JP2003257654A - Image display device and method of manufacturing the device - Google Patents

Abstract

<P>PROBLEM TO BE SOLVED: To achieve an accurate pattern transfer on a substrate having irregularities. <P>SOLUTION: Screen masks having mesh parts or openings are disposed on the substrate at specified gaps, and ink is filled in the mesh parts or the openings. Gas is supplied from the upper part thereof to transfer the ink at a predetermined position on the substrate. Thus an accurate pattern can be formed on the substrate without contaminating the surface of the substrate. <P>COPYRIGHT: (C)2003,JPO

Description

Detailed Description of the Invention

[0001]

BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to an image display device and a manufacturing method thereof, and more particularly to a pattern transfer method for forming a pattern on a substrate or the like.

[0002]

2. Description of the Related Art In recent years, image display devices have been used as devices for displaying high-level video information such as personal computers, digital satellite broadcasts and DVDs. The demand for flat panel displays tends to increase in place of CRTs that require a particularly large installation area. The flat panel display includes a liquid crystal display, a plasma display, an organic EL panel, etc., but further spread, it is necessary to provide a high performance and low cost.

Regarding the organic electroluminescence device, a three-layer structure of a hole transport layer, a light emitting layer, and a cathode, which is a typical structure in Patent Document 1, and a double layer type in Patent Document 2, which serves as an electron transport layer and a light emitting layer, are disclosed. And a method that serves as both a hole transport layer and a light emitting layer are described. Patent Document 3 describes a three-layer structure in which a carrier block layer is interposed between an electron transporting layer and a hole transporting layer so that the electron transporting light emitting layer and the hole transporting light emitting layer function separately. ing.

There is also a bipolar light emitting layer that transports with electrons and holes. If an excellent and highly efficient light emitting material is found for the bipolar light emitting layer, the simplest single layer type device including one organic layer becomes possible. in this way,
The function of the organic electroluminescence device can be controlled by changing the structure of the light emitting layer.

On the other hand, a liquid crystal display is composed of a glass substrate on which a TFT circuit is formed, a color filter for coloring and a glass substrate on which transparent electrodes are formed on the entire surface.
A liquid crystal panel containing a liquid crystal is sandwiched between polarizing plates that allow only light that vibrates in one direction to pass through, and a backlight that uses cold cathode tubes is placed outside the polarizing plate on the glass substrate side on which the TFT circuit is formed. The control circuit for controlling the TFT circuit, the printed circuit board on which electronic circuits such as a driving circuit are mounted, and the inverter circuit for controlling the light source.

Among the components of the liquid crystal display, the color filter has a high specific gravity in terms of cost. The color filter has a layer of red (R), green (G), and blue (B) formed on the opening of a film called a black matrix which is formed on a glass substrate in a pattern such as a lattice and has an excellent light-shielding property. Is. Conventional color filter colorant forming methods are described in Patent Documents 4 and 5.

The production facilities are disclosed in Patent Documents 6 and 7.

[0008]

[Patent Document 1] Japanese Patent Publication No. 6-32307

[Patent Document 2] Japanese Patent No. 2879080

[Patent Document 3] Japanese Patent No. 2937015

[Patent Document 4] Japanese Unexamined Patent Publication No. 11-337726

[Patent Document 5] Japanese Patent Laid-Open No. 2002-243928

[Patent Document 6] Japanese Patent No. 2734464

[Patent Document 7] Japanese Unexamined Patent Publication No. 8-227276

[Patent Document 8] Japanese Patent Laid-Open No. 10-12377

[0009]

In order to realize a full color display in an organic electroluminescence device, fine patterning of red, green and blue is required for each pixel. There are many proposals for full-color systems, but ones that are actually being prototyped are as follows: (1) Selectively form red, green, and blue light-emitting elements using a shadow mask. It is presumed to be a method, (2) a method of combining red, green, and blue color filters and a white light emitting element, and (3) a method of obtaining red and green light emission from a blue light emitting element in a color conversion layer.

Each of these methods has advantages and disadvantages. For example, when arranging red, green, and blue organic light emitting layers on a substrate, a wet process such as photolithography cannot be used because it may melt the organic layers. Then, the method of selectively forming the red, green, and blue light-emitting elements in the vacuum vapor deposition tank by using the shadow mask for the organic layer is described in Patent Documents 6 and 7 described above. Since this method requires film formation in a vacuum deposition tank, there are problems in mass productivity such as production tact, equipment cost, and installation area.

On the other hand, in recent years, there has been a movement to use the ink jet printing used in office color printers for industrial production. The on-demand method using a piezo element is characterized in that ink droplets having a uniform and clean shape are accurately ejected, and is described in Patent Document 8. Patterning of luminescent polymer using this inkjet printing is low cost
It is drawing attention as a method of separately coating organic light emitting layers of three colors of green and blue on a substrate.

However, in the ink jet printing, the limit of the absolute position accuracy on the substrate side is about 100 microns, and the dot diameter also spreads to 60 to 80 microns on the substrate, so it is difficult to control the edge position accuracy. is there. In order to form a high-definition full-color display, further miniaturization of ink droplets is required. on the other hand,
Depending on the nature of the ink material used, the inkjet head must incorporate solvent resistant or acid resistant parts and special ink repellent parts. From the viewpoint of solvent resistance, it is difficult to use a commercially available printer for a long period of time. Further, the production apparatus requires not only ink ejection control but also a maintenance mechanism such as cleaning. Furthermore, in order to minimize the flight bending of the ink when ejecting the ink from the inkjet head and selectively applying the ink to the substrate,
There are problems such as the need to narrow the distance between the nozzle of the inkjet head and the substrate.

Therefore, instead of ink jet printing, a screen printing method is conceivable in which patterning is performed using a screen mask which has been conventionally used. Off-contact printing and contact printing are generally used as the screen printing method.

Off-contact printing is a printing method in which a gap (clearance) is set between a substrate and a screen mask, and when a squeegee passes, a paste is formed on the substrate through an opening of the screen mask. However, as the pitch becomes finer due to the gap, blurring and bridges are likely to occur.

In order to solve this problem, contact printing, which is printing without a gap, was devised. The purpose of contact printing is to bring the substrate and the screen mask into close contact with each other and prevent bleeding and bridging. However, in the case of contact printing, it is necessary to add a plate separating step for separating the substrate and the screen mask after forming the paste on the substrate through the opening of the screen mask.

Further, in the method of separately coating the organic light emitting layers of three colors of red, green and blue on the substrate by using ink jet printing, since a small amount of ink is applied in multiple times, the number of ink jet heads is increased. Although it is necessary to shorten the working time, the screen printing method can pattern the entire surface of the substrate in a short time. Furthermore, in order to realize a full-color display, red, green, and
In order to perform blue fine patterning, it is necessary to form red, green, and blue fine patterns in the recesses in the bank formed to separate pixels.

However, these screen printing methods are
Since the pattern is formed by bringing the substrate and the screen mask into close contact with each other, it is difficult to selectively form a fine pattern in the recess. Further, since the screen mask is brought into close contact with the substrate, dirt on the back surface of the screen mask may adhere to the substrate. Therefore, there is a problem in that the substrate and the screen mask do not come into contact with each other, and a fine pattern of red, green, and blue is formed in the concave portion in the bank formed for separating pixels.

The paste used in these screen printing methods has a paste viscosity of several thousand Pa · s in order to maintain the shape of the paste when formed on a substrate.
Must be moderately high. However, the luminescent polymer ink used in inkjet printing is a luminescent polymer dissolved in an organic solvent to a concentration of about 1%, and its viscosity is extremely low at about 10 mPa · s. Cannot be applied.

Further, since the organic solvent capable of dissolving the light emitting polymer is limited, it is difficult to make the viscosity of the ink as high as the viscosity of the paste used in the screen printing method. Therefore, the second problem is to form a fine pattern of red, green, and blue in the recesses in the bank formed to separate the pixels, using the ink of the low-viscosity luminescent polymer.

On the other hand, regarding the formation of the colored layer of the color filter, as described in JP-A No. 11-33772, the conventional forming method requires further improvement in forming accuracy, throughput and cost. .

Therefore, an object of the present invention is to provide a pattern transfer method capable of forming a pattern in a concave portion such as a substrate and the like, which enables pattern formation with high material utilization rate, low cost and high accuracy in a short time. An object is to provide an image device device formed by using the method and a manufacturing method thereof.

[0022]

The pattern transfer method of the present invention is a pattern transfer method for forming a pattern on a substrate or the like by using a proximity transfer method, in which a screen mask on which the transfer pattern is formed is placed on the substrate. Set with a certain gap, then apply ink to the entire surface of the screen mask and fill the mesh part or opening part of the screen with ink, and scrape off excess ink other than the pattern part using a squeegee or scraper,
After that, the ink is sprayed from the mesh portion or the opening portion of the screen onto the substrate by using a jetting gas, whereby the ink is transferred onto the substrate according to the pattern of the screen mask.

Further, the proximity transfer device of the present invention is a proximity transfer device used for carrying out the above-described pattern transfer method of the present invention, wherein a mesh portion or an opening of a screen mask arranged on a substrate is used. A part is filled with ink, a means for scraping off excess ink other than the pattern part using a squeegee or a scraper, and an ink applied on the screen by spraying a jet gas from above the mesh part or opening part of the screen mask. And a jetting gas spraying means for dropping the gas onto the substrate through the mesh portion or the opening portion of the screen mask.

The pattern of the screen mask is made of stainless steel, polyester, tetron,
For example, a method of forming a pattern on the mesh using a photosensitive resin film, a photosensitive resin such as a photosensitive emulsion, or attaching a metal foil to the screen plate frame and etching the metal foil to a metal With a method of forming a film pattern, a method of forming a resin film pattern by laminating a resin foil on a screen plate frame and laser processing the resin foil, or a method of forming a metal pattern on a mesh by electroforming, etc. A screen mask having a pattern can be formed.

As described above, in the pattern transfer method and the proximity transfer apparatus of the present invention, the ink is applied to the entire surface of the screen mask, the mesh portion or the opening portion of the screen mask is filled with the ink, and the pattern is formed using the squeegee or the scraper. After scraping off the excess ink other than the area, the ink is dropped onto the substrate by spraying the ink from the mesh portion or the opening portion of the screen mask using a jet gas, and the pattern is transferred onto the substrate. It is possible.
Therefore, according to the present invention, unlike the conventional screen printing in which printing is performed while applying an external force to the screen mask, it is possible to form a pattern with high accuracy, and it is possible to accurately transfer the pattern into the concave portion of the substrate or the like. it can.

Screen printing can be carried out by the same method as the pattern transfer method of the present invention. That is, the gap between the screen mask mounted on the screen plate and the glass substrate is controlled by the gap control jig. The gap between the screen plate and the substrate fixing table is shielded from the outside by using a gap control jig, a slight amount of gas is introduced into the gap between the screen plate and the substrate fixing table, and the pressure is raised above the atmospheric pressure of the outside to make the screen. The gap between the mask and the glass substrate can be maintained.

With this, since the plate separation due to the tension of the screen mesh is not used, it is possible to form a pattern with high accuracy as in the pattern transfer method of the present invention, and the conventional pattern forming area is 10 of the screen plate 3. It is possible to expand the pattern forming region in the screen plate 3 to 30 to 50%, while it is to 15%.

