JP2008226471A - Manufacturing method of organic electroluminescent panel and organic electroluminescent panel - Google Patents

Abstract

<P>PROBLEM TO BE SOLVED: To provide a manufacturing method of an organic EL panel and an organic EL panel not causing performance degradation of organic EL elements without imposing any limit on adhesives or sealing members to be used, at the time of manufacturing of the organic EL panel having an airtight sealing structure by dint of the sealing members from organic EL elements provided with at least a first electrode layer, an organic compound layer including a light-emitting layer, and a second electrode layer on a substrate. <P>SOLUTION: In the manufacturing method of the organic electroluminescent panel with an airtight sealing structure for sealing an organic electroluminescent element by sealing members at least equipped with a first electrode layer, an organic compound layer including a light-emitting layer, and a second electrode layer on a substrate, at least a top face of the second electrode layer is put under a smoothing treatment, and after that, the sealing members are laminated. <P>COPYRIGHT: (C)2008,JPO&INPIT

Description

  The present invention relates to a method for producing an organic electroluminescence panel (hereinafter also referred to as an organic EL panel) and an organic EL panel produced by this production method.

  In recent years, organic EL elements using organic substances have been promising for use as solid light-emitting inexpensive, large-area full-color display elements and writing light source arrays, and active research and development have been promoted. The organic EL element includes a first electrode (anode or cathode) formed on a substrate, an organic compound layer (single layer portion or multilayer portion) containing an organic light emitting material laminated thereon, that is, a light emitting layer, It is a thin film type element having a second electrode (cathode or anode) laminated on the light emitting layer. When a voltage is applied to such an organic EL element, electrons are injected from the cathode and holes are injected from the anode into the organic compound layer. It is known that light is obtained by releasing energy as light when the electrons and holes recombine in the light emitting layer and the energy level returns from the conduction band to the valence band.

  As described above, since the organic EL element is a thin film type element, when an organic EL panel in which one or a plurality of organic EL elements are formed on a substrate is used as a surface light source such as a backlight, a surface light source. It is possible to easily make a device equipped with In addition, when a display device is configured using an organic EL panel in which a predetermined number of organic EL elements as pixels are formed on a substrate as a display panel, the liquid crystal display device has high visibility and no viewing angle dependency. There are benefits that cannot be obtained.

  Organic substances such as organic light emitting materials used in organic EL elements are weak against moisture and oxygen, and their performance deteriorates. Also, the characteristics of electrodes deteriorate rapidly in the atmosphere due to oxidation. In order to prevent such deterioration, a sealing layer is generally provided as the uppermost layer.

  Many studies have been made on the organic EL element sealing method so far, and it is roughly classified into two methods, a casing type sealing method and a close contact type sealing method.

  The casing type sealing method is to seal an organic EL element by placing it in a case and blocking the outside, and filling the case with a predetermined gas or fluid for sealing together with the organic EL element. Is the method. The close-contact type sealing method is to seal by sealing the surface of an organic EL element formed on the substrate (behind the element when viewed from the substrate side) with an adhesive such as a glass plate. Is the method.

  In the case of the casing type sealing method, there is a problem that it cannot be made thin, requires a process for filling the case with a sealing gas or fluid, and is unsuitable for mass production. Therefore, a close-contact type sealing method has become the mainstream because it can be made thin, mass production is relatively easy, and a high sealing effect can be easily obtained.

As a close-contact type sealing method, for example, as described in JP-A-5-182759, a glass substrate is fixed on a protective film made of an inorganic compound such as SiO ₂ via an adhesive, a photocurable resin, or the like. How to do is known. However, in this method, when the adhesive and the photo-curing resin are cured, a residual stress is generated because the volume shrinks. This residual stress is caused by the organic EL element to be sealed and the adhesive or photo-curing resin. Even if there is a film of SiO ₂ or the like between them, if the film thickness is as thin as μm, it is transmitted to the organic EL. As described in JP-A-5-101844, a method of coating a sealing film formed of a moisture-proof polymer film and an adhesive layer on the outer surface of an organic electroluminescence element is known. However, in this method, when the adhesive is cured, the volume shrinks, so that a residual stress is generated, and this residual stress is transmitted to the organic EL. As a result, for example, a light emission failure and a non-light emitting portion (also referred to as a spot-like light emission defect or a dark spot) are generated along with a minute deformation of the second electrode.

  In order to cope with these problems, measures for alleviating residual stress when the adhesive and the photocurable resin are cured by an adhesion type sealing method using an adhesive and a photocurable resin have been studied so far. For example, a sealant made of a thermoplastic adhesive resin having a melt flow rate of 5 g / 10 min or more and 20 g / 10 min or less as defined in JIS K 7210 in order to prevent a decrease in tensile strength, stress cracking resistance, workability, etc. as a barrier layer An organic EL element that is tightly sealed with a sealing film including a layer is known (see, for example, Patent Document 1).

  As an adhesive layer on the organic EL element, the adhesive shrinkage of the adhesive on the organic EL element side is set to two layers by using an adhesive smaller than the shrinkage ratio of the adhesive on the sealing material side to cure the adhesive. A method is known in which a sealing material is fixed with an adhesive so that the light emitting element is not affected by stress due to shrinkage (see, for example, Patent Document 2).

  The close-contact type sealing methods described in Patent Document 1 and Patent Document 2 enable relatively easy mass production and support a thin organic EL element having a high sealing effect. Damages to the light-emitting element due to (surface adhesion on the organic electroluminescence element) are occasionally observed, and the response is insufficient. In addition, the range of adhesives and sealing members to be used is limited, making it difficult to use versatile materials.

From such a situation, an organic electroluminescence panel (hereinafter referred to as organic EL) in which an organic electroluminescence element (hereinafter also referred to as organic EL element) is sealed by an adhesion type sealing method in which a sealing material is fixed via an adhesive. The manufacturing method of an organic EL panel and the development of an organic EL panel that does not cause deterioration of the performance of the organic EL element are desired. . In the present invention, a state where the first electrode, the organic layer, and the second electrode are formed on the substrate is referred to as an organic EL element, and a state in which the first electrode, the organic layer, and the second electrode are tightly sealed with a sealing member is referred to as an organic EL panel.
JP 2001-307871 A JP 2003-109750 A

  The present invention has been made in view of the above situation, and an object of the present invention is to seal an organic EL element having at least a first electrode layer, an organic compound layer including a light emitting layer, and a second electrode layer on a substrate. When manufacturing an organic EL panel having a close-sealing structure with a stop member, an organic EL panel manufacturing method and an organic EL that do not cause deterioration in performance of the organic EL element without limiting the adhesive and the sealing member to be used Is to provide a panel.

  The above object of the present invention has been achieved by the following constitution.

  1. In an organic electroluminescence panel manufacturing method, an organic electroluminescence element having at least a first electrode layer, an organic compound layer including a light emitting layer, and a second electrode layer on a substrate and having a close sealing structure with a sealing member. A method for producing an organic electroluminescence panel, comprising: laminating the sealing member after dry-treating at least a surface of the second electrode layer on which the sealing member is bonded.

  2. 2. The method for producing an organic electroluminescence panel according to 1 above, wherein the surface roughness Ra of the upper surface of the second electrode layer after the dry etching treatment is 30 nm or less.

  3. 3. The method of manufacturing an organic electroluminescence panel according to 1 or 2, wherein after the dry etching process is performed, an oxidation process is further performed.

  4). 3. The method for producing an organic electroluminescence panel according to 1 or 2, wherein an oxidation treatment is performed simultaneously with the dry etching treatment.

  5. 5. The organic electroluminescence panel according to claim 1, wherein an adhesive layer is formed on the second electrode layer subjected to the dry etching process, and then a sealing member is stacked. Production method.

  6). 5. The method of manufacturing an organic electroluminescence panel according to any one of 1 to 4, wherein an inorganic film is formed on the second electrode layer subjected to the dry etching process.

  7. The inorganic film is formed on the second electrode layer that has been subjected to the dry etching process, an adhesive layer is formed on the inorganic film, and then the sealing member is laminated. The manufacturing method of the organic electroluminescent panel of any one of -4.

  8). An inorganic film is formed on the second electrode layer that has been subjected to the dry etching process, and then the upper surface of the inorganic film is subjected to a dry etching process to have a surface roughness Ra of 30 nm or less. 5. The method for producing an organic electroluminescence panel according to any one of 1 to 4, wherein an adhesive layer is formed on the sealing member and the sealing member is laminated.

  9. 9. An organic electroluminescence panel manufactured by the manufacturing method according to any one of 1 to 8 above.

  When manufacturing an organic EL panel having an adhesion sealing structure with an organic EL element having at least a first electrode layer, an organic compound layer including a light emitting layer, and a second electrode layer on a substrate with a sealing member. It is possible to provide an organic EL panel manufacturing method and an organic EL panel that do not cause deterioration in performance of the organic EL element without limiting the adhesive and the sealing member to be used, and a high-quality thin and light organic EL panel Production is now possible.

  Embodiments of the present invention will be described with reference to FIGS. 1 to 7, but the present invention is not limited thereto.

  FIG. 1 is a schematic view showing an example of a manufacturing process of an organic EL panel having an organic EL element produced by using a single-wafer substrate and having a sealing and sealing structure with a sealing member. In addition, the description of the manufacturing method shown in this figure has already used an organic EL element formed in the order of a first electrode, a hole transport layer, a light emitting layer, an electron injection layer, and a second electrode on a single-wafer substrate. Therefore, the manufacturing process of the organic EL element is omitted.

  FIG. 1A will be described. In the figure, reference numeral 1a denotes a manufacturing process of the organic EL element. The manufacturing process 1 a includes an organic EL element supply step 101, a dry etching treatment step 102, an adhesive coating step 103, a sealing member bonding step 104, a punching step 105, and a recovery step 106. ing.

  The supply process 101 includes a supply device 101b that supplies an organic EL element 101a in which at least one organic EL element is formed on a single-wafer substrate to the next process.

  The dry etching process 102 includes a smoothing process 102a and an oxidation process 102b. In the smoothing process step 102a, the surface of the organic EL element 101a on the side where the sealing member for the second electrode is bonded is dry-etched (also referred to as smoothing process) with the dry etching apparatus 102a1. The surface roughness Ra of the surface to which the sealing member of the second electrode after the dry etching treatment is bonded is the second due to stress relaxation accompanying the expansion and contraction of the adhesive and the stress accompanying the expansion and contraction of the adhesive. Considering light emission failure accompanying minute deformation of the electrode, prevention of non-light emitting part (also called point light emission defect, dark spot), prevention of moisture permeation from the interface between the adhesive and the second electrode, etc. 30 nm or less is preferable. More preferably, it is 0.1 nm or more and 20 nm or less. The surface roughness Ra indicates a value measured by an atomic force microscope (AFM) SPA300 manufactured by SII Nano Technology.

  The dry etching apparatus 102a1 is not particularly limited. For example, a reactive gas etching apparatus, an atmospheric pressure plasma reactive ion etching apparatus, a low pressure plasma reactive ion etching apparatus, a reactive ion beam etching apparatus, an ion beam etching apparatus, and a reactive laser. Examples thereof include a beam etching apparatus and a laser beam etching apparatus. These dry etching apparatuses can use commercially available dry etching apparatuses.

  In the oxidation treatment step 102b, an oxide film is formed on the surface of the second electrode after the dry etching treatment (smoothing treatment) by the dry etching apparatus 102b1. The dry etching apparatus 102b1 is not particularly limited, and examples thereof include a reactive gas etching apparatus, an atmospheric pressure plasma reactive ion etching apparatus, a reactive ion beam etching apparatus, and a reactive laser beam etching apparatus that use oxygen as a reaction gas. It is done. It is also possible to use a surface treatment apparatus that irradiates a low-pressure mercury lamp or excimer lamp. These dry etching apparatuses can use commercially available dry etching apparatuses.

  By forming the oxide film, the surface of the second electrode becomes hard, light emitting failure accompanying micro deformation, non-light emitting part (also referred to as a spot-like light emitting defect, dark spot), adhesive and the second electrode This improves the adhesion and prevents moisture penetration from the interface. The oxidation treatment step can be omitted if necessary.

  The adhesive coating process 103 includes an adhesive coating apparatus 103a and a mounting table 103b on which the organic EL element sent from the oxidation treatment process 102b is mounted. In the adhesive coating step 103, an adhesive is coated around the light emitting region and the light emitting region except for the end portions of the extraction electrodes of the first and second electrodes of the organic EL element sent from the oxidation treatment step 102b. Is done.

  In the sealing member bonding step 104, the organic EL element coated with the adhesive in the adhesive coating step 103 is placed on the mounting table 104a, and the sheet-like sheet-like flexible sealing member 104b is stacked. After overlapping, bonding is performed by the flexible sealing member bonding apparatus 104c.

