepares the method for patterned Graphene electrodes, comprises the steps:
1) depositing metal films on substrate, and with described metallic film patterning;
2) substrate that will deposit the pattern metal film places chemical gas-phase deposition system, at pattern metal film surface chemical vapour deposition (CVD) Graphene, obtains patterned Graphene electrodes.
Wherein, the used carbon source of chemical vapour deposition (CVD) is methyl alcohol, ethanol, propyl alcohol, amylalcohol, benzene,toluene,xylene and methane etc.The temperature of chemical vapour deposition (CVD) is the 100-1200 degree; Carrier gas is N
2, Ar, N
2/ H
2Or Ar/H
2Metal electrode material is silver, copper, gold, aluminium, calcium, magnesium, tin, iron, sodium, barium or their alloy.
The patterned Graphene electrodes that the inventive method prepares also belongs to protection scope of the present invention.
It is the organic field effect tube and preparation method thereof of source electrode and drain electrode with patterned Graphene electrodes of the present invention that the present invention also provides a kind of.
Lower electrode arrangement organic field effect tube of the present invention comprises gate electrode, dielectric layer, organic semiconductor layer, source electrode and drain electrode, and wherein, source electrode and drain electrode are patterned Graphene electrodes of the present invention.
Wherein, gate electrode material comprises silver, copper, gold, aluminium, calcium, magnesium, tin, iron, sodium, barium or electric conducting materials such as their alloy, tin indium oxide or highly doped monocrystalline silicon.Dielectric layer material comprises Inorganic Dielectric Materials such as silicon dioxide, silicon nitride, aluminium oxide, tantalum oxide, yittrium oxide, cerium oxide or zirconia.
The preparation method of this lower electrode arrangement organic field effect tube comprises the steps:
A) sequential aggradation gate electrode and dielectric layer on substrate;
B) deposition layer of metal film on the substrate that deposits gate electrode and dielectric layer is realized described metallic film patterning by mask plate or photoetching technique;
C) step b) gained substrate is placed chemical gas-phase deposition system,, form patterned Graphene electrodes, as the source electrode and the drain electrode of organic field effect tube at pattern metal film surface chemical vapour deposition (CVD) Graphene;
D) on step c) gained substrate, prepare organic semiconductor layer, obtain described lower electrode arrangement organic field effect tube.
The present invention has and has following characteristics and advantage:
1: the present invention adopts the method for chemical vapour deposition (CVD) to prepare the Graphene of patterning, is a kind of novel simple preparation patterned Graphene method.
2: the present invention prepares Graphene electrodes and adopts cheaply that methyl alcohol, ethanol, propyl alcohol, amylalcohol, benzene,toluene,xylene and methane etc. are raw material, has characteristics cheaply based on the device of this electrode.
3: the lower electrode arrangement organic field effect tube of the present invention's preparation is a source-drain electrode with the Graphene electrodes of patterning, can guarantee that source-drain electrode and organic semiconductor have excellent contact, realize effective injection of charge carrier, can improve the performance of organic field effect tube, and preparation process is easier to realize mass preparation in conjunction with photoetching technique.
Description of drawings
Fig. 1 organic field effect tube upper electrode arrangement and lower electrode arrangement schematic diagram;
Fig. 2 is the preparation flow figure of patterned Graphene electrodes and organic field effect tube;
Fig. 3 is the transmission electron microscope photo of patterning graphite electrode of the present invention, x-ray photoelectron power spectrum and Raman spectrogram; Wherein Fig. 3 a is a transmission electron microscope picture, and Fig. 3 b is an x-ray photoelectron energy spectrogram, and Fig. 3 d is at the Raman spectrum of the Graphene on copper surface;
Fig. 4 is the stereoscan photograph of Graphene electrodes of the present invention on copper or silver; Wherein Fig. 4 b is that Graphene is at the lip-deep sem photograph of copper.
Fig. 5 for of the present invention be semiconductor based on pentacene, the copper that Graphene is modified is the curve of output and the transfer curve figure of the bottom electrode organic field effect tube of electrode.