[0028]

BEST MODE FOR CARRYING OUT THE INVENTION In the following description, an image display device using organic electroluminescence will be described as an example. The organic electroluminescence device is a step of forming a bank used for element isolation on an anode electrode formed on a glass substrate, at least introducing holes from the anode electrode contributing to light emission, and transporting holes to the light emitting layer. A step of forming a layer having a function of transporting holes, separating an organic film that emits red, green, and blue into banks for device isolation, emitting light, and transporting electrons from a cathode electrode, a cathode that supplies electrons The electrodes are formed by sequentially forming the steps.

The organic electroluminescence device is an element that excites a fluorescent compound by applying an electric field to emit light. The light emission mechanism is based on injecting electrons and holes from the outside and exciting recombination energies of the emission centers.

The structure of the organic electroluminescence device will be described below. First, an anode (ITO electrode), a hole transport layer, a light emitting layer, and a cathode are sequentially stacked above a glass substrate. When a voltage is applied between the anode and the cathode, holes are injected from the ITO electrode of the anode toward the hole transport layer, while electrons are injected from the cathode toward the light emitting layer, and the light is emitted at the light emitting layer. The electrons and holes combine to emit light. The material used here is a metal oxide (indium / tin oxide) for the anode and a metal (magnesium / aluminum, etc.) for the cathode, but the hole transport layer and the light emitting layer are organic compounds.

A typical structure of the organic electroluminescence device is a three-layer structure as described in Patent Document 1, but a two-layer type having both an electron transport layer and a light emitting layer and a hole transport layer. Patent Document 2 discloses a method that also serves as a light emitting layer.
It is described in. In this method, holes injected from the anode into the light emitting layer are confined in the light emitting layer by the electron transport layer. Therefore, the recombination efficiency is improved as in the case where the electron transport layer also serves as the light emitting layer.

Further, in Patent Document 3, there is a proposal that a carrier block layer is interposed between an electron transport layer and a hole transport layer in a three-layer structure so that the electron transport light emitting layer and the hole transport light emitting layer function separately. Have been described. In this method, since the upper and lower light emitting layers function independently, it is possible to mix emission colors.

There is also a bipolar light emitting layer that transports with electrons and holes. If an excellent and highly efficient light emitting material is found for the bipolar light emitting layer, the simplest single layer type device including one organic layer becomes possible. Thus, the function of the organic electroluminescence device can be controlled by changing the structure of the light emitting layer.

The charge carriers (carriers) are chemically radical anions (electrons) and radical cations (holes).
Is. That is, an electron is given to an organic molecule to reduce it at the cathode-organic compound interface to generate a radical anion, and an electron is deprived at the cathode-organic compound interface to oxidize to generate a radical cation. The transfer of electrons in this organic compound is a hopping mechanism by donating electrons between adjacent molecules. Conditions for the light emitting layer include high quantum yield, good film forming property, and high carrier transporting property. Regarding device characteristics, it is desired that the device has high luminance, high luminous efficiency (quantum yield), and long life.

As the luminescent substance, low molecular weight fluorescent dyes, fluorescent polymers, metal complexes, etc. are used. These substances are capable of injecting holes from the anode side and electrons from the cathode side when an electric field is applied. It is necessary to satisfy the conditions that the injected charges can be moved to provide a field where holes and electrons are recombined and that the luminous efficiency is high. Here, in order to facilitate injection of holes, it is desirable that the ionization energy of the light emitting layer be 6.0 eV or less, and in order to facilitate injection of electrons, the electron affinity should be 2.5 eV or more. Is preferred.

A well-known illuminant is Tris (8
-Quinolinolato) aluminum complex (Alq), bis (benzoquinolinolato) beryllium complex (BeBq),
Examples include tri (dibenzoylmethyl) phenanthroline europium complex (Eu (DBM) 3 (Phen)) and ditoluyl vinyl biphenyl (DTVBi). These compounds are disclosed in JP-A-59-194393 and JP-A-9-19493.
It is described in JP-A-241629, JP-A-11-185957, and the like.

As the polymer light emitter, fluorescent poly (p
-Phenylene vinylene) and δ-conjugated polymers such as polyalkylthiophenes. In these polymers, the carrier transportability can be controlled by introducing a substituent,
Various polymers have been synthesized from hole transporting properties to electron transporting properties. These compounds are described in JP-A-3-273087.

In the organic electroluminescence device,
Usually, it has a laminated structure in which a light emitting layer and a carrier transport layer are separated. Aromatic amine derivatives are often used for the hole transport layer. TPD has an ionization potential of 5.4e
Since it is as small as V and the deposited film has a high hole mobility of 0.001 cm 2 / Vs, it is widely used as a hole transport material. These compounds are disclosed in JP-A-4-212287.
It is described in Japanese Patent Publication No. A polymer compound hole transport material in which TPD is incorporated in the main chain or side chain has also been studied.

As the electron transport material, a 1,3,4-oxazole derivative or a 1,2,4-triazole derivative (TAZ) is used. These compounds are patent 2
It is described in Japanese Patent No. 937015, Japanese Patent Laid-Open No. 10-251634, and the like. In particular, TAZ has a large ionization potential of 5.9 eV and has a high hole blocking property.

Therefore, for a compound having a hole transporting property, T
By stacking AZ, a hole transporting light emitting layer can be formed, and TPD used as a hole transporting layer also functions as a light emitting layer by stacking with TAZ.

As the material used for the anode of the organic electroluminescence device, an electrically conductive compound of a metal or an alloy having a high hole injection ability and a large work function is used. Examples of such compounds are gold, copper iodide, tin oxide, ITO.
and so on. Since light emission is extracted from these electrodes, a substance having a high transmittance in the visible light region is preferable. ITO, which has a high transmittance, is most often used.

A metal or alloy having a small work function (4.0 eV or less) is used for the cathode. Alkali metals, alkaline earth metals and Group III metals such as gallium and indium are considered, but magnesium, which is inexpensive and relatively chemically stable, is the most widely used. Since magnesium alone is easily oxidized to air, silver and Copper is added in an amount of 5 to 10% to prevent oxidation, and this also improves the adhesion between the organic layer and the electrode. In addition, alloying for preventing deterioration has been studied.

Next, the most general ITO / hole transport layer /
A method of manufacturing an organic electroluminescence device including a light emitting layer / Mg alloy will be described. As the anode, a substrate obtained by forming an ITO thin film on glass by vapor deposition or sputtering is used. An organic thin film is formed on this ITO glass by a vacuum deposition method or the like. In the vacuum vapor deposition, first, a hole transport material and a light emitting material are put in separate boards or crucibles, which are put in a vacuum chamber and evacuated to a vacuum. Next, the board or crucible is heated (resistance heating) so that the vapor deposition rate of the organic compound becomes a predetermined value. The cathode is also formed on the organic thin film by the vacuum deposition method. A mask matching the shape of the electrodes is placed on the organic thin film, and vapor deposition is performed. Two
When making electrodes made of alloys of more than one metal, separate boards or crucibles are used to control the evaporation rate to achieve the desired composition.

As an alternative method to the vacuum evaporation method, there are a spin coating method and a casting method. These methods are methods in which an organic compound is dissolved in a volatile solvent, applied on a rotating substrate or a stationary substrate, and the solvent is evaporated to obtain a thin film.

An embodiment of the organic electroluminescent device of the present invention will be described in detail below with reference to the drawings. In the organic electroluminescence device, there are a low molecular weight material type and a high molecular weight material type as an organic material used for a portion that contributes to light emission, but the present invention is not limited to these and is a mixture of both. It doesn't matter.

The structure of an organic electroluminescence device based on a low molecular weight material is generally glass substrate / anode electrode / hole injection layer / hole transport layer / light emitting layer / electron transport layer / cathode electrode. On the other hand, the structure of the organic light-emitting diode device based on the polymer material is generally composed of glass substrate /
Anode electrode / hole transport layer / light emitting layer / cathode electrode.

In the case of a high molecular weight organic electroluminescence device, the hole injection layer / hole transport layer of the low molecular weight organic electroluminescence device may have both properties, and The electron transport layer / cathode electrode of the low molecular weight organic electroluminescence device may be replaced with only the cathode electrode of the high molecular weight organic electroluminescence device. Further, the material, composition, etc. used in the present embodiment are not limited, and it is one embodiment for realizing an organic electroluminescence device.

An apparatus for realizing the pattern transfer method of the present invention will be described with reference to the schematic view of FIG. In FIG. 1, 1 is a coating means (squeegee) for coating the ink 6, and 2 is a spraying means (beam-shaped jetting nozzle) for jetting the gas 7. Further, 3 is a screen plate on which a screen mask having a transfer opening pattern 4 is mounted, and 5 is a substrate with a bank for transferring the pattern. Reference numeral 8 denotes a jig (gap control jig) for controlling the gap between the screen mask mounted on the screen plate 3 and the banked substrate 5, and 9 fixes the banked substrate 5 by vacuum suction. It is a table (board fixed table).

As shown in FIG. 1, the substrate fixing table 9
The substrate 5 with a bank was set on the above, and it was fixed by vacuum suction using the fine holes provided in the substrate fixing table 9. Further, after aligning the transfer opening pattern 4 of the screen plate 3 with the screen mask mounted thereon and the transfer position of the substrate 5 with the bank, the screen mask and the bank mounted on the screen plate 3 by the gap control jig 8 are aligned. The gap with the attached substrate 5 is controlled.

It is expected that the screen slab 3 becomes large in size, the gap between the screen mask and the banked substrate 5 cannot be controlled only by the tension of the screen mesh, and the central portion of the screen mask is loosened by its own weight. It In this case, the gap between the screen plate 3 and the substrate fixing table 9 is blocked from the outside by using the gap control jig 8, and a slight amount of gas is introduced into the gap between the screen plate 3 and the substrate fixing table 9, The gap between the screen mask and the substrate with bank 5 can be maintained by increasing the pressure higher than the external atmospheric pressure.

At this time, it may be possible that the drying speed is fast depending on the properties of the ink. Therefore, the introduced gas may dry the ink 6, block the opening 4 of the screen mask, and the ink 6 may not be quantitatively transferred. At that time, by circulating the gas in the gap between the screen plate 3 and the substrate fixing table 9, the solvent contained in the ink can be kept under the gas atmosphere, and the drying by the ink 6 can be prevented.

Next, the ink 6 is placed on the screen mask, the squeegee 1 and the screen mask are brought into close contact with each other, and the ink 6 is scraped off by the squeegee 1 at an angle of about 70 ° between the screen mask and the squeegee 1, and a transfer opening pattern is formed. 4 is filled with ink 6. In FIG. 1, this is accomplished by moving the squeegee from left to right. Next, the beam-shaped jet nozzle 2 is brought into close contact with the screen mask, the jet gas 7 is sprayed from the nozzle, and the squeegee is moved from left to right in the same manner as the squeegee 1, whereby the transfer opening pattern 4 is formed.
The ink 6 filled in can be transferred into the bank of the substrate with bank 5.

An apparatus of another system for realizing the pattern transfer method of the present invention will be described with reference to the schematic view of FIG. Here, 10 is a coating means (scraper) for coating the ink 6, which is installed almost vertically to the screen mask and is a system for filling the transfer opening pattern 4 with the ink 6 while scraping the ink. The ink 6 can be transferred into the bank of the bank-equipped substrate 5 in the same manner as in FIG. 1 except for a coating means for coating the ink 6.

