WO2015129891A1

WO2015129891A1 - Organic electroluminescent element and method and device for manufacturing same

Info

Publication number: WO2015129891A1
Application number: PCT/JP2015/055971
Authority: WO
Inventors: 高嶋　伸彦; 福田　和浩; 伸明高橋
Original assignee: コニカミノルタ株式会社
Priority date: 2014-02-28
Filing date: 2015-02-27
Publication date: 2015-09-03
Also published as: JPWO2015129891A1

Abstract

Provided are: an organic electroluminescent element of simple construction and having an organic light-emitting layer, a positive pole extraction electrode, and a negative pole extraction electrode formed in a pattern with a high degree of freedom; and a method and device for manufacturing said element. A method for manufacturing an organic electroluminescent element, and a manufacturing device with which the method for manufacturing is employed, said method including: a step for forming a positive pole on a substrate; a step for forming a positive pole extraction electrode and a negative pole extraction electrode on the substrate; a step for forming an insulating layer on the positive pole extraction electrode; a step for forming an organic light-emitting layer on the substrate; a step for removing a portion of the organic light-emitting layer using a laser to form an organic light-emitting layer enclosed in a closed linear state; a step for forming a negative pole on the substrate to seal the upper surface and periphery of the organic light-emitting layer with a negative pole; a step for forming a sealing layer and/or a protective layer on the negative pole; and a step for removing portions of the organic light-emitting layer, the negative pole, the sealing layer, and the protective layer to expose the positive pole extraction electrode and the negative pole extraction electrode on the substrate.

Description

Organic electroluminescence element, manufacturing method and manufacturing apparatus thereof

The present invention relates to an organic electroluminescence element, a manufacturing method thereof, and a manufacturing apparatus thereof.

The mainstream of current organic electroluminescence elements (hereinafter sometimes referred to as “organic EL elements”) is a form in which a light emitting element is formed on a glass substrate. When an organic EL element is formed on a glass substrate, it is formed by laminating various functional films by using a single glass substrate to move between various film forming apparatuses with a robot or the like.

In recent years, attempts have been made to reduce the thickness and flexibility of organic EL devices due to their thin film and self-luminous characteristics. When a thin substrate is used, since the rigidity of the substrate is low, a method of manufacturing an organic EL element after bonding to an existing glass substrate or the like to improve handling is common. Since a thin substrate is generally manufactured in a continuous sheet form, a form wound in a roll form is common.

Generally, a film-formation process in a roll shape is used when a functional film is formed on the entire surface, and since it can be continuously processed, it is used as an efficient and highly productive process method. Therefore, even when manufacturing an organic EL element, if a film forming method in a roll shape can be applied, the productivity is good, and it is possible to manufacture a large amount at a low cost. It is being advanced.

However, in the case of an organic EL element, it is necessary to form a film in a pattern. Further, different mask patterns are required in a plurality of layer configurations. In the single wafer method, a plurality of metal masks are used after being adjusted in position (alignment). There are many problems regarding film formation in a pattern while transporting using a continuous sheet of a thin substrate, and there is currently no decisive method.

Patent Document 1 discloses a method of forming a pattern using a pattern forming mask that moves in synchronization with a support that is continuously conveyed. Patent Document 2 discloses a method of forming a strip-shaped pattern thin film by using a wire-shaped mask while moving it on a strip-shaped substrate that runs continuously.

Patent Document 3 discloses a method for finely patterning an organic EL element using a laser ablation method. After the formation of the cathode / organic compound layer / anode structure, laser beam irradiation is performed from the cathode side to perform fine processing.

JP 2000-183500 A International Publication No. 2011/021622 JP-A-8-222371

However, with the method disclosed in Patent Document 1, it is possible to form an arbitrary pattern shape, but positioning and the like are difficult when forming a multilayer film. Further, in the method disclosed in Patent Document 2, it is difficult to form a pattern in a direction orthogonal to the transport direction, and the pattern shape is limited.

The method disclosed in Patent Document 3 is not limited as in Patent Document 1 and Patent Document 2, but does not disclose a method of forming the anode extraction electrode and the cathode extraction electrode in a specific pattern shape.

The present invention has been made in view of such a situation. An object of the present invention is to provide an organic EL device having an organic light emitting layer, an anode extraction electrode and a cathode extraction electrode having a simple structure and a pattern (shape and position) with a high degree of freedom, a method for producing the same, and a method for producing the same. Is to provide a device.

The inventors of the present invention have studied about the solution of the above-mentioned problem, and can solve the above-mentioned problem by combining the process of forming each layer of the organic EL element and the process of forming a pattern by a laser. I found out.
The present invention has the following configuration.

1. A first step of forming a patterned anode on the substrate; a second step of forming a patterned anode extraction electrode and a patterned cathode extraction electrode on the substrate; and part of the anode extraction electrode A third step of forming a patterned insulating layer on the substrate, a fourth step of forming an organic light emitting layer on the substrate, the anode, the anode extraction electrode, the cathode extraction electrode, and the insulation layer; A part of the organic light-emitting layer on the cathode extraction electrode, a part of the organic light-emitting layer on the insulating layer, and a part of the organic light-emitting layer on the substrate are removed by a laser and surrounded by a closed line shape. A fifth step of forming an organic light emitting layer, the organic light emitting layer, a cathode extraction electrode from which the organic light emitting layer has been removed by the laser, an insulating layer from which the organic light emitting layer has been removed by the laser, and an organic light emitting layer by the laser Removed A sixth step of forming a cathode on the formed substrate, and sealing the upper surface and the periphery of the organic light emitting layer surrounded by the closed line shape with the cathode; and a sealing layer on the cathode; and A seventh step of forming at least one of a protective layer; and the organic light emitting layer, the cathode, the sealing layer, and the organic light emitting layer on each of the substrate, the anode extraction electrode, the insulating layer, and the cathode extraction electrode And an eighth step of removing at least one of the protective layers and exposing the anode extraction electrode and the cathode extraction electrode on the substrate surface.

