JP2011031472A - Film laminate and method for producing organic el element using the same - Google Patents

Abstract

In a solid sealing of a top emission organic EL element, a film laminate for sealing an organic EL element with a uniform gap and without mixing of air bubbles by a laminating method, and sealing Providing materials and methods for their production.
A first separator base material, an adhesive resin layer, and a second separator base material are laminated in this order, and at least one of the first separator base material and the second separator base material. One is a film laminate in which a slit is formed, and the slit is formed on a surface opposite to a surface where the first separator base material and the second separator base material are in contact with the adhesive resin layer. A film laminate characterized by being made.
[Selection] Figure 1

Description

  The present invention is an organic EL element expected to be widely used as a flat panel display used in a mobile terminal such as a television, a personal computer monitor, a mobile phone, a surface-emitting light source, illumination, a light-emitting advertising body, The present invention relates to a top emission type organic EL element and a manufacturing method thereof.

  The organic EL element is expected as a flat panel display that replaces a cathode ray tube or a liquid crystal display because of advantages such as a wide viewing angle, a high response speed, and low power consumption.

  An organic EL element has a structure in which an organic light-emitting medium layer is sandwiched between two electrode layers (anode layer and cathode layer), at least one of which has translucency, and a voltage is applied between both electrodes. It is a self-luminous display element in which light is emitted from the organic light emitting medium layer when an electric current is passed. However, since the organic EL element has a problem that it deteriorates due to the influence of moisture and oxygen in the atmosphere, a method of covering with a metal can or glass cap containing a desiccant and blocking from the atmosphere is generally used. .

  In recent years, in order to improve the light extraction efficiency of an active matrix type organic EL element, a top surface light emitting element for extracting light from a sealing member side has been proposed, and a cap sealing that includes a conventionally used desiccant has been proposed. Instead, solid sealing has been proposed in which a passivation film (sealing layer) having a barrier property, an adhesive, and a glass substrate are laminated without providing a space (Patent Documents 1 and 2).

In solid sealing, in order to maintain sealing performance, it is necessary to maintain a uniform thickness gap of several microns for the adhesive, and mixing of bubbles not only hinders light emission but also organic EL elements. Therefore, it is necessary to bond without bubbles.
In recent years, a method of laminating a film-like adhesive has been attempted as an example of a technique for uniformly bonding the gaps. The film-like adhesive sheet has a separator substrate on both sides, and after peeling off the separator substrate on one side and laminating it on a glass substrate to produce a sealing substrate, the other separator substrate is peeled off. The organic EL element can be sealed by laminating the glass substrate on which the organic EL element is formed. However, if the adhesive strengths of the separator substrates on both sides are the same, the other separator substrate is peeled off when one side is peeled off, causing a problem that the film is wrinkled and the sealing substrate is defective. For this reason, it is possible to prevent the separator base material B from being peeled off even if the separator base material A is peeled off by increasing the adhesive strength of the separator base material on one side. In the process, there is a problem that the adhesive is not peeled off from the separator base material B, and the yield is reduced.

JP 2002-231443 A JP 2004-164890 A

  The present invention relates to a film having an adhesive resin layer for sealing an organic EL element that can be stably bonded with a good yield by laminating the adhesive resin layer in solid sealing of a top emission organic EL element. It is providing the manufacturing method of a laminated body and an organic EL element using the same.

  As means for solving the above-mentioned problems, the invention according to claim 1 of the present invention is such that a first separator base material, an adhesive resin layer, and a second separator base material are laminated in this order, At least one of the separator base material and the second separator base material is a film laminate in which a slit is formed, and the slit is formed as a slit composed of at least one cut, and the slit is The film laminate is characterized in that the first separator substrate and the second separator substrate are formed on the surface opposite to the surface in contact with the adhesive resin layer.

  The invention according to claim 2 of the present invention is characterized in that the slit is formed at a corner portion of the film laminate, and the normal line of the slit passes through the apex of the corner portion where the slit is formed. 1. The film laminate according to 1.