By the way, screen printing can be carried out by the same method as the pattern transfer method of the present invention. The glass substrate is set on the substrate fixing table, and the glass substrate is fixed by vacuum suction using the fine holes provided in the substrate fixing table.
Further, after aligning the opening pattern of the screen plate on which the screen mask is mounted with the pattern formation position on the glass substrate, the gap between the screen mask mounted on the screen plate and the glass substrate is controlled by the gap control jig. .

However, it is expected that the size of the screen plate becomes large, the gap between the screen mask and the glass substrate cannot be controlled only by the tension of the screen mesh, and the central portion of the screen mask is loosened by its own weight. . In this case, the gap between the screen plate and the substrate fixing table is cut off from the outside by using a gap control jig, and a slight amount of gas is introduced into the gap between the screen plate and the substrate fixing table, and the pressure is higher than the external pressure. It is possible to maintain the gap between the screen mask and the glass substrate by increasing the height.

Since the plate separation due to the tension of the screen mesh is not used, the conventional pattern formation area is 10 to 15% of the screen plate, while the pattern formation area is 30 to 30%.
The pattern formation area in the screen plate is expanded to 50%. In addition, when a small amount of gas is introduced into the gap between the screen plate and the substrate fixing table, the drying speed may be high depending on the nature of the paste. Therefore, the introduced gas may dry the paste and block the opening of the screen mask, making it impossible to form a pattern. At that time, by circulating the gas in the gap between the screen plate and the substrate fixing table, the solvent contained in the paste can be kept in the gas atmosphere, and the paste can be prevented from being dried by the gas.

Next, the paste is placed on the screen mask, the scraper and the screen mask are brought into close contact with each other, and the paste is filled into the opening pattern while scraping the paste with the scraper at an angle of about 90 ° between the screen mask and the scraper. Next, the squeegee is brought into close contact with the screen mask, and the squeegee is moved similarly to the scraper, whereby the paste filled in the opening pattern can be transferred to the glass substrate.

As an embodiment of the present invention, an organic electroluminescence device will be shown, but the technique is not limited to this, and is also applied to an image display device such as an inorganic electroluminescence device, a plasma display device, a field emission display device and the like. It is possible.

For example, in an inorganic electroluminescence device, it can be used for forming transparent electrodes on the front substrate, bus electrodes, dielectric film formation, address electrodes on the rear substrate, dielectric film formation, light emitting layer formation and the like. Further, in the plasma display device, it can be utilized for bus electrode formation on the front substrate, dielectric film formation, address electrode formation on the rear substrate, dielectric film formation, rib formation, phosphor formation and the like. Also, in field emission display devices, it is possible to form transparent electrodes on the front substrate, black matrix formation, phosphor film formation, address electrodes formation on the rear substrate, electron source electrodes (containing carbon nanotubes), frit glass for fixing ribs, etc. Can be utilized.

Furthermore, these pattern transfer methods are not limited to the method of manufacturing an image display device, but can be utilized for general thick film electrode wiring and insulating layer formation.

Example 1 An example of the pattern transfer method of the present invention will be described with reference to FIG. In FIG. 3, reference numeral 1 is a coating means (squeegee) for coating ink.
And 2 is a blowing means (injection nozzle) for injecting gas. 3 is a screen plate equipped with a screen mask having a transfer opening pattern 4,
Reference numeral 5 is a substrate with a bank 14 for transferring a pattern. Here, the squeegee 1 should not affect the ink 6 used and the solvent contained in the ink 6. Therefore, in the manufacturing process of the organic electroluminescence device of the present invention, silicone rubber is used for the squeegee 1 in consideration of materials such as the hole transport layer and the light emitting layer. Further, although stainless steel was used for the scraper 10, a slight amount of corrosion occurred, so a resin coat was further applied to improve the corrosion resistance.

In the screen plate 3, a mesh of stainless steel, polyester, tetron, nylon or the like is attached to the screen plate frame, and a pattern (film pattern in which ink does not pass) opposite to the pattern transferred to the substrate is formed on the mesh. Prepress by doing so. This makes it possible to form a screen mask having an opening in the pattern portion to be transferred to the substrate.

In the pattern transfer method of the present invention, as shown in FIG.
As shown in (A), first, a film that does not allow ink to pass through is formed on a mesh, and then a screen mask having openings 4 formed in a predetermined pattern portion is formed on a substrate with bank 5 with a certain gap. The ink is set, the ink is placed on the screen mask, and the excess ink other than the pattern portion is scraped off by using the squeegee 1 or the scraper 10 to fill the mesh portion or the opening portion of the screen mask with the ink. After that, as shown in FIG. 3B, the jetting gas 7 is sprayed on the screen mask to drop the ink 6 filled in the mesh portion or the opening portion 4 of the screen mask onto the bank-equipped substrate 5, and the bank-equipped substrate 5. The pattern transfer is performed on 5. As a result, a substrate with a bank 5 on which the ink 6 is transferred as shown in FIG. 3C is formed. After that, the solvent contained in the ink 6 is dried and removed in a drying furnace, so that a substrate as shown in FIG.

An embodiment of the organic electroluminescence device of the present invention will be described with reference to FIGS. (1) Glass plate 11 with anode electrode formation size of 340 mm square and thickness of 0.7 mm
(Corning product # 1737) was coated with ITO having a sheet resistivity of about 10 Ω / cm 2 or less by sputtering. After applying a protective resist on the ITO film formation surface side of this glass plate, 1
The 25 mm square was cut and chamfered, and then the protective resist was removed with acetone.

Next, this glass plate 11 is ultrasonically cleaned with IPA and dried, and then the thickness of the ITO film forming surface side is 0.1 μm.
Cr was vapor-deposited. After ultrasonic cleaning with IPA and drying, a positive resist (OFPR-8 made by Tokyo Ohka Co., Ltd.
00, viscosity: 30 mPa · s) at a rotation speed of 1300 rpm
Spin coat for 60 seconds in an oven at 90 ° C x 25 mi
n pre-baked. The glass dry plate on which a predetermined mask pattern was formed was aligned, and exposed (20 sec) and developed (OFPR / DE-3 manufactured by Tokyo Ohka).
After the development, the Cr film was etched using a cerium secondary ammonium nitrate aqueous solution, washed with water and dried.

Since Cr patterning similar to that of the ITO wiring pattern was formed in this manner, the Cr pattern was inspected by transmitted light, and if a disconnection or a pinhole was generated, the resist pattern was formed at this point. Use to correct.
Here, by depositing the Cr film, not only the inspection with a microscope by transmitted light can be easily performed at the time of pattern inspection, but also the ITO can be protected at the time of etching the ITO. After that, post baking was performed in an oven at 120 ° C. for 30 minutes.

Next, the ITO film was etched at a liquid temperature of 30 ° C. using a mixed solution of ferric chloride and hydrochloric acid, washed with water and dried. Then, the positive resist was peeled off by applying ultrasonic waves with acetone, followed by ultrasonic cleaning with IPA and drying. The ITO pattern check was a leak check with a tester, and if there was a leak, laser cutting was performed using a laser method for repair. Also in this case, the tester needle does not directly touch the ITO film but the Cr film is used to prevent damage from the stylus.

Then, the Cr film was removed by etching with an aqueous solution of cerium secondary ammonium nitrate. At this time, in order to facilitate the alignment in the subsequent process, only the alignment mark portion was protected with asphalt before etching and removing the Cr film so as not to be etched. In this way, the anode electrode 12 was formed on the glass plate 11 as shown in FIG.

(2) Insulating layer formation The glass substrate 11 on which the anode electrode 12 is formed is ultrasonically cleaned with IPA and dried, and then Cu is deposited by an electron beam method under the deposition conditions of a deposition rate of 3 Å / sec and a temperature of 300 ° C. , A film thickness of 1 μm was deposited. After ultrasonic cleaning with IPA and drying, a positive resist (Oka
FPR-800, viscosity: 30 mPa · s), rotation speed 13
Spin coat at 00 rpm for 60 seconds, 90 ° C in oven
A pre-bake of × 25 min was performed. Align the glass plate with the specified mask pattern and expose (20
sec) and development (Tokyo Ohka's OFPR / DE-3)
Then, post baking was performed in an oven at 120 ° C. for 30 minutes. Then, the Cu film was etched using an aqueous solution of ammonium persulfate, washed with water and dried. Further, the positive resist was peeled off by applying ultrasonic waves with acetone, followed by ultrasonic cleaning with IPA and drying.

Next, by sputtering, SiO 2_TwoMembrane and
And Al_TwoO_ThreeA film was formed. SiO _TwoThe film thickness is 500
3 types of Å, 1000 Å, 2000 Å, Al_TwoO_Three
The film had a film thickness of 200Å. After that, a Cu film is formed with a nitric acid aqueous solution.
Was removed by etching, washed with water and dried. like this
On the insulating layer SiO_TwoThe film is a hydrofluoric acid-based etchant
Using SiO_TwoFormed without etching itself
Therefore, damage to the glass plate and ITO, surface changes, etc.
I was able to prevent it. Further, as the insulating material, Si
O_TwoAlthough insulation can be satisfied with only the film,
In the example, the density of the polyimide used for the bank formation in the later process
Al to improve wearability_TwoO_ThreeA film was formed. This
Thus, SiO as shown in FIG._TwoMembrane and A
l_TwoO_ThreeA pattern of insulating layer 13 of the film was formed.

(3) The glass substrate 11 on which the bank-forming insulating layer has been formed is ultrasonically cleaned with IPA and dried, and then a polyimide slurry (PIX manufactured by Hitachi Chemical Co., Ltd.) is used.
-3400) was spin-coated at a rotation speed of 2000 rpm for 80 seconds, and prebaked at 140 ° C. for 20 min in an oven. On top of that, a positive resist (OFPR-800 made by Tokyo Ohka Co., Ltd., viscosity 60 cp) is rotated at a rotation speed of 1300 r.
Spin coat for 60 seconds at pm, 90 ° C in oven
A pre-bake of × 25 min was performed. The film thickness of the polyimide after prebaking was 12 μm. The glass dry plate on which a predetermined mask pattern is formed is aligned and exposed (30
sec), OFR / DE-3 manufactured by Tokyo Ohka Co., Ltd. was used to pattern the polyimide simultaneously with the development of the positive resist. Post baking was performed in an oven at 120 ° C. for 30 minutes. Then, after washing with water and drying, the polyimide pattern was inspected with a microscope and immersed in acetone to remove the photoresist. After washing with IPA, washing with water,
It was dried.

The glass substrate having the polyimide bank shape was heat-treated at 200 ° C. × 30 min and then 350 ° C. × 1.
It was heat-treated and cured under the condition of hour. In this process,
When the surface of the ITO electrode, which is the anode electrode, is contaminated with organic substances, there are cases where a sufficient work function, which is the characteristic required for the ITO surface, cannot be obtained. Therefore, it is necessary to perform cleaning by oxygen plasma treatment, ultraviolet / ozone treatment, ultrasonic cleaning treatment, or the like.