2. 2. The method for producing an organic electroluminescent element according to 1, wherein the fourth to seventh steps are performed under vacuum and the eighth step is performed under atmospheric pressure.

3. In the eighth step, at least one of the organic light emitting layer, the cathode, the sealing layer, and the protective layer on each part of the substrate, the anode extraction electrode, the insulating layer, and the cathode extraction electrode. 3. The method for producing an organic electroluminescent element according to 1 or 2, wherein the removal is performed by a laser.

4. 4. The method for manufacturing an organic electroluminescence element according to any one of 1 to 3, wherein a position to be removed by the laser is adjusted by an adjustment mechanism based on position information.

5. 5. The method for producing an organic electroluminescence element according to any one of 1 to 4, wherein a long substrate is used as the substrate.

6. An apparatus for forming a patterned anode on a substrate, an apparatus for forming a patterned anode extraction electrode and a patterned cathode extraction electrode on the substrate, and an insulating layer patterned on the substrate An apparatus for forming, an apparatus for forming an organic light emitting layer on the substrate, an apparatus for removing a part of the organic light emitting layer by a laser, an apparatus for forming a cathode on the organic light emitting layer, and the substrate At least one of a device for forming a sealing layer on the substrate and a device for forming a protective layer on the substrate, and at least one of the organic light emitting layer, the cathode, the sealing layer, and the protective layer on the substrate. The apparatus for manufacturing an organic electroluminescence element having an apparatus for removing a portion.

7. An organic electroluminescence element configured by laminating an anode, an anode extraction electrode, a cathode extraction electrode, an insulating layer, an organic light emitting layer, and a cathode on a substrate, wherein the organic light emitting layer has a closed line shape, An organic electroluminescence device, wherein the upper surface and the periphery of the organic light emitting layer are sealed with the cathode, and at least one of a sealing layer and a protective layer is formed on the upper surface of the cathode.

According to the method and apparatus for producing an organic EL element of the present invention, an organic EL element having a simple structure and having an organic light emitting layer, an anode extraction electrode, and a cathode extraction electrode formed in a pattern with a high degree of freedom is provided. can do. The organic EL device of the present invention has a simple structure, can be manufactured by a simple manufacturing method, and has a structure that is not easily affected by the outside world.

It is a typical sectional view of a manufacturing device of an organic EL element concerning a 1st embodiment of the present invention. It is typical sectional drawing in each process of the manufacturing method of the organic EL element concerning 1st Embodiment of this invention. 1 is a schematic plan view of an organic EL element according to a first embodiment of the present invention and a schematic cross-sectional view of an extraction electrode portion thereof.

DETAILED DESCRIPTION OF THE PREFERRED EMBODIMENTS Modes for carrying out the present invention will be described below, but the present invention is not limited to the embodiments described below, and the embodiments are arbitrarily changed within the scope of the present invention. Is possible.

[First Embodiment]
(Organic EL device manufacturing apparatus of the first embodiment)
An organic EL device manufacturing apparatus according to a first embodiment of the present invention includes an apparatus for forming a patterned anode on a substrate, a patterned anode extraction electrode and a patterned cathode extraction electrode on the substrate. A device for forming, a device for forming a patterned insulating layer on a substrate, a device for forming an organic light emitting layer on a substrate, a device for removing a part of the organic light emitting layer by a laser, At least one of a device for forming a cathode on the substrate, a device for forming a sealing layer on the substrate, and a device for forming a protective layer on the substrate, and an organic light emitting layer, a cathode, a sealing layer, and a protective layer on the substrate And a device for removing a part of at least one of the above.

A specific embodiment of the organic EL element manufacturing apparatus of the first embodiment will be described with reference to FIG. FIG. 1A to FIG. 1C are schematic cross-sectional views of an organic EL element manufacturing apparatus according to the first embodiment of the present invention. The organic EL element manufacturing apparatus 100 according to the first embodiment includes a chamber 101 provided with a device for feeding out a long substrate, a chamber 102 provided with a device for forming an organic light emitting layer on the substrate, and a part of the organic light emitting layer. A chamber 103 having a device for removing by a laser, a chamber 104 having a device for forming a cathode on the organic light emitting layer, a chamber 105 having a device for forming a sealing layer on the substrate, and a protective layer on the substrate. A chamber 106 having a forming apparatus and a substrate winding device obtained, a chamber 107 having an apparatus for removing a part of the organic light emitting layer, the cathode, the sealing layer, and the protective layer on the substrate, and cutting the substrate And a chamber 108 provided with a device for performing the above.

Here, an apparatus for forming a patterned anode on a substrate, which is related to the first to third steps of the method of manufacturing an organic EL element according to the first embodiment of the present invention described later, and a pattern formed on the substrate. The apparatus for forming the anode extraction electrode and the patterned cathode extraction electrode and the apparatus for forming the patterned insulating layer on the substrate are not shown. These three devices are devices corresponding to the previous stage of the device shown in FIG.