  According to a third aspect of the present invention, a slit is formed in the first and second separator bases, and a slit formed in the first separator base and the second separator base are formed. The slits are formed at adjacent corners of the film laminate, and the straight line formed by the slit formed in the first separator substrate and the straight line formed by the slit formed in the second separator substrate are orthogonal to each other. It is a film laminated body of Claim 1 or 2 characterized by the above-mentioned.

  The invention according to claim 4 of the present invention is characterized in that a release layer is formed between the first and second separator substrates and the adhesive resin layer. It is a film laminate.

The invention according to claim 5 of the present invention is an organic material comprising a first base material, an adhesive resin layer, and a second base material on which at least an anode layer, an organic light emitting medium layer, and a cathode layer are formed. It is a manufacturing method of EL element, Comprising: The manufacturing method of the organic EL element characterized by including the following processes using the film laminated body of Claims 1 thru | or 4.
(1) The process of peeling a said 1st separator base material from the said film laminated body.
(2) A step of bonding the first substrate and the surface of the film laminate on which the adhesive resin layer is formed.
(3) The process of peeling the said 2nd separator base material from the said film laminated body bonded together with the said 1st base material, and forming the said adhesive resin layer on a said 1st base material.
(4) A step of bonding the second base material and the adhesive resin layer on the first base material together.

  The invention according to claim 6 of the present invention is the step of peeling the first and second separator substrates in the step (1) and the step (3), wherein the separator substrate is formed of the film laminate. It is a manufacturing method of the organic EL element of Claim 4 which peels in the diagonal direction of the said film laminated body from the angle | corner in which the slit was formed.

  The invention according to claim 7 of the present invention peels the separator base material using an adhesive sheet in the step of peeling the first and second separator base materials in the step (1) and the step (3). It is a manufacturing method of the organic EL element of Claim 5 characterized by the above-mentioned.

According to the present invention, since the slit made of one or more cuts is formed on at least one separator substrate, it becomes easy to peel the separator substrate from the adhesive resin layer, and the other separator substrate Undesirable peeling of the material can be prevented.
Further, according to the present invention, the slit is formed at the corner of the film laminate, and the normal of the slit passes through the apex of the corner, thereby separating the separator base material from the apex of the film laminate where the slit is formed. When peeling off, an excessive load is not generated in the slit, and the separator film is not cut from the slit portion.
Further, according to the present invention, the slits formed in the two separator bases are formed at the corners adjacent to each other of the film laminate, and the straight lines formed by the two slits are orthogonal to each other. It is possible to prevent the other from peeling off at the time of peeling.
Moreover, according to this invention, by forming the peeling layer between the separator base material and the adhesive resin layer, the separator base material can be peeled from the film laminate with a high yield.
Moreover, according to the present invention, the separator substrate can be easily peeled from the film laminate by manufacturing an organic EL element using a film laminate in which slits are formed in the separator substrate, and the other separator substrate Therefore, a stable adhesive resin layer with good yield and no defects can be formed on the organic EL element.

Cross section of film laminate The sealing process of the organic EL element using the film laminated body of this invention Cross section of organic EL element substrate

  Hereinafter, an example of the organic EL element produced by the present invention will be described with reference to FIGS. The present invention is not limited to the embodiment.

  The film laminated body 30 of this invention is demonstrated using FIG. 1, FIG.

  As shown in FIG. 1A, the film laminate 30 is formed by forming an adhesive resin layer 32 on one separator substrate 31 by coating an adhesive resin and laminating the other separator substrate 32. It is formed by.

  Here, as the separator base materials 31 and 33, commercially available plastic films such as PET, PES, PEN, and PC can be used, but the adhesive resin is used so that the separator base material and the adhesive resin layer are easily peeled off. It is necessary to form the release layers 34 and 35 in advance on the surface of the separator substrate on the side in contact with the layer. The release layers 34 and 35 are not particularly limited in the present invention. For example, a commercially available release agent such as a silicone type or a fluorine type is selected according to a desired peel strength, and a separator base material is used. What is necessary is just to coat the surface.