  In the punching step 105, unnecessary portions of the bonded flexible sealing member are removed, and the flexible sealing member is bonded onto the second electrode except for the end portions of the first electrode and the second electrode. In this state, at least one organic EL panel is formed on the single-wafer substrate, and then individual organic EL panel elements are punched and cut from the single-wafer substrate by the punching and cutting device 105a.

  In the recovery process 106, the individual organic EL panels 106a punched in the punching process 105 are recovered.

  FIG. 1B will be described. In the figure, 1b shows a manufacturing process of the organic EL element. The manufacturing process 1b includes an organic EL element supplying step 101, a dry etching treatment step 102, an inorganic film forming step 107, an adhesive coating step 103, a sealing member bonding step 104, a punching step 105, And a recovery step 106. The difference from the manufacturing process of the organic EL element shown in FIG. 1A is that an inorganic film forming step 107 is disposed after the oxidation treatment step 102b, and all other steps are the same. The oxidation treatment step 102b can be omitted if necessary.

  The inorganic film forming step 107 includes a vapor deposition apparatus 107b having an evaporation source container 107a. In the inorganic film forming step 107, an inorganic film is formed under reduced pressure by the vapor deposition apparatus 107b on the image forming region of the second electrode of the organic EL element sent from the oxidation treatment step 102b. Other reference numerals are the same as those in FIG.

  The method for forming the inorganic film is not particularly limited. For example, vacuum deposition, sputtering, reactive sputtering, molecular beam epitaxy, cluster ion beam, ion plating, plasma polymerization, atmospheric pressure plasma polymerization A plasma CVD method, a laser CVD method, a thermal CVD method, a coating method, or the like can be used, but an atmospheric pressure plasma polymerization method as described in JP-A-2004-68143 is particularly preferable.

  FIG. 1C will be described. In the figure, 1c represents a manufacturing process of the organic EL element. The manufacturing process 1c includes an organic EL element supply step 101, a dry etching treatment step 102, an inorganic film formation step 107, an inorganic film dry etching treatment step (also referred to as an inorganic film smoothing treatment step) 108, an inorganic film oxidation step It has a processing step 109, an adhesive coating step 103, a sealing member bonding step 104, a punching step 105, and a recovery step 106. The difference from the manufacturing process of the organic EL element shown in FIG. 1A is that an inorganic film forming process 107, an inorganic film smoothing process 108, and an inorganic film oxidation process 109 are arranged after the oxidation process 102b. That is, all other processes are the same. The oxidation treatment step 102b can be omitted if necessary. The inorganic film smoothing process 108 has the same dry etching apparatus 108a as the smoothing process 102a, and smoothes the surface adjacent to the upper layer of the inorganic film formed in the inorganic film forming process 107. The surface roughness Ra of the surface of the inorganic film after the smoothing treatment reduces the influence on the organic EL element due to stress relaxation accompanying the expansion and contraction of the adhesive, improves the adhesion between the adhesive and the inorganic film, and increases moisture from the interface. In consideration of prevention of penetration of water, etc., 30 nm or less is preferable. More preferably, it is 0.1 nm or more and 20 nm or less. The surface roughness Ra indicates a value measured by an atomic force microscope (AFM) SPA300 manufactured by SII Nano Technology.

  In the inorganic film oxidation treatment step 109, an oxide film is formed on the surface of the inorganic film that has been smoothed by the dry etching apparatus 109a.

  By forming an oxide film, the elastic modulus of the inorganic film decreases, further reducing the effect on the organic EL element due to stress relaxation accompanying the expansion and contraction of the adhesive and improving the adhesion between the adhesive and the inorganic film. An effect of preventing moisture permeation from the interface can be obtained. The inorganic film oxidation treatment step can be omitted if necessary.

  The dry etching apparatus 108a can use the same dry etching apparatus as the dry etching apparatus 102a1 shown in FIG. 1A, and the dry etching apparatus 109a can use the same dry etching apparatus as the dry etching apparatus 102b1 shown in FIG. is there. Other reference numerals are the same as those in FIGS. 1 (a) and 1 (b).

  FIG. 2 is a schematic view showing an example of a manufacturing process of an organic EL panel having an organic EL element produced using a belt-like base material and having a close sealing structure with a sealing member. In the description of the manufacturing method shown in this figure, the organic EL element already formed in the order of the first electrode, the hole transport layer, the light emitting layer, the electron injection layer, and the second electrode on the belt-like substrate is described. In order to use, the manufacturing process of the organic EL element is omitted.

  FIG. 2A will be described. In the figure, reference numeral 2a denotes a manufacturing process of the organic EL element. The manufacturing process 2 a includes an organic EL element supply step 201, a dry etching treatment step 202, an adhesive coating step 203, a sealing member bonding step 204, and a recovery step 205. The manufacturing process shown in this figure shows a case where the supply process 201 to the recovery process 205 are continuously performed under atmospheric pressure conditions.

  The supply process 201 has a feeding device (not shown) of the organic EL element 201a wound up in a roll shape. In the supply process 201, the organic EL element 201a wound up in a roll shape is continuously fed out to the next dry etching process 202.

  The dry etching process 202 has a smoothing process 202a and an oxidation process 202b. In the smoothing treatment step 202, the surface of the organic EL element 201a on the side where the sealing member for the second electrode is bonded is dry-etched (also referred to as smoothing treatment) with the dry etching apparatus 202a1. The surface roughness Ra of the surface on which the sealing member of the second electrode after the dry etching process (smoothing process) is bonded is related to the stress relaxation accompanying the expansion and contraction of the adhesive and the expansion and contraction of the adhesive. Emission failure due to minute deformation of the second electrode due to stress, prevention of non-emission part (also called spot-like emission defect, dark spot), improved adhesion between the adhesive and the second electrode, and from the interface In consideration of prevention of moisture permeation, etc., 30 nm or less is preferable. More preferably, it is 0.1 nm or more and 20 nm or less. The surface roughness Ra indicates a value measured by an atomic force microscope (AFM) SPA300 manufactured by SII Nano Technology.

  As the dry etching apparatus 202a1, it is possible to use the same dry etching apparatus as the dry etching apparatus 102a1 used in FIG.

  In the oxidation treatment process 202b, an oxide film is formed on the surface of the second electrode after the smoothing treatment by the dry etching apparatus 202b1. As the dry etching apparatus 202b1, it is possible to use the same dry etching apparatus as the dry etching apparatus 102b1 used in FIG.

  By forming the oxide film, the surface of the second electrode is hardened, and it is possible to prevent light emission failure accompanying non-deformation, non-light emitting portion (also referred to as point-like light emission defect, dark spot), etc., and adhesive Adhesion with the second electrode is improved, and moisture penetration from the interface can be prevented. The oxidation treatment step can be omitted if necessary. The accumulator 202c is arranged for speed adjustment with the adhesive coating process 203 of the next process.

  The adhesive coating process 203 includes an adhesive coating device 203a. In the adhesive application step 203, an adhesive is applied around the light emitting region and the periphery of the light emitting region except for the end portions of the first electrode and the second electrode lead electrode of the organic EL element sent from the oxidation treatment step 202b. Is done.

  In the sealing member bonding step 204, the organic EL element coated with the adhesive in the adhesive coating step 204 and the band-shaped sealing member 204b sent from the sealing member supply step 204a are bonded to the pressure roll 204c. Paste with.

  In the collection step 205, the band-shaped organic EL panel to which the sealing member 204b is bonded is wound up and collected in a roll shape. Reference numeral 205a denotes a rolled organic EL panel. Thereafter, the rolled organic EL panel 205a is cut into individual organic EL panels in a cutting process (not shown). The cut organic EL panel has the same configuration as the organic EL panel manufactured in FIG.

  FIG. 2B will be described. In the figure, 2b represents a manufacturing process of the organic EL element. The manufacturing process 2b includes an organic EL element supply step 201, a dry etching treatment step 202, an inorganic film forming step 206, an adhesive coating step 203, a sealing member bonding step 204, and a recovery step 205. Have. The manufacturing process shown in this figure shows a case where the inorganic film forming step 206 is performed under atmospheric pressure conditions except that it is performed under reduced pressure conditions. The difference from the manufacturing process of the organic EL element shown in FIG. 2A is that the inorganic film forming step 206 is disposed after the oxidation treatment step 202b, and all other steps are the same. The oxidation treatment step can be omitted if necessary.

  The inorganic film forming step 206 includes a vapor deposition device 206b having an evaporation source container 206a. In the inorganic film forming step 206, an inorganic film is formed under reduced pressure by the vapor deposition apparatus 206b on the image forming region of the second electrode of the organic EL element sent from the oxidation treatment step 202b. The material for forming the inorganic film is the same as the material for the inorganic film shown in FIG. The method for forming the inorganic film is the same as the method for forming the inorganic film shown in FIG. The thickness of the inorganic film is preferably 30 nm or more and 2000 nm or less in consideration of moisture permeability, gas permeability, cracking due to film stress, and the like. The accumulator 206c is disposed for speed adjustment with the adhesive coating step 203 of the next step. Other reference numerals are the same as those in FIG.

  FIG. 2C will be described. In the figure, reference numeral 2c denotes a manufacturing process of the organic EL element. The manufacturing process 2c includes an organic EL element supply step 201, a dry etching treatment step 202, an inorganic film formation step 206, an inorganic film smoothing treatment step 207, an inorganic film oxidation treatment step 208, and an adhesive coating step. 203, sealing member bonding step 204, and recovery step 205. The difference from the manufacturing process of the organic EL element shown in FIG. 2A is that after the oxidation treatment step 202b, an inorganic film formation step 206, an inorganic film dry etching treatment step (inorganic film smoothing treatment step) 207, and an inorganic film oxidation step. The processing step 208 is arranged, and all other steps are the same. The oxidation treatment step 202b and the inorganic film oxidation treatment step 208 can be omitted as necessary. The inorganic film smoothing process 207 has the same dry etching apparatus 207a as the smoothing process 202, and smoothes the surface adjacent to the upper layer of the inorganic film formed in the inorganic film forming process 206. As the dry etching apparatus 207a, the same dry etching apparatus as the dry etching apparatus 102a1 used in FIG. 1A can be used.

  The surface roughness Ra of the surface of the inorganic film after the smoothing treatment reduces the influence on the organic EL element due to stress relaxation accompanying the expansion and contraction of the adhesive, improves the adhesion between the adhesive and the inorganic film, and increases moisture from the interface. In consideration of prevention of penetration of water, etc., 30 nm or less is preferable. More preferably, it is 0.1 nm or more and 20 nm or less. The surface roughness Ra indicates a value measured by an atomic force microscope (AFM) SPA300 manufactured by SII Nano Technology. The accumulator 207b is provided for speed adjustment with the inorganic film oxidation treatment step 208 of the next step.

  In the inorganic film oxidation treatment step 208, the dry etching apparatus 208a forms an oxide film on the surface of the inorganic film after the smoothing treatment. As the dry etching apparatus 208a, the same dry etching apparatus as the dry etching apparatus 102b1 used in FIG. 1A can be used. The accumulator 208c is provided for speed adjustment with the adhesive coating step 203 of the next step.

  By forming an oxide film, the elastic modulus of the inorganic film decreases, further reducing the impact on the organic EL element by relaxing the stress accompanying the expansion and contraction of the adhesive, and improving the adhesion between the adhesive and the inorganic film The effect of preventing the penetration of moisture from the interface can be obtained. The inorganic film oxidation treatment step can be omitted if necessary. Other reference numerals are the same as those in FIGS. 2 (a) and 2 (b).

  The thickness of the adhesive layer applied in the adhesive application step shown in FIGS. 1 and 2 is preferably 1 μm or more and 200 μm or less. More preferably, it is 5 μm or more and 100 μm or less.

  FIG. 3 is a schematic view of the organic EL panel manufactured by the manufacturing process of the organic EL panel shown in FIG. FIG. 3A is a schematic perspective view of the organic EL panel. FIG. 3B is a schematic cross-sectional view along the line AA ′ in FIG. FIG.3 (c) is a schematic sectional drawing in alignment with BB 'of Fig.3 (a).

  In the figure, 3a represents an organic EL panel. The organic EL panel 3a includes a first electrode layer 302, a hole transport layer (hole injection layer) 303a, a light emitting layer 303b, an electron injection layer 303c, An organic EL element 305 having a two-electrode layer 304 and an adhesive sealing structure sealed by a sealing member 307 via an adhesive layer 306 provided around and on the surface of the organic EL element 305 is formed.

  FIG. 4 is an enlarged schematic flow chart until a portion indicated by P in FIG. 3C is formed.

