WO2017033823A1

WO2017033823A1 - Electronic device

Info

Publication number: WO2017033823A1
Application number: PCT/JP2016/074081
Authority: WO
Inventors: 勇也元村; 史和佐藤; 亜矢中山
Original assignee: 富士フイルム株式会社
Priority date: 2015-08-21
Filing date: 2016-08-18
Publication date: 2017-03-02
Also published as: JP2017041412A

Abstract

The present invention address the problem of providing an electronic device formed by sealing an electronic element such as an organic electro-luminescence element, the electronic device being capable of preventing deterioration of the electronic element due to moisture and the like over a long period of time. The problem is solved by including: an element substrate; an electronic element formed in the element substrate; a sealing substrate which seals the electronic element; a sealing member provided between the element substrate and the sealing substrate, in order to seal the electronic element by the sealing substrate; and a patterned interface adhesion layer disposed between the element substrate and the sealing member and/or between the sealing substrate and the sealing member.

Description

Electronic equipment

The present invention relates to an electronic device such as an organic electroluminescence device.

Electronic devices such as organic EL devices (organic electroluminescence devices) are often vulnerable to moisture. Therefore, for example, in an organic electroluminescence device (organic EL device) using an organic EL element, it has been proposed to seal the organic EL element with a sealing member having gas barrier properties.

For example, Patent Document 1 uses a gas barrier film having a base material, an intermediate layer formed on the base material, and a gas barrier layer obtained by subjecting a layer having polysilazane formed on the intermediate layer to vacuum ultraviolet irradiation. An organic EL device (organic EL panel) for sealing an organic EL element is described.
Specifically, in Patent Document 1, an organic EL element is formed on a gas barrier layer of a gas barrier film, the organic EL element is covered, and an aluminum foil / PET (polyethylene terephthalate) film composite seal is provided via an adhesive layer. There is described an organic EL device in which an organic EL element is sandwiched between a gas barrier film and an aluminum foil / PET film composite sealing member by covering a side surface and sealed by sticking a stop member.

Patent Document 2 discloses a base layer, a smooth layer formed by applying a coating solution containing a (meth) acrylate having a phosphate ester group and a polyfunctional (meth) acrylate, and a coating solution containing polysilazane. An organic EL device (organic EL panel) that seals an organic EL element by using a gas barrier film obtained by laminating a coating film that has been coated and dried with a gas barrier layer that has been subjected to a modification treatment that irradiates vacuum ultraviolet light. ) Is described.
Specifically, in Patent Document 2, a transparent electrode is formed on a gas barrier film, an organic EL element is formed on the transparent electrode, and an opposing film is attached via an adhesive layer, thereby organic An organic EL device in which an EL element is sealed is described. Moreover, in patent document 2, metal films, such as a gas barrier film which has the above-mentioned base material, a smooth layer, and a gas barrier layer, and aluminum foil, are illustrated as a counter film.

International Publication No. 2013/075255 JP 2014-76590 A

As shown in Patent Documents 1 and 2, the organic EL element in the organic EL device is sealed by covering the entire surface of the organic EL element with an adhesive layer, and covering the entire surface of the adhesive layer with a gas barrier film or the like. The organic EL element is sealed by sticking the sealing substrate.
However, with such a sealing method, deterioration of the organic EL element due to moisture or the like may not be sufficiently prevented.

According to the study by the present inventors, one reason is that the organic EL element deteriorates due to moisture entering from the end face of the adhesive layer.

In terms of preventing moisture from entering from the end face of the adhesive layer, the thinner the adhesive layer, the better.
On the other hand, when the adhesive is thinned, the elasticity of the adhesive layer is lowered. Therefore, the thinner the adhesive layer, the lower the adhesion between the organic EL element and the element substrate to be formed and the adhesive layer and / or the adhesion between the adhesive layer and the sealing substrate.
As a result, in applications that require flexibility, the adhesive layer and the sealing substrate are peeled off and moisture enters, the interface between the element substrate and the adhesive layer and / or the adhesive layer and the sealing. Problems such as deterioration of the organic EL element occur due to moisture entering from the interface with the substrate.

An object of the present invention is to solve such problems of the prior art. In an electronic device in which an electronic element such as an organic EL element is sealed with a sealing substrate such as a gas barrier film, flexibility is required. It is an object of the present invention to provide an electronic device that can seal an electronic element with a high adhesive force even when used for a long period of time, and prevent moisture from entering from an interface, thereby preventing deterioration of the electronic element due to moisture over a long period of time.

In order to achieve this object, an electronic device of the present invention includes an element substrate,
An electronic element formed on the element substrate;
A sealing substrate for sealing the electronic element;
A sealing member provided between the element substrate and the sealing substrate for sealing the electronic element with the sealing substrate;
There is provided an electronic device having a patterned interface adhesion layer provided between at least one of an element substrate and a sealing member and between a sealing substrate and a sealing member.

In such an electronic device of the present invention, the interfacial adhesion layer is patterned so that it is not positioned closer to the electronic element side than the intermediate position between the end of the sealing member and the electronic element in the surface direction of the element substrate. Is preferred.
Moreover, it is preferable that at least one of the contact part between the element substrate and the sealing member by the interface adhesion layer and the adhesion part between the sealing substrate and the sealing member by the interface adhesion layer is not more than the area of the sealing member. .
The ratio between the thickness t ₁ of the thickness t ₀ and the sealing member of the interface adhesion layer, t ₁ / t is preferably ₀ ≧ 100.
The water vapor permeability of the sealing member is preferably 50 g / (m ² · day) or less per 100 μm thickness at a temperature of 40 ° C. and a relative humidity of 90% RH.
Moreover, it is preferable that an interface contact | attachment layer contains 10 mass% or more of silicon atoms.
Moreover, it is preferable that at least one of the element substrate and the sealing substrate includes a support and one or more combinations of an inorganic layer provided on one surface of the support and an organic layer that forms the inorganic layer formation surface. .
Moreover, it is preferable that a sealing member is a sheet form which covers the whole surface of an electronic element.
Furthermore, it is preferable that the sealing member is a frame surrounding the electronic element in the surface direction of the element substrate.

According to such an electronic device of the present invention, the electronic element can be sealed with high adhesion even in applications requiring flexibility, and from between the sealing substrate and the sealing member. It is possible to obtain an electronic device that can prevent moisture from entering and prevent deterioration of the electronic element due to moisture over a long period of time.

FIG. 1A is a schematic cross-sectional view of an example in which the electronic device of the present invention is used in an organic electroluminescence device. FIG. 1B is a schematic plan view of the organic electroluminescence device shown in FIG. 1A. FIG. 2 is a view conceptually showing an example of a barrier film used in the electronic device of the present invention. FIG. 3A is a schematic cross-sectional view of another example in which the electronic device of the present invention is used in an organic electroluminescence device. FIG. 3B is a schematic plan view of the organic electroluminescence device shown in FIG. 3A.

Hereinafter, the electronic device of the present invention will be described in detail based on a preferred example shown in the accompanying drawings.
In the present specification, a numerical range expressed using “to” means a range including numerical values described before and after “to” as a lower limit value and an upper limit value.
In this specification, “(meth) acrylate” is used in the meaning of at least one of acrylate and methacrylate, or any one of them. The same applies to “(meth) acryloyl”.

FIG. 1A and FIG. 1B conceptually show an example in which the electronic device of the present invention is used in an organic electroluminescence device. In the following description, organic electroluminescence is also referred to as organic EL.

