WO2008023626A1

WO2008023626A1 - Organic electroluminescent device and method for manufacturing the same

Info

Publication number: WO2008023626A1
Application number: PCT/JP2007/065950
Authority: WO
Inventors: Hiroshi Otani; Hideo Taka; Hiroshi Kita; Kiyoshi Endo
Original assignee: Konica Minolta Holdings, Inc.
Priority date: 2006-08-25
Filing date: 2007-08-16
Publication date: 2008-02-28
Also published as: JPWO2008023626A1

Abstract

Disclosed is an organic EL device manufactured by a bonding method, wherein adhesion between organic layers bonded together is improved and separation or the like does not occur. This organic EL device is also improved in carrier movement between the bonding interfaces, while having no emission unevenness. Specifically disclosed is an organic EL device comprising at least one organic layer arranged between a first electrode and a second electrode, which is characterized in that an organic EL member A having a first electrode and at least one organic layer on a first substrate and an organic EL member B having a second electrode and at least one organic layer on a second substrate are bonded together so that the organic layers face each other. The organic EL device is further characterized in that the outer periphery of the substrates are sealingly bonded so that the organic layers of the organic EL member A and the organic EL member B are blocked off from the outside air, and the difference between the internal pressure and the external pressure of the sealed portion containing the organic layers is from -50 to -100 kPa.

Description

Specification

Organic electoluminescence device and manufacturing method thereof

Technical field

TECHNICAL FIELD [0001] The present invention relates to an organic electoluminescence (EU element and a method for producing the same) formed by a bonding method. More specifically, the first substrate and the second substrate each having an organic layer are reduced in a reduced pressure environment. The present invention relates to an organic EL element having improved adhesion by bonding together and a manufacturing method thereof.

Background art

[0002] Organic Electricular Luminescence (EU element is an all-solid-state element composed of an organic material film with a thickness of only 0.1 Hm between electrodes, and the element emits light of 2 to 20V. Because it can be achieved at a relatively low voltage, it is expected to be a next-generation flat display and illumination!

[0003] Furthermore, the recently discovered organic EL element using phosphorescence emission can in principle achieve light emission efficiency about 4 times that of the previous one using fluorescence emission. Research and development of light-emitting element layer configurations and electrodes are underway around the world.

[0004] In addition, the configuration of the organic EL element is simply a structure in which an organic layer is sandwiched between a transparent electrode and a counter electrode, and the number of components is overwhelming compared to a liquid crystal display that is a typical flat display. Because it is low, the manufacturing cost should be kept low. At present, liquid crystal displays are largely drained in terms of performance and cost.

[0005] In particular, in terms of cost, poor productivity is considered as a factor.

[0006] Most of the organic EL devices currently on the market are manufactured by a so-called vapor deposition method in which a low molecular material is deposited to form a film. In this vapor deposition method, low-molecular compounds that can be easily purified can be used as organic EL materials (high-purity materials are easy to obtain), and because it is easy to create a laminated structure, it is extremely efficient in terms of efficiency and life. contrary force is better, in order to perform evaporation under high vacuum conditions of 10- ⁴ Pa or less, joined by constraints apparatus for forming, in practice can only be applied to the substrate of the surface low product further plurality of layers stacked In that case, the disadvantage is that it takes time to deposit the film and the threshold is low. Especially for lighting applications, large area electronic displays If this is the case, the organic EL device will be used in such applications! /!

[0007] In contrast, when a polymer material is used, an organic compound layer in an organic EL element can be manufactured by a coating process such as spin coating, ink jet, printing, and spraying.

[0008] This can be manufactured under atmospheric pressure, so that the cost can be reduced. At the same time, when forming an organic layer of an organic EL element, necessary materials (polymer materials and / or (Or, low molecular weight materials) are prepared and applied in a thin film, so that multiple organic materials can be mixed precisely (for example, preparation of dopants for the light-emitting host material is not necessary). Features that light emission unevenness is difficult to produce and is very advantageous in terms of manufacturing cost S, and the counter electrode formed after forming an organic layer in a general manufacturing process is still a vacuum process such as evaporation or sputtering. In the end, this process becomes a bottleneck and cannot be an innovative production process.

[0009] In contrast to the above-mentioned vapor deposition system, the fact is that the purity of the polymer material cannot be increased and the lamination is difficult. Is not provided.

[0010] The above is the difference in the manufacturing method mainly due to the material, but when focusing on the method of forming the element itself,

(1) A method of sequentially forming a thin film on an electrode substrate (sequential film formation method),

(2) Method of bonding after forming a thin film as appropriate on the electrode substrate and the counter electrode substrate (bonding method),

And power ^s .

[0011] The advantage of the bonding method is

(1) In the sequential film formation method, the resistance electrode to be finally formed can be prepared in advance.

(2) The roll-to-roll continuous production becomes possible by using a film for the substrate.

(3) The organic layer can be easily stacked if the bonding surfaces are made of organic layers,

Etc. [0012] In particular, (1) and (2) will be the driving force for dramatically improving productivity, and if the technology is completed, it will be possible to significantly reduce the manufacturing cost, which was the biggest problem of OLED. It seems to be.

[0013] On the other hand, the roll-to-roll method is disclosed in a technique other than the bonding method.

[0014] For example, Japanese Patent Application Laid-Open No. 2005-327667 describes a method in which a hole transport material is continuously formed on an electrode substrate wound in a ribbon shape on a reel by an ink jet method. As described in the polymer coating method, since the formation of the counter electrode eventually becomes a vacuum process, the merit of the roll-to-roll method is greatly diminished, and the productivity is not substantially improved.

[0015] As described above, the bonding method is an effective technical means for innovatively improving productivity, but at present, the organic EL device manufactured by this method has a problem in performance, and No accurate breakthrough has been found and it is still developing.

[0016] There are several reasons for this, S. Considering in principle, the bonding surface when bonded is not necessarily in close contact at the molecular level, and as a result, the carrier cannot move smoothly. Furthermore, it is expected that the bonding surface will peel off and will not function as a light emitting element.

[0017] In particular, in the roll-to-roll method, there is always a winding process. Therefore, peeling of the joint surface occurs immediately when winding, and peeling immediately becomes a serious problem in manufacturing. When a flexible substrate is used, there is a risk that the element will be destroyed during use, resulting in a fatal defect.

[0018] <Conventional technology of bonding method>

From such a viewpoint, several techniques related to the bonding method for improving the bonding failure at the time of bonding are disclosed.

[0019] For example, Japanese Patent Application Laid-Open No. 9-7736 discloses a technique for improving the adhesion of a bonding surface by allowing a polymer binder to exist on the bonding surface and bonding or fusing the periphery of the element. Japanese Patent Application Laid-Open No. 2004-79300 describes that the same technical idea can be applied to phosphorescence emission in combination with a technique for forming a light emitting layer by a transfer method.

[0020] Further, Patent Document 1 discloses that both of the bonding layers are made of the same material, so that Patent Document 2 introduces a technique for improving the adhesion between the two, which are bonded to each other in a film that has not been completely dried. In both cases, the adhesion at the joint surface is inadequate and is a fundamental solution.

[0021] In addition, Patent Document 3 describes a method for improving the adhesion of the joint surface by pressure bonding using a metal substrate having a resin layer and an elastic layer.

[0022] Adhering the periphery contributes to reducing the adverse effects of moisture and oxygen during driving of the element and improving the light emission lifetime, but is not a technical means that can fundamentally solve the above-mentioned peeling of the joint surface.