The chamber 105 in FIG. 1A shows both an apparatus for forming a sealing layer on a substrate, and the chamber 106 shows an apparatus for forming a protective layer on a substrate. Depending on the embodiment, only an apparatus for forming a sealing layer on the substrate of the chamber 105 may be provided, or only an apparatus for forming a protective layer on the substrate of the chamber 106 may be provided.
Similarly, in the chamber 107 in FIG. 1B, an apparatus for removing a part of the organic light emitting layer, the cathode, the sealing layer, and the protective layer on the substrate is illustrated. Depending on the type, the chamber 107 may include a device for removing a part of the organic light emitting layer, the cathode, and the sealing layer on the substrate, or a part of the organic light emitting layer, the cathode, and the protective layer on the substrate. You may provide the apparatus which removes.

The chambers 101 to 108 can be evacuated, and can be processed under vacuum or atmospheric pressure as necessary. As will be described later, in the chambers 101 to 106, processing is continuously performed on a long substrate, and it is preferable that each chamber be in the same temperature, humidity, pressure, and gas environment, It is particularly preferable to be under vacuum. Moreover, it is preferable that the chamber 107 and the chamber 108 are under atmospheric pressure from the property of processing.

In the chamber 101, the long substrate 1 is unwound from the take-up roll 2 and is continuously processed in each chamber from the chamber 102 to the chamber 106. A buffering device may be provided between the chambers so that the substrate can be transported smoothly.

Thus, by using the long substrate 1, it is possible to continuously flow from the substrate feeding device of the chamber 101 to the substrate winding device of the chamber 106. By doing so, an organic EL element can be manufactured with high productivity by a roll-to-roll method. The winding roll 3 wound up after various processing in the chamber 106 is processed in the chamber 107 by a device for removing a part of the organic light emitting layer, the cathode, the sealing layer, and the protective layer on the substrate. It is wound up as a roll 4. Thereafter, the substrate is cut at a predetermined position in the chamber 108 to obtain the product 5 of the organic EL element.

(Manufacturing method of the organic EL device of the first embodiment)
Next, the manufacturing method of the organic EL element of 1st Embodiment is demonstrated.
The organic EL device manufacturing method according to the first embodiment includes a first step of forming a patterned anode on a substrate, and a patterned anode extraction electrode and a patterned cathode extraction electrode on the substrate. A second step, a third step of forming a patterned insulating layer on a portion of the anode extraction electrode, and an organic light emitting layer on the substrate, anode, anode extraction electrode, cathode extraction electrode and insulation layer A fourth step, a part of the organic light emitting layer on the cathode extraction electrode, a part of the organic light emitting layer on the insulating layer, and a part of the organic light emitting layer on the substrate are removed by a laser to form a closed line shape A fifth step of forming an organic light emitting layer surrounded by the organic light emitting layer, a cathode extraction electrode from which the organic light emitting layer has been removed by the laser, an insulating layer from which the organic light emitting layer has been removed by the laser, and an organic light emitting layer by the laser Substrate removed Forming a cathode thereon, sealing the upper surface and the periphery of the organic light emitting layer surrounded by the closed line shape with the cathode, and at least one of a sealing layer and a protective layer on the cathode A seventh step to be formed, and at least one of the organic light emitting layer, the cathode, the sealing layer, and the protective layer on each of the substrate, the anode extraction electrode, the insulating layer, and the cathode extraction electrode is removed, and the anode extraction electrode In the eighth step of exposing the cathode extraction electrode on the substrate surface and in the eighth step, the substrate is cut at a part of the substrate from which at least one of the organic light emitting layer, the cathode, the sealing layer, and the protective layer has been removed. And a ninth step of forming an organic EL element having an organic light emitting layer surrounded by a closed line shape.

FIG. 2 is a schematic cross-sectional view in each step of the method for manufacturing an organic EL element according to the first embodiment of the present invention. Each of the schematic cross-sectional views from (a) to (f) of FIG. 2 shows a cross-sectional form at the time of processing performed in the first to sixth steps of the method of manufacturing the organic EL element of the first embodiment. It is a thing. Each of the schematic cross-sectional views of (g) and (h) of FIG. 2 forms a sealing layer and a protective layer, which are performed in the seventh step of the method of manufacturing the organic EL element of the first embodiment. The form of the cross section of the process to perform is shown. Each of the schematic cross-sectional views of (i) and (j) of FIG. 2 shows a cross-sectional form at the time of processing performed in the eighth step and the ninth step of the method of manufacturing the organic EL element of the first embodiment. Is.
Hereinafter, each step will be described.

(First step)
The first step is a step of forming a patterned anode on the substrate. In FIG. 2 (a), a patterned anode 12 is shown on the substrate 11.

The substrate 11 can be a base material for forming an organic EL element. Examples of the material of the substrate 11 include polyacrylate, polymethacrylate, polyethylene terephthalate (PET), polybutylene terephthalate (PBT), polyethylene naphthalate (PEN), polycarbonate (PC), polyarylate, and polyvinyl chloride. (PVC), polyethylene (PE), polyethylene copolymers such as ethylene-cyclic olefin, polypropylene (PP), polystyrene (PS), polyamide (PA), polyetheretherketone, polysulfone, polyethersulfone, polyimide, polyether Polymers such as imide, heat-resistant transparent base film (product name: Sila-DEC, manufactured by Chisso Corporation) having a basic skeleton of silsesquioxane having an organic-inorganic hybrid structure, and further comprising two or more layers of the polymer. It can be given substrate or the like formed by laminating.

