WO2014147789A1 - Organic electroluminescence device, organic electroluminescence device manufacturing method, and film forming method - Google Patents

Abstract

The present invention includes the following: a step in which an organic EL element which includes an organic layer is formed on a lower substrate; and a step in which a laminated body which includes an amorphous silicon nitride film and a plasma polymerized film is formed on the organic EL element by using a surface wave excitation plasma chemical vapor deposition method.

Description

ORGANIC ELECTROLUMINESCENT DEVICE, ORGANIC ELECTROLUMINESCENT DEVICE MANUFACTURING METHOD AND FILM-FORMING METHOD

The present invention relates to an organic electroluminescent device in which a silicon nitride film is formed as a passivation layer, a method for manufacturing the organic electroluminescent device, and a film forming method.

In recent years, organic EL display devices using organic electroluminescence (organic EL) elements have attracted attention as a technology for liquid crystal display devices. In an organic EL display device, oxidation at the interface with an organic layer or an electrode in contact with the organic layer leads to serious deterioration in display performance. For this reason, a sealing method is used in which the periphery of a glass plate to which a glass frit used as a sealing material or a seal-type hygroscopic agent is attached is adhered with a resin.

Furthermore, since the size of the organic EL display device is increasing, a structure in which the space between the organic EL element and the sealing glass is filled with a thermosetting transparent filler or a desiccant (hygroscopic material) has been developed. . This is to maintain the strength of the organic EL display device by filling the space between the organic EL element and the sealing glass with a filler (see, for example, Patent Document 1).

However, in the structure as described above, there is a concern about deterioration of the organic layer and the electrode due to direct contact with the filler. For this reason, it is necessary to arrange a passivation layer between the organic layer and the electrode and the filler to suppress deterioration of the organic EL element.

The characteristics required for the passivation layer include that it can be formed at a temperature lower than the glass transition temperature (Tg) of the organic layer, and that it has high light transmissibility that is compatible with the top emission method. For example, a silicon nitride (SiN) film can be used as the passivation layer.

JP 2004-265776 A

When the SiN film is formed as a passivation layer on the organic EL element by a chemical vapor deposition (CVD) method or the like, fine pores are generated due to the defect growth of the SiN film. And the phenomenon considered that a water | moisture content permeate | transmits through this pore is seen. Even in a structure in which a transparent filler or a hygroscopic material is applied on the SiN film, damage to the electrodes and organic layers of the organic EL element is caused by the applied material itself or by moisture passing through the applied material. A similar problem is expected to arise.

For this reason, a method of increasing the film thickness of the SiN film can be considered, but increasing the film thickness increases the time of the film forming process. As a result, the throughput decreases and the manufacturing cost increases. Moreover, even if the film thickness of the SiN film is sufficiently increased, the barrier property against moisture is not necessarily improved in proportion to the film thickness, and a remarkable effect cannot be expected.

Here, it has been confirmed that when a polymer organic thin film is provided as an intermediate layer between SiN films, the barrier property is remarkably improved as compared with a SiN film having the same total film thickness. This is because the intermediate layer functions as a defect separation layer and a particle embedding layer. However, since the polymer organic thin film is basically formed by vapor deposition, it is a disadvantageous process for manufacturing an organic EL display device and the like in that a uniform film is formed over a large area.

In view of the above problems, the present invention provides an organic EL device, a method for manufacturing the organic EL device, and a film forming method that can suppress deterioration in quality due to moisture permeation into the interior.

According to one aspect of the present invention, an organic electroluminescent device is formed by forming a laminate including an amorphous silicon nitride film and a plasma polymerized film on an organic EL element including an organic layer by surface wave excitation plasma chemical vapor deposition. A method for manufacturing a sense device is provided.

According to another aspect of the present invention, there is provided a film forming method using a surface wave excited plasma chemical vapor deposition apparatus, wherein (a) silane gas and ammonia gas are used as film forming gases at a film forming temperature of 120 ° C. or less. And b) forming an amorphous silicon nitride film on the substrate; and (b) amorphous silicon oxycarbide using a hexamethyldisiloxane gas and an oxygen gas as a deposition gas at a deposition temperature of 120 ° C. or lower. Forming a film on the amorphous silicon nitride film.

According to still another aspect of the present invention, (a) a lower substrate, (b) an organic EL element that includes an organic layer and is disposed on the lower substrate, and (c) is disposed on the organic EL element. An organic electroluminescence device is provided that includes an amorphous silicon nitride film and a laminate including a plasma polymerized film, and the laminate is formed by surface wave excitation plasma chemical vapor deposition.

