JP2001326069A - Organic electroluminescent element and manufacturing method of the same - Google Patents

Abstract

PROBLEM TO BE SOLVED: To provide an electroluminescent element with high insulation property between elements, good sealing property, fine patterning, and uniform luminous property. SOLUTION: The organic electroluminescent element comprises a luminous element 17 having an organic layer 13 including a luminous layer interposed between a lower electrode 12 formed on a substrate 11 and an opposing electrode 14, and a non-luminous part 18 with an inter-layer insulation film 15 formed on the substrate and the lower electrode 12, and a moistureproof layer 16 at the outer surface of the non-luminous part.

Description

DETAILED DESCRIPTION OF THE INVENTION

[0001]

BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to an organic electroluminescence device (hereinafter abbreviated as "organic EL device"), and more particularly to a device having high definition, high uniform light emission, and excellent sealing performance. In particular, the present invention relates to an organic EL device having high utility for display.

[0002]

2. Description of the Related Art In recent years, organic EL elements for displays have been actively developed. An organic EL element used for a display is required to have high definition (precision) patterning and high uniform light emission.

Japanese Patent Application Laid-Open No. 3-250583 discloses an element having a light-emitting portion and a non-light-emitting portion formed of an interlayer insulating film, which has good pattern accuracy and high light emission uniformity. Japanese Patent Application Laid-Open No. Hei 5-275172 discloses a high-definition display having a line pitch of about 100 μm by providing a wall-shaped interlayer insulating film and forming a cathode by oblique vapor deposition.

However, in the organic EL device provided with the interlayer insulating film as described above, the light emitting element portions (pixels) adjacent to each other with the interlayer insulating film interposed therebetween may be insulated and not separated from each other. Precision may be insufficient. On the other hand, in an organic EL device provided with an interlayer insulating film, the thin film of the counter electrode is separated due to the presence of a step in the interlayer insulating film, so that the sealing performance is reduced, whereby the electrode is oxidized and deteriorated, and light is emitted. Defects (dark spots,
Dark area). Due to this light emission defect, the uniformity of light emission is significantly reduced. In addition, the decrease in the sealing ability causes a short circuit between the adjacent light emitting element portions because the electrodes come into contact with oxygen or moisture, which is a cause of lowering their insulation and separation properties. These problems are fatal defects for an organic EL element for a display.

[0005]

SUMMARY OF THE INVENTION The present invention has been made in view of the above, and has high insulation separation between light emitting element portions, excellent sealing ability, high definition patterning, and light emission. An object is to provide an organic EL device having excellent uniformity.

[0006]

Means for Solving the Problems As a result of intensive studies, the present inventors have found that the outer surface of the non-light emitting element portion, or the outer surface of the non-light emitting element portion and the outer surface of the light emitting element portion have a specific moisture-proof property. It has been found that the object of the present invention can be effectively achieved by forming an insulating film, and the present invention has been completed. That is, the gist of the present invention is as follows. <1> A light-emitting element portion having an organic layer including a light-emitting layer between a lower electrode provided on a substrate and a counter electrode, and a non-light-emitting element having an interlayer insulating film patterned on the substrate and the lower electrode And an organic electroluminescent element having a moisture-proof insulating film formed on an outer surface of the non-light-emitting element portion. <2> The organic electroluminescent device according to <1>, wherein the moisture-proof insulating film is formed on an outer surface of the non-light emitting element portion and an outer surface of the light emitting element portion. <3> The moisture vapor permeability of the moisture-proof insulating film is 10 g / (m ²
-24h) The organic electroluminescent device according to <1> or <2> above. <4> An oxide, nitride, or acid formed by oxidizing, nitriding, or oxynitriding a material used for a counter electrode with active oxygen and / or activated nitrogen as a main component of the moisture-proof insulating film. The organic electroluminescence device according to any one of <1> to <3>, which is a nitride. <5> The moisture-proof insulating film is made of AlOx (5/4 <x <3 /
The organic electroluminescence device according to any one of the above <1> to <4>, which includes item 2). <6> The moisture-proof insulating film is made of AlNy (4/5 <y <4 /
The organic electroluminescence device according to any one of the above <1> to <4>, which includes item 3). <7> The light-emitting element portions adjacent to each other with the interlayer insulating film interposed therebetween
The organic electroluminescent device according to any one of <1> to <6>, which is separated and insulated from each other. <8> The organic electroluminescent device according to any one of <1> to <7>, further including a stress relaxation layer between the interlayer insulating film and the moisture-proof insulating film and / or between the counter electrode and the moisture-proof insulating film. . <9> The material of the stress relaxation layer has a Young's modulus of 1 × 10 ⁵ N /
The organic electroluminescence device according to <8>, wherein the metal is m ² or less. <10> Step of forming lower electrode on substrate, step of providing patterned interlayer insulating film, step of forming organic layer including light emitting layer, step of forming counter electrode, and outer surface of non-light emitting element portion Alternatively, a method for manufacturing an organic electroluminescent device, comprising a step of forming a moisture-proof insulating film on an outer surface of a non-light emitting element portion and an outer surface of a light emitting element portion. <11> The organic electroluminescent device according to <9> or <10>, wherein the step of forming the moisture-proof insulating film forms a film having a water vapor moisture permeability of 10 g / (m ² · 24 h) or less. Production method. <12> The step of forming the moisture-proof insulating film comprises forming an oxide, nitride or oxynitride of the material used for the counter electrode with the activated oxygen and / or the activated nitrogen. > Or <11>, the method for producing an organic electroluminescence device according to <11>. <13> In the step of forming the moisture-proof insulating film, after the step of forming the counter electrode, the film formed in the step is oxidized, nitrided, or oxynitrided with activated oxygen and / or activated nitrogen. The method for producing an organic electroluminescence device according to any one of the above <10> to <12>. <14> The step of forming a moisture-proof insulating film is performed by oxidizing, nitriding, or oxynitriding with activated oxygen and / or activated nitrogen to form a film of a material used for a counter electrode, Wherein the material used for the nitrided or oxynitrided counter electrode is deposited.
The method for producing an organic electroluminescence device according to any one of <12> to <12>. <15> The organic device according to any one of <10> to <14>, further including a step of providing a stress relaxation layer between the interlayer insulating film and the moisture-proof insulating film and / or between the counter electrode and the moisture-proof insulating film. A method for manufacturing an electroluminescence element.

[0007]

Next, an embodiment of the present invention will be described. The present invention provides a non-light-emitting device in which a light-emitting element portion having an organic layer including a light-emitting layer is provided between a lower electrode provided on a substrate and a counter electrode, and an interlayer insulating film patterned on the substrate and the lower electrode is present. An organic electroluminescence device having an element portion, wherein a moisture-proof insulating film is formed on an outer surface of the non-light emitting element portion, or an outer surface of the non-light emitting element portion and an outer surface of the light emitting element portion. Element.