[0023] The peeling of the thin film interface is not only a problem of the bonding method.

[0024] All of the organic EL currently commercialized are non-flexible light-emitting elements that are made of glass as a substrate. However, organic EL elements that are all-solid-state elements as described above are flexible such as films. It is a great feature that it can be applied to a certain substrate (so-called flexible display).

[0025] At present, it is said that the gas barrier property of the flexible substrate is insufficient. It is said that its practical use is delayed, but as another problem, peeling between the organic layer and the counter electrode layer is also large. It is a problem.

[0026] This problem has not been taken up as an obvious problem in the current inflexible element, but in principle, the adhesion between the organic substance and the metal forming the counter electrode is low, and the fundamental problem is that Problem.

[0027] In addition, in a sequential film forming method that is usually applied, after forming an organic layer such as a light emitting layer and a carrier transport / injection layer, a counter electrode (usually a cathode, specifically, A1, Ca, Ba, etc.) is formed. The ability to deposit a metal with a small work function such as that) If the organic layer already deposited is damaged, the emission characteristics and lifetime of the organic EL element will be greatly degraded. There is a problem. In other words, it is impossible to form the counter electrode in a strong energy state in order to increase the adhesion between the counter electrode and the organic layer interface. In practice, the film is formed by vacuum evaporation or sputtering under mild conditions. It ’s the situation!

[0028] As means for solving this problem, a technique of providing a buffer layer made of a semiconductor material or metal on the organic layer closest to the counter electrode is also disclosed. Certainly such a buffer layer It is possible to reduce the damage at the time of forming the counter electrode by interposing it, but the load increases in the manufacturing process, which is not preferable from the viewpoint of productivity.

[0029] From this point of view, consider the manufacturing process of the bonding method.

[0030] Since the bonding is performed after forming all necessary layers, the transparent electrode and the counter electrode are formed first.

[0031] When a metal or metal oxide film is formed, in order to obtain a film with good performance, a force that is desired to apply high energy when depositing or after film formation, the bonding method enables this. It can also be thought of as one way to do this. In other words, if the bonding surface for bonding is made of organic layers, the transparent electrode and the counter electrode can be formed in advance by a method most suitable for performance and productivity. If an organic layer is appropriately laminated thereon and bonded, and even the defect on the joint surface is improved, it can be an innovative method with good performance and manufacturing process.

[0032] As a problem of the bonding method, the problem on the joint surface was mentioned earlier. As a result of diligent investigations on this problem, for example, when organic layers are bonded to each other, there are portions where carriers are likely to flow locally and difficult to flow, where carrier movement at the bonding interface is not uniform across the entire surface. I found it easy to do. In particular, the fluorescence method that emits light at the interface of the organic layer has a remarkable behavior, and it has been found that uneven light emission tends to occur. On the other hand, the phosphorescence method, unlike the fluorescence method, has a light-emitting region inside the light-emitting layer, and this phenomenon is relatively rare. In particular, the relative film thickness ratio of the entire organic layer of the light-emitting layer. When increasing the thickness of the light-emitting layer, increasing the thickness of the light-emitting layer, or joining the light-emitting layers to form two light-emitting layers, it is possible to suppress the light-emitting unevenness to the extent that even microscopic observation does not reveal it. I found out. This is a technology that effectively utilizes the phenomenon of slow carrier movement at the bonding interface, which is the biggest difficulty of the bonding method, and it can be said that it has never been seen before.

Patent Document 1: Japanese Patent Laid-Open No. 2002-203675

Patent Document 2: JP-A-9 36667

Patent Document 3: Japanese Patent Laid-Open No. 2004-296148

Disclosure of the invention Problems to be solved by the invention

[0033] An object of the present invention is to improve the adhesion between bonded organic layers in the production of an organic EL element by a bonding method, and to improve the carrier movement between bonding interfaces where peeling or the like is eliminated. The goal is to obtain an organic EL device without any problems.

Means for solving the problem

[0034] The object of the present invention is achieved by the following means.

[0035] 1. An organic electroluminescent device having at least one organic layer between a first electrode and a second electrode, wherein the organic electroluminescent device is formed on a first substrate, at least a first electrode, An organic electrification member A having one or more organic layers;

On the second substrate, a second electrode, an organic electoluminescence member B having at least one organic layer, and

Each of them is bonded so that the organic layers face each other,

And the organic layer of the organic electoluminescence member A and the organic layer of the organic electroluminescence member B are bonded together by sealing the periphery of the substrate so as to be shielded from the outside air,

An organic electoluminescence device, wherein a pressure difference between an internal pressure of a sealed portion including the organic layer and an external pressure (atmospheric pressure) is 50 lOOkPa.

[0036] 2. In the method of manufacturing an organic electroluminescent device having at least one organic layer between the first electrode and the second electrode, the first electrode and at least one organic layer are formed on the first substrate. An organic electroluminescent luminescence member A having a layer, and an organic electroluminescent luminescence member B having at least one organic layer on the second substrate,

Under pressure of 0 kPa that is cut off from the outside air, the organic layers are in close contact with each other, and the periphery of the substrate is adhered and sealed, and the organic electroluminescent luminescent member A and organic electroluminescent luminescent member B are bonded. A manufacturing method of an organic-elect mouth luminescence element characterized by the above.

[0037] 3. An organic elect having at least one organic layer between the first electrode and the second electrode In the method for manufacturing an oral luminescence element, a first electrode on the first substrate, an organic electoluminescence member A having at least one organic layer, and a second electrode on the second substrate, at least one organic layer. The organic electroluminescent luminescence member B having a layer and the organic layers are brought into close contact with each other,

Furthermore, a sealing member is laminated on the second substrate,

Under the pressure of 0-50kPa shut off from outside air,

A method for producing an organic electoluminescence device comprising adhering and sealing the periphery of a first substrate and a sealing member, and bonding the organic electroluminescence device A and the organic electroluminescence device B .

[0038] 4. The method for producing an organic electoluminescence device according to 2 or 3, wherein the sealing is performed with a photocurable adhesive.

[0039] 5. A photo-curable adhesive is preliminarily disposed around at least one organic layer of the first substrate or the second substrate,

Under a pressure of 0 to 50 kPa cut off from the outside air, the organic layer of the organic electoluminous luminescence member A and the organic layer of the organic electroluminescent luminescence member B are brought into close contact with each other,

3. The organic electoluminescence element according to 2, wherein the photocurable adhesive is cured, adhered, and sealed by irradiating light with at least one of the first substrate and the second substrate. Manufacturing method.

[0040] 6. A photo-curable adhesive is preliminarily disposed around at least one organic layer of the first substrate or the sealing member,

4. The organic electroluminescent element according to 3 above, wherein the photocurable adhesive is cured, adhered, and sealed by irradiating at least one of the first substrate and the sealing member. Production method.

[0041] 7. In the above 2 or 3, wherein the sealing is performed with a heat-fusible adhesive. The manufacturing method of the organic electoluminescence device of description.

[0042] 8. A heat-fusible adhesive is previously installed around at least one organic layer of the first substrate or the second substrate,

3. The organic electroluminescence device according to 2 above, wherein at least the periphery of the first substrate and the second substrate is heated to melt and bond and seal the heat-fusible adhesive. Manufacturing method.

[0043] 9. A heat-fusible adhesive is previously installed around at least one organic layer of the first substrate or the sealing member,

4. The organic electroluminescent mouth luminescence device according to 3 above, wherein at least the periphery of the first substrate and the sealing member is heated to thermally melt and bond and seal the heat-fusible adhesive. Production method.