According to the present invention, it is possible to provide an organic EL device, a method for manufacturing the organic EL device, and a film forming method that can suppress deterioration in quality due to moisture permeation into the interior.

It is a typical sectional view showing the composition of the organic EL device concerning the embodiment of the present invention. It is typical sectional drawing which shows the structure of the laminated body which concerns on embodiment of this invention. It is a schematic diagram which shows the example of the manufacturing apparatus used for the manufacturing method of the organic EL apparatus which concerns on embodiment of this invention. It is process sectional drawing for demonstrating the manufacturing method of the organic electroluminescent apparatus which concerns on embodiment of this invention (the 1). It is process sectional drawing for demonstrating the manufacturing method of the organic electroluminescent apparatus which concerns on embodiment of this invention (the 2). It is process sectional drawing for demonstrating the manufacturing method of the organic electroluminescent apparatus which concerns on embodiment of this invention (the 3). It is process sectional drawing for demonstrating the manufacturing method of the organic electroluminescent apparatus which concerns on embodiment of this invention (the 4). It is a graph which shows the effect of the manufacturing method of the organic EL device concerning the embodiment of the present invention.

Embodiments of the present invention will be described with reference to the drawings. In the following description of the drawings, the same or similar parts are denoted by the same or similar reference numerals. However, it should be noted that the drawings are schematic, and the relationship between the thickness and the planar dimensions, the ratio of the thickness of each layer, and the like are different from the actual ones. Therefore, specific thicknesses and dimensions should be determined in consideration of the following description. Moreover, it is a matter of course that portions having different dimensional relationships and ratios are included between the drawings.

Further, the embodiments described below exemplify apparatuses and methods for embodying the technical idea of the present invention, and the embodiments of the present invention include the material, shape, structure, arrangement, etc. of components. Is not specified as follows. The embodiment of the present invention can be variously modified within the scope of the claims.

As shown in FIG. 1, the organic EL device 1 according to the embodiment of the present invention includes a lower substrate 10, and a lower electrode 21, an organic layer 22, and an upper electrode 23 that are disposed on the lower substrate 10. An organic EL element 20, a stacked body 30 disposed on the organic EL element 20, a filler 40 disposed on the stacked body 30, and a sealing material 50 disposed on the filler 40 are provided.

The strength of the organic EL device 1 can be maintained by filling the space between the organic EL element 20 and the sealing material 50 with the filler 40. Further, a resin film 70 is disposed between the lower substrate 10 and the sealing material 50 so as to surround the periphery of the organic EL element 20, the stacked body 30, and the filler 40. By bonding the lower substrate 10 and the sealing material 50 with the resin film 70, deterioration or oxidation of the organic layer 22 can be suppressed.

The laminated body 30 is formed by a surface wave excitation plasma chemical vapor deposition method, which will be described in detail later. The stacked body 30 includes an amorphous silicon nitride (SiN) film and a plasma polymerization film. As shown in FIG. 2, the stacked body 30 includes a first amorphous SiN film 31 disposed on the organic EL element 20 and a plasma polymerization film 32 disposed on the first amorphous SiN film 31. And a second amorphous SiN film 33 disposed on the plasma polymerization film 32. As the plasma polymerized film 32, for example, an amorphous silicon oxycarbide (SiOC) film or the like can be adopted.

The first amorphous SiN film 31 and the second amorphous SiN film 33 function as a passivation layer disposed so that the organic EL element 20 and the filler 40 are not in direct contact with each other. Further, the plasma polymerization film 32 which is an intermediate layer of the passivation layer functions as a defect separation layer. That is, the plasma polymerized film 32 prevents pores from continuing between the first amorphous SiN film 31 and the second amorphous SiN film 33. Thereby, it is suppressed that the water | moisture from the outside reaches the organic EL element 20 through the pore which arises in a passivation layer.

The organic EL element 20 is disposed on the lower electrode 21 so as to be surrounded by the insulating separation film 60. Light emission occurs in the light emitting region where the lower electrode 21, the organic layer 22, and the upper electrode 23 are stacked. Therefore, a plurality of light emitting elements can be arranged on one lower substrate 10 by forming a plurality of organic EL elements 20 electrically insulated by the separation film 60. In order to supply power to the organic EL element 20, the lower electrode 21 extends to the outside of the resin film 70.