In addition, although the example shown in FIG. 1 is an example which utilized the electronic device of this invention for organic EL apparatuses, such as an organic EL display and organic EL illumination, this invention was formed in the element substrate besides this. The present invention can be used for various electronic devices in which electronic elements are sealed with a sealing substrate.
As an example, the electronic device of the present invention is suitably used for various electronic devices using various electronic elements such as photoelectric conversion devices such as organic solar cells, displays such as organic transistors and liquid crystal displays, electronic paper, and thermoelectric conversion devices. Is possible.

The organic EL device 10 shown in FIG. 1 basically includes an element substrate 12, an organic EL element 14, a sealing substrate 16, a sealing member 18, and an interface adhesion layer 20.
In the organic EL device 10, an organic EL element 14 is formed on one surface of an element substrate 12, and the organic EL element 14 is sealed with a sealing substrate 16 via a sealing member 18.
Here, in the organic EL device 10 of the present invention, an interface adhesion layer 20 is provided between the element substrate 12 and the sealing member 18. In addition, an interface adhesion layer 20 is provided between the sealing member 18 and the sealing substrate 16. In the present invention, the interfacial adhesion layer 20 is provided not by providing a uniform film (so-called solid film) over the entire surface of the element substrate 12 or the entire surface of the sealing substrate 16 but by patterning. It is done. This will be described in detail later.

1A is a schematic cross-sectional view of the organic EL device 10 of the present invention, and FIG. 1B is a schematic plan view (top view) of the organic EL device 10. In FIG. 1B, in order to clearly show the configuration, the sealing substrate 16 is omitted, the interface adhesion layer 20 is hatched, and the organic EL element 14 is shown by a solid line.
1A is a cross-sectional view taken along the line aa of FIG. 1B, and the plan view of FIG. 1B is a view of the organic EL device 10 as viewed from above FIG. 1A. That is, FIG. 1B is a view of the organic EL device 10 as viewed from a direction orthogonal to the substrate surface of the element substrate 12.
In FIG. 1A, hatching is omitted for the sake of brevity.

As the element substrate 12, various known sheet-like materials and film-like materials used as a substrate for forming various organic EL elements such as an organic EL display and organic EL lighting can be used.
As an example of the element substrate 12, polyethylene terephthalate (PET), polyethylene naphthalate (PEN), polyethylene (PE), polypropylene (PP), polystyrene, polyamide, polyvinyl chloride, polycarbonate, polyacrylonitrile, polyimide, polyacrylate, Films and sheets made of various resin materials (polymer materials) such as polymethacrylate, polycarbonate (PC), cycloolefin polymer (COP), cycloolefin copolymer (COC), triacetylcellulose (TAC), transparent polyimide, etc. Examples include a shape, a glass plate, a thin glass, and a metal plate.

As the element substrate 12, a gas barrier film formed by forming a gas barrier layer on a support, which is used for a sealing substrate 16 described later, can also be suitably used.
Among them, as a gas barrier layer, an organic / inorganic laminate type gas barrier film in which one or more combinations of an inorganic layer that exhibits gas barrier properties and an organic layer serving as a base layer of the inorganic layer are formed on the support, It is preferably used. In the present invention, a gas barrier film in which the gas barrier layer has only an inorganic layer exhibiting gas barrier properties, instead of the organic-inorganic laminated type, can also be suitably used.
By using a gas barrier film, in particular, an organic / inorganic laminated type gas barrier film as the element substrate 12, it is possible to prevent moisture from entering from the element substrate 12 side and obtain a longer-life organic EL device 10.
When the gas barrier film is used as the element substrate 12, the formation surface of the organic EL element 14 may be on the gas barrier layer side or the support side, but in terms of suitably preventing moisture from entering the organic EL element 14. The organic EL element 14 is preferably formed on the gas barrier layer side.

The thickness of the element substrate 12 may be appropriately set according to the type and size of the organic EL device 10.
Here, it is preferable that the thickness of the element substrate 12 is set to a thickness that can provide necessary flexibility in accordance with a forming material or the like in that the organic EL device 10 having flexibility can be realized.

The organic EL element 14 formed on such an element substrate 12 includes a transparent electrode layer (TFT (thin film transistor)), a hole injection layer, a hole transport layer, a light emitting layer, a hole blocking layer, an electron transport layer, an electron injection layer, It is a well-known organic EL element (organic EL device) that constitutes an organic EL device (OLED (Organic Light Emitting Diode)) such as an organic EL display or organic EL illumination having a cathode or the like.

As described above, the electronic device of the present invention can be various electronic devices other than the organic EL device.
Therefore, what is formed on the element substrate 12 is not only an organic EL element, but also a variety of known electrons such as a photoelectric conversion element such as a solar cell element, an organic semiconductor element such as an organic transistor, a thermoelectric conversion element, and an electronic paper element. The device is available.

Such an organic EL element 14 is sealed by a sealing substrate 16. In addition, a sealing member 18 for sealing the organic EL element 14 by the sealing substrate 16 is provided between the element substrate 12 and the sealing substrate 16.

The sealing substrate 16 is for preventing the organic EL element 14 from being deteriorated by moisture or the like by covering and sealing the organic EL element 14 from the side opposite to the element substrate 12.
The sealing substrate 16 is a known sheet used for sealing an organic EL element in an organic EL device as long as it has necessary gas barrier properties and satisfies required characteristics such as required transparency. Various shapes (plate-like / film-like) can be used.
The sealing substrate 16 preferably has a water vapor transmission rate of 1 × 10 ⁻² g / (m ² · day) or less, more preferably a water vapor transmission rate of 1 × 10 ⁻³ g / (m ² · day) or less. The sheet-like material is used.

As such a sealing substrate 16, what was illustrated by the above-mentioned element substrate 12, for example can be utilized variously. Of these, glass plates and thin glass are preferably used in terms of high gas barrier properties and high transparency.
Moreover, as the sealing substrate 16, a gas barrier film in which a gas barrier layer that exhibits gas barrier properties is formed on the resin film as exemplified in the element substrate 12 is also preferably exemplified. Among them, an organic / inorganic laminate type gas barrier film in which one or more combinations of an inorganic layer exhibiting gas barrier properties and an organic layer serving as a formation surface of the inorganic layer are formed on the support is particularly preferable. Used for
In the present invention, a gas barrier film in which the gas barrier layer has only an inorganic layer exhibiting gas barrier properties, instead of the organic-inorganic laminated type, can also be suitably used. In this case, as the inorganic layer, those similar to the inorganic layer 36 of the gas barrier film 30 described later are preferably exemplified. This also applies to the case where a gas barrier film having only an inorganic layer as the gas barrier layer is used for the element substrate 12 described above.

FIG. 2 conceptually shows an example of such an organic-inorganic laminated gas barrier film.
The gas barrier film 30 shown in FIG. 2 is obtained by laminating an organic layer 34 and an inorganic layer 36 on a support 32 in this order.

The gas barrier film 30 shown in FIG. 2 has one combination of the organic layer 34 and the inorganic layer 36 serving as a base, but has two combinations of the organic layer 34 and the inorganic layer 36. Or it may have three or more sets.
The greater the number of combinations of the organic layer 34 and the inorganic layer 36, the higher the gas barrier property. On the other hand, the greater the number of combinations of the organic layer 34 and the inorganic layer 36, the thicker the barrier film and the lower the transparency and flexibility. Therefore, the number of combinations of the organic layer 34 and the inorganic layer 36 may be appropriately set according to required gas barrier properties, flexibility, optical characteristics, and the like.

