JP2016119208A - Method for manufacturing organic light-emitting device - Google Patents

Abstract

PROBLEM TO BE SOLVED: To provide a method for manufacturing an organic light-emitting device, capable of reducing generation of dark spots and manufacturing the organic light-emitting device having a long emission life.SOLUTION: An organic light-emitting device includes a light extraction layer, a barrier layer, and a transparent electrode laminated in this order on a transparent substrate. The organic light-emitting device also includes an organic layer including an organic light-emitting material and a counter electrode of the transparent electrode, which are arranged on the transparent electrode. A method for manufacturing the organic light-emitting device comprises: a step S10 of forming the light extraction layer on the transparent substrate by pattern-coating in atmospheric environment; a step S20 of subjecting the formed light extraction layer to a vacuum heat treatment; a step S30 of forming the barrier layer on the light extraction layer continuously while keeping the light extraction layer subjected to the vacuum heat treatment in a pressure-reduced atmosphere; and a step S40 of forming the transparent electrode on the formed barrier layer.SELECTED DRAWING: Figure 2

Description

  The present invention relates to a method for manufacturing an organic light emitting device.

  An organic light-emitting device using electroluminescence (EL), an organic light-emitting material, is a thin-film complete solid-state device that can emit light at a low voltage of several volts to several tens of volts, and has high luminance and high luminous efficiency. It has many excellent features such as thinness and light weight. Therefore, in recent years, it has been attracting attention as a backlight for various displays, a display plate such as a signboard or emergency light, and a surface light emitter such as an illumination light source.

  The organic light emitting device has a pair of an anode and a cathode and an organic layer disposed between the anode and the cathode on a substrate. The organic layer includes an organic light emitting material, and has a layer structure including, for example, a light emitting layer containing the organic light emitting material and a layer having charge transporting properties. As a method for extracting emitted light to the outside in an organic light emitting device, there are a bottom emission method in which light is extracted from a substrate side on which a drive circuit and the like are provided, and a top emission method in which light is extracted from a side opposite to the substrate. In a bottom emission type organic light emitting device, a transparent substrate having light transmittance is usually used, and a transparent electrode serving as an anode is formed on the transparent substrate side.

  When taking out the emitted light generated in the light emitting layer to the outside, it is necessary to suppress total reflection of the emitted light at the interface between the transparent electrode and the transparent substrate. This is because, if the emitted light is totally reflected, for example, light in a waveguide mode confined in the element is generated, resulting in a decrease in luminous efficiency. Further, when taking out the emitted light to the outside, adjustment of luminous brightness, chromaticity, viewing angle, and the like may be required for required performance. For these reasons, organic light emitting devices have conventionally been provided with a so-called light extraction layer between a transparent substrate and a transparent electrode for the purpose of improving light extraction efficiency or adjusting optical characteristics. There are many.

  By the way, it is known that an organic material or the like constituting an organic light emitting element is easily deteriorated by oxygen, moisture or the like. Therefore, a surface of the organic light emitting element opposite to the substrate is provided with a sealing member or a layer having a high gas barrier property, or a material used for manufacturing the organic light emitting element is previously deaerated and dehydrated. On the other hand, outgas which deteriorates organic materials etc. may generate | occur | produce from the light extraction layer itself provided between the transparent substrate and the transparent electrode. Therefore, conventionally, a barrier layer is provided between the transparent electrode and the light extraction layer to prevent intrusion of the generated outgas.

  For example, Patent Document 1 describes an organic electroluminescence element in which a base layer and a smoothing layer are provided on a substrate, and a gas barrier layer is provided on the smoothing layer (see paragraphs 0039 and 0040). Patent Document 2 describes a light extraction sheet disposed on the surface of the organic electroluminescent device on the organic electroluminescent layer side of the organic electroluminescent device, and has a configuration having at least an adhesive layer, a base material, a fine particle layer, and a barrier layer in this order. (See paragraphs 0011 and 0012).

JP 2008-016347 A JP 2012-089313 A

  According to the techniques described in Patent Document 1 and Patent Document 2, since a barrier layer (gas barrier layer) is disposed on the substrate side of the transparent electrode, outgas, oxygen, moisture, and the like enter the inside of the device. It can be said that this can be suppressed. However, the light extraction layer such as the underlayer and smoothing layer of Patent Document 1 and the fine particle layer of Patent Document 2 is mainly composed of a resin material, and is formed by dispersing particles that adjust optical characteristics in the resin material. In general, it is often formed by full-surface application (solid application) of a resin particle mixed solution using a wet application method or the like.

  FIG. 4 is a cross-sectional view schematically showing an example of the configuration of the organic light emitting device according to the comparative example. An organic light emitting device 100C (conventional organic light emitting device) according to the comparative example includes, for example, a transparent substrate 1, a light extraction layer 2c, a barrier layer 3c, a transparent electrode 4, and an organic layer 5 as shown in FIG. And a counter electrode 6, an adhesive layer 7, and a sealing member 8. When the light extraction layer 2c is formed on the transparent substrate 1 by coating on the entire surface, as shown in FIG. 4, the side surface of the light extraction layer 2c is exposed to the side of the organic light emitting device 100C and is in contact with the outside air. Become. Therefore, outgas, oxygen, moisture, etc. existing in the atmosphere are likely to enter from the side surface of the light extraction layer 2c, and the organic light emitting element 100C may be easily deteriorated.

  The barrier property of the side surface of the light extraction layer can be enhanced by patterning the light extraction layer (pattern formation) and sealing the side surface of the patterned light extraction layer (the light of FIG. 1). (See take-out layer 2). However, when such a method is adopted, it is necessary to laminate a barrier layer on the light extraction layer patterned on the transparent substrate in manufacturing the organic light emitting device (see barrier layer 3 in FIG. 1). ). At this time, a film formation surface of the barrier layer tends to be deteriorated because a film formation surface on which the barrier layer is formed has a level difference due to the patterned light extraction layer. Therefore, pinholes and cracks are likely to occur around the vicinity of the step, and the performance of the barrier layer may be reduced.

  Since the light extraction layer is often formed in an atmospheric environment, there is a situation that oxygen, moisture, and the like easily enter during the manufacturing process. Further, since the formation is performed in an atmospheric pressure atmosphere, the outgas once released from the light extraction layer itself is likely to be reattached. For this reason, depending on the barrier layer whose performance has deteriorated because it was formed on the patterned light extraction layer, outgas, oxygen, moisture, etc. attached to and penetrated the light extraction layer are transmitted to the organic layer side. There is a fear that it will not be possible to sufficiently prevent it. The outgas, oxygen, moisture, etc. that have adhered to and penetrated the light extraction layer will continue to be transmitted to the organic layer side even in a reduced pressure atmosphere where the cleanliness is controlled so that the organic layer is formed. This causes a problem that the emission lifetime of the organic light emitting device is reduced.

  On the other hand, in a general manufacturing process of an organic light emitting device, a drying process is performed immediately before film formation of a transparent electrode, an organic layer, etc. in a reduced pressure atmosphere for the purpose of removing moisture contained in the base material. May be provided. However, even if drying is performed after the barrier layer is formed on the light extraction layer, it is difficult to sufficiently remove moisture and the like from the light extraction layer. Therefore, there is a problem that moisture or the like remaining in the light extraction layer is then transmitted to the organic layer side to cause a dark spot.

  Accordingly, an object of the present invention is to provide a method for manufacturing an organic light emitting device that can manufacture an organic light emitting device with reduced generation of dark spots and a good light emission lifetime.

  The above object of the present invention is achieved by the following configurations.

  1. A light extraction layer, a barrier layer, and a transparent electrode are sequentially laminated on the transparent substrate, and an organic layer containing an organic light emitting material and a counter electrode that is a counter electrode of the transparent electrode are disposed on the transparent electrode. A method for manufacturing an organic light emitting device, the step of forming the light extraction layer on the transparent substrate by pattern coating in an atmospheric environment, the step of subjecting the formed light extraction layer to vacuum heat treatment, and the vacuum heat treatment A step of continuously forming the barrier layer on the light extraction layer while maintaining the light extraction layer in a reduced pressure atmosphere, and a step of forming the transparent electrode on the formed barrier layer. A method for producing an organic light-emitting device.

  2. 2. The method for producing an organic light-emitting element according to 1 above, wherein the heating in the vacuum heat treatment is performed by infrared heating.

  3. 2. The method of manufacturing an organic light-emitting element according to 1 above, wherein the infrared heating is performed by infrared light whose wavelength is controlled in a non-absorption wavelength region of the transparent substrate.

  ADVANTAGE OF THE INVENTION According to this invention, generation | occurrence | production of a dark spot can be reduced and the manufacturing method of the organic light emitting element which made it possible to manufacture the organic light emitting element with the favorable light emission lifetime can be provided.

It is sectional drawing which shows typically an example of a structure of the organic light emitting element manufactured by the manufacturing method of the organic light emitting element which concerns on this embodiment. 3 is a flowchart illustrating an example of a method for manufacturing an organic light emitting device according to the present embodiment. It is a figure which shows schematic structure of an example of the manufacturing apparatus of the organic light emitting element which concerns on this embodiment. (A) is a schematic configuration of the light extraction layer forming portion, (b) is a schematic configuration of the barrier layer forming portion, and (c) is a diagram illustrating a schematic configuration of the element forming portion. It is sectional drawing which shows typically an example of a structure of the organic light emitting element which concerns on a comparative example.

  Hereinafter, a method for manufacturing an organic light emitting device according to an embodiment of the present invention will be described in detail. In addition, in each figure, about the same component, the same code | symbol is attached | subjected and the overlapping description is abbreviate | omitted.