[0044] 10. The organic electroluminescent mouth luminescence device as described in 1 above, wherein a moisture-proof layer is provided on at least one of the first substrate and the second substrate.

[0045] 11. The method for producing an organic electroluminescence device according to any one of 2 to 9, wherein at least one of the first substrate and the second substrate has a moisture-proof layer.

[0046] 12. The organic electoluminescence device according to 1 above, wherein a moisture absorbing member is provided on at least one of the first substrate and the second substrate.

[0047] 13. The method for producing an organic electroluminescence device according to any one of 2 to 9, wherein a moisture absorbing member is applied to at least one of the first substrate and the second substrate. .

The invention's effect [0048] According to the present invention, in the production of an organic EL device by a bonding method, the carrier movement between the bonding interfaces, such as good adhesion between organic layers, is improved, and an organic EL device free from uneven light emission can be obtained. Monkey.

Brief Description of Drawings

[0049] Fig. 1 is a diagram showing an example of manufacturing an organic EL element using a vacuum bonding apparatus.

2] It is a diagram showing another example of manufacturing an organic EL element using a vacuum bonding apparatus. FIG. 3] A diagram showing an example of an organic EL element in which a hygroscopic member is arranged.

4] A diagram showing an example of manufacturing an organic EL element by a roll bonding apparatus.

Explanation of symbols

[0050] 1 First substrate

2 Second board

3 Sealing material

101 Vacuum chamber

102 Elastic member

104 Heater

BEST MODE FOR CARRYING OUT THE INVENTION

[0051] The best mode for carrying out the present invention will be described in detail below, but the present invention is not limited thereto.

[0052] The present invention relates to production of an organic EL element by a bonding method,

In a method for manufacturing an organic electroluminescent element having at least one or more organic layers between a first electrode and a second electrode, an organic elect having a first electrode and at least one or more organic layers on a first substrate. The organic luminescence member A and the second electrode, the organic electoluminescence member B having at least one organic layer on the second substrate, are shielded from the outside air under the pressure of 0 to 50 kPa. Are bonded so that they face each other, and the periphery of the substrate is bonded and sealed, and the organic electroluminescent mouth luminescence member A and the organic electroluminescent mouth luminescence member B are bonded to each other. Is the method.

[0053] More specifically, the first substrate is, for example, a glass substrate, and IT is placed on the glass substrate. The anode composed of o (first electrode), hole injection layer, hole transport layer, light emitting layer, electron transport layer, etc. Therefore, this is an organic-elect mouth luminescence member A, and the organic EL member A is an anode-side member in this case. When the organic-elect mouth luminescence member A is an anode side member, the organic-elect luminescence member B is a cathode-side member, the second electrode is a cathode, and at least the remaining layers are formed on the cathode in this order from the cathode side. Is done.

[0054] For example, when the organic EL member A is an anode side member and is formed from the anode to the light emitting layer on the first substrate, the organic EL member B is used as the second electrode (cathode) on the second substrate. For example, at least the electron injection layer and the electron transport layer are formed (cathode side member).

[0055] Regarding the laminated structure of the organic layers, the number of organic layers formed on each substrate may include various organic layers as needed, such as an electron blocking layer and a hole blocking layer. Is not limited, and may be configured according to the order of layers constituting the organic EL element when bonded. Therefore, which organic layer of each layer of the organic EL element is formed on each member, and is used as the organic EL member A (or anode side member) or the organic EL member B (or cathode side member), respectively. The most appropriate material is selected from the viewpoints of properties such as the organic EL material constituting the organic layer, such as glass transition temperature, melting point, crystal structure, and adhesion.

[0056] Further, the same organic layer may be formed on each member. For example, in the above case, even if the light emitting layer is formed on both members, the light emitting layer may be integrated by bonding. Absent.

Accordingly, the organic EL element formed by the method for producing an organic EL element of the present invention includes a first electrode, an organic EL member A having at least one organic layer on the first substrate, and a second substrate. On top of this, the second electrode, the organic EL member B having at least one organic layer, is brought into close contact with each other under pressure of 0 to 50 kPa (under reduced pressure) shut off from the outside air. It is formed by adhering and sealing the periphery of the substrate, adhering the organic-elect mouth luminescence member A and the organic-elect luminescence member B, and returning to atmospheric pressure after sealing.

[0058] When this is returned to the atmosphere (at atmospheric pressure) by sealing under reduced pressure (eg, lOkPa) (sealing the organic layer), the first and second substrates are pushed to atmospheric pressure. The volume of the sealed space including the first substrate, the second substrate, and the organic layer formed by the sealing portion is slightly shrunk, Depending on how the gas (for example, air) remains in the sealed space, the internal pressure changes slightly when it is returned to atmospheric pressure (in general, the atmospheric pressure increases slightly because it is pushed by atmospheric pressure and the internal volume changes). However, if the pressure is sufficiently reduced by sealing under reduced pressure, the organic layers can be uniformly subjected to a differential pressure from the atmospheric pressure, thereby bonding the organic layers uniformly. I can do it.

[0059] Therefore, the organic EL element produced by the method of the present invention, in which the organic EL member A and the organic EL member B are bonded under reduced pressure, has an internal pressure in the sealed space portion containing the organic layer. And an external pressure (atmospheric pressure) in the range of −50 to −lOOkPa (that is, the internal pressure is low! /).

[0060] According to the method of the present invention, the final pressure can be controlled by adjusting the degree of vacuum at the time of bonding, and the bonding pressure can be controlled. Since a pressure of atmospheric pressure (internal pressure) can be applied uniformly to the surface in a non-contact manner, a stable bonding element can be obtained. It is difficult to apply pressure uniformly by mechanical pressure bonding.

[0061] In particular, it is advantageous in a flexible element in which it is difficult to apply pressure mechanically (physically).

[0062] Further, it is possible to obtain an advantage that sealing can be performed simultaneously with bonding.

[0063] Hereinafter, a method for producing an organic EL element by the bonding method of the present invention will be described in detail with reference to the drawings.

FIG. 1 shows an example of manufacturing the organic EL element of the present invention using a vacuum bonding apparatus.

FIG. 1 (a) shows an organic EL member A in which a first electrode 11 and an organic layer 12 are formed on a first substrate 1 and a second electrode 21 and an organic layer 22 formed on a second substrate. Each of the organic EL members B was shown. The organic EL member A represents, for example, an anode substrate, and the organic EL member B represents a cathode substrate. Accordingly, the first electrode 11 is an ITO electrode, the organic layer 12 is, for example, a hole transport layer and a light emitting layer, the second electrode is, for example, a cathode made of aluminum, and the organic layer 22 is, for example, an electron transport layer. By laminating these two substrates, finally, at least one or more organic layers (in this case, from the anode side) between the first substrate (first electrode) and the second substrate (second electrode) An organic electroluminescent device having a structure of a hole transport layer, a light emitting layer, an electron transport layer, and a cathode is obtained. [0066] The organic layer (bonding layer) to be bonded may be any of the functional layers constituting the organic EL element. For example, a hole injection layer, a hole transport layer, a light emitting layer, an electron transport layer, an electron injection layer Any of these may be used.

[0067] Fig. 1 (b) shows a sealing material (adhesive) S placed around the organic layer on the first substrate for sealing (adhesion). Alternatively, you can apply a thermosetting adhesive, or place it around using a thermosetting adhesive sheet.

