JPWO2008102867A1 - ORGANIC ELECTROLUMINESCENT ELEMENT AND METHOD FOR PRODUCING ORGANIC ELECTROLUMINESCENT ELEMENT - Google Patents

Abstract

A method for producing an organic EL element having no image defect by a bonding method, wherein a first member having at least an anode formed on a first substrate and at least a cathode formed on a second substrate. The second member is used, and at least one of the first member and the second member has an organic functional layer, and is produced by bonding so as to be configured in the order of anode-organic functional layer-cathode. In the organic electroluminescence element thus formed, the surface roughness Ra of the surface of the second member to be bonded to the first member is 3.0 nm or less.

Description

  The present invention relates to an organic electroluminescence element (hereinafter also referred to as an organic EL element) and a method for producing the organic EL element.

  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 is composed of an organic compound layer (single layer portion or multilayer portion) containing an organic light-emitting substance having a thickness of only about 0.1 μm between an anode and a cathode formed on a pair of supports. It is a thin film type all solid state device. When a relatively low voltage of about 2 to 20 V 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 emission can be 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. This technology is expected as a display and lighting. Furthermore, the recently discovered organic EL using phosphorescence emission can realize a light emission efficiency of about 4 times in principle compared to that using previous fluorescence emission. Research and development of device layer configurations and electrodes are performed all over the world.

  Thus, 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 support is used as a surface light source such as a backlight, the surface A device provided with a light source can be easily made thin. 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 support as a display panel, the liquid crystal display device has high visibility and no viewing angle dependency. There are advantages that cannot be obtained.

  As a manufacturing method of an organic EL element, a method of sequentially forming an anode, an organic functional layer, and a cathode on a substrate (sequential film forming method), a first substrate in which an anode and an organic functional layer are laminated, A method (bonding method) in which a second substrate on which a cathode is formed is prepared and bonded so that the anode and the cathode face each other between the first substrate and the second substrate is known.

  Disadvantages of the sequential deposition method are that the cathode is formed by a vapor deposition method where high temperature is applied. Therefore, when a substrate with a gas barrier layer is used, biased stress is generated due to a large temperature difference between the vapor deposition region and the non-vapor deposition region. There is a problem that cracks are easily generated in the gas barrier layer due to heat load, and the barrier property becomes unstable. In the roll-to-roll method, which is easy to produce a large-area full-color display device and has good production efficiency, the cathode is produced by a vacuum process such as vapor deposition or sputtering, so that process eventually becomes a bottleneck. However, the current situation is that production efficiency cannot be mentioned.

On the other hand, instead of the sequential film formation method, a first member in which an anode (first electrode) and a light emitting layer are sequentially formed on a support, and a second member in which a cathode (second electrode) is formed on the support, The method (bonding method) for bonding the anode (first electrode) and the cathode (second electrode) to face each other between the first member and the second member has the following advantages. Has been studied from.
(1) A first member in which an anode (first electrode) and a light emitting layer are sequentially formed on a support and a second member in which a cathode (second electrode) is formed on the support are sequentially formed separately. Prepare in advance by law. (2) Since the cathode (second electrode) formed separately by the vapor deposition method that requires high temperature is separately produced, the gas barrier layer provided on the first member side is not damaged by high temperature, so that the storability of the manufactured organic EL device is improved. Improvement and stabilization are possible.
(3) The roll-to-roll system can be continuously produced by using a flexible member for the support.
(4) There is a possibility of improvement in production efficiency and cost reduction which cannot be achieved by the roll-to-roll method in the sequential film formation method.
(5) The organic layer can be easily laminated by making the bonding surface of each other an organic layer.

  For example, an organic material layer including an organic light emitting material layer is laminated via a first striped electrode layer formed on a long support, and an adhesive is disposed around the first striped electrode layer. One laminate and a second laminate on which the other layer of the organic material layer is formed are overlapped via a second striped electrode layer formed on the elongated support, and at least After bonding (bonding) each other by heating and softening one of the layers, the first laminate and the second laminate are cut along the substrate width direction, and an adhesive ( A method of manufacturing an organic electroluminescence display panel by sealing with a sealing agent is known (for example, see Patent Document 1).

  The method described in Patent Document 1 is an effective production method for realizing high productivity in the roll-to-roll manufacturing method. However, the organic electroluminescence display panel (corresponding to the organic EL element of the present invention) produced by the method described in Patent Document 1 leaks from the organic electroluminescence display panel produced by the sequential film formation method. The yield is often poor due to image defects such as shorts.

From such a situation, development of the organic EL element which does not have an image defect by the bonding method, and the manufacturing method of an organic EL element is desired.
JP 2004-296147 A

  This invention is made | formed in view of the said situation, The objective is to provide the manufacturing method of the organic EL element which does not have an image defect by the bonding method, and an organic EL element.

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

  1. A first member having at least an anode and at least one organic functional layer formed on the first substrate; and a second member having at least a cathode formed on the second substrate. In the organic electroluminescence element produced by bonding so that the anode and the cathode are sandwiched between a base material and the second base material, the first member of the second member An organic electroluminescence device, wherein the surface roughness Ra of the surface to be bonded is 3.0 nm or less.

  2. 2. The organic electroluminescence device according to 1 above, wherein the edge around the cathode is chamfered.

  3. 3. The organic electroluminescence device according to 1 or 2 above, wherein at least one organic functional layer is formed on the cathode.

  4). 4. The organic electroluminescent element according to any one of 1 to 3, wherein at least one of the first base material and the second base material is formed of a flexible base material.

  5. Using the first member having at least an anode and at least one organic functional layer formed on the first substrate, and the second member having at least a cathode formed on the second substrate, Bonding is performed so that the anode and the cathode are sandwiched between one base material and the second base material, and a sealing member is provided between the first base material and the second base material. In the manufacturing method of the organic electroluminescence element sealed in step 1, the first supply step for supplying the first member, the second supply step for supplying the second member, the first member, and the second member, A second step of forming the cathode on the second substrate, and a surface roughness Ra of 3.0 nm or less on the cathode. Organic electroluminescence comprising a cathode surface smoothing step for performing a smoothing treatment Method of manufacturing a child.

  6). 6. The method for producing an organic electroluminescent element according to 5 above, wherein the smoothing treatment is performed by a dry etching treatment under a reduced pressure atmosphere.

  7). 7. The method for producing an organic electroluminescent element according to 5 or 6, further comprising a step of chamfering the edge of the cathode after the step of smoothing the cathode surface.

  8). 8. The method for producing an organic electroluminescent element according to 7, wherein the chamfering process is performed by polishing in an inert gas atmosphere.

  9. The method for producing an organic electroluminescent element according to any one of 5 to 8, wherein the bonding is performed by thermocompression bonding.

  10. 10. The method for manufacturing an organic electroluminescent element according to any one of 5 to 9, wherein the organic functional layer is formed by a wet process.

  11. Each of said 1st member and 2nd member is formed with a roll to roll process, The manufacturing method of the organic electroluminescent element in any one of said 5-10 characterized by the above-mentioned.

  The organic EL element which does not have an image defect by the bonding method, and the manufacturing method of the organic EL element can be provided, and the production efficiency of the organic EL element having excellent performance can be improved.

It is the schematic which shows an example of the organic EL element manufactured by the bonding method of this invention. It is a schematic diagram of the manufacturing process of the organic EL element which uses the strip | belt-shaped flexible support body for the 1st base material and the 2nd base material, and manufactures the organic EL element shown by FIG. 1 by the bonding method of a roll to roll system. . It is a schematic diagram of the manufacturing process of the organic EL element which manufactures the organic EL element shown by FIG. 1 by a bonding method, using a single-wafer base material for a 1st base material and a 2nd base material. It is an expansion schematic perspective view of the part shown by U of FIG. FIG. 5 is an enlarged schematic view of a portion indicated by V in FIG. 4. FIG. 3 is a schematic enlarged perspective view of a cathode surface smoothing step shown in FIG. 2. It is an expansion schematic of the chamfering process shown in FIG. It is the schematic of the part shown by W of FIG. It is the schematic of the bonding process shown by FIG. It is a general | schematic expanded sectional view of the other bonding apparatus used for the bonding process shown by FIG. It is the schematic which shows the state of the 1st member and 2nd member before and behind bonding by the bonding apparatus shown by FIG.

Explanation of symbols

DESCRIPTION OF SYMBOLS 1 Organic EL element 101, 201a, 201'a 1st base material 102, A anode (1st electrode)
103, B hole transport layer 104, C light emitting layer 105, F cathode buffer layer (electron injection layer)
106, E cathode (second electrode)
107, 201'b Second base material 108 Sealing member 2, 2 'Manufacturing process 2a, 2'a First supply process 2b, 2'b Second supply process 2c, 2'c Sealant coating process 2d, 2'd bonding process 2e punching process 201a1, 201'a1 first member 201b1, 201'b1 second member 4, 4 'hole transport layer forming process 7, 7' cathode (second electrode) forming process 5, 5 ′ Light emitting layer forming step 8, 8 ′ Cathode surface smoothing step 8a, 8′a Cathode surface smoothing processing device 9, 9 ′ Chamfering processing step 9a, 9′a Chamfering processing device 10, 10 ′ Cathode buffer layer (electronic Injection layer) formation process D Adhesive X, Y Alignment mark

  Embodiments of the present invention will be described with reference to FIGS. 1 to 11, but the present invention is not limited thereto.

  FIG. 1 is a schematic view showing an example of an organic EL element produced by the bonding method of the present invention. Fig.1 (a) shows the schematic perspective view which shows an example of the organic EL element manufactured by the bonding method of this invention. FIG.1 (b) is a schematic sectional drawing in alignment with GG 'of Fig.1 (a). FIG.1 (c) is a schematic sectional drawing in alignment with HH 'of Fig.1 (a).

  In the figure, 1 indicates an organic EL element. The organic EL element 1 includes an anode (first electrode) 102, a hole transport layer 103, a light emitting layer 104, a cathode buffer layer (electron injection layer) 105, and a cathode (first electrode) sequentially on the first base material 101. 2 electrodes) 106, a second base material 107, and a sealing member 108. The organic EL element 1 has a configuration in which an anode (first electrode) 102 and a cathode (second electrode) 106 are opposed to each other between a first base material 101 and a second base material 107. A close sealing structure is formed by sealing with a sealing member 108 except for an end portion of the extraction electrode 102a of the first electrode 102 and the extraction electrode 106a of the cathode (second electrode) 106.

  A gas barrier film (not shown) may be provided between the anode (first electrode) 102 and the first substrate 101 and between the second substrate 107 and the cathode (second electrode) layer 106.

  Either the first base material 101 or the second base material 107 may be a flexible support, or one of them may be a flexible support, and can be appropriately selected as necessary. .

  The present invention relates to an organic EL element 1 and a method for manufacturing the organic EL element 1 shown in the figure.

  The layer configuration of the organic EL element shown in this figure is an example, but as another typical organic EL element between the anode (first electrode) and the cathode (second electrode), The following configurations are listed.

(1) Anode (first electrode) / organic layer (light emitting layer) / cathode (second electrode)
(2) Anode (first electrode) / organic layer (light emitting layer) / electron transport layer / cathode (second electrode)
(3) Anode (first electrode) / hole transport layer / organic layer (light emitting layer) / hole blocking layer / electron transport layer / cathode (second electrode)
(4) Anode (first electrode) / hole transport layer (hole injection layer) / organic layer (light emitting layer) / hole blocking layer / electron transport layer / cathode buffer layer (electron injection layer) / cathode (second electrode)
(5) Anode (first electrode) / anode buffer layer (hole injection layer) / hole transport layer / organic layer (light emitting layer) / hole blocking layer / electron transport layer / cathode buffer layer (electron injection layer) / Cathode (second electrode) Each layer constituting the organic EL element will be described later.

  FIG. 2 is a schematic diagram of a manufacturing process of an organic EL element in which the organic EL element shown in FIG. 1 is manufactured by a roll-to-roll bonding method using a belt-like flexible support for the first base material and the second base material. FIG.