  First, the structure of the organic light emitting device manufactured by the method for manufacturing the organic light emitting device according to this embodiment will be described.

  FIG. 1 is a cross-sectional view schematically showing an example of the configuration of an organic light emitting device manufactured by the method for manufacturing an organic light emitting device according to this embodiment.

  As shown in FIG. 1, in the organic light emitting device 100, a light extraction layer 2 (2 a, 2 b), a barrier layer 3, and a transparent electrode 4 are sequentially laminated on a transparent substrate 1, and an organic layer 5 is formed on the transparent electrode 4. And a counter electrode 6 which is a counter electrode of the transparent electrode 4 are arranged. The light extraction layer 2 is patterned on the transparent substrate 1 and differs from the conventional organic light emitting device (100C) (see FIG. 4) in that it is provided only on a part of the transparent substrate 1. . In the manufacturing method of the organic light emitting device according to the present embodiment, the organic light emitting device 100 is manufactured in such a manner that the light extraction layer 2 is not exposed to the side of the device.

  For example, a drive circuit and a power source (not shown) are electrically connected to the transparent electrode 4 and the counter electrode 6 provided in the organic light emitting device 100 via a lead portion, for example. The transparent electrode 4 can be an anode and the counter electrode 6 can be a cathode. The organic layer 5 has a single layer configuration or a multiple layer configuration including at least a light emitting layer. Examples of other layers of the light emitting layer constituting the organic layer 5 include a hole injection layer, a hole transport layer, an electron blocking layer, a hole blocking layer, an electron transport layer, and an electron injection layer. When a voltage is applied between the transparent electrode 4 and the counter electrode 6, electrons and holes are respectively injected into the light emitting layer to emit light. The generated emitted light passes through the transparent electrode 4, the light extraction layer 2, and the transparent substrate 1, and is extracted outside the organic light emitting element 100.

  As shown in FIG. 1, the light extraction layer 2 includes a scattering layer 2 a and a smooth layer 2 b, and the end portion is located on the inner side of the side end surface of the transparent substrate 1 by pattern formation. . The scattering layer 2a and the smoothing layer 2b have a function of improving light extraction efficiency by scattering transmitted light and waveguide mode light to reduce total reflection and waveguide mode light confinement at the interface. Yes. Further, the scattering layer 2a and the smooth layer 2b have a high refractive index in order to take out light emitted from the transparent electrode 4 with high efficiency. The scattering layer 2a is a layer specialized for light scattering by Mie scattering or the like, and the smooth layer 2b is a layer that absorbs irregularities generated on the surface of the scattering layer 2a and smoothes the surface of the light extraction layer 2. It has become. However, the light extraction layer 2 is not limited to the configuration shown in FIG. 1, and other layers that perform optical functions may be used in combination. Moreover, it can also be set as the single | mono layer structure which has an equivalent function, and can also be set as the multilayered structure of 3 or more layers.

  The barrier layer 3 is a layer having a high gas barrier property against various gases such as oxygen and water vapor, and is interposed between the light extraction layer 2 and the transparent electrode 4. The barrier layer 3 is reduced in pressure using, for example, inorganic compounds such as silicon oxide, aluminum oxide, and magnesium oxide, and organic compounds such as silane, alkoxysilane, halogenated silane, organosiloxane, silazane, organopolysiloxane, and organopolysilazane as precursors. It is formed by vapor deposition below. The barrier layer 3 may have a single-layer configuration using any one of such inorganic compounds and organic compounds as a precursor, or may have a multi-layer configuration having a laminated structure. FIG. 1 schematically shows that the barrier layer 3 is formed only on the light extraction layer 2, but in detail, the upper surface of the transparent substrate 1 and the side of the light extraction layer 2 are shown. It may be formed so as to cover. Providing the barrier layer 3 prevents oxygen, moisture, and the like from entering the transparent electrode 4 side from the light extraction layer 2 side.

  A sealing member 8 is provided on the opposite side of the organic light emitting element 100 from the transparent substrate 1 with an adhesive layer 7 interposed therebetween. The adhesive layer 7 and the sealing member 8 prevent oxygen, moisture, and the like in the outside air from entering from the side of the organic light emitting element 100 opposite to the transparent substrate 1. The adhesive layer 7 covers the side of the patterned light extraction layer 2 and the like, and the light extraction layer 2 is not exposed to the side of the element. Such a structure is suitable for improving the barrier property of the side surface of the light extraction layer 2, and is effective in preventing oxygen, moisture, etc. in the outside air from directly entering the light extraction layer 2. . In a structure in which oxygen, moisture, etc. directly enter from the side surface of the light extraction layer 2, even if the barrier layer 3 is formed, oxygen, moisture, etc. are transmitted from the light extraction layer 2 to the transparent electrode 4 side. This is because it cannot be completely prevented.

  Next, a method for manufacturing the organic light emitting device according to this embodiment will be described.

  In general, an organic light emitting device 100 configured as shown in FIG. 1 is manufactured by sequentially laminating a light extraction layer 2, a barrier layer 3, a transparent electrode 4, an organic layer 5, and a counter electrode 6 on a transparent substrate 1. Yes. Therefore, even when the light extraction layer 2 is patterned to be not exposed to the side of the element as described above, outgas, oxygen, moisture in the environment during the manufacturing process of the organic light emitting element 100 May enter the light extraction layer 2 before the barrier layer 3 is laminated. On the other hand, the barrier layer 3 laminated on the light extraction layer 2 is not necessarily good in film formability because the light extraction layer 2 patterned on the transparent substrate 1 generates a step corresponding to the film thickness. The gas barrier property may be lowered. Therefore, outgas, oxygen, moisture and the like that have entered the light extraction layer 2 during the manufacturing process before the barrier layer 3 is laminated are used in the organic light emitting device 100 even after the barrier layer 3 is formed. Deterioration of organic materials may occur. Therefore, in the method for manufacturing the organic light emitting device according to this embodiment, the light extraction layer 2 immediately before the barrier layer 3 is laminated is subjected to vacuum heat treatment, and the outgas, oxygen, moisture, etc. present in the light extraction layer 2 are removed. It is supposed to reduce in advance.

  In the method for manufacturing an organic light emitting device according to this embodiment, the light extraction layer 2, the barrier layer 3, and the transparent electrode 4 are sequentially laminated, and the counter electrode 6 that is a counter electrode of the organic layer 5 and the transparent electrode 4 is formed on the transparent electrode 4. And, in particular, a step of forming the light extraction layer 2 on the transparent substrate 1 by pattern coating in an atmospheric environment, and vacuum heating the formed light extraction layer 2 A step of performing the treatment, a step of continuously forming the barrier layer 3 on the light extraction layer while keeping the light extraction layer 2 subjected to the vacuum heat treatment in a reduced-pressure atmosphere, and a transparent layer on the formed barrier layer 3 Forming at least the electrode 4.

  FIG. 2 is a flowchart showing an example of the method for manufacturing the organic light emitting device according to this embodiment.

  2 includes a light extraction layer forming step S10, a vacuum heat treatment step S20, a barrier layer forming step S30, a transparent electrode forming step S40, an organic layer forming step S50, and a counter electrode. In this method, the forming step S60 and the sealing step S70 are sequentially included. Among these steps, the light extraction layer forming step S10 is a step performed under an atmospheric environment. On the other hand, at least the barrier layer forming step S30, the transparent electrode forming step S40, the organic layer forming step S50, and the counter electrode forming step S60 are steps performed under a reduced pressure atmosphere with high cleanliness. This manufacturing method is particularly characterized in that the vacuum heat treatment step S20 is performed after the light extraction layer forming step S10 and before these steps performed in a reduced pressure atmosphere.

  The light extraction layer forming step S10 is a step of forming the light extraction layer 2 on the transparent substrate 1 by pattern coating in the atmospheric environment. Specifically, the environment in which the light extraction layer forming step S10 is performed is an environment in which the gas phase composition and pressure are an atmospheric atmosphere, and dust is reduced and the cleanliness is high. Since the light extraction layer 2 is a layer mainly composed of a resin material, a large-area layer can be efficiently formed by a coating method performed in an atmospheric environment. In addition, since there is no need to reduce the atmosphere as in vacuum film formation, there is an advantage that power costs, equipment costs, etc. for vacuuming are not required.

  The light extraction layer 2 can be formed by applying a coating liquid containing a material for forming the layer onto the transparent substrate 1 by a known coating method. The applied coating film is dried and then subjected to a curing treatment as necessary. For example, the scattering layer 2a can be made into a coating solution by dispersing light scattering particles and a curable resin as a binder resin in a solvent and adding a polymerization initiator as appropriate. Moreover, about the smooth layer 2b, it can be set as a coating liquid by disperse | distributing curable resin as fine particle and binder resin to a solvent, and adding a polymerization initiator suitably.

  Examples of the coating method of the light extraction layer 2 include an inkjet method, a gravure coating method, a micro gravure coating method, a screen printing method, a flexographic printing method, a nozzle printing method, a dip coating method, an air knife coating method, a curtain coating method, and a roller. A coating method, a wire bar coating method, an extrusion coating method, or the like can be used. A preferable coating method is an ink jet method, a gravure coating method, a micro gravure coating method or a nozzle printing method suitable for pattern coating.