  As a method of forming the adhesive resin layer 32 and the release layers 34 and 35, depending on the material and pattern, a coating method such as spin coating, spray coating, flexo, gravure, micro gravure, intaglio offset, roll coating, blade coating, Printing methods, ink jet methods, dispenser application, nozzle discharge, transfer methods, laminating methods, and the like can be used.

  Here, if only the same release layers 34 and 35 are coated on the separator base materials 31 and 33, when the other separator base material 31 is peeled off as shown in FIG. Also, peeling occurs, and when the film is applied to the sealing substrate as shown in FIG. 2B, a laminating defect is likely to occur, such as wrinkles in the adhesive resin layer. On the contrary, if the peelability is lowered so that the other separator base material 33 is not peeled off, there is a problem that in the step of peeling the separator base material (FIG. 2C), the separation cannot be made and the yield is lowered.

  Therefore, as shown in FIG. 1A, a linear slit 41 is formed in one separator base material 31, thereby making a difference in the peelability between the separator base material 31 and the adhesive resin layer of the separator base material 33. The separator base material 31 can be easily peeled off without the separator base material 33 peeling off. In addition, the slit in this invention means the linear thing with the continuous cut | interruption.

  The slit may be formed only on one separator base material 31, but when the slit is formed on the other separator base material 33, the separator base material on which the slit 41 is formed as shown in FIG. The slits 42 may be formed at the corners of the separator substrate 33 adjacent to the corners 31 so that the straight lines formed by the slits 41 and the straight lines formed by the slits 42 are orthogonal to each other. By forming the slits in this way, the peeling direction A of the separator base material 31 and the peeling direction B of the separator base material 33 intersect, so when peeling one separator base material, the other separator base material is peeled simultaneously. It is possible to prevent malfunctions that occur.

Usually, the peel strength of the film laminate 30 can be suitably used at 0.05 to 50.0 N / 25 mm in a 90-degree peel (300 mm / min) test.
For example, when a slit of about 5 to 10 μm is formed on a separator substrate (25 μm) having a peel strength of 0.5 N / 25 mm, the peel strength is reduced to 0.1 N / 25 mm. Thereby, it becomes possible to peel the separator base material in which the slit was formed, without peeling off the other separator base material.

  The method for forming the slit is not particularly limited. For example, the slit is formed by using a conventional method such as transporting a film in accordance with the slit forming direction and forming the slit using a disk cutter. Further, as shown in FIG. 1, a plurality of slits may be formed at the corners of the separator substrate, or only one slit may be formed.

As a method for peeling the separator substrate, a conventional method of peeling the release film by attaching an adhesive sheet to a laminate film having a release film having a laminated structure can be used.
For example, it is possible to use a device for fixing and supporting the film laminate, adhering to the film laminate by a peeling roller with an adhesive sheet, and rotating the peeling roller with an adhesive sheet to wind up a separate substrate. The separator substrate is peeled off at a high yield by setting the adhesive sheet and the film laminate to the corner where the slit of the film laminate is formed, and the other separator substrate is prevented from being undesirably peeled off. be able to.
In addition, a method other than the peeling method using the pressure-sensitive adhesive sheet can be used as appropriate, but even in that case, the separator base material can be easily peeled off by peeling from the corner where the slit is formed, and the other separator base material is used. Undesirable peeling can be prevented.

  Next, a method for sealing an organic EL element using the film laminate of the present invention will be described with reference to FIG.

  First, the separator base material 31 is peeled from the film laminate 30 including at least the separator base material 31, the adhesive resin layer 32, and the separator base material 33 (FIG. 2A). Next, the adhesive resin layer 32 and the separator base material 33 are bonded to the sealing base material 20 using a roll laminator (FIG. 2B). Next, the separator base material 33 is peeled off (FIG. 2C), and the sealing base material 20 on which the adhesive resin layer 32 is formed is bonded to the base material 10 on which the organic EL element is formed (FIG. 2). (d)). Thereby, an organic EL element can be sealed.