  In the figure, 2 indicates a manufacturing process. The manufacturing process 2 has the 1st supply process 2a, the 2nd supply process 2b, the sealing agent coating process 2c, the bonding process 2d, and the punching process 2e.

  The 1st supply process 2a has shown the case where the 1st member 201a1 by which the anode (1st electrode) and the at least 1 layer of organic functional layer were formed into a film is supplied to the 1st base material 201a. The first member 201a1 is also referred to as an anode side member. In the case of this figure, when the anode (first electrode) A (see FIG. 5), the hole transport layer B (see FIG. 5), and the light emitting layer C (see FIG. 5) are formed on the first substrate 201a. The hole transport layer and the light emitting layer correspond to the organic functional layer.

  In the first supply step 2a shown in the figure, an anode (first electrode) A (see FIG. 5) and a hole transport layer B (see FIG. 5) are formed on a first base material 201a for manufacturing an organic EL element used for illumination. Reference) and a step of supplying the first member 201a1 formed in the order of the light emitting layer C (see FIG. 5). In this figure, since the anode (first electrode) A (see FIG. 5) already formed on the first base material 201a is used, the anode (first electrode) formation step is omitted. A gas barrier layer may be provided between the first base material 201a and the anode (first electrode) A (see FIG. 5).

The first supply step 2a includes a supply step 3 of the roll-shaped first base material 201a, a hole transport layer forming step 4 for forming the hole transport layer B (see FIG. 5), and a light emitting layer C (see FIG. 5). And a light emitting layer forming step 5. The first supply process 2a shown in the figure is a process in which the supply process 3 to the light emitting layer formation process 5 are continuously performed under atmospheric pressure conditions. The supply process 3 includes a feeding unit 301 and a surface treatment unit 302. In the feeding portion 301, an anode (first electrode) A (see FIG. 5) is already formed, and the first base material 201a wound in a roll shape wound around a winding core is supplied. The surface treatment unit 302 includes a cleaning surface modification apparatus 302a and first antistatic means 302b. The cleaning surface modification apparatus 302a is a surface of the anode (first electrode) A (see FIG. 5) of the first base material 201a sent from the supply step 301 before applying the hole transport layer forming coating solution. For example, it is preferable to use a low-pressure mercury lamp, an excimer lamp, a plasma cleaning apparatus, or the like. As conditions for the cleaning surface modification treatment using a low-pressure mercury lamp, for example, a cleaning surface modification treatment is performed by irradiating a low-pressure mercury lamp with a wavelength of 184.2 nm at an irradiation intensity of 5 to ²⁰ mW / cm ² and a distance of 5 to 15 mm. Conditions are mentioned. For example, atmospheric pressure plasma is preferably used as the condition for the cleaning surface modification treatment by the plasma cleaning apparatus. Examples of the cleaning condition include conditions in which a gas containing oxygen of 1 to 5% by volume is used for argon gas, and the cleaning surface modification treatment is performed at a frequency of 100 kHz to 150 MHz, a voltage of 10 V to 10 kV, and an irradiation distance of 5 to 20 mm.

The first antistatic means 302b has a non-contact type antistatic device 302b1 and a contact type antistatic device 302b2. Examples of the non-contact type antistatic device 302b1 include a non-contact type ionizer, and the type of ionizer is not particularly limited, and the ion generation method may be either an AC method or a DC method. An AC type, a double DC type, a pulsed AC type, and a soft X-ray type can be used, but the AC type is particularly preferable from the viewpoint of precise static elimination. Air or N ₂ is used as the injection gas required when using the AC type, but it is preferable to use N ₂ with sufficiently high purity. From the viewpoint of in-line operation, the blower type or the gun type is selected.

  As the contact-type antistatic device 302b2, a static eliminating roll or a conductive brush connected to the ground is used. The static elimination roll as the static eliminator is grounded and removes the surface charge by rotatingly contacting the neutralized surface. Such static elimination rolls include rolls made of elastic plastic or rubber mixed with conductive materials such as carbon black, metal powder, and metal fibers in addition to rolls made of metal such as aluminum, copper, nickel, and stainless steel. used. In particular, an elastic material is preferable in order to improve the contact with the first base material 201a. Examples of the conductive brush connected to the earth include a neutralizing bar or a neutralizing yarn structure having a brush member made of conductive fibers arranged in a line or a linear metal brush. The neutralization bar is not particularly limited, but a corona discharge type is preferably used. For example, SJ-B manufactured by Keyence Corporation is used. There is no particular limitation on the static elimination yarn, but usually a flexible yarn is preferably used. For example, 12/300 × 3 manufactured by Naslon can be cited as an example.

  The non-contact type antistatic device 302b1 is used on the anode (first electrode) surface side formed on the first base material 201a, and the contact type antistatic device 302b2 is used on the back surface side of the first base material 201a. It is preferable. The first antistatic means removes the charge of the first base material 201a and prevents the adhesion of the dust and the dielectric breakdown, thereby improving the yield of the organic EL element.

  The hole transport layer forming step 4 includes a backup roll 401a that holds the first substrate 201a and a first wet coating that applies a hole transport layer forming coating solution to the first substrate 201a held by the backup roll 401a. A first drying device 401c that removes the solvent of the hole transport layer B (see FIG. 5) formed on the anode (first electrode) A (see FIG. 5) on the first substrate 201a; The first heat treatment device 401d for heating the hole transport layer B (see FIG. 5) from which the solvent has been removed, and the second antistatic means 401e.

  The coating liquid for forming a hole transport layer by the first wet coater 401b is the anode (first) except for the extraction electrode A1 (see FIG. 5) of the anode (first electrode) A (see FIG. 5) that has already been formed. It is applied on the electrode A (see FIG. 5).

  Examples of the wet coater that can be used for the first wet coater 401b include a die coating method, a screen printing method, a flexographic printing method, an ink jet method, a Mayer bar method, a cap coating method, a spray coating method, a casting method, and a roll coating method. It is possible to use a coating machine such as a bar coating method or a gravure coating method. The use of these wet coating machines can be appropriately selected according to the material of the organic compound layer.

  As drying conditions for removing the solvent of the hole transport layer in the first drying device 401c, in consideration of drying unevenness, blown rough surface of the coating film, etc., the discharge air speed of the dry air from the discharge port is 0.1 to 5 m / s, Airflow drying in which the wind speed distribution in the width direction is 0.1 to 10% can be mentioned.

  As a heat treatment condition of the hole transport layer in the first heat treatment unit 401d, the glass transition temperature of the hole transport layer is considered in consideration of improvement in smoothness of the hole transport layer, removal of residual solvent, curing of the hole transport layer, and the like. On the other hand, it is preferable to perform the back-surface heat transfer type heat treatment at −30 to + 30 ° C. and at a temperature not exceeding the decomposition temperature of the organic compound constituting the hole transport layer.

  Although there is no restriction | limiting in particular about the film thickness of the positive hole transport layer B (refer FIG. 5) formed, Usually, 5 nm-about 5 micrometers, Preferably it is 5-200 nm. The hole transport layer may have a single layer structure. 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.

  The second antistatic means 401e has a non-contact type antistatic device 401e1 and a contact type antistatic device 401e2. The non-contact type antistatic device 401e1 is preferably used on the hole transport layer side, and the contact type antistatic device 401e2 is preferably used on the back surface side of the first substrate 201a. The second antistatic means removes the charge on the hole transport layer surface and the back surface of the first base material 201a, and prevents dust from adhering and dielectric breakdown, thereby improving the yield of the organic EL element. The non-contact type antistatic device 401e1 and the contact type antistatic device 401e2 used for the second antistatic unit 401e are the same as the non-contact type antistatic device 302b1 and the contact type antistatic device 302b2 used for the first antistatic unit 302b. Those are preferred.

  In the light emitting layer forming step 5, the light emitting layer is formed on the hole transport layer B (see FIG. 5) formed on the first base material 201a having the hole transport layer B (see FIG. 5) held by the backup roll 501a. A second wet coater 501b for applying the forming coating liquid; a second drying device 501c for removing the solvent of the light emitting layer C (see FIG. 5) formed on the hole transport layer B (see FIG. 5); And a second heat treatment device 501d for heating the light emitting layer C (see FIG. 5) from which the solvent has been removed, and a third antistatic means 501e.

  The coating liquid for forming the light emitting layer by the second wet coater 501b is applied to the hole transport layer B (see FIG. 5) that has already been formed except for the extraction electrode A1 of the anode (first electrode) A (see FIG. 5). It is applied on top.

  The second wet coater 501b is preferably of the same type as the first wet coater 401b. In this figure, since the organic EL element used for illumination is taken as an example, the second wet coater 501b is of the whole surface coating type. However, when the organic EL element is a full color system, it is patterned. For example, an ink jet method, a flexographic printing method, an offset printing method, a gravure printing method, a screen is used for applying a light emitting layer on the anode (first electrode) in accordance with the pattern of the anode (first electrode) formed It is possible to use various coating apparatuses used for a printing method, a spray coating method using a mask, and the like.

  The second drying device 501c has the same structure as the first drying device 401c. The second heat treatment apparatus 501d has the same structure as the first heat treatment apparatus 401d, and the light emitting layer C (see FIG. 5) formed on the hole transport layer B (see FIG. 5) is used as the first base material 201a. It is designed to heat from the back side by using the back side heat transfer method. As heat treatment conditions for the light emitting layer C (see FIG. 5) in the second heat treatment apparatus 501d, the smoothness of the light emitting layer C (see FIG. 5) is improved, the residual solvent is removed, the light emitting layer C (see FIG. 5) is cured, and the like. In consideration of the glass transition temperature of the light emitting layer C (see FIG. 5) and at a temperature not exceeding the decomposition temperature of the organic compound constituting the light emitting layer C (see FIG. 5). It is preferable to perform heat treatment using a back surface heat transfer method.

  When the light emitting layer C (see FIG. 5) is a multilayer, it is necessary to dispose units for the application / drying unit in accordance with the number of layers to be laminated. For example, a white element can be manufactured by forming a light emitting layer in multiple layers. 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 in 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.

  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 third antistatic means 501e has a non-contact type antistatic device 501e1 and a contact type antistatic device 501e2. The non-contact type antistatic device 501e1 is preferably used on the light emitting layer C (see FIG. 5) side, and the contact type antistatic device 501e2 is preferably used on the back surface side of the first substrate 201a. The third antistatic means removes the charge on the light emitting layer surface and the back surface of the first base material 201a, and prevents a failure due to dust adhering in the bonding step 2d, thereby improving the yield of the element. The non-contact type antistatic device 501e1 and the contact type antistatic device 501e2 used for the third antistatic unit 501e are the same as the noncontact type antistatic device 302b1 and the contact type antistatic device 302b2 used for the first antistatic unit 302b. Those are preferred.

  Thus, by completing the light emitting layer forming step 5, the anode (first electrode) A (see FIG. 5), the hole transport layer B (see FIG. 5), and light emission are formed on the first base material 201a. A first member 201a1 formed in the order of layer C (see FIG. 5) is prepared. The first member 201a1 is subsequently sent to the sealant coating step 2c. It is preferable to arrange an accumulator between the hole transport layer forming step 4 and the light emitting layer forming step 5 for speed adjustment.

  In addition, although this figure has shown the case where it sends to the sealing agent coating process 2c continuously, you may wind up and collect | recover the 1st member 201a1 once in roll shape.

  The hole transport layer forming step and the light emitting layer forming step 5 shown in this figure show a case where there is one wet coating device, a drying device, and a heat treatment device, respectively, but may increase as necessary. It is possible.

  Variations in the transport speed of the first substrate 201a when applying the hole transport layer forming coating solution with the first wet coater 401b, and when applying the light emitting layer forming coating solution with the second wet coater 501b The variation in the conveyance speed of the first base material 201a is preferably 0.2 to 10% with respect to the average conveyance speed in consideration of the light emission luminance unevenness associated with the coating film thickness unevenness in the longitudinal direction.