  As a method for the curing treatment, an appropriate method can be used according to the curability of the binder resin. For example, heat treatment or electron beam irradiation treatment can be used for the thermosetting resin, and ultraviolet irradiation treatment or the like can be used for the photocurable resin. For the electron beam irradiation treatment, various electron beam accelerators such as a Cockrowalton type, a bandegraph type, a resonant transformation type, an insulating core transformer type, a linear type, a dynamitron type, and a high frequency type can be used. For example, it is possible to use an electron beam having an energy of 10 to 1000 keV, preferably 30 to 300 keV. For the ultraviolet irradiation treatment, an excimer lamp, an ultrahigh pressure mercury lamp, a high pressure mercury lamp, a low pressure mercury lamp, a carbon arc, a xenon arc, a metal halide lamp, or the like can be used.

  The patterning of the light extraction layer 2 is such that a region where the light extraction layer 2 is not formed is left on the surface near the end of the transparent substrate 1. That is, the pattern of the light extraction layer 2 can be formed by applying the coating liquid of the light extraction layer 2 while limiting the coating width on the transparent substrate 1. As long as such a region in which the light extraction layer 2 is not formed is left, patterning in which a plurality of organic light emitting elements are formed in the width direction or the length direction of the transparent substrate 1 may be performed. Moreover, you may perform pattern application | coating using a mask according to the application | coating method.

  The vacuum heat treatment step S20 is a step of subjecting the light extraction layer 2 formed in the light extraction layer formation step S10 to vacuum heat treatment. By subjecting the light extraction layer 2 to a vacuum heat treatment, oxygen, moisture, etc. present in the light extraction layer 2, components of the coating solution used to form the light extraction layer 2, and these are cured. Components (outgas) such as reacted reactants can be removed by volatilization and diffusion, and the residual amount in the light extraction layer 2 can be reduced.

  The vacuum heat treatment can be performed by any one of radiation heating and conduction heating. Examples of radiant heating include infrared heating, microwave heating, and high-frequency dielectric heating. Moreover, as conductive heating, for example, heating by a hot plate, heating by a roll heater, or the like can be used. Among these, a preferable heating method is infrared heating, and a more preferable heating method is infrared heating using infrared light whose wavelength is controlled in the non-absorption wavelength region of the transparent substrate 1. In the case of infrared heating with such wavelength control, when a resin film is used as the transparent substrate 1, it is possible to avoid thermal deformation of the transparent substrate 1.

The vacuum heat treatment can promote the removal of outgas, moisture and the like, and the temperature condition and the heating can be used as long as the thermal deformation and the volatilization of the constituent materials do not occur excessively for the transparent substrate 1 and the light extraction layer 2. Time etc. can be set suitably. However, for example, when a resin film is used as the transparent substrate 1, the heating temperature is preferably in the range of 40 ° C. or more and 80 ° C. or less as the surface temperature of the light extraction layer 2. Note that the degree of vacuum of the atmosphere in the vacuum heat treatment is preferably about 1 × 10 ⁻⁶ Pa to 1 × 10 ⁻² Pa.

The barrier layer forming step S30 is a step of continuously forming the barrier layer 3 on the light extraction layer 2 subjected to the vacuum heat treatment in the vacuum heat treatment step S20. That is, the transparent substrate 1 on which the light extraction layer 2 is formed is subjected to the barrier layer forming step S30 while being held in a reduced-pressure atmosphere after the vacuum heat treatment, whereby the light extraction layer 2 or the transparent substrate 1 is carried out to the atmospheric environment or the like. The barrier layer is formed without doing so. The barrier layer 3 can be formed by performing vacuum film formation under a reduced pressure atmosphere. Specific examples of the method for forming the barrier layer 3 include chemical vapor deposition (CVD) methods such as plasma CVD, laser CVD, and thermal CVD, vacuum deposition methods, sputtering methods, ion plating methods, and the like. And physical vapor deposition (PVD) method. The barrier layer 3 may be patterned by film formation using a mask, etching, or the like. The degree of vacuum of the atmosphere in the barrier layer forming step S30 is preferably about 1 × 10 ⁻⁶ Pa to 1 × 10 ⁻² Pa.

  Transparent electrode formation process S40 is a process of forming the transparent electrode 4 on the barrier layer 3 formed in barrier layer formation process S30. After the electrode material is formed as a thin film using a method such as vapor deposition or sputtering, a pattern having a desired shape may be formed by a photolithography method. When pattern accuracy is not required (about 100 μm or more), the desired shape is formed. A pattern may be formed by forming a film by a method such as vapor deposition or sputtering through the mask. Moreover, when using the electrode substance which can be apply | coated like an organic electroconductivity compound, wet application methods, such as a printing system and a coating system, can also be used.

  The organic layer forming step S50 is a step of forming the organic layer 5 on the transparent electrode 4 formed in the transparent electrode forming step S40. As the organic layer 5, in addition to the light emitting layer, for example, a plurality of layers including a hole injection layer, a hole transport layer, an electron blocking layer, a hole blocking layer, an electron transport layer, an electron injection layer, and the like can be formed. . Specifically, it can be formed using a wet coating method, PVD, or the like depending on the material constituting each layer. Examples of the wet coating method include an inkjet method, a gravure coating method, a micro gravure coating method, a screen printing method, a flexographic printing method, a nozzle printing method, a dip coating method, a spray coating method, an air knife coating method, a curtain coating method, and a roller. A coating method, a wire bar coating method, an extrusion coating method, or the like can be used. As these forming methods, the same method may be used for each layer constituting the organic layer 5, or different methods may be used. Moreover, each layer which comprises the organic layer 5 may be patterned by the film-forming using a mask, pattern application | coating, etc., and may be patterned by wiping off after whole surface application | coating.

  The counter electrode forming step S60 is a step of forming the counter electrode 6 on the organic layer 5 formed in the organic layer forming step S50. The counter electrode 6 can be formed by depositing an electrode material using a PVD method or the like. The counter electrode 6 may be patterned by film formation using a mask, photolithography, or the like.

  The sealing step S <b> 70 is a step of sealing the formed transparent electrode 4, organic layer 5, and counter electrode 6. Sealing can be performed by bonding the sealing member 8 with an adhesive. The sealing member 8 is fixed between the non-formation region of the light extraction layer 2 remaining on the transparent substrate 1 and the surface of the counter electrode 6 opposite to the organic layer 5 with the adhesive. As a result, the sides of the light extraction layer 2, the barrier layer 3, the transparent electrode 4, the organic layer 5 and the counter electrode 6 are covered with an adhesive layer 7 made of an adhesive, and intrusion of oxygen, moisture, etc. in the outside air Is prevented. After the sealing step S70, the organic light emitting device 100 can be manufactured by subjecting it to subsequent steps such as instrumentation and heat treatment such as a drive circuit, a power source, and a protective material.

  In the manufacturing method of the organic light emitting element according to the above-described embodiment, the light extraction layer forming step S10 is suitable for forming a large area layer and is performed in an atmospheric environment that does not require decompression. In addition, there is a possibility that oxygen, moisture, etc. in the environment may enter. Moreover, since a solvent and binder resin are used for formation of the light extraction layer 2, in these light extraction layers 2, these solvent, binder resin, the reaction material which these reacted in the process of hardening, etc. May remain. In addition, since the light extraction layer forming step S10 is performed in a closed atmospheric environment in which the cleanliness is controlled, such components are once released into the environment as outgas, and then are again applied to the light extraction layer 2. There is a risk of intrusion again. However, by carrying out the vacuum heat treatment step S20, the residual amount of the solvent, binder resin, their reactants (outgas), oxygen, moisture, etc. existing in the light extraction layer 2 can be reduced. Can do. Therefore, it is possible to produce an organic light-emitting device that has good light emission efficiency and high side barrier properties while allowing the light extraction layer 2 to be patterned in an atmospheric environment.

  Further, in this manufacturing method, since the light extraction layer 2 is patterned, a step corresponding to the film thickness of the light extraction layer 2 is formed on the transparent substrate 1 immediately after the light extraction layer formation step S10. Yes. Therefore, the barrier layer 3 formed in the subsequent process is in a state where the film density is lowered in the vicinity of the step and there is a risk of causing cracks. In addition, since the light extraction layer forming step S10 is performed in an atmospheric environment, oxygen, moisture, or the like enters the light extraction layer 2 or outgas derived from the light extraction layer 2 is likely to remain in the light extraction layer 2. A large amount of outgas, oxygen, moisture, and the like are released when the barrier layer 3 is formed, so that pinholes are easily formed. However, since the vacuum heat treatment step S20 is performed, these components (outgas), oxygen, moisture, etc. present in the light extraction layer 2 can be volatilized and diffused to be removed. It is possible to produce an organic light-emitting device that is excellent in soundness of the barrier layer 3 and has high side-barrier properties and good weather resistance.

  Next, the manufacturing apparatus of the organic light emitting element according to this embodiment will be described.

  FIG. 3 is a diagram showing a schematic configuration of an example of an organic light emitting device manufacturing apparatus according to the present embodiment. (A) is a schematic configuration of the light extraction layer forming portion, (b) is a schematic configuration of the barrier layer forming portion, and (c) is a diagram illustrating a schematic configuration of the element forming portion.

  The organic light emitting device manufacturing apparatus 200 shown in FIG. 3 includes a light extraction layer forming unit 10, a barrier layer forming unit 20, and an element forming unit 30. In particular, the manufacturing apparatus 200 employs a roll-to-roll production method to continuously form the organic light-emitting element 100 on the long transparent belt-shaped transparent substrate 1. It is a device that makes it possible. In FIG. 3, the manufacturing apparatus 200 takes up the transparent substrate 1 in a roll shape and transfers it to a subsequent process in each of the light extraction layer forming unit 10, the barrier layer forming unit 20, and the element forming unit 30. However, the arrangement of the winder is arbitrary, and for example, the light extraction layer forming unit 10, the barrier layer forming unit 20, and the element forming unit 30 may be connected.