Here, the patterned interlayer insulating film is a portion (light emitting element portion: pixel) which is located on the substrate and the lower electrode and has an opening where the interlayer insulating film does not exist by the pattern processing. )
An insulating film that exists as an insulating film and forms a non-light emitting element portion which does not itself form a light emitting element. On top of this membrane
Further, when the organic layer and the counter electrode are formed, only the opening where the patterned interlayer insulating film does not exist can be energized, and accurate light emission can be obtained only in that portion. Due to the presence of such an interlayer insulating film, light emission with high pattern accuracy can be obtained.

The shape of the interlayer insulating film is not particularly limited, and examples thereof include those having a tapered cross section, a vertical cross section, and a reverse taper. In the present invention, among these, those having a tapered shape or a vertical sectional shape are preferable, and those having a tapered shape are more preferable. The thickness (height) of the interlayer insulating film may be a thickness having an insulating effect, and is usually preferably 50 nm to 20 μm, and preferably 5 nm to 20 μm.
00 nm to 10 μm is more preferably used.

[0010] The material of the interlayer insulating film used in the present invention may be any material as long as it is an insulator and is capable of high-definition patterning.
Various insulating polymers, insulating oxides, nitrides, and the like can be given. Specific examples of preferred insulating polymers include:
Polyimide, fluorinated polyimide, polyolefin, polyacrylate, fluorinated polymer, polyquinoline, etc. are preferred. Preferred insulating oxides and nitrides include AlOp (1/2 <p ≦ 3/2), SiOq, and fluorine addition. SiOq (1 <q <2), Si ₃ N _{4 and the} like.

Further, as for the material of the interlayer insulating film, a material having low hygroscopicity is more preferable. Specifically, ASTM-D
It is preferably 0.5% by mass or less, particularly preferably 0.1% by mass or less, as measured by the 570 method. This is because an interlayer insulating film having high hygroscopicity causes oxidation and deterioration of an electrode of an organic EL element due to bleeding of water mixed during the element production, causing light emission defects (dark spots) and the like. Examples of the material of such a low hygroscopic interlayer insulating film include a fluoropolymer and a polyolefin. Further, as a means for improving the hygroscopicity of the interlayer insulating film, the interlayer insulating film may contain a water absorbing agent. The water absorbing agent also adsorbs water invading from the outside in addition to the water contained in the above-described element, thereby suppressing the occurrence of dark spots and dark areas due to oxidation of the element constituting materials including the electrodes. This has the effect of maintaining the uniformity of the light emitting surface of the device. The water-absorbing agent used here is not particularly limited as long as it is a material that adsorbs moisture. However, it is desirable that the water-absorbing agent has a large amount of water absorption and has a property of hardly releasing once-adsorbed water. The shape of such a water-absorbing agent is not particularly limited, but a powdery one is preferable because it has a large adsorption area and a high water-absorbing ability. The average particle size of the water absorbing agent is 0.03 to 2 μm.
m is preferable in terms of enhancing water absorption performance, and more preferably 0.1 to 2 μm in average particle size. The content of the water-absorbing agent in the interlayer insulating film is not particularly limited because it depends on the type and particle size of the water-absorbing agent, but is generally preferably 1 to 90 vol%, more preferably 10 to 30 vol%. 1v
If the amount is less than 90% by volume, the effect of adsorbing moisture may be insufficient, and if it exceeds 90% by volume, the patterning accuracy of the interlayer insulating film may be reduced. Further, a water-absorbing agent that has been activated or dehydrated is preferred because of its high water-absorbing ability.

Specific examples of the water-absorbing agent usable in the present invention include silica gel, zeolite, activated alumina, titania, diatomaceous earth, activated carbon, hemihydrate gypsum, phosphorus pentoxide,
Magnesium perchlorate, potassium hydroxide, calcium sulfate, calcium bromide, calcium oxide, barium oxide,
Inorganic compounds such as zinc oxide, zinc bromide, and anhydrous copper sulfate, and metals such as lithium, beryllium, potassium, sodium, magnesium, rubidium, strontium, and calcium, and metal alloys containing these, and further, a water-absorbing resin, for example, Examples include polyamide, polyimide, acrylic polymer, and methacrylic polymer.
These may be used alone or in combination of two or more.

Further, the material of the interlayer insulating film of the present invention may have a photosensitive function. When a material having this function is used, photolithography can be performed without using a photoresist, and there is an effect that a patterning process of an element is simplified. As the material having the photosensitivity, a commercially available material of this type can be used.

In the present invention, the interlayer insulating film needs to be patterned so as to provide a light emitting element portion. This pattern processing method is not particularly limited, and can be performed by various methods. As a typical method, there is a method using photolithography. In this method, first, an interlayer insulating film is formed, then the photoresist is exposed and developed, and then patterned. When an insulating polymer is used for forming an interlayer insulating film, a polymer solution or a polymer precursor solution is usually applied by a coating method, a spin coating method, a dipping method, and the like.
In the case of oxides and nitrides, a normal vapor deposition method and a chemical vapor deposition method (CV
D method), plasma CVD method, ECR (Electron)
Cyclotron Resonance) -CVD
, Sputtering, ECR-sputtering, or the like. In order to expose and develop the photoresist, first, a photoresist and an exposure method suitable for a desired pattern definition are selected. Examples of the exposure method include a contact exposure method and a reduction exposure method. Subsequently, patterning is performed. Here, the portion where the photoresist does not remain is removed by etching. Examples of the etching method include a wet etching method in which the interlayer insulating film is dissolved and removed by a solvent, and a dry etching method in which the interlayer insulating film is decomposed and removed by plasma or the like. In the case of using the wet etching method, it is preferable to use a solvent which has a high etching rate of the interlayer insulating film in a direction perpendicular to the substrate. When this solvent is present depending on various interlayer insulating films, it is preferable to use a wet etching method because it leads to reduction of production cost and improvement of productivity. When using a dry etching method, it is important to select an etching gas. For polymers such as polyimide, fluorinated polyimide, polyolefin, polyacrylate, and polyquinoline, etching is preferably performed using oxygen plasma. On the other hand, it is preferable to use, as an etching gas, a fluoropolymer, an oxide, a nitrogen compound, or the like, which is obtained by radicalizing a fluorocarbon gas by plasma. As the fluorocarbon gas, CHF ₃ , CF _{4 and the} like are particularly preferable. Alternatively, a boron halide gas may be used, or oxygen, argon, or the like may be mixed with a fluorocarbon gas and used.

The interlayer insulating film can be prepared as described above. In addition to this method, for example, a paste mixed with an oxide is formed into a film forming pattern by screen printing or the like, and then fired at several hundred degrees. Thus, a method of producing a patterned interlayer insulating film is also effective.