As the material of the substrate 11, polyethylene terephthalate (PET), polybutylene terephthalate (PBT), polyethylene naphthalate (PEN), polycarbonate (PC), and the like are preferably used in terms of cost and availability. Further, in terms of optical transparency, heat resistance, and adhesion to an inorganic layer, a heat resistant transparent film having a basic skeleton of silsesquioxane having an organic-inorganic hybrid structure is preferably used.

The thickness of the substrate 11 is preferably 5 to 500 μm, more preferably 25 to 250 μm, from the viewpoints of handleability and mechanical strength.

The substrate 11 preferably has a function of blocking oxygen and moisture in the atmosphere. In the case of an organic EL element, oxygen and moisture may enter the inside, which may cause deterioration in light emission performance over time. Therefore, it is preferable to block the organic EL element from the outside by sealing it with a gas barrier layer or a sealing material. Therefore, it is preferable that a gas barrier layer is formed on at least one surface of the substrate 11. The gas barrier layer may be organic or inorganic. Examples of the material for the inorganic gas barrier layer include metal oxides such as silicon, aluminum, and titanium, metal nitrides, and metal oxynitrides.

The anode 12 is an electrode film that supplies (injects) holes to the organic light emitting layer. The material type and physical properties of the anode 12 are not particularly limited and can be arbitrarily set. For example, the anode 12 can be formed of a material having a high work function (4 eV or more), for example, an electrode material such as a metal, an alloy, an electrically conductive compound, and a mixture thereof. The anode 12 may be made of a light-transmitting material (transparent electrode) such as indium tin oxide (ITO) or indium zinc oxide. At this time, light emitted from the organic light emitting layer can be extracted from the substrate 11 side.

As a method for forming the anode 12, there are a dry film forming method and a wet film forming method. Dry (vacuum) film forming methods include vapor deposition and sputtering. As a method for forming a pattern by a dry film formation method, a method such as pattern film formation using a metal mask, wet etching using a photoresist or printing, lift-off, or the like can be used.
On the other hand, examples of the wet film forming method include a coating method and an ink jet method. In these methods, it is possible to form a pattern directly.

In the case of a dry film forming method, it is preferable to use wet etching or lift-off in consideration of pattern accuracy, flexibility, productivity, and the like. On the other hand, when a coating method or an inkjet method can be used as the wet film formation method, it is more preferable because a pattern can be directly drawn.

The sheet resistance of the anode 12 is preferably several hundred Ω / □ or less. Further, although the film thickness depends on the material, it is usually selected in the range of 10 to 1000 nm, preferably 10 to 200 nm.

(Second step)
The second step is a step of forming a patterned anode extraction electrode and a patterned cathode extraction electrode on the substrate. In FIG. 2B, a patterned anode extraction electrode 13 and a patterned cathode extraction electrode 14 are shown on the substrate 11.

The anode extraction electrode 13 and the cathode extraction electrode 14 are used when a voltage is applied by connecting the anode and cathode of the organic EL element to an external power source or the like, respectively. As materials for the anode extraction electrode 13 and the cathode extraction electrode 14, metal materials such as Al, Cr, Mo, Ti, Ta, Cu, Ag, Au, and alloys thereof are generally used. The method of forming the anode extraction electrode 13 and the cathode extraction electrode 14 is the same as that of the anode 12. Known methods such as a vapor deposition method, a sputtering method, a coating method, and an ink jet method can be applied. As a method for forming the pattern, a method similar to the method described in the first step can be used.

(Third step)
The third step is a step of forming a patterned insulating layer on a part of the anode extraction electrode. In FIG. 2C, the insulating layer 15 patterned on a part of the anode extraction electrode 13 is shown.

The insulating layer 15 is a layer provided so that the anode extraction electrode 13 and the cathode are not short-circuited when the cathode described later is formed. Examples of the material constituting the insulating layer 15 include inorganic materials such as SiO ₂ , Si ₃ N ₄ , Al ₂ O ₃ , TiO ₂ , SiOxCy, and SiOxNy, and insulating organic materials such as a photoresist. . The method for forming the insulating layer 15 is the same as that for the anode 12. Known methods such as a vapor deposition method, a sputtering method, a coating method, and an ink jet method can be applied. As a method for forming the pattern, a method similar to the method described in the first step can be used.

(4th process)
The fourth step is a step of forming an organic light emitting layer on the substrate, the anode, the anode extraction electrode, the cathode extraction electrode, and the insulating layer. In FIG. 2D, the organic light emitting layer 16 is illustrated on the substrate 11, the anode 12, the anode extraction electrode 13, the cathode extraction electrode 14, and the insulating layer 15.

The organic light-emitting layer 16 has a structure in which holes injected directly from the anode or from the anode through the hole transport layer and the like and electrons injected directly from the cathode or from the cathode through the electron transport layer and the like are regenerated. It is a layer that emits light when bonded. Note that the portion that emits light may be inside the light emitting layer, or may be an interface between the light emitting layer and a layer adjacent thereto.

The organic light emitting layer 16 is preferably formed of an organic light emitting material including a host compound (host material) and a light emitting material (light emitting dopant compound). When the organic light emitting layer 16 is configured in this manner, an arbitrary emission color can be obtained by appropriately adjusting the type of the light emitting material to be included. As the light emitting material included in the organic light emitting layer 16, for example, a phosphorescent light emitting material (phosphorescent compound, phosphorescent light emitting compound), a fluorescent light emitting material, or the like can be used. The organic light emitting layer 16 may contain one type of light emitting material, or may contain a plurality of types of light emitting materials having different light emission maximum wavelengths. About a specific luminescent material, it can select from a well-known material suitably and can be used.

