CN1280708A - Process for fabricating organic semiconductor devices using ink-jet printing technology and device and system employing same - Google Patents

Process for fabricating organic semiconductor devices using ink-jet printing technology and device and system employing same Download PDF

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CN1280708A
CN1280708A CN98811747A CN98811747A CN1280708A CN 1280708 A CN1280708 A CN 1280708A CN 98811747 A CN98811747 A CN 98811747A CN 98811747 A CN98811747 A CN 98811747A CN 1280708 A CN1280708 A CN 1280708A
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conjugation
organic
electrode
deposit
buffer layer
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杨洋
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University of California
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University of California
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    • H01L21/4846—Leads on or in insulating or insulated substrates, e.g. metallisation
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    • H10K71/10—Deposition of organic active material
    • H10K71/12—Deposition of organic active material using liquid deposition, e.g. spin coating
    • H10K71/13—Deposition of organic active material using liquid deposition, e.g. spin coating using printing techniques, e.g. ink-jet printing or screen printing
    • H10K71/135—Deposition of organic active material using liquid deposition, e.g. spin coating using printing techniques, e.g. ink-jet printing or screen printing using ink-jet printing
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    • H10K50/11—OLEDs or polymer light-emitting diodes [PLED] characterised by the electroluminescent [EL] layers
    • H10K50/125—OLEDs or polymer light-emitting diodes [PLED] characterised by the electroluminescent [EL] layers specially adapted for multicolour light emission, e.g. for emitting white light
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Abstract

An emission system for presenting visual image is disclosed. The emissive system typically contains first electrodes (90) deposited over and in contact with a substrate. One or more conjugated organic buffer layers (40) are then deposited over and in contact with the first electrodes, and second electrodes (22) are subsequently deposited over the conjugated organic buffer layers. The conjugated organic buffer layers (40) regulate current flow between the first electrodes (90) and the second electrodes (22). Either before or after the deposition of each conjugated organic buffer layer (40), but before the deposition of the second electrodes (22), conjugated organic deposits (34, 36, 38) are ink-jet printed such that they are in contact with at least one conjugated organic buffer layer. The conjugated organic deposits (34, 36, 38) help to generate an indicator when a voltage stimulus is applied across the first electrodes (90) and the second electrodes (22). Depending on the material of the conjugated organic deposits (34, 36, 38), the indicator may be luminescence, fluorescence, conductivity, or the like. A voltage source is used for selectively applying the voltage stimulus across the first electrodes (90) and the second electrodes (22).

Description

Utilize ink-jet printing technology to make method and the device and the system that utilizes this device of organic semiconductor device
The background of invention
1, FIELD OF THE INVENTION
The present invention relates generally to organic semiconductor device, particularly utilize ink-jet printing technology to make the method for organic semiconductor device, and the system of device and this device of use.
2, the introduction of correlation technique
For example inorganic semiconductor such as silicon generally is used to make modern semiconductors and photonic device.The processing of these inorganic semiconductor devices may be complicated and expensive, and the polishing that generally comprises for example crystal growth, section and wafer reaches processing steps such as forming integrated electronic circuit on wafer.By comparison, conventional polymer (being called plastics sometimes) is easier to processing.For example, the manufacturing of conventional plastic parts comprises for example with the better simply processing steps such as plastic material injection mould that melt.Conventional polymer also has characteristics such as pliable and tough and in light weight, can the high surface area manufacturing.Yet conventional plastics are not semiconductive, therefore can not be used for producing the semiconductor devices.
Conjugated polymer is a kind of organic material that combines the machinability of semi-conductive electricity and optical characteristics and conventional plastics.The semiconduction of conjugated polymer comes from and for example is formed on poly-(phenylene vinylidene), polythiophene (PT), poly-(2-methoxyl group-5-(2 '-ethyl-own oxygen base)-1, the delocalization π track in the 4-phenylene vinylidene carbon compounds such as (MEH-PPV).Different with conventional polymer, conjugated polymer contains makes the material semiconductive and on-insulated two keys.Conjugated polymer has the advantage of low-cost processing, and is pliable and tough, in light weight, and has the large-scale processing of conventional polymer, and has the common semiconductive characteristic of silicon.
Conjugated polymer device general using spin-coating method is made.Make the substrate that contains big dropping liquid attitude conjugated polymer around the axle high speed rotating, make liquid conjugated polymer to outflow, thereby use the material film coated substrates, this spin-coating method has utilized the advantage of polymer solution processability.Yet still there be the shortcoming relevant with spin coating in this method.The substrate because most liquid conjugated polymers have flown out is not coated on the substrate surface, and spin coating has caused the waste of solution.In addition, because any protrusion all can produce shadow effect when liquid organic material intersperses among on the substrate surface,, can stay radially vestige of thin organic material in the back of defective so spin-coating method is very sensitive to the dust on the substrate surface or other defective.
Do not allow manageable liquid conjugated polymers logistics also can't form the figure of hope during the spin coating, limited the commerce of conjugated polymer and used.For example, be clipped in two interelectrode luminescent conjugated polymers and can be used for making LEDs and luminous sign (light-emitting logos, LELs), but the conjugated polymer that spin coating forms not the composition individual layer this device is restricted to monochrome devices, and need carry out composition to electrode.In addition, because the two keys in the conjugated organic materials can be destroyed because of photoetching process, can't be used for the composition conjugated polymer layer so generally be used to form the photoetching technique of composition electrode.
Another kind of organic semiconducting materials is the little organic molecule class of conjugation.Here conjugation organic compound (organic substance) is defined as and comprises polymer (each strand has the organic substance of two above repetitives) and little organic molecule (organic substance that individual molecule constitutes).Little organic molecule has and the similar physics of conjugated polymer (electricity and optics) character, but utilizes different process technologies.Organic molecule in ultra-high vacuum environment, utilizes the processing of heat sublimation method usually, forms desirable film, the general about 100nm of thickness.Little organic molecule is general to be adopted and the similar device architecture of conjugated polymer, and promptly organic film accompanies between two electrodes.The composition of organic film can utilize orifice plate (shadow mask) to finish, but this method need accurately be aimed at orifice plate, is the technology that a kind of speed is slow and cost is high.In addition, lateral resolution also is restricted.Organic molecule also can utilize conventional spin coating proceeding processing, but this method can't composition.Generally process little organic molecule, make mixture keep polymer in the advantage of the mechanical property of film formation aspect by these molecules are mixed with main conjugated polymer.Figure 18 a, 18b and 18c have provided the example of the typical organic compound that is applicable to resilient coating and ink jet printing deposit.