The coating liquid for forming a hole transport layer used in the first wet coater 401b and the coating liquid for forming the light emitting layer used in the second wet coater 501b include at least one organic compound material and at least one solvent. The surface tension is preferably 15 × 10 ^{−3 to} 55 × 10 ⁻³ N / m in consideration of repelling during coating and uneven coating.

  The process of forming the hole transport layer and the light emitting layer, which are the constituent layers of the organic EL element shown in this figure, considers the maintenance of the performance of the hole transport layer and the light emitting layer, the prevention of failure defects due to foreign matter adhesion, etc. Dew point temperature is −20 ° C. or lower, conforms to JISB 9920, measured cleanliness is class 5 or lower, and is formed under atmospheric pressure conditions of 10 to 45 ° C. excluding the first drying section and the second drying section. It is preferable. In the present invention, cleanliness of class 5 or less means class 3 to class 5.

  In the second supply step 2b, the second member 201b1 having at least a cathode (second electrode) formed on the second base 201b is supplied. In the case of this figure, the second member 201b1 in which the cathode (second electrode) E (see FIG. 11) and the cathode buffer layer (electron injection layer) F (see FIG. 11) are formed on the second substrate 201b. Is shown. The second member 201b1 is also called a cathode side member.

  In the second supply step 2b shown in the figure, a cathode (second electrode) E (see FIG. 11), a cathode buffer layer (electron injection layer) are formed on a second substrate 201b for manufacturing an organic EL element used for illumination. ) Shows a step of supplying the second member 201b1 formed in the order of F (see FIG. 11). In addition, you may provide a gas barrier layer between the 2nd base material 201b and the cathode (2nd electrode) E (refer FIG. 11).

  The second supply step 2b includes a supply step 6 for the roll-shaped second base material 201b, a cathode formation step 7 for forming the cathode (second electrode) E (see FIG. 11), and a cathode E (see FIG. 11). A cathode surface smoothing step 8 for performing a smoothing treatment, a chamfering step 9 for performing a chamfering treatment on an edge around the cathode E (see FIG. 11), and a cathode for forming a cathode buffer layer (electron injection layer) F And a buffer layer (electron injection layer) forming step 10. The second supply step shown in the figure is a step (dry process step) in which the cathode forming step 7 and the cathode buffer layer (electron injection layer) forming step 10 are performed under reduced pressure conditions.

  In the supplying step 6, the second base material 201b wound in a roll shape is supplied.

  In the cathode (second electrode) formation step 7, the cathode (second electrode) is formed on the second base material 201b at the cathode (second electrode) forming portion 701 in accordance with the position of the anode (first electrode) A (see FIG. 5). ) E (see FIG. 11) is formed. Reference numeral 701a denotes a vapor deposition apparatus, and 701b denotes an evaporation source container.

  The cathode surface smoothing step 8 includes a cathode surface smoothing processing device 8a and an accumulator 8b. The accumulator 8b can adjust the supply speed from the cathode (second electrode) forming step 7 and the processing speed in the cathode surface smoothing step 8. The surface of the cathode (second electrode) E (see FIG. 11) formed on the second base material 201b is smoothed by the cathode surface smoothing apparatus 8a. The cathode surface smoothing step 8 will be described in detail with reference to FIG.

  The chamfering process 9 includes a chamfering processing apparatus 9a and an accumulator 9b. It is possible to adjust the supply speed from the cathode surface smoothing process 8 and the processing speed in the chamfering process 9 by the accumulator 9b. A chamfering process is performed on the peripheral edges of the cathode (second electrode) E (see FIG. 11) formed on the second base material 201b by the chamfering processing apparatus 9a. The chamfering process 9 will be described in detail with reference to FIGS. In addition, the chamfering process 9 can be disposed as necessary.

  The cathode buffer layer (electron injection layer) forming step 10 is a cathode (second electrode) E processed in the cathode surface smoothing step 8 and the chamfering step 9 in the cathode buffer layer (electron injection layer) forming portion 1001 (FIG. 11), a cathode buffer layer (electron injection layer) F (see FIG. 11) is formed except for the extraction electrode E1 (see FIG. 11). Reference numeral 1001a denotes a vapor deposition apparatus, and reference numeral 1001b denotes an evaporation source container. By completing the cathode buffer layer (electron injection layer) forming step 10, the cathode (second electrode) E (see FIG. 11) and the cathode buffer layer (electron injection layer) layer F (see FIG. 11) are formed on the second substrate 201b. 11), the second member 201b1 formed in this order is prepared. The second member 201b1 is subsequently sent to the bonding step 2d. In addition, although this figure has shown the case where the 2nd member 201b1 is sent to the bonding process 2d continuously, you may wind up and collect | recover the 2nd member 201b1 once in roll shape.

  In this figure, the cathode (second electrode) forming step 7 and the cathode buffer layer (electron injection layer) forming step 8 are shown in the case of the vapor deposition apparatus. However, the cathode (second electrode) and the cathode buffer layer (electron injection layer) are shown. There is no particular limitation on the forming method of, for example, sputtering method, reactive sputtering method, molecular beam epitaxy method, cluster ion beam method, ion plating method, plasma polymerization method, atmospheric pressure plasma polymerization method, plasma CVD method, A laser CVD method, a thermal CVD method, a coating method, or the like can be used.

  The cathode buffer layer (electron injection layer) is desirably 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. 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.

  The sealant coating process 2c includes a sealant coating device 2c1, a mounting table 2c2 for mounting the first member 201a1 sent from the first supply process 2a, and an alignment mark attached to the first member 201a1. And a detection device 2c3 for X (see FIG. 4). By the sealant coating device 2c1, an adhesive as a sealant is formed around the functional layer laminated (anode (first electrode) / hole transport layer / light emitting layer) on the first substrate 201a. (First electrode) It is applied except for the extraction electrode A1 (see FIG. 5) of A (see FIG. 5).

  In the bonding step 2d, the first member 201a1 sent from the first supply step 2a and the second member 201b1 sent from the second supply step 2b are combined with the first substrate 201a and the second substrate 201b. The anode (first electrode) A (see FIG. 5) and the cathode (second electrode) E (see FIG. 11) are bonded to each other. By bonding, the organic EL element 202 connected in a band shape is produced. The bonding step 2d will be described with reference to FIGS.

  The punching process 2e includes a punching device 2e1 and an accumulator 2e2. The punching device 2e1 performs punching for individually separating the organic EL elements 202 connected from the bonding process 2d in a band shape. When the punching step 2e is completed, the organic EL element T having the configuration shown in FIG. 1 is manufactured. S shows the roll-shaped skeleton which wound up and collect | recovered the skeleton which punched the organic EL element T. FIG.

  1st supply process 2a, 2nd supply process 2b shown in this figure, sealing agent application process 2c, pasting process 2d, and 1st member 201a1, 2nd member 201b1 to punching process 2e, and belt shape The transportation of the connected organic EL elements 202 is controlled by an EPC (not shown) disposed in the transportation path of each process.

  FIG. 3 is a schematic diagram of a manufacturing process of an organic EL element in which the organic EL element shown in FIG. 1 is manufactured by using a single-wafer base material as a first base material and a second base material, and a bonding method. The case where a glass plate is used as the first substrate and a flexible support is used as the second substrate is shown.

  In the figure, 2 'indicates a manufacturing process. The production process 2 ′ includes a first supply process 2′a, a second supply process 2′b, a sealant coating process 2′c, a bonding process 2′d, and a recovery process 2′e. is doing. The first supply step 2'a shows a case where a first member 201'a1 having at least an anode (first electrode) and at least one organic functional layer formed thereon is supplied to the first base material 201'a. Yes. In the case of this figure, an anode (first electrode) A (see FIG. 5), a hole transport layer B (see FIG. 5), and a light emitting layer C (see FIG. 5) are formed on the first base material 201′a. The hole transport layer and the light emitting layer correspond to the organic functional layer.

  In the first supply step 2'a shown in the figure, an anode (first electrode) A (see FIG. 5), a hole transport layer, and a first base material 201'a for manufacturing an organic EL element used for illumination. The process of supplying the 1st member 201a1 formed in order of B (refer FIG. 5) and the light emitting layer C (refer FIG. 5) is shown. In this figure, since the anode (first electrode) A (see FIG. 5) already formed on the first base material 201′a is used, the anode (first electrode) formation step is omitted. .

  The first supply step 2'a includes a supply step 3 'for the first substrate 201'a, a hole transport layer forming step 4' for forming the hole transport layer B (see Fig. 5), and light emission. And a light emitting layer forming step 5 ′ for forming the layer C (see FIG. 5). The first supply step 2'a shown in this figure is a step in which the supply step 3 'to the light emitting layer forming step 5' are continuously performed under atmospheric pressure conditions. Supply process 3 'has supply part 301'. In the supply part 301 ′, the anode (first electrode) A (see FIG. 5) is already formed, and the first substrate 201′a of the single wafer is supplied. In addition, it is possible to arrange | position the surface treatment part shown by FIG. 2 as needed.

  In the hole transport layer forming step 4 ′, the holding base 401′a for holding the first base material 201′a and the first base material 201′a held by the holding base 401′a are used for forming a hole transport layer. Hole transport layer B (FIG. 5) formed on first wet coater 401′b for applying the coating solution and anode (first electrode) A (see FIG. 5) on first base material 201′a. The first drying device 401′c for removing the solvent (see FIG. 5) and the first heat treatment device 401′d for heating the hole transport layer B (see FIG. 5) from which the solvent has been removed are provided. If necessary, the second antistatic means shown in FIG. 2 can be provided.

  The coating liquid for forming a hole transport layer by the first wet coater 401′b is an anode (except for the extraction electrode A1 (see FIG. 5) of the anode (first electrode) A (see FIG. 5) that has already been formed. The first electrode is applied on A (see FIG. 5).

  As a wet coater that can be used for the first wet coater 401′b, for example, a slit coat method, an inkjet method, a spray method, or the like can be used. The use of these wet coating machines can be appropriately selected according to the material of the organic compound layer.

  As drying conditions for removing the solvent of the hole transport layer in the first drying device 401′c, in consideration of drying unevenness, blown coating surface roughness, etc., the discharge air velocity of the dry air from the discharge port is 0.1 to 5 m / s, airflow drying with a wind speed distribution in the width direction of 0.1 to 10%.

  As the heat treatment conditions for the hole transport layer in the first heat treatment section 401′d, considering the improvement of the smoothness of the hole transport layer, the removal of the residual solvent, the curing of the hole transport layer, etc., the glass of the hole transport layer It is preferable to perform the back surface heat transfer type heat treatment at a temperature that is −30 to + 30 ° C. with respect to the transition temperature and that does not exceed the decomposition temperature of the organic compound constituting the hole transport layer.

  The film thickness of the formed hole transport layer B (see FIG. 5) is the same as that of the hole transport layer shown in FIG. 2, and the materials used are also the same.

  In the light emitting layer forming step 5 ′, the hole transport layer B (FIG. 5) formed on the first base material 201′a having the hole transport layer B (see FIG. 5) held on the holding base 501′a. Remove the solvent of the light emitting layer C (see FIG. 5) formed on the second wet coater 501′b and the hole transport layer B (see FIG. 5). And a second heat treatment apparatus 501'd for heating the light emitting layer C (see FIG. 5) from which the solvent has been removed. If necessary, a third antistatic means shown in FIG. 2 can be provided.

  The coating solution for forming the light emitting layer by the second wet coater 501′b is applied on the hole transport layer B (see FIG. 5) that has already been formed except for the extraction electrode A1 of the anode (first electrode) A. Is done.

  The second wet coater 501'b is preferably of the same type as the first wet coater 401'b.

The hole transport layer forming coating solution used in the first wet coater 401′b and the light emitting layer forming coating solution used in the second wet coater 501′b are at least one organic compound material and at least one. It is preferable that the surface tension is 15 × 10 ^{−3 to} 55 × 10 ⁻³ N / m in consideration of repelling during coating, coating unevenness, and the like.