Moreover, the organic-inorganic laminated gas barrier film may have an organic layer that acts as a protective layer for the inorganic layer 36 as the uppermost layer, if necessary. The uppermost layer is a layer on the surface opposite to the support 32.
However, in view of preventing deterioration of the organic EL element 14 due to moisture entering from the end face of the uppermost organic layer, the uppermost layer is the inorganic layer 36, and the inorganic layer 36 is the organic EL element 14 side, that is, a sealing described later. The member 18 side is preferable. For the same reason, when an organic / inorganic laminated gas barrier film is used for the element substrate 12, it is preferable to form the organic EL element 14 on the surface of the inorganic layer 36 with the uppermost layer being the inorganic layer 36.

In the gas barrier film 30, the support 32 is preferably a film or sheet made of various resin materials exemplified for the element substrate 12 described above.

The thickness of the support 32 may be appropriately set according to the use of the organic EL device 10 or the like. Specifically, the thickness of the support 32 is preferably 20 to 500 μm.

On one surface of the support 32, an organic layer 34 and an inorganic layer 36 constituting a barrier layer are formed.
The organic layer 34 is a layer made of an organic substance, and is obtained by crosslinking (polymerizing) a polymerizable compound that becomes the organic layer 34.
The organic layer 34 functions as a base layer for properly forming the inorganic layer 36 that exhibits gas barrier properties. By having such a base organic layer 34, the surface on which the inorganic layer 36 is formed can be flattened and made uniform, and a state suitable for the formation of the inorganic layer 36 can be achieved. The gas barrier film 30 having an organic-inorganic laminated structure in which the underlying organic layer 34 and the inorganic layer 36 are laminated, thereby making it possible to form a proper inorganic layer 36 on the entire surface without any gaps. Expresses gas barrier properties.

Various known organic materials can be used as the material for forming the organic layer 34.
Specific examples of the material for forming the organic layer 34 include polyester, acrylic resin, methacrylic resin, methacrylic acid-maleic acid copolymer, polystyrene, transparent fluororesin, polyimide, fluorinated polyimide, polyamide, polyamideimide, and polyether. Imido, cellulose acylate, polyurethane, polyether ether ketone, polycarbonate, alicyclic polyolefin, polyarylate, polyether sulfone, polysulfone, fluorene ring modified polycarbonate, alicyclic ring modified polycarbonate, fluorene ring modified polyester, (meth) acryloyl compound, etc. The thermoplastic resin is preferably exemplified. Moreover, as a forming material of the organic layer 34, polysiloxane and other organosilicon compounds are also preferably exemplified. A plurality of these forming materials may be used in combination.

Among these, the organic layer 34 composed of a polymer of a radical polymerizable compound and / or a cationic polymerizable compound having an ether group as a functional group is preferable in terms of excellent glass transition temperature and strength.

In particular, acrylic resin or methacrylic resin having a glass transition temperature of 120 ° C. or higher, mainly composed of an acrylate and / or methacrylate monomer or oligomer polymer in terms of strength, transparency and excellent optical properties. The resin is preferably exemplified as the organic layer 34.
Among them, dipropylene glycol di (meth) acrylate (DPGDA), 1,9-nonanediol di (meth) acrylate (A-NOD-N), 1,6 hexanediol diacrylate (A-HD-N), Bifunctional or higher acrylate and / or methacrylate monomers such as trimethylolpropane tri (meth) acrylate (TMPTA), (modified) bisphenol A di (meth) acrylate, dipentaerythritol hexa (meth) acrylate (DPHA), etc. An acrylic resin and a methacrylic resin mainly composed of a polymer are preferably exemplified. It is also preferable to use a plurality of these acrylic resins and methacrylic resins.

By forming the organic layer 34 with an acrylic resin or a methacrylic resin, particularly an acrylic resin or a methacrylic resin having a bifunctional or higher functionality, the inorganic layer 36 can be formed on a base having a solid skeleton, so that the denser and higher gas barrier property is achieved. The inorganic layer 36 can be formed.

The thickness of the organic layer 34 may be set as appropriate according to the thickness of the target gas barrier film 30, the number of combinations of the underlying organic layer 34 and the inorganic layer 36, the type of the inorganic layer 36, and the like.
Specifically, the thickness of the organic layer 34, particularly the thickness of the organic layer 34 formed on the surface of the support 32 is preferably 0.1 μm or more, and more preferably 0.5 μm or more. By setting the thickness of the organic layer 34 to 0.1 μm or more, the unevenness on the surface of the support 32 is suitably filled, and the organic layer 34 having high surface flatness can be obtained. Moreover, since the organic layer 34 acts as a suitable stress buffer layer by setting the thickness of the organic layer 34 to 0.1 μm or more, the inorganic layer 36 can be prevented from cracking when the organic EL device 10 is bent. .
Further, the thickness of the organic layer 34 is preferably 3 μm or less, and more preferably 1.5 μm or less. By setting the thickness of the organic layer 34 to 3 μm or less, it is possible to suitably prevent deterioration of the organic EL element 14 due to moisture release from the organic layer 34.

The organic layer 34 may be formed by a known method corresponding to the material for forming the organic layer 34.
Generally, the organic layer 34 is a coating composition (paint) containing an organic solvent, a polymerizable compound (monomer, dimer, trimer, oligomer, polymer, etc.) that becomes the organic layer 34, a surfactant, a silane coupling agent, and the like. The coating solution is applied, dried, and then polymerized (crosslinked) by a UV irradiation or the like as necessary. In addition, by using a coating method, the organic layer 34 having a very high surface flatness can be formed by a so-called leveling effect.

The inorganic layer 36 is formed using such an organic layer 34 as a base layer. The inorganic layer 36 mainly exhibits gas barrier properties in the gas barrier film 30.
As the material for forming the inorganic layer 36, various materials made of an inorganic material exhibiting gas barrier properties can be used.
Specifically, metal oxides such as aluminum oxide, magnesium oxide, tantalum oxide, zirconium oxide, titanium oxide, and indium tin oxide (ITO); metal nitrides such as aluminum nitride; metal carbides such as aluminum carbide; silicon oxide, Silicon oxides such as silicon oxynitride, silicon oxycarbide and silicon oxynitride carbide; silicon nitrides such as silicon nitride and silicon nitride carbide; silicon carbides such as silicon carbide; hydrides thereof; mixtures of two or more of these; and Inorganic compounds such as these hydrogen-containing materials are preferably exemplified.
In particular, silicon nitride, silicon oxide, silicon oxynitride, and aluminum oxide are preferably used because they are highly transparent and can exhibit excellent gas barrier properties. Among these, silicon nitride is particularly suitable because it has high transparency in addition to excellent gas barrier properties.

The thickness of the inorganic layer 36 may be appropriately set according to the required gas barrier properties, the thickness of the target gas barrier film 30, the number of combinations of the underlying organic layer 34 and the inorganic layer 36, and the like.
Specifically, the thickness of the inorganic layer 36 is preferably 10 nm or more, and more preferably 15 nm or more. By setting the thickness of the inorganic layer 36 to 10 nm or more, good gas barrier properties can be obtained.
In addition, the thickness of the inorganic layer 36 is preferably 300 nm or less, and more preferably 150 nm or less. By setting the thickness of the inorganic layer 36 to 300 nm or less, cracking of the inorganic layer 36 when the organic EL device 10 is bent can be prevented.