  Here, as the sealing substrate 20, inorganic glass such as quartz glass, borosilicate glass and soda glass, plastic substrates such as PET, PES, and PC, or silicon oxide or aluminum oxide on these glass substrates or plastic substrates. In addition, an inorganic thin film such as silicon nitride or silicon oxynitride can be used. Furthermore, it may be colored with a color filter layer depending on the application, and the light extraction efficiency may be improved by imparting irregularities to the scattering particles and the surface. Moreover, if it is a bottom emission type organic EL element, it does not need to be transparent and metal sheets and films, such as stainless steel and Al, can also be used.

  The material of the adhesive resin layer 32 is not particularly limited, and a known adhesive resin layer can be used. For example, a photocurable adhesive resin such as an epoxy resin, an acrylic resin, or a silicone resin, Thermosetting adhesive resins, photocurable adhesive resins, thermosetting adhesive resins, thermoplastic adhesive resins made of acid-modified products such as polyethylene and polypropylene can be used. If necessary, the adhesive layer may contain a spherical or rod-like spacer made of glass or resin for gap control, or may contain a desiccant or an oxygen absorbent.

  Next, the organic EL element manufactured by this invention is demonstrated using FIG.

  The organic EL device manufactured according to the present invention uses an electrode substrate as the substrate 10. As the electrode base material, it is sufficient that at least a pixel electrode 11 described later is formed on a plastic film such as glass, quartz, polyethersulfone, and polycarbonate. Hereinafter, a driving substrate on which a thin film transistor (TFT) is formed. The case where is used will be described.

  A known thin film transistor can be used as the thin film transistor. Specifically, a thin film transistor mainly including an active layer in which a source / drain region and a channel region are formed, a gate insulating film, and a gate electrode can be given. The structure of the thin film transistor is not particularly limited, and examples thereof include a staggered type, an inverted staggered type, a top gate type, and a coplanar type.

The active layer is not particularly limited, and examples thereof include amorphous semiconductor materials such as amorphous silicon, polycrystalline silicon, microcrystalline silicon, cadmium selenide, thiophene oligomers, poly (p-ferylene vinylene), and the like. It can be formed of an organic semiconductor material. These active layers are formed by, for example, depositing amorphous silicon by plasma CVD, ion doping, forming amorphous silicon by LPCVD using SiH ₄ gas, and crystallizing amorphous silicon by solid phase growth. After obtaining silicon, ion doping is performed by ion implantation, LPCVD using Si ₂ H ₆ gas, and amorphous silicon is formed by PECVD using SiH ₄ gas, and laser such as excimer laser is used. After annealing and crystallizing amorphous silicon to obtain polysilicon, polysilicon is deposited by ion doping (low temperature process), low pressure CVD or LPCVD, and thermally oxidized at 1000 ° C. or higher. Gate break Film is formed, a gate electrode of the n + polysilicon is formed thereon, then, a method of ion doping (high temperature process), and the like by an ion implantation method.

As the gate insulating film, typically, it can be used that is used as a gate insulating film, for example, PECVD method, SiO formed by the LPCVD method or the like _2; SiO obtained polysilicon film was thermally oxidized ₂ Etc. can be used.

  As a gate electrode, what is normally used as a gate electrode can be used, for example, metals, such as aluminum and copper, refractory metals, such as titanium, tantalum, and tungsten, polysilicon, silicide of a refractory metal, Polycide etc. are mentioned. The thin film transistor may have a single gate structure, a double gate structure, or a multi-gate structure having three or more gate electrodes. Moreover, you may have a LDD structure and an offset structure. Further, two or more thin film transistors may be arranged in one pixel.