  The second drying device 501'c has the same structure as the first drying device 401'c. The second heat treatment apparatus 501′d has the same structure as the first heat treatment apparatus 401′d, and the light emitting layer C formed on the hole transport layer B (see FIG. 5) is used as the first base material 201 ′. Heating is performed from the back side of a by the back side heat transfer method. As heat treatment conditions for the light emitting layer C (see FIG. 5) in the second heat treatment apparatus 501′d, the smoothness of the light emitting layer C (see FIG. 5) is improved, the residual solvent is removed, and the light emitting layer C (see FIG. 5) is heated. Considering curing and the like, the glass transition temperature of the light emitting layer C (see FIG. 5) is −30 to + 30 ° C., and does not exceed the decomposition temperature of the organic compound constituting the light emitting layer C (see FIG. 5). It is preferable to carry out heat treatment of the back surface heat transfer system at a temperature.

  When the light emitting layer C (see FIG. 5) is a multilayer, it is necessary to dispose units for the application / drying unit in accordance with the number of layers to be laminated. For example, a white element can be manufactured by forming a light emitting layer in multiple layers. The total film thickness when the light emitting layer is multilayered is the same as that shown in FIG.

  In this way, by completing the light emitting layer forming step 5 ′, the anode (first electrode) A, the hole transport layer B, and the light emitting layer C are formed in this order on the first base material 201′a. The first member 201'a1 is prepared. The first member 201'a1 is subsequently sent to the sealant coating step 2'c. In addition, although this figure has shown the case where it sends to the sealing agent coating process 2c continuously, you may collect | recover 1st member 201'a1 once.

  The hole transport layer forming step and the light emitting layer forming step 5 shown in this figure show a case where there is one wet coating device, a drying device, and a heat treatment device, respectively, but may increase as necessary. It is possible.

  The process of forming the hole transport layer and the light emitting layer, which are the constituent layers of the organic EL element shown in this figure, considers the maintenance of the performance of the hole transport layer and the light emitting layer, the prevention of failure defects due to foreign matter adhesion, etc. Dew point temperature is −20 ° C. or lower, conforms to JISB 9920, measured cleanliness is class 5 or lower, and is formed under atmospheric pressure conditions of 10 to 45 ° C. excluding the first drying section and the second drying section. It is preferable. In the present invention, cleanliness of class 5 or less means class 3 to class 5.

  In the second supply step 2'b, the second member 201b1 having at least a cathode (second electrode) formed on the second base 201'b is supplied. The case of this figure shows the case of the second member 201b1 in which the cathode (second electrode) (not shown) and the cathode buffer layer (electron injection layer) are formed on the second base material 201′b.

  In the second supply step 2'b shown in this figure, a cathode (second electrode) E (see FIG. 11), cathode 2 (second electrode) 201 for producing an organic EL element used for illumination, The process of supplying 2nd member 201'b1 formed in order of the buffer layer (electron injection layer) F (refer FIG. 11) is shown. In addition, you may provide a gas barrier layer between 2nd base material 201'a and cathode (2nd electrode) E (refer FIG. 11).

  The second supply process 2'b includes a supply process 6 'for the sheet-like second base material 201'b, a cathode formation process 7' for forming a cathode (second electrode) E (see FIG. 11), and a cathode E (See FIG. 11) a cathode surface smoothing step 8 ′ for performing a smoothing process, a chamfering step 9 ′ for performing a chamfering process on the peripheral edge of the cathode E (see FIG. 11), and a cathode buffer layer (electronic A cathode buffer layer (electron injection layer) forming step 10 ′ for forming the injection layer) F. The second supply step shown in this figure is a step (dry process step) in which the cathode forming step 7 'and the cathode buffer layer (electron injection layer) forming step 10' are performed under reduced pressure conditions.

  Supply process 6 'has supply part 601' which supplies 2nd substrate 201'b of a sheet to the following process.

  In the cathode (second electrode) forming step 7 ′, the cathode (second electrode) forming portion 701 ′ is positioned on the second base material 201′b at the position of the anode (first electrode) A (see FIG. 5). (Second electrode) E (see FIG. 11) is formed. 701'a indicates a vapor deposition apparatus, and 701'b indicates an evaporation source container.

  The cathode surface smoothing step 8 'has a cathode surface smoothing processing device 8'a. The surface of the cathode (second electrode) E (see FIG. 11) formed on the second base material 201′b is smoothed by the cathode surface smoothing apparatus 8′a. The cathode surface smoothing apparatus 8'a is the same as the cathode surface smoothing apparatus 8a shown in FIG.

  The chamfering process 9 'has a chamfering processing apparatus 9'a. A chamfering process is performed on the peripheral edge of the cathode (second electrode) E (see FIG. 11) formed on the second base material 201′b by the chamfering processing apparatus 9′a. The chamfering processing apparatus 9'a has the same method as the chamfering processing apparatus 9a shown in FIGS. However, the chamfering processing apparatus 9'a shown in this figure has a structure in which a polishing tape 9a3 (see FIG. 7) is disposed on the upper side. The chamfering process 9 'can be arranged as necessary.

  The cathode buffer layer (electron injection layer) forming step 10 ′ includes a cathode buffer layer (electron injection layer) forming portion 1001 ′. In the cathode buffer layer (electron injection layer) forming portion 1001 ′, the extraction electrode E1 is formed on the cathode (second electrode) E (see FIG. 11) processed in the cathode surface smoothing step 8 ′ and the chamfering step 9 ′. A cathode buffer layer (electron injection layer) F (see FIG. 11) is formed except for (see FIG. 6). Reference numeral 1001'a denotes a vapor deposition apparatus, and 1001'b denotes an evaporation source container. By completing the cathode buffer layer (electron injection layer) forming step 10 ′, the cathode (second electrode) E (see FIG. 11) and the cathode buffer layer (electron injection layer) F are formed on the second base material 201′b. A second member 201′b1 formed in the order of (see FIG. 11) is prepared. The second member 201′b1 is subsequently sent to the bonding step 2′d. In addition, although this figure has shown the case where 2nd member 201'b1 is sent to the bonding process 2d continuously, you may collect | recover 1st member 201'b1 once.

  This figure shows the case where the cathode (second electrode) forming step 7 'and the cathode buffer layer (electron injection layer) forming step 9' are vapor deposition apparatuses, but the cathode (second electrode) and the cathode buffer layer (electron injection layer). The method for forming the layer) is not particularly limited, and various methods shown in FIG. 2 can be used.

  The cathode buffer layer (electron injection layer) is desirably 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. 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.

  The sealant coating process 2'c includes a sealant coating apparatus 2'c1 and a mounting table 2'c2 on which the first member 201'a1 sent from the first supply process 2'a is mounted. is doing. The sealant is applied around the functional layer (anode (first electrode) / hole transport layer / light emitting layer) laminated on the first base material 201′a by the sealant coating apparatus 2′c1. The adhesive is applied except for the extraction electrode A1 (see FIG. 5) of the anode (first electrode) A (see FIG. 5).

  In the bonding step 2'd, the first member 201'a1 sent from the first supply step 2'a and the second member 201'b1 sent from the second supply step 2'b The anode (first electrode) A (see FIG. 5) and the cathode (second electrode) E (see FIG. 11) are opposed to each other between the one substrate 201′a and the second substrate 201′b. Paste like so. By bonding, an individual organic EL element 202 ′ is produced and collected in the collecting step 2′e. The bonding step 2′d is the same as the bonding step 2d shown in FIG.

  FIG. 4 is an enlarged schematic perspective view of a portion indicated by U in FIG.

  In the figure, 2c represents a sealing agent coating step. Reference numeral 2c31 denotes a housing of the alignment mark X detection device 2c3. The alignment marks X are attached to the four corners of each functional layer to indicate the position of the functional layer laminated (anode (first electrode) / hole transport layer / light emitting layer) on the first substrate 201a.

  The sealant coating device 2c1 applies a sealant around the functional layer (anode (first electrode) / hole transport layer / light emitting layer) laminated on the first base material 201a according to the information of the detection device 2c3. It is controlled to paint. In order to fix the first member 201a1 on the mounting table 2c2, the mounting table 2c2 is preferably configured to be capable of being fixed by suction, for example. There is no limitation in particular as sealing agent coating apparatus 2c1, For example, a screen printing system, an inkjet system, a dispenser system etc. can be used suitably according to the liquid physical property of sealing agent. The sealing agent coating step shown in this figure is the same as the sealing agent coating step 5 'shown in FIG.

  FIG. 5 is an enlarged schematic view of a portion indicated by V in FIG. FIG. 5A is an enlarged schematic plan view of a portion indicated by V in FIG. FIG. 5B is a schematic cross-sectional view taken along line JJ ′ in FIG.

  In the figure, A indicates an anode (first electrode) laminated on the first base material 201a. B represents a hole transport layer laminated on the anode (first electrode) A including the periphery of the anode (first electrode) A, excluding the extraction electrode A1 of the anode (first electrode) A. C represents a light emitting layer laminated on the hole transport layer B. D shows the adhesive of the sealing agent coated around the functional layer laminated | stacked on the 1st base material 201a (anode (1st electrode) / hole transport layer / light emitting layer). The adhesive D should just have the height which contacts the 2nd base material 201b, when bonding 2nd member 201b1 at a bonding process. The state in which the adhesive D shown in this figure is applied is the same as that in the case of the first base material 201′a shown in FIG.

  FIG. 6 is a schematic enlarged perspective view of the cathode surface smoothing step shown in FIG.

  In the figure, 8a represents a cathode surface smoothing apparatus. Reference numeral 8a1 denotes a detection device for the alignment mark Y provided to indicate the position of the cathode (second electrode) E formed on the second base material 201b, and 8a11 denotes a housing of the detection device 8a1. The alignment mark Y is provided to indicate the positions of the four corners of the cathode (second electrode) E. The cathode (second electrode) surface smoothing processing device 8a fixes the second member 201b1 in the cathode (second electrode) surface smoothing processing device 8a according to the information of the detection device 8a1, and the cathode (second electrode) E It is possible to perform a smoothing process on the surface E2.

  The surface roughness Ra of the cathode (second electrode) after the smoothing treatment is preferably from 0.3 nm to 3.0 nm, and more preferably from 0.3 nm to 1.5 nm. When the surface roughness Ra is less than 0.3 nm, there is no problem on the performance because it is smooth, but it is not preferable from the viewpoint of production because the processing time required to satisfy the required level becomes long. When the surface roughness Ra exceeds 3.0 nm, the smoothness as an electrode is insufficient, which causes an image defect such as a leak or a short circuit due to a projection or the like, which is not preferable.

  The surface roughness Ra indicates a value measured by an atomic force microscope (AFM) SPA300 manufactured by SII Nano Technology. A dry etching apparatus is used as the cathode (second electrode) surface smoothing apparatus 8a. The cathode (second electrode) surface smoothing apparatus 8a is not particularly limited. For example, a reactive gas etching apparatus, an atmospheric pressure plasma reactive ion etching apparatus, a reduced pressure plasma reactive ion etching apparatus, a reactive ion beam etching apparatus, Examples thereof include an ion beam etching apparatus, a reactive laser beam etching apparatus, and a laser beam etching apparatus. Among these, a low pressure plasma reactive ion etching apparatus is preferable. These various dry etching apparatuses can use commercially available dry etching apparatuses. 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.

The step of surface smoothing treatment of the cathode (second electrode) will be described below using a reduced pressure plasma reactive ion etching device as the cathode surface smoothing treatment device 8a.
In S1, conditions (pressure reduction degree, introduced gas concentration, plasma output) of the reduced pressure plasma reactive ion etching apparatus are set according to the material of the second electrode.
In S2, the alignment mark (not shown) attached to the fixing base (not shown) and the alignment mark Y attached to the second member 201b1 are aligned and then fixed.
In S3, the smoothing process is started.
In S4, after the smoothing process is finished, the fixation from the fixing base (not shown) is once released, and the second member 201b1 moves until the position of the next second electrode comes to the position of the fixing base (not shown). By performing the process of S3, the surface smoothing process of each second electrode E of the second member 201b1 is sequentially performed.