The present invention is an organic electroluminescent device in which a moisture-proof insulating film is formed on the outer surface of a non-light emitting device portion where the above-described patterned interlayer insulating film exists. This moisture-proof insulating film is a film having moisture-proof and insulating properties. The moisture of the moisture-proof insulating film is required to be vapor moisture permeability is 10g / (m ² · 24h) or less, more preferably 5g / (m ² · 24h) or less, 1 g / (M ² · 24h) or less is particularly preferred. If the moisture vapor transmission rate of the moisture-proof insulating film exceeds 10 g / (m ² · 24 h), deterioration of the element constituting material cannot be suppressed, and a dark spot or the like is generated.

The value of the water vapor permeability mentioned here is 40.
℃, relative humidity 90%, specifically,
It can be measured by JIS-Z-0208 (test method of moisture permeability of moisture-proof packaging material) or substantially the same method.

The moisture-proof insulating film as described above only needs to be present on the outer surface of the non-light-emitting element portion. The moisture-proof property of the moisture-proof insulating film allows the electrode to come into contact with external oxygen or moisture. By suppressing the release of oxygen and moisture inside the interlayer insulating film, thereby suppressing the occurrence of dark spots and dark areas.
This has the effect of maintaining the uniformity of the light emitting surface. Further, the moisture-proof insulating film has an effect of insulating and separating adjacent light emitting element portions by its insulating property, and also has an effect of increasing the fineness of patterning.

There are various modes for the position where the moisture-proof insulating film is formed. For example, there is an embodiment in which a moisture-proof insulating film exists on the entire outer surface of the light emitting element portion as well as on the entire outer surface of the non-light emitting element portion (see FIG. 1). This embodiment is a particularly preferable embodiment in that the insulating property is enhanced and the moisture-proof property of the entire organic EL element is further enhanced.

Further, there is an embodiment in which the moisture-proof insulating film is present in a portion located on the outer surface of the interlayer insulating film in the outer surface of the non-light emitting element portion (see FIG. 3). In such an embodiment, both the moisture-proof property and the insulating property of the moisture-proof insulating film are satisfied, so that the object of the present invention can be achieved, and the production time of the moisture-proof insulating film can be further shortened.

Further, a mode in which a moisture-proof insulating film is formed only on the bottom of the interlayer insulating film on the outer surface of the non-light emitting element portion (see FIG. 4). Since the bottom portion of the interlayer insulating film often has the lowest moisture-proof property, the moisture-proof insulating film is concentrated on that portion. Therefore,
The object of the present invention can be achieved even with the moisture-proof insulating film having such an embodiment.

As described above, the moisture-proof insulating film of the present invention necessarily insulates the adjacent light-emitting element portions from each other, and as long as the moisture-proof property of the interlayer insulating film can be ensured, the moisture-proof insulating film does not necessarily cover the outer surface of the non-light-emitting element portion or the light-emitting element portion. It does not have to cover the whole surface.

The thickness of the moisture-proof insulating film in the present invention is not particularly limited, and varies depending on the material. However, it is usually only required to be about 10 nm.

The material of the moisture-proof insulating film is not particularly limited as long as it has the moisture-proof property and the insulating property as described above. It is preferable to use a film containing oxide, nitride, or oxynitride as a main component. These are particularly preferably oxides, nitrides, or oxynitrides formed by oxidizing, nitriding, or oxynitriding with activated oxygen and / or activated nitrogen. The term "activated oxygen" or "activated nitrogen" as used herein refers to a gas in which the energy level of an oxygen atom-containing gas or a nitrogen atom-containing gas is increased to increase reactivity. For example, it refers to an excited state, a radical state, an ionized state, or a plasma state.

Here, as the metal used as the material for the counter electrode, a metal having high conductivity, specifically, for example, a metal having a specific resistance of 1 × 10 ⁻³ Ω · cm or less is used. And those having a specific resistance of 1 × 10 ⁻⁴ Ω · cm or less are more preferably used. Representative examples of these metals include:
Al, Cu, Ag, Cr, Ta, Mg,
W, Zn, Ti and the like can be mentioned. Also, as an alloy,
Alloys formed from the aforementioned metals, especially alloys with Al and various metals, for example, Al: Si, Al: Ta, Al: L
i, Al: Ca, Al: In and the like. Among these, the case where the material used for the counter electrode is Al or an Al-containing alloy is preferable.

As the material used for the counter electrode, an oxide, a nitride or an oxynitride of a simple metal or an alloy is generally used as the moisture-proof insulating film. That is, specifically, aluminum oxide, copper oxide, silver oxide, chromium oxide, tantalum oxide, magnesium oxide, tungsten oxide, zinc oxide, titanium oxide, and oxides of the aluminum alloys, and furthermore, aluminum nitride, copper nitride, nitride Silver, chromium nitride, tantalum nitride, magnesium nitride, tungsten nitride, zinc nitride, titanium nitride, nitrides of the above-mentioned aluminum alloy, and the like. The films of these oxides and nitrides do not have to have a regular composition. It is not always necessary to be transparent, and a black defective oxide film (a film having a composition deviating from the normal composition), an oxide film in which fine metal particles are dispersed, or a nitride film in which fine metal particles are dispersed may be used. These can be black light-absorbing films, and have an effect of improving the contrast of a light-emitting element or a light-emitting device by forming a light-absorbing moisture-proof insulating film on the surface of a non-light-emitting element portion.

Among these, it is preferable that the moisture-proof insulating film contains aluminum oxide or aluminum nitride. In particular, aluminum oxide is AlOx (5/4 <x <3 /
In the case of containing the compound represented by 2), it is preferable that the aluminum nitride contains the compound represented by AlNy (4/5 <y <4/3).

Next, the method for forming such a moisture-proof insulating film is not particularly limited, but the main component of the moisture-proof insulating film is oxide, nitride or oxynitride of the material used for the counter electrode. The description will be given taking a case as an example. For example, the following method (1) or method (2) can be given.

Method (1) The material used for the counter electrode is formed by vapor deposition or sputtering.
After the formation, activated oxygen and / or
Activated nitrogen, specifically, for example, oxygen, nitrogen, N
O, ammonia, or a mixture of these with a rare gas
By plasma or ionizing and irradiating or exposing
is there. As a result, it is formed of the material used for the counter electrode.
The deposited film is oxidized, nitrided, or oxynitrided. Plasma formation
There are various methods, but microwave, exchange, and
Is to convert gas into plasma by electromagnetic wave (RF)
It is simple. For example, a parallel plate type electrode or
Barrel type electrode is provided and AC or electromagnetic wave is applied to it.
Then, a method of turning into plasma is given. Gas in this case
Conditions such as pressure and degree of vacuum are appropriately selected, and oxidation, nitridation,
Alternatively, oxynitriding may be performed.
2 to 400 mW / cm ^Two, Vacuum degree 10^-2~ 5 × 10^-1P
The condition of a is preferred. On the other hand, when it is ionized and irradiated
In this case, it is also preferable to use an ion gun. Ion gun
Various methods such as ECR type and Kauffman type
There is a formula, the acceleration potential for normal irradiation is 10 V to 3 KV,
Current is 0.1μA ~ 200mA, vacuum degree 10^-6~ 5 × 1
0^-1Perform at Pa.