  S1 shows the state of the surface 304a of the second electrode 304 of the organic EL element before being processed by the dry etching apparatus 102a in the smoothing processing step 102 shown in FIG. Reference numeral 304a1 denotes a convex portion on the surface 304a. When an adhesive is applied on the second electrode 304 in the state shown in this figure to form the adhesive layer 306, and then the sealing member 307 (see FIG. 3) is pasted, the adhesive layer 306 expands and contracts. As a result of concentration of the stress accompanying the convex portion 304a1, cracks accompanying the minute deformation of the second electrode 304, peeling from the lower layer, and the like occur, and light emitting defects and non-light emitting portions (dot-like light emitting defects, Cause of failure such as shortening of the life of the organic EL element due to moisture permeation from the interface due to insufficient adhesion between the second electrode 304 and the adhesive layer 306. Become.

  S2 shows the state of the surface 304a of the second electrode 304 of the organic EL element after being processed by the dry etching apparatus 102a in the smoothing process step 102 shown in FIG. By processing with the dry etching apparatus 102a, the convex portion 304a1 indicated by S1 is removed, and the roughness Ra of the surface 304a becomes 30 nm or less. After that, it is preferable to perform an oxidation treatment in an oxidation treatment step 102b shown in FIG.

  In S3, after the surface 304a of the second electrode 304 is brought into the state shown in S2, an adhesive is applied in the adhesive application step 104 shown in FIG. The state which bonded the sealing member by the stop member bonding process 105 is shown (corresponding to the part shown by P in FIG. 3C). As shown in this figure, by setting the surface 304a of the second electrode 304 to 30 nm or less, even when the adhesive layer 306 formed on the second electrode 304 expands and contracts, the stress accompanying the expansion and contraction is dispersed. Therefore, the influence on the second electrode 304 is mitigated. In addition, with the improvement of the adhesion at the interface between the surface 304a of the second electrode 304 and the adhesive layer 306, the penetration of moisture from the interface is prevented, and the life of the organic EL is extended.

  FIG. 5 is a schematic view of an organic EL panel manufactured by the manufacturing process of the organic EL panel shown in FIGS. 1 (b) and 1 (c). FIG. 5A shows a schematic perspective view of an organic EL panel. FIG. 5B is a schematic cross-sectional view along CC ′ of FIG. FIG.5 (c) is a schematic sectional drawing in alignment with DD 'of Fig.5 (a).

  In the figure, 3b represents an organic EL panel. The organic EL panel 3b includes a first electrode layer 302, a hole transport layer (hole injection layer) 303a, a light emitting layer 303b, an electron injection layer 303c, An organic EL element 305 having two electrode layers 304, an inorganic film 308 laminated on the second electrode layer 304, and an adhesive layer 306 provided around the organic EL element 305 and on the surface of the inorganic film 308. Thus, the contact sealing structure is sealed with the sealing member 307. The organic EL panel 3b shown in this figure has the same configuration as the organic EL panel 3a shown in FIG. 3 except that an inorganic film 308 is formed.

  FIG. 6 is an enlarged schematic flow diagram until a portion indicated by Q in FIG. 5C is formed.

  S′1 shows the state of the surface 304 a of the second electrode 304 of the organic EL element before being processed by the dry etching apparatus 102 a in the smoothing processing step 102 shown in FIG. Reference numeral 304a1 denotes a convex portion on the surface 304a.

  S′2 shows the state of the surface 304a of the second electrode 304 of the organic EL element after being processed by the dry etching apparatus 102a of the smoothing process step 102 shown in FIG. By processing with the dry etching apparatus 102a, the convex portion 304a1 indicated by S'1 is removed, and the roughness Ra of the surface 304a becomes 30 nm or less. After that, it is preferable to perform an oxidation treatment in an oxidation treatment step 103 shown in FIG.

  In S′3, after the surface 304a of the second electrode 304 is brought into the state shown in S′2, the inorganic film is formed on the second electrode 304 smoothed in the inorganic film forming step 108 shown in FIG. The state where the film 308 is formed is shown. The surface 308 a of the inorganic film 308 is a smooth surface according to the surface 304 a of the second electrode 304.

  S′4 shows a state in which the adhesive layer 306 is formed by applying an adhesive to the surface 308a of the inorganic film 308 formed in S′3 in the adhesive applying step 104 shown in FIG.

S′5 shows a state in which the sealing member 307 is bonded onto the adhesive layer 306 formed in S′4 in the sealing member bonding step 105 shown in FIG. 1B (FIG. 5C). Corresponds to the part indicated by Q)). As shown in the figure, since the surface 304a of the second electrode 304 is in a state of 50 nm or less, an inorganic film 308 is formed on the second electrode 304, and an adhesive layer formed on the inorganic film 308 is formed. The stress accompanying expansion / contraction of 306 is relieved for the following reason, and the influence on the second electrode 304 is relieved (eliminated).
1) Since the surface 308a of the inorganic film 308 is a smooth surface to some extent following the surface 304a of the second electrode 304, there are few places where stress is concentrated, so the stress propagated to the inorganic film 308 is small, and many Dispersed in the adhesive layer 306.
2) The stress propagated to the inorganic film 308 is dispersed inside the inorganic film 308 because the surface 304a of the second electrode 304 is smoothed.

  FIG. 7 is an enlarged schematic flow chart until a portion indicated by Q in FIG. 5C is formed.

  S ″ 1 indicates the state of the surface 304a of the second electrode 304 of the organic EL element before being processed by the dry etching apparatus 102a in the smoothing process step 102 shown in FIG. 1C. 304a1 is on the surface 304a. A convex part is shown.

  S ″ 2 shows the state of the surface 304a of the second electrode 304 of the organic EL element after being processed by the dry etching apparatus 102a in the smoothing process step 102 shown in FIG. 1C. Processing by the dry etching apparatus 102a As a result, the convex portion 304a1 indicated by S ″ 1 is removed, and the roughness Ra of the surface 304a becomes 30 nm or less. In addition, after that, it is preferable to perform an oxidation treatment in an oxidation treatment step 103 shown in FIG.

  In S ″ 3, after the surface 304a of the second electrode 304 is brought into the state shown in S ″ 2, the inorganic film is formed on the second electrode 304 smoothed in the inorganic film forming step 108 shown in FIG. The state where the film 308 is formed is shown.

  S ″ 4 shows a state in which the surface 308a of the inorganic film 308 shown in S ″ 3 is smoothed in the inorganic film smoothing treatment step 108 shown in FIG. 1C, and the surface roughness Ra is set to 30 nm or less. After that, it is preferable to perform an oxidation treatment in an inorganic film oxidation treatment step 109 shown in FIG.

  S ″ 5 shows a state in which the adhesive layer 306 is formed by applying an adhesive to the surface 308a of the inorganic film 308 formed in S ″ 3 in the adhesive applying step 103 shown in FIG.

  S′5 shows a state in which the sealing member 307 is bonded onto the adhesive layer 306 formed in S′4 in the sealing member bonding step 105 shown in FIG. 1C (FIG. 5C). Corresponds to the part indicated by Q)). As shown in this figure, the roughness Ra of the surface 304a of the second electrode 304 is set to 30 nm or less, and the roughness Ra of the surface 308a of the inorganic film 308 formed on the second electrode 304 is set to 30 nm or less. Therefore, the stress accompanying expansion and contraction of the adhesive layer 306 formed on the inorganic film 308 is dispersed in the adhesive layer 306 shown without being propagated to the inorganic film 308, and the influence on the second electrode 304 is mitigated. (Or disappear).

The following effect is mentioned by the manufacturing method of the organic electroluminescent panel shown in FIGS.
1. An organic EL panel that does not cause deterioration in performance of the organic EL element can be produced without limiting the adhesive and the sealing member to be used.
2. Even if an inorganic film is formed in the middle in order to improve moisture resistance, it is possible to manufacture an organic EL panel that does not cause deterioration in performance of the organic EL element, and it is also possible to manufacture a high-quality organic EL panel.
3. The use of specific adhesives and sealing members is eliminated, and a wide range of materials can be selected, thereby making it possible to reduce manufacturing costs.
4). Adhesion with the adhesive is improved, and the moisture-proof performance of the organic EL panel can be improved.

  Next, the members used for the configuration of the organic EL panel shown in FIGS. 3 and 5 manufactured by the method of manufacturing the organic EL panel of the present invention will be described.

(Sealing member)
The base material of the sealing member is not particularly limited. For example, ethylene tetrafluoroethyl copolymer (ETFE), high density polyethylene (HDPE), expanded polypropylene (OPP), polystyrene (PS), polymethyl methacrylate (PMMA), Uses thermoplastic resin film materials, glass, metal foil, etc. used for general packaging films such as stretched nylon (ONy), polyethylene terephthalate (PET), polycarbonate (PC), polyimide, polyether styrene (PES) I can do it. As these thermoplastic resin films, a multilayer film produced by coextrusion with a different film, a multilayer film produced by bonding with different stretching angles, etc. can be used as required. Further, it is naturally possible to combine the density and molecular weight distribution of the film used to obtain the required physical properties.

  In the case of a thermoplastic resin film, it is necessary to form a barrier layer by vapor deposition or coating. Examples of the barrier layer include a metal vapor deposition film and a metal foil. As inorganic vapor deposition films, thin film handbooks p879-p901 (Japan Society for the Promotion of Science), vacuum technology handbooks p502-p509, p612, p810 (Nikkan Kogyo Shimbun), vacuum handbook revised editions p132-p134 (ULVAC Japan Vacuum Technology KK) The metal vapor deposition film as described in the above. For example, metals such as In, Sn, Pb, Au, Cu, Ag, Al, Ti, and Ni are used. Moreover, as a material of the metal foil, for example, a metal material such as aluminum, copper, or nickel, or an alloy material such as stainless steel or an aluminum alloy can be used, but aluminum is preferable in terms of workability and cost. The film thickness is about 1 to 100 μm, preferably about 10 to 50 μm. In order to facilitate handling during production, a film such as polyethylene terephthalate or nylon may be laminated in advance. When a resin film is used for the flexible sealing member, it is preferable to have a thermoplastic adhesive resin layer on the side in contact with the liquid sealing agent.

  Further, a protective layer may be provided on the barrier layer. The thickness of the protective layer is preferably 100 nm to 200 μm in consideration of stress cracking resistance, electrical insulation resistance of the barrier layer, adhesiveness (adhesive force, step following ability), etc. when used as a sealing agent layer. As the protective layer, a thermoplastic resin film having a JIS K 7210 standard melt flow rate of 5 to 20 g / 10 min is preferable, and a thermoplastic resin film of 6 to 15 g / 10 min or less is more preferably used. This is because if a resin with a melt flow rate of 5 (g / 10 min) or less is used, the gap formed by the steps of the extraction electrode of each electrode cannot be completely filled, and a resin of 20 (g / 10 min) or more cannot be filled. This is because if used, the tensile strength, stress cracking resistance, workability and the like are lowered. The thermoplastic resin film is not particularly limited as long as it satisfies the above numerical values. For example, low-density polyethylene (LDPE), which is a polymer film described in Toray Research Center, Inc., a new development of functional packaging materials, HDPE, linear low density polyethylene (LLDPE), medium density polyethylene, unstretched polypropylene (CPP), OPP, ONy, PET, cellophane, polyvinyl alcohol (PVA), stretched vinylon (OV), ethylene-vinyl acetate copolymer ( EVOH), ethylene-propylene copolymer, ethylene-acrylic acid copolymer, ethylene-methacrylic acid copolymer, vinylidene chloride (PVDC), and the like can be used. Among these thermoplastic resin films, it is particularly preferable to use LDPE, LLDPE produced by using LDPE, LLDPE and a metallocene catalyst, or a film using a mixture of these films and HDPE films.

  The flexible sealing member used to form the sealing layer is a laminated film in which a barrier layer (a protective layer if necessary) is formed on the resin base material in order to facilitate handling during production. It is preferable to use it in the state. As a method for producing a laminated film, various methods generally known on the inorganic layer of a thermoplastic resin film on which an inorganic material is deposited and a thermoplastic resin film on which an aluminum foil is laminated, such as a wet laminating method and a dry laminating method. It can be made by using a method, a hot melt laminating method, an extrusion laminating method, or a thermal laminating method.

The water vapor permeability of the flexible sealing member used in the present invention is preferably 0.01 g / m ² · day or less in consideration of gas barrier properties and the like required for commercialization as an organic EL panel. The oxygen permeability is preferably 0.1 ml / m ² · day · MPa or less. The moisture permeability is a value measured mainly by the MOCON method by a method based on the JIS K7129B method (1992), and the oxygen permeability is a value measured mainly by the MOCON method by a method based on the JIS K7126B method (1987). is there. The Young's modulus of the flexible sealing member is 1 × 10 ⁻³ GPa to 80 GPa and the thickness is 10 μm to 500 μm in consideration of adhesion to the organic EL element, prevention of spreading of the liquid adhesive, and the like. preferable.