  Incidentally, the cathode (second electrode) surface smoothing process by the cathode (second electrode) surface smoothing apparatus 8'a shown in FIG. 3 is also performed at the same stage as S1 to S4, and after the surface smoothing process is performed. The surface roughness of the cathode (second electrode) has the same result.

A second electrode that has been subjected to a surface smoothing treatment of the second electrode by a cathode (second electrode) surface smoothing treatment apparatus as shown in the figure is produced and bonded to the first member to produce an organic EL element. The following effects were obtained.
1) The distance between the first electrode and the second electrode becomes stable, there is no place where electric field concentration occurs, leakage current from the surface of the second electrode is suppressed, and power consumption can be reduced and luminous efficiency can be improved. It became.
2) With the improvement of the quality of organic EL elements, it has become possible to improve production efficiency and industrial utility value.

  FIG. 7 is an enlarged schematic view of the chamfering process shown in FIG. FIG. 7A is an enlarged schematic perspective view of the chamfering process shown in FIG. FIG. 7B is a schematic cross-sectional view along KK ′ in FIG.

  In the figure, reference numeral 9a denotes a chamfering processing apparatus. 9a1 indicates a detection device for the alignment mark Y provided to indicate the position of the cathode (second electrode) E formed on the second base material 201b, and 9a11 indicates a housing of the detection device 9a1. The alignment mark Y is provided to indicate the positions of the four corners of the cathode (second electrode) E. The chamfering processing device 9a fixes the second member 201b1 sent from the cathode surface smoothing step 8 in the chamfering processing device 9a according to the information of the detection device 9a1, and ends around the cathode (second electrode) E. It is possible to perform chamfering processing on the sides E2 to E5.

  The chamfering processing apparatus 9a has a main body 9a1 and a fixing base 9a2 for fixing the second member 201b1. The method for fixing the second member 201b1 to the fixing base 9a2 is not particularly limited, and examples thereof include vacuum suction, electrostatic suction, and a holding member method. This figure shows the case of the suction method. Reference numeral 9a21 denotes a suction pipe for fixing the second member 201b1 to the fixing base 9a2, and is connected to a suction pump (not shown). A plurality of suction holes (not shown) are formed in the contact surface 9a22 of the fixing base 9a2 with the second member 201b1. The number of holes (not shown) can be appropriately changed depending on the size of the second member 201b1.

  Also, the size of the hole (not shown) can be selected from the suction pressure required for fixing since it is important that the flatness of the second member 201b1 does not change when sucked. Yes.

  Reference numeral 9a12 denotes a suction tube for discharging dust (dust) generated when chamfering the edges E3 to E6 around the cathode (second electrode) to the outside of the main body 9a1, and the polishing tape 9a3 and the cathode (first electrode) A plurality of suction pipes are arranged along the width direction on both sides in contact with the two electrodes, and each suction pipe is connected to a suction pump (not shown).

  Reference numeral 9a3 denotes an abrasive tape. As the polishing tape 9a3, one obtained by uniformly applying a polishing material (for example, cerium oxide having a particle size of 0.1 to 9 μm) to a substrate (for example, PET) can be used. Reference numeral 9a31 denotes a supply portion of the polishing tape 9a1, and 9a312 denotes an original winding roll wound around the winding core 9a311. Reference numeral 9a32 denotes a winding portion of the polishing tape 9a3, and 9a322 denotes a used roll wound around the winding core 9a321 after use.

  The winding core 9a311 and the winding core 9a321 are rotatably arranged on the frame of the main body 9a1, and in the case of this figure, the winding core 9a321 is attached to a driving rotary shaft (not shown). The drive rotation shaft (not shown) is connected to a drive motor (not shown). The winding core 9a311 of the original winding roll 9a312 is attached to a rotating shaft (not shown) with a brake. The tension of the polishing tape 9a3 can be adjusted by the brake.

  In consideration of the chamfering processability of the edges E2 to E5 around the cathode (second electrode) E, the conveying speed of the polishing tape 9a3 during polishing is preferably 1 to 50 mm / sec. The width of the polishing tape 9a3 is preferably +5 to + 10% with respect to the processed width of the cathode (second electrode) in consideration of chamfering processability, processing accuracy, and the like.

  Reference numeral 9a4 denotes a contact roll for bringing the polishing tape 9a3 into contact with the edges E2 to E5 around the cathode (second electrode) E formed on the second substrate 201b. The contact roll 9a4 is in contact with only the edges E2 to E5 around the polishing tape 9a3 and the cathode (second electrode) E, in the vertical direction (in the direction of the arrow in the figure) and in the diagonal direction (one side is on the edge). And the other side is controlled so as to be movable away from the edge, and is arranged on the frame of the main body.

  As the polishing tape 9a3, it is possible to select and use one that meets the conditions from among commercially available tapes. For example, Nippon Micro Coating Co., Ltd. Mipox ultra-precision polishing tape is mentioned.

  The pressing weight during polishing is preferably 0.5 to 10 N in consideration of the chamfered shape of the edge around the cathode (second electrode) E.

  The rubber hardness of the contact roll 9a4 is preferably 30 to 90 ° in consideration of the chamfered shape of the edge around the cathode (second electrode) E. The rubber hardness is a value measured according to JIS K6253. The width of the contact roll 9a4 is equal to the width of the cathode (second electrode) E in consideration of the transportability of the abrasive tape, the abrasiveness of the edges around the cathode (second electrode) E, and the like relative to the width of the abrasive tape 9a3. It is preferable that it is + 5- + 20% with respect to.

  The main body 9a1 contacts the polishing tape 9a3 with the edges E2 to E5 around the cathode (second electrode) E formed on the second base 201b fixed to the contact surface 9a22 of the fixing base 9a2. It can move at a speed of 5 to 50 mm / sec along the longitudinal direction of the two electrodes.

The stage of the chamfering process of the cathode (second electrode) using the polishing apparatus 9a shown in this figure will be described next.
In S1, the count of the polishing tape 9a3 to be used, the rubber hardness of the contact roll 9a4, and the pressing weight are determined by the material of the second electrode.
In S2, the winding speed of the polishing tape 9a3 and the moving speed of the main body are determined.
In S3, the alignment mark (not shown) attached to the contact surface 9a22 of the fixing base 9a2 and the alignment mark Y attached to the second member 201b1 are aligned, and then fixed by suction.
In S4, the contact roll 9a4 is lowered to bring the polishing tape 9a3 into contact with the end E4 of the cathode (second electrode). At this time, the chamfering process is performed in a state where the entire surface of the polishing tape 9a3 is in contact with the entire length in the width direction of the end E4. After the chamfering process for the edge E3 is completed, the chamfering process for the edge E2 is performed. At this time, one side of the contact roll 9a4 is raised upward so that only a part of one side of the polishing tape 9a3 comes into contact with the end E2, and the main body extends in the longitudinal direction of the cathode (second electrode) E. 9a moves and a chamfering process is performed. After the end edge E2 is chamfered, the end edge E5 is chamfered. At this time, the polishing tape 9a3 comes into contact with the end side E5 and the processing is performed in the same manner as the chamfering processing of the end side E4. After the chamfering process for the edge E5 is completed, the chamfering process for the edge E3 is performed. At this time, one side of the contact roll 9a4 is raised upward so that only a part of one side of the polishing tape 9a3 comes into contact with the end E3, and the main body extends in the longitudinal direction of the cathode (second electrode) E. 9a moves and a chamfering process is performed. In this figure, the order of the chamfering processing is shown in the case of the end side E4, the end side E2, the end side E5, and the end side E3, but the order is not particularly limited. In addition, it is preferable that the contact between the polishing tape 9a3 and the end sides E2 to E5 and the movement of the main body 9a1 can be automatically controlled according to the order of the chamfering processing. While the chamfering process is being performed, suction by the suction pipe 9a12 is performed, and dust is discharged outside.
In S5, after the chamfering process of the end sides E2 to E5 is finished, the fixation from the contact surface 9a22 is once released, and the second member 201b1 is positioned at the position of the contact surface 9a22 of the fixing base 9a2. The chamfering process is sequentially performed on the end sides E2 to E5 of the respective cathodes (second electrodes) E of the second member 201b1 by moving to S3 and performing the operation from S3.

  The chamfering process of the edge of the cathode (second electrode) by the chamfering processing apparatus shown in this figure can be performed by the same method even when the single wafer support shown in FIG. 3 is used.

  FIG. 8 is a schematic view of a portion indicated by W in FIG. FIG. 8A is a schematic enlarged plan view of a portion indicated by W in FIG. 7 showing a state where the chamfering processing is performed by the chamfering processing apparatus shown in FIG. FIG. 8B is a schematic cross-sectional view taken along line LL ′ of FIG. FIG. 8C is a schematic cross-sectional view showing the shape of the other end of FIG. 8B.

  This will be described with reference to FIG. This figure shows the state where the edges C3 to E6 around the second electrode E have been subjected to the chamfering processing by the chamfering processing apparatus shown in FIG.

  This will be described with reference to FIG. This figure has shown the case where chamfering was performed to the surface shape in which the edge side inclined.

  In the figure, E51 indicates an inclined surface formed by cutting the end E6 by chamfering processing. θ is the slope E51 when the plane E2 of the cathode (second electrode) E (the organic functional layer of the first member (for example, the surface facing the light emitting layer) when bonded to the first member) is used as a reference. Indicates the angle. The angle θ depends on the chamfering variation, the edge part protrudes from the horizontal surface of the electrode surface, the distance between the first electrode and the second electrode is shortened, electric field concentration occurs, and due to the shadowing phenomenon when forming the organic compound layer, In consideration of electric field concentration due to the generation of the thin film portion, leakage due to contact with the first electrode, short circuit, etc., 5 ° to 80 ° is preferable. The angle θ represents a value obtained by measuring the step shape with an atomic force microscope (AFM) SPA300 manufactured by SII Nano Technology. The other end sides E3 to E5 are also chamfered as shown in the figure.

  This will be described with reference to FIG. This figure shows a case where chamfering is performed to a surface shape with curved edges.

  In the figure, E52 indicates a curved surface formed by cutting off the edge E6 by the chamfering process. R of the curved surface is the occurrence of electric field concentration because the thin film portion is generated due to the shadowing phenomenon during the formation of the organic compound layer when the thickness of the cathode (second electrode) E is t, and the first electrode edge portion The region where the thickness is reduced becomes large, and t / 20 to 2t is preferable in consideration of generation of light emission unevenness, leakage due to contact with the first electrode, short circuit, and the like. The other end sides E3 to E5 are also chamfered as shown in the figure.

  The chamfered shape of the edge around the cathode (second electrode) shown in this figure is the same when the single wafer support shown in FIG. 3 is used.

The following effects can be obtained by chamfering the peripheral edge of the cathode (second electrode) with a chamfering apparatus as shown in FIGS. 7 and 8 and bonding it to the first member to produce an organic EL element. It was.
1) In addition to the effect of smoothing the surface of the cathode (second electrode) shown in FIG. 6, the distance between the edge of the cathode (second electrode) and the first electrode is stabilized, and electric field concentration occurs. Further, the leakage current from the edge portion of the second electrode is suppressed, and the power consumption can be reduced and the light emission efficiency can be improved.
2) With the improvement of the quality of organic EL elements, it has become possible to improve production efficiency and industrial utility value.

  FIG. 9 is a schematic view of the bonding step shown in FIG. Fig.9 (a) is a general | schematic expanded perspective view of the bonding process shown by FIG. FIG. 9B is a schematic enlarged sectional view taken along line MM ′ of FIG.

