JP2011044378A - Method of manufacturing organic electroluminescence light emitting device - Google Patents

Abstract

<P>PROBLEM TO BE SOLVED: To provide a method of manufacturing an organic electroluminescence light emitting device, capable of improving the reliability of an organic electroluminescent device by arranging a diffraction grating in the vicinity of an organic light emitting layer only by adhesion without causing any damage to the element. <P>SOLUTION: The method of manufacturing an organic electroluminescence light emitting device includes an organic electroluminescent device forming step of forming an organic electroluminescent device by laminating a reflection electrode, an organic light emitting layer, and an electrode in this order on a substrate, a diffraction grating structure forming step of forming a diffraction grating structure by forming a diffraction grating on a transparent substrate, and an adhesion step of causing the organic electroluminescent device and the diffraction grating structure to adhere to each other by an adhesive layer having a refractive index different from that of the diffraction grating while the organic electroluminescent device and the diffraction grating structure are opposed to each other. <P>COPYRIGHT: (C)2011,JPO&INPIT

Description

  The present invention relates to a method for manufacturing an organic electroluminescence light emitting device.

Conventionally, in order to improve the light extraction efficiency of an organic electroluminescent light emitting device (organic electroluminescent device), in the vicinity of an organic electroluminescent element having an opposing electrode and an organic light emitting layer sandwiched between the opposing electrodes. The diffraction grating surface is arranged so as to be parallel to the organic light emitting layer, and guided mode light propagating in the organic light emitting layer is extracted in a direction substantially perpendicular to the diffraction grating surface using the diffraction effect. ing.
Patent Document 1 discloses an organic electroluminescence element having a top emission structure in which a diffraction grating is disposed on an organic light emitting layer. A diffraction grating composed of fine irregularities is generally finely processed by a photolithography process, a nanoimprint process, or the like.
When a wet process is used in the photolithography process, there is a problem in that the organic light emitting layer is damaged because the solution barrier properties such as the periphery of the organic light emitting layer are not sufficient. Further, when a dry process is used in the photolithography process, there is a problem that the surface temperature becomes high and the organic light emitting layer is damaged.
In the nanoimprint process, when a heating process is used, there is a problem that the surface temperature becomes high and the organic light emitting layer is damaged. Further, in the nanoimprint process, when a photocuring process is used instead of a heating process, there is a problem that the organic light emitting layer is damaged because of a stamper pressing process.
Patent Document 2 discloses an organic electroluminescence element having a base surface on which a plurality of projections and depressions (diffraction gratings) are formed, a pair of electrodes facing each other and the organic light-emitting layer interposed therebetween, and An organic electroluminescent light emitting device having a high refractive index layer containing a resin and inorganic fine particles interposed between a base surface and the organic electroluminescent element is disclosed.
In the organic electroluminescence light emitting device, in order to realize a good light extraction efficiency, the high refractive index layer needs to be as thin as possible, but the high refractive index layer contains fine particles, and the surface Since unevenness due to fine particles occurs, it is difficult to flatten the high refractive index layer. Therefore, when an organic electroluminescence layer including an electrode is stacked on the high refractive index layer, the organic electronics layer including the electrode is uneven due to the unevenness due to the fine particles, and the film thickness is not uniform. There was a problem that a leak occurred, a large current flowed locally, and the organic electroluminescence element was destroyed. Here, in order to flatten the high refractive index layer, it is necessary to thicken the flattening layer, the distance between the unevenness and the organic light emitting layer becomes long, the light extraction efficiency decreases, and the organic electroluminescence element There was a problem that the reliability of the system would be lowered.
From the above, in organic electroluminescence light emitting devices with a top emission structure, a diffraction grating is laminated in the vicinity of the organic electroluminescence element without damaging the organic light emitting layer, improving the light extraction efficiency and organic electroluminescence. There is a problem that it is difficult to improve the reliability of the element.
Patent Document 3 discloses a light-emitting device in which a drive panel and a sealing panel are bonded to each other with an adhesive layer. However, since this light-emitting device is not provided with a diffraction grating, There was a problem that the extraction efficiency could not be improved and the reliability of the organic electroluminescence element could not be improved.
Further, in Patent Document 4, in an organic electroluminescence display in which an optical filter and an organic electroluminescence element are combined, an organic electroluminescence element is formed on the surface of the optical filter by forming a fine uneven surface having a pitch equal to or less than the wavelength of light. In this organic electroluminescence display, the efficiency of extracting light from the organic electroluminescence element to the outside is improved, and the organic electroluminescence element is improved. There was a problem that reliability could not be improved.