Method (2) After the counter electrode is formed, an atmosphere of oxidation, nitridation or oxynitridation is activated by activated oxygen and / or activated nitrogen, and the material used for the counter electrode is formed by vapor deposition or sputtering. This is a method of depositing a material used for an oxidized, nitrided, or oxynitrided counter electrode by forming a film. This is a so-called reactive evaporation method. As a method for forming the oxidizing atmosphere in this case, a method of introducing a small amount of oxygen or ozone into the vacuum atmosphere during the deposition and sputtering of the counter electrode is given. For example, if the degree of vacuum is 10 ^-1 to 10 ^-4 P
Oxygen or ozone is introduced into the vacuum chamber so as to satisfy a. The place where oxygen or ozone is introduced may be the entire vacuum chamber, or may be sprayed near the substrate or on the surface of the counter electrode. Further, oxygen and ozone may be used by being mixed with a rare gas or the like. As a method for forming an oxidizing atmosphere, a plasma atmosphere is formed, through which vapor-deposited particles of a material used for a counter electrode are passed and oxidized.
It may be deposited. As the plasma forming method, there are various methods as described above. Another preferable method of forming an oxidizing atmosphere is a method of ionizing oxygen and depositing a material used for a counter electrode while irradiating the ionized oxygen.
Examples of the method of the ion gun used here include the same method and conditions as described above. Further, as a method of forming the nitriding or nitriding atmosphere, a method of introducing a small amount of nitrogen or ammonia into a vacuum atmosphere during vapor deposition or sputtering of a material used for the counter electrode may be used. More preferably, the atmosphere is formed by a method in which a plasma atmosphere is formed, through which vapor-deposited particles of the material used for the counter electrode are passed, thereby nitriding or nitriding and depositing. Examples of the gas to be turned into plasma include oxygen, nitrogen, NO, ammonia, and the like, or a gas obtained by mixing these with a rare gas. Another method of forming the atmosphere is a method of ionizing nitrogen, NO, and ammonia, and depositing a material used for the counter electrode while irradiating the ionized nitrogen, NO, and ammonia. The method of the ion gun used here is the same as that described above.

The moisture-proof insulating film thus obtained is
A denser film such as an oxide film that has been oxidized in a normal oxygen or nitrogen atmosphere is formed, and becomes a moisture-proof insulating film exhibiting the above-described specific effects.

Subsequently, a light emitting element portion such as a substrate, an electrode and an organic layer in the organic EL element of the present invention will be described.
First, in the present invention, the substrate of the organic EL device is preferably a substrate having transparency, and generally, glass, transparent plastic, quartz, or the like is used.

In the present invention, the lower electrode may be a cathode or an anode. For example, when the lower electrode is an anode, a conductive transparent oxide electrode may be generally used. Specifically, In oxide, Sn-added In oxide, fluorine-added zinc oxide, In-zinc oxide, and the like can be given. Further, the lower electrode may be composed of a wiring layer and a semiconductive electrode. For example, various inorganic semiconductors and organic semiconductors are used as the semiconductive electrode. Specifically, for example, C, DLC (diamond-like carbon), ZnS, ZnSe, ZnSSe, MgS, MgS
Se, polyaniline and its derivatives, polythiophene and its derivatives, Lewis acid-added amine compound layers, and the like can be used.

The counter electrode in the present invention may be an anode or a cathode. For example, when the counter electrode is a cathode, the material is preferably an alkali metal-containing alloy or an alkaline earth metal-containing alloy. Specifically, for example, Mg: Ag, Al: Li, Pb: L
i, Zn: Li, Bi: Li, In: Li, Al: Ca
And the like. These are corrosion resistant and have a low work function. As another preferred example, an ultrathin film of an alkali metal compound, an alkaline earth metal compound, or a rare earth compound (having a thickness of 0.1 to 10 n) is provided on the interface with the organic layer.
m), on which the above-mentioned metal simple substance or alloy is used. That is, Al, C
u, Ag, Cr, Ta, Mg, W, Zn, Ti, etc.
As the alloy, an alloy formed from the above-mentioned metals, particularly an alloy of Al and various other metals, for example, Al: Si, A
l: Ta, Al: Li, Al: Ca, Al: In and the like. Further, an alkali metal compound, an alkaline earth metal compound or a rare earth compound may be added to the organic layer close to the cathode to enhance the electron injecting and transporting properties, and then the above metal or alloy may be used.

Next, the organic layer of the organic EL device according to the present invention is not particularly limited. For example, the following structure may be mentioned. Anode / light-emitting layer / cathode anode / hole-transport layer / light-emitting layer / cathode anode / hole-transport layer / light-emitting layer / electron-transport layer / cathode anode / hole-injection layer / hole-transport layer / light-emitting layer / electron-transport layer / Cathode The organic layer in the present invention means the above-described hole injection layer, hole transport layer, light emitting layer, and electron transport layer. However, other than the light emitting layer, it is not always necessary to be formed from an organic material, and an inorganic semiconductor material, an inorganic insulating material, or the like may be used as necessary. In the present invention, the material used for each layer is not particularly limited, and any material can be used. For example, as the organic material used for the light emitting layer, a distyryl derivative, an 8-hydroxyquinoline-based metal complex, or the like is effective as the light emitting material, and a polyfluorene derivative, a polyarylene vinylene derivative, or the like is also useful.

The organic layer can be formed by a vapor deposition method,
Various methods such as a spin coating method and a bar coating method can be used. When an organic compound having a molecular weight of 300 to 2,000 is used, it is preferable to use a vapor deposition method from the viewpoint of uniformity of film thickness and no defect, and when the organic compound has a molecular weight of 2,000 or more, a wet method is used. It is preferable to use a spin coating method, a bar coating method, a spray method, or the like.

As a method for forming these films, a vapor deposition method and a sputtering method are preferably used, and a vapor deposition method is particularly preferable. The vapor deposition method used in the present invention may be any method, but it is more preferable that the vapor deposition is performed from directly below the substrate surface.

Next, the second invention of the present invention will be described. The second invention of the present invention is an organic EL device having a stress relaxation layer between the interlayer insulating film and the moisture-proof insulating film and / or between the counter electrode and the moisture-proof insulating film.

By providing this stress relaxation layer, it is possible to suppress the occurrence of cracks in the moisture-proof insulating film due to the stress mainly generated due to the difference in the coefficient of thermal expansion between the interlayer insulating film or the counter electrode and the moisture-proof insulating film. And the effect of maintaining and improving the moisture-proof and sealing effects of the moisture-proof insulating film. Thereby, the effect of imparting uniformity of light emission of the organic EL element in the present invention is further increased.