[0068] Further, a photo-curable adhesive may be used. When using a photocurable adhesive, it is preferable to provide a light source in the vacuum bonding apparatus so that light (ultraviolet rays) can be irradiated from the first substrate or the second substrate side.

[0069] In FIG. 1 (b), a thermosetting adhesive sheet is disposed around the organic layer on the first substrate of the organic EL member A, and then the organic EL member A is adhered and laminated so that the organic layers face each other. Then, temporarily paste.

[0070] Here, the force of disposing a thermosetting sheet around the first substrate may be on the second substrate, or may be disposed on both substrates.

[0071] Next, the first electrode 11 on which the thermosetting sheet is disposed, the first substrate 1 having the organic layer 12, and the second substrate 21 having the second electrode 21 and the organic layer 22 are connected to the organic layers 12 and 22 with each other. The laminated body facing each other is placed in the vacuum chamber 101 of the vacuum bonding apparatus shown in FIG. 1 (c). The vacuum bonding apparatus according to the present invention shown in FIG. 1 (c) includes a vacuum chamber (including a frame) 101 on which organic EL members A and B to be bonded are placed, and a laminated organic EL member A. The elastic member 102 that applies pressure to B and B, and fixes them tightly, the cylinder 103 that drives them, and the shape of the thermosetting adhesive sheet so as to surround the periphery of the substrate and the organic layer A heater 104 is provided. The heater 104 is also provided with a cylinder 105, and has a mechanism that allows the heater to be heat-bonded to the adhesive sheet from the back surface of the substrate by the operation of the cylinder. Further, the vacuum chamber 1 can be evacuated by a pressure reducing device (not shown), and is sealed so that the vacuum chamber 1 is shut off from the outside air.

[0072] The elastic member 102 that presses the two members into close contact to release gas between the two members and forms a surface layer with a heat-resistant elastic body such as silicon rubber or silicon sponge. Plate or the like is used.

[0073] The heater 104 is, for example, a heat block that can be heated by energization and is arranged in a predetermined shape surrounding the periphery of the substrate and the organic layer. It is possible to perform pressure bonding for a predetermined time.

[0074] When the organic EL member A and the organic EL member B are laminated and placed in the vacuum chamber 101, the elastic member 102 is then applied to the back surface of the second substrate with a predetermined pressure by driving the cylinder 103. When pressed, the organic layer 12 on the first substrate and the organic layer 22 on the second substrate are brought into close contact and fixed (FIG. 1 (d)).

[0075] Next, the vacuum chamber 101 is closed, shut off from the outside air, and evacuated to a reduced pressure, that is, a pressure of 0 to 50 kPa (FIG. 1 (e)). At this stage, the pressure in the vicinity of the organic layer and in the organic layer interface is the same as that in the vacuum chamber 101.

[0076] FIG. 1 (f) shows the next step in which the heater 104 is lowered by driving the cylinder 105 in a state of being cut off from the outside air, and the energy necessary for the substrates to be cured and bonded is applied. In order to do this, pressure is applied to the back side and heating is performed. When a thermosetting adhesive sheet is used as the sealing material S, the temperature is 50 to 100 ° C, and the pressure is 0.05 to 0. Hold at about 20MPa;! ~ 10 seconds.

[0077] Thereby, the first substrate and the second substrate are bonded by the thermosetting sheet, and the organic EL element is sealed and bonded.

[0078] Of course, the bonding may be performed by using a thermosetting adhesive or a photocurable adhesive described later! /,

Yes

[0079] After adhering and sealing the periphery of the substrate by predetermined heating, the heaters 104 and the elastic member 102 are then pulled back to their original positions by driving the cylinders 105 and 103, and further, the vacuum chamber 1 The release of the pressure is released (Fig. 1 (g)), and the sealing and bonding of the organic EL element is completed.

[0080] In the state of Fig. 1 (f), the sealing space P blocked by the two substrates and the sealing material has the same degree of vacuum as that of the vacuum chamber. When the pressure increases, the degree of decompression of the sealed space P slightly increases depending on factors such as the volume of the sealed space, but basically the increase is slight, and the external pressure When A large pressure difference with the sealed space is maintained, whereby the organic layer on the first substrate and the organic layer on the second substrate are adhered uniformly and tightly.

In the present invention, in order to seal the organic EL element under reduced pressure (for example, lOkPa) (the organic layer portion is sealed), for example, in the state of FIG. 1 (f), two substrates and a sealing material are used. The sealed space P blocked by the pressure S has the same degree of vacuum as that of the vacuum chamber S. By returning it to the atmosphere, when sealing under reduced pressure, the gas in the sealed space of the organic layer (for example, When the pressure is returned to atmospheric pressure due to the remaining air), the internal volume changes by being pushed to atmospheric pressure, so the internal pressure changes and generally the atmospheric pressure increases slightly (for example, ~ 50kPa), but the organic layer is included. The pressure difference between the internal pressure of the sealed space and the external pressure (atmospheric pressure) is in the range of -50 lOOkPa. Basically, the first and second substrates are uniformly pressed by this differential pressure from the atmospheric pressure. Therefore, it is possible to obtain a preferable adhesion state for carrier movement between organic layers.

FIG. 1 (h) shows a cross-sectional view of the extracted organic EL device and a view of the organic EL device viewed from above. The substrates are bonded to each other by a sealing material (adhesive or adhesive sheet) disposed around the organic layer, and the organic layers are bonded to form an organic EL element.

[0083] Further, in the above production, in the bonding and sealing with a thermosetting adhesive sheet in a vacuum, the thermosetting sheets arranged on the substrate are opposed to each other rather than bonding the periphery at once. It is preferable that the pair of sides are bonded by heat and bonded, and then the remaining pair of sides are bonded, closed, and sealed for uniform bonding.

[0084] For this purpose, it is preferable that the heater can be driven by an individual cylinder at least for each pair of sides.

[0085] In these bonding and sealing processes, both the first substrate and the second substrate may be glass substrates, but it is preferable that at least one of them is a flexible substrate. By making the first substrate a glass substrate and the second substrate a flexible film, pressure can be applied between the organic layers to be bonded more uniformly without contact, and even adhesion, bonding, sealing Can be stopped.

[0086] Further, in the vacuum bonding apparatus, at least one of the first substrate and the second substrate, for example, in the case of FIG. 1, the second substrate is used as a flexible substrate (for example, a base material made of a plastic film). For example, the second substrate is continuously supplied in a strip shape (for example, toward the plane of FIG. (From left to right), an organic EL element can be formed by sequentially bonding and sealing the organic EL member A with an electrode and organic layer formed on a separately formed first substrate. .

As described above, by using at least one of the first substrate and the second substrate as a strip-shaped flexible substrate, this can be continuously supplied to improve the productivity of the organic EL element.

[0088] In the present invention, it is preferable to have a moisture-proof layer on at least one of the first substrate and the second substrate in order to maintain the force sealing effect.

[0089] The moisture-proof layer is not limited as long as it is a layer composed of a material having gas barrier properties such as water vapor, oxygen, etc. For example, a ceramic vapor-deposited layer such as silicon oxide and aluminum oxide, and these Moisture-proof layers with a structure in which ceramic layers and impact-relieving polymer layers are laminated alternately, and metal foils such as laminate layers (6 to 50 111 thickness) of copper (Cu) foil, aluminum (A1) foil, etc. It is preferable to have such a moisture-proof layer on the opposite side (outside) of the organic layer of the first electrode or the second electrode layer.