JP 2006-190573 A JP 2007-335253 A JP 2003-86358 A JP 2004-258586 A

  An object of the present invention is to solve the conventional problems and achieve the following objects. That is, the present invention provides an organic electroluminescent light emitting device in which a diffraction grating is arranged in the vicinity of an organic electroluminescent element to improve the light extraction efficiency, without performing any chemical process or physical process in the vicinity of the organic light emitting layer. Therefore, a method of manufacturing an organic electroluminescent light emitting device that can improve the reliability of an organic electroluminescent element by arranging a diffraction grating in the vicinity of the organic light emitting layer by adhesion alone without causing any damage to the element. The purpose is to provide.

Means for solving the problems are as follows. That is,
<1> A reflective electrode, an organic light emitting layer, and an electrode are laminated on the base material in this order to form an organic electroluminescent element, and a diffraction grating is formed on the transparent base material. The organic electroluminescence element is formed by a diffraction grating structure forming step for forming a diffraction grating structure, the organic electroluminescence element and the diffraction grating structure facing each other, and an adhesive layer having a refractive index different from that of the diffraction grating. It is a manufacturing method of the organic electroluminescent light-emitting device characterized by including the adhesion process which adhere | attaches a luminescent element and the said diffraction grating structure.
<2> The method for producing an organic electroluminescence light-emitting device according to <1>, wherein the refractive index of the adhesive layer is larger than the refractive index of the diffraction grating.
<3> The method for producing an organic electroluminescence light-emitting device according to <2>, wherein inorganic fine particles are dispersed in the adhesive layer.
<4> The method for producing an organic electroluminescence light-emitting device according to any one of <1> to <3>, further including a sealing layer laminating step of laminating a sealing layer on the organic electroluminescence element.
<5> The method for producing an organic electroluminescence light-emitting device according to any one of <1> to <4>, further including a circularly polarizing member forming step of forming a circularly polarizing member between the transparent substrate and the diffraction grating. It is.
<6> The method according to any one of <1> to <4>, further including a circularly polarizing member forming step of forming a circularly polarizing member on a surface opposite to the surface on which the diffraction grating of the transparent substrate is formed. This is a method for producing an organic electroluminescence light-emitting device.
<7> The method for producing an organic electroluminescence light-emitting device according to any one of <1> to <6>, further including a color filter member forming step of forming a color filter member between the transparent substrate and the diffraction grating. It is.
<8> The method according to any one of <1> to <6>, further including a color filter member forming step of forming a color filter member on a surface opposite to the surface on which the diffraction grating of the transparent substrate is formed. This is a method for producing an organic electroluminescence light-emitting device.

  According to the present invention, in the organic electroluminescence light-emitting device which can solve the conventional problems and achieve the object, and arranges the diffraction grating in the vicinity of the organic electroluminescence element to improve the light extraction efficiency. Without applying any chemical process or physical process in the vicinity of the layer, and therefore, without damaging the element, the diffraction grating is disposed in the vicinity of the organic light emitting layer only by adhesion, and the organic electroluminescent element It is possible to provide a method for manufacturing an organic electroluminescence light emitting device capable of improving reliability.