In this embodiment, a dry etching apparatus is used, the flow rate of oxygen gas is 150 sccm, the pressure in the chamber is controlled to 200 mTorr, and the RF power is 1 kW.
Oxygen plasma treatment was performed for 2 seconds. Further, in the formation of the hole transport layer in the subsequent step, it is necessary to perform plasma treatment with CF ₆ gas in order to reduce the wettability of the hole transport layer on the surface of the bank material and form the anode transport electrode with a uniform thickness. is there. Similar to the oxygen plasma treatment, a dry etching apparatus is used, the flow rate of CF ₄ gas is 100 sccm, the chamber internal pressure is controlled to 200 mTorr, and RF is used.
A liquid repellent treatment was performed by performing CF ₆ plasma treatment for 15 seconds at an electric power of 1 kW.

In this way, the glass substrate 11 having the polyimide banks 14 as shown in FIG. 4B could be manufactured. This polyimide bank shape has a thickness of 9.
6 μm, upper opening is 72 μm × 128 μm rectangular, lower (glass substrate side) opening is 56 μm × 112
It was a rectangle of μm.

In this embodiment, the polyimide bank is formed by using the normal photolithography process, but the present invention is not limited to this embodiment as long as a predetermined shape can be obtained. For example, the bank can be formed by using the pattern transfer method of the present invention or the conventional screen printing technique. As the bank material used at this time, there are polyimide paste for screen printing, maleimide varnish, polyamide imide paste and the like, but those having a high thixotropy from the shape-retaining property are preferable, and even those in which an organic or inorganic filler is dispersed Good. Further, the bank material is not limited to the polyimide material as long as it has a low hygroscopic property and generates little gas due to the manufacturing process and the use environment of the display. Further, by dispersing a black pigment in the bank material to blacken the bank, it can be used as a black matrix.

(4) Formation of Hole Transport Layer First, a method of forming the screen mask 15 used for forming the hole transport layer by the pattern transfer method will be described.
The screen version is made of stainless steel,
A mesh 16 made of polyester, tetron, nylon or the like is attached, and a pattern (film pattern 17 through which ink does not pass) opposite to the pattern to be transferred to the substrate is formed on the mesh 16 for plate making. As a result, the screen mask 15 having an opening in the pattern portion to be transferred onto the substrate can be formed.

As a method of forming a transfer opening pattern on the screen mask 15, a stainless mesh 16 was attached to a screen plate frame, and a pattern was formed on the screen mask 15 using a photosensitive emulsion 17. In addition to this, as a method of forming a transfer opening pattern on the screen mask 15, a mesh 16 made of polyester, tetron, nylon or the like is attached to the screen plate frame,
For example, a method of forming a pattern on a mesh using a photosensitive resin 17 such as a photosensitive resin film or a photosensitive emulsion,
A method of attaching a metal foil to the screen plate frame and forming a metal film pattern by etching the metal foil, a method of attaching a resin foil to the screen plate frame and forming a resin film pattern by laser processing the resin foil, or electroforming There is a method of forming a metal pattern on the mesh by the method. In any case, the screen mask 15 having a highly accurate transfer opening pattern could be formed.

By the way, in this embodiment,
A pattern was formed on the mesh of the screen plate using a photosensitive resin for screen mask formation manufactured by Tokyo Process Service (screen mask pattern formation). that time,
As the stainless steel mesh, a 500 mesh product having a wire diameter of 18 μm, an opening size of 33 μm and an opening area of 42% was used. As a photosensitive resin for forming a screen mask, an emulsion excellent in solvent resistance ((shares ) Tokyo Process Service's product name: NSL) having a film thickness of 15 μm was used. Further, the pattern of the opening may have a volume that can hold the amount of ink to be filled in the bank formed on the substrate.

The screen mask used in this example had a discharge rate of 14.3 ml / m 2 and a film thickness of 14.3 μm.
It can be formed. Therefore, it is necessary to calculate the volume with which the bank formed on the substrate is filled with ink and determine the screen mask opening. Therefore, the area of the screen mask opening is smaller than the area of the upper part of the bank by about 40%.

For the screen plate frame, an aluminum casting which has no distortion and is compatible with high tension and high precision printing was used. When an aluminum pipe is used as the screen plate frame in order to reduce the weight, it is preferable to provide a brace inside the pipe in order to increase the rigidity.

In the pattern transfer method of the present invention, as shown in FIG.
As shown in (C), first, a film (emulsion 17) through which ink does not pass is formed on the mesh 16, and then the screen mask 15 having openings in predetermined pattern portions is formed with the bank 14 and the insulating layer 13. The glass mask 11 is set on the glass substrate 11 with a certain gap, and the screen mask 15
The ink 18 of the hole transporting material is placed on the upper surface, and the excess ink 18 of the hole transporting material other than the pattern portion is scraped off by using a squeegee or a scraper to remove the ink 18 of the hole transporting material on the mesh portion 16 or the opening portion of the screen mask. Fill.

Here, as the ink 18 of the hole transport material, a water colloidal solution containing poly (3,4-ethylenedioxythiophene) which is a conductive polymer and polystyrene sulfonic acid which is a dopant (BYTRO manufactured by Bayer) is used.
NP-CH-8000) was used. The concentration of this ink is about 1%, and the volume after drying is about 1/100. Therefore, in order to form a thickness of 100 nm,
It is necessary to transfer the thickness of about 100 times that. It is important to adjust the transfer amount according to the height of the bank 14, the size of the mesh 16 used for the screen mask, the thickness of the emulsion 17, the size of the opening, etc. from the density of the ink used and the thickness to be formed. Is.

Further, in this embodiment, the mesh portion 1 of the screen mask 15 is formed by using a squeegee or a scraper.
6 or the opening portion is filled with the ink 18 of the hole transport material, but the mesh portion 16 of the screen mask 15 or the opening portion may be filled with the ink by a roll or the like.

Thereafter, as shown in FIG. 4 (D), by spraying a jetting gas on the screen mask 15,
Ink 18 of the hole transport material filled in the mesh portion 16 or the opening portion of the screen mask 15 is stored in the bank 14.
Then, the ink was ejected onto the glass substrate 11 on which the insulating layer 13 was formed, and the ink 18 of the hole transport material was transferred into the bank 14. As a result, as shown in FIG. 4D, a substrate with a bank, in which the ink 18 of the hole transport material was transferred into the bank 14, was formed.

At this time, the gap between the substrate and the screen mask 15 was kept at 0.15 mm so that the bank 14 on the substrate and the screen mask 15 did not come into contact with each other. The gap between the substrate and the screen mask 15 varies depending on the characteristics of the ink used, and is not defined by this gap. In addition, a jet air is blown from a beam-shaped gas jet nozzle at an air pressure of 0.5 kg / cm 2 from a slit having a width of 0.1 mm, whereby the ink 18 filled in the mesh portion 16 or the opening portion of the screen mask is banked. Then, the ink was ejected onto the glass substrate 11 on which the insulating layer 13 was formed, and the ink 18 of the hole transport material was transferred in a predetermined frame surrounded by the bank 14. As a result, it was possible to eject a sufficient amount of ink to fill a bank formed on the substrate and having a height of about 10 μm.

As described above, according to the pattern transfer method of this embodiment, since the ink is sprayed onto the substrate by the jetting gas to transfer the pattern, the screen mask can be deformed like the conventional screen printing method. It is possible to form a pattern with high accuracy. In addition, a pattern on the recess was easily formed, which was difficult with the conventional screen printing method.

Further, according to the pattern transfer method of the present embodiment, it was possible to form the pattern in about 1/100 times or less (about 10 seconds) as compared with the case of the inkjet printing having the multi-head. After that, the solvent contained in the ink 18 of the hole transport material was dried and removed in a drying furnace to prepare a substrate in which the hole transport layer 18 was formed in each bank as shown in FIG. 4 (E).

(5) Light-Emitting Layer Formation As shown in FIG. 5A, the light-emitting layer was formed on the substrate on which the hole-transporting layer 18 was formed in the same manner as the hole-transporting layer 18. In the pattern transfer method of the present invention, FIG.
As shown in (B), first, a film (emulsion 17) through which ink does not pass is formed on the mesh 16, and then the screen mask 15 having an opening formed in a predetermined pattern portion is provided with a hole transport layer in the bank 14. The glass mask 11 is set on the formed glass substrate 11 with a certain gap, and the screen mask 15
An ink 19 of a light emitting material that emits green light is placed on the upper surface, and an excess ink 19 of the light emitting material other than the pattern portion is scraped by using a squeegee or a scraper, and the ink 1 of the light emitting material is applied to the mesh portion 16 or the opening portion of the screen mask.
Fill 9.

Here, the ink 1 of the light emitting material that emits green light
As for 9, Green-K made by Dow 1, 2, 3, 4
An ink prepared with tetramethylbenzene was used. The density of this ink is about 1.43%, and the volume after drying is about 1/70. Therefore, in order to form a thickness of 100 nm, it is necessary to transfer the thickness of about 70 times the thickness.

Thereafter, as shown in FIG. 5 (C), by spraying a jetting gas on the screen mask 15,
The ink 19 of the light emitting material filled in the mesh portion 16 or the opening portion of the screen mask 15 is ejected to a predetermined position on the glass substrate 11 having the hole transport layer 18 formed in the bank 14, and the hole transport layer 18 in the bank 14 is discharged. The ink 19 of the light emitting material was transferred onto the above. As a result, FIG.
As shown in (C), a substrate was formed in which the ink 19 of the light emitting material was transferred onto the hole transport layer 18 in the bank 14. After that, the solvent contained in the ink 19 of the light emitting material was dried and removed in a drying oven to prepare a substrate in which a green light emitting layer 19 was formed in a predetermined bank as shown in FIG. 5D.

Further, a red light emitting layer 20 and a blue light emitting layer 21 are formed by the same method as that for the green light emitting layer 19, and as shown in FIG.
As shown in (E), a substrate was prepared in which a red light emitting layer 20 and a blue light emitting layer 21 were formed in a predetermined bank. Here, as the ink 20 of the light emitting material that emits red light, Do is
Red-F manufactured by w was used as an ink prepared with 1,2,3,4-tetramethylbenzene. Also, as the ink 21 of a light emitting material that emits blue light, Blue-made by Dow-
An ink prepared by mixing J with 1,3,5-trimethylbenzene was used.

(6) Formation of Cathode Electrode As shown in FIG. 6 (A), the substrate in which the red, green, and blue light emitting layers (20, 19, 21) are formed in predetermined banks is formed as shown in FIG.
As shown in FIG. 6B, a metal mask 22 formed in a predetermined pattern is aligned and set, and the cathode electrode 23 made of Al / Ca as shown in FIG. It was formed only in 22 openings. Thereby, the cathode electrode pattern was formed. The cathode electrode may be any one as long as it has a small work function, and is not limited to Al / Ca. In this way, an organic electroluminescence device as shown in FIG. 6D could be formed.

(7) Display Formation A method of producing a display using the organic electroluminescence device formed by the present invention will be described with reference to FIGS. 7 and 8. First, the sealing can 29 used to shield the organic electroluminescence device (image display unit) 25 from the outside air will be described. The sealing can 29 is formed by hot press forming a glass plate into a cross-sectional shape as shown in FIG. The physical property value of the sealing can 29 is preferably the same as the physical property value of the substrate material forming the organic electroluminescence device (image display portion). Further, in order to reduce the thermal stress after sealing, it is preferable that the glass material has the same thickness. In this example, the same material was used for press molding.