[0090] For this purpose, a film having these moisture-proof layers may be used as a substrate. Typically, as a film having these moisture-proof layers, for example, on a resin film substrate (10 to 200 111) such as a PET film. In addition, the above ceramic layer is formed by vapor deposition, or a metal foil or the like is laminated with a polyethylene resin film.

[0091] As the film having the vapor deposition layer, a resin film on which vapor deposition of silicon oxide, aluminum oxide or the like is deposited is available. For example, a letterpress printing GX film can be obtained. In addition, a metal laminate film in which one side of a metal foil is coated with a polymer film is commercially available for packaging materials. For example, a dry laminate film (adhesive layer / aluminum film 9 m / polyethylene terephthalate (PET) 38 11 m) (a two-component urethane adhesive with an adhesive layer thickness of 1.5 m) is used. is there.

[0092] Therefore, by using these as any force of the substrate and the base material, a moisture-proof layer can be incorporated, and the moisture-proof effect by sealing can be improved.

[0093] Another production example of an organic EL device by bonding according to the present invention is shown based on FIG.

FIG. 2 (a) shows a first substrate (organic EL member A) having the first electrode 11 and the organic layer 12 and a second substrate (organic EL member having the second electrode 21 and the organic layer 22 in the same manner as described above. B) is shown respectively. Figure 2 (b) shows a thermosetting adhesive sheet as the sealing material S around the organic layer of the organic EL member A. The organic EL member A and the organic EL member B are laminated with the respective organic layers facing each other, and the second substrate of the organic EL member B is opposite to the organic layer (outside). ) Force The sealing member 3 is laminated and temporarily bonded.

[0095] The sealing member 3 is a flexible plastic sheet or film having a high gas barrier property such as water vapor or oxygen. A resin film having the moisture-proof layer is preferred. For example, a vapor deposition film using PET as a base material, such as a GX film manufactured by Toppan Printing, can be mentioned.

[0096] If the first substrate is made of a gas-noble base material such as glass, by using such a sealing member 3, the organic EL element can be efficiently sealed from the outside air, such as water vapor and oxygen. The influence of degradable gas can be suppressed.

[0097] Next, a first electrode 11, a first substrate 1 having an organic layer 12, and a second electrode 21, a second substrate 2 having an organic layer 22, and a sealing, on which a thermosetting adhesive sheet is disposed The material 3 laminated and temporarily bonded is placed in the vacuum chamber 101 of the same vacuum bonding apparatus as shown in FIG. 1 (c) (FIG. 2 (c)).

[0098] The vacuum bonding apparatus drives a vacuum chamber 101 (including a frame) on which a laminate of the organic EL member A and the organic EL member B to be bonded is placed and an elastic member 102 for pressing. A cylinder 103 is provided. The elastic member is a pressing plate whose surface is made of a material having elasticity such as silicon rubber or silicon sponge. The cylinder 103 is moved up and down by the cylinder, thereby pressing the laminated body from the back surface. In addition, the gas between the stacked bodies can be released and the stacked body can be tightly fixed between the stacks.

[0099] In addition, a heater 104 is provided in substantially the same shape as the sealing material S (thermosetting adhesive sheet) so as to surround the periphery of the organic layer. The heater 104 also includes a cylinder 105, and has a function of heating by moving the heater up and down by the cylinder and pressing the heater against the back surface of the sealing member. Further, the vacuum chamber 101 can be evacuated by a decompression device (not shown) after being sealed, and has a structure in which the vacuum chamber 1 is shut off from the outside air to come to decompression.

[0100] When the organic EL member A and the organic EL member B laminated with the sealing member 3 are placed in the vacuum chamber 1101 (FIG. 2 (c)), the cylinder 103 is then driven. As a result, the elastic member 102 is lowered and pressed against the back surface of the sealing member 3 laminated on the back surface of the second substrate with a predetermined pressure. Thus, the organic layer 12 on the first substrate and the organic layer 22 on the second substrate are fixed in contact with each other (FIG. 2 (d)).

[0101] Next, the vacuum chamber 101 is closed, shut off from the outside air, and evacuated to a pressure of 0 to 50 kPa (FIG. 2 (e)). At this stage, the pressure in the vicinity of the organic layer and in the organic layer interface is the same as that in the vacuum chamber.

[0102] With this air shut off and the degree of vacuum maintained at 0 to 50 kPa, the cylinder 105 is then driven to lower the heater 104 and seal from the back of the sealing member 3 Material S (thermosetting adhesive sheet) is heated and pressed to give the energy required for curing (Fig. 2 (f)). When a thermosetting adhesive sheet is used, the temperature may be in the range of 50 to 100 ° C., the pressure may be 0.05 to 0.20 Pa, and the time may be 1 to 10 seconds. By this step, the sealing member 3 and the first substrate are bonded by the thermosetting adhesive sheet in a state where the organic layers of the organic EL member A and the organic EL member B are in close contact with each other.

[0103] From the viewpoint of improving the adhesion between the organic layers, bonding with a sealing material is performed by bonding a pair of opposite sides around the substrate in advance and then bonding and closing the remaining pair of sides under reduced pressure. It is preferable to bond the heater block in two stages so that the preferred heater block can be driven separately in this way.

In any case, sealing is performed by bonding the sealing member 3 and the first substrate by pressure bonding and heating of the heater 104, and the organic layers of the organic EL member A and the organic EL member B are in close contact with each other at the same time. A bonded organic EL element is formed.

[0105] Next, the cylinders 103 and 105 are driven to raise the elastic member 102 and the heater 104. After returning to their original positions, the decompression is released (Fig. 2 (g)), and The EL element is sealed and bonded.

[0106] Fig. 2 (h) shows a cross-sectional view of the extracted organic EL device and a view of the organic EL device viewed from above. The organic EL elements are sealed and formed by bonding the substrates together and bonding the organic layers together with an adhesive placed around the organic layer.

[0107] As the sealing member, for example, a flexible gas barrier resin film such as a metal vapor-deposited film can be used. Even when the first substrate is a rigid substrate such as glass, a uniform pressure is applied. Because it is applied between organic layers, the layers between the layers that have better adhesion between the organic layers As a result, a uniform element with less unevenness in the movement of the carrier can be obtained. In addition, since the sealing member can be continuously supplied, the continuous productivity of the element is also excellent.

[0108] In order to more uniformly bond the first organic layer formed on the first substrate and the second organic layer formed on the second substrate, heat treatment is performed in a state where the elastic member is pressed. This is also preferable. As a heating method, a heating function may be imparted to the elastic member, or a heater may be imparted (hot plate) to a gantry provided in the vacuum chamber.

[0109] The heating temperature is lower than the melting point of any organic layer used, generally 80 to 80 ° C; the softening temperature of the organic material constituting the organic layer that is about 160 ° C, and the lowest glass transition temperature! The temperature is lower than the temperature, and is preferably 0 ° C or higher and 80 ° C or lower, and more preferably 40 ° C or higher and 80 ° C or lower. In view of temperature controllability, it is preferably 40 ° C or higher.

[0110] Further, after the organic layers are formed on the first substrate and the second substrate, the surface of each organic layer is preferably subjected to a pre-beta treatment. Pre-beta treatment can remove some of the solvent contained in the organic layer. Lower than the heating at the time of pasting, short at the temperature! It is particularly effective for a large area element to remove a certain amount of solvent beforehand by pre-beta treatment before bonding. For the same reason as the heat treatment at the time of pasting, the heating temperature of the pre-beta treatment is a softening temperature lower than the melting point of any organic layer used, and the lowest glass transition temperature! /, A temperature lower than the temperature. , Temperature is preferred! The pre-beta treatment is performed on the surface of both organic layers, but in some cases it may be single-sided. As the heating method, oven drying, hot plate drying, vacuum drying, etc. can be used.