  In the manufacturing apparatus 200, the long transparent belt-shaped transparent substrate 1 is conveyed while being supported by a conveyance roller and a backup roller schematically shown in FIG. 3. Then, the light extraction layer forming step S10, the vacuum heat treatment step S20, the barrier layer forming step S30, the transparent electrode forming step S40, the organic layer forming step S50, the counter electrode forming step S60, and the sealing step S70, Then, the organic light emitting device 100 is formed on the transparent substrate 1. In FIG. 3, the intermediate process of the element forming unit 30 in which the organic layer forming process S50 and the counter electrode forming process S60 are performed, the sealing process S70, and the subsequent processes are omitted.

  The light extraction layer forming unit 10 has a device configuration for forming the light extraction layer 2 on the transparent substrate 1. Specifically, as shown in FIG. 3A, the light extraction layer forming unit 10 includes a feeding unit 11, a tension control unit 12, a first application unit 13A, a first primary drying unit 14A, First secondary drying unit 15A, first curing processing unit 16A, second coating unit 13B, second primary drying unit 14B, second secondary drying unit 15B, second curing processing unit 16B, It has an inspection unit 17 and a winding unit 18. The light extraction layer forming unit 10 is in an atmospheric environment, and the part from the feeding unit 11 to the winding unit 18 is in an atmosphere with a gas phase composition and pressure in an air atmosphere, and is highly clean with reduced dust. . The first application unit 13A, the first primary drying unit 14A, the first secondary drying unit 15A, and the first curing processing unit 16A are steps for forming the scattering layer 2a constituting the light extraction layer 2, and the second application The part 13B, the second primary drying part 14B, the second secondary drying part 15B, and the second curing processing part 16B are processes for forming the smoothing layer 2b constituting the light extraction layer 2.

  The feeding unit 11 has a function of unwinding and feeding the transparent substrate 1 wound in a roll shape. An original winding roll 111 of the transparent substrate 1 having a protective film bonded to the surface is attached to the feeding unit 11. Then, while the transparent substrate 1 is fed out while the protective film is peeled off, the protective film is wound around the winding roll 112 in a roll shape and collected.

  The tension control unit 12 has a function of controlling the tension in the transport direction and the like of the drawn transparent substrate 1. The tension control may be either speed control or torque control, and the tension load may be applied by any of control by a dancer roll, control by a feed roll, and the like. Further, the tension measuring means 121 may be provided for feedback control or the like. The transparent substrate 1 is transported to the first application unit 13 </ b> A after the transport speed is adjusted by the accumulator 110 and also subjected to EPC control (Edge Position Control) or CPC control (Center Position Control) by the position control unit 120.

  13 A of 1st application parts have the function to form the coating film of the scattering layer 2a on the transparent substrate 1 by pattern application | coating. The first application section 13A is provided with an application means 130 such as an ink jet application apparatus or a printing application apparatus capable of applying a pattern, and applies an application liquid on the transparent substrate 1 with a limited application width. The coating liquid used in the first coating part 13A is, for example, a dispersion in which at least light scattering particles and an ultraviolet curable resin are dispersed in a solvent, and a polymerization initiator is added as necessary.

  The first primary drying unit 14A has a function of primarily drying the coating film of the scattering layer 2a. The first application unit 13A is provided with a drying means 140 such as a hot air drying device, and the solvent is removed from the coating film of the scattering layer 2a by hot air drying or the like. The transparent substrate 1 is transported to the first secondary drying unit 15 </ b> A after the transport speed is adjusted by the accumulator 110.

  The first secondary drying unit 15A has a function of secondary drying the coating film of the scattering layer 2a. The first secondary drying unit 15A is provided with a heat treatment radiation source 150 such as an infrared heating device, and the coating film of the scattering layer 2a is dried to about the decreasing rate drying period by infrared heating or the like.

  The first curing processing unit 16A has a function of curing the coating film of the scattering layer 2a. The first curing processing unit 16A is provided with a curing treatment radiation source 160 that irradiates ultraviolet rays, and the scattering layer 2a is formed by curing the curable resin contained in the coating film of the scattering layer 2a by ultraviolet irradiation. It has come to be. The transport speed of the transparent substrate 1 is adjusted by the accumulator 110, and EPC control or CPC control is performed by the position control means 120, so that the transparent substrate 1 is transported to the second coating unit 13B.

  As the curing treatment radiation source 160, a rare gas excimer lamp that emits vacuum ultraviolet rays of 100 to 230 nm is suitable. As the rare gas, Xe, Kr, Ar, Ne, or the like can be used. As a method for generating excimer, a method using dielectric barrier discharge, a method using electrodeless electric field discharge, or the like can be used. The excimer lamp has an advantage that it can be lit with low power because of high generation efficiency of ultraviolet rays. In addition, since a sharp spectrum by a rare gas excimer can be obtained, generation of radiant heating can be suppressed.

  The 2nd application part 13B has a function which forms the application film of smooth layer 2b on transparent substrate 1 by pattern application. The coating liquid used in the second coating part 13B is, for example, one in which fine particles and an ultraviolet curable resin are dispersed in a solvent and a polymerization initiator is added as necessary. Other configurations of the second coating unit 13B, the second primary drying unit 14B, the second secondary drying unit 15B, and the second curing processing unit 16B are the first coating unit 13A, the first primary drying unit 14A, the first The configuration is the same as that of the secondary drying unit 15A and the first curing processing unit 16A. In the second curing processing unit 16B, the transparent substrate 1 on which the smooth layer 2b is formed is conveyed to the inspection unit 17, and the inspection unit 17 performs a failure inspection such as a coating defect on the transparent substrate 1.

  The winding unit 18 has a function of winding the transparent substrate 1 on which the light extraction layer 2 is formed in a roll shape. The winding unit 18 is provided with an original winding roll 181 of a protective film wound in a roll shape. As for the transparent substrate 1 conveyed, the protective film unwound from the original winding roll 181 is bonded to the surface side of the light extraction layer 2. Thereafter, the transparent substrate 1 to which the protective film is bonded is wound around the take-up roll 182 in a roll shape, collected, and transferred to the barrier layer forming unit 20 (see FIG. 3B).

The barrier layer forming unit 20 has a device configuration in which the light extraction layer 2 formed on the transparent substrate 1 is subjected to vacuum heat treatment, and the barrier layer 3 is formed on the light extraction layer 2 subjected to vacuum heat treatment. Yes. Specifically, as shown in FIG. 3B, the barrier layer forming unit 20 includes a feeding unit 21, a tension control unit 22, a film forming unit 23, and a winding unit 28. The barrier layer forming unit 20 is in a vacuum atmosphere, and the degree of vacuum is, for example, about 1 × 10 ⁻⁶ Pa or more and 1 × 10 ⁻² Pa or less from the feeding unit 21 to the winding unit 28. Is managed. The film forming unit 23 is a step of forming a barrier layer. In this manufacturing apparatus 200, a single-layer structure barrier layer is formed by the single unit film forming unit 23, but the number of units in the film forming unit is not limited to this.

  The feeding unit 21 has a function of unwinding and feeding out the transparent substrate 1 wound in a roll shape. An original winding roll 211 of the transparent substrate 1 in which a protective film is bonded onto the light extraction layer 2 is attached to the feeding portion 11. And while the transparent substrate 1 is drawn out while the protective film is peeled off, the protective film is wound around the take-up roll 212 in a roll shape and collected.

  The tension control unit 22 has a function of controlling the tension in the transport direction and the like of the drawn transparent substrate 1. The transparent substrate 1 is heated by the vacuum heating means 210 while the conveyance speed is adjusted by the accumulation conveyor 110. Then, the position is controlled by the position control means 120 and conveyed to the film forming unit 23. The tension control unit 22 can have the same configuration as the tension control unit 12.

  As the vacuum heating means 210, for example, a heat treatment source such as an infrared heating device is provided. The vacuum heating means 210 volatilizes outgas, oxygen, moisture, etc., which cannot be removed sufficiently only by heating the light extraction layer 2 formed on the transparent substrate 1 in a vacuum atmosphere and reducing the pressure. Evaporate and remove to reduce these residual amounts. Note that the number, shape, and arrangement of the heat treatment radiation source are not particularly limited, and a reflective material may be used in combination with the heat treatment radiation source. Further, the vacuum heating means 210 may be a heating device that conducts conduction heating.

  The vacuum heating means 210 is preferably a wavelength controlled infrared heating device. The wavelength-controlled infrared heating device can be configured to include, for example, a filament, a protective tube, and a filter. By accommodating a filament serving as an infrared source in a protective tube and covering the periphery of the protective tube with a filter, infrared (for example, a wavelength of 3.5 μm or more) that is an absorption region of the transparent substrate 1 can be absorbed by the filter. The filament may be covered with a single filter, or a plurality of filters may be overlaid. Further, a coolant such as cooling air may be passed between the protective tube and the filter or between the filters. By cooling the filter with the refrigerant, infrared radiation by the filter itself can be suppressed. Examples of the material of the filter of the wavelength control infrared heating device include quartz glass and borosilicate glass. Of these, quartz glass is preferred from the viewpoint of heat resistance and thermal shock resistance.