The inorganic layer 36 may be formed by a known method depending on the material for forming the inorganic layer 36.
In general, the inorganic layer 36 is formed by a vapor deposition method (vapor deposition method) such as plasma CVD (Chemical Vapor Deposition), sputtering, or vacuum deposition.

The thickness of the sealing substrate 16 may be appropriately set according to the type and size of the organic EL device 10 and the gas barrier properties required for the sealing substrate 16.
Here, the thickness of the sealing substrate 16 is preferably set to a thickness that can provide the necessary flexibility according to the forming material and the like in that the organic EL device 10 having flexibility can be realized. .

A sealing member 18 is provided between the element substrate 12 and the sealing substrate 16. The sealing member 18 is for sealing the organic EL element 14 with the sealing substrate 16. In the illustrated example, the sealing member 18 has the same rectangular planar shape as the sealing substrate 16 including the size.
In the illustrated organic EL device 10, the sealing member 18 entirely covers the organic EL element 14, and the sealing substrate 16 is provided on the entire surface of the sealing member 18. The organic EL element 14 is sealed.

As the sealing member 18, as long as it has sufficient transparency, in the organic EL device in which the organic EL element is sealed with a sealing substrate such as a gas barrier film, the organic EL element is sealed with the sealing substrate. Various publicly known ones used for the purpose can be used.
Examples include (meth) acrylic acid ester resins, polyurethanes, (meth) acrylic resins, ethylene-vinyl acetate copolymers (EVA), polyolefins, silicone resins, epoxy resins, rubber-based materials, adhesive sheets, Examples thereof include an adhesive tape, an adhesive film, an adhesive, and a sealant.
A commercially available product can also be used as the sealing member 18. A commercially available product that can be used as the sealing member 18 is preferably a so-called OCA (Optical Clear Adhesive). As an example, teas Barrier Transfer Tape 3rdG manufactured by TESA Tape, CELVENUS series manufactured by Daicel, and various highly transparent adhesive transfer tape series manufactured by 3M are exemplified.

The sealing member 18 preferably has a high gas barrier property. Specifically, the sealing member 18 preferably has a water vapor transmission rate per 100 μm of 50 g / (m ² · day) or less in an environment of a temperature of 40 ° C. and a relative humidity of 90% RH, and 25 g / ( m ² · day) or less is more preferable.
By setting the gas barrier property of the sealing member 18 to 50 g / (m ² · day) or less, the deterioration of the organic EL element 14 due to moisture can be more suitably prevented.

In the embodiment shown in FIG. 1A and the like in which the sealing member 18 covers the organic EL element 14 in its entirety, the thickness of the sealing member 18 is sufficient depending on the forming material of the sealing member 18 and the like. ) May be set as appropriate so that the element substrate 12 and the sealing substrate 16 can be attached to each other.
In order to prevent deterioration of the organic EL element 14 due to moisture, the sealing member 18 is preferably thin in order to reduce moisture intrusion from the end face of the sealing member 18.
On the other hand, the thicker sealing member 18 is advantageous in terms of adhesion. Here, in this invention, since it has the interface contact | adherence layer 20 mentioned later, even if the sealing member is thin, sufficient adhesive force can be obtained.
Considering this point, the thickness of the sealing member 18 is preferably 0.5 to 100 μm, and more preferably 1 to 50 μm.
By setting the thickness of the sealing member 18 within this range, the element substrate 12 is sealed with sufficient adhesion by the interaction with the interface adhesion layer 20 described later while preventing the deterioration of the organic EL element due to moisture. The substrate 16 can be in close contact.

In addition, the thickness of the sealing member 18 is, in other words, the size of the sealing member 18 in the direction orthogonal to the substrate surface of the element substrate 12. Further, the end surface of the sealing member 18 is an end surface in the substrate surface direction of the element substrate 12 that is not the main surface (maximum surface).

In the embodiment shown in FIG. 1A and the like in which the sealing member 18 covers the organic EL element 14 in its entirety, the sealing member 18 preferably has an elastic modulus of 0.1 to 520 N / mm ² , and is preferably 0.2 to 480 N. / Mm ² is more preferable.
By setting the elastic modulus of the sealing member 18 to 0.1 N / mm ² or more, the sealing member 18 having good gas barrier properties can be formed. In addition, when a force is applied in a direction in which the sealing substrate 16 is peeled off, if the elastic modulus of the sealing member 18 is low, the sealing member 18 is stretched and broken, and the sealing is broken. Such inconvenience can be prevented by setting the elastic modulus of the member to 0.1 N / mm ² or more.
By setting the elastic modulus of the sealing member 18 to 520 N / mm ² or less, it is preferable in that the organic EL device 10 having good flexibility can be obtained.

In the organic EL device 10, an interface adhesion layer 20 is formed between the element substrate 12 and the sealing member 18 and between the sealing member 18 and the sealing substrate 16.

In the illustrated organic EL device 10, the interface adhesion layer 20 is provided both between the element substrate 12 and the sealing member 18 and between the sealing member 18 and the sealing substrate 16.
However, as in the example shown in FIG. 3A and the like described later, when the adhesion is sufficient, the interface adhesion layer 20 is interposed between the element substrate 12 and the sealing member 18 and between the sealing member 18 and the sealing member 18. The structure provided only in one side between the stop board | substrates 16 may be sufficient.

Here, in the present invention, the interfacial adhesion layer 20 is formed not by a solid pattern corresponding to the entire surface of the element substrate 12 or the sealing substrate 16 but by patterning. As shown in FIGS. 1A and 1B, in the organic EL device 10, the interfacial adhesion layer 20 has a rectangular frame shape according to the peripheral end portions of the rectangular sealing substrate 16 and the sealing member 18. Patterned.
The organic EL device 10 of the present invention has the interface adhesion layer 20 thus patterned between the element substrate 12 and the sealing member 18 and / or between the sealing member 18 and the sealing substrate 16. As a result, sufficient adhesion is ensured, and performance deterioration due to the interface adhesion layer 20 is prevented, thereby realizing a long-life organic EL device 10.

As shown in Patent Documents 1 and 2, in an organic EL device that seals an organic EL element with a sealing substrate, a sealing member such as an adhesive layer is usually provided so as to cover the entire surface of the organic EL element. The organic EL element is sealed with the sealing substrate by sticking the sealing substrate to the sealing member.
However, as described above, according to the study by the present inventors, in such an organic EL device, deterioration of the organic EL element may not be sufficiently prevented due to moisture entering from the end face of the sealing member.
In order to prevent moisture from entering from the end face, it is advantageous that the sealing member is thin. However, if the sealing member is thinned, sufficient adhesion cannot be obtained.

In order to prevent this reduction in adhesion, an interface adhesion layer is used between the element substrate 12 and the sealing member 18 or between the sealing member 18 and the sealing substrate 16 using a silane coupling agent or the like. Can be considered.
Although it is not the interface of the sealing member 18, in patent document 1, in a gas barrier film, as an intermediate | middle layer provided between a base material and a gas barrier layer, the interface for improving the adhesive force of a base material and a gas barrier layer It is described that an adhesion layer (anchor coat layer) is provided.