The method for forming the organic light emitting layer 16 is the same as that in the first step, but a vapor deposition method is generally used as a method for forming the layer of the organic light emitting material. In the chamber 102 of FIG. 1A, an apparatus for forming the organic light emitting layer 16 by vapor deposition is described.

In addition to the organic light emitting layer 16, an electron transport layer, a hole transport layer, a hole blocking layer, an electron blocking layer, an electron injection layer (cathode buffer layer), a hole injection layer (anode buffer layer), etc., as necessary. These layers can be formed as appropriate. The specific contents of each layer can be appropriately selected from known knowledge and applied. As a method for forming each of these layers, a vapor deposition method is generally used.

(5th process)
In the fifth step, a part of the organic light-emitting layer on the cathode extraction electrode, a part of the organic light-emitting layer on the insulating layer, and a part of the organic light-emitting layer on the substrate are removed with a laser to form a closed line shape. This is a step of forming an enclosed organic light emitting layer. In FIG. 2 (e), a part of the organic light emitting layer 16 on the cathode extraction electrode 14 and a part of the organic light emitting layer 16 on the insulating layer 15 are removed by laser, and the portions indicated as 17b and 17a are respectively shown. It is shown in the figure.

FIG. 3A is a schematic plan view of the organic EL element according to the first embodiment of the present invention. FIG. 3B is a schematic cross-sectional view of the anode extraction electrode portion AA. FIG. 3C is a schematic cross-sectional view of the cathode extraction electrode portion BB. In FIG. 3, a portion described as L3 is a portion removed by the laser in the fifth step. Due to the presence of L3, the organic light emitting layer 16 surrounded by the closed line shape is formed, and the light emitting part C having the organic light emitting layer 16 surrounded by the closed line shape is formed. .

The organic light emitting layer 16 basically includes an organic compound as a main component. Therefore, by heating to a high temperature, the organic compound can be thermally decomposed, volatilized and scattered. A part of the organic light emitting layer 16 on the cathode extraction electrode 14, a part of the organic light emitting layer 16 on the insulating layer 15 and a part of the organic light emitting layer 16 on the substrate are removed by heating to a high temperature. A part of the extraction electrode 14, a part of the insulating layer 15, and a part of the substrate 11 are exposed to the outside. Thereafter, the cathode can be formed thereon in the next step.

A laser is used as means for removing a part of the organic light emitting layer 16 by heating to a high temperature. A laser is excellent in directivity and convergence, and it is possible to irradiate only a specific fine portion and heat only the fine portion to a high temperature.

Laser processing includes thermal processing and non-thermal processing. Thermal processing is processing performed while laser light is absorbed on the surface of a solid material and converted into heat, and the material is melted with the thermal energy. Infrared lasers that are susceptible to thermal effects are used. On the other hand, non-thermal processing is also called laser ablation processing, which is a processing that instantly melts, absorbs, and scatters the portion where the laser beam is absorbed, even if the material melts at a fairly high temperature under atmospheric pressure. is there. An infrared laser, an ultraviolet laser, a pulse laser, or the like is used depending on the processing content.

In this embodiment, laser ablation processing is preferable because there is little thermal damage to the periphery of the processing portion, and it is possible to remove organic compounds by evaporation and scattering under vacuum and atmospheric pressure.

The wavelength of the laser used in this embodiment is preferably 300 to 700 nm from the viewpoint of energy absorption in the organic layer, but is not limited thereto.

Further, as the laser used in the present embodiment, a pulse laser that can take a wide range of processing conditions such as output, frequency, duty ratio, etc. is preferably used.

The laser medium classification includes solid laser, liquid laser, gas laser, semiconductor laser, and the like. From the viewpoint of high speed and low thermal damage, solid laser or gas laser is preferable. As the solid-state laser, a ruby laser, a YAG laser, a sapphire laser, a titanium sapphire laser or the like can be used, and a YVO ₄ laser is particularly preferable. As the gas laser, a CO ₂ laser, a helium neon laser, an argon ion laser, an excimer laser or the like can be used, and an excimer laser is particularly preferable.

In such a method of removing with a laser, the organic light emitting layer 16 is instantaneously melted, evaporated and scattered. Since the pyrolyzed material becomes a low-molecular substance, it can be scattered far away and can be easily removed and discarded from the system using a vacuum pump or the like.
The chamber 103 in FIG. 1A describes an apparatus for removing a part of the organic light emitting layer with a laser under vacuum.

In this embodiment, the pattern (shape, position) of the organic light emitting layer to be removed by the laser can be formed with high flexibility and accuracy by adjusting the position to be removed by the laser by the adjusting mechanism based on the position information. In the fifth step, the shape and position of part of the organic light emitting layer on the cathode extraction electrode, part of the organic light emitting layer on the insulating layer, and part of the organic light emitting layer on the substrate to be removed Various adjustments can be made by appropriately adjusting the irradiation conditions. As a result, the pattern of the closed organic light emitting layer can be formed with a high degree of freedom and accuracy.

(6th process)
The sixth step includes an organic light emitting layer, a cathode extraction electrode from which the organic light emitting layer has been removed by a laser, an insulating layer from which the organic light emitting layer has been removed by a laser, and a substrate on which the organic light emitting layer has been removed by the laser. It is a process of forming. 2F, the organic light emitting layer 16, the cathode extraction electrode 14 from which the organic light emitting layer 16 has been removed by the laser, the insulating layer 15 from which the organic light emitting layer 16 has been removed by the laser, and the organic light emitting layer have been removed by the laser. A cathode 18 is shown on the substrate 11.