  The film forming unit 23 has a function of forming the barrier layer 3 on the light extraction layer 2 subjected to the vacuum heat treatment. The film forming unit 23 includes a pair of roll electrodes 230 arranged with a space therebetween, a gas supply unit 231, and a gas exhaust unit 233 connected to a vacuum pump 232. Each of the pair of roll electrodes 230 is connected to a plasma generation power source (not shown) via an electric wire so that a voltage such as a high-frequency AC voltage is applied. The gas supply unit 231 supplies a source gas for forming the barrier layer 3 to the space between the pair of roll electrodes 230. As the source gas, an inert gas containing an inorganic compound or a precursor of an organic compound that forms the barrier layer 3 is used.

  The supplied source gas is exhausted through a gas exhaust unit 233 that is set to a negative pressure by a vacuum pump 232. During this time, the source gas generates plasma by applying a voltage to the pair of roll electrodes 230, and forms a barrier layer on the light extraction layer 2 of the transparent substrate 1 that is conveyed while being supported by the roll electrodes 230. When the film forming unit 23 is configured by a plurality of units, the composition, supply amount, and the like of the source gas in each unit, the applied voltage, the frequency, and the like may be the same or different. The transport speed of the transparent substrate 1 is adjusted by the accumulator 110, and EPC control or CPC control is performed by the position control means 120, so that the transparent substrate 1 is transported to the winding unit 28.

  The winding unit 28 has a function of winding the transparent substrate 1 on which the barrier layer 3 is formed in a roll shape. The winding portion 28 is provided with an original winding roll 281 of a protective film wound in a roll shape. As for the transparent substrate 1 conveyed, the protective film unwound from the original winding roll 281 is bonded to the surface side of the barrier layer 3. Thereafter, the transparent substrate 1 to which the protective film is bonded is wound around the take-up roll 282 in a roll shape, collected, and transferred to the element forming unit 30 (see FIG. 3C).

The element forming unit 30 has a device configuration for forming the transparent electrode 4, the organic layer 5, and the counter electrode 6 on the barrier layer 3. Specifically, as shown in FIG. 3 (c), the element shaper 30 includes a feeding part 31, a tension controller 32, a transparent electrode forming part 33, an organic layer forming part and a counter electrode (not shown). It has a forming part, a winding part 38 and the like. In addition, in FIG.3 (c), illustration of an organic layer formation part, a counter electrode formation part, etc. is abbreviate | omitted. The element shape portion 30 is in a reduced pressure atmosphere, and the degree of vacuum is about 1 × 10 ⁻⁶ Pa or more and 1 × 10 ⁻² Pa or less, for example, from the feeding portion 31 to the winding portion 38. Is managed.

  The feeding unit 31 has a function of unwinding and feeding the transparent substrate 1 wound in a roll shape. An original winding roll 311 of the transparent substrate 1 having a protective film bonded on the barrier layer 3 is attached to the feeding portion 31. Then, while the transparent substrate 1 is fed out while the protective film is peeled off, the protective film is wound around the winding roll 312 and collected.

  The tension control unit 32 has a function of controlling the tension in the transport direction and the like of the drawn transparent substrate 1. The transport speed of the transparent substrate 1 is adjusted by the accumulator 110, the position of the transparent substrate 1 is controlled by the position controller 120, and the transparent substrate 1 is transported to the transparent electrode forming unit 33. The tension control unit 32 can have the same configuration as the tension control unit 12.

  The transparent electrode forming part 33 has a function of forming the transparent electrode 4 on the barrier layer 3. The transparent electrode forming part 33 in FIG. 3 is configured to form a transparent electrode by a vacuum vapor deposition method. The transparent electrode forming unit 33 includes a vapor deposition roll 330 that supports the transparent substrate 1 to be vapor-deposited, and a vapor deposition source 331. On the transparent substrate 1 conveyed while being supported by the vapor deposition roll 330, the transparent electrode 4 is formed by vapor deposition of the electrode material vaporized from the vapor deposition source 331. Subsequently, the transparent substrate 1 on which the transparent electrode 4 is formed is transported to an organic layer forming unit (not shown) to form an organic layer 5, and then transported to a counter electrode forming unit (not illustrated) to connect the counter electrode 6. It is formed. The organic layer forming unit is configured by combining one or a plurality of wet coating apparatuses, vacuum film forming apparatuses, and the like suitable for forming each layer according to the desired layer configuration of the organic layer 5.

  The winding unit 38 has a function of winding the transparent substrate 1 on which the transparent electrode 4, the organic layer 5, and the counter electrode 6 are formed in a roll shape. The transparent substrate 1 is wound up and collected in a roll shape by a take-up roll 382, and is subjected to a subsequent process such as a sealing process, whereby the organic light emitting device 100 is manufactured. Although the post-process such as the sealing process is a separate process here, it may be a continuous process.

  According to the organic light emitting device manufacturing apparatus 200 having the above-described configuration, the barrier layer forming unit 20 in a vacuum atmosphere is provided immediately after the light extraction layer forming unit 10 in the atmospheric environment. The transparent substrate 1 on which the light extraction layer 2 is formed is kept in a reduced-pressure atmosphere after the step of performing the vacuum heat treatment until the step of forming the barrier layer is completed. A vacuum heating unit 210 is provided immediately before the film forming unit 23 for forming the barrier layer. Therefore, the remaining amount of outgas, oxygen, moisture, etc. is reduced by vacuum heat treatment in a state where the outgas, oxygen, moisture, etc. in the atmosphere is difficult to enter the formed light extraction layer 2. Is done. Therefore, it is possible to manufacture an organic light-emitting element that is less deteriorated due to outgas, oxygen, moisture, and the like and that has good light emission efficiency.

  Next, the detail of each element which comprises an organic light emitting element is demonstrated.

[Transparent substrate]
As the transparent substrate 1, a plate-like body or a film-like body having appropriate light transmittance such as a resin plate, a resin film, a glass plate, or the like can be used. The light transmittance of the transparent substrate 1 is such that the transmittance is 70% or more, preferably 80% or more, more preferably 90% or more, and further preferably 95% or more. Particularly preferred as the transparent substrate 1 is a resin film having flexibility. The thickness of the resin film is preferably 10 to 500 μm, more preferably 20 to 250 μm, and still more preferably 30 to 150 μm. When the thickness of the resin film is in the range of 10 to 500 μm, it is easy to ensure the gas barrier property on the substrate side, and it can be suitably used for production of a roll-to-roll system.

  Examples of the resin film include acrylic acid ester, methacrylic acid ester, polyethylene terephthalate (PET), polybutylene terephthalate, polyethylene naphthalate (PEN), polycarbonate (PC), polyarylate, polyvinyl chloride (PVC), polyethylene (PE ), Polypropylene (PP), polystyrene (PS), nylon (Ny), aromatic polyamide, polyetheretherketone, polysulfone, polyethersulfone, polyimide, polyetherimide, and the like can be used. Such a resin film may be uniaxially stretched, biaxially stretched, annealed, or the like. Moreover, it may have a multilayer structure, and a barrier layer having gas barrier properties may be laminated.

[Light extraction layer]
The light transmittance of the light extraction layer 2 is preferably 50% or more, more preferably 55% or more, and further preferably 60% or more. The refractive index of the light extraction layer 2 can be set according to the use of the organic light emitting device 100. For example, the refractive index at a wavelength of 550 nm may be in a range of 1.7 or more and less than 2.5. preferable. The haze value is preferably 30% or more and less than 90%, more preferably 35% or more and less than 85%, still more preferably 40% or more and less than 80%, and particularly preferably 45% or more and less than 75%.

[Scattering layer]
The scattering layer 2a can be formed of a single material having light scattering properties, or light scattering particles and a binder resin. The refractive index of the scattering layer 2a is preferably in the range of 1.7 or more and less than 3.0.

As the light scattering particles, any of inorganic compound particles, organic compound particles, and composite particles thereof may be used. As the inorganic compound particles, for example, ZrO ₂ , TiO ₂ , BaTiO ₃ , In ₂ O ₃ , ZnO, Sb ₂ O ₃ , ITO, CeO ₂ , Nb ₂ O ₅ , WO _{3 and the} like can be used. Also, as organic compound particles, for example, polymethyl methacrylate beads, acrylic-styrene copolymer beads, melamine beads, polycarbonate beads, styrene beads, crosslinked polystyrene beads, polyvinyl chloride beads, benzoguanamine-melamine formaldehyde beads, etc. Can do.

  The average particle diameter of the light scattering particles is preferably in the range of 0.2 μm or more and less than 1 μm. If the average particle diameter is 0.2 μm or more, visible light can be scattered well. Moreover, if the average particle diameter is less than 1 μm, the scattering layer 2a can be formed smooth and thin, so that the film thickness of the light extraction layer 2 can be suppressed.

  The refractive index of the light scattering particles is 1.7 or more, preferably 1.85 or more, more preferably 2.0 or more. Further, the difference in refractive index between the light scattering particles and the binder resin is 0.03 or more, preferably 0.1 or more, more preferably 0.2 or more, and further preferably 0.3 or more. When the light scattering particles have such a refractive index, the scattered light intensity can be easily increased, so that the light extraction efficiency is improved satisfactorily.

  The light scattering particles preferably have a filling rate of 1% by volume or more and 70% by volume or less per scattering layer 2a, and more preferably a filling rate of 5% by volume or more and 50% by volume or less. Further, the in-plane occupation ratio per fluoroscopic plane with respect to the main surface of the scattering layer 2a is preferably 30% or more, more preferably 50% or more, and further preferably 70% or more.