The purpose of the stress relaxation layer can be achieved if it exists between the interlayer insulating film and the moisture-proof insulating film and / or between the counter electrode and the moisture-proof insulating film. The thickness of the stress relaxation layer is not particularly limited, but may be 10 nm to 10 nm.
μm is preferred. Further, as the material of the stress relaxation layer, a metal having a Young's modulus softer than the material used for the counter electrode is preferable. For example, the Young's modulus is 1 × 10 ⁵ N / m ^2.
(1 × 10 ⁴ kg / m ² ), preferably 6 × 10 4
Metals of ⁴ N / m ² (6 × 10 ³ kg / m ² ) or less are more preferable, and Young's modulus is 3 × 10 ⁴ N / m ² (3 × 10 ³ k).
g / m ² ) or less are particularly preferred. Young's modulus is 1 ×
In the case of a metal exceeding 10 ⁴ N / m ² , stress is generated, and a dark spot is easily enlarged, which is not preferable. Specific preferred materials include In, Pb, Sn, Sb, and B.
i and their alloys and various solders. Further, as another preferred embodiment, the above-described intermediate composition or graded composition of the material of the moisture-proof insulating film and the counter electrode is exemplified. Examples of the intermediate composition include a mixed composition of a counter electrode material and an inorganic compound such as an oxide or a nitride which is a moisture-proof insulating film. As the graded composition, at the boundary between the counter electrode and the inorganic compound film, as the counter electrode shifts to the inorganic compound film, the degree of oxidation of the counter electrode gradually increases and approaches the composition of the moisture-proof insulating film, or In this embodiment, the same composition is used to form a moisture-proof insulating film.

As a method for forming the stress relaxation layer, a vacuum evaporation method or a sputtering method is preferable. This is because the above soft metal has a low melting point and is extremely easy to vapor-deposit. For example, a stress relaxation layer can be formed by vacuum-depositing these metals after forming a film of the material used for the counter electrode in the counter electrode forming step. Another method is to gradually evaporate or sputter the material used for the counter electrode to an oxidizing or nitriding atmosphere,
A method of forming a mixed composition or a graded composition of the counter electrode material and the inorganic compound is exemplified. If the atmosphere is gradually oxidized or nitrided, the degree of oxidation or nitridation of the above-described counter electrode gradually increases and approaches the composition of the moisture-proof insulating film, or
It is possible to realize a form that has the same composition and becomes a moisture-proof insulating film.

As a method of gradually changing the atmosphere to an oxidizing atmosphere or a nitriding atmosphere, there is a method of increasing the amount of introducing a small amount of oxygen or ozone into a vacuum atmosphere during vapor deposition or sputtering of a counter electrode, as described above. . As another method of forming the atmosphere, a plasma atmosphere is formed, and vaporized particles of the material used for the counter electrode are passed through the plasma atmosphere to oxidize the atmosphere.
A method of depositing while nitriding or oxynitriding may be used. In this case, a method of increasing the plasma output may be used. As still another method, it is also preferable to increase the ionization acceleration potential or increase the ion current value when depositing a material to be used for the counter electrode while ionizing nitrogen, NO, and ammonia while irradiating them. .

Next, the organic EL device of the present invention can be efficiently and economically manufactured by the following method. The method for manufacturing an organic EL device according to the present invention includes a step of forming a lower electrode on a substrate, a step of providing a patterned interlayer insulating film, a step of forming an organic light emitting layer, a step of forming a counter electrode, and a step of non-light emitting. An organic EL device manufacturing method including a step of forming a moisture-proof film on an outer surface of an element portion, an outer surface of a non-light emitting element portion, and an outer surface of a light emitting element portion.

In the above manufacturing method, first, a lower electrode is formed on a substrate by an ordinary method. Usually, a conductive transparent oxide is formed by a vapor deposition method, a sputtering method, or a CVD method. When the lower electrode is patterned, a photoresist is formed in a desired pattern on the conductive oxide film by a photolithographic method, and the conductive oxide is etched with an etchant using the photoresist as a mask to perform pattern processing. Can be used. As the etchant used here, acids and the like that are commercially available for this purpose can be used.

Next, as a step of providing a patterned interlayer insulating film, various methods can be selected depending on the material and the like. The above-described interlayer insulating film is formed, a photoresist is exposed and developed, and then the pattern is formed. What is necessary is just to form an interlayer insulating film by a lining process. A screen printing method other than this method may be used.

Subsequently, an organic layer including a light emitting layer is formed.
In this step, the above-described method of forming an organic thin film may be used, and examples thereof include a vapor deposition method and a method of performing vapor deposition a plurality of times using a mask as disclosed in JP-A-3-250583. Subsequently, a step of providing a counter electrode is performed. In this step, as described above, the material used for the counter electrode is formed on the organic thin film by vapor deposition or sputtering.

Next, in the present invention, a moisture-proof insulating film is formed on the outer surface of the non-light emitting element portion. The moisture-proof insulating film may be formed on the entire outer surface of the light emitting element portion together with the outer surface of the non-light emitting element portion as described above,
It may be formed only on a part of the outer surface of the non-light emitting element portion.

[0048] Also, the moisture-proof insulating film is required to be vapor moisture permeability is 10g / (m ² · 24h) or less, more preferably 5g / (m ² · 24h) or less, 1g / (M ² · 24h) or less is particularly preferred.

In the step of forming the moisture-proof insulating film, a film mainly composed of an oxide, nitride or oxynitride of the material used for the counter electrode is formed on the outer surface of the non-light emitting element portion or the like. The step is preferred in that the formation of the film is easy.

As a method of forming a film mainly composed of an oxide, nitride or oxynitride of the material used for the counter electrode, as in the above-mentioned method (1), a film used for the counter electrode is used. After the step of forming a film of the material, a method of oxidizing, nitriding or oxynitriding the film formed by the step, or forming the film under an oxidizing, nitriding or oxynitriding atmosphere as in the method (2). And a method of depositing a material used for the oxidized, nitrided or oxynitrided counter electrode.

In the present invention, as described above, a moisture-proof insulating film such as a film mainly containing an oxide, a nitride or an oxynitride of the material used for the counter electrode is formed. Thereby, the adjacent light emitting element portions are insulated and separated. In particular, a portion of the outer surface of the non-light emitting element portion corresponding to the outer surface of the interlayer insulating film usually has a thin counter electrode layer. Therefore, after forming a film of a material used for the counter electrode, the film is strongly applied. If the substrate is oxidized, nitrided or oxynitrided, the two opposing electrodes separated by the interlayer insulating film are insulated and separated. In the present invention, it is not always necessary to use an interlayer insulating film having a reverse tapered cross section, and if an interlayer insulating film having a stepped cross section is used, the counter electrode layer provided on this side outer surface is completely oxidized or nitrided, The opposing electrodes can be separated and independent. Particularly, in a preferred embodiment of the present invention, a step of forming a lower electrode as a plurality of parallel electrode lines on a substrate, forming an interlayer insulating film for forming a non-light emitting element portion in a plurality of ribs, and forming the lower electrode into a lower electrode Forming at right angles to the line, forming an organic layer including a light-emitting layer, forming a counter electrode, an outer surface of a non-light-emitting element portion, or an outer surface of a non-light-emitting element portion and an outer surface of a light-emitting element portion Forming a moisture-proof insulating film mainly composed of an oxide, nitride or oxynitride of the material used for the counter electrode and completely insulating the material used for the counter electrode on the side of the rib, Is a method for manufacturing an organic EL element, which comprises at least a step of separating and independent parallel electrode lines from each other. By doing so, an XY matrix type organic EL element can be manufactured.