Ink jet printing (IJP) technology is the ordinary skill of desktop publishing, can be used for the conjugated organic materials of high-resolution ground deposit composition.People such as T.R Hebner are entitled as " being used for the ink jet printing of an organic light-emitting device doped polymer " literary composition Applied PhysicsLetters (Applied Physics communication) the 72nd volume the 519th page (1998), introduce the application of IJP aspect the conjugation organic substance of deposit composition, quoted the document here.Yet,, can only print the low concentration polymer solution that contains pigment in order to utilize existing IJP technology.The result has formed inapplicable inferior film for high quality semiconductor device.
Even, still there is other problem can be on bottom electrode during the conjugation organic substance of the suitable composition of deposit.Because the point of IJP formation property utilizes the organic membrane of IJP printing to have many pin holes.Upper electrode material deposit on the composition conjugation organic thin film can cause some upper electrode material to contact with bottom electrode by pin hole, produces to cause the short circuit that makes component failure.
General introduction of the present disclosure
Therefore, the purpose of each embodiment of the present invention provides a kind of method of utilizing the hybrid ink jet printing technology to make organic semiconductor device, and the device of system and this system of introducing, this method is more insensitive to the substrate surface defective, and combine conventional semi-conductive electricity and optical property and low-cost processability, pliability, in light weight and have a conventional organic large-scale processing.
A purpose again of each embodiment of the present invention provides a kind of method of utilizing the hybrid ink jet printing technology to make organic semiconductor device, and the device of system and this system of introducing, this method can form monochrome or polychrome emission display, device, sign and the gray level image etc. of the high precision composition of the emitter region that comprises isolation.
An also purpose of each embodiment of the present invention provides a kind of method of utilizing the hybrid ink jet printing technology to make organic semiconductor device, and the device of system and this system of introducing, this method can be formed for the high-quality mask of semiconductor device, biology sensor, photovoltaic device and photo-detector etc.
A kind of emission system that is used for the display of visually image can reach these and other objects.This emission system generally has first electrode that is deposited on the substrate and contacts with it.Then, one or more conjugation organic buffer layers are deposited on first electrode and contact with it, and then, second electrodeposition is on the conjugation organic buffer layer.The conjugation organic buffer layer is regulated first electrode and the second interelectrode electric current.Before or after each conjugation organic buffer layer deposit, but before second electrodeposition, the organic deposit of ink jet printing conjugation contacts them at least with a conjugation organic buffer layer.
When being added on first electrode and second electrode in the voltage drive source, the organic deposit of conjugation assists in and produces an indication item.According to the material of the organic deposit of conjugation, this indication item can be luminous, fluoresce, conduction etc.Voltage source is used for optionally the voltage drive source being added on first and second electrodes.
When reading accompanying drawing and appended claims, from following detailed introduction to embodiment of the present invention, the those skilled in the art can understand these and other objects, characteristics and the advantage of each embodiment of the present invention.
Brief description of drawings
Fig. 1 is the diagrammatic sketch of the organic deposit of IJP conjugation on the conjugation organic buffer layer according to an embodiment of the invention.
Fig. 2 a is the diagrammatic sketch of conjugation organic semiconductor device according to an embodiment of the invention, said conjugation organic semiconductor device comprises one second electrode and one first electrode, clips the organic deposit of individual layer conjugation that is printed on single conjugation organic buffer layer between two electrodes.
Fig. 2 b is the diagrammatic sketch of conjugation organic semiconductor device according to an embodiment of the invention, said conjugation organic semiconductor device comprises a plurality of second electrodes and a plurality of first electrode (can't see) from figure, clip the organic deposit of individual layer conjugation that is printed on single conjugation organic buffer layer between two electrodes.
Fig. 3 a is the diagrammatic sketch of conjugation organic semiconductor device according to an embodiment of the invention, said conjugation organic semiconductor device comprises one second electrode and one first electrode, clips the single conjugation organic buffer layer that is deposited on the organic deposit layer of individual layer conjugation between two electrodes.
Fig. 3 b is the diagrammatic sketch of conjugation organic semiconductor device according to an embodiment of the invention, said conjugation organic semiconductor device comprises a plurality of second electrodes and a plurality of first electrode (can't see) from figure, clip the single conjugation organic buffer layer that is deposited on the organic deposit of individual layer conjugation between two electrodes.
Fig. 4 a is the diagrammatic sketch of conjugation organic semiconductor device according to an embodiment of the invention, said conjugation organic semiconductor device comprises one second electrode and one first electrode, clips the organic deposit of multilayer conjugation that is printed on a plurality of conjugation organic buffer layers between two electrodes.
Fig. 4 b is the diagrammatic sketch of conjugation organic semiconductor device according to an embodiment of the invention, said conjugation organic semiconductor device comprises a plurality of second electrodes and a plurality of first electrode (can't see) from figure, clip the organic deposit of multilayer conjugation that is printed on a plurality of conjugation organic buffer layers between two electrodes.
Fig. 5 a is the diagrammatic sketch of conjugation organic semiconductor device according to an embodiment of the invention, said conjugation organic semiconductor device comprises one second electrode and one first electrode, clips a plurality of conjugation organic buffer layers that are deposited on the organic deposit of multilayer conjugation between two electrodes.
Fig. 5 b is the diagrammatic sketch of conjugation organic semiconductor device according to an embodiment of the invention, said conjugation organic semiconductor device comprises a plurality of second electrodes and a plurality of first electrode (can't see) from figure, clip a plurality of conjugation organic buffer layers that are deposited on the organic deposit of multilayer conjugation between two electrodes.
Fig. 6 is the diagrammatic sketch of conjugation organic semiconductor device according to an embodiment of the invention, and said conjugation organic semiconductor device comprises a plurality of second electrodes and a plurality of first electrode (can't see) from figure, clip single conjugation organic buffer layer between two electrodes.