  As binder resin which comprises the scattering layer 2a, curable resins, such as a thermosetting resin which has a light transmittance, a photocurable resin, blend resin by the combination of these and a thermoplastic resin, etc. can be used. Specifically, as the curable resin, for example, a silicone resin, an epoxy resin, a vinyl ester resin, an acrylic resin, an allyl ester resin, a polyimide resin, or the like can be used. Specific examples of the thermoplastic resin include a polyvinyl chloride resin, a polyvinylidene chloride resin, a polyvinyl acetate resin, a polymethacrylate resin, a polyacrylate resin, a polystyrene resin, a polyamide resin, and a polyethylene resin. Polypropylene resin, fluorine resin, polyurethane resin, polyacrylonitrile resin, polyvinyl ether resin, polyvinyl ketone resin, polyether resin, polyvinyl pyrrolidone resin, saturated polyester resin, polycarbonate resin, chlorinated polyether resin, etc. can be used. . Among these, the binder resin is preferably a polymer having a saturated hydrocarbon or a polyether as a main chain, and more preferably a polymer having a saturated hydrocarbon as a main chain. The binder is preferably crosslinked. The polymer having a saturated hydrocarbon as the main chain is preferably obtained by a polymerization reaction of an ethylenically unsaturated monomer. In order to obtain a crosslinked binder, it is preferable to use a monomer having two or more ethylenically unsaturated groups.

  As a solvent for the coating solution, an appropriate solvent can be used depending on the material. For example, water, alcohols such as methanol, ethanol, 1-propanol, 2-propanol, 1-butanol and 2-butanol, and multivalents such as ethylene glycol, diethylene glycol, triethylene glycol, propanediol, butanediol and glycerin Alcohols, esters such as methyl acetate, ethyl acetate, butyl acetate, isopropyl acetate, diethyl ether, tetrahydrofuran, dioxane, ethylene glycol monomethyl ether, ethylene glycol dimethyl ether, diethylene glycol monomethyl ether, diethylene glycol dimethyl ether, triethylene glycol monomethyl ether, Ethers such as triethylene glycol dimethyl ether, hexane, heptane, decane, cyclohexane Hydrocarbons such as toluene, xylene, halogenated hydrocarbons such as dichloromethane, trichloroethane, chlorobenzene, amides such as dimethylformamide, N-methylpyrrolidone, acetone, methyl ethyl ketone, acetylacetone, cyclohexanone, isophorone, etc. An appropriate solvent such as ketones, DMF, DMSO, N-methylpyrrolidone, γ-butyrolactone, acetonitrile or the like can be used. The solvent may be a composition composed of a single species or a composition in which a plurality of species are mixed.

[Smooth layer]
The smooth layer 2b can be formed of a single material or fine particles and a binder resin. The refractive index of the smooth layer 2b is preferably in the range of 1.7 or more and less than 2.5. The smooth layer 2b has an average surface roughness Ra of the surface on the transparent electrode 4 side of less than 100 nm, preferably less than 30 nm, more preferably less than 10 nm, and even more preferably less than 5 nm. In addition, average surface roughness Ra is arithmetic average roughness based on JISB0601: 2001.

  The particle diameter of the fine particles is preferably 5 nm or more, more preferably 10 nm or more, and further preferably 15 nm or more. When the particle diameter of the fine particles is within such a range, aggregation of the fine particles can be suppressed, and light transmittance of the smooth layer 2b can be easily ensured. On the other hand, the particle diameter of the fine particles is preferably 70 nm or less, more preferably 60 nm or less, and further preferably 15 nm or less. When the particle diameter of the fine particles is within such a range, the smoothness due to the smooth layer 2b is hardly impaired.

As the fine particles, for example, particles of the same material as the light scattering particles can be used, and TiO ₂ is particularly preferable. As the TiO _2, the rutile type is more preferable. If rutile type titanium dioxide is used, the catalytic activity is low compared to the anatase type, so that it is easy to ensure the weather resistance, and the smooth layer 2b can have a high refractive index.

  The binder resin constituting the smooth layer 2b can be selected from the same resins as the scattering layer 2a.

[Barrier layer]
The barrier layer 3 is a layer having a high gas barrier property, and is provided between the light extraction layer 2 and the transparent electrode 4. The barrier layer 3 is formed using, for example, an inorganic compound such as silicon oxide, aluminum oxide, or magnesium oxide, or an organic compound such as silane, alkoxysilane, halogenated silane, organosiloxane, silazane, organopolysiloxane, or organopolysilazane as a precursor. can do. The barrier layer 3 may have a single layer configuration of any one of such inorganic compounds and organic compounds, or may have a multi-layer configuration having a laminated structure. The barrier layer 3 can prevent outgas, oxygen, moisture, etc. present in the atmosphere from permeating and diffusing from the light extraction layer 2 side to the transparent electrode 4 side and entering the organic layer 5 and the like. The gas barrier property means that the water vapor permeability (60 ± 0.5 ° C., relative humidity (90 ± 2)% RH) measured by a method according to JIS K 7129-1992 is 1 × 10 ⁻³ g / (M ² · 24h) or less, and the oxygen permeability measured by a method according to JIS K 7126-1987 is 1 × 10 ^-3 ml / m ² · 24h · atm or less.

[Transparent electrode]
The transparent electrode 4 can be formed of a light-transmitting anode material generally used for organic light-emitting elements. Examples of the anode material include metals, alloys, electrically conductive compounds, mixtures thereof, and the like having a large work function (4 eV or more). Specifically, for example, a conductive transparent material such as a metal such as Au, CuI, indium tin oxide (ITO), SnO ₂ , or ZnO can be used. Alternatively, an amorphous material such as IDIXO (In ₂ O ₃ —ZnO) that can form a transparent conductive film can be used.

  The film thickness of the transparent electrode 4 can be set appropriately according to the material, but is 10 to 1000 nm, preferably 10 to 200 nm. The sheet resistance of the transparent electrode 4 is preferably several hundred Ω / □ or less.

[Counter electrode]
The counter electrode 6 can be formed of a cathode material generally used for an organic light emitting device. Examples of the cathode material include an electrode using a metal, an alloy, an electrically conductive compound, or a mixture thereof having a low work function (4 eV or less) as an electrode material. Specifically, for example, sodium, sodium-potassium alloy, magnesium, lithium, magnesium / copper mixture, magnesium / silver mixture, magnesium / aluminum mixture, magnesium / indium mixture, aluminum / aluminum oxide (Al ₂ O ₃ ) mixture, Examples include indium, lithium / aluminum mixture, aluminum, silver, silver-based alloy, aluminum / silver mixture, and rare earth metal.

  The thickness of the counter electrode 6 can be appropriately determined according to the material, but is in the range of 10 nm to 5 μm, preferably 50 to 200 nm. The sheet resistance of the counter electrode 6 is preferably several hundred Ω / □ or less.

[Organic layer]
The organic layer 5 can have an appropriate layer configuration adopted in a general organic light emitting device. Specifically, the following configuration can be exemplified.
(1) Hole transport layer / light emitting layer / electron transport layer (2) Hole transport layer / light emitting layer / electron transport layer (3) Hole transport layer / electron blocking layer / light emitting layer / hole blocking layer / electron transport Layer (4) hole injection layer / hole transport layer / light emitting layer / electron transport layer / electron injection layer (5) hole injection layer / first hole transport layer / second hole transport layer / light emitting layer / first 1 electron transport layer / second electron transport layer / electron injection layer (6) hole injection layer / hole transport layer / light emitting layer / hole blocking layer / electron transport layer / electron injection layer (7) hole injection layer / Hole transport layer / electron blocking layer / light emitting layer / hole blocking layer / electron transport layer / electron injection layer

≪Luminescent layer≫
The light emitting layer is a layer that emits light by recombination of electrons and holes injected from the electrode. The light emitting layer contains an organic light emitting material that emits light. The organic light emitting material preferably contains a host compound and a dopant compound. Note that the light emitting portion may be in the light emitting layer or at the interface between the light emitting layer and the adjacent layer.

  Each light emitting layer may contain a plurality of host compounds and dopant compounds. By using a plurality of types of host compounds, the movement of charges can be adjusted, and the efficiency of the organic light-emitting element can be increased.

  As the dopant compound, a phosphorescent dopant compound or a fluorescent dopant compound can be used. Further, the dopant compound may be contained at a uniform concentration with respect to the film thickness direction of the light emitting layer, or may have a concentration distribution.

<Phosphorescent dopant compound>
A phosphorescent dopant compound is a compound in which light emission from an excited triplet is observed. Specifically, it is a compound that emits phosphorescence at room temperature (25 ° C.), and is defined as a compound having a phosphorescence quantum yield of 0.01 or more at 25 ° C. As the phosphorescent dopant compound, a known compound used for a light emitting layer of a general organic light emitting device can be used. The phosphorescent quantum yield of the phosphorescent dopant compound is preferably 0.1 or more.

<Fluorescent luminescent dopant compound>
As the fluorescent light emitting dopant compound, a known compound used for a light emitting layer of a general organic light emitting device can be used. Specifically, for example, coumarin dyes, pyran dyes, cyanine dyes, croconium dyes, squalium dyes, oxobenzanthracene dyes, fluorescein dyes, rhodamine dyes, pyrylium dyes, perylene dyes, stilbene dyes. System dyes, polythiophene dyes, rare earth complex phosphors, and the like.

  The thickness of the light emitting layer is preferably 5 nm to 200 nm, more preferably 10 nm to 100 nm. When the thickness of the light emitting layer is in such a range, the uniformity of the formed light emitting layer is easily ensured, and the possibility that the driving voltage becomes excessively high is reduced.

<Host compound>
The host compound is a compound mainly responsible for charge transport in the light emitting layer. As a host compound, the compound whose phosphorescence quantum yield of phosphorescence emission in room temperature (25 degreeC) is less than 0.1 is preferable, and the compound less than 0.01 is more preferable. Moreover, it is preferable that the mass ratio in the layer is 20% or more among the compounds contained in a light emitting layer as a host compound.