(Inorganic film)
The material for forming the inorganic film may be any material that has a function of suppressing intrusion of elements that cause deterioration of elements such as moisture and oxygen. For example, In, Sn, Pb, Au, Cu, Ag, Al, Ti, metals such as _{Ni, MgO, SiO, SiO 2,} Al 2 O 3, GeO, NiO, CaO, BaO, Fe 2 O 3, Y 2 O 3, TiO 2 or the like can be used. The thickness of the inorganic film is preferably 30 nm or more and 2000 nm or less in consideration of moisture permeability, gas permeability, film stress and the like.

(adhesive)
Examples of the adhesive according to the present invention include a liquid adhesive, a sheet adhesive, and a thermoplastic resin. Examples of the liquid adhesive include photo-curing and thermosetting sealing agents having reactive vinyl groups such as acrylic acid oligomers and methacrylic acid oligomers, moisture-curing adhesives such as 2-cyanoacrylate, epoxy-based adhesives, etc. And heat curing and chemical curing type (two-component mixing) adhesives, cationic curing type ultraviolet curing epoxy resin adhesives, and the like. It is preferable to add a filler to the liquid adhesive as necessary. The addition amount of the filler is preferably 5 to 70% by volume in consideration of adhesive strength. In addition, the size of the filler to be added is preferably 1 μm to 100 μm in consideration of the adhesive strength, the adhesive thickness after pasting and pressure bonding, and the like. The kind of filler to be added is not particularly limited, and examples thereof include soda glass, non-alkali glass, or silica, titanium dioxide, antimony oxide, titania, alumina, zirconia, tungsten oxide, and other metal oxides.

When bonding a sealing member and an organic EL element using a liquid adhesive, the bonding part 504 has bonding stability, prevention of air bubbles mixing into the bonding part, and flatness of the flexible sealing member. In view of the above, it is preferable to carry out under reduced pressure conditions of 10 to 1 × 10 ⁻⁵ Pa.

  The sheet-like adhesive refers to an adhesive that is non-flowable at room temperature (about 25 ° C.) and exhibits fluidity in the range of 50 ° C. to 100 ° C. when heated and is formed into a sheet shape. As an adhesive to be used, for example, a photocurable resin mainly composed of a compound having an ethylenic double bond at the terminal or side chain of a molecule and a photopolymerization initiator can be mentioned. In use, for example, it is preferable to use it at a normal temperature (about 25 ° C.) or less by pasting it on the sealing member side in advance.

  As the thermoplastic resin, a thermoplastic resin having a melt flow rate of JIS K 7210 specified in a range of 5 to 20 g / 10 min is preferable, and a thermoplastic resin of 6 to 15 g / 10 min or less is more preferably used. This is because if a resin with a melt flow rate of 5 (g / 10 min) or less is used, the gap formed by the steps of the extraction electrode of each electrode cannot be completely filled, and a resin of 20 (g / 10 min) or more cannot be filled. This is because if used, the tensile strength, stress cracking resistance, workability and the like are lowered. These thermoplastic resins are preferably formed into a film and bonded to a flexible sealing member (a strip-shaped flexible sealing member or a single-sheet flexible sealing member). The laminating method can be made by using various generally known methods such as a wet laminating method, a dry laminating method, a hot melt laminating method, an extrusion laminating method, and a thermal laminating method.

  The thermoplastic resin is not particularly limited as long as it satisfies the above numerical values. For example, low density polyethylene (LDPE) which is a polymer film described in the new development of functional packaging materials (Toray Research Center, Inc.). ), HDPE, linear low density polyethylene (LLDPE), medium density polyethylene, unstretched polypropylene (CPP), OPP, ONy, PET, cellophane, polyvinyl alcohol (PVA), stretched vinylon (OV), ethylene-vinyl acetate copolymer A combination (EVOH), ethylene-propylene copolymer, ethylene-acrylic acid copolymer, ethylene-methacrylic acid copolymer, vinylidene chloride (PVDC), or the like can be used. Among these thermoplastic resins, LDPE, LLDPE produced using LDPE, LLDPE and a metallocene catalyst, or a thermoplastic resin using a mixture of LDPE, LLDPE and HDPE films is preferably used.

(Base material of organic EL element)
As a base material, a sheet-like sheet-like board | substrate and a strip | belt-shaped flexible board | substrate are mentioned. Examples of the sheet-like base material include a transparent glass plate and a sheet-like transparent resin film. Examples of the resin film include polyesters such as polyethylene terephthalate (PET) and polyethylene naphthalate (PEN), polyethylene, polypropylene, cellophane, cellulose diacetate, cellulose triacetate, cellulose acetate butyrate, cellulose acetate propionate (CAP), Cellulose esters such as cellulose acetate phthalate (TAC) and cellulose nitrate or derivatives thereof, polyvinylidene chloride, polyvinyl alcohol, polyethylene vinyl alcohol, syndiotactic polystyrene, polycarbonate, norbornene resin, polymethylpentene, polyether ketone, polyimide , Polyethersulfone (PES), polyphenylene sulfide, polysulfones, poly Cycloolefin resins such as ether imide, polyether ketone imide, polyamide, fluororesin, nylon, polymethyl methacrylate, acrylic or polyarylate, Arton (trade name, manufactured by JSR) or Apel (trade name, manufactured by Mitsui Chemicals) Can be mentioned. A transparent resin film is mentioned as a strip | belt-shaped flexible base material, The same resin film as a sheet-fed sheet-like base material can be used.

When using a transparent resin film as a substrate, a gas barrier film is preferably formed on the surface of the resin film as necessary. Examples of the gas barrier film include an inorganic film, an organic film, or a hybrid film of both. As a characteristic of the gas barrier film, it is preferable that the water vapor permeability is 0.01 g / m ² · day or less. Furthermore, a high barrier film having an oxygen permeability of 0.1 ml / m ² · day · MPa or less and a water vapor permeability of 10 ⁻⁵ g / m ² · day or less is preferable.

  As a material for forming the barrier film, any material may be used as long as it has a function of suppressing intrusion of elements that cause deterioration of elements such as moisture and oxygen. For example, silicon oxide, silicon dioxide, silicon nitride, or the like can be used. Further, in order to improve the brittleness of the film, it is more preferable to have a laminated structure of these inorganic layers and layers made of organic materials. Although there is no restriction | limiting in particular about the lamination | stacking order of an inorganic layer and an organic layer, It is preferable to laminate | stack both alternately several times. The method for forming the barrier film is not particularly limited, and for example, vacuum deposition, sputtering, reactive sputtering, molecular beam epitaxy, cluster ion beam, ion plating, plasma polymerization, atmospheric pressure plasma polymerization A plasma CVD method, a laser CVD method, a thermal CVD method, a coating method, or the like can be used, but an atmospheric pressure plasma polymerization method as described in JP-A-2004-68143 is particularly preferable.

(electrode)
In the case of an organic EL panel, since the anode (first electrode) side is usually the observation side, an electrode having a high light transmittance is used as the first electrode. As the first electrode, an electrode material made of a metal, an alloy, an electrically conductive compound, or a mixture thereof having a high work function (4 eV or more) is preferably used. Specific examples of such an electrode substance include metals such as Au, and conductive transparent materials such as CuI, indium tin oxide (ITO), SnO ₂ , and ZnO. Alternatively, an amorphous material such as IDIXO (In ₂ O ₃ .ZnO) capable of forming a transparent conductive film may be used. For the anode, these electrode materials may be formed into a thin film by a method such as vapor deposition or sputtering, and a pattern having a desired shape may be formed by a photolithography method, or when the pattern accuracy is not required (about 100 μm or more) ), A pattern may be formed through a mask having a desired shape when the electrode material is deposited or sputtered. When light emission is taken out from the anode, it is desirable that the transmittance is greater than 10%, and the sheet resistance as the anode is preferably several hundred Ω / □ or less. Further, although the film thickness depends on the material, it is usually selected in the range of 10 to 1000 nm, preferably 10 to 200 nm.

As the second electrode, a material having a work function (4 eV or less) metal (referred to as an electron injecting metal), an alloy, an electrically conductive compound, and a mixture thereof as an electrode material is used. Specific examples of such electrode materials include 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 ) Mixtures, indium, lithium / aluminum mixtures, rare earth metals and the like. Among these, from the point of durability against electron injection and oxidation, etc., a mixture of an electron injecting metal and a second metal which is a stable metal having a larger work function than this, for example, a magnesium / silver mixture, Suitable are a magnesium / aluminum mixture, a magnesium / indium mixture, an aluminum / aluminum oxide (Al ₂ O ₃ ) mixture, a lithium / aluminum mixture, aluminum and the like. The cathode can be produced by forming a thin film of these electrode materials by a method such as vapor deposition or sputtering. The sheet resistance as the cathode is preferably several hundred Ω / □ or less, and the film thickness is usually selected in the range of 10 nm to 5 μm, preferably 50 to 200 nm. In order to transmit the emitted light, if either one of the first electrode (anode) or the second electrode (cathode) of the organic EL element is transparent or translucent, the emission luminance is advantageously improved.

  Moreover, after producing the metal with a thickness of 1 to 20 nm on the second electrode, the conductive transparent material mentioned in the description of the first electrode is produced thereon, so that a transparent or translucent second electrode ( A cathode) can be manufactured, and by applying this, an element in which both the first electrode (anode) and the second electrode (cathode) are transmissive can be manufactured.

(Organic compound layer including light emitting layer)
The following structure is mentioned as a layer structure of the organic compound layer containing the light emitting layer of the organic electroluminescent panel shown by FIG.3 and FIG.5.

(1) Hole transport layer (hole injection layer) / light emitting layer / electron injection layer (2) Light emitting layer / electron transport layer (3) Hole transport layer / light emitting layer / hole blocking layer / electron transport layer (4) ) Hole transport layer (hole injection layer) / light emitting layer / hole blocking layer / electron transport layer / cathode buffer layer (electron injection layer)
(5) Anode buffer layer (hole injection layer) / hole transport layer / light emitting layer / hole blocking layer / electron transport layer / cathode buffer layer (electron injection layer)
Hereinafter, the hole transport layer, the light emitting layer, and the electron injection layer will be described.

(Hole transport layer)
A hole injection layer (anode buffer layer) may be present between the first electrode and the light emitting layer or the hole transport layer. The hole injection layer is a layer provided between the electrode and the organic layer in order to lower the driving voltage and improve the luminance of light emission. “The organic EL element and the forefront of industrialization (November 30, 1998, NTS) The details are described in the second volume, Chapter 2, “Electrode Materials” (pages 123 to 166) of “The Company”. Examples of the material used for the anode buffer layer (hole injection layer) include materials described in JP-A No. 2000-160328.

  The hole transport layer is made of a hole transport material having a function of transporting holes, and in a broad sense, a hole injection layer and an electron blocking layer are also included in the hole transport layer. The hole transport layer can be provided as a single layer or a plurality of layers. The hole transport material has any one of hole injection or transport and electron barrier properties, and may be either organic or inorganic. For example, triazole derivatives, oxadiazole derivatives, imidazole derivatives, polyarylalkane derivatives, pyrazoline derivatives and pyrazolone derivatives, phenylenediamine derivatives, arylamine derivatives, amino-substituted chalcone derivatives, oxazole derivatives, styrylanthracene derivatives, fluorenone derivatives, hydrazone derivatives, Examples include stilbene derivatives, silazane derivatives, aniline copolymers, and conductive polymer oligomers, particularly thiophene oligomers.

  The above-mentioned materials can be used as the hole transport material, but it is preferable to use a porphyrin compound, an aromatic tertiary amine compound and a styrylamine compound, particularly an aromatic tertiary amine compound. Representative examples of aromatic tertiary amine compounds and styrylamine compounds include N, N, N ', N'-tetraphenyl-4,4'-diaminophenyl; N, N'-diphenyl-N, N'- Bis (3-methylphenyl)-[1,1′-biphenyl] -4,4′-diamine (TPD); 2,2-bis (4-di-p-tolylaminophenyl) propane; 1,1-bis (4-di-p-tolylaminophenyl) cyclohexane; N, N, N ′, N′-tetra-p-tolyl-4,4′-diaminobiphenyl; 1,1-bis (4-di-p-tolyl) Aminophenyl) -4-phenylcyclohexane; bis (4-dimethylamino-2-methylphenyl) phenylmethane; bis (4-di-p-tolylaminophenyl) phenylmethane; N, N'-diphenyl-N, N ' − (4-methoxyphenyl) -4,4'-diaminobiphenyl; N, N, N ', N'-tetraphenyl-4,4'-diaminodiphenyl ether; 4,4'-bis (diphenylamino) quadriphenyl; N, N, N-tri (p-tolyl) amine; 4- (di-p-tolylamino) -4 '-[4- (di-p-tolylamino) styryl] stilbene; 4-N, N-diphenylamino- (2-diphenylvinyl) benzene; 3-methoxy-4′-N, N-diphenylaminostilbenzene; N-phenylcarbazole, and also two of those described in US Pat. No. 5,061,569. Having a condensed aromatic ring in the molecule, for example, 4,4'-bis [N- (1-naphthyl) -N-phenylamino] biphenyl (NPD), JP-A-4-3086 4,4 ', 4 "-tris [N- (3-methylphenyl) -N-phenylamino] triphenylamine in which three triphenylamine units described in Japanese Patent No. 8 are linked in a starburst type ( MTDATA) and the like.