Fig. 7 a is the diagrammatic sketch of conjugation organic semiconductor device according to an embodiment of the invention, said conjugation organic semiconductor device comprises one second electrode and one first electrode, clips the organic deposit of individual layer conduction/charge transfer conjugation that is printed on single conjugation organic buffer layer between two electrodes.
Fig. 7 b is the diagrammatic sketch of conjugation organic semiconductor device according to an embodiment of the invention, said conjugation organic semiconductor device comprises one second electrode and one first electrode, clips the single conjugation organic buffer layer that is deposited on the organic deposit of individual layer conduction/charge transfer conjugation between two electrodes.
Fig. 8 a is the diagrammatic sketch of conjugation organic semiconductor device according to an embodiment of the invention, said conjugation organic semiconductor device comprises one second electrode and one first electrode, clips the luminescent conjugated organic deposit of individual layer that is printed on the single-shot light conjugation organic buffer layer between two electrodes.
Fig. 8 b is the diagrammatic sketch of conjugation organic semiconductor device according to an embodiment of the invention, said conjugation organic semiconductor device comprises one second electrode and one first electrode, clips the single-shot light conjugation organic buffer layer that is deposited on the luminescent conjugated organic deposit of individual layer between two electrodes.
Fig. 9 is the diagrammatic sketch of conjugation organic semiconductor device according to an embodiment of the invention, said conjugation organic semiconductor device comprises one second electrode and one first electrode, clips the luminous and organic deposit of diffusion conjugation of the individual layer that is printed on the single-shot light conjugation organic buffer layer between two electrodes.
Figure 10 a is deposit organic mask, second electrode material, adhesive sheet according to an embodiment of the invention, so that form the diagrammatic sketch of a plurality of second electrodes on the conjugation organic semiconductor device.
Figure 10 b removes adhesive sheet and organic mask according to an embodiment of the invention, so that form the diagrammatic sketch of a plurality of second electrodes on the conjugation organic semiconductor device.
Figure 11 a is the diagrammatic sketch of the redness in passive matrix polychrome emission display, green and blue conjugation organic LED s according to an embodiment of the invention.
Figure 11 b is the diagrammatic sketch of the redness in active matrix polychrome emission display, green and blue conjugation organic LED s and oxide-semiconductor control transistors according to an embodiment of the invention.
Figure 12 a is when showing according to an embodiment of the invention the luminescent conjugated organic blended material of introducing variable concentrations in luminescent conjugated organic buffer layer, the curve chart that the glow color of conjugation organic LED changes.
Figure 12 b be show according to an embodiment of the invention no matter be incorporated in the luminescent conjugated organic buffer layer luminescent conjugated organic blended concentration of material how, the curve chart of the I-V characteristic that the conjugation organic LED keeps.
Figure 13 a utilizes the silica separator to be formed for the diagrammatic sketch of the conjugation organic LED s array of polychrome emission display according to an embodiment of the invention.
Figure 13 b utilizes the silica separator to be formed for the end view of the conjugation organic LED s array of polychrome emission display according to an embodiment of the invention
Figure 14 a has showed the situation of making LEL according to an embodiment of the invention.
Figure 14 b is the end view that the LEL shown in Figure 14 a makes.
Figure 15 is typical brightness-voltage (L-V) curve chart that has and do not have the device of the organic deposit of conjugation, shows to come from according to an embodiment of the invention strengthening the property of the organic deposit of conjugation that adds.
Figure 16 a has showed according to an embodiment of the invention the level Four gray scale that is limited by the luminous point density that is used to produce luminescent image.
Figure 16 b is the brightness curve figure of typical relation between the gray scale luminous point density of expression brightness and Figure 16 a.
Figure 17 a is the artificial nose that has the conductive finger aspect according to an embodiment of the invention.
Figure 17 b is the artificial nose that has the fluorescence indication item according to an embodiment of the invention.
Figure 18 a, 18b and 18c are the examples that is applicable to the typical organic compound of resilient coating and ink jet printing deposit.
Detailed description of the preferred embodiments
In following introduction,, can realize that with illustration the mode of particular of the present invention shows among the figure with reference to each accompanying drawing that constitutes a part of the present invention to preferred embodiment.Should be understood that and under the situation of the scope that does not deviate from the preferred embodiment of the invention, can utilize other embodiment, and also can change on the structure.
The conjugation organic substance has the advantage of low-cost processing, and is pliable and tough, in light weight, and has conventional organic large-scale processing, and has the general semiconductive characteristic of inorganic semiconductor.Fig. 1 shows conjugation organic semiconductor device 10 according to an embodiment of the invention.In conjugation organic semiconductor device 10, utilize conventional deposition technology, on substrate 12, form first electrode 14 that constitutes by metal or metal oxide.Substrate 12 can and have the solid material such as metallic plate of thin dielectric layer or for example plastics and the flexible materials such as metal forming that have thin dielectric layer on it constitute by for example glass, plastics, semiconductor wafer on it.In preferred embodiments, first electrode 14 is made of tin indium oxide (ITO).Then, utilize spin-coating method, heat sublimation method or other conventional applying method, on first electrode 14, form the basic conjugation organic buffer layer 16 uniformly of thick about 1-1000nm.Then, with IJP 18, on conjugation organic buffer layer 16, print the organic deposit 20 of one deck conjugation at least.Adopting IJP is because different with spin coating, IJP can print the organic deposit 20 of conjugation of micron resolution, because the organic deposit 20 of conjugation vertically is sprayed on the surface of conjugation organic buffer layer 16, rather than level trickling, so, IJP is more insensitive to dust and defect of substrate, and does not waste more materials during applying technology.
Shown in Fig. 2 a, then, utilize the common metal deposition technology, on organic deposit 20 of conjugation and conjugation organic buffer layer 16, deposit second electrode 22.Because conjugation organic buffer layer 16 insulating properties are strong, 14 at second electrode 22 and first electrode can not be short-circuited.
In the alternate embodiment of the present invention shown in Fig. 3 a, on first electrode 14, directly utilize the organic deposit 20 of IJP deposit conjugation.Then, utilize spin coating or other conventional applying method, on the organic deposit 20 of conjugation and first electrode 14, form conjugation organic buffer layer 16.Then, utilize the common metal deposition technology, deposit second electrode 22 on conjugation organic buffer layer 16.