  As a host compound, the well-known compound used for the light emitting layer of a general organic light emitting element can be used. Specifically, for example, compounds having a basic skeleton such as carbazole derivatives, triarylamine derivatives, aromatic derivatives, nitrogen-containing heterocyclic compounds, thiophene derivatives, furan derivatives, oligoarylene compounds, carboline derivatives, diazacarbazole Derivatives (wherein at least one carbon atom of the hydrocarbon ring constituting the carboline ring of the carboline derivative is substituted with a nitrogen atom), and the like. The host compound may be a low molecular compound, a high molecular compound having a repeating unit, or a compound having a reactive group such as a vinyl group or an epoxy group. As the host compound, a compound having a hole transporting ability or an electron transporting ability, preventing emission light from being long-wavelength, and having a high glass transition temperature (Tg) is preferable. The Tg of the host compound is preferably 90 ° C. or higher, more preferably 120 ° C. or higher. In addition, Tg is a value calculated | required by the method based on JIS-K-7121 using DSC (Differential Scanning Colorimetry: Differential scanning calorimetry).

≪Hole transport layer≫
The hole transport layer is a layer having a function of transporting injected holes to the light emitting layer side.

  Examples of materials applicable to the hole transport layer include porphyrin derivatives, phthalocyanine derivatives, oxazole derivatives, oxadiazole derivatives, triazole derivatives, imidazole derivatives, pyrazoline derivatives, pyrazolone derivatives, phenylenediamine derivatives, hydrazone derivatives, stilbene derivatives, Polyarylalkane derivatives, triarylamine derivatives, carbazole derivatives, indolocarbazole derivatives, isoindole derivatives, acene derivatives such as anthracene and naphthalene, fluorene derivatives, fluorenone derivatives, polyvinylcarbazole, aromatic amines in the main chain or side chain Introduced polymer material or oligomer, polysilane, conductive polymer or oligomer (for example, PEDOT: PSS, aniline copolymer, polyaniline) Polythiophene, etc.) and the like.

  The thickness of the hole transport layer is not particularly limited, but is usually 5 nm to 5 μm, preferably 2 nm to 500 nm, more preferably 5 nm to 200 nm.

≪Electron transport layer≫
The electron transport layer is a layer having a function of transporting injected electrons to the light emitting layer side. The electron transport layer may be a single layer or a plurality of layers.

  Examples of materials applicable to the electron transport layer include nitrogen-containing aromatic heterocyclic derivatives, aromatic hydrocarbon ring derivatives, dibenzofuran derivatives, dibenzothiophene derivatives, silole derivatives, and the like. Examples of the nitrogen-containing aromatic heterocyclic derivative include carbazole derivatives, azacarbazole derivatives (one or more carbon atoms constituting the carbazole ring are substituted with nitrogen atoms), pyridine derivatives, pyrimidine derivatives, pyrazine derivatives, pyridazine derivatives, triazines. Derivatives, quinoline derivatives, quinoxaline derivatives, phenanthroline derivatives, azatriphenylene derivatives, oxazole derivatives, thiazole derivatives, oxadiazole derivatives, thiadiazole derivatives, triazole derivatives, benzimidazole derivatives, benzoxazole derivatives, benzthiazole derivatives, and the like. Examples of the aromatic hydrocarbon ring derivative include naphthalene derivatives, anthracene derivatives, and triphenylene derivatives.

The film thickness of the electron transport layer is not particularly limited, but is 2 nm to 5 μm, preferably 2 nm to 500 nm, and more preferably 5 nm to 200 nm. Further, the electron mobility of the electron transport layer is preferably 10 ⁻⁵ cm ² / Vs or more.

≪Hole injection layer≫
The hole injection layer is a layer provided between the anode and the light emitting layer in order to lower the driving voltage and improve the light emission luminance. The hole injection layer can be interposed, for example, between the anode and the light emitting layer or between the anode and the hole transport layer. For the hole injection layer, see “Organic EL devices and their forefront of industrialization” (November 30, 1998, issued by NTT), Chapter 2, Chapter 2, “Electrode materials” (pages 123-166). It is described in detail.

≪Electron injection layer≫
The electron injection layer is a layer provided between the cathode and the light emitting layer in order to lower the driving voltage and improve the light emission luminance. The electron injection layer can be interposed, for example, between the cathode and the light emitting layer, or between the cathode and the electron transport layer. The details of the electron injection layer are described in Volume 2, Chapter 2, “Electrode Materials” (pages 123-166) of “Organic EL devices and their industrialization front line (issued by NTT Corporation on November 30, 1998)”. It is described in.

  The thickness of the electron injection layer is not particularly limited, but is preferably 0.1 nm to 5 μm.

≪Hole blocking layer≫
The hole blocking layer has a function of an electron transport layer in a broad sense, and has a function of transporting electrons while having a very small ability to transport holes. By blocking holes while transporting electrons, the recombination probability of electrons and holes can be improved.

  Examples of the hole blocking material applicable to the hole blocking layer include compounds listed as materials applicable to the electron transport layer, compounds listed as host compounds, and the like.

  The thickness of the hole blocking layer is preferably 3 nm to 100 nm, more preferably 5 nm to 30 nm.

≪Electron blocking layer≫
The electron blocking layer has a function of a hole transport layer in a broad sense, and has a function of transporting holes while having a remarkably small ability to transport electrons. By blocking electrons while transporting holes, the probability of recombination of electrons and holes can be improved.

  As an electron blocking material applicable to the electron blocking layer, for example, the same species as the hole transporting material can be used. Examples thereof include compounds similar to materials applicable to the hole transport layer and compounds similar to host compounds.

  The thickness of the electron blocking layer is preferably 3 nm to 100 nm, more preferably 5 nm to 30 nm.

[Sealing member]
The sealing member 8 seals the organic light emitting element through an adhesive layer 7 made of an adhesive. The sealing member 8 should just be arrange | positioned so that the display area | region of an organic light emitting element may be covered, and may be concave plate shape or flat plate shape. The transparency and electrical insulation of the sealing member 8 are not particularly limited.

  Examples of the sealing member 8 include a glass plate, a polymer plate, a polymer film, a metal plate, and a metal film. Specific examples of the glass plate include soda-lime glass, barium / strontium-containing glass, lead glass, aluminosilicate glass, borosilicate glass, barium borosilicate glass, and quartz. Specific examples of the polymer plate and polymer film include polycarbonate, acrylic, polyethylene terephthalate, polyether sulfide, and polysulfone. Specifically, as the metal plate and metal film, one or more metals selected from the group consisting of stainless steel, iron, copper, aluminum, magnesium, nickel, zinc, chromium, titanium, molybdenum, silicon, germanium, and tantalum, or these The thing which consists of these alloys is mentioned. In order to process the sealing member into a concave shape, sandblasting, chemical etching, or the like can be used. Particularly preferred as the sealing member 8 is a resin film having flexibility. As a resin film, it can select from the thing similar to the said transparent substrate 1, and can be used. Moreover, it may have a multilayer structure, and a barrier layer having gas barrier properties may be laminated.

  As an adhesive for adhering the sealing member, a photo-curing or thermosetting adhesive having a reactive vinyl group such as an acrylic acid oligomer or a methacrylic acid oligomer, or a moisture curing type such as 2-cyanoacrylate Adhesives, epoxy-based thermosetting or chemical-curing (two-component mixed) adhesives, hot-melt polyamide-based, polyester-based, polyolefin-based adhesives, and cationic-curing UV-curable epoxy A resin adhesive is mentioned.

  The adhesive is preferably one that can be adhesively cured from room temperature to 80 ° C. The adhesive may be applied using a commercially available dispenser or screen printing.

≪Usage≫
The organic light emitting device according to the present invention as described above can be used as a display device, a display, and various light emission sources. Examples of light emission sources include home lighting, interior lighting, clock and liquid crystal backlights, billboard advertisements, traffic lights, light sources of optical storage media, light sources of electrophotographic copying machines, light sources of optical communication processors, light sensors Examples include a light source. The organic light emitting element may have a resonator structure or may be used by causing laser oscillation.

  EXAMPLES Hereinafter, the present invention will be described more specifically with reference to examples of the present invention, but the present invention is not limited thereto.

<Manufacture of organic light emitting devices>
Examples of the present invention include a light extraction layer forming step S10, a vacuum heat treatment step S20, a barrier layer forming step S30, a transparent electrode forming step S40, an organic layer forming step S50, a counter electrode forming step S60, Through the sealing step S70, the light extraction layer 2, the barrier layer 3, and the transparent electrode 4 are sequentially stacked, and the organic layer 5 and the counter electrode 6 that is a counter electrode of the transparent electrode 4 are disposed on the transparent electrode 4. A sample of an organic light emitting device was manufactured. And the luminous efficiency was evaluated about the sample of the organic light emitting element.

[Example 1]
The organic light emitting device according to Example 1 was manufactured by subjecting a light extraction layer formed by pattern coating in an atmospheric environment to vacuum heat treatment. The light extraction layer 2 has a two-layer structure including a scattering layer 2a and a smooth layer 2b.