The adsorbent (drying agent) 25 for adsorbing the gas generated from the organic electroluminescence device (image display section) 25, the gas generated in the manufacturing process and the gas penetrating and penetrating the sealing material 30 is filtered. The material 27 was set inside the sealing can 29, and the sealing material 30 was applied to the periphery of the sealing can 29 in a dry nitrogen atmosphere using a dispenser. Next, the sealing can 29 created in the above step is aligned in dry nitrogen on the glass substrate 24 on which the organic electroluminescence device (image display unit) 25 is formed,
Sealing was performed at 80 ° C. for 30 seconds. As a result, the nitrogen gas (dry) 28 could be enclosed inside.

Depending on the sealing material, there is an ultraviolet curing material, but when the ultraviolet light is irradiated, the organic electroluminescence device (image display portion) 25 near the sealing material is diffused and irradiated with the ultraviolet light to deteriorate the brightness (lifetime). Decrease). As for the sealing conditions, if sealing is performed at a temperature exceeding 100 ° C., there is a possibility that luminance deterioration (life shortening) may occur as in the case of ultraviolet rays.

Next, a display could be made by connecting a circuit to the external terminal 31. In this display, an image could be seen through a glass substrate on which an organic electroluminescence device (image display section) was formed. In the image display device of the present invention, the hole transport layer having a uniform thickness and the light emitting layer for achieving desired light emitting characteristics can be formed on the entire surface without unevenness.

Further, as shown in FIG. 8, instead of the sealing can 29, the sealing film 32 is directly adhered to the organic electroluminescence device (image display portion) 25 with the organic resin 33 and sealed at 80 ° C. for 30 seconds. I stopped. In this case, the image could be seen from the opposite side of FIG. 7 (from the top through the sealing film 32). Therefore, in this case, it is important to make the cathode electrode transparent, and in order to reduce the wiring resistance, a bus electrode is formed on the bank for power supply to the cathode electrode. The organic electroluminescence device of the present invention has an aperture ratio of 1.
Since it is 6 times larger, much light can be extracted to the outside even when the same light emission is performed, and the brightness is about 1.
Improved 6 times.

(Embodiment 2) Same as Embodiment 1 except that the ink material for forming the light emitting layer, which is a material for emitting red, green and blue, is sequentially supplied into the same bank. An organic electroluminescence device was prepared by the method. That is, after forming a bank for element isolation on a substrate on which an anode electrode is formed, an ink fixed amount supply jig is placed in non-contact with this bank, and at least holes individually supplied to the ink fixed amount supply jig are arranged. An ink material for forming a layer having functions of introduction, hole transport, light emission, and electron transport was sequentially supplied into the above-mentioned bank, and then a cathode electrode was formed above the electron transport layer. At this time, the ink material for forming the light emitting layer is a material that develops red, green, and blue, and is sequentially supplied to the same bank.

In this case, since red, green and blue emit light in the same bank, white light is emitted. The materials that emit red, green, and blue have different emission characteristics, so the thicknesses of the materials that emit red, green, and blue were controlled in order to set the color temperature of white. By emitting light in the same manner as in Example 1, it could be used as a monochrome display.

Further, the realization of a full-color display can be achieved by forming, for each pixel, red, green, and blue color filters equivalent to those used in a liquid crystal panel.

On the glass substrate of the liquid crystal panel, a black matrix is formed as a light-shielding film so that the transmitted light from unnecessary gaps is not emitted to the display surface side and the contrast ratio is not lowered. However, in the present embodiment, the material of the bank can be blackened to serve also as a light shielding film. The light-shielding film has a light-shielding property and is formed of a film having a high insulating property so as not to affect the electrodes. In this embodiment, a black pigment is mixed with polyimide, which is a bank material, to form the film. did. The light-shielding film is formed on the pixels in each row in a matrix in the vertical and horizontal directions, and the effective display area of each row and each column is partitioned by these lines. Therefore, there is an effect that the contour of the pixel in each row and each column is made clear by the light shielding film.

A method of forming a color filter on a glass substrate will be described with reference to FIG. The color filters are formed in stripes by repeating red, green, and blue at positions facing the pixels. The color filter is formed so as to overlap the edge portion of the black bank material used as the light shielding film. Here, the color filter can be formed as follows. First, a base material in which red, green, and blue pigments such as acrylic resin are mixed is formed on the surface of the glass substrate 34, and the base material is patterned by a photolithography technique, and each color (red, green,
Blue filters (35, 36, 37) are sequentially formed.
In some cases, pigments of other colors such as cyan are mixed in order to improve the color purity.

The overcoat film 38 is provided, for example, in order to prevent leakage of dye in the color filter and to flatten the step due to the color filter. The overcoat film 38 is formed of a transparent resin material such as acrylic resin or epoxy resin. By forming the color filter substrate on the inside of the glass substrate 34 on the image viewing side, a clear image could be seen.

Example 3 An organic electroluminescence device was prepared in the same manner as in Examples 1 and 2 except that a glass substrate having a thin film transistor was used instead of the glass substrate having an anode electrode.
A method of manufacturing a thin film transistor includes a step of applying organosilicon nanoclusters on a substrate having an insulating surface, a step of oxidizing the organosilicon nanoclusters to form a silicon oxide film, a source region, a drain region, and those. Forming an island-shaped non-single-crystal silicon film having a channel region sandwiched between two, forming a gate insulating film on the island-shaped non-single-crystal silicon film, and forming a gate insulating film on the channel region through the gate insulating film. Although it is formed through the steps of forming an electrode, generally well known methods can be used in each step.

Here, the organosilicon nanocluster refers to an organic silicon compound which is soluble in an organic solvent and has a band gap of 3 eV to 1.2 eV, and tetrahalogenated silane and an organic halide are treated with an alkali metal or an alkaline earth metal. It is obtained by reacting in the presence of a metal and then treating with hydrofluoric acid. Part of the tetrahalogenated silane may be replaced with trihalogenated silane or dihalogenated silane.

The organosilicon nanoclusters thus obtained are soluble in common organic solvents such as hydrocarbons, alcohols, ethers, aromatic solvents and polar solvents.
In addition, by performing hydrofluoric acid treatment at the end of the synthesis, oxygen atoms and water in the reaction system and oxygen atoms taken into the silicon nanoclusters can be eliminated from the stopper.
These oxygen atoms are not preferable because they cause formation of a silicon oxide film when obtaining a silicon thin film. By carrying out the hydrofluoric acid treatment, silicon nanoclusters as a silicon thin film precursor containing no oxygen atom can be obtained.

The thin film of the organosilicon nanocluster can be obtained from a solution of the organosilicon nanocluster dissolved in an appropriately selected solvent by a general thin film forming method such as a spin coating method or a dipping method. A thin silicon film can be obtained by heating the formed organosilicon nanoclusters in a substantially oxygen-free atmosphere or a reducing atmosphere or irradiating with ultraviolet light, and by heating or irradiating in an oxidizing atmosphere with ultraviolet light. You can

The above heating and ultraviolet irradiation may be combined. It is also possible to obtain a silicon thin film by performing laser irradiation in an atmosphere substantially free of oxygen or a reducing atmosphere.

A TFT is formed on the silicon oxide film using the organosilicon nanocluster as a precursor. As described above, the organosilicon nanocluster is made of tetrahalogenated silane as a raw material, and the silicon oxide film having the organosilicon nanocluster as a precursor contains halogen. Halogen has the effect of segregating sodium ions, potassium ions, etc. to capture and getter, and effectively prevents impurity diffusion from the glass substrate to the TFT. Further, in order to prevent the diffusion of impurities, the larger the silicon oxide film thickness, the greater the effect.

Organosilicon nanoclusters can be formed by spin coating, a large-area thick film can be easily formed, and threshold variation due to impurities can be suppressed.
No warpage or cracks occur. Therefore, the present invention is extremely useful for manufacturing an organic electroluminescence device using a large area glass substrate.

Further, the silicon oxide film can be formed so as to surround the island-shaped silicon layer and its periphery by appropriately combining the step of oxidizing the organosilicon nanoclusters and the step of forming a silicon thin film without oxidation.
It is possible to realize a structure in which the step difference at the end of the island-shaped semiconductor layer is reduced, and it is possible to prevent a decrease in withstand voltage due to thinning of the gate insulating film. Moreover, this technology reduces the manufacturing cost because the island-shaped semiconductor layer and the insulating film around it can be formed in a smaller number of steps than the conventional island-shaped semiconductor layer forming method of exposing, developing, and etching after forming the semiconductor layer. It is possible to

A thin film transistor according to the present invention comprises a silicon oxide film provided on a substrate having an insulating surface, a plurality of island-shaped non-single-crystal semiconductor layers having a main surface and end faces, and the island-shaped non-single-crystal. A first insulating film on a silicon oxide film, which has a source region, a drain region, and a channel region sandwiched between them in a semiconductor layer and is in contact with only an end surface of the island-shaped non-single-crystal semiconductor layer; A second insulating film covering the single crystal semiconductor layer and the first insulating film, a gate electrode formed over the channel region with the second insulating film interposed therebetween, a source region and a drain region, a source region and a drain The silicon oxide film has a structure including a source electrode and a drain electrode in contact with the region, and the silicon oxide film contains a halogen element.

Since the island-shaped non-single-crystal semiconductor layer and the first insulating film are in contact with each other only at their end faces, there are few steps, and it is possible to prevent a decrease in withstand voltage due to the thinning of the gate insulating film. And
Since the silicon oxide film contains a halogen element, it is possible to effectively prevent diffusion and penetration of impurities from the glass substrate into the gate oxide film.

First, a method for preparing an organosilicon nanocluster solution will be described. Scraped Mg metal (64 mmol) is placed as an alkali metal in a round bottom flask, heated under vacuum at 120 ° C. for activation and cooling, and dehydrated tetrahydrofuran (THF) is added to the above reaction system as a nitrogen atmosphere. While irradiating ultrasonic waves (60 W) at 0 ° C., tetrachlorosilane (16 mmol) is added and reacted. After reacting for 2.5 hours, tert-butyl bromide (16 mmol) is reacted with the resulting black-brown reaction solution. After reacting for 1 hour, the temperature of the reaction solution is adjusted to 50
The temperature is set to 0 ° C. and the reaction is continued for 0.5 hours. The reaction solution is dropped into distilled water and the insoluble matter is collected by a filtration method. The recovered insoluble matter is dispersed in 47% hydrofluoric acid, stirred and reacted for 30 minutes, and another insoluble matter is obtained by filtration. A 16 wt% solution of this insoluble matter is prepared using toluene as a solvent to prepare an organosilicon nanocluster solution.

A method of forming a thin film transistor on a glass substrate will be described with reference to FIG. On the alkali-free glass substrate 39 (600 mm x 400 mm) having a strain point of 670 ° C,
The organosilicon nanocluster solution is applied by a spin coating method in which the rotation speed is adjusted so that the film thickness becomes 500 nm, and dried on a hot plate at 80 ° C. for 1 minute.
After that, ultraviolet rays are irradiated for 3 minutes using a 500 W ultra-high mercury lamp in an oxygen atmosphere, and silicon oxide (SiO ₂ )
A film 40 is obtained. Further, an amorphous silicon layer is deposited to a thickness of 50 nm by the plasma CVD method. Next, XeCl excimer laser is irradiated to crystallize the amorphous silicon layer to obtain a polysilicon film.