[0111] Further, it is preferable that the sealing material applied to the periphery of the display portion of both the substrates to adhere the substrates to each other is moisture-proof.

[0112] As the sealing material, an adhesive, for example, an adhesive generally used for glass, plastic substrates and the like can be used without limitation.

[0113] Particularly preferred adhesives include acrylic adhesives and epoxy adhesives. Among them, an epoxy adhesive having a small shrinkage upon curing is preferable.

[0114] The epoxy adhesive is composed of an epoxy resin as a main agent and a curing agent, and a compound (main agent) containing an epoxy group and a curing agent containing an amine oxalic anhydride are mixed together. An adhesive that adheres by a curing reaction.

[0115] Examples of the compound containing an epoxy group include bisphenol A type as described above, and amines are often used as curing agents.

[0116] These adhesives can be applied on the substrate without any particular restrictions such as potting, coating, spraying, printing, etc., and can be polymerized and cured by irradiation with energy rays such as ultraviolet rays and electron beams, and heat. Touch with force S.

[0117] A thermoactive epoxy resin curing agent comprising a bisphenol-based glycidyl epoxy resin and a thermosetting adhesive component that forms a three-dimensional network when heated is also preferable.

[0118] The adhesive used as the sealing material may be an ultraviolet curable adhesive. In the case of a thermosetting adhesive, when the curing temperature affects the characteristics of the device, an actinic ray curable adhesive that is polymerized and cured by energy rays such as ultraviolet rays and electron beams is preferred. in this case

Acrylic adhesives can be used, and specific examples include Three Bond Co., Ltd., 3003, 3027B, 3033B, 3042B, etc., and Cemedine Co., Ltd., Cemedine Y600, Y600H.

[0119] In the case of an ultraviolet curable adhesive, the vacuum bonding apparatus is provided with a light source capable of irradiating ultraviolet rays from the back surface of the first substrate, the second substrate or the sealing member. For example, the adhesion may be cured by irradiating the substrate with a light amount of about 10 to 100 mW / cm ² over a range of! To 30 seconds.

[0120] The "ultraviolet region (light)" in the specification of the present application refers to light having a wavelength in the range of 250 nm to 400 nm, and can be obtained by a high pressure mercury lamp or a halogen lamp.

[0121] These adhesives are applied onto the substrate by a process such as coating or printing, and a pre-formed thermosetting adhesive sheet or hot-melt adhesive is used as the sealing material. I can do it. For example, TBF series manufactured by Sumitomo 3EM, among them low-temperature adhesive type thermosetting adhesive sheets such as TBF560, etc., and these sheets are cut into a desired shape and placed on a substrate by sealing material. This is preferable because it can be applied on a substrate.

[0122] In addition, in the manufacture of an organic EL element by bonding according to the present invention, a moisture absorbing member is provided on a substrate and is present in the sealing region, thereby adsorbing moisture in the element space and degrading the element. Can be suppressed. For example, a method of adhering a powdery moisture absorbing member such as calcium oxide or zeolite onto a base material around the display unit is employed. The moisture absorbing member may be provided on any base material. When the sealing material is disposed, the moisture absorbing member may be disposed, for example, in a region around the organic layer. Figure 3 shows an example of an organic EL device in which the moisture absorbing member D is placed around the organic layer inside the sealed space (around the organic layer).

[0123] An organic EL element has a structure in which one or more organic layers are laminated between electrodes. For example, anode / hole injection, transport layer / light emitting layer / electron injection, transport layer / cathode, etc. are the simplest. Is a structure composed of an anode / light-emitting layer / cathode. The thickness of each organic layer and each thin film in these organic EL devices is a force ranging from 1 nm to several in. These organic layers are the first substrate and the second substrate. The organic EL element of the present invention is formed by separately forming on a substrate and bonding them.

Next, in the present invention, each organic layer constituting the organic EL element formed on the substrate will be described.

[0125] An organic EL element has a structure in which one or more organic layers are laminated between electrodes. For example, anode / hole injection, transport layer / light emitting layer / electron injection, transport layer / cathode, etc. are the simplest. Has a structure consisting of an anode / light-emitting layer / cathode, and other layers such as an electron blocking layer, a hole blocking layer, and a buffer layer are laminated in a predetermined layer order and injected from both electrodes. It is configured so that carriers such as holes and electrons can move smoothly.

[0126] In each of these organic layers constituting the organic EL element, the organic light-emitting material contained in the light-emitting layer includes aromatic heterocyclic compounds such as canolevazole, carboline, diazacanolevazole, and triarylamine. Mining derivatives, stilbene derivatives, polyarylenes, aromatic condensed polycyclic compounds, aromatic heterocondensed ring compounds, metal complex compounds, and the like, and powers such as single oligo or composite oligos are not limited thereto. ! /

[0127] Further, the layer (film forming material) preferably contains about 0.;! To about 20% by mass of a dopant in the light emitting material. Examples of the dopant include known fluorescent pigments such as perylene derivatives and pyrene derivatives, and in the case of phosphorescent light emitting layers, for example, tris (2-phenylpyridine) iridium, bis (2-phenylpyridine) ( Orthometasylated by acetylylacetonate) iridium, bis (2,4-difluorofurpyridine) (picolinato) iridium, etc. Similarly, a complex compound such as an iridium bromide complex is contained in an amount of about 0 .;

[0128] The phosphorescence emission method has a light-emitting region inside the light-emitting layer. Because it is difficult to cause the phenomenon, it is compatible with the bonding method of the present invention.

[0129] The hole-injection transport layer is typified by phthalocyanine derivatives, heterocyclic azoles, aromatic tertiary amines, polybutylcarbazole, polyethylenedioxythiophene / polystyrene sulfonic acid (PEDOT: PSS), etc. A high-molecular material such as a conductive polymer, and a power rubazole-based light-emitting material such as 4,4′-dicarbazolylbiphenyl, 1,3-dicarbazolylbenzene, etc. Polymers typified by low molecular luminescent materials such as azacarbazoles, pyrene-based luminescent materials such as 1,3,5 tripyrenylbenzene, polyphenylenevinylenes, polyfluorenes, polybulur rubazoles, etc. Examples include luminescent materials.

[0130] Examples of the electron injection / transport layer material include metal complex compounds such as 8-hydroxyquinolinatotritium and bis (8-hydroxyquinolinato) zinc, and the following nitrogen-containing five-membered ring derivatives. That is, oxazole, thiazole, oxadiazole, thiadiazole or triazole derivatives are preferred. Specifically, 2, 5 bis (1-phenyl) -1,3,4-oxazole, 2,5-bis (1-phenyl) 1,3,4, thiazole, 2,5— Bis (1 phenyl) 1, 3, 4 oxaziazole, 2- (4'-tert-butylphenyl) -5- (4 "-biphenyl) 1, 3, 4-oxoxadiazole, 2, 5-bis (1 naphthinole) -1 , 3, 4 oxadiazole, 1, 4 bis [2— (5 phenyloxadiazolyl)] benzene, 1, 4 bis [2— (5-phenyl oxaziazolyl) 4— tert butylben Zen], 2-(4 '-tert butylphenyl) 1-5- (4 "-biphenyl) 1 1, 3, 4 thiadiazole, 2,5 bis (1 naphthyl) 1, 3, 4 thiadiazole, 1, 4 bis [2- (5 phenylthiadiazolyl)] benzene, 2— (4 '—tert butylphenyl) 5 — (4 ”—biphenyl) 1 1, 3, 4 triazolene, 2, 5 bis (1— Na Chinore) one 1, 3, 4 Toriazoru, 1, 4-bis [2- (5-phenylpropyl tri § benzisoxazolyl)] benzene, and the like

Yes

[0131] The thickness of the organic EL element and each organic layer needs to be about 0.05 to 0.3 μm, preferably 0 • 1—about 0.2 mm.