Fig. 6: for of the present invention be organic semiconductor based on pentacene, the copper that Graphene is modified is the performance under the different channel lengths of bottom electrode organic field effect tube of electrode.
Fig. 7 for of the present invention be semiconductor based on pentacene, the Graphene of growing on silver-colored film is the curve of output and the transfer curve figure of organic field effect tube of the lower electrode arrangement of source-drain electrode, wherein, the curve of output of Fig. 7 (a), the transfer curve when Fig. 7 (b) is-60 volts for source-drain voltage.
Embodiment
The present invention at first prepares a kind of patterned Graphene electrodes, then, prepares a kind of organic field effect tube of lower electrode arrangement as source-drain electrode with this patterned Graphene electrodes.
The process of making the organic field effect tube of this lower electrode arrangement and patterned Graphene electrodes is as follows:
The first step, elder generation is sequential aggradation gate electrode and dielectric layer on substrate according to a conventional method;
In second step, make source-drain electrode---patterned Graphene electrodes
1) preparation of pattern metal film:
To deposit the substrate of gate electrode and insulating barrier,, prepare one deck metallic film at least then, realize its patterning by mask plate or photoetching technique with oven for drying after deionized water, ethanol, the acetone ultrasonic cleaning.
2) preparation of patterned Graphene source-drain electrode:
The substrate that will have the metallic film of patterning is positioned in the chemical gas-phase deposition system, at pattern metal film surface chemical vapour deposition (CVD) Graphene, obtains patterned Graphene electrodes, as the source-drain electrode of organic field effect tube.
The 3rd step, the deposition of organic semiconducting materials:
On the substrate that has Graphene source-drain electrode and insulating barrier, preparation thickness is the organic semiconductor layer of 10～150 nanometers, promptly obtains organic field effect tube.
In organic field effect tube, gate electrode is to constitute by having low-resistance material, comprise electric conducting materials such as various metals such as gold, silver, aluminium, copper and alloy material and metal oxide (as tin indium oxide), highly doped monocrystalline silicon, deposition process can be the various deposition processs such as chemical vapour deposition (CVD) of vacuum thermal evaporation, magnetron sputtering, plasma enhancing.Dielectric layer has excellent dielectric properties, comprise oxide and other inorganic insulating materials such as inorganic insulating material silicon dioxide, silicon nitride, aluminium oxide, tantalum oxide, yittrium oxide, cerium oxide, zirconia, the preparation method can be the chemical vapour deposition (CVD), the thermal oxidation that strengthen of plasma, get rid of film, vacuum evaporation or inkjet printing etc.Organic semiconductor is the organic semiconducting materials with field effect behavior, comprises organic small molecule material, macromolecule polymer material or their mixtures, and thin film-forming method can be vacuum evaporation, gets rid of film, drip technology such as film, printing.
Making source-drain electrode---in the patterned Graphene electrodes step, metallic film material comprises silver, copper, gold, aluminium, calcium, magnesium, tin, iron, sodium, barium and their alloy, deposition process can be various deposition processs such as the chemical vapour deposition (CVD) that strengthens of vacuum thermal evaporation, magnetron sputtering, plasma, printing, and metal layer thickness is 10～300 nanometers; After the metal deposition by chemical gaseous phase depositing process at metallic film superficial growth Graphene, the shape of the pattern of graphene film is that the patterning of metallic film can be realized by mask technique or photoetching technique by the decision of the figure of metallic film.
The condition of a chemical vapour deposition (CVD) Graphene is as follows:
Small amount of methanol, ethanol, propyl alcohol, amylalcohol, benzene, toluene or dimethylbenzene and the substrate that deposits the metallic film of patterning are placed the low-temperature zone and the high temperature section of two-part high temperature furnace quartz ampoule respectively, feed N
2, Ar, N
2/ H
2Or Ar/H
2Be carrier gas, throughput is 1-500sccm, treats that furnace body temperature is increased to 100-1200 when spending, and quartz ampoule is placed body of heater, heats and takes out quartz ampoule after 1-30 minute.