In the other alternate embodiment shown in Fig. 4 a and the 5a, can form the organic deposit 20 of multilayer conjugation organic buffer layer 16 and multilayer conjugation, increased vertical or three-dimensional dimension, improved the functional density of semiconductor device.
Although Fig. 2 is a, 3a, 4a and 5a show the embodiment with one first electrode 14 and one second electrode 22, but in the alternate embodiment of the present invention shown in Fig. 2 b, 3b, 4b, the 5b and 6, can be on the organic deposit 20 of each conjugation, the deposit a plurality of first (14) and second (22) electrode.Do not show a plurality of first electrodes 14 although it should be noted that the diagrammatic sketch of Fig. 2 b, 3b, 4b and 5b and 6, can intersect to form (end view in Fig. 2 b, 3b, 4b, 5b and 6 can be seen) with a plurality of second electrodes 22.
In the embodiment of Fig. 6, a plurality of first electrodes 14 (from figure, can't see) by ink jet printing to substrate 12.Then, utilize spin coating or other conventional applying method, on a plurality of first electrodes 14, form conjugation organic buffer layer 16.Then, on conjugation organic buffer layer 16, a plurality of second electrodes 22 of ink jet printing.
In the alternate embodiment of the present invention shown in Fig. 7 a and the 7b, for the purpose of discussing, only show an organic deposit 20 of conjugation, the organic deposit 20 of conjugation comprises conduction or electric charge transmitting material.Owing to compare with electrode material, the organic deposit 20 of conduction/charge transfer conjugation has electric charge injection properties preferably, so when voltage is added on second electrode 22 and first electrode 14, electric current 24 flows at second electrode 22 and 14 at first electrode, and by only having printed the conjugation organic buffer layer 16 of conduction/organic deposit 20 of charge transfer conjugation thereon.
In various organic semiconductor devices, electroluminescence (EL) device is especially noticeable, and this is because their potential application aspect following light source, list or multicolor display, LELs, polychrome ballistic device, greeting card and low and high density information display.So in another alternate embodiment, first electrode 14 and substrate 12 are transparent, conjugation organic buffer layer 16 comprises luminescent material.In these embodiments, the electric current 24 by conjugation organic buffer layer 16 causes from luminous 32 of conjugation organic semiconductor device 10.
In the alternate embodiment of the present invention shown in Fig. 8 a and the 8b, for the purpose of discussing, only show an organic deposit 20 of conjugation, organic deposit 20 of conjugation and conjugation organic buffer layer 16 are made of luminous organic material, and first electrode 14 and substrate 12 are transparent.When sufficiently high voltage was added on second electrode 22 and first electrode 14, electric current 24 flowed at second electrode 22 and 14 at first electrode, and by conjugation organic buffer layer 16.In the zone that does not have the organic deposit 20 of conjugation, conjugation organic buffer layer 16 will send colourama (index mark 26) according to the composition of conjugation organic buffer layer 16.In the zone that the organic deposit 20 of conjugation is arranged, luminous color will depend on compound (recombine) in electronics and hole.In general, if the organic deposit 20 of conjugation is enough thick, electronics and hole will be compound in the organic deposit 20 of conjugation, and luminous color (index mark 32) will depend on the composition of the organic deposit 20 of conjugation.If the organic deposit 20 of conjugation is enough thin, then electronics and hole are compound in conjugation organic buffer layer 16, and luminous color depends on the composition of conjugation organic buffer layer 16.Yet, if the thickness of the organic deposit 20 of conjugation is roughly identical with conjugation organic buffer layer 16, then electronics will be compound at the boundary vicinity of organic deposit 20 of conjugation and conjugation organic buffer layer 16, the luminous color that can comprise the composition that depends on organic deposit 20 of conjugation and conjugation organic buffer layer 16.
In alternate embodiment of the present invention shown in Figure 9, for the purpose of discussing, only show an organic deposit 20 of conjugation, the organic deposit 20 of conjugation comprises the conjugated organic materials that can partly be diffused in the conjugation organic buffer layer 16.Conjugation organic buffer layer 16 comprises poly--9-vinylcarbazole (PVK) or poly-fluorenes (polyfluorene, PF) or other similar compound, the organic deposit 20 of conjugation comprise can contain intermingle with (p-phenylene vinyl) (PPV), MEH-PPV, organic pigment, PF derivative or other similar compound.In these embodiments, the organic deposit 20 of the conjugation of conducting electricity on a small quantity will be diffused into (index mark 30) in the conjugation organic buffer layer 16, and image charge transmits, and dopant is the same to work in conjugation organic buffer layer 16.Object dopant (the organic deposit 20 of conjugation) spreads in main body buffer layer (conjugation organic buffer layer 16), is the effect of the material behavior of Subjective and Objective material and the solvent compatibility of Subjective and Objective material (polarity or nonpolar).Only need small amounts of dopants, promote the energy delivery from the main body to the object, in the time of on voltage being added on second and first electrode 22 and 14, in the zone of the organic deposit 20 of conduction conjugation, produce electric current 24 at second electrode 22 and 14 at first electrode.
In the other alternate embodiment, conjugation organic buffer layer 16 and the organic deposition materials of conjugation that can partly be diffused in the conjugation organic buffer layer 16 are luminous, and first electrode 14 and substrate 12 are transparent.When the electric current 24 by conjugation organic buffer layer 16 produces, organic deposit 20 parts of conjugation are diffused into the zone (index mark 30) of conjugation organic buffer layer 16 will send colourama according to the band gap and the energy level of the material that comprises organic deposit 20 of conjugation and conjugation organic buffer layer 16.In general, if the band gap of the organic deposition materials of conjugation less than the band gap of conjugation organic buffer layer, energy level is lower than the energy level of conjugation organic buffer layer, then luminous color (index mark 28) will depend on the composition of the organic deposit 20 of conjugation.Otherwise luminous color depends on the composition of conjugation organic buffer layer 16.