[0132] As the method for forming the organic layer of the present invention, coating and printing are preferred.

As the coating, spin coating, transfer coating, extension coating, or the like can be used. Considering the efficiency of material use, transfer coating and transfer coating are preferred, and pattern coating such as transfer coating is preferred. Transfer coating is particularly preferable.

[0133] For printing, screen printing, offset printing, inkjet printing, or the like can be used.

As the display element, the element is thin and the element size is minute, and high precision and high definition printing such as offset printing and ink jet printing is preferable in consideration of overlapping of RGB patterns.

[0134] Each organic material has solubility characteristics (solubility parameters, ionization potential, polarity), and there are limitations on the solvents that can be dissolved. In this case, since the solubility is different, the concentration cannot be generally determined, but the type of the solvent used in the present invention is suitable for the above conditions depending on the organic EL material to be formed. Can be selected from known solvents, for example, halogenated carbonization such as dichloromethane, dichloroethane, chloroform, carbon tetrachloride, tetrachloroethane, trichloroethane, chlorobenzene, dichlorobenzene, chlorotolenene, etc. Hydrogen solvents, ether solvents such as dibutyl ether, tetrahydrofuran, dioxane, and anisole, alcohols such as methanol, ethanol, isopropanol, butanol, cyclohexanol, 2-methoxyethanol, ethylene glycol and glycerin Solvents, benzene, toluene, xylene , Aromatic hydrocarbon solvents such as ethenylbenzene, paraffin solvents such as hexane, octane, decane, and tetralin, ester solvents such as ethyl acetate, butyl acetate, and amyl acetate, N, N-dimethinoformamide, N, N —Amid solvents such as dimethylacetamide and N-methylpyrrolidone; ketone solvents such as acetone, methyl ethyl ketone, cyclohexanone and isophorone; amine solvents such as pyridine, quinoline and aniline; Examples include nitrile solvents such as tolyl and sulfur solvents such as thiophene and carbon disulfide.

[0135] The usable solvent is not limited to these, and two or more of these may be mixed and used as the solvent.

[0136] Among these, preferred! /, For example, an organic EL material! /, Depending on each functional layer material, generally, good solvents include, for example, aromatic solvents and halogen-based solvents. Melting Medium, ether solvents, and the like, preferably aromatic solvents and ether solvents. In addition, examples of the poor solvent include leaves, alcohol solvents, ketone solvents, paraffin solvents, and the like. Among them, alcohol solvents and norafin solvents.

[0137] As the electrode material, in the present invention, the first electrode can be formed on the first substrate and the second electrode can be formed on the second substrate in advance. Can be formed.

[0138] Of the two electrodes, as the conductive material used for the anode for injecting holes, those having a work function larger than 4 eV are suitable. Silver, gold, platinum, palladium, etc. Metal oxides such as alloys, tin oxide, indium oxide and ITO, and organic conductive resins such as polythiophene polypyrrole are used. ITO is preferred as a transparent electrode that is preferably translucent. The method for forming the ITO transparent electrode is not limited to the force capable of using mask vapor deposition or photolithography patterning.

[0139] As the conductive material used as the cathode, a material having a work function smaller than 4 eV is suitable, such as magnesium and aluminum. Typical examples of alloys include magnesium / silver and lithium / aluminum. The formation method can be mask vapor deposition, photolitho patterning, plating, printing, etc., but is not limited thereto.

[0140] In the present invention, a glass substrate and a transparent resin film are used as the substrate. Examples of transparent resin films include polyethylene, ethylene acetate butyl copolymer, ethylene monobutyl alcohol copolymer, polypropylene, polystyrene, polymethyl methacrylate, polychlorinated butyl, polybutyl alcohol, polybutyl butyral, naychitone, and polyethylenol. Ethenoleketones, polysanolethone, polyethenoresanorephones, tetrafluoroethylene perfluoroalkyl butyl ether copolymers, polybulufluoride, tetrafluoroethylene ethylene copolymers, tetrafluoroethylene monohexaph Fluoropropylene copolymer, polychloroethylene, polyvinylidene fluoride, polyester, polycarbonate, polyurethane, polyimide, polyetherimide, polyimide, polypropylene Ren, and the like.

[0141] Furthermore, the organic EL device of the present invention has a light-emitting layer of the organic layer that is filtered for each of three colors of RGB. It is possible to make it a full-color display by configuring it with a turn and incorporating a drive circuit.

Example

[0142] Hereinafter, the production of an organic EL element using a vacuum bonding apparatus will be specifically described, but the present invention is not limited thereto.

[0143] <Production of anode side member>

A transparent support substrate was prepared by depositing ITO (indium oxide) with a film thickness of lOOnm as an anode on a lOOmmX lOOmm X l. 1 mm glass substrate. This was ultrasonically cleaned with isopropyl alcohol, dried with dry nitrogen gas, and UV ozone cleaned for another 5 minutes.

[0144] On this transparent support substrate, a solution of poly (3,4 ethylenedioxythiophene) polystyrene sulfonic acid (PEDOT / PSS Bayer, Baytron P A1 4083) diluted to 70% with pure water was prepared. A film was formed by spin coating at 3000 rpm for 30 seconds and then dried at 200 ° C. for 1 hour to provide a hole injection layer having a thickness of 30 nm.

[0145] Next, on this hole injection layer, 60 mg of PVK (polybulur rubazole) and 1 of Ir (ppy)

A solution in which 5 mg was dissolved in dichlorobenzene was similarly applied by spin coating, and after film formation, vacuum dried at 60 ° C. for 1 hour to form a light emitting layer having a dry film thickness of 30 nm.

[0146] [Chemical 1] ir (ppy) ₃

[0147] Production of cathode side member

Next, 80mm X 80mm X O. 3mm thick Aluminum 120 nm was vapor-deposited as a cathode, and then lithium fluoride lnm was vapor-deposited as a cathode buffer layer. This was transferred from a vacuum chamber to a nitrogen atmosphere, and a solution of BCP (20 mg) dissolved in 10 ml of toluene using a spin coater was used. Spin coating (film thickness of about 10 nm) at 60 ° C under the conditions of lOOOrpm and 30 sec. Vacuum-dried for 1 hour to form an electron transport layer.

[0148] Next, on this electron transport layer, PVK (60mg) and 1.5mg Ir (ppy)

Three

The solution dissolved in 6 ml of the solution was similarly applied by spin coating, and after film formation, vacuum-dried at 60 ° C. for 1 hour to form a light-emitting layer having a dry film thickness of 30 m.

[0149] [Chemical 2]

[0150] Formed above,

Organic EL member A (anode member);

Glass substrate // ITO (anode: lOOnm) // PEDOT / PSS (hole injection layer: film thickness 30nm) // PVK + Ir (ppy) (light emitting layer: film thickness 30nm),

Organic EL member B (cathode member);

Polyethersulfone (PES) film // aluminum (120 nm) cathode / lithium fluoride (lnm) cathode buffer layer // BCP (film thickness about 10 nm) electron transport layer // PVK (60 mg) and 1.5 mg Ir ( ppy) (film thickness 30nm) light emitting layer,

Was bonded using a vacuum bonding apparatus as shown in FIG.