In the sixth step, the upper surface and the periphery of the organic light emitting layer 16 surrounded by the closed line shape formed in the fifth step are sealed with the cathode 18. As a result, the organic light emitting layer 16 has a structure in which the lower surface is sealed with the substrate 11 and the other periphery and the upper surface are sealed with the cathode 18. The metal material usually used for the cathode 18 is excellent in gas barrier properties. Therefore, while having a simple structure, the organic light emitting layer 16 is not easily affected by a gas such as oxygen in the outside world, and the durability of the light emitting performance as the organic EL element can be improved.

The cathode 18 is an electrode that supplies (injects) electrons to the light emitting layer. The material constituting the cathode is not particularly limited, but is usually an electrode material such as a material having a low work function (4 eV or less), for example, a metal (electron injecting metal), an alloy, an electrically conductive compound, and a mixture thereof. It is formed.

As a method for forming the cathode 18, a vapor deposition method is generally used. In the chamber 104 of FIG. 1A, an apparatus for forming the cathode 14 by vapor deposition is described.

The cathode 18 can be formed of a light-transmitting electrode material like the anode. In this case, for example, after forming a metal film made of an electrode material for forming a cathode so as to have a film thickness of 1 nm or more and 20 nm or less, a film made of a conductive transparent material described in the anode 12 is formed on this metal film. Thus, a transparent or translucent cathode can be formed. At this time, the light emitted from the organic light emitting layer 16 can be extracted from the opposite side of the substrate 11.

(Seventh step)
The seventh step is a step of forming at least one of a sealing layer and a protective layer on the cathode. In the seventh step, any one of the three methods of forming only the sealing layer on the cathode, forming only the protective layer, and forming both the sealing layer and the protective layer is performed. You may apply.

In FIG. 2G, the formation of the sealing layer 19 on the cathode 18 is illustrated. FIG. 2 (h) shows that the protective layer 20 is formed on the sealing layer 19. In the seventh step, when forming both the sealing layer and the protective layer, it is usually preferable to first form the sealing layer 19 and then form the protective layer 20 thereon.

The sealing layer 19 is for shielding and protecting the organic light emitting layer 16 from the external environment. The sealing layer 19 has a gas barrier property against water vapor and oxygen.

As a material constituting the sealing layer 19, for example, an inorganic material such as SiO ₂ , Si ₃ N ₄ , Al ₂ O ₃ , TiO ₂ , SiOxCy, or SiOxNy is used.

Also for the method of forming the sealing layer 19, a known method such as a vapor deposition method, a sputtering method, a CVD method, or an ion plating method can be applied. In the chamber 105 of FIG. 1A, an apparatus for forming the sealing layer 19 by a sputtering method is described.

The protective layer 20 is a layer that is installed on the sealing layer 19 and protects the internal organic EL element from an external physical external force.
Examples of the material constituting the protective layer 20 include, for example, ethylene tetrafluoroethylene copolymer, polyethylene, polypropylene, polystyrene, polymethyl methacrylate, nylon, polyethylene terephthalate, polyethylene naphthalate, polycarbonate, polyimide, and polyethersulfone. Examples thereof include curable resins such as thermoplastic resins, urea resins, melamine resins, phenol resins, resorcinol resins, epoxy resins, unsaturated polyester resins, polyurethane resins, and acrylic resins. Furthermore, the protective layer 20 preferably has a function of blocking oxygen and moisture in the atmosphere. That is, it is preferable that a gas barrier layer is formed on at least one surface of the protective layer 20. The gas barrier layer may be organic or inorganic. Examples of the material for the inorganic gas barrier layer include metal oxides such as silicon, aluminum, and titanium, metal nitrides, and metal oxynitrides. If it is the protective layer 20 provided with such a gas barrier layer, the structure without the sealing layer 19 is also possible.

Furthermore, in order to adhere a layer made of these resins to the sealing layer or the like, an adhesive layer may be provided and laminated. As a material constituting the adhesive layer, any of a thermosetting resin, a photocurable resin, and a thermoplastic resin can be used. As the thermosetting resin, for example, epoxy resin, acrylic resin, silicone resin, urea resin, melamine resin, phenol resin, resorcinol resin, unsaturated polyester resin, polyurethane resin, etc. Resin. Examples of the photocurable resin include radical curable resins such as ester acrylates, urethane acrylates, epoxy acrylates, melamine acrylates, acrylic resin acrylates, etc., or radical photocurable resins using resins such as urethane polyesters, epoxies, vinyl ethers, and the like. Examples thereof include a cationic photocurable resin using a resin. Examples of the thermoplastic resin include polyethylene, polypropylene, polyamide, polyethylene terephthalate (PET), polyvinyl alcohol (PVA), ethylene-vinyl acetate copolymer (EVA), ethylene-propylene copolymer, ethylene-acrylic acid copolymer. Polymers, ethylene-methacrylic acid copolymers, polyvinylidene chloride (PVDC), ionomers and the like can be used.

As a method of forming the protective layer 20, a known method such as a laminating method can be applied. In the chamber 106 of FIG. 1A, an apparatus for forming the protective layer 20 by a laminating method is described.

From the fourth step to the seventh step, it is possible to process continuously by using a long substrate. Therefore, the chamber provided with the apparatus which performs each process can be connected, and an organic EL element can be manufactured with high productivity by a roll-to-roll system. Further, since it is preferable to use a vapor phase method such as a vapor deposition method or a sputtering method, the fourth to seventh steps are preferably performed under vacuum.