Also can utilize IJP, on the organic deposit 20 of each conjugation, form a plurality of first and second electrodes (14 and 22), shown in Fig. 2 b, 3b, 4b, 5b and 6.Shown in Figure 10 a,, utilize IJP, at first deposit organic mask 72 on conjugation organic buffer layer 16 for forming a plurality of second electrodes 22 of Fig. 2 b.Then, utilize spin-coating method or other conventional applying method, on organic mask 72 and conjugation organic buffer layer 16, deposit second electrode material 74.Select second electrode material 74 and the material that is included in the organic mask 72, second electrode material 74 is bonded on the conjugation organic buffer layer 16 securely, the material that is included in simultaneously in the organic mask 72 is bonded on the conjugation organic buffer layer 16 insecurely.Then, on second electrode material 74, press for example adhesive sheet 76 of adhesive tape securely.When removing adhesive sheet 76, shown in Figure 10 b, the different adhesivenesss of second electrode material 74 and organic mask 72 make organic mask 72 and part second electrode material 74 be removed with adhesive sheet 76.All the other second electrode materials 74 comprise a plurality of second electrodes 22.This method that forms a plurality of second electrodes 22 also can be applicable to a plurality of first and second electrodes 14 and 22 of Fig. 3 b, 4b, 5b and 6.
Each embodiment of the present invention provides the method that forms micron-scale organic LED s regular array, and wherein the size of LEDs only is subjected to the restriction of IJP nozzle.A kind of application of conjugation organic LED s regular array is polychrome such as a television screen or computer display emission display for example, wherein is used to produce coloured image with the red, green and blue point.Shown in Figure 11 a, in band gap and energy level on the conjugation organic buffer layer 40 corresponding to blue light, each band gap and energy level of deposit is corresponding to the several different luminous of red, green and blue look and the organic deposit 34,36 and 38 of diffusion conjugation.Luminous and the diffusion organic deposit 34,36 of conjugation and 38 parts are diffused in the resilient coating 40, change the EL spectrum of resilient coating 40, so that when voltage is added on second and first electrode 22 and 14, luminous and the diffusion the organic deposit 34,36 of conjugation and 38 below resilient coating 40 with red-emitting 42, green glow 44 and blue light 46.By making alive on each second electrode 22 and first electrode 14 optionally, can each red, green and blue LEDs of switch, and make passive matrix polychrome emission display.
In the alternate embodiment shown in Figure 11 b, show active matrix polychrome emission display.Utilize IJP or other conventional deposition technology, a plurality of grids 92 of contact deposit with it on substrate 12.On a plurality of grids 92, make and have insulating material 50, source electrode 90 and 88 the transistor 48 of draining.Then, utilize spin-coating method or other conventional applying method, deposit conjugation organic buffer layer 40 on transistor, conjugation organic buffer layer 40 contacts with drain electrode 88.Then, on conjugation organic buffer layer 40, the luminous and organic deposit 34,36 and 38 of diffusion conjugation of ink jet printing.At last, one second electrode 22 of deposit on luminous and the diffusion organic deposit 34,36 of conjugation and 38.Electric current spreads the luminous voltage control that is subjected on the grid end 52 of conjugation organic buffer layer 40 by source electrode 90, transistor 48, conjugation resilient coating 40, the organic deposit 34,36 of conjugation and 38 and second electrode.It should be noted that Figure 11 b is exemplary, alternate embodiment of the present invention can adopt other method of making transistor base active matrix multicolor display.
In general, with identical or (for example than the luminescent material of low band gaps and energy level, the organic deposit 34,36 and 38 of the red, green, blue of Figure 11 a) mix have higher band gap and energy level luminescent material (for example, the blue light resilient coating 40 of Figure 11 a) time, when biasing, the gained material production is than the color of low band gaps and energy level material.In preferred embodiments, need be less than about 25% dopant material and be diffused in the resilient coating 40, to realize the change of this color.As shown in the figure, when Figure 12 a showed the MEH-PPV that introduces variable concentrations in polymer system, how poly-(to phenylene) (PPP) glow color of LED changed.Figure 12 b show no matter the concentration of MEH-PPV how, the I-V characteristic keeps identical situation.
In the other alternate embodiment shown in Figure 13 a and the 13b, utilize the silica (SiO that is arranged on the transparent substrate 12 that is printed with pre-composition column electrode 56 2) or polymer separator 54, make red, green and blue LEDs.SiO 2Separator 54 allows directly IJP conjugation organic buffer layer 16 and red, green, blue conduction/ charge transfer polymer 34,36 and 38 on column electrode 56, and is used as the mask of deposit second electrode 22.
The Another Application of luminescent conjugated organic semiconductor device 10 is organic LELs and monochrome or polychrome ballistic device, and wherein IJP is controlled to be printing conductive/charge transfer conjugated organic materials figure.Opposite with multicolor display, color graphics, as the observer see constant variation, LELs and monochrome or polychrome ballistic device generally comprise big but the emitter region of constant color.For forming this device, directly conjugation organic buffer layer 16 (see Fig. 7 a) go up or in alternate embodiment directly on transparent first electrode 14 (seeing Fig. 7 b), printing conductive/charge transfer and/or luminescent conjugated organic deposit 20.The figure of the organic deposit 20 of conjugation limits the luminous zone.By at second electrode 22 and 14 making alives of first electrode, LELs can be luminous.Because electric current flows through the organic deposit 20 of conjugation, but carrying of can't help, the organic deposit 20 of conjugation can have cut-off point (physical isolation figure).By regulating bias voltage, can obtain to have the LELs of high-contrast, and the brightness of LEL can be from tens candelas (cd)/m with background 2Arrive greater than 100cd/m 2Wide range in regulate.
The LEL that Figure 14 a shows according to a preferred embodiment of the present invention makes.At first, utilize washing agent, deionization (DI) water, acetone and ethanol successively, the ITO electrode 58 that is deposited on the glass substrate 60 is carried out customary ultrasonic waves for cleaning, wash surface contamination off.Then, cure ITO electrode 58 and glass substrate at elevated temperatures 60 about 12 hours.Then, use IJP, by 3, the aqueous solution of 4-polyethylene dioxythiophene-polystyrolsulfon acid ester (PEDOT), deposit conducting polymer sign 62 on ITO electrode 58.Then, under about 100 ℃ temperature, air drying PEDOT conducting polymer sign 62 about 12 hours.In an alternative embodiment, can use other method of deposit PEDOT conducting polymer sign 62, for example people such as J.A.Rogers is at Adv.Materials the 9th volume, the die pressing of introducing in " micro-contact printing on bent substrate and plating: the manufacturing of independent three-dimensional metal micro structure " literary composition among the 475-477 (1997) is quoted the document here.Shown in Figure 14 b, then, on PEDOT conducting polymer sign 62, change (RPM) with per minute about 2500, spin coating is by the MEH-PPV resilient coating 64 of about 1% MEH-PPV formulations prepared from solutions, and on MEH-PPV resilient coating 64 deposit calcium (Ca) cathode material 66.With the active cathodic region of epoxy resin bonding and aluminium or cover glass 68, thereby seal the device of finishing.It should be noted that this manufacturing process also can be with other material that has with above-mentioned certain material similar characteristics.