  In the figure, 2d indicates a bonding step. The bonding step 2d includes a bonding device 2d1, a first alignment mark detection device 2d2, and a second alignment mark detection device 2d3 each having an outer box 2d11 and a pair of upper and lower thermocompression bonding rolls 2d12. Reference numeral 2d21 denotes a housing of the first alignment mark detection device 2d1. Reference numeral 2d31 denotes a second alignment mark detection device 2d3 casing. Reference numeral 2d13 denotes a suction pipe, which is connected to a vacuum pump (not shown). When laminating the first member 201a1 and the second member 201b1, it is possible to operate a vacuum pump (not shown) and make the inside of the outer box 2d11 in a reduced pressure environment.

  The first alignment mark detection device 2d2 detects the alignment mark X (see FIG. 4) attached to the first member 201a1 sent from the sealant coating step 2c (see FIGS. 2 and 4). The information detected by the alignment mark detection device 2d2 is input to a control unit (not shown), and the second member sent from the second supply step 2b (see FIGS. 6 to 8) determines the conveyance speed of the first member 201a1. Control can be performed so as to coincide with the alignment mark Y (see FIGS. 6 to 8) attached to 201b1.

  The second alignment mark detection device 2d3 detects the alignment mark Y (see FIGS. 6 to 8) attached to the second member 201b1 sent from the second supply step 2b (see FIGS. 6 to 8). Information detected by the second alignment mark detection device 2d3 is input to a control unit (not shown) and attached to the first member 201a1 sent from the sealant coating step 2c (see FIGS. 2 and 4). Control can be performed so as to coincide with the alignment mark X.

  In the bonding step 2d, the light emitting layer C of the first member 201a1 and the cathode buffer layer (electron injection layer) F of the second member 201b1 sent from the sealant coating step 2c (see FIGS. 2 and 4). And the cathode buffer layer (electron injection layer) F and the light emitting layer C are bonded together by thermocompression bonding under reduced pressure. After bonding, the individual organic EL elements in a state where the anode (first electrode) and the cathode (second electrode) face each other between the first base material and the second base material are continuously connected. It becomes.

  Sealing agent applied around the functional layer laminated (anode (first electrode) / hole transport layer / light emitting layer) on the first base material 201a of the first member 201a1 in accordance with the pasting. The adhesive D and the second base material 201b of the second member 201b1 are bonded to each other, and the individual organic EL elements 202 (FIG. 5) are sealed between the first base material 201a and the second base material 201b with an adhesive. 2) is completed.

  Bonding using the bonding apparatus shown in this figure shows a case using a thermocompression bonding roll in a reduced pressure environment, but the heating method is not particularly limited, for example, heating the entire interior, using a heating roll, etc. Can be mentioned. Among these, it is preferable to use a heating roll to which heat is directly transmitted from the viewpoint of bonding stability and adhesion stability. This figure has shown the case where a heating roll is used.

  The temperature and pressure reduction during the press bonding of the laminating apparatus 2d1 shown in this figure vary depending on the type of adhesive used, the type of light emitting layer, and the type of cathode buffer layer (electron injection layer), so it must be uniquely determined. Although it is difficult, it is necessary to determine by prior experiments within a range that does not affect each layer constituting the organic EL element.

  FIG. 10 is a schematic enlarged cross-sectional view of another bonding apparatus used in the bonding step shown in FIG.

In the figure, 2d′1 represents a bonding apparatus. The laminating apparatus 2d′1 has a main body 2d′12 having a fixing base 2d′13, a first crimping member 2d′14, and a second crimping member 2d′15.
Reference numeral 2d'12 denotes a suction pipe disposed in the main body 2d'12 and is connected to a vacuum pump (not shown). Reference numeral 2d'131 denotes a suction pipe disposed on the fixed base 2d'13, which is connected to a vacuum pump (not shown). When the first member 201a1 and the second member 201b1 are bonded, a vacuum pump (not shown) is connected. ) And the inside of the outer box 2d11 can be performed in a reduced pressure environment.

  Reference numeral 2d'16 denotes an alignment mark detection device disposed on the main body 2d'12. The alignment mark detection device is arranged at the same position as the alignment mark Y (see FIG. 9) attached to the second member 201b1.

  A plurality of suction holes (not shown) are formed in the surface 2d'132 of the fixing base 2d'13. The number of holes (not shown) can be appropriately changed depending on the sizes of the first member 201a1 and the second member 201b1 to be bonded. The size of the hole (not shown) is also selected from the suction pressure required for fixing because it is important that the flatness of the first member 201a and the second member 201b does not change when sucked. It is possible.

  Fixing to the fixing base 2d'13 is performed with the alignment mark X (see FIG. 9) attached to the first member 201a1 and the alignment mark Y (see FIG. 9) attached to the second member 201b1 being aligned. When sent onto the table 2d'13, the alignment mark X attached to the first member 201a1 (see FIG. 9) or the alignment mark Y attached to the second member 201b1 by the alignment mark detector 2d'16. (See FIG. 9), and a vacuum pump (not shown) connected to the suction pipe 2d'131 disposed on the fixing base 2d'13 is operated to fix it to the fixing base 2d'13. It is like.

  The first crimping member 2d'14 preferably has a rectangular shape in order to crimp the adhesive D (see FIG. 5) at a time. Moreover, it is preferable to be able to heat depending on the kind of adhesive to be used. Reference numeral 2d'141 denotes a cylinder for moving the first pressure-bonding member 2d'14 in the upward and downward direction (in the direction of the arrow in the figure).

  The second pressure-bonding member 2d'15 is formed on the portion corresponding to the anode (first electrode) / hole transport layer / light-emitting layer formed on the first base material 201a or on the second base material 201b. One of the portions corresponding to the cathode (second electrode) / cathode buffer layer (electron injection layer) is pressure-bonded. Reference numeral 2d'151 denotes a cylinder that moves the second pressure-bonding member 2d'15 upward and downward (in the direction of the arrow in the drawing). The second crimping member 2d'15 has a heating means so that thermocompression bonding can be performed.

  The temperature at the time of pressure bonding of the laminating apparatus 2d'1 shown in this figure and the degree of reduced pressure vary depending on the type of adhesive used, the type of light emitting layer, and the type of cathode buffer layer (electron injection layer). Although it is difficult to determine, it is necessary to determine by prior experiments within a range that does not affect each layer constituting the organic EL element.

Next, the step of bonding the first member 201a1 and the second member 201b1 using the bonding apparatus 2d'1 shown in this figure will be described.
In S1, the bonding apparatus 2d'1 matched with the first member 201a1 and the second member 201b1 is prepared.
In S2, the temperature of the first pressure-bonding member 2d'14 and the pressure to be pressure-bonded are determined according to the type of adhesive, and the first pressure-bonding member 2d'14 is heated and the cylinder 2d'14 is adjusted. Further, the temperature of the second pressure-bonding member 2d'15 and the pressure for pressure-bonding are determined according to the types of the light-emitting layer and the cathode buffer layer (electron injection layer), and the heating of the second pressure-bonding member 2d'15 and the adjustment of the cylinder 2d'151. Is done.
In S3, the alignment mark X (see FIG. 9) attached to the first member 201a1 is aligned with the alignment mark Y (see FIG. 9) attached to the second member 201b1. Then, the alignment mark detection device 2'd16 reads the alignment mark Y (see FIG. 9) attached to the second member 201b1, and the suction pipe 2d'131 provided on the fixed base 2d'13. The vacuum pump (not shown) connected to is operated and fixed to the fixing base 2d'13. If necessary, the inside of the main body 2d'12 is decompressed by operating a vacuum pump (not shown).
In S4, the first pressure-bonding member 2d'14 and the second pressure-bonding member 2d'14 are lowered and thermocompression bonding is performed. The pressure bonding is preferably performed first by the second pressure bonding member 2d'14 in order to increase the adhesion between the light emitting layer and the cathode buffer layer (electron injection layer).
In S5, after the crimping is finished, the first crimping member 2d'14 and the second crimping member 2d'14 are raised, the fixation is released, and they are sent out of the pasting device 2d'1, and the next pasting part Is sent to the fixed base 2d'13. Thereafter, the operation from S3 is performed, so that the anode (first electrode) A (see FIG. 11) and the cathode (second electrode) E are sequentially placed between the first substrate 201a and the second substrate 201b. (Refer to FIG. 11), and an organic EL element 202 is manufactured in which individual organic EL elements in which the space between the first base material 201a and the second base material 201b is sealed with the adhesive D are continuously connected. Is done.

  The pasting of the first base material and the second base material by the pasting apparatus shown in FIGS. 9 and 10 can also be used in the pasting step 2′d shown in FIG. 3 and shown in FIGS. The 1st base material and the 2nd base material which use a sheet support in the same conditions and a stage as a pasting device are attained.

  FIG. 11 is a schematic view showing a state of the first member and the second member before and after bonding by the bonding apparatus shown in FIG. Fig.11 (a) is a schematic enlarged view which shows the state (part shown by Q of FIG. 10) of the 1st member and 2nd member before bonding by the bonding apparatus shown by FIG. FIG.11 (b) is a schematic enlarged view which shows the state (part shown by R of FIG. 10) of the 1st member and 2nd member after bonding by the bonding apparatus shown by FIG.

  A description will be given of the state shown in FIG. Information related to the alignment mark X (see FIG. 9) attached to the first member 201a1 read by the alignment mark detection device 2d2 disposed before the bonding step 2d and read by the alignment mark detection device 2d3. In addition, the alignment mark X (see FIG. 9) and the alignment mark Y (see FIG. 9) are sent together from the information regarding the alignment mark Y (see FIG. 9) attached to the second member 201b1. . At this stage, the anode (first electrode) A and the cathode (second electrode) E are opposed to each other.

  A description will be given of the state shown in FIG. Heat is applied in a state where the portion of the second base material 201b corresponding to the portion where the adhesive D is applied is reduced in pressure by the first pressure-bonding member 2d'14 (see FIG. 10) of the bonding apparatus 2d′1 (see FIG. 10). The 2nd base material 201b and the 1st base material 201a are pasted up via adhesive D by carrying out pressure bonding. Further, the portion of the second base material 201b corresponding to the portion where the cathode (second electrode) is formed by the second pressure-bonding member 2d'15 (see FIG. 10) of the bonding apparatus 2d′1 (see FIG. 10) is decompressed. By thermocompression bonding in this state, the light emitting layer C and the cathode buffer layer (electron injection layer) are brought into close contact with each other, and an organic EL element sealed with an adhesive as shown in FIG. 1 is manufactured.

The following effect is mentioned by manufacturing an organic EL element with the manufacturing method by the bonding method shown by FIGS.
1. For each layer constituting the organic EL element, a member from the first electrode (anode) to the light emitting layer that can be formed by a wet coating method, and a vapor deposition method under a reduced pressure condition that has conventionally been a rate-limiting improvement in production efficiency Production efficiency can be improved by dividing the members including the second electrode (cathode) to be formed separately and separately manufacturing and bonding them.
2. At the time of bonding, the distance between the first electrode and the second electrode becomes stable, there is no place where electric field concentration occurs, leakage current from the surface of the second electrode is suppressed, power consumption is reduced, and luminous efficiency is improved. It has become possible.
3. With the improvement in the quality of organic EL elements, it has become possible to improve production efficiency and industrial utility value.
4). Since close-sealing is possible at the same time as pasting, the process can be simplified and the production efficiency can be improved.

  Hereinafter, the first substrate, gas barrier layer, first electrode, hole transport layer, light emitting layer, cathode buffer layer (electron injection layer), second electrode, and second substrate constituting the organic EL device of the present invention. A description will be given of the sealing member and the like.

1st base material When using a strip | belt-shaped base material as a 1st base material, a transparent resin film is mentioned. 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, Cycloolefin resins such as polyether imide, polyether ketone imide, polyamide, fluororesin, nylon, polymethyl methacrylate, acrylic or polyarylate, Arton (trade name, manufactured by JSR) or Appel (trade name, manufactured by Mitsui Chemicals) Is mentioned. Moreover, when using a sheet | seat base material, in addition to these resin films, a transparent glass plate is mentioned.