  The organic EL element manufactured by the present invention is connected so that the thin film transistor functions as a switching element of the organic EL element, and the drain electrode of the transistor and the pixel electrode 11 of the organic EL element are electrically connected. The thin film transistor, the drain electrode, and the pixel electrode 11 of the organic EL element are connected through a connection wiring formed in a contact hole that penetrates the planarization film. FIG. 3 is a schematic view in which the thin film transistor portion is omitted and the pixel electrode 11, the partition wall 12, the organic light emitting medium layer 13, the counter electrode layer 14, and the passivation layer 15 are formed on the base material 10.

  In the embodiment of the present invention, the pixel electrode 11 is partitioned by the partition wall 12 and becomes a pixel electrode corresponding to each pixel. As a material of the pixel electrode 11, it is preferable to select a material having a high work function such as ITO, a metal composite oxide such as ITO (indium tin composite oxide), indium zinc composite oxide, zinc aluminum composite oxide, Either a single layer or a laminate of a metal material such as gold or platinum, or a fine particle dispersion film in which fine particles of these metal oxides or metal materials are dispersed in an epoxy resin or an acrylic resin can be used. In addition, in a top emission type organic EL device manufactured according to the present invention, an ITO film is laminated on a metal material such as Ag or Al when the pixel electrode needs to have hole injection property and reflectivity. That's fine.

  The optimum value of the film thickness of the pixel electrode 11 varies depending on the element configuration of the organic EL element, but it is 100 to 10,000 mm, more preferably 3000 or less, regardless of whether it is a single layer or a stacked layer.

  As the formation method of the pixel electrode 11, depending on the material, dry film forming methods such as resistance heating vapor deposition method, electron beam vapor deposition method, reactive vapor deposition method, ion plating method, sputtering method, gravure printing method, screen printing, etc. A wet film forming method such as a method can be used.

  The partition wall 12 is formed so as to partition the light emitting region corresponding to the pixel. In general, an active matrix drive type display device is formed so that a pixel electrode 11 is formed for each pixel, and each pixel occupies as wide an area as possible so as to cover an end portion of the pixel electrode 11. The most preferable shape of the partition wall 12 is basically a lattice shape that divides each pixel electrode 11 by the shortest distance.

As a method of forming the partition wall 12, as in the conventional method, an inorganic film is uniformly formed on a substrate, masked with a resist, and then dry-etched, or a photosensitive resin is laminated on the substrate, and a photolithography method is used. The method of setting to a predetermined pattern is mentioned. If necessary, a water repellent can be added, or plasma or UV can be irradiated to impart liquid repellency to the ink after formation.
A preferable height of the partition wall 12 is not less than 0.1 μm and not more than 10 μm, and more preferably not less than 0.5 μm and not more than 2 μm. If the height of the partition wall 12 exceeds 10 μm, the formation and sealing of the counter electrode is hindered, and if it is less than 0.1 μm, the end of the pixel electrode 11 cannot be covered, or the adjacent pixels are formed when the light emitting medium layer is formed. This is because they are short-circuited or mixed colors.

  The organic light emitting medium layer 13 in the present invention can be formed of a single layer film or a multilayer film containing a light emitting substance. Examples of the configuration in the case of forming a multilayer film include a hole transport layer, an electron transporting light emitting layer or a hole transporting light emitting layer, a two-layer structure comprising an electron transport layer, a hole transport layer, a light emitting layer, and an electron transport layer. By further separating the hole (electron) injection function and the hole (electron) transport function as necessary, or by inserting a layer that blocks the transport of holes and electrons, if necessary, It is more preferable to form a multilayer.