Figure 15 has showed typical brightness-voltage (L-V) curve that has (index mark 70) and do not have the device of (index mark 78) PEDOT conductive polymer coating, shows strengthening the property of the PEDOT conductive polymer coating that has benefited from adding.For example, when device was worked under 5V, the LEDs with PEDOT conductive polymer coating can produce and be about 200cd/m 2Brightness, and do not have the LEDs of PEDOT conductive polymer coating to produce brightness about little 3 orders of magnitude.
In alternate embodiment of the present invention, the application-specific of LELs can be used for producing the gray scale luminescent image.Figure 16 a shows the level Four gray scale 80 that the density by luminous point limits, and Figure 16 b shows the brightness curve 82 of typical relation between expression brightness and luminous point density.By changing spot definition or dot density, can regulate the gray scale of utilizing each embodiment of the present invention continuously.
Except that organic EL sign and display, each embodiment of the present invention also can be applicable to other organic electronic and opto-electronic device.Example has transistor, photovoltaic cell, emulation nose, physical device, chemical device, biological device and electronic integrated circuit, but is not limited to these.Physical device comprises optical sensor (array), X-ray detector (array), imageing sensor (array), photodetector and photovoltaic device etc., but is not limited to these.Chemical device comprises gas sensor (array) and humidity (solvent) transducer, but is not limited to these.The bio-sensing device comprises transducers such as being used to survey blood sugar (glucose), enzyme, but is not limited to these.In addition, IJP is provided on the semiconductor wafer and makes LEDs as being used in the chips such as computer, communication device and the effective means of the light source of the outer contact of chip.Be applicable to that material that embodiment of the present invention is patterned into electronic device comprises organic conjugated molecule, conjugated polymer, inorganic nanocrystal, organic nano crystal, pigment molecule, and their combination, but be not limited to these.As discussed previously, that these devices can provide is luminous, the output of conduction or fluorescence form.
Do to use conduction or fluorescence illustrated example with artificial nose (artificial nose) as the embodiment of the present invention of indication item form.Shown in Figure 17 a, utilize previous described technology, on substrate 12, form organic deposit 20 of multilayer conjugation and conjugation organic buffer layer 16.Yet, before the IJP of the organic deposit 20 of each conjugation, two electrodes 84 are set, the organic deposit 20 of conjugation is formed on two electrodes 84.The organic deposit 20 of each conjugation can be made of unique material, so that when fluid or steam sample 86 are diffused in conjugation organic buffer layer 16 and the organic deposit 20 of conjugation, the conductivity of the organic deposit 20 of each conjugation changes.The conductivity of the organic deposit 20 of each conjugation is surveyed by two electrodes 84 in the organic deposit 20 of conjugation.The organic deposit 20 of a plurality of conjugation on every layer can provide the conductivity " feature " of the chemical composition that can be used for discerning fluid or steam sample 86.In other alternate embodiment, a plurality of conjugation organic buffer layers 16 can be made of unique material, so that each conjugation organic buffer layer 16 is as fluid or steam barrier film.So every layer of organic deposit 20 of conjugation can be designed to only test a kind of fluid or steam of particular category, and the fluid of other classification or steam will be leached by a plurality of conjugation organic buffer layers 16.
In alternate embodiment of the present invention shown in Figure 17 b, the organic deposit 20 of a plurality of conjugation fluoresces under certain conditions, and does not have electrode in the organic deposit 20 of conjugation.The organic deposit 20 of each conjugation can be made of unique material, so that when fluid or steam sample 86 were diffused in conjugation organic buffer layer 16 and the organic deposit 20 of conjugation, the fluorescence of the organic deposit 20 of each conjugation can change.By using ultraviolet (UV) light irradiation device, can detect the fluorescence of the organic deposit of each conjugation.The organic deposit 20 of a plurality of conjugation on every layer can be provided for discerning the fluorescence " feature " of fluid or steam sample 86 chemical compositions.In other alternate embodiment, a plurality of conjugation organic buffer layers 16 can be made of unique material, so that each conjugation organic buffer layer 16 is as fluid or steam barrier film.So every layer of organic deposit 20 of conjugation can be designed to only test a kind of fluid or steam of particular category, and the fluid of other classification or steam will be leached by a plurality of conjugation organic buffer layers 16.
Therefore, according to above-mentioned introduction, each embodiment of the present invention provides a kind of method of utilizing ink-jet printing technology to make organic semiconductor device, and the device of system and this system of introducing, this method is more insensitive for the substrate surface defective, and combine conventional semi-conductive electricity and optical property and low-cost processability, pliable and tough, in light weight and have a conventional organic large-scale processing.In addition, each embodiment of the present invention allows accurately to form monochrome or polychrome emission display, device, sign and the gray level image of composition, comprises isolating the emitter region.Each embodiment of the present invention can also form makes semiconductor device, biology sensor, photovoltaic device and the contour quality mask of photodetector.
For the purpose of illustration and introduction, the preferred embodiments of the invention have been introduced above.Do not want the present invention exhaustively to disclosed precise forms, or limit the invention to these precise forms.Scope of the present invention can't help that these are introduced in detail and limit, and is defined by the following claims.

Claims (28)

1, a kind of semiconductor device in response to driving source generation indication item, this semiconductor device comprises:
Support the substrate of this semiconductor device;
At least one first electrode by substrate support;
By at least one second electrode of substrate support, be used between at least one first electrode and at least one second electrode, producing electric current;
Be supported at least one first electrode and at least one second interelectrode at least one conjugation organic buffer layer, be used to regulate this at least one first electrode and this at least one second interelectrode electric current; And
The organic deposit of at least one ink jet printing conjugation, this deposit contacts with a conjugation organic buffer layer at least, and be positioned between this at least one first electrode and this at least one second electrode, be used to produce the indication item that forms in driving source by semiconductor device responds.