Gas Barrier Layer Examples of the gas barrier layer provided on the surface of the resin film as needed include inorganic and organic gas barrier films or a hybrid gas barrier film of both.

  As a material for forming the gas barrier film, any material may be used as long as it has a function of suppressing intrusion of an element such as moisture or oxygen that causes deterioration of the element. 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. For example, the vacuum deposition method, the sputtering method, the reactive sputtering method, the molecular beam epitaxy method, the cluster ion beam method, the ion plating method, the plasma polymerization method, the atmospheric pressure plasma weighting. A combination method, a plasma CVD method, a laser CVD method, a thermal CVD method, a coating method, and the like can be used, but an atmospheric pressure plasma polymerization method as described in JP-A-2004-68143 is particularly preferable. The material used for these gas barrier layers can also be used for the second strip-shaped flexible support and the strip-shaped flexible adhesive member.

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, the oxygen permeability ^{10- 3 ml / m 2 / day} / atm or less, is preferably a high barrier film follows the water vapor transmission rate ^{10- 5 g / m 2 / day} .

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. Or when using the substance which can be apply | coated like an organic electroconductive compound, wet film-forming methods, such as a printing system and a coating system, can also be used. 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.

(Hole injection layer (anode buffer 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”. The details of the anode buffer layer (hole injection layer) are described in JP-A Nos. 9-45479, 9-260062, and 8-288069. Specific examples thereof include copper phthalocyanine. Examples thereof include a phthalocyanine buffer layer, an oxide buffer layer typified by vanadium oxide, an amorphous carbon buffer layer, and a polymer buffer layer using a conductive polymer such as polyaniline (emeraldine) or polythiophene.

Hole transport layer 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.

Light emitting layer The material used for the light emitting layer according to the present invention is not particularly limited. For example, Toray Research Center Co., Ltd. Latest trends of flat panel displays Current state of EL displays and latest technological trends Various types of materials as described on pages 228 to 332 Materials.

  The light emitting layer according to the present invention 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 refers to 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 organic EL device according to the present invention and the color emitted by the compound are shown in FIG. 4.16 on page 108 of “New Color Science Handbook” (Edited by the Japan Color Society, University of Tokyo Press, 1985). -1000 (manufactured by Konica Minolta Sensing Co., Ltd.) is determined by the color when the result of fitting to the CIE chromaticity coordinates.

Electron transport layer In addition to the electron transport material used for the electron transport layer adjacent to the light emitting layer (also serves as a hole blocking material), as long as it has a function of transmitting electrons injected from the cathode to the light emitting layer Well, as the material, any one of conventionally known compounds can be selected and used. For example, nitro-substituted fluorene derivatives, diphenylquinone derivatives, thiopyrandioxide derivatives, carbodiimides, fluorenylidenemethane derivatives, Anthraquinodimethane and anthrone derivatives, oxadiazole derivatives and the like can be mentioned. 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 electron transport layer can also be formed by thinning the electron transport material by a known method such as wet coating or vacuum deposition.

Electron injection layer (cathode buffer layer)
The electron injection layer (cathode buffer layer) formed in the electron injection layer forming step 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). Details of the electron injection layer (cathode buffer layer) are described in JP-A-6-325871, JP-A-9-17574, JP-A-10-74586, and the like. Specifically, strontium, aluminum, etc. A metal buffer layer typified by lithium fluoride, an alkali metal compound buffer layer typified by lithium fluoride, an alkaline earth metal compound buffer layer typified by magnesium fluoride, an oxide buffer layer typified by aluminum oxide, etc. .

Second Electrode As the second electrode, a material having a low work function (4 eV or less) metal (referred to as an electron injecting metal), an alloy, an electrically conductive compound, and a mixture thereof 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.

  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.

As the second substrate, the same substrate as the transparent glass plate and the first substrate can be used. Moreover, the same thing as a 1st base material can be used as a strip | belt-shaped base material.

Sealing member (adhesive)
As sealing members (adhesives), photo-curing and thermosetting adhesives having reactive vinyl groups such as acrylic acid oligomers and methacrylic acid oligomers, and moisture-curing adhesives such as 2-cyanoacrylates , Epoxy and other heat and chemical curable adhesives (mixed with two components), polyamide, polyester and polyolefin hot melt adhesives, and cationic curable UV curable epoxy resin adhesives. I can do it. In addition, since the organic layer which comprises an element may deteriorate with heat processing, what can be adhesive-hardened from room temperature to 80 degreeC is preferable. Moreover, it is preferable that the above-mentioned gas barrier layer is formed on the back surface side of the adhesive layer of the belt-like flexible adhesive member as necessary.

  The organic EL device of the present invention preferably uses the following method in combination 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 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 gratings is preferably two-dimensionally repeated, such as a square lattice, a triangular lattice, or a honeycomb lattice.

  Furthermore, the organic EL device of the present invention is processed so as to provide, for example, a structure on the microlens array on the light extraction side of the substrate in order to efficiently extract light generated in the light emitting layer, or so-called condensing. By combining with the sheet, the luminance in the specific direction can be increased by collecting light in a specific direction, for example, in 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, a substrate may be formed with a Δ-shaped stripe having an apex angle of 90 degrees and a pitch of 50 μm, or the apex angle is rounded and the pitch is changed randomly. Other shapes may be used. 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
Using the manufacturing process shown in FIG. 2, the first substrate / anode (first electrode) / hole transport layer / light emitting layer / cathode buffer layer (electron injection layer) / cathode (second electrode) / second substrate A surface-emitting organic EL device having the layer structure was prepared. In addition, the chamfering process of the edge around the second electrode was not performed.

Preparation of first member <Preparation of first base material having gas barrier layer and anode (first electrode) layer in this order on first base material>
Using a polyethersulfone film (made by Sumitomo Bakelite, hereinafter abbreviated as PES) having a thickness of 200 μm and a width of 200 mm as a first base material, a gas barrier layer and a first electrode are formed by the method described below, and a gas barrier is formed. A first substrate having a layer and an anode (first electrode) in this order was prepared. In addition, the alignment mark was previously provided in the position which forms an anode (1st electrode) in the 1st base material as shown in FIG.

(Formation of a transparent gas barrier layer)
A transparent gas barrier layer having a thickness of about 90 nm was formed on the prepared PES 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 / atm or less.

(Formation of anode (first electrode))
On the formed barrier layer, ITO (indium tin oxide) with a thickness of 120 nm is patterned by vapor deposition, and an anode (first electrode) having a 40 mm × 40 mm take-out electrode as shown in FIG. Formed. The effective pixel area of the anode (first electrode) is 100 mm square.

(Preparation of coating solution for hole transport layer formation)
A solution prepared by diluting polyethylene dioxythiophene / polystyrene sulfonate (PEDOT / PSS, Baytron P AI 4083 manufactured by Bayer) with pure water at 65% and methanol at 5% was prepared as a coating solution for forming a hole transport layer. 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).

(Formation of hole transport layer)
A prepared hole transport layer is formed on the entire upper surface of the anode (first electrode) formed by using the first substrate prepared using the step shown in FIG. The forming coating solution was applied and dried by a wet coating method using an extrusion coating machine to form a hole transport layer having a thickness of 50 nm.

Before applying the coating liquid for forming the hole transport layer, the surface modification treatment of the first substrate was performed 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. . The charge removal treatment was performed using a static eliminator with weak X-rays.

  The conveyance speed was 2 m / min. The conveyance speed was measured with a laser Doppler velocimeter LV203 manufactured by Mitsubishi Electric Corporation.

Application conditions The temperature at the time of application | coating of the coating liquid for positive hole transport layer formation was 25 degreeC, and it was performed by the atmospheric environment of 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 coating the hole transport layer forming coating solution, the first drying device and the first heat treatment device shown in FIG. 2 are used. After removing the solvent at a height of 100 mm, a discharge wind speed of 1 m / s, a wide wind speed distribution of 5%, and a temperature of 100 ° C., a backside heat transfer system heat treatment is subsequently performed at a temperature of 200 ° C. in a first heat treatment apparatus. A hole transport layer was formed.

(Preparation of light emitting layer forming coating solution)
The dopant material Ir (ppy) ₃ is mixed with the host material polyvinyl carbazole (PVK) so as to be 5% by mass and dissolved in 1,2-dichloroethane to form a 1% by mass solution as a light emitting layer forming coating solution. Got ready. 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.

(Formation of light emitting layer)
The process shown in FIG. 2 is used, followed by electrification. Excluding the anode (first electrode) extraction electrode portion on the entire surface of the formed hole transport layer, the prepared light emitting layer forming coating solution is exposed. A light emitting layer having a thickness of 100 nm was formed by coating and drying by a wet coating method using a roux coating machine. The conveyance speed was 2 m / min. The conveyance speed was measured with a laser Doppler velocimeter LV203 manufactured by Mitsubishi Electric Corporation.

Application conditions The temperature at the time of application | coating of the coating liquid for light emitting layer formation was performed in the atmospheric environment of 25 degreeC environment. The wet coating process was performed with a dew point temperature of −20 ° C. or lower and a cleanliness class of 5 or lower (JIS B 9920).

Drying and heat treatment conditions After applying the light emitting layer forming coating solution, the second drying device and the second heat treatment device are used. In the second drying device, the height from the slit nozzle type discharge port to the film formation surface is 100 mm. Then, after removing the solvent at a discharge wind speed of 1 m / s, a wide wind speed distribution of 5%, and a temperature of 60 ° C., heat treatment was subsequently performed at a temperature of 200 ° C. in a second heat treatment apparatus to form a light emitting layer.

(Coating agent coating)
An adhesive (manufactured by Nagase ChemteX Corporation, UV resin XNR5570-B1) was prepared as a sealant. As shown in FIG. 5, around the laminate of the anode (first electrode) / hole transport layer / light emitting layer formed on the first substrate, preparation is made except for the portion serving as the extraction electrode for the anode (first electrode). The prepared adhesive was applied to form a first member.

Preparation of second member <Preparation of second substrate having cathode (second electrode) layer and cathode buffer layer (electron injection layer) in this order on second substrate>
Preparation of second base material The same base material as the first base material was prepared. An alignment mark is provided as shown in FIG. 6 at a position where the cathode (second electrode) is formed in advance, in alignment with the position of the alignment mark provided for the anode (first electrode) shown in FIG.

(Formation of cathode (second electrode))
On the second substrate prepared in the cathode (second electrode) forming step shown in FIG. 2, the mask is adjusted to the size and position of the anode (first electrode) under a vacuum condition of 5 × 10 ⁻⁴ Pa. As shown in FIG. 6, a cathode (second electrode) having an extraction electrode with a thickness of 100 nm and a size of 40 mm × 20 mm was formed. The effective pixel area of the second electrode is 100 mm square.

(Smoothing of the surface of the cathode (second electrode))
A second base material with a cathode (second electrode) in which the surface roughness Ra of the surface of the cathode (second electrode) was changed as shown in Table 1 using a cathode surface smoothing apparatus shown in FIG. a to i.

  As the cathode surface smoothing apparatus, a reduced pressure plasma reactive ion etching apparatus was used, and the surface of the cathode (second electrode) was smoothed under the following conditions.

Cathode surface smoothing treatment conditions: Decompression degree 10 ^-1 Pa
Introduced gas Oxygen
Oxygen gas introduction amount 20 sccm
Output 200W
Temperature 25 ° C
The surface roughness Ra indicates a value measured by an atomic force microscope (AFM) SPA300 manufactured by SII Nano Technology.

(Formation of cathode buffer layer (electron injection layer))
Subsequently, in the cathode buffer layer (electron injection layer) forming step shown in FIG. 2 on the cathode (second electrode) of each of the second base materials a to i having the cathode (second electrode) subjected to smoothing treatment, Except for the extraction electrode under 5 × 10 ⁻⁴ Pa vacuum, a LiF layer (electron injection layer) having a thickness of 0.5 nm was deposited on the entire surface to form a cathode buffer layer (electron injection layer). 1-1 to 1-9.