FIG. 1 is a diagram illustrating an example of an organic electroluminescence light-emitting device manufactured by the method for manufacturing an organic electroluminescence light-emitting device of the present invention. FIG. 2 is a diagram showing another example of an organic electroluminescence light emitting device manufactured by the method for manufacturing an organic electroluminescence light emitting device of the present invention. FIG. 3: A is a figure which shows an example of the manufacturing method of the TFT substrate for organic EL in an organic electroluminescent light-emitting device (the 1). FIG. 3B is a diagram illustrating an example of a method for producing a TFT substrate for organic EL in an organic EL light emitting device (part 2). FIG. 3: C is a figure which shows an example of the manufacturing method of the TFT substrate for organic EL in an organic electroluminescent light-emitting device (the 3). FIG. 3D is a diagram showing an example of a method for producing an organic EL TFT substrate in an organic EL light emitting device (part 4). FIG. 4 is a diagram illustrating an example of an organic EL TFT substrate in a top emission type organic EL light emitting device.

  Hereafter, the manufacturing method of the organic electroluminescent light-emitting device of this invention is demonstrated in detail.

(Manufacturing method of organic electroluminescence light emitting device)
The manufacturing method of the organic electroluminescence light emitting device of the present invention includes at least an organic electroluminescence element formation step, a diffraction grating structure formation step, and an adhesion step, and includes a sealing layer lamination step, a circularly polarizing member formation step, a color It further includes a filter member forming step and, if necessary, other steps.

-Organic electroluminescence device formation process-
The organic electroluminescence element forming step is a step of forming an organic electroluminescence element by laminating a reflective electrode, an organic light emitting layer, and an electrode in this order on a substrate.

--Base material--
There is no restriction | limiting in particular as said base material, Although it can select suitably according to the objective, It is preferable that it is a base material which does not scatter or attenuate the light emission from an organic layer. Specific examples include yttria-stabilized zirconia (YSZ), inorganic materials such as glass, polyesters such as polyethylene terephthalate, polybutylene phthalate, and polyethylene naphthalate, polystyrene, polycarbonate, polyethersulfone, polyarylate, polyimide, and polycycloolefin. , Norbornene resins, and organic materials such as poly (chlorotrifluoroethylene).
For example, when glass is used as the base material, it is preferable to use alkali-free glass for the material in order to reduce ions eluted from the glass. Moreover, when using soda-lime glass, it is preferable to use what gave barrier coatings, such as a silica. In the case of an organic material, it is preferable that it is excellent in heat resistance, dimensional stability, solvent resistance, electrical insulation, and workability.

  There is no restriction | limiting in particular about the shape of the said base material, a structure, a magnitude | size, etc., It can select suitably according to the use and objective of a light emitting element. Generally, the shape of the substrate is preferably a plate shape. The structure of the substrate may be a single layer structure, a laminated structure, may be formed of a single member, or may be formed of two or more members. Good.

The base material may be provided with a moisture permeation preventing layer (passivation film) on the front surface or the back surface.
As a material for the moisture permeation preventing layer (passivation film), inorganic materials such as silicon nitride and silicon oxide are preferably used. The moisture permeation preventing layer (passivation film) can be formed by, for example, a high frequency sputtering method.
When a thermoplastic substrate is used, a hard coat layer, an undercoat layer, or the like may be further provided as necessary.

  There is no restriction | limiting in particular as a refractive index of the said base material, According to the objective, it can select suitably.

  There is no restriction | limiting in particular as thickness of the said base material, Although it can select suitably according to the objective, It needs to be a film thickness which has sufficient barrier property.

-Organic electroluminescence device (organic EL device)-
The organic electroluminescence element has a reflective electrode (anode) and an electrode (cathode), and an organic compound layer including a light emitting layer (organic light emitting layer) between both electrodes. In view of the properties of the light emitting element, the electrode (cathode) is preferably transparent or translucent.

The organic compound layer is preferably laminated in the order of the hole transport layer, the organic light emitting layer, and the electron transport layer from the reflective electrode (anode) side. Further, a hole injection layer is provided between the hole transport layer and the reflective electrode (anode), and / or an electron transport intermediate layer is provided between the organic light emitting layer and the electron transport layer. In addition, a hole transporting intermediate layer may be provided between the organic light emitting layer and the hole transport layer, and similarly, an electron injection layer may be provided between the electrode (cathode) and the electron transport layer.
Each layer may be divided into a plurality of secondary layers.