(8th step)
In the eighth step, at least one of the organic light-emitting layer, the cathode, the sealing layer, and the protective layer on each of the substrate, the anode extraction electrode, the insulating layer, and the cathode extraction electrode is removed, and the anode extraction electrode and the cathode are removed. In this step, the extraction electrode is exposed on the substrate. In FIG. 2 (i), the organic light emitting layer 16, the cathode 18, the sealing layer 19 and the protective layer 20 on each part of the substrate 11, the anode extraction electrode 13, the insulating layer 15 and the cathode extraction electrode 14 are removed. Thus, the anode extraction electrode 13 and the cathode extraction electrode 14 are exposed on the substrate, and the portions indicated as 21a and 21b are illustrated.

A laser is used as a method for removing the organic light emitting layer 16, the cathode 18, the sealing layer 19 and the protective layer 20 on each of the substrate 11, the anode extraction electrode 13, the insulating layer 15 and the cathode extraction electrode 14. A method using an electron beam, a method using an ion beam, and the like. Among these, a method using a laser is preferable because it can be processed with a relatively simple apparatus.

In the eighth step, part of the organic light emitting layer 16, the cathode 18, the sealing layer 19 and the protective layer 20 in the vicinity of a part of the anode extraction electrode 13 and the part of the cathode extraction electrode 14 are heated to a high temperature by a laser. As a result, a part of the anode extraction electrode 13 and a part of the cathode extraction electrode 14 are exposed to the outside. Therefore, after cutting the organic EL element in the next ninth step, it is easy to connect an external power source or the like to each electrode of the organic EL element when the individual organic EL element is actually caused to emit light.

The specific content of the method of removing with a laser is the same as the content described in the fifth step, and the description thereof is omitted.
In general, the organic light emitting layer is easily scattered by a laser. Therefore, the sealing layer and the protective layer existing on the organic light emitting layer can be simultaneously scattered. However, since what is removed by the laser may include a high molecular weight protective layer, it is preferable to appropriately adjust the laser irradiation conditions depending on the object to be removed.

Also, what is thermally decomposed by the laser has a relatively high molecular weight compared to the case of the fifth step, so that it can be scattered and easily removed and discarded from the system at atmospheric pressure. It is preferable to carry out below.

In the eighth step, the shapes and positions of the organic light emitting layer 16, the cathode 18, the sealing layer 19 and the protective layer 20 to be removed can be variously changed by appropriately adjusting the irradiation conditions such as laser. As a result, regardless of the pattern (shape and position) of the patterned anode extraction electrode 13 and the patterned cathode extraction electrode 14, the exposed anode extraction electrode and cathode extraction electrode patterns can be formed with high flexibility and accuracy. can do.

In this embodiment, the degree of freedom and accuracy of the pattern of the organic light emitting layer 16, the anode extraction electrode 13 to be exposed, and the cathode extraction electrode 14 are adjusted by adjusting the position to be removed by a laser or the like by an adjustment mechanism based on position information. Can be increased.

(9th step)
The ninth step is the eighth step, in which the organic light emitting layer surrounded by a closed line shape is cut by cutting a part of the substrate from which the organic light emitting layer, the cathode, the sealing layer and the protective layer have been removed. This is a step of forming an organic EL element. In FIG. 2 (j), the substrate 11 is cut by a part of the substrate 11 from which the organic light emitting layer 16, the cathode 18, the sealing layer 19 and the protective layer 20 have been removed, and is surrounded by a closed line shape. An organic EL element having a light emitting layer is illustrated. The obtained organic EL element has the light emission part E, the anode extraction electrode part T1, and the cathode extraction electrode part T2.

The method for cutting the substrate can be applied by appropriately selecting a known method. At that time, it is preferable to adjust the cutting position by an adjustment mechanism based on position information. In the chamber 108 of FIG. 1C, there is described an apparatus for cutting a substrate by an upper and lower cutter under atmospheric pressure.

FIG. 3A is a schematic plan view of the organic EL element according to the first embodiment of the present invention. FIG. 3B is a schematic cross-sectional view of the anode extraction electrode portion AA. FIG. 3C is a schematic cross-sectional view of the cathode extraction electrode portion BB. L1 and L2 indicate locations removed in the eighth step.

An organic light emitting layer surrounded by a closed line shape by applying a voltage to the exposed anode extraction electrode 13 and cathode extraction electrode 14 in the anode extraction electrode portion L1 and the cathode extraction electrode portion L2 of the organic EL element, respectively. The light emitting part C having the light emits light.

[Modification of First Embodiment]
The first embodiment uses a long substrate. As a modification of the first embodiment, a single-wafer substrate can be used as the substrate. In that case, there is no ninth step in the manufacturing method of the first embodiment. By separating the chambers 102 to 107 corresponding to the respective steps shown in FIG. 1 and performing the steps from the first step to the eighth step in order, a single wafer type organic EL element can be manufactured. .

(Effect of 1st Embodiment)
According to the manufacturing method of the first embodiment, in the fifth step, the organic light emission surrounded by the closed line shape with a wider degree of freedom is obtained by removing with the laser in the fifth step than when not removing with the laser. A layer pattern can be formed.
In addition, when a long substrate is used, it is possible to form a simple and highly flexible pattern continuously in a roll-to-roll manner, increasing the productivity and reducing the cost.