  Furthermore, a polymer material in which these materials are introduced into a polymer chain or these materials are used as a polymer main chain can also be used. In addition, inorganic compounds such as p-type-Si and p-type-SiC can also be used as the hole injection material and the hole transport material.

  JP-A-11-251067, J. Org. Huang et. al. A so-called p-type hole transport material described in a book (Applied Physics Letters 80 (2002), p. 139) can also be used. In the present invention, it is preferable to use these materials because a light-emitting element with higher efficiency can be obtained.

  Although there is no restriction | limiting in particular about the film thickness of a positive hole transport layer, Usually, 5 nm-about 5 micrometers, Preferably it is 5-200 nm. This hole transport layer may have a single layer structure composed of one or more of the above materials. A hole transport layer having a high p property doped with impurities can also be used. Examples thereof include JP-A-4-297076, JP-A-2000-196140, JP-A-2001-102175, J.A. Appl. Phys. 95, 5773 (2004), and the like. It is preferable to use such a hole transport layer having a high p property because an organic EL element with lower power consumption can be produced.

(Light emitting layer)
In the present invention, the light emitting layer refers to a blue light emitting layer, a green light emitting layer, and a red light emitting layer. There is no restriction | limiting in particular as a lamination order in the case of laminating | stacking a light emitting layer, You may have a nonluminous intermediate | middle layer between each light emitting layer. In the present invention, it is preferable that at least one blue light emitting layer is provided at a position closest to the anode among all the light emitting layers. Also, when four or more light emitting layers are provided, for example, blue light emitting layer / green light emitting layer / red light emitting layer / blue light emitting layer, blue light emitting layer / green light emitting layer / red light emitting layer / blue light emitting from the order close to the anode. Layered / green light emitting layer, blue light emitting layer / green light emitting layer / red light emitting layer / blue light emitting layer / green light emitting layer / red light emitting layer, etc. It is preferable for improving luminance stability. A white element can be manufactured by forming a light emitting layer in multiple layers.

  The total thickness of the light emitting layer is not particularly limited, but is usually selected in the range of 2 nm to 5 μm, preferably 2 to 200 nm in consideration of the uniformity of the film and the voltage required for light emission. Furthermore, it is preferable that it exists in the range of 10-20 nm. A film thickness of 20 nm or less is preferable because it has the effect of improving the stability of the emission color with respect to the driving current as well as the voltage surface. The film thickness of each light emitting layer is preferably selected in the range of 2 to 100 nm, and more preferably in the range of 2 to 20 nm. Although there is no restriction | limiting in particular about the film thickness relationship of each light emitting layer of blue, green, and red, It is preferable that the blue light emitting layer (the sum total when there are two or more layers) is the thickest among three light emitting layers.

  The light emitting layer includes at least three layers having different emission spectra, each having an emission maximum wavelength in the range of 430 to 480 nm, 510 to 550 nm, and 600 to 640 nm. If it is three or more layers, there will be no restriction | limiting in particular. When there are more than four layers, there may be a plurality of layers having the same emission spectrum. A layer having an emission maximum wavelength in the range of 430 to 480 nm is referred to as a blue light emitting layer, a layer in the range of 510 to 550 nm is referred to as a green light emitting layer, and a layer in the range of 600 to 640 nm is referred to as a red light emitting layer. Moreover, in the range which maintains the said maximum wavelength, you may mix a several luminescent compound in each light emitting layer. For example, the blue light emitting layer may be used by mixing a blue light emitting compound having a maximum wavelength of 430 to 480 nm and a green light emitting compound having the same wavelength of 510 to 550 nm.

  The organic light emitting material used as the material of the light emitting layer is (a) charge injection function, that is, holes can be injected from the anode or hole injection layer when an electric field is applied, and electrons are injected from the cathode or electron injection layer. (B) a transport function, that is, a function that moves injected holes and electrons by the force of an electric field, and (c) a light emission function, that is, a recombination field of electrons and holes. However, there is no particular limitation as long as it has the three functions of connecting these to light emission. For example, fluorescent whitening agents such as benzothiazole, benzimidazole, and benzoxazole, and styrylbenzene compounds can be used. Specific examples of the above-mentioned optical brightener include 2,5-bis (5,7-di-t-pentyl-2-benzoxazolyl) -1,3,4-thiadiazole in the benzoxazole series, 4 , 4'-bis (5,7-t-pentyl-2-benzoxazolyl) stilbene, 4,4'-bis [5,7-di- (2-methyl-2-butyl) -2-benzoxa Zoolyl] stilbene, 2,5-bis (5,7-di-t-pentyl-2-benzoxazolyl) thiophene, 2,5-bis [5-α, α-dimethylbenzyl-2-benzoxazoli Ru] thiophene, 2,5-bis [5,7-di- (2-methyl-2-butyl) -2-benzoxazolyl] -3,4-diphenylthiophene, 2,5-bis (5-methyl) -2-benzoxazolyl) thiophene, 4,4'-bis (2 -Benzoxazolyl) biphenyl, 5-methyl-2- [2- [4- (5-methyl-2-benzoxazolyl) phenyl] vinyl] benzoxazole, 2- [2- (4-chlorophenyl) vinyl Naphtho [1,2-d] oxazole and the like. Examples of the benzothiazole type include 2,2 '-(p-phenylenedivinylene) -bisbenzothiazole, and examples of the benzimidazole type include 2- [2- [4- (2-benzimidazolyl) phenyl] vinyl] benzimidazole. 2- [2- (4-carboxyphenyl) vinyl] benzimidazole and the like. In addition, other useful compounds are listed in Chemistry of Synthetic Soybean (1971), pages 628-637 and 640.

  Specific examples of the styrylbenzene compound include 1,4-bis (2-methylstyryl) benzene, 1,4-bis (3-methylstyryl) benzene, 1,4-bis (4-methylstyryl). ) Benzene, distyrylbenzene, 1,4-bis (2-ethylstyryl) benzene, 1,4-bis (3-methylstyryl) benzene, 1,4-bis (2-methylstyryl) -2-methylbenzene, 1,4-bis (2-methylstyryl) -2-ethylbenzene and the like can be mentioned.

  Further, in addition to the above-described optical brightener and styrylbenzene compound, for example, 12-phthaloperinone, 1,4-diphenyl-1,3-butadiene, 1,1,4,4-tetraphenyl-1,3- Butadiene, naphthalimide derivatives, perylene derivatives, oxadiazole derivatives, aldazine derivatives, pyrazirine derivatives, cyclopentadiene derivatives, pyrrolopyrrole derivatives, styrylamine derivatives, coumarin compounds, international publications WO 90/13148 and Appl. Phys. Lett. , Vol 58, 18, P1982 (1991), and aromatic dimethylidin compounds. Specific examples of the aromatic dimethylidin compounds include 1,4-phenylene dimethylidin, 4,4'-phenylene dimethylidin, 2,5-xylylene dimethylidin, 2,6-naphthylene dimethylidin, 1,4-biphenylenedimethylidin, 1,4-p-terephenylenedimethylidin, 4,4'-bis (2,2-di-t-butylphenylvinyl) biphenyl, 4,4'-bis (2 , 2-diphenylvinyl) biphenyl and the like, and derivatives thereof. Specific examples of the compound represented by the general formula (I) include bis (2-methyl-8-quinolinolato) (p-phenylphenolate) aluminum (III), bis (2-methyl-8-quinolinolato). ) (1-naphtholate) aluminum (III) and the like.

  In addition, a compound in which the above-described organic light-emitting material is used as a host and the host is doped with a strong fluorescent dye from blue to green, for example, coumarin-based or the same fluorescent dye as the host, is also suitable as the organic light-emitting material. When the above-described compound is used as the organic light-emitting material, blue to green light emission (the emission color varies depending on the type of dopant) can be obtained with high efficiency. Specific examples of the host that is the material of the compound include organic light-emitting materials having a distyrylarylene skeleton (particularly preferably, for example, 4,4′-bis (2,2-diphenylvinyl) biphenyl). Specific examples of the dopant which is a material of diphenylaminovinylarylene (particularly preferably, for example, N, N-diphenylaminobiphenylbenzene and 4,4′-bis [2- [4- (N, N-di- -P-tolyl) phenyl] vinyl] biphenyl).

  The light emitting layer preferably contains a known host compound and a known phosphorescent compound (also referred to as a phosphorescent compound) in order to increase the light emission efficiency of the light emitting layer.

  The host compound is a compound contained in the light-emitting layer, the mass ratio in the layer is 20% or more, and the phosphorescence quantum yield of phosphorescence emission is 0.1 at room temperature (25 ° C.). Is defined as less than a compound. The phosphorescence quantum yield is preferably less than 0.01. A plurality of host compounds may be used in combination. By using a plurality of types of host compounds, it is possible to adjust the movement of charges, and the organic EL element can be made highly efficient. In addition, by using a plurality of phosphorescent compounds, it is possible to mix different light emission, thereby obtaining an arbitrary emission color. White light emission is possible by adjusting the kind of phosphorescent compound and the amount of doping, and can also be applied to illumination and backlight.

  As these host compounds, compounds having a hole transporting ability and an electron transporting ability, preventing emission light from being increased in wavelength, and having a high Tg (glass transition temperature) are preferable. Known host compounds include, for example, JP-A Nos. 2001-257076, 2002-308855, 2001-313179, 2002-319491, 2001-357777, and 2002-334786. Gazette, 2002-8860, 2002-334787, 2002-15871, 2002-334788, 2002-43056, 2002-334789, 2002-75645 2002-338579, 2002-105445, 2002-343568, 2002-141173, 2002-352957, 2002-203683, 2002-363227 2002-231453, 2003-3165, 2002-234888, 2003-27048, 2002-255934, 2002-260861, 2002-280183, Examples thereof include compounds described in 2002-299060, 2002-302516, 2002-305083, 2002-305084, 2002-308837 and the like.

  In the case of having a plurality of light emitting layers, it is preferable that 50% by mass or more of the host compound in each layer is the same compound because it is easy to obtain a uniform film property over the entire organic layer. It is more preferable that the light emission energy is 2.9 eV or more because it is advantageous in efficiently suppressing energy transfer from the dopant and obtaining high luminance. Phosphorescence emission energy means the peak energy of the 0-0 band of phosphorescence emission when the photoluminescence of a deposited film of 100 nm is measured on a substrate with a host compound.

  The host compound has a phosphorescence emission energy of 2.9 eV or more and a Tg of 90 ° C. or more in consideration of deterioration of the organic EL device over time (decrease in luminance and film properties), market needs as a light source, and the like. Preferably there is. That is, in order to satisfy both luminance and durability, it is preferable that phosphorescence emission energy is 2.9 eV or more and Tg is 90 ° C. or more. Tg is more preferably 100 ° C. or higher.

  A phosphorescent compound (phosphorescent compound) is a compound in which light emission from an excited triplet is observed, is a compound that emits phosphorescence at room temperature (25 ° C.), and has a phosphorescence quantum yield of 25. The compound is 0.01 or more at ° C. When used in combination with the host compound described above, an organic EL device with higher luminous efficiency can be obtained.

  The phosphorescent compound according to the present invention preferably has a phosphorescence quantum yield of 0.1 or more. The phosphorescent quantum yield can be measured by the method described in Spectroscopic II, page 398 (1992 version, Maruzen) of Experimental Chemistry Course 4 of the 4th edition. Although the phosphorescence quantum yield in a solution can be measured using various solvents, the phosphorescence quantum yield used in the present invention only needs to achieve the phosphorescence quantum yield in any solvent.

  There are two types of light emission of the phosphorescent compound in principle. One is the recombination of the carrier on the host compound to which the carrier is transported to generate an excited state of the host compound, and this energy is transferred to the phosphorescent compound. The energy transfer type is to obtain light emission from the phosphorescent compound by moving to the other, and the other is that the phosphorescent compound becomes a carrier trap, and carrier recombination occurs on the phosphorescent compound, and the phosphorescent compound emits light. Although it is a carrier trap type in which light emission can be obtained, in any case, it is a condition that the excited state energy of the phosphorescent compound is lower than the excited state energy of the host compound.

  The phosphorescent compound can be appropriately selected from known compounds used for the light emitting layer of the organic EL device. The phosphorescent compound is preferably a complex compound containing a group 8-10 metal in the periodic table of elements, more preferably an iridium compound, an osmium compound, or a platinum compound (platinum complex compound), rare earth Of these, iridium compounds are the most preferred.