2, according to the device of claim 1, wherein the organic deposit of at least one conjugation comprises electric conducting material, be used in response to the voltage drive source that is added at least one first electrode and at least one second electrode, make electric current pass through the conjugation deposit and by at least one conjugation organic buffer layer.
3, according to the device of claim 2, wherein this substrate and at least one first electrode are transparent, and at least one conjugation organic buffer layer is by constituting by luminous material when electric current flows through this material.
4, according to the device of claim 2, wherein this substrate and at least one first electrode are transparent, and the organic deposit of at least one conjugation is by constituting by luminous material when electric current flows through this material.
5, according to the device of claim 1, wherein this substrate and at least one first electrode are transparent, the organic deposit of at least one conjugation is made of the guest materials that can become luminous, at least one conjugation organic buffer layer is the material of main part that can become luminous, and, guest materials partly is diffused in the material of main part
Guest materials has the band gap and the energy utmost point that is not more than material of main part, make this semiconductor device responds in the voltage drive source that is added at least one first electrode and at least one second electrode, luminous according to guest materials, make electric current flow through at least one first electrode and at least one second interelectrode guest materials and material of main part.
6, according to the device of claim 5, comprising the organic deposits of many group conjugation, every group comprises three by the organic deposit of conjugation that can guest materials rubescent, green and blue light constitutes.
7, according to the device of claim 5, wherein at least one conjugation organic buffer layer is made of poly-fluorene derivative, the organic deposit of at least one conjugation constitutes by containing intermingle with (to the phenylene vinyl) derivative and poly-fluorene derivative, and this at least one first electrode is made of tin indium oxide.
8, a kind of semiconductor device in response to driving source generation indication item, this semiconductor device comprises:
Support the substrate of this semiconductor device;
A plurality of source electrodes by this substrate support are used to produce electric current;
A plurality of grids by this substrate support are used to control said electric current,
Be supported in a plurality of source electrodes and be used to control a plurality of transistors between a plurality of grids of said electric current, each transistor has the source end that is coupled to source electrode, is coupled to the grid end of grid, and drain terminal;
By second electrode that a plurality of transistors support, be used for promoting at a plurality of transistorized drain terminals and the second interelectrode electric current;
Be supported on a plurality of transistors and the second interelectrode conjugation organic buffer layer, this resilient coating contacts with second electrode with a plurality of transistorized drain terminals, is used to be adjusted in a plurality of transistorized drain terminals and the second interelectrode electric current; And
By the organic deposit of a plurality of ink jet printing conjugation that each transistor supports, this deposit contacts with the conjugation organic buffer layer, is used to produce the indication item that is formed in driving source by semiconductor device responds.
9, a kind of semiconductor device in response to driving source generation indication item, this semiconductor device comprises:
The substrate of support semiconductor device;
By at least one conjugation organic buffer layer of this substrate support, be used to filter fluid stream; And
The organic deposit of at least one ink jet printing conjugation, this deposit is arranged at least one conjugation organic buffer layer, is used to produce the indication item that is formed in driving source by this semiconductor device responds.
10, according to the device of claim 9, wherein the organic deposit of each conjugation sends fluorescence in response to the driving source that is diffused into the fluid sample in the organic deposit of conjugation.
11, according to the device of claim 9, also comprise first and second electrode pairs that are arranged in the organic deposit of each conjugation, be used to survey the conductivity of the organic deposit of conjugation, wherein the conductivity of the organic deposit of each conjugation changes in response to the driving source that is diffused into the fluid sample in the organic deposit of conjugation.
12, a kind of manufacturing can produce the method for the semiconductor device of indication item in response to driving source, and this method comprises:
At at least one first electrode of substrate upper support;
At at least one at least one conjugation organic buffer layer of the first electrode upper support, make a conjugation organic buffer layer contact with each first electrode;
The organic deposit of at least one conjugation of ink jet printing at least one first electrode makes the organic deposit of each conjugation contact with at least one conjugation organic buffer layer; And
At least one second electrode of conjugation organic buffer layer upper support in the superiors.
13, according to the method for claim 12, wherein the step at least one second electrode of conjugation organic buffer layer upper support of the superiors may further comprise the steps:
On the superiors' conjugation organic buffer layer, at least one organic mask of ink jet printing, and make it to contact with the said the superiors, when the superiors conjugation organic buffer layers contacts, at least one organic mask has low bonding strength;
On at least one organic mask and the superiors' conjugation organic buffer layer, support second electrode material, make it to contact with the superiors conjugation organic buffer layers with said organic mask, when contacting with this at least one organic mask with this superiors' conjugation organic buffer layer, said second electrode material has high bonding strength;
On second electrode material, add adhesive sheet; And
Remove this adhesive sheet, wherein also will remove this at least one organic mask and second electrode material on this at least one organic mask.
14, according to the method for claim 12, wherein the step at the superiors' at least one second electrode of conjugation organic buffer layer upper support may further comprise the steps:
Utilize separator, shelter zone that part of the superiors conjugation organic buffer layer of not deposit second electrode material; And
Ink jet printing second electrode material between separator.
15, a kind of manufacturing can produce the method for the semiconductor device of indication item in response to driving source, and this method comprises:
At a plurality of source electrodes of substrate upper support;
At a plurality of grids of substrate upper support;
Support a plurality of transistors between a plurality of source electrodes and a plurality of grid, each transistor has the source end that is coupled to source electrode, grid end and the drain terminal that is coupled to grid;
At a plurality of transistor upper support second electrodes;
Between a plurality of transistors and second electrode, support the conjugation organic buffer layer, this conjugation organic buffer layer is contacted with second electrode with a plurality of transistorized drain terminals;
On each transistor, the organic deposit of a plurality of conjugation of ink jet printing makes that the organic deposit of these a plurality of conjugation contacts with second electrode with the conjugation organic buffer layer.