Then, the polysilicon film is patterned by a known photoetching process to obtain an island-shaped polysilicon layer 41. Then, a SiO ₂ film to be the gate insulating film 42 is deposited to 70 nm by plasma CVD method, and Nb is deposited to 250 nm by sputtering method. Patterning Nb by a known photo-etching process,
The gate electrode 43 is formed.

Next, a high resistance N type polysilicon layer 44 is formed by ion implantation using the gate electrode 43 as a mask for the N channel thin film transistor, and then a low resistance N type polysilicon layer 45 is formed using the resist as a mask. Form. On the other hand, for the P-channel thin film transistor, the low resistance P-type polysilicon layer 46 is formed by ion implantation using the gate electrode 43 as a mask.

The sheet resistance value of the high resistance polysilicon layer is 20 kΩ to 100 kΩ, and the sheet resistance value of the low resistance polysilicon layer is 500 Ω to 10000 Ω. Further, an interlayer insulating film 47 made of SiO ₂ is formed so as to cover the whole, and a source electrode 50 made of a three-layer metal film of Ti / Al / Ti and a drain are formed through a contact through hole provided in the interlayer insulating film 47. Electrode 51
And wiring is formed. Here, the reason why the three-layer metal film is used is to reduce the contact resistance between the low-resistance polysilicon layer and Al and the contact resistance between the pixel electrode (ITO) 48 and Al.

After patterning the source electrode 50, the drain electrode 51, and the wiring, Si ₃ N is formed so as to cover the entire surface.
A protective insulating film 49 made of ₄ and having a film thickness of 500 nm,
Further, the pixel electrode (ITO) 48 is in contact with the source electrode 50 of the N-channel thin film transistor 45 in the image display section through a contact through hole provided in the protective insulating film 49.

Oxidation of the silicon nanoclusters at the time of forming the base film may be performed by a heating method or a combination of an ultraviolet irradiation method and a heating method. in this case,
Ultraviolet irradiation is effective in improving throughput, and heating is effective in improving film quality such as film densification. Further, as the base film, not only a silicon oxide film but also a laminated film of silicon oxide and thin silicon nitride may be used. By using silicon nitride as the buffer layer, it is possible to more effectively prevent the impurities in the glass substrate from diffusing and penetrating into the gate insulating film.

The crystallization method of amorphous silicon may be a solid phase growth method by thermal annealing or a combination of thermal annealing and laser annealing. The gate insulating film may be an oxide film of organosilicon nanoclusters. The action of halogen in the film suppresses the movement of sodium and potassium. The insulating film such as the interlayer film and the protective film may be deposited by a known deposition method such as a plasma CVD method. Further, the gate, source, and drain electrode materials may be known electrode materials such as Al, Ti, and Ta.

Before irradiation with the XeCl excimer laser, heating is performed under vacuum conditions (1 × 10 ⁻⁵ torr) at 500 ° C. for 1 hour. This step is performed in an atmosphere substantially free of oxygen or a reducing atmosphere. Ultraviolet irradiation may be performed, or both may be combined. Ultraviolet irradiation is effective in improving throughput, and heating is effective in improving film quality such as film densification. Further, this step may be omitted, and laser irradiation may be performed in an atmosphere substantially free of oxygen or a reducing atmosphere to crystallize. In this case, the manufacturing cost can be reduced because the process is simplified.

The method for oxidizing the organosilicon nanocluster may be heating in an oxidizing atmosphere. In this case, it is desirable to form the island-shaped semiconductor layer before the oxidation. A dense film can be obtained by heat treatment after forming the island-shaped semiconductor layer. As another manufacturing method, a method in which the island-shaped semiconductor layer is covered with a mask and the island-shaped semiconductor layer and its surrounding insulating film are simultaneously formed by heating in an oxidizing atmosphere is also effective in simplifying the manufacturing process. is there. Furthermore, the film quality of the semiconductor layer is improved by removing the mask and irradiating with ultraviolet rays or laser.

Since the silicon oxide film or the non-single crystal silicon film is formed after forming the organosilicon nanoclusters by the spin coating method, it is effective for the process using a large substrate. Further, since the silicon oxide film formed from the organosilicon nanoclusters contains a halogen element, it is possible to prevent the thin film transistor characteristics from being deteriorated by impurities in the glass substrate.

Further, since the structure in which the step difference at the end of the island-shaped semiconductor layer is reduced can be realized, it is possible to prevent the breakdown voltage from decreasing due to the thinning of the gate insulating film. Compared with conventional island-shaped semiconductor layer formation methods such as exposure, development, and etching, this technique forms an island-shaped semiconductor layer and its surrounding insulating film in fewer steps than conventional methods, such as exposure and heating, or only exposure. Therefore, it is possible to reduce the manufacturing cost. Also,
Since the island-shaped semiconductor layer and the insulating film around the island-shaped semiconductor layer contain a halogen element, it is possible to prevent the deterioration of the thin film transistor characteristics due to the diffusion of impurities from the glass substrate into the gate insulating film.

In the above-mentioned manufacturing method of the present invention, the conventional C
Since the spin coating method is used instead of the VD method, the power consumption during film formation can be reduced. Therefore, a highly reliable and inexpensive liquid crystal display device can be provided. Of course, even if the method for producing a non-single-crystal silicon thin film is changed from the conventional CVD method to the spin coating method of the present invention, uniform film formation can be performed on a large-sized substrate, and power consumption during film formation can be reduced. Due to the advantages, the manufacturing cost can be reduced and an inexpensive liquid crystal display device can be provided.

In the above-mentioned film forming method, after the organosilicon nanoclusters are formed by the spin coating method, the heating is carried out even if ultraviolet irradiation is carried out in an atmosphere substantially free of oxygen or a reducing atmosphere. You may. Furthermore, both may be combined. Ultraviolet irradiation is effective in improving throughput, and heating is effective in improving film quality such as film densification. When laser irradiation is further performed after ultraviolet irradiation or heating, the crystallinity of silicon is improved and the characteristics of the thin film transistor are improved. Further, the step of ultraviolet irradiation or heating may be omitted, and laser irradiation may be performed in an atmosphere substantially free of oxygen or a reducing atmosphere to crystallize. In this case, the manufacturing cost can be reduced because the process is simplified.

The method of manufacturing the thin film transistor is not limited to this embodiment, and may be one used in a conventional liquid crystal panel or the like.

Example 4 A color filter having a colored layer formed by the pattern transfer method of the present invention will be described with reference to the sectional view of FIG. In FIG. 11, 52 is a glass substrate, 53 is a black matrix having a light-shielding property, 5
4 is a red colored layer formed by the pattern transfer method of the present invention, 55 is a green colored layer formed by the same method, 56 is a blue colored layer formed by the same method, 57 is a surface step relaxation and coloring layer, The overcoat layer for preventing diffusion of impurities from the black matrix is shown.

The black matrix 53 can be formed by forming chromium on the glass substrate 52 by sputtering and then patterning by photolithography, or by mixing black pigment dispersed in epoxy or polyimide resin. There are a method of forming a film on the entire surface of a glass substrate by a spinner or a coating method, and then patterning by a photolithography method, a method of simultaneously forming a film and patterning the same material by screen printing, and the like. The black matrix made of chromium formed by sputtering has a large reflection, and for low reflection, a two-layer film structure of chromium and chromium oxide is used.

The material for the colored layers of red 54, green 55 and blue 56 is a curable colored resin composition containing a colorant such as a dye or a pigment and a resin which is cured by heat application or energy application such as light irradiation. To use. As the resin composition, a combination of a known resin and a cross-linking material described in JP-A-2002-243928 can be used.

Specific examples of the thermosetting resin include melamine resin, epoxy resin, and polyimide resin. As the photocurable resin composition, a commercially available negative resist is preferably used. The overcoat layer 57 is formed by a spinner method or a coater method and is made of a highly transparent material such as epoxy resin or polyimide resin.

FIG. 12 is an explanatory view showing a series of steps in a method of manufacturing a color filter showing a fourth embodiment of the present invention. In FIG. 12, 52 is a glass substrate, 58 is a chromium oxide film, 59 is a chromium film, 60 is a black matrix, 61 is a colored layer transfer opening pattern, and 62 is a red colored layer material.

In this embodiment, first, as shown in FIG. 12A, a chromium oxide film 58 having a thickness of 0.05 μm is formed on the entire surface of one side of the glass substrate 12 by sputtering, and chromium is formed thereon in the same manner. A film 59 having a film thickness of 0.05 μm was laminated and then patterned by a photo process to form a black matrix 60. As the glass substrate 12, a glass substrate (Corning # 1737) having a size of 348 mm × 267 mm and a thickness of 0.7 mm was used, and the black matrix 60 was formed in a grid pattern. The size of the black matrix 60 is 280 μm x 80 μm in opening size.
The line width is 20 μm in both the vertical and horizontal directions, and the line width is 768 in the vertical direction and 1024 × 3 colors (R, G,
A total of 3072 pieces of B) were formed in a 4: 3 diagonal 15 inch area.

Next, as shown in FIG. 12B, the glass substrate 12 on which the black matrix 60 is formed is fixed on the substrate fixing table 9 and is formed on the colored layer transfer opening pattern 61 of the screen plate 3 and the glass substrate 12. The openings of the black matrix 60 are aligned, and the screen plate 3 is arranged in a state of being separated from the glass substrate 12 by a small amount, and the squeegee 1 is used to fill the red color layer material 62 into the color layer transfer opening pattern 61 of the screen plate 3. did.

The size of the colored layer transfer opening pattern 61 is smaller than the opening size of the black matrix 60.
The black matrix 60 was formed to have a size of 0 μm × 60 μm, and the black matrix 60 was formed by arranging it at intervals of three in the lateral direction with respect to the openings of the black matrix 60 and at a pitch where the centers overlap. This is because different colored layers are formed on both sides so that one pixel is formed by three openings of the black matrix 60 in which colored layers of three colors (R, G, B) are formed. In addition, as the red layering material 62, a polyimide resin and Nanotech red pigment manufactured by CI Kasei Co., Ltd. in a volume ratio of 5 are used.
The one mixed at a concentration of% was used.

Next, as shown in FIG. 12C, the colored layer transfer opening pattern 61 of the screen plate 3 is filled with the red colored layer material 62 by the air as the gas 7 for jetting from the beam-shaped gas jet nozzle. Extruded, screen version 3
Every third coat was applied in the lateral direction to the openings of the black matrix 60 on the glass substrate 52 fixed to the lower side.

Next, as shown in FIG. 12 (D), the red coloring layer material 62 applied to the openings of the black matrix 60 at intervals of three is heated at 90 degrees for 30 minutes, and then further heated at 180 degrees for 30 minutes. And cured to form a red colored layer 54 having a thickness of 1.5 μm.

Then, as shown in FIG. 12E, the opening of the black matrix 60 adjacent to the red colored layer 54 of the glass substrate on which the red colored layer 54 is formed and the colored layer transfer of the screen plate 3 are transferred. After aligning the opening pattern 61 and applying the green coloring layer material next to the red coloring layer 54 in the same manner as in FIG.
By heating under the same curing conditions as in No. 4, a green colored layer 55 having a film thickness of 1.5 μm was formed.