Be the copper electrode that Graphene is modified for example below, be illustrated based on the preparation of the organic field effect tube of pentacene, but the present invention is not limited thereto electrode.
The first step, elder generation is sequential aggradation gate electrode and dielectric layer on substrate according to a conventional method;
Selecting highly doped N-type monocrystalline silicon is substrate and gate electrode, by thermal oxidation process growthing silica dielectric layer.
Second step, preparation patterned Graphene source-drain electrode
1, patterned copper depositing of thin film:
As Fig. 2, will deposit the substrate of gate electrode and insulating barrier, with oven for drying behind the deionized water, ethanol, acetone ultrasonic cleaning, the deposition process of the vacuum thermal evaporation that strengthens with plasma prepares 30 nanometer thick copper layers then; The film for preparing interdigital shape when evaporation by masking method has been realized the patterning of copper film;
2, the preparation of patterned Graphene source-drain electrode:
Small amount of ethanol and the substrate that deposits the copper film of patterning are placed the low-temperature zone and the high temperature section of two-part high temperature furnace quartz ampoule respectively, feed Ar/H
2Be carrier gas, throughput is 100sccm, treats that furnace body temperature is increased to 800 when spending, and quartz ampoule is placed body of heater, heats and takes out quartz ampoule after five minutes, promptly obtains the patterned Graphene source-drain electrode.
The 3rd step, the deposition of organic semiconducting materials:
The lower electrode arrangement substrate for preparing is placed in the vacuum coating equipment, is 4 * 10 in vacuum degree
-4Under the condition of Pa with
Speed evaporation pentacene, thickness is 50 nanometers, promptly obtains the organic field effect tube of lower electrode arrangement.
Fig. 3 is transmission electron microscope, x-ray photoelectron power spectrum and the Raman spectrogram of patterning graphite electrode; Wherein Fig. 3 a is a transmission electron microscope picture, and Fig. 3 b is an x-ray photoelectron energy spectrogram, and Fig. 3 d is at the Raman spectrum of the Graphene on copper surface.Fig. 4 is the stereoscan photograph of Graphene on copper or silver; Wherein Fig. 4 b is that Graphene is at the lip-deep sem photograph of copper.The result shows, has formed Graphene at the copper film.
Utilize the HP4140B semi-conductor test instrument under atmospheric environment, under the room temperature device performance to be tested afterwards.Pentacene device mobility when channel length is 5 microns based on this structure can reach 0.53cm
2V
-1s
-1, on-off ratio is 10
7As a comparison, directly be that the mobility of organic field effect tube of the lower electrode arrangement of source-drain electrode can reach 0.02cm with the copper electrode
2V
-1s
-1, on-off ratio is 10
5The result shows, be that the organic field effect tube of source-drain electrode is better than on performance with copper with the Graphene is the performance of the device of electrode, and that is to say: with the copper ratio, Graphene electrodes is more suitable for the source-drain electrode as the lower electrode arrangement organic field effect tube.
Referring to Fig. 5, for of the present invention be semiconductor based on pentacene, the Graphene of growing on the copper film is the curve of output and the transfer curve figure of organic field effect tube of the lower electrode arrangement of source-drain electrode, wherein, the curve of output of Fig. 5 (a), Fig. 5 (b) for source-drain voltage is-transfer curve during 60V.
Referring to Fig. 6, for of the present invention be semiconductor based on pentacene, be the device mobility under the different channel lengths of organic field effect tube of lower electrode arrangement of source-drain electrode at the Graphene of growing on the copper film.
Embodiment 2:
Press the preparation of embodiment 1, the employing photoetching technique prepares the film of interdigital shape, has realized the patterning of silver-colored film; Then, on silver-colored film, grow graphene film as source-drain electrode; All the other steps are identical with embodiment 1.
Transistor is carried out performance test, and managing field-effect mobility based on the crystal of pentacene when channel length is 5 microns is 0.48cm
2V
-1s
-1, on-off ratio is 10
7As a comparison, directly be that the mobility of organic field effect tube of the lower electrode arrangement of source-drain electrode can reach 0.026cm with the silver electrode
2V
-1s
-1, on-off ratio is 10
4The result shows, be that the organic field effect tube of source-drain electrode is better than on performance with silver with the Graphene is the device of electrode, and that is to say: with the silver ratio, Graphene electrodes is more suitable for the source-drain electrode as the lower electrode arrangement organic field effect tube.