--- Reflective electrode (anode) ---
The reflective electrode (anode) usually has a function as an electrode for supplying holes to the organic compound layer, and there is no particular limitation on the shape, structure, size, etc. of the light emitting device. Depending on the application and purpose, it can be appropriately selected from known electrode materials.

  Suitable examples of the material for the reflective electrode (anode) include metals, alloys, metal oxides, conductive compounds, and mixtures thereof. Specific examples of the reflective electrode (anode) material include Al, Ag, Al—Ni, a laminate of these and ITO, and the like.

  The reflective electrode (anode) is, for example, a wet method such as a printing method or a coating method, a physical method such as a vacuum deposition method, a sputtering method or an ion plating method, or a chemical method such as CVD or plasma CVD method. From the above, it can be formed on the substrate according to a method appropriately selected in consideration of suitability with the material constituting the anode.

  In the organic electroluminescence element, the formation position of the anode is not particularly limited and can be appropriately selected according to the use and purpose of the light-emitting element, but it is preferably formed on the substrate. In this case, the anode may be formed on the entire one surface of the base material, or may be formed on a part thereof.

  The patterning for forming the reflective electrode (anode) may be performed by chemical etching using photolithography or the like, or may be performed by physical etching using a laser or the like. It may be performed by vapor deposition, sputtering, or the like, or may be performed by a lift-off method or a printing method.

The thickness of the reflective electrode (anode) can be appropriately selected depending on the material constituting the reflective electrode (anode) and cannot be generally specified, but is usually about 10 nm to 100 μm, and 20 nm to 100 μm. Is preferred.
If the thickness of the reflective electrode (anode) is less than 10 nm, sufficient reflection characteristics cannot be obtained. (If it exceeds 100 μm, the manufacturing cost will increase.)

The resistance value of the reflective electrode (anode) is preferably 10 ³ Ω / □ or less, and more preferably 10 ² Ω / □ or less.

---- Electrode (cathode) ---
As long as the electrode (cathode) has a function as an electrode that transmits light emitted from the organic light emitting layer and injects electrons into the organic compound layer, the shape, structure, size, and the like are not particularly limited. However, it can be appropriately selected from known electrode materials according to the use and purpose of the light-emitting element.

  Examples of the material constituting the electrode (cathode) include metals, alloys, metal oxides, electrically conductive compounds, and mixtures thereof. Specific examples of the electrode (cathode) include Ag, Mg—Ag, and Al—Li.

  The materials for the electrodes (cathodes) are described in detail in JP-A-2-15595 and JP-A-5-121172, and the materials described in these public relations also apply to the present invention. Can do.

  There is no restriction | limiting in particular about the formation method of the said electrode (cathode), According to a well-known method, it can carry out. For example, the cathode described above is configured from a wet method such as a printing method or a coating method, a physical method such as a vacuum deposition method, a sputtering method, or an ion plating method, or a chemical method such as CVD or plasma CVD method. It can be formed according to a method appropriately selected in consideration of suitability with the material. For example, when a metal or the like is selected as the cathode material, one or more of them can be simultaneously or sequentially performed according to a sputtering method or the like.

  The patterning for forming the electrode (cathode) may be performed by chemical etching such as photolithography, or may be performed by physical etching using a laser or the like. It may be performed by a lift-off method or a printing method.

In the organic electroluminescence element, the cathode formation position is not particularly limited, and may be formed on the entire organic compound layer or a part thereof.
Further, a dielectric layer made of an alkali metal or alkaline earth metal fluoride or oxide may be inserted between the electrode (cathode) and the organic compound layer with a thickness of 0.1 nm to 5 nm. . This dielectric layer can also be regarded as a kind of electron injection layer. The dielectric layer can be formed by, for example, a vacuum deposition method, a sputtering method, an ion plating method, or the like.

The thickness of the electrode (cathode) can be appropriately selected depending on the material constituting the cathode and cannot be generally defined. However, when a metal, an alloy, or the like is used, it is usually about 10 nm to 30 nm, and preferably 20 nm. .
When the thickness of the electrode (cathode) is less than 10 nm, it is difficult to form a uniform and uniform film, and good current injection characteristics cannot be obtained. In addition, when a microcavity is used, sufficient light reflectance is obtained. May not be obtained. On the other hand, if the thickness of the electrode (cathode) exceeds 30 nm, sufficient light transmittance may not be obtained, and the light output may decrease.