The organic layer 22 is electrically connected to the lower electrode 21 and the upper electrode 23. For example, the current flowing between the lower electrode 21 and the upper electrode 23 is controlled by a control circuit (not shown) arranged around the organic EL element 20 or in the lower substrate 10, so that each region of the organic layer 22 is controlled. Light emission is controlled.

For example, light is generated in the organic layer 22 by applying an electric field to the organic layer 22 using the lower electrode 21 in contact with the organic layer 22 as a metal cathode electrode and the upper electrode 23 as a transparent anode electrode. Specifically, holes are supplied from the upper electrode 23 to the organic layer 22, and electrons are supplied from the lower electrode 21 to the organic layer 22. Then, light generated by recombination of holes and electrons is emitted from the organic layer 22, passes through the upper electrode 23, the laminate 30, the filler 40 and the sealing material 50, and is output to the outside of the organic EL device 1. Light L is output.

Therefore, a light-transmitting material such as a glass plate is used for the sealing material 50, and a transparent filler is used for the filler 40. In addition, it can suppress that a water | moisture content reaches the organic EL element 20 from the exterior by using a hygroscopic material for the filler 40. FIG.

The upper electrode 23 which is a transparent electrode includes an indium tin oxide (ITO) film, an indium oxide / zinc oxide (IZO) film, a zinc oxide (ZnO) film, an aluminum (Al) -doped titanium oxide (TiO ₂ ) film, an oxide A tin (SnO ₂ ) film or the like can be used. For the lower electrode 21, an aluminum (Al) film, a magnesium (Mg) -Ag alloy film, or the like can be used.

The organic layer 22 can employ a structure in which a hole transport layer, an electron transport layer, or the like made of an organic compound or the like is laminated. For example, a diphenylnaphthyldiamine (NPD) film or the like can be used for the hole transport layer, and a quinolinol aluminum complex (Alq ₃ ) film or the like can be used for the electron transport layer. The organic layer 22 may have a structure including a light emitting layer disposed between the hole transport layer and the electron transport layer.

A glass substrate or the like can be used for the lower substrate 10. Polyimide or the like can be used for the separation membrane 60. Since the polyimide passes moisture, the separation membrane 60 is covered with the laminate 30. Further, a filler 40 that retains moisture is applied to the outside of the laminate 30.

As already described, when a SiN film is used as a passivation layer between the organic EL element 20 and the filler 40, there is a problem that moisture reaches the organic EL element 20 from the outside through pores generated in the SiN film. . Moreover, it is difficult for the organic polymer thin film that can be used as the defect separation layer to form a uniform film over a large area by the conventional vapor deposition method.

However, in the organic EL device 1 shown in FIG. 1, a plasma polymerization film 32 such as an amorphous SiOC film formed by surface wave excitation plasma chemical vapor deposition is provided in the middle of a passivation layer made of an amorphous SiN film. Are arranged as defect separation layers. According to the surface wave excitation plasma chemical vapor deposition method, it is easy to form a uniform film over a large area. For this reason, even if the organic EL device 1 has a large area, it is possible to easily prevent moisture from the outside from reaching the organic EL element 20 through the pores generated in the passivation layer.

The nitride film deposited by the plasma CVD method is basically amorphous. For manufacturing the organic EL device 1 shown in FIG. 1, for example, a surface wave excitation plasma CVD device 110 as shown in FIG. 3 can be used.

The surface wave excitation plasma CVD apparatus 110 includes a waveguide 112 into which a microwave 111 is introduced, a chamber 114 in which the substrate 100 is stored, a stage 115 on which the substrate 100 to be processed is mounted, and a substrate in the chamber 114. 100, a dielectric 116 disposed opposite to 100, a discharge gas introduction port 117 for introducing a discharge gas into the chamber 114, a film formation gas introduction port 118 for introducing a film formation gas into the chamber 114, and a chamber 114 And an exhaust port 119 for exhausting the gas.

Below, the case where the laminated body 30 of the organic EL apparatus 1 is manufactured using the surface wave excitation plasma CVD apparatus 110 shown in FIG. 3 is demonstrated. In addition, the film-forming process by the surface wave excitation plasma CVD apparatus 110 is performed as follows.

The microwave 111 output from a microwave power source (not shown) and introduced into the waveguide 112 reaches the dielectric 116 via the slot antenna 113 formed in the waveguide 112. In addition, the arrow described in FIG. 3 has shown the moving direction of the microwave.