  In the present invention, the phosphorescence emission maximum wavelength of the phosphorescent compound is not particularly limited, and can be obtained in principle by selecting a central metal, a ligand, a ligand substituent, and the like. The emission wavelength can be changed.

  The light emission color of the organic EL device of the present invention and the compound according to the present invention is shown in FIG. 4.16 on page 108 of “New Color Science Handbook” (edited by the Japan Color Society, University of Tokyo Press, 1985). It is determined by the color when the result measured with the total CS-1000 (manufactured by Konica Minolta Sensing) is applied to the CIE chromaticity coordinates.

The white element referred to in the present invention means that when the front luminance at 2 ° viewing angle is measured by the above method, the chromaticity in the CIE1931 color system at 1000 cd / m ² is X = 0.33 ± 0.07, It is in the region of Y = 0.33 ± 0.07.

(Electron injection layer)
The electron injection layer is made of a material having a function of transporting electrons and is included in the electron transport layer in a broad sense. The electron injection layer is a layer provided between the electrode and the organic layer for lowering the driving voltage and improving the luminance of the light emission. “Organic EL element and its forefront of industrialization (NST 30, November 30, 1998) Issue) ”, Chapter 2, Chapter 2,“ Electrode Materials ”(pages 123-166). The details of the electron injection layer (cathode buffer layer) are also described in JP-A-6-325871, JP-A-9-17574, JP-A-10-74586, and the like. Specifically, strontium, aluminum, etc. Metal buffer layer typified by lithium, alkali metal compound buffer layer typified by lithium fluoride, alkaline earth metal compound buffer layer typified by magnesium fluoride, oxide buffer layer typified by aluminum oxide, etc. . The buffer layer (injection layer) is preferably a very thin film, and the film thickness is preferably in the range of 0.1 nm to 5 μm although it depends on the material.

  In addition, as an electron transport material (also serving as a hole blocking material) used for the electron transport layer adjacent to the light emitting layer side, it is sufficient if it has a function of transmitting electrons injected from the cathode to the light emitting layer. As a material, any one of conventionally known compounds can be selected and used. For example, nitro-substituted fluorene derivatives, diphenylquinone derivatives, thiopyran dioxide derivatives, carbodiimides, fluorenylidenemethane derivatives, anthraquinodisides. Examples include methane and anthrone derivatives, oxadiazole derivatives and the like. Furthermore, in the above oxadiazole derivatives, thiadiazole derivatives in which the oxygen atom of the oxadiazole ring is substituted with a sulfur atom, and quinoxaline derivatives having a quinoxaline ring known as an electron-withdrawing group can also be used as the electron transport material. Furthermore, a polymer material in which these materials are introduced into a polymer chain or these materials are used as a polymer main chain can also be used.

  Also, metal complexes of 8-quinolinol derivatives such as tris (8-quinolinol) aluminum (Alq), tris (5,7-dichloro-8-quinolinol) aluminum, tris (5,7-dibromo-8-quinolinol) aluminum. Tris (2-methyl-8-quinolinol) aluminum, tris (5-methyl-8-quinolinol) aluminum, bis (8-quinolinol) zinc (Znq), and the like, and the central metals of these metal complexes are In, Mg, Metal complexes replaced with Cu, Ca, Sn, Ga or Pb can also be used as the electron transport material. In addition, metal-free or metal phthalocyanine, or those having terminal ends substituted with an alkyl group or a sulfonic acid group can be preferably used as the electron transporting material. Distyrylpyrazine derivatives can also be used as electron transport materials, and inorganic semiconductors such as n-type-Si and n-type-SiC are also used as electron transport materials in the same manner as the hole injection layer and hole transport layer. I can do it. Although there is no restriction | limiting in particular about the film thickness of an electron carrying layer, Usually, 5 nm-about 5 micrometers, Preferably it is 5-200 nm. The electron transport layer may have a single layer structure composed of one or more of the above materials.

  An electron transport layer having a high n property doped with impurities can also be used. Examples thereof include JP-A-4-297076, JP-A-10-270172, JP-A-2000-196140, JP-A-2001-102175, J. Pat. Appl. Phys. 95, 5773 (2004), and the like. It is preferable to use such an electron transport layer having a high n property because an element with lower power consumption can be manufactured.

  The external extraction efficiency at room temperature of light emission of the organic EL device according to the present invention is preferably 1% or more, more preferably 5% or more. Here, the external extraction quantum efficiency (%) = the number of photons emitted to the outside of the organic EL element / the number of electrons sent to the organic EL element × 100.

  In addition, a hue improvement filter such as a color filter may be used in combination, or a color conversion filter that converts the emission color from the organic EL element into multiple colors using a phosphor may be used in combination. In the case of using a color conversion filter, the λmax of light emission of the organic EL element is preferably 480 nm or less.

(Other)
The organic EL device according to the present invention is preferably used in combination with the following method in order to efficiently extract light generated in the light emitting layer. The organic EL element emits light inside a layer having a refractive index higher than that of air (refractive index is about 1.7 to 2.1), and only about 15% to 20% of the light generated in the light emitting layer can be extracted. It is generally said that there is no. This is because the light incident on the interface (interface between the transparent substrate and air) at an angle θ greater than the critical angle causes total reflection and cannot be taken out of the element, or the transparent electrode or light emitting layer and the transparent substrate This is because the light undergoes total reflection between them, the light is guided through the transparent electrode or the light emitting layer, and as a result, the light escapes in the direction of the side surface of the device.

  As a method for improving the light extraction efficiency, for example, a method of forming irregularities on the surface of the transparent substrate to prevent total reflection at the interface between the transparent substrate and the air (US Pat. No. 4,774,435). A method for improving efficiency by providing a substrate with a light condensing property (JP-A-63-314795). A method of forming a reflective surface on the side surface of an element (Japanese Patent Laid-Open No. 1-220394). A method of forming an antireflection film by introducing a flat layer having an intermediate refractive index between a substrate and a light emitter (Japanese Patent Laid-Open No. 62-172691). A method of introducing a flat layer having a lower refractive index than the substrate between the substrate and the light emitter (Japanese Patent Laid-Open No. 2001-202827). There is a method of forming a diffraction grating between any one of the substrate, the transparent electrode layer, and the light emitting layer (including between the substrate and the outside) (Japanese Patent Laid-Open No. 11-283951).

  In the present invention, these methods can be used in combination with an organic EL element. However, a method of introducing a flat layer having a lower refractive index than the substrate between the substrate and the light emitter, or a substrate, a transparent electrode layer, A method of forming a diffraction grating between any layers of the light emitting layer (including between the substrate and the outside) can be suitably used. In the present invention, by combining these means, it is possible to obtain an element having higher luminance or durability.

  When a low refractive index medium is formed between the transparent electrode and the transparent substrate with a thickness longer than the wavelength of light, the light extracted from the transparent electrode has a higher extraction efficiency to the outside as the refractive index of the medium is lower. . Examples of the low refractive index layer include aerogel, porous silica, magnesium fluoride, and a fluorine-based polymer. Since the refractive index of the transparent substrate is generally about 1.5 to 1.7, the low refractive index layer preferably has a refractive index of about 1.5 or less. Further, it is preferably 1.35 or less. The thickness of the low refractive index medium is preferably at least twice the wavelength in the medium. This is because the effect of the low refractive index layer is diminished when the thickness of the low refractive index medium is about the wavelength of light and the electromagnetic wave that has exuded by evanescent enters the substrate. The method of introducing a diffraction grating into an interface or any medium that causes total reflection is characterized by a high effect of improving light extraction efficiency. This method is generated from the light emitting layer by utilizing the property that the diffraction grating can change the direction of light to a specific direction different from refraction by so-called Bragg diffraction such as first-order diffraction and second-order diffraction. Of the light, the light that cannot go out due to total reflection between layers, etc. is diffracted by introducing a diffraction grating into any layer or medium (inside a transparent substrate or transparent electrode) , Trying to extract light out. The introduced diffraction grating desirably has a two-dimensional periodic refractive index. This is because light emitted from the light-emitting layer is randomly generated in all directions, so in a general one-dimensional diffraction grating having a periodic refractive index distribution only in a certain direction, only light traveling in a specific direction is diffracted. The light extraction efficiency does not increase so much. However, by making the refractive index distribution a two-dimensional distribution, light traveling in all directions is diffracted, and light extraction efficiency is increased.

  As described above, the position where the diffraction grating is introduced may be in any of the layers or in the medium (in the transparent substrate or the transparent electrode), but is preferably in the vicinity of the organic light emitting layer where light is generated. At this time, the period of the diffraction grating is preferably about 1/2 to 3 times the wavelength of light in the medium. The arrangement of the diffraction grating is preferably two-dimensionally repeated, such as a square lattice, a triangular lattice, or a honeycomb lattice.

  Furthermore, the organic EL device according to the present invention can be processed to provide, for example, a structure on a microlens array on the light extraction side of the substrate in order to efficiently extract the light generated in the light emitting layer, or so-called collection. By combining with the light sheet, the luminance in the specific direction can be increased by condensing light in a specific direction, for example, the front direction with respect to the element light emitting surface. As an example of the microlens array, quadrangular pyramids having a side of 30 μm and an apex angle of 90 degrees are two-dimensionally arranged on the light extraction side of the substrate. One side is preferably 10 μm to 100 μm. If it becomes smaller than this, the effect of diffraction will generate | occur | produce and color, and if too large, thickness will become thick and is not preferable.

  As the condensing sheet, for example, a sheet that is put into practical use in an LED backlight of a liquid crystal display device can be used. As such a sheet, for example, a brightness enhancement film (BEF) manufactured by Sumitomo 3M Limited can be used. As the shape of the prism sheet, for example, the substrate may be formed with a triangle stripe having a vertex angle of 90 degrees and a pitch of 50 μm, or the vertex angle is rounded, and the pitch is randomly changed. The shape may be other shapes. Moreover, in order to control the light emission angle from a light emitting element, you may use a light-diffusion plate and a film together with a condensing sheet. For example, a diffusion film (light-up) manufactured by Kimoto Co., Ltd. can be used.

  Hereinafter, although an example is given and the concrete effect of the present invention is shown, the mode of the present invention is not limited to this.

Example 1
(Production of organic EL element)
An organic EL device in which the first electrode, the hole transport layer, the light emitting layer, the electron transport layer, and the second electrode were formed on the substrate in this order by the method described below was produced.

(Preparation of substrate)
A soda-lime glass having a thickness of 1.1 mm, a width of 40 mm, and a length of 60 mm was prepared as a substrate. In addition, the surface of the soda-lime glass used was a silica-coated glass for protection from acid and alkali.

(Formation of the first electrode)
The prepared glass substrate was cleaned by irradiation at a distance of 12 mm with an irradiation intensity of 15 mW / cm ² using a low-pressure mercury lamp having a wavelength of 184.2 nm. Then, using a vapor deposition apparatus, using indium tin oxide (ITO) under a vacuum of 5 × 10 ⁻⁴ Pa, the deposited film formation region (first electrode formation region) of the prepared glass substrate As shown in FIG. 1, a patterned first electrode having a width of 2 mm, a length of 50 mm, an interval of 2 mm, a thickness of 150 nm, and 10 rows was formed.

(Formation of hole transport layer)
N, N′-diphenyl-N is used as a material for forming a hole transport layer in a vapor transport layer forming vapor deposition apparatus under a vacuum of 5 × 10 ⁻⁴ Pa using a glass substrate on which a first electrode is formed. , N′-m-tolyl 4,4′-diamino-1,1′-biphenyl is deposited on the first electrode except for one end of the first electrode formed on the glass substrate. Vapor phase deposition).

(Formation of light emitting layer)
Each glass substrate on which a hole transport layer is formed is used, and Alq ₃ is used as a light emitting layer forming material in a region where the hole transport layer is formed, and light is emitted under a vacuum of 5 × 10 ⁻⁴ Pa. Vapor deposition was performed with a layer-forming vapor deposition apparatus.

(Formation of electron transport layer)
Using a glass substrate on which a light emitting layer is formed, using LiF as a material for forming an electron transport layer in a region where a hole transport layer is formed including the light emitting layer, under a vacuum of 5 × 10 ⁻⁴ Pa LiF was deposited using an electron transport layer forming vapor deposition apparatus.

(Formation of second electrode)
Using a glass substrate on which an electron transport layer is formed, using Al as a second electrode forming material on the electron transport layer in a direction perpendicular to the first electrode as shown in FIG. 1, 5 × 10 ⁻ Al was vapor-deposited with a vapor deposition apparatus under a vacuum of ⁴ Pa. The formed second electrode had a width of 2 mm, a length of 35 mm, an interval of 2 mm, a thickness of 150 nm, and a 7-row pattern.