--- Organic compound layer ---
The organic electroluminescence device has at least one organic compound layer including an organic light emitting layer, and other organic compound layers other than the organic light emitting layer include a hole transport layer, an electron transport layer, and a hole block layer. , Electron blocking layer, hole injection layer, electron injection layer, and the like.

  In the organic electroluminescence element, each layer constituting the organic compound layer is formed by a dry film forming method such as a vapor deposition method or a sputtering method, a wet coating method, a transfer method, a printing method, a coating method, an ink jet method, a spray method, or the like. It can form suitably.

---- Organic light emitting layer ----
The organic light emitting layer receives holes from an anode, a hole injection layer, or a hole transport layer when an electric field is applied, receives electrons from a cathode, an electron injection layer, or an electron transport layer, and recombines holes and electrons. It is a layer having a function of providing light and emitting light.
The organic light emitting layer may be composed only of a light emitting material, or may be a mixed layer of a host material and a light emitting dopant. The luminescent dopant may be a fluorescent material or a phosphorescent material, and may be two or more kinds. The host material is preferably a charge transport material. The host material may be one type or two or more types, and examples thereof include a configuration in which an electron transporting host material and a hole transporting host material are mixed. Furthermore, the organic light emitting layer may contain a material that does not have charge transporting properties and does not emit light.
Further, the organic light emitting layer may be one layer or two or more layers, and each layer may emit light in different emission colors.

As the light-emitting dopant, any of phosphorescent light-emitting materials, fluorescent light-emitting materials, and the like can be used as dopants (phosphorescent light-emitting dopants and fluorescent light-emitting dopants).
The organic light emitting layer may contain two or more kinds of luminescent dopants in order to improve color purity or to expand a light emission wavelength region. The luminescent dopant further has an ionization potential difference (ΔIp) and an electron affinity difference (ΔEa) of 1.2 eV>ΔIp> 0.2 eV and / or 1.2 eV> with the host compound. A dopant satisfying the relationship of ΔEa> 0.2 eV is preferable from the viewpoint of driving durability.

The phosphorescent dopant is not particularly limited and may be appropriately selected depending on the purpose. Examples thereof include a complex containing a transition metal atom or a lanthanoid atom.
The transition metal atom is not particularly limited and may be appropriately selected depending on the intended purpose. Ruthenium, rhodium, palladium, tungsten, rhenium, osmium, iridium, gold, silver, copper, and platinum are preferable, and rhenium. , Iridium, and platinum are more preferable, and iridium and platinum are particularly preferable.
The lanthanoid atom is not particularly limited and may be appropriately selected depending on the intended purpose. , Etc. Among these, neodymium, europium, and gadolinium are preferable.