16, a kind of manufacturing can produce the method for the semiconductor device of indication item in response to driving source, and this method comprises:
The organic deposit of at least one conjugation of ink jet printing on substrate; And
At the organic deposit upper support first conjugation organic buffer layer of each conjugation, the organic deposit of each conjugation is contacted with the first conjugation organic buffer layer.
17, according to the method for claim 16, wherein carry out the step of the organic deposit of at least one conjugation of ink jet printing on substrate, this method also is included in the step of at least one first electrode of substrate upper support and second electrode pair, make the organic deposit of each conjugation by ink jet printing on first electrode and second electrode pair.
18, according to the method for claim 16, further comprising the steps of:
On the first conjugation organic buffer layer, an extra play of the organic deposit of at least one conjugation of ink jet printing; And
On each extra play of the organic deposit of at least one conjugation, support an additional conjugation organic buffer layer, make each extra play of the organic deposit of a plurality of conjugation contact with additional conjugation organic buffer layer.
19, according to the method for claim 18, wherein, carry out on the first conjugation organic buffer layer, the step of at least one extra play of the organic deposit of at least one conjugation of ink jet printing, this method also is included in the step of organic slow station layer at least one first electrode of upper support of first conjugation and second electrode pair, make the organic deposit of each conjugation by ink jet printing on first electrode and second electrode pair.
20, a kind of emission system of display of visually image, this emission system comprises:
Support the substrate of emission system;
At least one first electrode by this substrate support;
By at least one second electrode of this substrate support, be used for producing electric current between at least one first electrode and this at least one second electrode at this;
Be supported on this at least one first electrode and this at least one second interelectrode at least one conjugation organic buffer layer, be used to regulate said electric current;
The organic deposit of the conjugation of a plurality of ink jet printings, the organic deposit of each conjugation contacts with at least one conjugation organic buffer layer, and be positioned between one first electrode and one second electrode, produce indication item when being used for being added on this first electrode and this second electrode in the voltage drive source; And
Voltage source is used at this selectivity making alive driving source at least one first electrode and this at least one second electrode.
21, according to the system of claim 20, wherein substrate and at least one first electrode are transparent, the organic deposit of a plurality of conjugation is made of electric conducting material, be used in response to being added on the voltage drive source, make local current pass through the organic deposit of at least one conjugation and each conjugation organic buffer layer by contacting with the organic deposit of conjugation, wherein at least one conjugation organic buffer layer luminous luminescent material when flowing through this conjugation organic buffer layer at electric current constitutes.
22, according to the system of claim 21, wherein print at least one group of organic deposit of contiguous conjugation, when electric current flow through at least one conjugation organic buffer layer, the contiguous organic deposit of conjugation of each group formed luminous sign.
23, according to the system of claim 21, wherein the different organic deposits of conjugation is organized in printing more, every group has the organic deposit density of substantially invariable conjugation, and when electric current flow through at least one conjugation organic buffer layer, printed many groups formed the gray scale luminescent image.
24, according to the system of claim 20, wherein substrate and at least one first electrode are transparent, the organic deposit of a plurality of conjugation is arranged in the regular array of the organic deposit group of conjugation, every group comprises three by the organic deposit of conjugation that can guest materials rubescent, green and blue light constitutes, when electric current flow through the organic deposit of conjugation, regular array constituted multicolor luminous display.
25, according to the system of claim 20, wherein substrate and at least one first electrode are transparent, the organic deposit of a plurality of conjugation is made of the guest materials that can become luminous, at least one conjugation organic buffer layer is the material of main part that can become luminous, guest materials partly is diffused in the material of main part, and
The organic deposit of wherein a plurality of conjugation is arranged in the regular array of the organic deposit group of conjugation, every group comprises three by the organic deposit of conjugation that can guest materials rubescent, green and blue light constitutes, guest materials has the band gap and the energy utmost point that is not more than material of main part, make when the making alive driving source, every group of rubescent, green and blue light
When electric current flow through the organic deposit of conjugation, regular array constituted multicolor luminous display.
26, a kind of emission system of display of visually image, this emission system comprises:
Support the substrate of emission system;
A plurality of source electrodes by this substrate support are used to produce electric current;
A plurality of grids by this substrate support are used to control said electric current,
Be supported in a plurality of source electrodes and be used to control a plurality of transistors between a plurality of grids of said electric current, each transistor has the source end that is coupled to source electrode, is coupled to the grid end of grid, and drain terminal;
Second electrode by a plurality of transistors support is used to promote a plurality of transistorized drain terminals and the second interelectrode electric current;
Be supported on a plurality of transistors and the second interelectrode conjugation organic buffer layer, this resilient coating contacts with second electrode with a plurality of transistorized drain terminals, is used to regulate a plurality of transistorized drain terminals and the second interelectrode electric current;
Be supported in the organic deposit of a plurality of ink jet printing conjugation on each transistor, this deposit contacts with the conjugation organic buffer layer, when being used for being added on the source electrode and second electrode in the voltage drive source, produces indication item; And
Be electrically coupled to the voltage source of emission system, be used for selectivity making alive driving source on a plurality of source electrodes and second electrode.
27, according to the system of claim 26, wherein substrate and at least one first electrode are transparent, the organic deposit of a plurality of conjugation is arranged in the regular array of the organic deposit group of conjugation, every group comprises three by the organic deposit of conjugation that can guest materials rubescent, green and blue light constitutes, when electric current flow through the organic deposit of conjugation, regular array constituted multicolor luminous display.
28, according to the system of claim 26, wherein substrate and at least one first electrode are transparent, the organic deposit of a plurality of conjugation is made of the guest materials that can become luminous, at least one conjugation organic buffer layer is the material of main part that can become luminous, guest materials partly is diffused in the material of main part, and
The organic deposit of wherein a plurality of conjugation is aligned to the regular array of the organic deposit group of conjugation, every group comprises three by the organic deposit of conjugation that can guest materials rubescent, green and blue light constitutes, guest materials has the band gap and the energy utmost point that is not more than material of main part, make when the making alive driving source, every group of rubescent, green and blue light
When electric current flow through the organic deposit of conjugation, regular array constituted multicolor luminous display.
CN98811747A 1997-10-17 1998-10-14 Process for fabricating organic semiconductor devices using ink-jet printing technology and device and system employing same Pending CN1280708A (en)

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