In the method of manufacturing an organic EL device according to the present invention, in addition to the steps of the above-described manufacturing method, a method may be employed between the interlayer insulating film and the moisture-proof insulating film and / or between the counter electrode and the moisture-proof insulating film. A step of providing a stress relaxation layer can also be adopted.

As for the method of providing the stress relaxation layer, the vacuum evaporation method or the sputtering method is preferably used as described above. In this case, the stress relaxation layer can be formed by vacuum-depositing a metal for the stress relaxation layer after the material used for the counter electrode is deposited and thinned. As another method, while depositing or sputtering the material used as the counter electrode, gradually setting the material in the nitriding atmosphere or the oxidizing atmosphere to a mixed or graded composition of the material used for the counter electrode and the inorganic compound. There is a method of forming. If the atmosphere is gradually changed to an oxidizing atmosphere, the degree of oxidation of the material used as the above-described counter electrode gradually increases, and the composition of the moisture-proof insulating film becomes close to or the same as that of the moisture-proof insulating film. it can.

[0054]

〔Preliminary experiment〕

(Confirmation of Composition and Properties of Moisture-Proof Insulating Film 1) A 20 μm-thick A on polyethylene terephthalate (PET) film
l: Li alloy was deposited. Next, this was arranged at the center of the parallel plate type electrode in the plasma irradiation chamber, and the degree of vacuum was 1.2 ×
Oxygen plasma irradiation was performed under the conditions of 10 ⁻² Pa, a volume ratio of Ar: O ₂ of 200: 75, and an RF output of 92 mW / cm ² . The obtained oxide film was analyzed by an X-ray photoelectron spectroscopy (XPS), and as a result, it was found to be AlOx (x = 1.30). The water vapor permeability of this film was 2.5 g / (m ² · 24 h). (Confirmation 2 of composition and properties of moisture-proof insulating film) Instead of oxygen plasma irradiation of confirmation 1, vacuum degree 1.2 × 10 ^-2 Pa, A
r: nitrogen volume ratio 200: 60, RF output 140 mW /
Irradiation with nitrogen plasma was performed under the condition of cm ² . This nitride film is A
10Oy (y = 1.22), and the water vapor permeability is 1.8
g / (m ² · 24 h). (Confirmation of composition and properties of moisture-proof insulating film 3) In place of oxygen plasma in confirmation 1 of composition and properties of moisture-proof insulating film,
O ₂ was ozonized and irradiated. This oxide film is made of AlOx
(X = 0.9), and the water vapor transmission rate is 20 g / (m ^2).
24h). (Confirmation of Composition and Properties of Moisture-Proof Insulating Film 4) Instead of the oxygen plasma irradiation of Confirmation 1, aluminum was vapor-deposited in an oxygen plasma atmosphere at a degree of vacuum of 1.2 × 10 ⁻² Pa to deposit aluminum oxide. This oxide film is formed of AlOx (x = 1.
35) and the water vapor transmission rate is 1.2 g / (m ² · 24
h).

Example 1 (1) Formation of a rib-like interlayer insulating film On a glass substrate 2 having a thickness of 0.7 mm, 300 μm of ITO was deposited.
A substrate having a lower electrode striped at an m pitch was prepared. On this lower electrode, a photosensitive polyolefin-based negative type resist (manufactured by Zeon Corporation; ZCOAT-
1410) by spin coating with a spinner rotation speed of 150
The film was formed by rotating at 0 rpm for 35 seconds. This film thickness is 5.
It was 3 μm. Then in a hot oven at 70 ° C, 3
Dried (baked) for 0 minutes. Next, using a photomask,
Exposure was performed at an irradiation amount of 120 mJ / cm ² by UV exposure at 365 nm. In this exposure pattern, a photosensitive polyolefin-based negative resist, which is an interlayer insulating film having a width of 20 μm, is left as a linear rib line perpendicular to the ITO pattern every 300 μm. Thereafter, the film was developed and cured at 200 ° C. for 2 hours in a clean oven under a dry nitrogen atmosphere to form a rib-like interlayer insulating film. When an image of the cross section of the rib was observed with a scanning electron microscope (SEM), the step of the rib was almost vertical. (2) Preparation of organic EL element The glass substrate on which the interlayer insulating film obtained in the above (1) was formed was subjected to ultrasonic cleaning with isopropyl alcohol for 3 minutes, and further cleaned for 30 minutes with a cleaning device using ozone. Was done. Next, this was mounted on a substrate holder of a vacuum evaporation apparatus (manufactured by Nippon Vacuum Engineering Co., Ltd.). N, N'-diphenyl- was added to the molybdenum resistance heating boat of the vacuum evaporation system.
N, N'-bis- (3-methylphenyl)-(1,1 '
-Biphenyl) -4,4'-diamine (hereinafter abbreviated as TPD), 200 mg, and tris (8-hydroxyquinolinol) aluminum (hereinafter abbreviated as Alq) in another molybdenum resistance heating boat. 2
Then, the vacuum tank was evacuated to 1 × 10 ⁻⁶ torr. Then, the boat was heated to form a hole transport layer having a thickness of 80 nm. Next, without removing the boat from the vacuum tank, the boat was heated and Alq was placed on the hole transport layer.
A light emitting layer having a thickness of 75 nm was formed. Further, without opening the vacuum chamber, Al previously provided in the vacuum chamber:
The resistance heating boat containing the Li alloy was heated to form a 200 nm thick Al: Li counter electrode at a deposition rate of 0.8 nm / s.

Subsequently, the organic EL thus obtained was obtained.
The element was placed at the center of the parallel plate type electrode in the plasma irradiation chamber, the degree of vacuum was 1.2 × 10 ⁻² Pa, and the volume ratio of Ar: O ₂ was 2
At 00:75, an RF plasma was irradiated from above the counter electrode at an RF output of 92 mW / cm ² to oxidize the film deposited as an electrode material on the side of the rib. As a result of analyzing the oxide film on this side by XPS, the main component has a composition of AlOx (x
= 1.30). Also,
When this was observed with an SEM, the outer surfaces of the ribs were all covered with moisture-proof alumina. Next, a sealing plate was bonded to the upper side of the organic EL element using a glass plate having a thickness of 0.7 mm. Seal in inert gas (in dry nitrogen gas)
Then, an ultraviolet curable adhesive was applied to the periphery of the sealing plate, and the sealing plate and the organic EL element were bonded and irradiated with ultraviolet rays.