Examples of the ligand of the complex include G.I. Wilkinson et al., Comprehensive Coordination Chemistry, Pergamon Press, 1987, H.C. Examples include ligands described in Yersin's "Photochemistry and Photophysics of Coordination Compounds" published by Springer-Verlag 1987, Akio Yamamoto "Organic Metal Chemistry-Fundamentals and Applications-" .
Examples of the ligand include a halogen ligand (preferably a chlorine ligand), an aromatic carbocyclic ligand (for example, a cyclopentadienyl anion, a benzene anion, a naphthyl anion, etc.). Preferably 6 to 30 carbon atoms, more preferably 6 to 20 carbon atoms, still more preferably 6 to 12 carbon atoms, and nitrogen-containing heterocyclic ligands (for example, phenylpyridine, benzoquinoline, quinolinol) , Bipyridyl, phenanthroline and the like, preferably having 5 to 30 carbon atoms, more preferably having 6 to 30 carbon atoms, further preferably having 6 to 20 carbon atoms, and particularly preferably having 6 to 12 carbon atoms), a diketone ligand ( For example, acetylacetone etc. are mentioned), carboxylic acid ligands (for example, acetic acid ligand etc. are mentioned, and C2-C30 is preferable. , More preferably 2 to 20 carbon atoms, particularly preferably 2 to 16 carbon atoms), an alcoholate ligand (for example, a phenolate ligand), preferably 1 to 30 carbon atoms, and 1 to 20 carbon atoms. More preferably, C6-C20 is more preferable), silyloxy ligands (for example, trimethylsilyloxy ligand, dimethyl-tert-butylsilyloxy ligand, triphenylsilyloxy ligand, etc., carbon A number 3 to 40 is preferable, a number 3 to 30 is more preferable, a number 3 to 20 is particularly preferable, a carbon monoxide ligand, an isonitrile ligand, a cyano ligand, a phosphorus ligand (for example, A triphenylphosphine ligand, and the like, preferably having 3 to 40 carbon atoms, more preferably 3 to 30 carbon atoms, still more preferably 3 to 20 carbon atoms, and 6 carbon atoms. 20 is particularly preferred), thiolato ligands (for example, phenylthiolato ligands, etc. are mentioned, preferably having 1 to 30 carbon atoms, more preferably 1 to 20 carbon atoms, and further preferably 6 to 20 carbon atoms). Phosphine oxide ligands (for example, triphenylphosphine oxide ligands, etc., preferably having 3 to 30 carbon atoms, more preferably 8 to 30 carbon atoms, and particularly preferably 18 to 30 carbon atoms) Are preferred, and nitrogen-containing heterocyclic ligands are more preferred.
The complex may have one transition metal atom in the compound, or may be a so-called binuclear complex having two or more. Different metal atoms may be contained simultaneously.

  Among these, as the luminescent dopant, for example, US6303238B1, US6097147, WO00 / 57676, WO00 / 70655, WO01 / 08230, WO01 / 39234A2, WO01 / 41512A1, WO02 / 02714A2, WO02 / 15645A1, WO02 / 44189A1, WO05 / 19373A2, JP-A No. 2001-247859, JP-A No. 2002-302671, JP-A No. 2002-117978, JP-A No. 2003-133074, JP-A No. 2002-233502, JP-A No. 2003-123982, JP-A No. 2002-170684, EP No. 121157, JP-A No. 2002-2002 226495, JP 2002-234894, JP 2001-247859, JP 2001-298470, JP 2002-1736 4, JP 2002-203678, JP 2002-203679, JP 2004-357799, JP 2006-256999, JP 2007-19462, JP 2007-84635, JP 2007-96259, etc. And phosphorescent compounds. Among them, Ir complex, Pt complex, Cu complex, Re complex, W complex, Rh complex, Ru complex, Pd complex, Os complex, Eu complex, Tb complex, Gd complex, Dy complex, and Ce complex are preferable, and Ir complex, Pt More preferred are complexes and Re complexes. Among Ir complexes, Pt complexes, and Re complexes, those containing at least one coordination mode of metal-carbon bond, metal-nitrogen bond, metal-oxygen bond, and metal-sulfur bond are preferable, luminous efficiency, driving durability, In view of chromaticity and the like, those containing a tridentate or higher polydentate ligand are more preferable.

  The fluorescent light-emitting dopant is not particularly limited and may be appropriately selected depending on the intended purpose. , Pyran, perinone, oxadiazole, aldazine, pyralidine, cyclopentadiene, bisstyrylanthracene, quinacridone, pyrrolopyridine, thiadiazolopyridine, cyclopentadiene, styrylamine, aromatic dimethylidin compound, condensed polycyclic aromatic compound (anthracene, Phenanthroline, pyrene, perylene, rubrene, pentacene, etc.), 8-quinolinol metal complexes, various metal complexes represented by pyromethene complexes and rare earth complexes, polythiophene Polyphenylene, polyphenylene vinylene polymer compounds such as organosilanes, and derivatives thereof.

  Examples of the luminescent dopant include the following, but are not limited thereto.

  The light-emitting dopant in the organic light-emitting layer is contained in an amount of 0.1% by mass to 50% by mass with respect to the total compound mass generally forming the organic light-emitting layer in the organic light-emitting layer. From the viewpoint of efficiency, the content is preferably 1% by mass to 50% by mass, and more preferably 2% by mass to 40% by mass.