Referring to Fig. 7, for of the present invention be semiconductor based on pentacene, the Graphene of growing on silver-colored film is the curve of output and the transfer curve figure of organic field effect tube of the lower electrode arrangement of source-drain electrode, wherein, the curve of output of Fig. 7 (a), the transfer curve when Fig. 7 (b) is-60 volts for source-drain voltage.
Adopt similar method, alloy firm surface at metals such as gold, aluminium, calcium, magnesium, tin, iron, sodium, barium and silver, copper, gold, aluminium, calcium, magnesium, tin, iron, sodium, barium all can grow Graphene, obtain patterned Graphene electrodes, the organic field effect tube that with these patterned Graphene electrodes is the lower electrode arrangement of source-drain electrode all has good performance, and all to be better than be the device of source-drain electrode with the metal directly.
Claims (10)
1. a method for preparing patterned Graphene electrodes comprises the steps:
1) depositing metal films on substrate, and with described metallic film patterning;
2) substrate that will deposit the pattern metal film places chemical gas-phase deposition system, at pattern metal film surface chemical vapour deposition (CVD) Graphene, obtains patterned Graphene electrodes.
2. method according to claim 1 is characterized in that: described metallic film comprises silver, copper, gold, aluminium, calcium, magnesium, tin, iron, sodium, barium or their alloy.
3. method according to claim 1 is characterized in that: described metallic film patterning is adopted mask technique or photoetching technique.
4. method according to claim 1 is characterized in that: the used carbon source of chemical vapour deposition (CVD) is methyl alcohol, ethanol, propyl alcohol, amylalcohol, benzene,toluene,xylene or methane; The temperature of chemical vapour deposition (CVD) is the 100-1200 degree; Carrier gas is N
2, Ar, N
2/ H
2Or Ar/H
2
5. the patterned Graphene electrodes for preparing of claim 1 or 2 or 3 or 4 described methods.
6. a lower electrode arrangement organic field effect tube comprises gate electrode, dielectric layer, organic semiconductor layer, source electrode and drain electrode, it is characterized in that: described source electrode and drain electrode are the described patterned Graphene electrodes of claim 5.
7. lower electrode arrangement organic field effect tube according to claim 6 is characterized in that: described gate electrode material comprises silver, copper, gold, aluminium, calcium, magnesium, tin, iron, sodium, barium or their alloy, tin indium oxide or highly doped monocrystalline silicon.
8. lower electrode arrangement organic field effect tube according to claim 6 is characterized in that: described dielectric layer material comprises silicon dioxide, silicon nitride, aluminium oxide, tantalum oxide, yittrium oxide, cerium oxide or zirconia.
9. lower electrode arrangement organic field effect tube according to claim 6 is characterized in that: described organic semiconductor is organic molecule or macromolecular material.
10. the preparation method of the described lower electrode arrangement organic field effect tube of claim 6 comprises the steps:
A) sequential aggradation gate electrode and dielectric layer on substrate;
B) deposition layer of metal film on the substrate that deposits gate electrode and dielectric layer is realized described metallic film patterning by mask plate or photoetching technique;
C) step b) gained substrate is placed chemical gas-phase deposition system,, form patterned Graphene electrodes, as the source electrode and the drain electrode of organic field effect tube at pattern metal film surface chemical vapour deposition (CVD) Graphene;
D) on step c) gained substrate, prepare organic semiconductor layer, obtain described lower electrode arrangement organic field effect tube.
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| US20070187694A1 (en) * | 2006-02-16 | 2007-08-16 | Pfeiffer Loren N | Devices including graphene layers epitaxially grown on single crystal substrates |
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| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103019493A (en) * | 2012-12-24 | 2013-04-03 | 无锡力合光电石墨烯应用研发中心有限公司 | Electrode structure for capacitive touch screens and preparation method thereof |
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