The upper surface and the periphery of the organic light-emitting layer surrounded by the closed line shape are sealed with a cathode, so that the influence from the outside can be eliminated and a highly durable organic EL element can be obtained.
Furthermore, since it can be manufactured by a relatively simple method, the manufacturing cost can be reduced.
Further, by increasing the accuracy of removal processing by laser, it becomes possible to manufacture an organic EL element in which the shape and position of the organic light emitting layer are finely and complicatedly installed.

Further, the removal by the laser in the fifth step is to remove only the organic light emitting layer before forming the cathode, it is a scattering of only the organic light emitting layer that is relatively easily decomposed, there is little contamination to other layers, and the organic Defects as EL elements are unlikely to occur.

[Organic EL device]
An organic EL device comprising an anode, an anode extraction electrode, a cathode extraction electrode, an insulating layer, an organic light emitting layer, and a cathode stacked on a substrate by using the manufacturing method and the manufacturing apparatus of the first embodiment. The organic light emitting layer has a closed linear shape, the organic light emitting layer has an upper surface and a periphery sealed with a cathode, and at least one of a sealing layer and a protective layer is formed on the upper surface of the cathode. Can be formed.

Such an organic EL element has a linear shape in which the organic light emitting layer is closed. A substrate is present on the lower surface of the organic light emitting layer. On the other hand, a cathode exists on the upper surface and the periphery of the organic light emitting layer, and the organic light emitting layer is sealed with the cathode. Further, at least one of a sealing layer and a protective layer is present on the upper surface of the cathode.

Since the thickness of the cathode increases in the end face direction around the organic light emitting layer, the gas barrier property in the end face direction of the organic light emitting layer is good even with only the cathode.
Further, not only the cathode but also at least one of a sealing layer and a protective layer is present in the upper surface direction of the organic light emitting layer. Therefore, the gas barrier property in the upper surface direction of the organic light emitting layer is also good.
For these reasons, the organic EL element has a simple structure and can be manufactured by a simple manufacturing method, but the organic light emitting layer is blocked from the outside world and is not easily affected by the outside world. The light-emitting performance is excellent in durability.

DESCRIPTION OF SYMBOLS 11 Substrate 12 Anode 13 Anode extraction electrode 14 Cathode extraction electrode 15 Insulating layer 16 Organic light emitting layer 18 Cathode 19 Sealing layer 20 Protective layer 100 Organic EL device manufacturing apparatus

Claims

A first step of forming a patterned anode on a substrate;
A second step of forming a patterned anode extraction electrode and a patterned cathode extraction electrode on the substrate;
A third step of forming a patterned insulating layer on a portion of the anode extraction electrode;
A fourth step of forming an organic light emitting layer on the substrate, the anode, the anode extraction electrode, the cathode extraction electrode and the insulating layer;
A part of the organic light-emitting layer on the cathode extraction electrode, a part of the organic light-emitting layer on the insulating layer, and a part of the organic light-emitting layer on the substrate are removed by a laser and surrounded by a closed line shape. A fifth step of forming the organic light emitting layer;
Forming a cathode on the organic light emitting layer, a cathode extraction electrode from which the organic light emitting layer has been removed by the laser, an insulating layer from which the organic light emitting layer has been removed by the laser, and a substrate from which the organic light emitting layer has been removed by the laser; A sixth step of sealing the upper surface and the periphery of the organic light emitting layer surrounded by the closed line shape with the cathode;
A seventh step of forming at least one of a sealing layer and a protective layer on the cathode;
Removing at least one of the organic light emitting layer, the cathode, the sealing layer, and the protective layer on each of the substrate, the anode extraction electrode, the insulating layer, and the cathode extraction electrode; And an eighth step of exposing the extraction electrode and the cathode extraction electrode on the surface of the substrate.
The method for producing an organic electroluminescent element according to claim 1, wherein the fourth step to the seventh step are performed under vacuum and the eighth step is performed under atmospheric pressure.
In the eighth step, at least one of the organic light emitting layer, the cathode, the sealing layer, and the protective layer on each part of the substrate, the anode extraction electrode, the insulating layer, and the cathode extraction electrode. 3. The method for manufacturing an organic electroluminescence element according to claim 1, wherein the removal is performed by a laser.
The method for manufacturing an organic electroluminescence element according to any one of claims 1 to 3, wherein a position to be removed by the laser is adjusted by an adjustment mechanism based on position information.
5. The method of manufacturing an organic electroluminescence element according to claim 1, wherein a long substrate is used as the substrate.
An apparatus for forming a patterned anode on a substrate;
An apparatus for forming a patterned anode extraction electrode and a patterned cathode extraction electrode on the substrate;
An apparatus for forming a patterned insulating layer on the substrate;
An apparatus for forming an organic light emitting layer on the substrate;
An apparatus for removing a part of the organic light emitting layer with a laser;
An apparatus for forming a cathode on the organic light emitting layer;
At least one of an apparatus for forming a sealing layer on the substrate and an apparatus for forming a protective layer on the substrate;
An apparatus for producing an organic electroluminescence element, comprising: an apparatus for removing at least one of the organic light emitting layer, the cathode, the sealing layer, and the protective layer on the substrate.
An organic electroluminescence device configured by laminating an anode, an anode extraction electrode, a cathode extraction electrode, an insulating layer, an organic light emitting layer, and a cathode on a substrate,
The organic light emitting layer has a closed line shape;
The upper surface and the periphery of the organic light emitting layer are sealed with the cathode,
An organic electroluminescent element, wherein at least one of a sealing layer and a protective layer is formed on an upper surface of the cathode.