(Production of organic EL panel)
An organic EL panel was produced according to the manufacturing process shown in FIG.

(Second electrode surface smoothing treatment)
An organic EL element was prepared by changing the surface roughness Ra of the prepared organic EL element on the side to which the sealing member for the second electrode sealing member was bonded as shown in Table 1 by the following smoothing treatment. 1-1 to 1-7. An organic EL element that is not subjected to a smoothing treatment was prepared as a comparative sample. 1-8.

  A reactive ion etching apparatus was used as the smoothing process, and the second electrode was processed to a desired surface roughness by changing the radio frequency power (RF) power, the introduced gas type, the introduced gas amount, and the pressure in the chamber.

  The surface roughness Ra indicates a value measured by an atomic force microscope (AFM) SPA300 manufactured by SII Nano Technology.

In the table, RF power indicates high-frequency power supply power. Ar represents argon gas, and Cl ₂ represents chlorine gas.

(Applying adhesive)
The prepared organic EL element No. A thermosetting liquid adhesive (epoxy resin system) is used around the light emitting region and the light emitting region except for the end portions of the first electrode and the second electrode leading electrodes 1-1 to 1-8. Coating was performed at 30 μm.

(Pasting of sealing member)
Thereafter, the organic EL element No. 1 prepared with the sealing member shown below was prepared. 1-1-1-8 are stacked on the adhesive coating surface, pressed in a 1 Pa vacuum environment with a pressing force of 0.1 MPa, and then left to stand for 3 hours in an atmospheric pressure 80 ° C. environment. The organic EL panel was prepared and the sample No. 101-108.

(Preparation of sealing member)
As a sealing member, a sheet-shaped sealing member having a two-layer configuration using a PEN film (manufactured by Teijin / DuPont) as a base material and an aluminum foil of a conductive material as a barrier layer was prepared. The PEN thickness was 100 μm, and the barrier layer thickness was 7 μm. The base material and the barrier layer were joined by a dry laminating method using a polyester adhesive, and the thickness of the sealing member after joining was 110 μm. The water vapor permeability measured by the MOCON method by a method based on the JIS K-7129B method (1992) was 0.01 g / m ² · day. The oxygen permeability measured mainly by the MOCON method by a method based on JIS K7126B method (1987) was 0.1 ml / m ² · day · MPa. The prepared sheet-shaped sealing member was cut according to the size of the prepared organic EL element.

Evaluation Each sample No. Table 2 shows the results of testing the occurrence ratio of dark spots (spot-shaped non-light-emitting portions) according to the following evaluation ranks in accordance with the evaluation ranks shown below.

Test method for the rate of occurrence of dark spots (spot-shaped non-light-emitting parts) Using a constant voltage power supply, 5V DC is applied to one dot of the organic EL panel, and the presence or absence of dark spots is visually observed using a loupe (magnification 8 times). Observed. Measurement was performed for all 70 dots (light emitting area), and the dark spot generation ratio was calculated from the number of dots in which dark spots were generated.

Evaluation rank of occurrence ratio of dark spots (spot-like non-light-emitting portions) A: Occurrence rate 0% (no occurrence of dark spots)
○: Occurrence rate 1% or more and less than 5% △: Occurrence rate 5% or more and less than 10% ×: Occurrence rate 10% or more

  The effectiveness of the present invention was confirmed.

Example 2
(Production of organic EL element)
The same organic EL element as Example 1 was produced.

(Production of organic EL panel)
An organic EL panel was produced according to the manufacturing process shown in FIG.

(Second electrode surface smoothing treatment and oxidation treatment)
After smoothing the surface of the prepared organic EL element on the side where the sealing member for the second electrode is bonded, the surface of the second electrode smoothed in the oxidation treatment step is oxidized under the conditions shown in Table 3. No. 2-1 to 2-6.

  As the smoothing treatment, the same reactive ion etching apparatus as in Example 1 was used. As the oxidation treatment, a reactive ion etching apparatus is used, and the surface of the smoothed second electrode is changed to a desired state by changing the radio frequency power (RF) power, the introduced gas type, the introduced gas amount, and the pressure in the chamber. Oxidized.

In the table, RF power indicates high-frequency power supply power. Ar represents argon gas, and O ₂ represents oxygen gas.

(Applying adhesive)
The prepared organic EL element No. A thermosetting liquid adhesive (epoxy resin system) is used around the light emitting region and the light emitting region except for the end portions of the lead electrodes of the 2-1 to 2-6 first electrode and the second electrode. Coating was performed at 30 μm.

(Pasting of sealing member)
Then, the organic EL element No. which prepared the same sealing member as Example 1 was prepared. After stacking on the adhesive coated surface of 2-1 to 2-6 and pressing with a pressing force of 0.1 MPa in a vacuum environment of 100 Pa, it is left to stand for 3 hours in an environment of atmospheric pressure 80 ° C. and fixed. The organic EL panel was prepared and the sample No. 201-206.

Evaluation Each sample No. Table 4 shows the results obtained by testing the occurrence ratio of dark spots in 201 to 206 by the same method as in Example 1 and evaluating according to the same evaluation rank as in Example 1.

  The effectiveness of the present invention was confirmed.

Example 3
(Production of organic EL element)
The same organic EL element as Example 1 was produced.

(Production of organic EL panel)
An organic EL panel was produced according to the manufacturing process shown in FIG.

(Second electrode surface smoothing treatment)
The surface on the side where the sealing member for the second electrode of the prepared organic EL element is bonded is smoothed under the conditions shown in Table 5 to obtain No. It was set as 3a-3f.

In the table, RF power indicates high-frequency power supply power. Ar represents argon gas, and Cl ₂ represents chlorine gas.

(Formation of inorganic film)
Smoothed organic EL element No. On the second electrodes 3a to 3f, an inorganic film (SiN) is laminated by a sputtering method to a thickness of 100 μm, and the organic EL element No. 1 with inorganic films formed thereon is formed. 3-1 to 3-6.

(Applying adhesive)
The prepared inorganic EL element No. A thermosetting liquid adhesive (epoxy resin system) is used around the light emitting area and the light emitting area except for the ends of the first and second electrode electrodes 3-1 to 3-6. Coating was performed at 30 μm.

(Pasting of sealing member)
Thereafter, the same organic EL element No. 1 with inorganic film formation prepared as the sealing member as in Example 1 was prepared. After stacking on the adhesive coated surface of 3-1 to 3-6 and pressing with a pressing force of 0.1 MPa in a vacuum environment of 100 Pa, it is left to stand for 3 hours in an environment of atmospheric pressure 80 ° C. The organic EL panel was prepared and the sample No. 301 to 306.

Evaluation Each sample No. Table 6 shows the results of the evaluation of the dark spot generation ratios 301 to 306 according to the same evaluation rank as that of the first example.

  The effectiveness of the present invention was confirmed.

Example 4
(Production of organic EL element)
The same organic EL element as Example 1 was produced.

(Production of organic EL panel)
An organic EL panel was produced according to the manufacturing process shown in FIG.

(Second electrode surface smoothing treatment and oxidation treatment)
After smoothing the surface of the prepared organic EL element on the side where the sealing member for the second electrode is bonded, the surface of the second electrode oxidized in the oxidation treatment step is oxidized under the conditions shown in Table 7 and No. . 4a to 4f.

  As the smoothing treatment, the same reactive ion etching apparatus as in Example 1 was used. As the oxidation treatment, a reactive ion etching apparatus is used, and the surface of the smoothed second electrode is changed to a desired state by changing the radio frequency power (RF) power, the introduced gas type, the introduced gas amount, and the pressure in the chamber. Oxidized.

In the table, RF power indicates high-frequency power supply power. Ar represents argon gas, and Cl ₂ represents chlorine gas.

(Formation of inorganic film)
Oxidized organic EL element No. On the second electrodes 4a to 4f, an inorganic film (SiN) is laminated with a thickness of 100 nm by a sputtering method, and the organic EL element no. 4-1 to 4-6.

(Applying adhesive)
The prepared inorganic EL element No. A thermosetting liquid adhesive (epoxy resin system) is used around the light emitting region and the light emitting region except for the ends of the first and second electrode electrodes 4-1 to 4-6. Coating was performed at 30 μm.

(Pasting of sealing member)
Thereafter, the same organic EL element No. 1 with inorganic film formation prepared as the sealing member as in Example 1 was prepared. 4-1 to 4-6 are stacked on the adhesive coating surface, pressed in a 100 Pa vacuum environment with a pressing force of 0.1 MPa, and then left to stand for 3 hours in an atmospheric pressure 80 ° C. environment. The organic EL panel was prepared and the sample No. 401 to 406.

Evaluation Each sample No. Table 8 shows the results of the dark spot generation ratios 401 to 406 tested by the same method as in Example 1 and evaluated according to the same evaluation rank as in Example 1.

  The effectiveness of the present invention was confirmed.

Example 5
(Production of organic EL element)
The same organic EL element as Example 1 was produced.

(Production of organic EL panel)
An organic EL panel was produced according to the manufacturing process shown in FIG.

(Smoothing treatment and oxidation treatment of the second electrode)
The surface on the side where the sealing member for the second electrode of the prepared organic EL element is bonded is designated as sample No. 2 in Example 2. Smoothing was performed under the same conditions as in 2-3, and the surface roughness Ra was set to 20 nm.

(Formation of inorganic film)
On the second electrode of the oxidized organic EL element, an inorganic film (SiN) was laminated with a thickness of 100 nm by a sputtering method to obtain an organic EL element with an inorganic film formed thereon.

(Smoothing treatment of inorganic film)
An organic EL element in which the surface roughness Ra was changed as shown in Table 9 was prepared by performing the following smoothing treatment on the surface of the inorganic film of the organic EL element on which the prepared inorganic film was formed. 5-1 to 5-7. A reactive ion etching apparatus was used as a smoothing treatment, and the inorganic film was processed to a desired surface roughness by changing the high frequency power (RF) power, the introduced gas type, the introduced gas amount, and the pressure in the chamber. The surface roughness Ra indicates a value measured by an atomic force microscope (AFM) SPA300 manufactured by SII Nano Technology.

In the table, RF power indicates high-frequency power supply power. Ar represents argon gas, and CF ₄ represents freon gas.

(Applying adhesive)
The prepared organic EL element No. 1 after smoothing treatment of the inorganic film. A thermosetting liquid adhesive (epoxy resin system) is used around the light emitting area and the light emitting area except for the ends of the first electrode and the second electrode leading electrodes of 5-1 to 5-7, and the thickness Coating was performed at 30 μm.

(Pasting of sealing member)
Thereafter, the organic EL element No. 1 in which the inorganic film prepared with the same sealing member as in Example 1 was smoothed was used. After stacking on the adhesive coating surface of 5-1 to 5-7 and pressing with a pressing force of 0.1 MPa in a vacuum environment of 100 Pa, it is left to stand for 3 hours in an environment of atmospheric pressure 80 ° C. The organic EL panel was prepared and the sample No. 501-507.

Evaluation Each sample No. Table 10 shows the results of the evaluation of the dark spot generation ratio in the same method as in Example 1 and evaluation according to the same evaluation rank as in Example 1.

  The effectiveness of the present invention was confirmed.

Example 6
(Production of organic EL element)
The same organic EL element as Example 1 was produced.

(Production of organic EL panel)
An organic EL panel was produced according to the manufacturing process shown in FIG.

(Smoothing treatment and oxidation treatment of the second electrode)
The surface on the side where the sealing member for the second electrode of the prepared organic EL element is bonded is designated as sample No. 2 in Example 2. The surface roughness Ra was set to 40 nm by performing a smoothing treatment and an oxidation treatment under the same conditions as in 2-5.

(Formation of inorganic film)
On the second electrode of the oxidized organic EL element, an inorganic film (SiN) was laminated at a thickness of 100 nm by a vapor phase volume method using a sputtering method to obtain an organic EL element with an inorganic film formed.

(Oxidation treatment of inorganic film)
An organic EL element in which the surface roughness Ra was changed as shown in Table 11 by the smoothing treatment shown below on the surface of the inorganic film of the organic EL element on which the prepared inorganic film was formed, and the surface is shown below. Oxidation treatment was performed under the conditions. 6-1 to 6-7.

  A reactive ion etching apparatus was used as the smoothing treatment and oxidation treatment, and the inorganic film was subjected to desired surface roughness and oxidation treatment by changing the radio frequency power (RF) power, the introduced gas species, the introduced gas amount, and the pressure in the chamber. . The surface roughness Ra indicates a value measured by an atomic force microscope (AFM) SPA300 manufactured by SII Nano Technology.

In the table, RF power indicates high-frequency power supply power. Ar represents argon gas, CF ₄ represents freon gas, and O ₂ represents oxygen gas.