  Although the thickness of an organic light emitting layer is not specifically limited, Usually, it is preferable that it is 2 nm-500 nm, Especially, from a viewpoint of external quantum efficiency, it is more preferable that it is 3 nm-200 nm, and it is 5 nm-100 nm. It is particularly preferred.

  As the host material, a hole-transporting host material having excellent hole-transporting property (may be described as a hole-transporting host) and an electron-transporting host compound having excellent electron-transporting property (described as an electron-transporting host) May be used).

Examples of the hole transporting host in the organic light emitting layer include the following materials.
Pyrrole, indole, carbazole, azaindole, azacarbazole, triazole, oxazole, oxadiazole, pyrazole, imidazole, thiophene, polyarylalkane, pyrazoline, pyrazolone, phenylenediamine, arylamine, amino-substituted chalcone, styrylanthracene, fluorenone, hydrazone , Stilbene, silazane, aromatic tertiary amine compound, styrylamine compound, aromatic dimethylidin compound, porphyrin compound, polysilane compound, poly (N-vinylcarbazole), aniline copolymer, thiophene oligomer, polythiophene, etc. Conductive polymer oligomers, organic silanes, carbon films, derivatives thereof, and the like.
Indole derivatives, carbazole derivatives, aromatic tertiary amine compounds, and thiophene derivatives are preferable, those having a carbazole group in the molecule are more preferable, and compounds having a t-butyl-substituted carbazole group are particularly preferable.

  The electron transporting host in the organic light emitting layer preferably has an electron affinity Ea of 2.5 eV or more and 3.5 eV or less from the viewpoint of improving durability and lowering driving voltage, and is 2.6 eV or more and 3.4 eV or less. More preferably, it is 2.8 eV or more and 3.3 eV or less. Further, from the viewpoint of improving durability and reducing driving voltage, the ionization potential Ip is preferably 5.7 eV or more and 7.5 eV or less, more preferably 5.8 eV or more and 7.0 eV or less, and 5.9 eV or more. It is particularly preferable that it is 6.5 eV or less.

Specific examples of such an electron transporting host include the following materials.
Pyridine, pyrimidine, triazine, imidazole, pyrazole, triazole, oxazole, oxadiazol, fluorenone, anthraquinodimethane, anthrone, diphenylquinone, thiopyran dioxide, carbodiimide, fluorenylidenemethane, distyrylpyrazine, Fluorine-substituted aromatic compounds, heterocyclic tetracarboxylic anhydrides such as naphthalene perylene, phthalocyanines, derivatives thereof (which may form condensed rings with other rings), metal complexes of 8-quinolinol derivatives and metal phthalocyanines And various metal complexes represented by metal complexes having benzoxazole or benzothiazol as a ligand.

As the electron transporting host, metal complexes, azole derivatives (benzimidazole derivatives, imidazopyridine derivatives, etc.), and azine derivatives (pyridine derivatives, pyrimidine derivatives, triazine derivatives, etc.) are preferable. Among them, metal complex compounds are preferred from the viewpoint of durability. Is more preferable. The metal complex compound (A) is more preferably a metal complex having a ligand having at least one of a nitrogen atom, an oxygen atom and a sulfur atom coordinated to the metal.
The metal ion in the metal complex is not particularly limited and can be appropriately selected depending on the purpose, but beryllium ion, magnesium ion, aluminum ion, gallium ion, zinc ion, indium ion, tin ion, platinum ion, or Palladium ions are preferable, beryllium ions, aluminum ions, gallium ions, zinc ions, platinum ions, or palladium ions are more preferable, and aluminum ions, zinc ions, or palladium ions are particularly preferable.

  There are various known ligands contained in the metal complex. For example, “Photochemistry and Photophysics of Coordination Compounds”, Springer-Verlag, H.C. Examples include ligands described in Yersin, published in 1987, “Organometallic Chemistry: Fundamentals and Applications”, Saika Hanafusa, Yamamoto Akio, published in 1982, and the like.