Here, as shown in Patent Document 1, the interfacial adhesion layer is usually provided corresponding to the entire interface to be bonded.
However, according to studies by the present inventors, in an organic EL device that seals an organic EL element with a sealing substrate using a sealing member, when an interface adhesion layer is formed on the entire surface of the element substrate or the sealing substrate, Deterioration of the organic EL element due to degassing from the interfacial adhesion layer, degradation of the organic EL element due to the decomposed interfacial adhesion layer, change in the color of irradiation light due to coloring of the interfacial adhesion layer, etc. Inconveniences such as shortening the lifetime of the organic EL device and deteriorating the optical characteristics of the organic EL device occur.

On the other hand, in the organic EL device 10 of the present invention, the interface adhesion layer 20 is provided by patterning.
Therefore, compared with the case where the interfacial adhesion layer is formed on the entire surface, it is possible to prevent deterioration of the organic EL element 14 and optical characteristics due to the interfacial adhesion layer 20.
Further, by having the interfacial adhesion layer 20, peeling between the element substrate 12 and the sealing member 18 and peeling between the sealing member 18 and the sealing substrate 16 can be prevented, and intrusion of moisture from the peeling portion can also be prevented. In addition, it is possible to prevent moisture from entering from the interface between the element substrate 12 and the sealing member 18 and from the interface between the sealing member 18 and the sealing substrate 16.

In the organic EL device 10 of the present invention, the patterning of the interface adhesion layer is not limited to the frame shape in which the organic EL element 14 is surrounded by the surface direction of the element substrate 12 like the interface adhesion layer 20 in the illustrated example. Various patterns can be used according to the shape of the apparatus 10 and the shape of the organic EL element 14.
Preferably, as conceptually shown in FIG. 1B, the interfacial adhesion layer 20 is more organic than the intermediate position S between the end of the sealing member 18 and the organic EL element 14 in the surface direction of the element substrate 12. Patterning is preferably performed so as not to exist on the 14 side. In other words, the interface adhesion layer 20 is L / 2 or more from the organic EL element 14 when the shortest distance between the end of the sealing member 18 and the organic EL element 14 is L in the surface direction of the element substrate 12. Patterning is preferably performed so as to be separated from each other.

Further, as shown in FIGS. 1A and 1B, an adhesion portion between the element substrate 12 and the sealing member 18 by the interface adhesion layer 20 and an adhesion portion between the sealing substrate 16 and the sealing member 18 by the interface adhesion layer 20. It is preferable that at least one of these is not more than the area of the sealing member 18.

By having such a configuration, it is possible to suitably prevent the lifetime of the organic EL element 14 due to the interface adhesion layer 20 described above, the deterioration of the optical characteristics of the organic EL device 10, and the like.

In addition, the interfacial adhesion layer 20 is more preferably a frame-like pattern that surrounds the organic EL element 14 in the surface direction of the element substrate 12 as shown in the example in that moisture can be prevented from entering the organic EL element 14. Is preferred.
Further, the formation pattern of the interfacial adhesion layer 20 may be a pattern formed to the outside in the surface direction of the element substrate 12 rather than at least one of the element substrate 12 and the sealing member 18. The pattern may be formed to the outside in the surface direction of the element substrate 12 rather than at least one of the sealing substrate 16.

In the embodiment shown in FIG. 1A in which the sealing member 18 covers the organic EL element 14 in its entirety, if there is no optical problem, interfacial adhesion provided between the sealing substrate 16 and the sealing member 18. The layer may be formed as a uniform layer on the entire surface of the sealing member 18 without patterning.
That is, in the embodiment shown in FIG. 1A in which the sealing member 18 covers the entire surface of the organic EL element 14, only the interface adhesion layer 20 provided between the element substrate 12 and the sealing member 18 is patterned. Good.

In the organic EL device 10 of the present invention, the thickness of the interfacial adhesion layer 20 depends on the forming material of the interfacial adhesion layer 20, the adhesion between the interfacial adhesion layer 20 and the sealing substrate 16, the sealing member 18, the element substrate 12, and the like. Accordingly, it may be set appropriately.
Here, according to the study by the present inventors, the thickness of the interface adhesion layer 20 t _0, when the thickness t ₁ of the sealing member 18, the thickness t ₀ of the interface adhesion layer 20 and the sealing The ratio of the member 18 to the thickness t ₁ is preferably t ₁ / t ₀ ≧ 50, and more preferably t ₁ / t ₀ ≧ 150. That is, the interfacial adhesion layer 20 is preferably much thinner than the sealing member 18.
By setting t ₁ / t ₀ ≧ 50, moisture can be prevented from entering the organic EL element 14 through the interfacial adhesion layer 20, and deterioration of the organic EL element 14 due to moisture can be more suitably prevented. It is preferable in that it can be performed.

In the present invention, the material for forming the interface adhesion layer 20 may be appropriately selected according to the material for forming the element substrate 12, the sealing substrate 16, and the sealing member 18.
A silane coupling agent is illustrated as an example. Various known silane coupling agents can be used. Moreover, a commercial item can also be suitably used for the silane coupling agent. Specifically, Z series made by Toray Dow Corning, KBM series made by Shin-Etsu Silicone, KBE series, and the like are exemplified.

In the present invention, for example, an active layer made of one or more of silicon, germanium, iron, nickel, palladium, titanium, gold, silver, copper, aluminum, indium and the like is formed as the interfacial adhesion layer 20, So-called normal temperature bonding in which the sealing member 18 is bonded to the element substrate 12 and / or the sealing substrate 16 can also be suitably used.
Room temperature bonding may be performed by a known method using a vacuum chamber or the like. In addition, when performing room temperature bonding, an active layer serving as the interface adhesion layer 20 may be formed on both the sealing member 18 and the element substrate 12 and / or the sealing substrate 16 to perform room temperature bonding. Good.
Regarding room temperature bonding, for example, “Room Temperature SiO 2 Wafer Bonding by Adhesion Layer Method Source: Proceedings of the 61st Electronic Components and Technology Conference (ECTC) 2011, May 31-June 3, 2011” may be referred to.

Here, in the organic EL device 10 of the present invention, the interfacial adhesion layer 20 preferably contains 10% by mass or more of silicon atoms.
It is preferable that the interfacial adhesion layer 20 contains 10% by mass or more of silicon atoms in that the adhesion between the sealing member 18 and the element substrate 12 and / or the sealing substrate 16 can be increased.

Such an organic EL device 10 can be manufactured using various known methods.
As an example, the interface adhesion layer 20 is formed on the surface of the element substrate 12, and then the organic EL element 14 is formed on the element substrate 12. The formation of the interfacial adhesion layer 20 may be performed by a known method according to the forming material such as a coating method. Further, the organic EL element 14 may be formed by a known method.
On the other hand, the interfacial adhesion layer 20 is formed on the sealing substrate 16, and then the sealing member 18 is formed on the sealing substrate 16 by positioning. The formation of the interfacial adhesion layer 20 and the sealing member 18 may be performed by a known method according to the forming material of the interfacial adhesion layer 20 and the sealing member 18 such as a coating method or sticking.
Finally, the element substrate 12 and the sealing substrate 16 are aligned and bonded through the sealing member 18, and the sealing member 18 is cured by ultraviolet irradiation or the like as necessary, thereby organic EL. Device 10 is fabricated.

3A and 3B conceptually show another example of the organic EL device of the present invention.
3B is a schematic plan view similar to FIG. 1B, and FIG. 3A is a schematic cross-sectional view of FIG. 3B similar to FIG. 1A.