As the material of the green coloring layer 54, a polyimide resin mixed with Nanotech green pigment manufactured by CI Kasei Co. at a concentration of 5% by volume was used. Screen version 3
May be common to the color layer materials of three colors (R, G, B) as long as the color layer transfer opening pattern 61 can be completely cleaned. However, in order to prevent color mixture of the colored layer material due to poor cleaning, it is preferable to prepare a screen plate for each color. Further, if a device is prepared for each color, it is possible to further improve the throughput.

Next, as shown in FIG. 12 (F), the openings of the black matrix 60 where the colored layers of the glass substrate on which the red colored layer 54 and the green colored layer 55 are not formed are formed, and the screen plate 3 of the screen plate 3. Colored layer transfer opening pattern 61
And aligning the blue colored layer material with the red colored layer 54 and the green colored layer 5 in the same manner as in FIGS.
After being applied between 5 and 5, it was heated under the same curing conditions as the red colored layer 54 and the green colored layer 55 to form a blue colored layer 56 having a film thickness of 1.5 μm. As the material for the blue colored layer 56, a polyimide resin mixed with a nanotech blue pigment manufactured by CI Kasei Co., Ltd. at a concentration of 5% by volume was used.

After that, as shown in FIG. 12G, an overcoat layer 57 was formed on the upper side of the colored layers of red 54, green 55, and blue 56 and the black matrix 60 by a spinner to a film thickness of 1.0 μm. A polyimide resin was used for the overcoat layer, which was heated at 90 degrees for 30 minutes and then further heated at 180 degrees for 60 minutes to be cured. The film thickness of the black matrix 60 is 0.1 μm in total for the chromium layer and the chromium oxide layer, whereas the film thickness of the colored layers for each color is 1.5 μm and 1.4 μm, but there is a surface step. The surface level difference could be reduced to 0.7 μm by the coat layer 57.

In this example, the curing conditions of the respective coloring layer materials were the same, but the curing conditions may be different as long as the respective coloring materials do not cause discoloration by heating each other. Further, it is necessary to cure the overcoat layer in a range that does not cause discoloration in the colored layer. When a 15-inch TFT liquid crystal display was manufactured using this color filter, a good color image could be seen.

(Embodiment 5) The above embodiment 4 is carried out except that the black matrix is formed by the screen printing method.
A color filter was manufactured by the same method as. FIG. 13 is an explanatory diagram showing a series of steps for forming a black matrix by the screen printing method according to the fifth embodiment of the present invention.
In FIG. 13, 63 is a black matrix transfer opening pattern, 64 is a black matrix paste, and 65.
Is the print-formed black matrix.

In this embodiment, first, as shown in FIG. 13A, the center of the formation area of the black matrix transfer opening pattern 63 of the screen plate 3 and the center of the glass substrate 12 are aligned with each other to fix the substrate fixing table 9. The glass substrate 12 was fixed on top. Next, the black matrix paste 64 is placed on the screen plate 3, the scraper 10 is moved in a state of being in contact with the screen plate 3, and the black matrix paste 64 is scraped off while the black matrix paste 64 is placed on the black matrix transfer opening pattern 63. Filled. In FIG. 13A, this is achieved by moving the scraper 10 from right to left.

In this example, as the black matrix paste 64, a polyimide resin mixed with black ultrafine particles NanoTek Black-1 manufactured by CI Kasei Co. at a concentration of 3% by volume was used. The screen plate 3 has a wire diameter of 18 μm and an opening size of 33 μm.
A pattern was formed on a No. 500 stainless steel mesh product having an opening area of 42% and a photosensitive resin for screen mask formation having excellent solvent resistance (product name: NSL) manufactured by Tokyo Process Service Co., Ltd. I used one.

Next, as shown in FIG. 13B, with the squeegee 1 in contact with the screen plate 3, the black matrix paste 62 is rolled by moving it from left to right to form the black matrix transfer opening pattern 63. Filled black matrix paste 6
4 was transferred onto the glass substrate 12.

The screen printing method used here can be formed by the same method as the pattern transfer method of the present invention. The glass substrate 12 was set on the substrate fixing table 9 and was adsorbed under reduced pressure using the fine holes provided in the substrate fixing table 9 to be fixed. Further, after aligning the black matrix transfer opening pattern 63 of the screen plate 3 with the screen mask mounted thereon and the pattern forming position of the glass substrate 12, the screen mask mounted on the screen plate 3 with the gap control jig 8 is used. The gap with the glass substrate 12 is controlled.

It is expected that the screen plate 3 becomes large in size, the gap between the screen mask and the glass substrate 12 cannot be controlled only by the tension of the screen mesh, and the central portion of the screen mask is loosened by its own weight. . In this case, the gap between the screen plate 3 and the substrate fixing table 9 is cut off from the outside by using the gap control jig 8, and a slight amount of gas is introduced into the gap between the screen plate 3 and the substrate fixing table 9. By increasing the pressure from the outside atmospheric pressure, the gap between the screen mask and the glass substrate 12 can be maintained at 0.1 mm to 2.0 mm with respect to the screen plate frame size of 850 mm square.

Since the plate separation due to the tension of the screen mesh is not used, the conventional pattern forming area is 10 to 15% of the screen plate 3, whereas
The pattern formation area in the screen plate 3 was expanded to -50%. Further, when a small amount of gas is introduced into the gap between the screen plate 3 and the substrate fixing table 9, it is possible that the drying speed is high depending on the nature of the paste. Therefore, the introduced gas may dry the black matrix paste 64 and block the opening 4 of the screen mask, making it impossible to form the black matrix transfer opening pattern 63. At that time, by circulating the gas in the gap between the screen plate 3 and the substrate fixing table 9, it is possible to keep the solvent contained in the black matrix paste 64 under the gas atmosphere, and the black matrix paste 64 is dried by the gas. It can be prevented.

Next, the black matrix paste 64 is placed on the screen mask, the scraper 10 and the screen mask are brought into close contact with each other, and the scraper 10 scrapes the black matrix paste 64 at an angle of about 90 ° between the screen mask and the scraper 10. The black matrix transfer opening pattern 63 is filled with the black matrix paste 64. Next, the squeegee 1 is brought into close contact with the screen mask, and the squeegee 1 is moved similarly to the scraper 10, whereby the black matrix paste 64 filled in the black matrix transfer opening pattern 63 can be formed on the glass substrate 12.

Next, as shown in FIG. 13C, the black matrix paste 6 transferred onto the glass substrate 12 is formed.
After heating No. 2 at 90 ° C. for 30 minutes, it was further heated at 180 ° C. for 60 minutes to be cured to form a print forming black matrix 65 having a film thickness of 1.5 μm. The pattern size of the print-formed black matrix 6 is the same as that of the black matrix 60 made of chromium and chromium oxide in Example 4, the opening size is 280 μm × 80 μm, the line width is 20 μm in both length and width, and the formation area is 4: 3. It is 15 inches square.

Next, the fourth embodiment (FIG. 12 (B)-
Similar to (D), the R, G, and B colored layers having a film thickness of 1.5 μm were sequentially formed by the pattern transfer method of the present invention. Then, an overcoat layer was formed on the surface with a spinner to a thickness of 0.2 μm. A cross-sectional view of the color filter manufactured according to this example is shown in FIG. A flat color filter having a small surface step can be obtained by forming the print forming black matrix 65 and the respective colored layers so as to have the same thickness.

In the present embodiment, the film thickness is designed to be 1.5 μm, so that the surface step can be suppressed to 0.1 μm or less. An overcoat layer 57 was formed on the surface by a spinner so as to have a film thickness of 0.2 μm in order to prevent the diffusion of impurities from the print-formed black matrix and each colored layer, not to alleviate the surface step. When a 15-inch TFT liquid crystal display was manufactured using this color filter, a good color image could be seen.

Example 6 A TFT circuit substrate having a color filter was manufactured by forming a colored layer having conductivity on the ITO electrode pattern of the substrate on which the TFT circuit was formed by the pattern transfer method of the present invention. .

15 and 16 are explanatory views showing a series of manufacturing steps of a TFT circuit substrate having a color filter according to the sixth embodiment of the present invention. In FIG. 15, 66 is T
FT glass substrate, 67 is an ITO electrode. In FIG. 16, 68 is a red conductive colored layer material, 69 is a red conductive colored layer, 70 is a green conductive colored layer, and 71 is a blue conductive colored layer.

In this embodiment, first, as shown in FIG. 15A, the TFT circuit and the IT are formed on the TFT glass substrate 66.
The O electrode 67 was formed. The ITO electrode 67 has a vertical length of 280 μ
m, width 80 μm, patterning is performed so as not to overlap the TFT element, and the patterning is performed in the vertical direction at a pitch of 20 μm.
A total of 3072 pieces of 1024 × 3 pieces (three colors of R, G, and B) in the lateral direction were arranged in a region of a diagonal length of 15 inches of 4: 3. This is the pattern of the print-formed black matrix 65 formed in Example 5 above and Examples 4 and 5 above.
The size corresponds to the pattern of each colored layer formed in.

Next, as shown in FIGS. 15B to 15D,
The non-formed portion of the ITO electrode 67 on the TFT glass substrate 66 and the black matrix transfer opening pattern 63 of the screen plate 3 were aligned and fixed on the substrate fixing table 9. Then, in the same manner as in FIGS. 13A to 13C, a print forming black matrix 65 having a film thickness of 1.5 μm.
Was formed on the TFT glass substrate 66.

Next, as shown in FIGS. 16 (A) to 16 (C),
The TFT circuit board 65 was fixed to the board fixing table 9 by aligning the positions of the openings of the printed black matrix 65 and the colored layer transfer opening patterns 61 of the screen plate 3.
Next, the red conductive coloring layer material 68 is applied to FIGS.
After coating in the same manner as above and drying, a red conductive coloring layer 69 having a film thickness of 1.5 μm was formed. For the red conductive coloring layer material 68, 5% by volume of a nanotech red pigment manufactured by CI Kasei Co., Ltd. in a polyimide resin and 1% by weight of an ITO slurry are used.
The one mixed at a concentration of 0% was used. The curing conditions were heating at 90 degrees for 30 minutes and then heating at 200 degrees for 60 minutes.

Next, as shown in FIGS. 16D to 16E,
Similar to FIGS. 16A to 16C, a green conductive coloring layer 70 and a blue conductive coloring layer 71 having a film thickness of 1.5 μm were sequentially formed. For the green conductive colored layer material, a polyimide resin and Nanotech green pigment manufactured by CI Kasei Co., Ltd. are used in a volume ratio of 5
%, ITO slurry mixed at a concentration of 10% by weight, and for the blue conductive coloring layer material, 5% by volume of a nanotech blue pigment manufactured by CI Kasei Co., Ltd.
A mixture containing TO slurry in a concentration of 10% by weight was used. The curing conditions are the same as those for the red conductive coloring layer material 68.

Although the TFT glass substrate having the unevenness on which the ITO electrode 67 is formed is used, the film thickness design value of the print forming black matrix 65 and each conductive coloring layer is 1.5.
Since the color filter was formed according to μm, a color filter having a flat surface was obtained. Also, a T having this color filter
The surface of the FT circuit board cannot be used with an overcoat layer that lowers the conductivity in order to secure the conductivity of the conductive colored layers of each color, and since it directly contacts the liquid crystal, each conductive colored layer and printing It is necessary to remove impurities that deteriorate the electrical characteristics from the formed black matrix 65 as much as possible.