[0151] First, a thermosetting adhesive sheet is disposed around the organic layer on the glass substrate of the organic EL member A produced as described above, and further, the organic EL member B is opposed to the organic EL member A and the respective light emitting layers. Further, a moisture-proof film as a sealing member was further laminated on the back side of the cathode member and temporarily bonded. Figure 2 (b) shows this. S shows the adhesive sheet cut and placed around the organic layer on the glass substrate. As the thermosetting adhesive sheet, a thermosetting adhesive sheet TBF560 (ethylene-butyl acetate copolymer) manufactured by Sumitomo 3EM was used. Also sealed As the moisture-proof film as a stopper, a GX film made by Toppan Printing, which is a ceramic vapor-deposited film, was used. The sealing member was approximately the same size (100 mm × 100 mm) as the glass substrate of the organic-elect mouth luminescence member A (anode member). Figure 2 (b) shows this state.

[0152] Next, the above laminate is placed on a frame in the vacuum chamber 101 of the vacuum laminating apparatus with the organic substrate luminescence member A (anode member) facing down on the glass substrate, and the cylinder is driven. Then, the elastic member 102 was lowered and pressed from the back side of the sealing member 3 to bring the organic layers into close contact with each other, thereby fixing the laminate (FIG. 2 (d)). At the same time, the vacuum chamber was shut off from the outside air and evacuated with a vacuum pump (not shown) to raise the vacuum to a pressure of about lkPa (Fig. 2 (e)).

[0153] The degree of vacuum is adjusted and maintained within the above range. This time, the heater driving cylinder 105 is driven to lower the heater 104, and the sealing material S (thermal The sealing member was pressed onto the cured adhesive sheet) and heated (temperature 80 ° C, pressure 0.15 MPa, 5 seconds). Thereby, the sealing member and the glass substrate were bonded. This is shown in Figure 2 (f).

[0154] When the heater 104 and the elastic member 102 are raised again by driving the cylinder, the sealing member and the glass substrate are bonded around the organic layer, and a bonded body of an organic EL element having a sealing structure is obtained. .

[0155] After the bonded portion was cooled, the vacuum chamber of the bonding apparatus was opened, the pressure was returned to atmospheric pressure, and the bonded organic EL element was taken out.

[0156] By returning to atmospheric pressure, pressure is received from both substrates by the difference between the sealed space and atmospheric pressure, so the pressure inside the sealed space finally returned to a pressure of about lOkPa. But

Thus, an organic EL device was obtained in which the light emitting layers were uniformly and closely adhered and bonded together by the differential pressure from atmospheric pressure (101.3 kPa).

[0157] Comparative Example

A temporary laminate of a laminate of the organic electoluminescence member A (anode member), organic electroluminescence member B (cathode member), and sealing member (GX film) used in the examples (Fig. 2 ( b) Using), an organic EL element was produced by a roll laminating apparatus.

[0158] Using MMC-650Y as a roll laminating device (Fig. 4), adjusting the gap between rolls, surface pressure 0.5MPa, speed 10mm / sec, temperature 80 Heating at ° C By passing a rubber roll, the thermosetting adhesive sheet (encapsulant) is thermoset to seal the sealing member and glass. The organic EL element was fabricated by adhering and sealing the substrate and bonding the anode and cathode members together.

When the above elements were energized ( ^2.5 mA / cm ² ) and allowed to emit light continuously, the organic EL elements bonded by the method of the present invention were compared in terms of all of the light emission unevenness and light emission luminance. It was an element superior to the organic EL element bonded and fabricated using the roll bonding device.

Claims

The scope of the claims

[1] In an organic electroluminescence element having at least one organic layer between a first electrode and a second electrode, the organic electoluminescence element comprises:

On the first substrate, a first electrode, an organic electoluminescence member A having at least one organic layer, and

Each of them is bonded so that the organic layers face each other,

[2] In the method for manufacturing an organic electroluminescent element having at least one or more organic layers between the first electrode and the second electrode, the first electrode and at least one or more organic layers are formed on the first substrate. The organic electroluminescent port luminescence member A and the second electrode, the organic electroluminescent port luminescent member B having at least one organic layer on the second substrate, were shielded from the outside air at a pressure of 50 kPa, respectively. A method for producing an organic electoluminescence device, comprising adhering layers so as to face each other, adhering and sealing the periphery of the substrate, and laminating the organic electroluminescence device A and the organic electroluminescence device B.

[3] In the method of manufacturing an organic electroluminescent element having at least one or more organic layers between the first electrode and the second electrode, the first electrode and at least one or more organic layers are formed on the first substrate. The organic electroluminescent port luminescence member A having the second electrode and the organic electroluminescent port luminescent material B having at least one or more organic layers are brought into close contact with each other so that the respective organic layers face each other. ,

Furthermore, a sealing member is laminated on the second substrate,

0 0 kPa shut off from outside air A method for producing an organic electoluminescence device comprising adhering and sealing the periphery of a first substrate and a sealing member, and bonding the organic electroluminescence device A and the organic electroluminescence device B .

[4] The method for producing an organic electoluminescence device according to claim 2 or 3, wherein the sealing is performed with a photocurable adhesive.

[5] A photocurable adhesive is previously installed around at least one organic layer of the first substrate or the second substrate,

3. The organic elect according to claim 2, wherein at least one of the first substrate and the second substrate is irradiated with light to cure, bond and seal the photocurable adhesive. A method for manufacturing an oral luminescence element.

[6] A photocurable adhesive is previously installed around at least one organic layer of the first substrate or the sealing member,

4. The organic layer according to claim 3, wherein the photocurable adhesive is cured, adhered, and sealed by irradiating at least one of the first substrate and the sealing member. A method for producing a recto-luminescence device.

[7] The method for producing an organic electoluminescence device according to [2] or [3], wherein the sealing is performed with a heat-fusible adhesive.

[8] A heat-fusible adhesive is previously installed around at least one organic layer of the first substrate or the second substrate,

Under a pressure of 0 to 50 kPa cut off from the outside air, the organic layer of the organic electoluminous luminescence member A and the organic layer of the organic electroluminescent luminescence member B are brought into close contact with each other, 3. The organic electric device according to claim 2, wherein at least the periphery of the first substrate and the second substrate is heated to thermally melt and bond and seal the heat-fusible adhesive. A method for producing a troluminescence element.

[9] A heat-fusible adhesive is previously installed around at least one organic layer of the first substrate or the sealing member,

4. The organic elect mouth according to claim 3, wherein at least the periphery of the first substrate and the sealing member is heated to thermally melt and bond and seal the heat-fusible adhesive. Manufacturing method of luminescence element.

10. The organic electroluminescent mouth luminescence device according to claim 1, wherein a moisture-proof layer is provided on at least one of the first substrate and the second substrate.

[11] The organic electroluminescent device according to any one of claims 2 to 9, wherein at least one of the first substrate and the second substrate has a moisture-proof layer. Manufacturing method.

12. The organic electroluminescent mouth luminescence element according to claim 1, wherein a hygroscopic member is provided on at least one of the first substrate and the second substrate.

[13] The organic electoluminescence according to any one of [2] to [9], wherein a moisture absorbing member is applied to at least one of the first substrate and the second substrate. A manufacturing method of a capacitance element.