In the organic EL device 10 shown in FIG. 1A and the like described above, a sealing member 18 for sealing the organic EL element 14 by the sealing substrate 16 is provided so as to cover the organic EL element 14 entirely. The organic EL element 14 is sealed by the sealing substrate 16 by sticking the sealing substrate 16 to the sealing member 18.
On the other hand, the organic EL device 40 shown in FIGS. 3A and 3B uses a frame-shaped sealing member 42 surrounding the organic EL element 14 in the substrate surface direction of the element substrate 12, and a frame is formed on the upper surface of the sealing member 42. The organic EL element 14 is sealed by the sealing substrate 16 by providing the sealing substrate 16 on the sealing member 42 on which the interface adhesive layer 20 is formed. is doing.
In the organic EL device 40, as an example, the interface adhesion layer 20 is not provided between the element substrate 12 and the sealing member 42.

That is, in the organic EL device 40 shown in FIG. 3A and the like, the organic EL element 14 is not covered by the adhesive sealing member 18 but by the frame-shaped sealing member 42 having necessary gas barrier properties. And the upper surface of the sealing member 42 is closed with the sealing substrate 16, thereby sealing the organic EL element 14 with the sealing substrate 16 and preventing deterioration due to moisture or the like.
Therefore, in this example, the thickness (height) of the sealing member 42 may be set as appropriate according to the thickness required for the organic EL device 40 and the like.

The frame-shaped sealing member 42 may be formed by a known method according to a forming material, using various known materials such as a resin material or an inorganic material, as long as it has a required gas barrier property.
As a suitable example, a sealing member 42 in which a resin frame is formed by a coating method, adhesion, or the like, and the surface of the frame is covered with an inorganic material is exemplified.
According to this method, it is possible to obtain an adhesive force between the high element substrate 12 and the sealing member 42, eliminate the need for an interfacial adhesive layer therebetween, and form the sealing member 42 having a high gas barrier property.

As an inorganic substance which coat | covers the frame which consists of resin materials, the various inorganic compounds illustrated by the inorganic layer 36 of the above-mentioned gas barrier film 30 are illustrated suitably. When this inorganic compound is used, not only the frame but also the organic EL element 14 may be covered with this inorganic compound. Thereby, deterioration of the organic EL element 14 due to moisture can be more suitably prevented.
In addition to the above inorganic compounds, metals and the like can be used as the inorganic material for covering the frame made of the resin material.
Covering the resin frame with an inorganic material may be performed by a known method according to the forming material, such as plasma CVD, sputtering, or vacuum deposition.

In the sealing member 42 in which the surface of such a resin frame is covered with an inorganic material, the water vapor permeability of the inorganic material covering the frame is 100 μm under the conditions of a temperature of 40 ° C. and a relative humidity of 90% RH. It is preferably 50 g / (m ² · day) or less per unit.

Moreover, in the structure using the sealing member 42 which coat | covered the surface of the resin-made frame body with the inorganic substance, as the interface adhesion layer 20, the active layer which consists of silicon etc. is formed as the interface adhesion layer 20, and a sealing member is carried out by normal temperature joining A configuration in which the substrate 18 and the sealing substrate 16 are bonded together is preferably used.

In the embodiment shown in FIG. 3A using the frame-shaped sealing member 42, the sealing member 42 preferably has an elastic modulus of 0.1 to 520 N / mm ² , and is preferably 0.2 to 480 N / mm ² . Is more preferable.
By setting the elastic modulus of the sealing member 42 to 0.1 N / mm ² or more, the sealing member 42 with good gas barrier properties can be formed. In addition, when a force is applied in a direction in which the sealing substrate 16 is peeled off, if the elastic modulus of the sealing member 42 is low, the sealing member 42 is extended and broken, and the sealing is broken. Such inconvenience can be prevented by setting the elastic modulus of the material to 0.1 N / mm ² or more.
By setting the elastic modulus of the sealing member 42 to 520 N / mm ² or less, it is preferable in that the organic EL device 40 having good flexibility can be obtained.

Even in the configuration using the frame-shaped sealing member 42 shown in FIG. 3A and the like, the interfacial adhesion layer 20 has an intermediate position S between the end of the sealing member 42 and the organic EL element 14 in the surface direction of the element substrate 12. It is preferable that the patterning is performed so as not to exist on the organic EL element 14 side.
Here, when such a frame-shaped sealing member 42 is used, as conceptually shown in FIG. 3B, the end of the sealing member 42 is on the organic EL element 14 side of the sealing member 42. Point to the end.

That is, in the configuration using the frame-shaped sealing member 42, as shown conceptually in FIG. 3B, the interfacial adhesion layer 20 includes the organic EL and the inner end of the sealing member 42 in the surface direction of the element substrate 12. It is preferable that patterning is performed so that the organic EL element 14 side does not exist with respect to the intermediate position S with respect to the element 14.
In other words, the interface adhesion layer 20 has an organic EL element of L / 2 or more when the shortest distance between the inner end of the sealing member 42 and the organic EL element 14 is L in the surface direction of the element substrate 12. The patterning is preferably performed so as to be away from 14.

Therefore, in the configuration using the frame-shaped sealing member 42 as in the organic EL device 40, the interface adhesion layer 20 is not only from the upper surface of the sealing member 42 but also from the inner side surface of the sealing member 42. This includes the case where it reaches the surface.

Such an organic EL device 40 can also be manufactured using various known methods.
As an example, first, the sealing member 42 is formed on the surface of the element substrate 12, and then the organic EL element 14 is formed on the element substrate 12. The sealing member 42 may be formed by a known method according to the forming material such as a coating method. Further, the organic EL element 14 may be formed by a known method.
Next, if necessary, the entire surface of the sealing member 42 or the element substrate 12 is coated with an inorganic material such as silicon nitride. As described above, the sealing member 42 may be coated with an inorganic material by a known method such as sputtering according to the forming material.
Next, an active layer made of silicon or the like is formed as the interfacial adhesion layer 20 on the upper surface of the sealing member 42. The formation of the interfacial adhesion layer 20 may be performed by a known method such as sputtering according to the forming material.
On the other hand, an active layer made of silicon or the like is similarly formed on the sealing substrate 16 as the interface adhesion layer 20 in alignment with the interface adhesion layer 20 previously formed on the sealing member 42.
Finally, in the vacuum chamber, the interfacial adhesion layers 20 are face-to-face and aligned, the element substrate 12 and the sealing substrate 16 are stacked, and are bonded at room temperature in a vacuum to produce the organic EL device 10. .

The electronic device of the present invention has been described in detail above. However, the present invention is not limited to the above-described example, and various improvements and modifications may be made without departing from the gist of the present invention. Of course.

Hereinafter, specific examples of the present invention will be given and the present invention will be described in more detail.

[Example 1]
<Preparation of gas barrier film 30>
A PET film (A4300, manufactured by Toyobo Co., Ltd.) having a thickness of 100 μm was prepared as the support 32.

TMPTA (manufactured by Daicel Celltech), silane coupling agent (KBM-5103, manufactured by Shin-Etsu Chemical Co., Ltd.) and polymerizable acidic compound (KARAMER PM-21, manufactured by Nippon Kayaku Co., Ltd.) in a mass ratio of 14.1: 3. A composition was prepared by mixing at 5: 1.
18.6 g of this composition, 1.4 g of an ultraviolet polymerization initiator (ESACURE KTO46, manufactured by Lamberti) and 180 g of 2-butanone were mixed to prepare a coating material for forming the organic layer 34.