On the other hand, a discharge gas such as argon (Ar) gas is introduced into the chamber 114 from the discharge gas introduction port 117. The argon plasma 120 is excited in the chamber 114 by the energy of the microwave 111 introduced into the chamber 114 via the dielectric 116. At this time, under the condition that the electron density in the plasma 120 is 7.45 × 10 ¹⁰ pieces / cm ⁻³ or more, the plasma 120 behaves like a metal, and the microwave 111 does not propagate in the plasma 120 and does not propagate. 116 extends laterally along 116. That is, when the electron density of the plasma 120 exceeds the critical density of surface wave generation, the microwave 111 becomes a surface wave and propagates along the boundary surface between the plasma 120 and the dielectric 116. This state is called “surface wave plasma mode”. The film forming process using the surface wave excitation plasma CVD apparatus 110 in the present embodiment is mainly performed under conditions of the surface wave plasma mode.

Hereinafter, a method for manufacturing the organic EL device 1 shown in FIG. 1 will be described. In addition, the manufacturing method of the organic EL device 1 described below is an example, and it is needless to say that it can be realized by various other manufacturing methods including this modification.

The organic EL element 20 is formed on the lower substrate 10 by a known method or the like. For example, the lower electrode film is formed on the lower substrate 10 by vapor deposition or the like. The lower electrode film is patterned by a lift-off method or an etching method using a photolithography technique to form a lower electrode 21 as shown in FIG.

Next, a separation film 60 having an opening as shown in FIG. 5 is formed on the lower substrate 10 and the lower electrode 21 using a vapor deposition mask.

Then, the organic layer 22 is formed on the lower electrode 21 so as to fill the opening of the separation membrane 60. Thereafter, an upper electrode film is formed on the organic layer 22. The upper electrode film is patterned into a desired pattern by an etching method using a photolithography technique or the like to form the upper electrode 23. Thus, as shown in FIG. 6, the organic EL element 20 is formed on the lower substrate 10.

Next, using the surface wave excitation plasma CVD apparatus 110 shown in FIG. 3, the laminate 30 shown in FIG. 2 is formed on the organic EL element 20 as follows. In the following, an amorphous SiOC film is formed as the plasma polymerization film 32.

In the formation of the first amorphous SiN film 31 and the second amorphous SiN film 33, Ar gas as a discharge gas is introduced into the chamber 114 from the discharge gas inlet 117, and silane gas and ammonia are used as the film forming gas. A gas is introduced into the chamber 114 from the deposition gas inlet 118. The film formation conditions are, for example, that the flow rate of silane gas is 70 sccm, the flow rate of ammonia gas is 500 sccm, the flow rate of argon gas is 350 sccm, and the pressure in the chamber 114 during film formation is 10 Pa.

In forming the amorphous SiOC film, vaporized hexamethyldisiloxane and oxygen (O ₂ ) gas are introduced into the chamber 114 from the film forming gas inlet 118. As the film forming conditions, for example, the flow rate of hexamethyldisiloxane is 200 sccm, the flow rate of O ₂ gas is 400 sccm, and the pressure in the chamber 114 during film formation is 5 Pa.

In any film formation, the distance between the plasma and the substrate is 200 mm, and the microwave power density is 1.57 W / cm ² . When there is no stage cooling under these conditions, the substrate surface temperature rises to 80 ° C. and stabilizes.

In the film forming process by the surface wave excitation plasma CVD apparatus 110, the temperature of the stacked body 30 during film formation is maintained at a temperature lower than the glass transition temperature of the organic layer 22. For example, the film forming temperature is set to 120 ° C. or lower.

Further, in the film forming process by the surface wave excitation plasma CVD apparatus 110, the distance between the substrate 100 and the dielectric 116 is preferably about 150 mm to 250 mm. When the distance between the substrate 100 and the dielectric 116 is constant, the barrier property of the formed SiN film is improved. The inventors have confirmed that the above effect can be obtained when the distance between the substrate 100 and the dielectric 116 is 150 mm to 250 mm.

Note that, in order to make the film thickness distribution of each film constituting the stacked body 30 uniform, the lower substrate 10 on which the organic EL element 20 is formed is reciprocated below the dielectric 116 while being reciprocated on the organic EL element 20. The stacked body 30 may be formed. The film thicknesses of the first amorphous SiN film 31, the plasma polymerized film 32, and the second amorphous SiN film 33 are formed by a moving film forming method in which the lower substrate 10 is reciprocated in parallel with the main surface, which is the film forming surface. The distribution can be made uniform.