The organic EL of the present invention thus obtained
Among the element lines, one ITO line and one Al line were selected, and a voltage of 7 V was applied using ITO as a positive (positive) electrode and Al as a negative (negative) electrode. Upon examination, light was emitted only at the intersection of the ITO and Al stripes. That is, it was found that the adjacent Al line was separated and independent. As a result of sequentially applying and applying a voltage to all the Al lines, there were no short-circuited and connected portions, and it was found that the separation patterning of the counter electrode of the organic EL element of the present invention was good. At the same time, the non-emission state of the pixel at the edge of the Al line was examined. The non-emission width was 5 μm or less, and the edge was well defined.

Example 2 An organic EL device according to the present invention was produced in the same manner as in Example 1 except that the organic EL device was irradiated with nitrogen plasma and nitrided instead of being oxidized by irradiating oxygen plasma. The conditions for nitriding are as follows: vacuum degree 1.2 × 10 ^-2 P
a, Ar: nitrogen volume ratio 200: 60, RF output 140
mW / cm ² . As a result of analyzing the nitride film on the rib side after nitriding by XPS, the main component was AlNy (y = 1.2
2), and when this was observed by SEM, all the outer surfaces of the ribs were covered with SiNx. From the lines of the organic EL element after sealing the sealing plate, one ITO line and one Al line were selected, and the ITO was + (positive).
When a voltage of 7 V was applied with the negative electrode and Al as a negative electrode, the accuracy of the pattern was examined under an optical microscope.
Only the intersection of the stripes emitted light. That is, it was found that the adjacent Al line was separated and independent. In addition, as a result of sequentially applying and applying voltage to all Al lines,
There were no short-circuited and connected portions, and it was found that the separation patterning of the counter electrode of the organic EL device of the present invention was good. At the same time, when the non-emission state of the pixel at the edge of the Al line was examined, it was found that the non-emission width was 4.5 μm or less, and the edge was well defined. Therefore, this AlNx functions as a moisture-proof insulating film.

Comparative Example 1 An organic EL device was manufactured in the same manner as in Example 1 except that no oxygen plasma was irradiated. In this device, a large number of portions other than the intersection of the ITO and Al stripes emitted light, and the independence of the cathode was incomplete.

Comparative Example 2 A photosensitive acrylate negative type resist (V259, manufactured by Nippon Steel Chemical Co., Ltd.) was spin-coated on a substrate having the same lower electrode as in Example 1 in the same manner as in Example 1. A film was formed (the film thickness was 5.3 μm).
m). Next, the film was baked in a hot oven at 70 ° C. for 30 minutes, and then exposed using a photomask at an irradiation amount of 450 mJ / cm ^{2 by} UV exposure at 365 nm. Exposure pattern is 300 μm of a photosensitive acrylate negative type resist which is an interlayer insulating film having a width of 20 μm as in Example 1.
Every other time, it was made to remain as a linear rib line perpendicular to the ITO pattern on the substrate. Thereafter, development was performed, and curing was performed in a clean oven at 160 ° C. for 0.5 hour in a dry nitrogen atmosphere to form an interlayer insulating film rib. When an image of the cross section of the rib was observed with an SEM, the rib had a reverse tapered shape.

Thereafter, an organic EL device was manufactured in the same manner as in Example 1. For this element, XPS and section SE
Observation at M showed that the deposited film of the counter electrode material did not cover the outer surface of the rib. It is considered that this was because the ribs were projections having an inverse taper, and thus the counter electrode material was not deposited. However, when the cross section was observed by SEM, a part of the rib did not form an inverse taper, and the deposited film of the counter electrode was continuous at this point.

Next, a sealing plate was adhered to the organic EL element in the same manner as in Example 1 without performing oxygen plasma irradiation. From the obtained device lines, one ITO line and one Al line were selected, and ITO was set to + (positive) electrode, Al
When a voltage of 7 V was applied with-as a (negative) pole, and the accuracy of the pattern was examined under an optical microscope, light was emitted only at the intersection of the ITO and Al stripes. That is, it was found that the adjacent Al line was separated and independent. However, when another line was selected and the same test was repeated, it was found that a number of lines where the counter electrode was not separated occurred. It is considered that this non-separation is caused by the fact that a part does not form a reverse taper.

Comparative Example 3 An element was manufactured in the same manner as in Example 1. However, instead of the parallel plate type plasma irradiation, O ₂ was ozonized and irradiated to the Al: Li counter electrode (the same conditions as in confirmation 3 of the composition and properties of the moisture-proof insulating film). The oxide film thus formed was analyzed by XPS and found to be AlOx (x = 0.9). Further, it was a porous film as observed by SEM. The device was left at room temperature for 24
In the one stored for a long time, many non-emission points were generated.

Example 3 An element was produced in the same manner as in Comparative Example 2. However, after forming the counter electrode, oxygen plasma was irradiated from above the counter electrode in the same manner as in Example 1 to oxidize the electrode material deposited film on the side of the rib. The oxide film was analyzed by XPS, and it was found that the main component was alumina. Then, it sealed with the sealing plate similarly to the comparative example 2.
Of the element lines, one ITO line and one Al line were selected, and ITO was set to a positive (positive) pole and Al was set to-.
When a voltage of 7 V was applied as a (negative) pole and the accuracy of the pattern was examined under an optical microscope, light was emitted only at the intersection of the ITO and Al stripes. That is, it was found that the adjacent Al line was separated and independent. As a result of sequentially applying and applying a voltage to all the Al lines, there were no short-circuited and connected portions, and it was found that the separation patterning of the counter electrode of the organic EL element of the present invention was good. In other words, where the separation of adjacent counter electrode lines is insufficient,
It can be seen that the side portions of the ribs were completely turned into insulators by plasma irradiation.

Example 4 An organic EL device was prepared in the same manner as in Example 1. In this state, alumina as an inorganic compound was coated on the ribs and the counter electrode. In this example, aluminum oxide was further deposited on the alumina surface using a reactive deposition method. In this reactive vapor deposition method, while depositing aluminum as a counter electrode material, the deposit is passed through oxygen plasma formed at a degree of vacuum of 1.2 × 10 ⁻² Pa to deposit aluminum oxide. As a result, a 0.3 μm-thick aluminum oxide film was further deposited on the alumina as a part of the moisture-proof insulating film.
Analysis of the aluminum oxide film by XPS revealed that the main component was alumina having a composition of AlOx (x = 1.35). When this was observed by SEM, it was found that the entire outer surface of the rib was covered with moisture-proof alumina. The organic E of the present invention thus obtained
One line of ITO and one line of Al are selected from the L element lines, and ITO is a + (positive) pole and Al is-(negative).
When a voltage of 7 V was applied as a pole and the accuracy of the pattern was examined under an optical microscope, light was emitted only at the intersection of the ITO and Al stripes. Further, as a result of sequentially applying voltages to all the Al lines and examining them, there were no short-circuited and connected portions, and it was found that the separation patterning of the counter electrode of the organic EL element of the present invention was good. At the same time, the non-emission state of the pixel at the edge of the Al line was examined. The non-emission width was 5 μm or less, and the edge was well defined.