The prepared paint was applied to the surface of the prepared support 32 (PET film). The coating was applied using a wire bar so that the coating thickness was 5 μm.
After applying the paint, the paint was dried by allowing it to stand at room temperature.
Next, the composition of the coating was cured by irradiating with ultraviolet rays from a high-pressure mercury lamp (integrated irradiation amount: about 1 J / cm ² ) in a chamber in which the oxygen concentration was 0.1% by a nitrogen substitution method. Thereby, an organic layer 34 having a thickness of 1 μm was formed on the surface of the support 32.

A silicon nitride film having a thickness of 35 nm was formed as an inorganic layer 36 on the organic layer 34.
The inorganic layer 36 (silicon nitride film) was formed using a general CCP (capacitively coupled plasma) -CVD apparatus. As source gases, silane gas (flow rate 160 sccm), ammonia gas (flow rate 370 sccm), hydrogen gas (flow rate 590 sccm), and nitrogen gas (flow rate 240 sccm) were used. The film forming pressure was 40 Pa. The power supply was a high frequency power supply with a frequency of 13.56 MHz, and the plasma excitation power was 2.5 kW.
Thereby, the gas barrier film 30 as shown in FIG. 2 which had the organic layer 34 on the support body 32 and had the inorganic layer 36 on it was produced.

[Example 1]
The produced gas barrier film 30 was cut into a 50 mm square to form an element substrate 12.
The element substrate 12 was bonded to a glass substrate of 50 mm square for transportation, and a laminate film (PAC3, manufactured by Sanei Kaken Co., Ltd.) cut out to 38 mm square was bonded to the center to make a mask.
The element substrate 12 to which the mask was bonded was set on a spin coater, and a silane coupling agent (KBM-403, manufactured by Shin-Etsu Silicone) diluted to 1 w% with pure water was applied. This silane coupling agent contains 10% by mass of silicon atoms.
Then, the silane coupling agent was wiped off with a dry cotton swab at a width of 4 mm from the end, and patterned so that the silane coupling agent remained in a frame shape. Then, the element board | substrate 12 which dried in 110 degreeC oven for 1 hour and formed the interface adhesion layer 20 which consists of a silane coupling agent patterned into the frame shape of 2 mm width was obtained.

The organic EL element 14 was formed on the surface of the element substrate 12 where the interface adhesion layer 20 was formed as follows.
First, ITO was formed on the surface of the element substrate 12 by sputtering so as to have a film thickness of 60 nm, thereby forming an anode. Hole injection of HAT-CN layer (2,3,6,7,10,11-Hexacyano-1,4,5,8,9,12-hexaazatriphenylene layer) into the formed anode surface using a vacuum evaporation system The layer was formed to a thickness of 2 nm, and a hole transport layer (α-NPD: Bis [N- (1-naphthyl) -N-phenyl] benzidine) was formed on the surface of the HAT-CN layer in order of 29 nm and CBP ( The emission layer doped with 5% Ir (ppy) ₃ (Tris (2-phenylpyridinato) iridium) with 4,4'-Bis (carbazol-9-yl) biphenyl) as the host material and 20 nm as the hole blocking layer and BAlq The (Bis- (2-methyl-8-quinolinolato) -4- (phenyl-phenolate) -aluminium (III)) layer is 10 nm, and the Alq3 (Tris (8-hydroxy-quinolinato) aluminium) layer is 20 nm as the electron transport layer. An organic electroluminescent layer was formed by vapor deposition with each film thickness.
Subsequently, on the surface of the obtained organic light emitting layer, LiF was deposited to a thickness of 1.5 nm and Al was deposited to a thickness of 200 nm in this order to form a cathode, and an organic EL element 14 was formed on the surface of the element substrate 12. .

On the other hand, the produced gas barrier film 30 was cut into a 42 mm square to form a sealing substrate 16. An interfacial adhesion layer 20 made of a silane coupling agent patterned in a frame shape having a width of 2 mm was formed on the sealing substrate 16 in the same manner as the element substrate 12.
In the glove box, an adhesive (teas Barrier Transfer Tape 3rdG, manufactured by TESA Tape) was bonded as a sealing member 18 to the sealing substrate 16 on which the interfacial adhesion layer 20 was formed.
Furthermore, the element substrate 12 on which the organic EL element 14 was formed was conveyed into the glove box and bonded to the sealing substrate 16 to which the sealing member 18 was bonded.
Thereafter, an ultraviolet ray having a wavelength of 365 nm was irradiated from the sealing substrate 16 side in an integrated amount of 400 mJ / cm ² to produce an organic EL device 10 as shown in FIGS. 1A and 1B.

[Example 2]
As the element substrate 12, a 50 mm square glass substrate (OA-10G, manufactured by Nippon Electric Glass Co., Ltd.) was prepared. An ITO film having a thickness of 100 nm was formed on the surface of the element substrate 12 as an anode.
A PI varnish (polyimide varnish) was applied to the element substrate 12 on which the anode was formed and dried, followed by patterning to form a frame shape having an outer dimension of 42 mm and an inner dimension of 38 mm. In this way, a frame-shaped sealing member 42 was formed on the element substrate 12.

The organic EL element 14 was formed on the element substrate 12 on which the sealing member 42 was formed in the same manner as in Example 1 except that the anode was formed.

The element substrate 12 on which the organic EL element 14 was formed was introduced into a vacuum chamber (pressure 10 ⁻⁴ Pa or less), and a silicon nitride film having a thickness of 20 nm was formed on the entire surface by sputtering.
Then, the mask was set using the frame-shaped mask whose opening part is 42 mm in outer dimension and 38 mm in inner dimension so that an opening part and the upper surface of the sealing member 42 may overlap. Then, a patterned interface adhesion layer 20 made of silicon was formed on the upper surface of the sealing member 42 by forming a silicon film having a thickness of 10 nm by sputtering.

The produced gas barrier film 30 was cut into a 44 mm square to form a sealing substrate 16. This sealing substrate 16 was bonded to a glass substrate for conveyance.
The sealing substrate 16 is introduced into a vacuum chamber, a rectangular frame mask having an opening of 42 mm and an inner dimension of 38 mm is bonded to the center, and silicon is deposited to a thickness of 10 nm by sputtering. A patterned interface adhesion layer 20 made of silicon was formed on the upper surface of the member 42.

An organic EL device 14 is formed, and an element substrate 12 formed by patterning the interface adhesion layer 20 made of silicon and a sealing substrate 16 formed by patterning the interface adhesion layer 20 made of silicon are connected to the interface. The adhesion layer 20 was aligned and faced, and bonded at room temperature under reduced pressure in a vacuum chamber to produce an organic EL device 40 as shown in FIGS. 3A and 3B.

[Comparative Example 1]
An organic EL device was produced in the same manner as in Example 1 except that the interface adhesion layer 20 was not formed on the element substrate 12 and the sealing substrate 16.
[Comparative Example 2]
An organic EL device was produced in the same manner as in Example 1 except that the interface adhesion layer was formed on the entire surface of the element substrate 12 and the sealing substrate 16 without patterning.