As shown in FIG. 7, after patterning the laminated body 30, the filler 40 is formed on the laminated body 30. Then, by bonding the lower substrate 10 and the sealing material 50 with the resin film 70, the organic EL device 1 shown in FIG. 1 is completed.

By forming the laminate 30 using the surface wave excitation plasma CVD method as described above, the first amorphous SiN film 31, the plasma polymerization film 32, and the second amorphous SiN film 33 are formed on the same surface. It can be formed continuously using the wave excitation plasma CVD apparatus 110. Thereby, increase in the manufacturing time of the organic EL device 1 can be suppressed.

The following samples S1 to S5 having different structures of the laminate 30 are manufactured by the film forming method using the surface wave excitation plasma CVD apparatus 110 described above, and the samples S1 to S5 are placed in a constant temperature and humidity chamber of 85 ° C. and 85% RH. An acceleration test for storing sample S5 was performed. Samples S1 to S5 have a structure in which the filler 40 is formed on the laminate 30 formed on the organic EL element 20, and the outer periphery of the glass plate of the sealing material 50 is adhered and sealed with resin. The structure of the laminate 30 of Samples S1 to S5 is as follows:
Sample S1: SiN film with a thickness of 200 nm Sample S2: SiN film with a thickness of 400 nm Sample S3: SiN film with a thickness of 1 μm Sample S4: SiN film with a thickness of 100 nm / SiOC film with a thickness of 3 μm / SiN film with a thickness of 100 nm Sample S5: SiN film with a thickness of 200 nm / SiOC film with a thickness of 3 μm / SiN film with a thickness of 200 nm That is, samples S1 to S3 have a single layer of SiN film, and samples S4 to S5 have hexamethyldisiloxane. And a laminate 30 having a three-layer structure in which an SiOC film as a raw material is an intermediate layer. The total film thickness of the SiN film is the same between sample S1 and sample S4. Further, the total film thickness of the SiN film is the same between the sample S2 and the sample S5.

Using the surface wave excitation plasma CVD apparatus 110 shown in FIG. 3, in the case of samples S1 to S3, SiN films are formed in various film thicknesses, and in the case of samples S4 to S5, SiN films, SiOC films, SiN films are formed. Were sequentially formed to form a laminate 30.

FIG. 8 shows the result of the acceleration test performed on samples S1 to S5. In the acceleration test, the ratio of lighting elements that maintain lighting even after a certain period of time was investigated.

In Sample S1 to Sample S2 in which the laminated body 30 is a single layer of SiN film and the SiN film is relatively thin, the number of lighting elements became zero around 400 hours. In the sample S3 with a thick SiN film, the number of lighting elements after 600 hours is about 40%.

On the other hand, when the laminate 30 having a three-layer structure having an intermediate layer made of a SiOC film is employed, the number of lighting elements in the sample S4 is maintained even after 600 hours as in the sample S3. Since the total film thickness of the SiN film in sample S4 is 200 nm, which is the same as that in sample S1, it was confirmed that the effect of defect separation by the intermediate layer appeared. In the sample S5 in which the total film thickness of the SiN film is 400 nm, which is the same as the sample S2, the ratio of the lighting elements is higher than that in the sample S4.

In addition, the refractive index of the plasma polymerization film 32 formed by this embodiment is about 1.5, and the light transmittance is high. For this reason, the organic EL device 1 can sufficiently cope with a top emission method of outputting light from the sealing material 50 side to the outside.

As described above, according to the method for manufacturing the organic EL device 1 according to the embodiment of the present invention, the stacked body 30 including the amorphous SiN film and the plasma polymerization film is formed by the surface wave excitation plasma chemical vapor deposition method. It is formed on the organic EL element 20. As a result, it is possible to provide the organic EL device 1 that can suppress deterioration in quality due to moisture permeation into the interior.

Further, by forming the intermediate layer of the passivation layer made of the SiN film as a plasma polymerized film whose growth rate is about 20 times faster than that of the SiN film, an increase in manufacturing time can be suppressed as compared to manufacturing the SiN film thicker.

(Other embodiments)
As mentioned above, although this invention was described by embodiment, it should not be understood that the description and drawing which form a part of this indication limit this invention. From this disclosure, various alternative embodiments, examples and operational techniques will be apparent to those skilled in the art.