(Applying adhesive)
The prepared inorganic film is subjected to oxidation treatment of organic EL element No. A thermosetting liquid adhesive (epoxy resin system) is used around the light emitting region and the light emitting region except for the end portions of the lead electrodes of the first electrode and the second electrode of 6-1 to 6-7. Coating was performed at 30 μm.

(Pasting of sealing member)
Thereafter, the organic EL element No. 1 was prepared by oxidizing the inorganic film prepared with the same sealing member as in Example 1. 6-1 to 6-7 are stacked on the adhesive-coated surface, pressed under a pressure of 0.1 MPa in a 100 Pa vacuum environment, and then left to stand for 3 hours in an atmosphere of atmospheric pressure 80 ° C. The organic EL panel was prepared and the sample No. 601-607.

Evaluation Each sample No. Table 12 shows the results of the evaluation of the ratio of occurrence of dark spots 601 to 607 by the same method as in Example 1 and the evaluation according to the same evaluation rank as in Example 1.

  The effectiveness of the present invention was confirmed.

Example 7
(Preparation of organic EL elements)
<Preparation of strip-shaped flexible support having gas barrier layer and first electrode layer in this order>
Using a polyethylene terephthalate film having a thickness of 100 μm (a film made by Teijin DuPont, hereinafter abbreviated as PET), a gas barrier layer, a first electrode layer, a hole transport layer, a light emitting layer, an electron injection layer, and a second electrode A band-shaped organic EL element was prepared by sequentially stacking layers.

(Formation of a transparent gas barrier layer)
On the prepared PET, a transparent gas barrier layer having a thickness of about 90 nm was formed by an atmospheric pressure plasma discharge treatment method. As a result of measuring the water vapor transmission rate by a method based on JISk-7129B, it was 10 ⁻³ g / m ² · day or less. As a result of measuring the oxygen transmission rate by a method based on JISk-7126B, it was 10 ⁻³ g / m ² · day or less.

(Formation of the first electrode)
On the barrier layer thus formed, ITO (indium tin oxide) having a thickness of 120 nm was patterned by a vapor deposition method to form a first electrode.

(Formation of hole transport layer and light emitting layer)
The following coating liquid for forming a hole transport layer is applied and dried on the first electrode by a wet coating method using an extrusion coating machine, followed by charging treatment, and subsequently emitting light onto the hole transport layer. After coating and drying the layer-forming coating solution by a wet coating method using an extrusion coating machine to form a light emitting layer, it is charged and cooled to the same temperature as the room temperature, and then wound around the winding core. It was. The conveyance speed was 2 m / min. The conveyance speed was measured with a laser Doppler velocimeter LV203 manufactured by Mitsubishi Electric Corporation.

Before applying the coating liquid for forming the hole transport layer, the surface of the belt-like flexible support is subjected to a cleaning surface modification treatment using a low-pressure mercury lamp with a wavelength of 184.9 nm at an irradiation intensity of 15 mW / cm ² and a distance of 10 mm. Carried out. The charge removal treatment was performed using a static eliminator with weak X-rays.

  The coating liquid for forming the hole transport layer was applied so that the thickness after drying was 50 nm. The light emitting layer forming coating solution was applied so that the thickness after drying was 100 nm. The conveyance speed was 2 m / min.

Preparation of coating solution for forming hole transport layer Polyethylene dioxythiophene / polystyrene sulfonate (PEDOT / PSS, Baytron P AI 4083 manufactured by Bayer) diluted with pure water 65% and methanol 5% to form hole transport layer It was prepared as a coating solution. The surface tension of the coating liquid for forming a hole transport layer was 40 × 10 ⁻³ N / m (manufactured by Kyowa Interface Chemical Co., Ltd .: surface tension meter CBVP-A3).

Preparation of a coating solution for forming a light emitting layer 5% by mass of a dopant material Ir (ppy) 3 is dissolved in 1,2-dichloroethane in polyvinyl carbazole (PVK) as a host material to prepare a coating solution for forming a light emitting layer. did. The surface tension of the coating solution for forming the light emitting layer was 32 × 10 ⁻³ N / m (manufactured by Kyowa Interface Chemical Co., Ltd .: surface tension meter CBVP-A3). The glass transition temperature of the light emitting layer was 225 degreeC. In addition, although the material which has green light emission was used for this example, it is possible to produce a white organic EL element by laminating | stacking further using blue, red, and a dopant material.

Coating conditions The temperature at the time of application of the hole transport layer forming coating solution was 25 ° C., and the temperature at the time of coating of the light emitting layer forming coating solution was 25 ° C. in an atmospheric environment. The wet coating process was performed with a dew point temperature of −20 ° C. or lower and a cleanliness class 5 or lower (JIS B 9920).

Drying and Heat Treatment Conditions After applying the hole transport layer forming coating solution, the solvent was removed at a discharge air velocity of 1 m / s, a wide air velocity distribution of 5%, and a temperature of 100 ° C. A hole transport layer was formed by heat treatment. After the light emitting layer forming coating solution was applied, the solvent was removed at a discharge wind speed of 1 m / s, a wide wind speed distribution of 5%, and a temperature of 60 ° C., followed by heat treatment at a temperature of 220 ° C. to form a light emitting layer. .

(Formation of electron injection layer and second electrode)
Subsequently, a LiF layer (electron injection layer) having a thickness of 0.5 nm is vapor-deposited on the formed light emitting layer under a vacuum of 5 × 10 ⁻⁴ Pa, and is orthogonal to the first electrode through a mask. Thus, after forming a 100 nm thick aluminum layer (second electrode) with a width of 50 μm and a pattern of 30 μm by vapor deposition, a sealing layer was subsequently formed by vapor deposition and cooled to room temperature.

(Production of organic EL panel)
An organic EL panel was produced according to the manufacturing process shown in FIG.

(Second electrode surface smoothing treatment and oxidation treatment)
The surface of the prepared organic EL element on the side where the sealing member for the second electrode is bonded is simultaneously subjected to the following smoothing treatment and oxidation treatment, and the surface roughness Ra is changed as shown in Table 13 An element was prepared and 7-1 to 7-7. In addition, an organic EL element that is not subjected to the smoothing treatment and the oxidation treatment was prepared as a comparative sample. 7-8.

  A reactive ion etching apparatus was used as a smoothing process and an oxidation process, and the second electrode was processed to a desired surface roughness by changing the RF power (RF) power, the introduced gas type, the introduced gas amount, and the pressure in the chamber. .

  The surface roughness Ra indicates a value measured by an atomic force microscope (AFM) SPA300 manufactured by SII Nano Technology.

In the table, RF power indicates high-frequency power supply power. Ar represents argon gas, CF ₄ represents freon gas, and O ₂ represents oxygen gas.

(Applying adhesive)
The prepared organic EL element No. Using an ultraviolet curing liquid adhesive (epoxy resin system) around the light emitting region and the light emitting region except for the ends of the first and second electrode electrodes 7-1 to 7-8, the thickness Coating was performed at 30 μm.

(Pasting of sealing member)
Thereafter, the organic EL element No. 1 prepared with the continuous sheet-like sealing member shown below was prepared. 7-1 to 7-8 are stacked on the adhesive coating surface by a roll laminator method, and after pressure-bonding with a pressure of 0.1 MPa in an atmospheric pressure environment, a high-pressure mercury lamp with a wavelength of 365 nm is irradiated with an irradiation intensity of 5 An organic EL panel was prepared by irradiating and adhering at 20 mW / cm ² at a distance of 5 to 15 mm for 1 minute to make an organic EL panel. 701 to 708.

(Preparation of sealing member)
As a sealing member, a continuous sheet-shaped sealing member having a two-layer structure using a PEN film (manufactured by Teijin / DuPont) as a base material and an inorganic film (SiN) as a barrier layer was prepared. The PEN thickness was 100 μm, and the barrier layer thickness was 200 nm. The barrier layer was formed on the substrate by sputtering, and the thickness of the sealing member after film formation was 110 μm. The water vapor permeability measured by the MOCON method by a method based on the JIS K-7129B method (1992) was 0.01 g / m ² · day. The oxygen permeability measured mainly by the MOCON method by a method based on JIS K7126B method (1987) was 0.1 ml / m ² · day · MPa. The prepared continuous sheet-shaped sealing member was side-slit according to the size of the prepared organic EL element to form a winding roll.

Evaluation Each sample No. Table 14 shows the results of 701 to 708, where the dark spot generation ratio was tested by the same method as in Example 1 and evaluated according to the same evaluation rank as in Example 1.

  The effectiveness of the present invention was confirmed.

Example 8
(Production of organic EL element)
The same organic EL element as Example 1 was produced.

(Production of organic EL panel)
An organic EL panel was produced according to the manufacturing process shown in FIG.

(Second electrode surface smoothing treatment)
The surface on the side where the sealing member for the second electrode of the prepared organic EL element is bonded is smoothed under the conditions shown in Table 15 and No. 8-1 to 8-6. An organic EL element that is not subjected to a smoothing treatment was prepared as a comparative sample. 8-7.

In the table, RF power indicates high-frequency power supply power. Ar represents argon gas, and Cl ₂ represents chlorine gas.
(Formation of inorganic film)
Smoothed organic EL element No. On the second electrodes 8-1 to 8-7, an inorganic film (SiN) was laminated with a thickness of 100 nm by a sputtering method to produce an organic EL panel. 801 to 807.

Evaluation Each sample No. Table 16 shows the results of the evaluation of the ratio of occurrence of dark spots in 801 to 807 by the same method as in Example 1 and the evaluation according to the same evaluation rank as in Example 1.

  The effectiveness of the present invention was confirmed.

It is a schematic diagram which shows an example of the manufacturing process of the organic electroluminescent panel which has the close_contact | adherence sealing structure with the sealing member for the organic EL element produced using the sheet | seat base material. It is a schematic diagram which shows an example of the manufacturing process of the organic EL panel which has the close_contact | adherence sealing structure with the sealing member for the organic EL element produced using the strip | belt-shaped base material. It is the schematic of the organic electroluminescent panel manufactured by the manufacturing process of the organic electroluminescent panel shown to Fig.1 (a). FIG. 4 is an enlarged schematic flow diagram until a portion indicated by P in FIG. It is the schematic of the organic electroluminescent panel manufactured by the manufacturing process of the organic electroluminescent panel shown in FIG.1 (b) and FIG.1 (c). FIG. 6 is an enlarged schematic flow diagram until a portion indicated by Q in FIG. 5C is formed. FIG. 6 is an enlarged schematic flow diagram until a portion indicated by Q in FIG. 5C is formed.

Explanation of symbols

1a, 2a Manufacturing process 101, 201 Supply process 101a, 201a Organic EL element 102, 202 Smoothing process 102a, 202a, 208a Dry etching apparatus 103, 203 Oxidation process 103a, 203a, 209a Oxygen gas spraying apparatus 104, 204 Adhesion Agent coating process 105, 205 Sealing member bonding process 105b, 205b Sealing member 106 Punching process 107 Recovery process 107a Organic EL panel 108, 207 Inorganic film forming process 108b, 207b Deposition apparatus 109, 208 Inorganic film smoothing process 110, 209 Inorganic film oxidation treatment process 206a Rolled organic EL panel

Claims (9)

In an organic electroluminescence panel manufacturing method, an organic electroluminescence element having at least a first electrode layer, an organic compound layer including a light emitting layer, and a second electrode layer on a substrate and having a close sealing structure with a sealing member. ,
After dry-etching the surface of the second electrode layer on the side where the sealing member is bonded,
A method for producing an organic electroluminescence panel, comprising laminating the sealing member. 2. The method of manufacturing an organic electroluminescence panel according to claim 1, wherein the surface roughness Ra of the upper surface of the second electrode layer after the dry etching treatment is 30 nm or less. 3. The method of manufacturing an organic electroluminescence panel according to claim 1, wherein an oxidation treatment is further performed after the dry etching treatment. The method for manufacturing an organic electroluminescence panel according to claim 1, wherein an oxidation process is performed simultaneously with the dry etching process. The organic electroluminescence panel according to claim 1, wherein an adhesive layer is formed on the second electrode layer that has been subjected to the dry etching treatment, and then a sealing member is laminated. Manufacturing method. 5. The method of manufacturing an organic electroluminescence panel according to claim 1, wherein an inorganic film is formed on the second electrode layer subjected to the dry etching process. The inorganic film is formed on the second electrode layer that has been subjected to the dry etching process, and then an adhesive layer is formed on the inorganic film, and then the sealing member is laminated. The manufacturing method of the organic electroluminescent panel of any one of 1-4. An inorganic film is formed on the second electrode layer that has been subjected to the dry etching process, and then the upper surface of the inorganic film is subjected to a dry etching process to have a surface roughness Ra of 30 nm or less. The method for producing an organic electroluminescence panel according to claim 1, wherein an adhesive layer is formed on the substrate and the sealing member is laminated. An organic electroluminescence panel manufactured by the manufacturing method according to claim 1.

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