<Bonding>
The prepared first member and each prepared second member No. 1-1 to 1-9 are combined with a cathode buffer layer (electron injection layer) and a light emitting layer by a thermocompression-bonding roll in a reduced pressure environment as shown in FIG. The anode (first electrode) and the cathode (second electrode) were sandwiched between the second base materials so as to face each other). At this stage, individual organic EL elements having a configuration in which the anode (first electrode) and the cathode (second electrode) are sandwiched between the first substrate and the second substrate are continuously connected. It is in the state. Thereafter, in order to obtain a single organic EL element, it is transported to a punching process, and individual organic EL elements are punched out. 101-109.

  The alignment of the cathode buffer layer (electron injection layer) and the light emitting layer is performed by detecting the alignment marks attached to both of them and adjusting the transport speed of the first member and the first member. It was. The degree of pressure reduction during bonding was 0.1 Pa, the temperature during bonding was 200 ° C., and the pressure was 5 MPa.

(Evaluation)
Each prepared sample No. Table 2 shows the results of the leak current characteristics tested by the test method shown below and evaluated according to the evaluation rank shown below.

Test Method for Leakage Current Characteristics Using a constant voltage power source, a reverse voltage (reverse bias) was applied at 5 V for 5 seconds, and the current flowing through the organic EL element at that time was measured. Measurement was performed on the light emission region of 10 samples, and the maximum current value was defined as a leakage current.

Evaluation rank of leakage current A: Maximum current value is less than 1 × 10 ⁻⁸ A ○: Maximum current value is 1 × 10 ⁻⁸ A or more and less than 1 × 10 ⁻⁶ A Δ: Maximum current value is 1 × 10 ⁻⁶ A or more, less than 1 × 10 ⁻⁴ A ×: Maximum current value is 1 × 10 ⁻⁴ A or more

  Sample No. No. 101 showed the same performance as the sample of the present invention, but it was judged that the practical application was impossible due to a decrease in productivity due to an increase in processing time. The effectiveness of the present invention was confirmed.

Example 2
A surface having the layer structure of the first substrate / first electrode / hole transport layer / light emitting layer / cathode buffer layer (electron injection layer) / second electrode / second substrate using the manufacturing process shown in FIG. A light emitting organic EL element was produced.

<Preparation of the first member>
The same base material as in Example 1 was used, and the same first member as in Example 1 was prepared under the same conditions.

<Preparation of second member>
Preparation of a second base material having a smoothed second electrode When prepared in Example 1, the second base material No. 2 having a smoothed second electrode was prepared. A second substrate having a smoothed second electrode having the same surface roughness Ra of the second electrode as in c was prepared and prepared under the same conditions as in Example 1.

Preparation of a second base material having a second electrode that has been chamfered and processed The second edge of the prepared second base material around the second electrode is subjected to a chamfer processing apparatus shown in FIG. A second substrate with a chamfered second electrode was prepared by changing the angle θ of the shape shown in FIG. A to I. The angle θ was changed by changing the contact roll angle.

Abrasive tape: PET having a thickness of 50 μm coated with cerium oxide having a particle size of 0.1 μm (Mipox ultra-precision abrasive tape No. 30000 manufactured by Nippon Micro Coating Co., Ltd. was used)
Polishing tape transport speed: 100 mm / sec
Width of polishing tape: + 5% relative to the width of the cathode (second electrode).

Addition weight during polishing: 0.5-10N
Contact roll rubber hardness: 90 °
Contact roll width: + 5% of the width of the cathode (second electrode).

(Formation of cathode buffer layer (electron injection layer))
Subsequently, the cathode buffer layer (electron injection layer) forming step shown in FIG. 2 is formed on the second electrode of each of the second base materials A to I having the second electrode subjected to the chamfering process under the same conditions as in the first embodiment. A cathode buffer layer (electron injection layer) is formed as a second member. 2-1 to 2-9.

<Bonding>
The prepared first member and each prepared second member No. It bonded on the same conditions as Example 1 except having changed the pressure reduction degree when bonding 2-1 to 2-9 with the bonding apparatus shown in FIG. Thereafter, in order to obtain a single organic EL element, it is transported to a punching process, and individual organic EL elements are punched out. 201 to 211.

(Evaluation)
Each prepared sample No. Table 4 shows the results of evaluating the leakage current characteristics by the same test method as in Example 1 and evaluating according to the same evaluation rank as in Example 1.

  It can be seen that the leak characteristics are improved by bonding using the second member that has been chamfered. Moreover, conventionally, it was necessary to reduce the pressure at the time of bonding, but it was found that bonding under atmospheric pressure was possible, and the effectiveness of the present invention was confirmed.

Example 3
Using the manufacturing process shown in FIG. 3, a surface-emitting organic EL device having a layer configuration of first substrate / first electrode / hole transport layer / light emitting layer / second electrode / second substrate was produced. . In addition, the chamfering process of the edge around the second electrode was not performed.

Production of first member <Preparation of first base material having anode (first electrode) layer on first base material>
As a first base material, a glass substrate of 100 mm × 100 mm × 1.1 mm is used, and a first base material in which ITO (indium tin oxide) is formed to a thickness of 100 nm as an anode (first electrode) on the glass substrate. Got ready. The effective pixel area of the first electrode is 100 mm square.

(Formation of hole transport layer)
The first substrate on which the anode (first electrode) was formed was ultrasonically cleaned with isopropyl alcohol, dried with dry nitrogen gas, and UV ozone cleaning was further performed for 5 minutes. Thereafter, a solution obtained by diluting poly (3,4-ethylenedioxythiophene) -polystyrene sulfonic acid (manufactured by PEDOT / PSS Bayer, Baytron P Al 4083) to 70% with IPA on the first base material is 3000 rpm. After forming the film by spin coating in 30 seconds, the film was dried at 200 ° C. for 1 hour to provide a hole transport layer having a thickness of 30 nm.

(Formation of light emitting layer)
Using the process shown in FIG. 3, a solution obtained by dissolving 60 mg of PVK and 1.5 mg of Ir (ppy) ₃ in 6 ml of dichlorobenzene was similarly applied by spin coating on the formed hole transport layer. Then, it vacuum-dried at 60 degreeC for 1 hour, and formed the light emitting layer with a dry film thickness of 30 nm.

(Coating agent coating)
An adhesive (manufactured by Nagase ChemteX Corporation, UV resin XNR5570-B1) was prepared as a sealant. As shown in FIG. 5, around the laminate of the anode (first electrode) / hole transport layer / light emitting layer formed on the first substrate, preparation is made except for the portion serving as the extraction electrode for the anode (first electrode). The prepared adhesive was applied to form a first member.

Preparation of second member <Preparation of second substrate having cathode (second electrode) layer on second substrate>
Polyethersulfone (PES) 100 mm × 100 mm 0.3 mm thick was prepared as the second substrate. An alignment mark was provided at the position where the cathode (second electrode) was previously formed in alignment with the position of the alignment mark provided for the anode (first electrode).

(Formation of cathode (second electrode))
On the second base material prepared in the cathode (second electrode) forming step shown in FIG. 2, the cathode (second electrode) aluminum is deposited in a thickness of 120 nm in accordance with the size of the anode (first electrode). did. The effective pixel area of the second electrode is 100 mm square.

(Smoothing of the surface of the cathode (second electrode))
A second base material with a cathode (second electrode) was prepared by changing the surface roughness Ra of the surface of the cathode (second electrode) as shown in Table 5 using the cathode surface smoothing apparatus shown in FIG. Member No. 3-1 to 3-9.

  As the cathode surface smoothing apparatus, a reduced pressure plasma reactive ion etching apparatus was used, and the surface of the cathode (second electrode) was smoothed under the following conditions.

Cathode surface smoothing treatment conditions: Decompression degree 10 ^-1 Pa
Introduced gas Oxygen
Oxygen gas introduction amount 20 sccm
Output 200W
Temperature 25 ° C
The surface roughness Ra indicates a value measured by an atomic force microscope (AFM) SPA300 manufactured by SII Nano Technology.

<Bonding>
The prepared first member and each prepared second member No. 3-1 to 3-9 are combined with the cathode (second electrode) and the light-emitting layer as shown in FIG. 11 by thermocompression bonding under a reduced pressure environment using the bonding apparatus shown in FIG. The anode (first electrode) and the cathode (second electrode) were sandwiched between the materials. At this stage, an organic EL element having a configuration in which the anode (first electrode) and the cathode (second electrode) are sandwiched between the first substrate and the second substrate so as to face each other is manufactured. 301 to 309.

  The alignment of the cathode buffer layer (electron injection layer) and the light emitting layer was performed by detecting the alignment marks attached to both using an alignment mark detector. The degree of pressure reduction during bonding was 0.1 Pa, the temperature during bonding was 200 ° C., and the pressure was 5 MPa.

Evaluation Each sample No. Table 6 shows the results of the leakage current characteristics tested by the same test method as in Example 1 and evaluated according to the same evaluation rank as in Example 1.

  Sample No. Although 301 showed the same performance as the sample of this invention, it was judged that it cannot be put into practical use due to a decrease in productivity due to an increase in processing time. The effectiveness of the present invention was confirmed.

Claims (15)

A first member having at least an anode formed on the first base material; and a second member having at least a cathode formed on the second base material, wherein at least one of the first member and the second member is used. In the organic electroluminescent element produced by bonding so that it has an organic functional layer on one side and is configured in the order of anode-organic functional layer-cathode,
Surface roughness Ra of the surface bonded with the said 1st member of a said 2nd member is 3.0 nm or less, The organic electroluminescent element characterized by the above-mentioned. 2. The organic electroluminescence element according to claim 1, wherein at least one organic functional layer is formed on the anode of the first member. The organic electroluminescence device according to claim 1 or 2, wherein the surface roughness Ra of the cathode surface formed on the second member is 3.0 nm or less. The organic electroluminescent element according to any one of claims 1 to 3, wherein an edge around the cathode is chamfered. The organic electroluminescence element according to any one of claims 1 to 3, wherein an angle of the chamfering process is 5 ° to 80 °. The organic electroluminescent element according to any one of claims 1 to 5, wherein at least one organic functional layer is formed on the cathode. The organic electroluminescence element according to any one of claims 1 to 6, wherein at least one of the first base material and the second base material is formed of a flexible base material. . Using the first member having at least an anode and at least one organic functional layer formed on the first substrate, and the second member having at least a cathode formed on the second substrate, Bonding is performed so that the anode and the cathode are sandwiched between one base material and the second base material, and a sealing member is provided between the first base material and the second base material. In the manufacturing method of the organic electroluminescence element sealed with
A first supply step for supplying the first member;
A second supply step for supplying the second member;
A bonding step of bonding the first member and the second member;
The second supplying step includes a cathode forming step of forming the cathode on the second base material, and a cathode surface smoothing step of performing a smoothing treatment on the cathode so that the surface roughness Ra is 3.0 nm or less. A method for producing an organic electroluminescence element, comprising: The method of manufacturing an organic electroluminescence element according to claim 8, wherein the smoothing process is performed by a dry etching process under a reduced pressure atmosphere. 10. The method of manufacturing an organic electroluminescent element according to claim 8, further comprising a chamfering process of the edge of the cathode after the cathode surface smoothing process. The method of manufacturing an organic electroluminescence element according to claim 10, wherein the chamfering step is performed by polishing in an inert gas atmosphere. The method for producing an organic electroluminescent element according to any one of claims 8 to 11, wherein the pasting is performed by thermocompression bonding. The method for producing an organic electroluminescent element according to any one of claims 8 to 12, wherein the bonding is performed under atmospheric pressure. The method for producing an organic electroluminescent element according to any one of claims 8 to 13, wherein the organic functional layer is formed by a wet process. Each of the said 1st member and a 2nd member is formed by the roll to roll process, The manufacturing method of the organic electroluminescent element of any one of Claims 8-14 characterized by the above-mentioned.