When a 15-inch displayable liquid crystal display was manufactured using the TFT circuit substrate having this color filter, good color development and uniform image could be seen.

[0163]

According to the present invention, after the ink is applied to the entire surface of the screen and the mesh portion or the opening portion of the screen mask is filled with the ink, the jet gas is supplied to the mesh portion or the opening portion so that the ink is applied on the substrate. Since it is transferred onto the substrate, it is possible to form a pattern with higher accuracy and to form a pattern on a substrate having irregularities, as compared with a conventional general screen printing method.

[Brief description of drawings]

FIG. 1 is a schematic view of a pattern transfer device for explaining a first pattern transfer method.

FIG. 2 is a schematic view of a pattern transfer device for explaining a second pattern transfer method.

FIG. 3 is a schematic diagram for explaining the pattern transfer method according to the first embodiment.

FIG. 4 is a process drawing for explaining the manufacturing method of the first organic electroluminescence device.

FIG. 5 is a diagram for explaining formation of a light emitting layer in the first organic electroluminescent device.

FIG. 6 is a diagram for explaining formation of electrodes in the first organic electroluminescence device.

FIG. 7 is a schematic diagram for explaining a display using the organic electroluminescence device of the first embodiment.

FIG. 8 is a schematic diagram for explaining a display using the organic electroluminescence device of the first embodiment.

FIG. 9 is a diagram for explaining a method of forming a color filter that is a second embodiment.

FIG. 10 is a drawing for explaining the method of forming the thin film transistor of the third embodiment.

FIG. 11 is a cross-sectional view illustrating the configuration of a color filter that is a fourth embodiment.

FIG. 12 is a drawing for explaining a series of manufacturing steps of the color filter manufactured in the fourth embodiment.

FIG. 13 is a diagram for explaining a process of forming a black matrix by screen printing manufactured in the fifth embodiment.

FIG. 14 is a cross-sectional view for explaining the structure of the color filter manufactured in the fifth embodiment.

FIG. 15 is a diagram for explaining a manufacturing process up to formation of a black matrix of a TFT circuit substrate having a color filter manufactured in the sixth embodiment.

FIG. 16 is a diagram for explaining a manufacturing process from formation of a colored layer of a TFT circuit substrate having a color filter manufactured in the sixth embodiment.

[Explanation of symbols]

1 ... Squeegee, 2 ... Beam-shaped gas injection nozzle, 3 ...
Screen plate, 4 ... Transfer opening pattern, 5 ... Banked substrate, 6 ... Ink, 7 ... Jetting gas, 8 ... Gap control jig, 9 ... Substrate fixing table 10 ... scraper, 11 ... glass plate, 12 ... anode electrode (IT
O), 13 ... Insulating layer, 14 ... Bank, 15 ... Screen mask (ink quantitative supply jig), 16 ... Mesh, 17 ... Emulsion, 18 ... Hole transport material, 19 ... Light emitting material (green), 20 ... Light emitting material (red), 21 ... Light emitting material (blue), 22 ... Metal mask, 23 ... Cathode electrode, 24 ... Glass substrate , 25 ... Organic electroluminescence device, 26 ... Adsorbent (drying agent), 27 ... Filter material, 28 ... Nitrogen gas (drying), 29 ... Sealing can, 3
0 ... Sealing material, 31 ... External electrode, 32 ... Sealing film, 33 ... Glass plate, 34 ... Sealing resin, 35 ... Color filter (red), 36 ... ..Color filters (green), 3
7 ... Color filter (blue), 38 ... Overcoat film, 39 ... Alkali-free glass substrate, 40 ... Silicon oxide (SiO ₂ ) film, 41 ... Island-like polysilicon film, 42・
..Gate insulating film, 43 ... Gate electrode, 44 ... High resistance N
Type polysilicon layer, 45 ... Low resistance N type polysilicon layer, 46 ... Low resistance P type polysilicon layer, 47 ... Interlayer insulating film, 48 ... Pixel electrode (ITO), 49 ... .Protective insulating film, 50 ... Source electrode, 51 ... Drain electrode, 52 ...
・ Glass substrate, 53 ... Black matrix, 54 ...
Red colored layer, 55 ... Green colored layer, 56 ... Blue colored layer,
57 ... Overcoat layer, 58 ... Chrome film, 59 ...
Chromium oxide film, 60 ... Black matrix (chromium film and chromium oxide film), 61 ... Colored layer transfer opening pattern, 62 ... Red coloring material, 63 ... Black matrix transfer opening pattern, 64 ...・ Black matrix paste, 65 ・ ・ ・ Printing black matrix, 66 ・
..TFT glass substrate, 67 ... ITO electrode, 68 ... Red conductive coloring material, 69 ... Red conductive coloring layer, 70 ... Green conductive coloring layer, 71 ... Blue conductivity Colored layer

─────────────────────────────────────────────────── ─── Continuation of front page (51) Int.Cl. ⁷ Identification code FI theme code (reference) H05B 33/12 H05B 33/12 B 33/14 33/14 A 33/22 33/22 Z (72) Invention Person Takashi Inoue 292 Yoshida-cho, Totsuka-ku, Yokohama-shi, Kanagawa, Ltd., Hitachi, Ltd., Production Technology Laboratory (72) Inventor Keiko Nakano 292, Yoshida-cho, Totsuka-ku, Yokohama, Kanagawa, Japan F-Term, Hitachi, Ltd. (Reference) 2C035 AA06 FA27 FD01 FD31 2H091 FA02X FA02Y FA02Z FA34X FA34Y FA34Z FC01 GA13 LA12 LA17 2H113 AA01 AA03 AA04 BA10 BB22 BC09 CA17 3K007 AB04 AB18 BA06 BB01 BB05 DB03 EA00 FA01 FA02

Claims (18)

[Claims] 1. A bank for element isolation above a substrate, and hole introduction, hole transport, and light emission that contribute at least to light emission,
A method of manufacturing an organic electroluminescent device comprising a layer having an electron transporting function and an electrode, for forming a layer having at least the function of introducing holes, contributing to light emission, hole transporting, light emitting, and electron transporting. 2. The method for manufacturing an image display device, wherein the ink material according to item 1 is transferred and supplied into the bank through an ink fixed amount supply jig that is arranged in non-contact with the substrate. 2. A device isolation bank is formed on a substrate on which an anode electrode is formed, and an ink quantitative supply jig is placed in non-contact with the bank, and the ink quantitative supply jig is individually provided. Supplying at least the ink material for forming a layer having a function of introducing holes, contributing to the emission, hole transport, emission, and electron transport into the bank,
A method of manufacturing an image display device, comprising forming a cathode electrode above the layer having a function of transporting electrons. 3. A device isolation bank is formed on a substrate on which an anode electrode is formed, and an ink quantitative supply jig is placed in non-contact with the bank, and the ink quantitative supply jig is individually provided. Introduction of supplied holes that contribute at least to light emission,
After sequentially supplying an ink material for forming a layer having a function of transporting holes, emitting light, and transporting electrons into the bank,
A cathode electrode is formed above the electron transport layer,
The method of manufacturing an image display device, wherein the ink material for forming the light emitting layer is a material that develops red, green, and blue, and is supplied separately for each bank. 4. A device isolation bank is formed on a substrate on which an anode electrode is formed, and an ink quantitative supply jig is placed in non-contact with the bank, and the ink quantitative supply jig is individually provided. Introduction of supplied holes that contribute at least to light emission,
After sequentially supplying an ink material for forming a layer having a function of transporting holes, emitting light, and transporting electrons into the bank,
A cathode electrode is formed above the layer having the function of transporting electrons, and the ink material for forming the light emitting layer is a material that develops red, green, and blue, and is sequentially in the same bank. A method for manufacturing an image display device, characterized in that the image display device is supplied. 5. A step of (1) forming an anode electrode on a substrate, (2) a step of forming an element isolation bank on the anode electrode, and (3) introducing holes into the bank and transporting holes. A step of forming a layer having the function of
(4) Red, green, on the layer having the function of transporting holes,
A step of separately forming a light emitting layer that emits blue color, and (5)
The method further comprises a step of forming a layer having an electron transporting function on the light emitting layer, and (6) a step of forming a cathode electrode on the electron transporting layer, and at least the above (3) to (5)
In the method of manufacturing an image display device, the step (1) transfers and supplies the ink material made of an organic material supplied to an ink fixed amount supply jig arranged above the bank in a non-contact manner. 6. The ink quantitative supply jig is a transfer mask having an opening formed in a mesh using an emulsion, and a predetermined amount of the ink material is held in the opening. The method for manufacturing an image display device according to claim 1, wherein 7. The ink quantitative supply jig is a transfer mask in which an opening is formed by patterning a base material, and a predetermined amount of the ink material is held in the opening. A method for manufacturing an image display device according to claim 1. 8. The ink material held in the opening of the ink fixed amount supply jig is supplied into the bank by using a jet gas, according to any one of claims 1 to 5. Of manufacturing image display device of. 9. The method for manufacturing an image display device according to claim 1, wherein a cross section of the element isolation bank is formed in a shape that widens toward the substrate side. 10. A device comprising a gate electrode, a gate insulating film, a semiconductor film, a source electrode, a drain electrode, and a pixel electrode on a substrate, and an element above the pixel electrode electrically connected to the drain electrode. A method for manufacturing an organic electroluminescent device, comprising: a bank for separation, a layer having a function of introducing holes that contributes to light emission, hole transport, light emission, and electron transport, and an electrode, and at least a hole that contributes to the light emission. Ink material for forming a layer having functions of introduction, hole transportation, light emission, and electron transportation is transferred and supplied into the bank through an ink quantitative supply jig arranged in non-contact with the substrate. And a method for manufacturing an image display device. 11. The method of manufacturing an image display device according to claim 10, wherein the semiconductor film is made of a polycrystalline silicon film. 12. A method for manufacturing a liquid crystal display type image device device comprising a black matrix for blocking leakage light between elements above a substrate, wherein an ink material for forming red, green and blue colored layers. The method for producing an image display is characterized in that the color filter is transferred and supplied to the inside of the black matrix through an ink fixed amount supply jig arranged in non-contact with the substrate. 13. The black matrix is formed by a screen printing method.
2. The method for manufacturing the image display device according to 2. 14. A leaking light between elements of a drive circuit board, wherein a conductive colored layer formed by transferring and supplying a material having conductivity of red, green, and blue through a fixed amount ink supply jig arranged in a non-contact manner An image display device characterized by a structure arranged on a drive electrode inside a black matrix that shields light. 15. A substrate, a sealing can, a sealing material, and an external terminal are provided, and an image display section produced by the method according to claim 1 is formed above the substrate, and The image display section and the external terminal are electrically connected,
An image display device, characterized in that the substrate and the sealing can are integrated so as to include the image display unit through the sealing material formed around the substrate. 16. The image display device according to claim 15, wherein physical properties of materials forming the substrate and the sealing can are substantially equal to each other. 17. The image display device according to claim 15, wherein the sealing can is a transparent sealing film. 18. A thin film transistor, which is formed above a substrate and has a pixel electrode, and an image display section manufactured by the method according to claim 1, wherein the anode electrode of the image display section is the pixel. An image display device, which is formed above the thin film transistor so as to also serve as an electrode.