[Comparative Example 3]
The element substrate 12 was formed in the same manner as in Example 1, and the organic EL element 14 was formed without providing the interface adhesion layer 20.
The produced gas barrier film 30 was cut into a 42 mm square to form a sealing substrate 16.
The sealing substrate 16 was bonded to a glass substrate for transportation. A UV adhesive (XNR5516Z, manufactured by Nagase ChemteX Corporation) is applied in a frame shape along four sides to a position 1 mm inside from the edge of the barrier film of the sealing substrate 16 by a dispenser, and the sealing member 42 ( Uncured) was formed.
The element substrate 12 on which the organic EL element 14 was formed and the sealing substrate 16 on which the sealing member 42 was formed were conveyed into a glove box, aligned, and bonded together.
Thereafter, an ultraviolet ray having a wavelength of 365 nm was applied from the sealing substrate 16 side in an integrated manner to 6000 mJ / cm ² to cure the uncured sealing member 42 to produce an organic EL device.

In addition, about each produced organic EL apparatus, the thickness of the sealing member, the water vapor transmission rate of the sealing member, the elasticity modulus of the sealing member, and the thickness of the interface adhesion layer were measured as follows.
<Thickness of sealing member>
Example 1 and Comparative Examples 1 and 2 were measured using a micrometer, and Example 2 and Comparative Example 3 were measured using a contact-type step gauge (Dectaku, manufactured by VEECO).

<Water vapor transmission rate of sealing member>
In Example 1 and Comparative Examples 1 and 2, since the sealing member was a sheet, it was bonded to a TAC film, and in JIS Z 0208: 1976 by the cup method in an environment of a temperature of 40 ° C. and a relative humidity of 90% RH. Measured in conformity.
In Comparative Example 3, a UV adhesive was applied to a Teflon (registered trademark) sheet in the form of a sheet, and cured by irradiation with ultraviolet rays. After curing, the sample was peeled from the Teflon (registered trademark) sheet and measured according to JIS Z 0208: 1976 by the cup method in an environment of a temperature of 40 ° C. and a relative humidity of 90% RH.
In Example 2, a device having the same configuration as that of the organic EL device was produced except that a calcium film having a thickness of 100 nm was used instead of the organic EL element 14, and an environment having a temperature of 40 ° C. and a relative humidity of 90% RH was prepared. The water vapor transmission rate of the sealing member was estimated from the corrosion rate of calcium below.
The water vapor transmission rate is a water vapor transmission rate per 100 μm thickness.

<Elastic modulus of sealing member>
In Example 1 and Comparative Examples 1 and 2, 20 layers of sealing members were stacked to a thickness of 1 mm, and this was cut into a 5 mm × 4 cm strip. The elastic modulus was measured by pulling both ends of the strip sample with a 180 ° C. tensile tester (Autograph, manufactured by Shimadzu Corporation).
In Example 2 and Comparative Example 3 as well, a film formed so as to have a thickness of 1 mm was cut out into a 5 mm × 4 cm strip and measured.

<Thickness of interfacial adhesion layer>
The cross section was measured by photographing with a scanning electron microscope.

The produced organic EL device was evaluated as follows.
A sealing member / interface adhesion layer / sealing substrate is formed on a glass substrate in the same manner as each organic EL device, and the sealing substrate and the sealing member are formed by a 180 ° C. tensile tester (Autograph, manufactured by Shimadzu Corporation). The peel strength was measured. Evaluation was performed as follows.
A: Peel strength is over 3 N / cm B: Peel strength is 1 to 3 N / cm
C: Peel strength is less than 1 N / cm

<Durability>
The organic EL device was allowed to stand for 100 hours in a high-temperature and high-humidity environment (temperature 60 ° C., relative humidity 90% RH). Evaluation was performed as follows.
A: Total area of dark spots with respect to light emitting surface is less than 3% B: Total area of dark spots with respect to light emitting surface is 3% to 40%
C: Total area of dark spots on the light emitting surface exceeds 40% or does not light up

<Water vapor transmission rate at the end>
A frame-shaped sealing member having a width of 2 mm and a side of 2 cm is formed of the same material as each organic EL device on a glass substrate on which a calcium film is deposited, and an interfacial adhesion layer is formed thereon, as in each organic EL device. After forming, the frame of the sealing member was sealed with a sealing substrate similarly to each organic EL device.
In this state, in an environment of a temperature of 40 ° C. and a relative humidity of 90% RH, the amount of moisture that permeates was determined by the corrosion rate of the calcium film in the frame, and the water vapor permeability at the end was estimated.
In Comparative Example 2, the interface adhesion layer is formed on the entire surface, and the end portion cannot be defined.
The results are shown in the table below.

As shown in Table 1, Example 1 uses a patterned silane coupling agent as an interfacial adhesion layer. For this reason, the adhesion is high and moisture permeation at the interface is suppressed, and the organic EL device has good durability because it is patterned. In Example 2, since patterned Si was used as an interfacial adhesion layer and sealing was performed using a room temperature bonding technique, strong adhesion was exhibited. Moreover, since moisture permeation from between the element substrate 12 and the sealing substrate 16 is suppressed, the organic EL durability is also good.
On the other hand, in Comparative Example 1, compared with Example 1, since there is no interfacial adhesion layer, moisture permeation from the interface occurs and the durability of the organic EL device is C. Also, the adhesion is low and weak against bending. In Comparative Example 2, since the interface adhesion layer is not patterned, the silane coupling agent damages the organic EL element, and the durability of the organic EL device is C. Comparative Example 3 uses a UV curable resin as a sealing material and is hard because of its low adhesion, and, similarly to Comparative Example 1, moisture penetration from the interface occurs due to the absence of the interface adhesion layer, and the durability of the organic EL device Sex is also C.
From the above results, the effects of the present invention are clear.

It can be suitably used for various electronic devices such as organic EL devices such as organic EL displays and organic EL lighting.

10,40 Organic EL device (Organic electroluminescence device)
12 element substrate 14 organic EL element (organic electroluminescence element)
16 sealing

substrate

18, 42 sealing member 20 interface adhesion layer 30 gas barrier film 32 support 34 organic layer 36 inorganic layer

Claims

An element substrate;
An electronic element formed on the element substrate;
A sealing substrate for sealing the electronic element;
A sealing member provided between the element substrate and the sealing substrate to seal the electronic element with the sealing substrate;
An electronic device comprising a patterned interface adhesion layer provided on at least one of the element substrate and the sealing member and between the sealing substrate and the sealing member.
The interface adhesion layer is patterned so as not to be positioned closer to the electronic element than an intermediate position between the end of the sealing member and the electronic element in the surface direction of the element substrate. Electronic devices.
At least one of the adhesion portion between the element substrate and the sealing member by the interface adhesion layer and the adhesion portion between the sealing substrate and the sealing member by the interface adhesion layer is equal to or less than the area of the sealing member. The electronic device according to claim 1.
The electronic device according to any one of claims 1 to 3, wherein a ratio between a thickness t 0 of the interface adhesion layer and a thickness t 1 of the sealing member is t 1 / t 0 ≥100.
The electron according to any one of claims 1 to 4, wherein the sealing member has a water vapor transmission rate of 50 g / (m 2 · day) or less per 100 µm thickness at a temperature of 40 ° C and a relative humidity of 90% RH. apparatus.
6. The electronic device according to claim 1, wherein the interfacial adhesion layer contains 10 mass% or more of silicon atoms.
The at least one of the element substrate and the sealing substrate has a support and one or more combinations of an inorganic layer provided on one surface of the support and an organic layer serving as a formation surface of the inorganic layer. 7. The electronic device according to any one of 1 to 6.
The electronic device according to any one of claims 1 to 7, wherein the sealing member has a sheet shape covering the entire surface of the electronic element.
The electronic device according to any one of claims 1 to 7, wherein the sealing member is a frame surrounding the electronic element in a surface direction of the element substrate.