Examples of hole transport materials include metal phthalocyanines such as copper phthalocyanine and tetra (t-butyl) copper phthalocyanine and metal-free phthalocyanines, quinacridone compounds, 1,1-bis (4-di-p-tolylaminophenyl) Cyclohexane, N, N′-diphenyl-N, N′-bis (3-methylphenyl) -1,1′-biphenyl-4,4′-diamine, N, N′-di (1-naphthyl) -N, Aromatic amine low molecular hole injection and transport materials such as N′-diphenyl-1,1′-biphenyl-4,4′-diamine, polyaniline, polythiophene, polyvinylcarbazole, poly (3,4-ethylenedioxythiophene) ) and polymer hole transport materials such as a mixture of polystyrene sulfonic acid, polythiophene oligomer _{materials, Cu 2 O, Cr 2 O} 3, Mn 2 O _{, FeOx (x~0.1), NiO,} CoO, Pr 2 O 3, Ag 2 O, MoO 2, Bi 2 O 3, ZnO, TiO 2, SnO 2, ThO 2, V 2 O 5, Nb 2 O ₅ , Ta ₂ O ₅ , MoO ₃ , WO ₃ , MnO ₂ and other inorganic materials, and other existing hole transport materials can be selected.

  In the case of a polymer EL display, an interlayer layer is preferably formed on the hole transport material. Examples of materials used for the interlayer layer include polymers containing aromatic amines such as polyvinyl carbazole or derivatives thereof, polyarylene derivatives having aromatic amines in the side chain or main chain, arylamine derivatives, and triphenyldiamine derivatives. . These materials can be dissolved or dispersed in a solvent and formed using various coating methods such as spin coating or letterpress printing.

  As the light-emitting material, 9,10-diarylanthracene derivatives, pyrene, coronene, perylene, rubrene, 1,1,4,4-tetraphenylbutadiene, tris (8-quinolinolato) aluminum complex, tris (4-methyl-8-) Quinolinolato) aluminum complex, bis (8-quinolinolato) zinc complex, tris (4-methyl-5-trifluoromethyl-8-quinolinolato) aluminum complex, tris (4-methyl-5-cyano-8-quinolinolato) aluminum complex, Bis (2-methyl-5-trifluoromethyl-8-quinolinolato) [4- (4-cyanophenyl) phenolate] aluminum complex, bis (2-methyl-5-cyano-8-quinolinolato) [4- (4- Cyanophenyl) phenolate] aluminum complex, tri (8-quinolinolato) scandium complex, bis [8- (para-tosyl) aminoquinoline] zinc complex and cadmium complex, 1,2,3,4-tetraphenylcyclopentadiene, pentaphenylcyclopentadiene, poly-2,5- Diheptyloxy-para-phenylene vinylene, coumarin phosphor, perylene phosphor, pyran phosphor, anthrone phosphor, porphyrin phosphor, quinacridone phosphor, N, N'-dialkyl-substituted quinacridone phosphor , Naphthalimide-based phosphors, N, N′-diaryl-substituted pyrrolopyrrole-based phosphors, low-molecular light-emitting materials such as phosphorescent phosphors such as Ir complexes, polyfluorene, polyparaphenylene vinylene, polythiophene, polyspiro, etc. Of these low molecular weight materials. Or copolymerized material and can be used other conventional fluorescent light emitting material or phosphorescent material.

Examples of electron transport materials include 2- (4-biphenylyl) -5- (4-tert-butylphenyl) -1,3,4-oxadiazole, 2,5-bis (1-naphthyl) -1 , 3,4-oxadiazole, oxadiazole derivatives, bis (10-hydroxybenzo [h] quinolinolato) beryllium complexes, triazole compounds, and the like can be used.
Alternatively, these electron transport materials may be used as an electron injection layer by doping a small amount of alkali metal or alkaline earth metal having a low work function such as sodium, barium, or lithium.

  The film thickness of the organic light emitting medium layer is 1000 nm or less, preferably about 50 to 200 nm, even when formed by a single layer or a stacked layer.

  Depending on the material, the organic luminescent medium layer can be formed by vacuum deposition, coating, printing such as slit coating, spin coating, spray coating, nozzle coating, flexo, gravure, micro gravure, intaglio offset, inkjet, etc. The method etc. can be used.