In the above description, the case where the laminated body 30 having the SiOC film is formed as the plasma polymerization film 32 has been described. However, a plasma polymerization film other than the SiOC film may be used as an intermediate layer of the passivation layer. Alternatively, the bottom substrate 10 may be a transparent substrate, and the lower electrode 21 may be a transparent electrode, so that the organic EL device 1 may employ a bottom emission method that emits light from the lower substrate 10 side.

Thus, it goes without saying that the present invention includes various embodiments that are not described herein. Therefore, the technical scope of the present invention is defined only by the invention specifying matters according to the scope of claims reasonable from the above description.

The present invention can be used for the purpose of suppressing moisture permeation through the passivation film.

Claims (15)

Fabrication of an organic electroluminescent device comprising a laminate including an amorphous silicon nitride film and a plasma polymerized film formed on an organic EL element including an organic layer by surface wave excitation plasma chemical vapor deposition Method. Forming the laminate comprises:
Forming the first amorphous silicon nitride film on the organic EL element;
Forming the plasma polymerized film on the first amorphous silicon nitride film;
The method of manufacturing an organic electroluminescence device according to claim 1, further comprising: forming a second amorphous silicon nitride film on the plasma polymerization film. Forming the amorphous silicon nitride film at a temperature lower than the glass transition temperature of the organic layer using a silane gas and an ammonia gas as a deposition gas;
The plasma polymerized film is an amorphous silicon oxycarbide film, and the amorphous silicon oxycarbide film is formed at a temperature lower than the glass transition temperature of the organic layer using hexamethyldisiloxane gas and oxygen gas as a film forming gas. The method for producing an organic electroluminescent device according to claim 1, wherein: Forming a filler on the laminate;
Forming a sealing material on the filler;
Forming a resin film between the lower substrate on which the organic EL element is disposed and the sealing material so as to surround the organic EL element, the laminate, and the filler. The manufacturing method of the organic electroluminescent apparatus of Claim 1. The method of manufacturing an organic electroluminescence device according to claim 4, wherein the stacked body is formed on the organic EL element while the lower substrate is reciprocated in parallel with the main surface of the lower substrate. The distance between the dielectric in the surface wave excited plasma chemical vapor deposition apparatus used for the surface wave excited plasma chemical vapor deposition method and the amorphous silicon nitride film being formed is 150 mm to 250 mm. Item 2. A method for producing an organic electroluminescent device according to Item 1. A film forming method using a surface wave excitation plasma chemical vapor deposition apparatus,
Forming an amorphous silicon nitride film on a substrate using a silane gas and an ammonia gas as a deposition gas at a deposition temperature of 200 ° C. or less;
Forming an amorphous silicon oxycarbide film on the amorphous silicon nitride film using a hexamethyldisiloxane gas and an oxygen gas as a film forming gas at a film forming temperature of 200 ° C. or lower. A film forming method. Forming a first amorphous silicon nitride film;
Forming the plasma polymerized film on the first amorphous silicon nitride film;
Forming a second amorphous silicon nitride film on the plasma polymerized film. The film forming method according to claim 7, further comprising a step of forming a filler on the laminated body including the amorphous silicon nitride film and the amorphous silicon oxycarbide film. 8. The film forming method according to claim 7, wherein the amorphous silicon nitride film and the amorphous silicon nitride film are formed while reciprocating the substrate in parallel with the main surface of the substrate. The film forming method according to claim 7, wherein a distance between the dielectric in the surface wave excitation plasma chemical vapor deposition apparatus and the amorphous silicon nitride film being formed is 150 mm to 250 mm. A lower substrate,
An organic EL element including an organic layer and disposed on the lower substrate;
A laminate including an amorphous silicon nitride film and a plasma polymerized film disposed on the organic EL element;
An organic electroluminescence device, wherein the laminate is formed by surface wave excitation plasma chemical vapor deposition. The laminate is
A first amorphous silicon nitride film disposed on the organic EL element;
The plasma polymerized film disposed on the first amorphous silicon nitride film;
The organic electroluminescence device according to claim 12, further comprising: a second amorphous silicon nitride film disposed on the plasma polymerization film. The organic electroluminescent device according to claim 12, wherein the plasma polymerized film is an amorphous silicon oxycarbide film. A filler disposed on the laminate;
A sealing material disposed on the filler;
The organic material according to claim 12, further comprising: a resin film disposed between the lower substrate and the sealing material so as to surround the organic EL element, the stacked body, and the filler. Electroluminescence device.

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