  The coating solution for the smooth layer 2b is composed of a titanium oxide dispersion in which titanium oxide is dispersed in toluene, a curable resin solution in which a curable resin is dissolved in toluene, and a polymerization initiator solution, each having a solid content ratio of 44 parts by mass. , 55 parts by mass and 1 part by mass. As the titanium oxide dispersion, a highly transparent titanium oxide slurry “HTD-760T” (manufactured by Teika Co., Ltd., average particle diameter of 15 nm, 40% toluene) was used. As the curable resin solution, a fluorene derivative “OGSOL EA-0200” (manufactured by Osaka Gas Chemical Co., Ltd.) was used. As the polymerization initiator, an oil-soluble azo polymerization initiator “V-65” (manufactured by Wako Pure Chemical Industries, Ltd.) was used.

  The coating solution for the scattering layer 2a is composed of a titanium oxide dispersion in which titanium oxide is dispersed in toluene, a curable resin solution in which a curable resin is dissolved in toluene, and a polymerization initiator solution, each having a solid content ratio of 44 parts by mass. The light scattering particles were mixed and dispersed so that the solid content ratio was 40 parts by mass and 60 parts by mass, respectively. In addition, the same thing as the coating liquid of the smooth layer 2b was used for the titanium oxide dispersion liquid, the curable resin solution, and the polymerization initiator. Further, as the light scattering particles, particles “Optobead 2000M” (manufactured by Nissan Chemical Industries, Ltd., average particle size 2.0 μm) made of melamine resin and silica were used.

  First, the transparent substrate 1 was ultrasonically cleaned in a neutral detergent solution, and then ultrasonically cleaned in pure water, and the cleaned transparent substrate 1 was heated and dried at 120 ° C. for 120 minutes. As the transparent substrate 1, a non-alkali glass substrate “Eagle XG” (manufactured by Corning) having a thickness of 0.7 mm and a refractive index (nD) of 1.51 was used.

  Subsequently, a coating liquid for the scattering layer 2a was applied onto the transparent substrate 1 by patterning using an ink jet method, and was thermally cured by heat treatment to form a scattering layer 2a having an average film thickness of 25 μm. Next, the smoothing layer 2b having a mean film thickness of 10 μm was formed on the scattering layer 2a formed by applying a coating solution of the smoothing layer 2b by patterning using an ink-jet method and heat-treating it by heat treatment.

The formed light extraction layer 2 was subjected to a vacuum heat treatment. The vacuum heat treatment was performed by an infrared heating apparatus using an infrared heating source (halogen lamp) in a reduced pressure atmosphere with a degree of vacuum of 1.0 × 10 ⁻⁵ Pa. The heat treatment time was 30 minutes, and the heating temperature was set so that the substrate temperature was 80 ° C. Subsequently, a barrier layer 3 having an average film thickness of 300 nm using SiN as a precursor was formed on the entire surface of the formed smooth layer 2b and the non-coated region of the transparent substrate 1 by a capacitively coupled plasma CVD apparatus.

  Next, a transparent electrode 4 made of ITO and having a thickness of 100 nm was formed on the barrier layer 3 by sputtering. As the organic layer 5, seven layers of a hole injection layer, a first hole transport layer, a second hole transport layer, a light emitting layer, a first electron transport layer, a second electron transport layer, and an electron injection layer are as follows. Formed.

  First, 99.7 parts by mass of 4,4 ′, 4 ″ -tris (N, N- (2-naphthyl) -phenylamino) triphenylamine (2-TNATA) was formed on the transparent electrode 4 by vacuum deposition. And 0.3 part by mass of F4-TCNQ were co-evaporated to form a hole injection layer having a thickness of 150 nm. Next, α-NPD was deposited on the hole injection layer by a vacuum deposition method to form a first hole transport layer having a thickness of 7 nm. Then, a hole transport material represented by the following chemical formula was deposited on the first hole transport layer by a vacuum deposition method to form a second hole transport layer having a thickness of 3 nm.

  Subsequently, 60 parts by mass of the following host material and 40 parts by mass of the phosphorescent light-emitting material represented by the following chemical formula are co-evaporated on the second hole transport layer by a vacuum deposition method, thereby emitting light having a thickness of 30 nm. A layer was formed.

  Subsequently, BAlq (bis (2-methyl-8-quinolinolate) -4- (phenylphenolate) aluminum) is vapor-deposited on the light emitting layer by a vacuum vapor deposition method, and the first electron transport layer having a film thickness of 39 nm is formed. Formed. Next, BCP (2,9-dimethyl-4,7-diphenyl-1,10-phenanthroline) is vapor-deposited on the first electron transport layer by a vacuum deposition method, and the second electron transport layer having a film thickness of 1 nm. Formed. And LiF was vapor-deposited on the 2nd electron carrying layer with the vacuum evaporation method, and the electron injection layer with a film thickness of 1 nm was formed.

  Next, Al was vapor-deposited on the electron injection layer by vacuum vapor deposition to form a counter electrode 6 having a thickness of 100 nm. And the sealing member was bonded and sealed on the side in which the counter electrode 6 of the transparent substrate 1 was formed, and it was set as the organic light emitting element which concerns on an Example.

[Comparative Example 1]
The organic light emitting device according to Comparative Example 1 was manufactured in the same manner as Example 1 except that the manufacturing process was not performed by vacuum heat treatment.

[Comparative Example 2]
The organic light emitting device according to Comparative Example 2 was manufactured in the same manner as in Example 1 except that the scattering layer 2a and the smoothing layer 2b were respectively coated on the transparent substrate 1.

[Comparative Example 3]
The organic light emitting device according to Comparative Example 3 is the same as Example 1 except that the scattering layer 2a and the smooth layer 2b are respectively applied on the entire surface of the transparent substrate 1 and the manufacturing process does not include vacuum heat treatment. Manufactured.

<Evaluation of dark spots>
About the organic light emitting element which concerns on the above Example 1, and the organic light emitting element which concerns on Comparative Example 1- Comparative Example 3, the generation | occurrence | production degree of a dark spot was evaluated. Note that the degree of occurrence of dark spots was evaluated by visual observation using a loupe after causing each organic light emitting element to emit light at 100 cd / m ² after high-temperature treatment and after long-term driving at room temperature.

<Evaluation of dark spot (outgas) after high temperature treatment>
About the organic light emitting device according to Example 1 and the organic light emitting devices according to Comparative Examples 1 to 3, generation of dark spots after heating each organic light emitting device for 10 hours in a high temperature environment of 85 ° C. The degree was evaluated.
The dark spot evaluation rank shown in Table 1 is based on the following criteria.
○: Generation of dark spots is not observed Δ: Minute dark spots are recognized, but the size is difficult to visually recognize ×: Dark spots that are easily visible are generated

<Evaluation of dark spots (lifetime) after long-term operation at room temperature>
For the organic light-emitting device according to Example 1 and the organic light-emitting devices according to Comparative Examples 1 to 3, each organic light-emitting device has a constant current of ^2.5 mA / cm ² in a room temperature environment of 25 ° C. and 50% RH. The degree of occurrence of dark spots after driving for 500 hours under the conditions was evaluated.
The dark spot evaluation rank shown in Table 1 is based on the following criteria.
◯: Generation of dark spots is not observed Δ: A minute dark spot is recognized, but the size is difficult to visually recognize x: Dark spots that can be easily recognized are generated.

  In Table 1, the pattern application “+” indicates that the light extraction layer is formed by patterning, and the pattern application “−” indicates that the entire surface of the light extraction layer is applied. Further, the vacuum heat treatment “+” indicates that the heat treatment was performed in a reduced pressure atmosphere, and the vacuum heat treatment “−” indicates that the pressure reduction was performed only (the barrier layer was formed under a reduced pressure). As shown in Table 1, it can be seen that in Comparative Example 1 in which the light extraction layer is patterned, dark spots that can be visually recognized are more likely to occur than in Comparative Example 3 in which the light extraction layer is applied over the entire surface. This is because the performance of the barrier layer formed on the light extraction layer is lower in Comparative Example 1 in which the light extraction layer is patterned than in Comparative Example 3 in which the entire surface of the light extraction layer is applied. This is thought to be due to the increased occurrence of dark spots under the influence of outgas in the environment. On the other hand, in Example 1 which performed the vacuum heat processing, it turns out that generation | occurrence | production of a dark spot is reduced although the light extraction layer is patterned. This is considered to be because the outgas of the light extraction layer was reduced by the vacuum heat treatment before the barrier layer was formed. In Comparative Example 2 and Comparative Example 3 in which the light extraction layer was applied over the entire surface, external moisture or the like damages the element through the light extraction layer, so that dark spots are likely to occur after long-time driving, and the light emission lifetime. It turns out that becomes short.

S10 Light extraction layer formation step S20 Vacuum heat treatment step S30 Barrier layer formation step S40 Transparent electrode formation step S50 Organic layer formation step S60 Counter electrode formation step S70 Sealing step

Claims (3)

A light extraction layer, a barrier layer, and a transparent electrode are sequentially laminated on the transparent substrate, and an organic layer containing an organic light emitting material and a counter electrode that is a counter electrode of the transparent electrode are disposed on the transparent electrode. A method of manufacturing an organic light emitting device,
Forming the light extraction layer on the transparent substrate by pattern application in an atmospheric environment;
A step of subjecting the formed light extraction layer to a vacuum heat treatment;
Forming the barrier layer continuously on the light extraction layer while maintaining the light extraction layer that has been vacuum-heated in a reduced-pressure atmosphere; and
And a step of forming the transparent electrode on the formed barrier layer.   The method for manufacturing an organic light-emitting element according to claim 1, wherein the heating in the vacuum heat treatment is performed by infrared heating.   The method for manufacturing an organic light-emitting element according to claim 1, wherein the infrared heating is performed by infrared light whose wavelength is controlled in a non-absorption wavelength region of the transparent substrate.

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