  The counter electrode layer 14 according to the present invention only needs to have at least a role as an electron-injecting cathode, but in the case of a top emission type organic EL element, it must also serve as a transparent electrode. As the electron-injecting cathode, an alkali metal or alkaline earth metal such as Li, Ba, Mg, or Ca having a low work function, or a compound such as an oxide or fluoride of these metals can be used. Although these materials are excellent in electron injecting property, they are poor in stability. Therefore, it is more preferable to use a laminated film or an alloy film with a metal having excellent stability such as Al or Ag.

  As a method for forming the cathode, a resistance heating vapor deposition method, an electron beam vapor deposition method, a reactive vapor deposition method, an ion plating method, or a sputtering method may be selected depending on the material. Further, the thickness of the counter electrode layer 14 is not particularly limited, but the counter electrode layer 14 can be used with a thickness of about 10 nm to 1000 nm. In the case of a top emission type EL display, an alkaline metal such as Ba may be about 5 nm, a stable metal such as Al may be about 10 nm, and a transparent electrode such as ITO may be stacked to reduce the resistance.

  As the passivation layer 15 in the present invention, metal oxides such as silicon oxide and aluminum oxide, metal fluorides such as aluminum fluoride and magnesium fluoride, metal nitrides such as silicon nitride, aluminum nitride and carbon nitride, silicon oxynitride A laminated film of a metal oxynitride such as silicon carbide, a metal carbide such as silicon carbide, and a polymer resin film such as an acrylic resin, an epoxy resin, a silicone resin, or a polyester resin may be used as necessary. In particular, it is preferable to use silicon oxide, silicon nitride, or silicon oxynitride from the viewpoint of barrier properties and transparency. Furthermore, a laminated film or a gradient film with a variable film density may be used depending on the film forming conditions. .

As a method for forming the passivation layer 15, a resistance heating vapor deposition method, an electron beam vapor deposition method, a reactive vapor deposition method, an ion plating method, a sputtering method, and a CVD method can be used depending on the material. Further, it is preferable to use the CVD method in terms of translucency. As the CVD method, a thermal CVD method, a plasma CVD method, a catalytic CVD method, a VUV-CVD method, or the like can be used. In addition, as a reaction gas in the CVD method, a gas such as N ₂ , O ₂ , NH ₃ , H ₂ , N ₂ O is added to an organic silicon compound such as monosilane, hexamethyldisilazane (HMDS), or tetraethoxysilane. It may be added as necessary. For example, the density of the film may be changed by changing the flow rate of silane, and hydrogen or carbon may be contained in the film by the reactive gas used. The film thickness of the sealing layer varies depending on the electrode step of the organic EL element, the height of the partition walls of the substrate, the required barrier characteristics, and the like, but generally about 10 nm to 10,000 is generally used.

  EXAMPLES Hereinafter, although an Example and a comparative example further demonstrate this invention, this invention is not restrict | limited to the following example.

First, the organic EL element substrate 51 is produced (FIG. 3). Glass was used as the substrate 10, and an ITO film (150 nm) was patterned on the substrate 10 as the pixel electrode layer 11 by sputtering. Next, as the partition pattern 12, a positive photosensitive polyimide resin (2 μm) was formed into a pattern film by using a photolithography method.
Next, as the organic light-emitting medium layer 13, a mixture (20 nm) of poly (3,4-ethylenedioxythiophene) and polystyrenesulfonic acid is used for the hole transport layer, and poly [2-methoxy-5- (2 '-Ethyl-hexyloxy) -1,4-phenylenevinylene] (MEHPPV) (100 nm) was patterned using a relief printing method. Next, as the transparent electrode layer 14, a Ca film (5 nm) and an Al film (20 nm) were laminated using a vapor deposition method. Next, an organic EL element substrate 51 was produced by forming a SiNx film of 5000 nm as the passivation layer 15.
Next, a PET film (25 μm) 31 and 33 coated with silicone release layers 34 and 35 and a film laminate 30 using a photocurable epoxy resin 32 as an adhesive resin layer are shown in FIG. As described above, the separator base material 31 is peeled off and bonded to the glass substrate that is the sealing base material 20, and then the separator base material 33 is peeled off to place the sealing base material 32 on the organic EL element substrate 51. Bonding is performed via the adhesive resin layer 32.
At this time, as shown in FIG. 1A, the separator base 31 is formed with slits 41, so that the separator base 31 has a peel strength of 0.1 N / 25 mm, and the separator base 33 has a peel strength of 0. Since a difference in peel strength from 0.5 N / 25 mm was generated, the separator base material 33 was not peeled when the separator base material 31 was peeled off, and sealing could be performed without causing poor bonding.
The produced organic EL element (number of pixels: 960 × 540) was free from bubbles and pixel defects even when stored at 85 ° C. and 90 RH% for 3000 hours.