[Embodiment 5] In the process of fabricating the device in the same manner as in Embodiment 1, after forming a counter electrode, In was added with In.
3 μm was deposited to form a stress relaxation layer. Next, AlOx having a thickness of 2 μm was formed by the same reactive evaporation method as in Example 4.
Was formed. Observation of the surface of this device by SEM revealed that AlOx had no cracks.

[0067]

As described above, the organic EL device according to the present invention has high insulation separation between light emitting element portions, excellent sealing ability, high definition patterning, and excellent light emission uniformity. Further, the organic EL element further provided with the stress relaxation layer
The sealing and insulating effects of the moisture-proof insulating film can be further enhanced. Furthermore, the method for manufacturing an organic EL device of the present invention can efficiently and economically manufacture the organic EL device of the present invention.

[Brief description of the drawings]

FIG. 1 is a conceptual cross-sectional view of an organic EL element according to an embodiment of the present invention (when a moisture-proof insulating film is formed on the outer surface of a non-light emitting element portion and the entire outer surface of a light emitting element portion).

FIG. 2 is a plan view in a cross section along XY of FIG. 1;

FIG. 3 is a conceptual cross-sectional view of an organic EL device according to an embodiment of the present invention (in a case where a moisture-proof insulating film is formed on a portion of an outer surface of a non-light emitting element portion located on an outer surface of an interlayer insulating film). )

FIG. 4 is a conceptual cross-sectional view of an organic EL element according to an embodiment of the present invention (in the case where a moisture-proof insulating film is formed on the outer surface of the non-light-emitting element at the bottom of the outer surface of the interlayer insulating film). )

[Explanation of symbols]

 11, 21, 31, 41 Substrate 12, 22, 32, 42 Lower electrode 13, 33, 43 Organic layer 14, 34, 44 Counter electrode 15, 25, 35, 45 Interlayer insulating film 16, 36, 46 Moistureproof insulating film 17 Light-emitting element part 27 Light-emitting element part (pixel) 18 Non-light-emitting element part

──────────────────────────────────────────────────続 き Continued on the front page (51) Int.Cl. ⁷ Identification code FI Theme coat ゛ (Reference) H01L 21/318 H01L 21/318 A H05B 33/10 H05B 33/10 33/12 33/12 B 33/14 33/14 A 33/22 33/22 Z F term (reference) 3K007 AB00 AB05 AB13 AB15 AB18 BA06 BB01 CA01 CB01 DA01 DB03 EA01 EB00 FA01 FA02 4K029 BA41 BA43 BA44 BA58 BC00 BC05 BD00 CA06 DC03 DC04 5F058 AA04 AD04 AD08 AD10 AF01 AG06 AH02 5G435 AA13 AA14 AA16 AA17 BB05 CC09 GG31 HH14 HH18 KK05

Claims (15)

[Claims] 1. A light-emitting element portion having an organic layer including a light-emitting layer between a lower electrode provided on a substrate and a counter electrode, and a non-light-emitting device having an interlayer insulating film patterned on the substrate and the lower electrode. An organic electroluminescent element having a light emitting element portion, wherein a moisture-proof insulating film is formed on an outer surface of the non-light emitting element portion. 2. The organic electroluminescent device according to claim 1, wherein the moisture-proof insulating film is formed on the outer surface of the non-light emitting element portion and the outer surface of the light emitting device portion. 3. The moisture-proof insulating film has a water vapor permeability of 10 g /
(M ² · 24h) or less organic electroluminescent device according to claim 1 or 2. 4. An oxide or nitride formed by oxidizing, nitriding, or oxynitriding a material used for a counter electrode as a main component of the moisture-proof insulating film with activated oxygen and / or activated nitrogen. 4. The organic electroluminescence device according to claim 1, wherein the device is an oxynitride. 5. The method according to claim 1, wherein the moisture-proof insulating film is made of AlOx (5/4 <x
2. A compound containing a compound represented by <3/2).
5. The organic electroluminescent device according to any one of items 1 to 4, 6. The moisture-proof insulating film is made of AlNy (4/5 <y
The compound containing the compound represented by <4/3).
5. The organic electroluminescent device according to any one of items 1 to 4, 7. The organic electroluminescent element according to claim 1, wherein the light emitting element portions adjacent to each other via the interlayer insulating film are separated from each other and insulated. 8. between the interlayer insulating film and the moisture-proof insulating film, and / or
The organic electroluminescence device according to claim 1, further comprising a stress relaxation layer between the counter electrode and the moisture-proof insulating film. 9. The material of the stress relaxation layer has a Young's modulus of 1 × 10.
⁵ N / m ² or less of an organic electroluminescent device according to claim 8 which is a metal. 10. A step of forming a lower electrode on a substrate, a step of providing a patterned interlayer insulating film, a step of forming an organic layer including a light emitting layer, a step of forming a counter electrode, and a step of forming a non-light emitting element portion. A method for manufacturing an organic electroluminescent device, comprising a step of forming a moisture-proof insulating film on an outer surface, an outer surface of a non-light emitting element portion, and an outer surface of a light emitting element portion. 11. The method for manufacturing an organic electroluminescence device according to claim 10, wherein the step of forming the moisture-proof insulating film is a step of forming a film having a water vapor permeability of 10 g / (m ² · 24 h) or less. 12. The step of forming a moisture-proof insulating film is to form an oxide, a nitride or an oxynitride of a material used for a counter electrode with activated oxygen and / or activated nitrogen. Item 12. The method for producing an organic electroluminescence device according to item 10 or 11. 13. The step of forming a moisture-proof insulating film comprises, after the step of forming a counter electrode, oxidizing the film formed in the step with activated oxygen and / or activated nitrogen.
The method for producing an organic electroluminescent device according to claim 10, wherein nitriding or oxynitriding is performed. 14. A step of forming a moisture-proof insulating film by forming an oxide, nitridation or oxynitriding atmosphere with activated oxygen and / or activated nitrogen to form a film of a material used for a counter electrode. The method for manufacturing an organic electroluminescent device according to claim 10, wherein a material used for an oxidized, nitrided, or oxynitrided counter electrode is deposited. 15. An inter-layer insulating film and a moisture-proof insulating film, and / or
The method for manufacturing an organic electroluminescent device according to claim 10, further comprising a step of providing a stress relaxation layer between the counter electrode and the moisture-proof insulating film.