<Comparative Example 1>
In the organic EL element described in Example 1, the separator substrate 31 was bonded without forming a slit in the film. Since the peeling strength of the separator base material 31 is the same as the peeling strength of the separator base material 33, when the separator base material 31 is peeled, the separator base material 33 is also peeled at the same time, and the adhesive resin layer is wrinkled. When the organic EL element substrate 51 was bonded, the organic EL element was sealed with wrinkles generated at the end portions of the adhesive resin layer 32.
The produced organic EL device (pixel number: 960 × 540) has a pixel defect when it is stored at 85 ° C. and 90 RH% for 500 hours, and about 50% of all pixels are not emitting light. Non-luminous.

DESCRIPTION OF SYMBOLS 10 Base material 11 Pixel electrode 12 Partition pattern 13 Organic luminescent medium layer 14 Transparent electrode 15 Passivation layer 20 Sealing base material 30 Film laminated body 31 Separator base material 32 Adhesive resin layer 33 Separator base materials 34 and 35 Release layers 41 and 42 Slit 51 Organic EL element substrate

Claims (7)

A first separator base material, an adhesive resin layer, and a second separator base material are laminated in this order, and at least one of the first separator base material and the second separator base material is slit. Is a film laminate in which is formed,
The slit is formed as a slit composed of at least one cut, and the slit is formed on a surface opposite to a surface where the first separator substrate and the second separator substrate are in contact with the adhesive resin layer. A film laminate characterized by being made.   The film laminate according to claim 1, wherein the slit is formed at a corner of the film laminate, and a normal line of the slit passes through a vertex of the corner where the slit is formed.   A slit is formed in the first and second separator bases, and the slit formed in the first separator base and the slit formed in the second separator base are adjacent corners of the film laminate. The straight line formed by the slit formed in the first separator base material and the straight line formed by the slit formed in the second separator base material are orthogonal to each other. The film laminated body of description.   The film laminate according to any one of claims 1 to 3, wherein a release layer is formed between the first and second separator substrates and the adhesive resin layer. A method for producing an organic EL device comprising: a first base material; an adhesive resin layer; and a second base material on which at least an anode layer, an organic light emitting medium layer, and a cathode layer are formed. The manufacturing method of the organic EL element characterized by including the following processes using the film laminated body of 1 thru | or 4.
(1) The process of peeling a said 1st separator base material from the said film laminated body.
(2) A step of bonding the first substrate and the surface of the film laminate on which the adhesive resin layer is formed.
(3) The process of peeling the said 2nd separator base material from the said film laminated body bonded together with the said 1st base material, and forming the said adhesive resin layer on a said 1st base material.
(4) A step of bonding the second base material and the adhesive resin layer on the first base material together.   In the step of peeling off the first and second separator base materials in the step (1) and the step (3), the separator base material is formed from the corner where the slit of the film laminate is formed. The method for producing an organic EL element according to claim 4, wherein the organic EL element is peeled in a diagonal direction.   The separator base material is peeled off using an adhesive sheet in the step of peeling off the first and second separator base materials in the step (1) and the step (3). Manufacturing method of organic EL element.

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