As said ligand, a nitrogen-containing heterocyclic ligand (C1-C30 is preferable, C2-C20 is more preferable, C3-C15 is especially preferable). Further, the ligand may be a monodentate ligand or a bidentate or more ligand, but is preferably a bidentate or more and a hexadentate or less ligand. Also preferred are bidentate to hexadentate ligands and monodentate mixed ligands.
Examples of the ligand include an azine ligand (for example, a pyridine ligand, a bipyridyl ligand, a terpyridine ligand, etc.), a hydroxyphenylazole ligand (for example, hydroxyphenylbenzimidazole). Ligands, hydroxyphenylbenzoxazole ligands, hydroxyphenylimidazole ligands, hydroxyphenylimidazopyridine ligands, etc.), alkoxy ligands (eg, methoxy, ethoxy, butoxy, 2-ethylhexyl). Siloxy etc. are mentioned, C1-C30 is preferable, C1-C20 is more preferable, C1-C10 is especially preferable.), An aryloxy ligand (for example, phenyloxy, 1-naphthyloxy, 2-naphthyloxy, 2,4,6-trimethylphenyloxy, 4- Such as phenyloxy and the like, 6 to 30 carbon atoms, more preferably 6 to 20 carbon atoms, particularly preferably 6 to 12 carbon atoms) and the like.

  Heteroaryloxy ligands (for example, pyridyloxy, pyrazyloxy, pyrimidyloxy, quinolyloxy, etc. are mentioned, preferably having 1 to 30 carbon atoms, more preferably 1 to 20 carbon atoms, and particularly preferably 1 to 12 carbon atoms). Alkylthio ligands (for example, methylthio, ethylthio and the like are mentioned, preferably having 1 to 30 carbon atoms, more preferably having 1 to 20 carbon atoms, and particularly preferably having 1 to 12 carbon atoms), arylthio ligands (for example, Phenylthio etc. are mentioned, C6-C30 is preferable, C6-C20 is more preferable, C6-C12 is especially preferable,) heteroarylthio ligand (for example, pyridylthio, 2-benzimidazole). Ruthio, 2-benzoxazolylthio, 2-benzthiazolylthio and the like, and those having 1 to 30 carbon atoms More preferably, carbon number 1-20 is more preferable, and carbon number 1-12 is particularly preferable.), Siloxy ligand (for example, triphenylsiloxy group, triethoxysiloxy group, triisopropylsiloxy group, etc.) 1-30 are preferable, C3-C25 is more preferable, C6-C20 is particularly preferable, and aromatic hydrocarbon anion ligands (for example, phenyl anion, naphthyl anion, anthranyl anion, etc.). 6 to 30 carbon atoms, more preferably 6 to 25 carbon atoms, and particularly preferably 6 to 20 carbon atoms), an aromatic heterocyclic anion ligand (for example, a pyrrole anion, a pyrazole anion, a pyrazole anion, Triazole anion, oxazole anion, benzoxazole anion, thiazole anion A benzothiazole anion, a thiophene anion, a benzothiophene anion, and the like, preferably having 1 to 30 carbon atoms, more preferably 2 to 25 carbon atoms, and particularly preferably 2 to 20 carbon atoms), an indolenine anion ligand Preferred are nitrogen-containing heterocyclic ligands, aryloxy ligands, heteroaryloxy groups, siloxy ligands, etc., nitrogen-containing heterocyclic ligands, aryloxy ligands, siloxy ligands More preferred are aromatic hydrocarbon anion ligands, aromatic heterocyclic anion ligands, and the like.

  Examples of the metal complex electron transporting host include, for example, Japanese Patent Application Laid-Open No. 2002-235076, Japanese Patent Application Laid-Open No. 2004-214179, Japanese Patent Application Laid-Open No. 2004-221106, Japanese Patent Application Laid-Open No. 2004-221068, Japanese Patent Application Laid-Open No. 2004-227313, etc. And the compounds described in the above.

  In the organic light emitting layer, the triplet lowest excitation level (T1) of the host material is preferably higher than T1 of the phosphorescent light emitting material in terms of color purity, light emission efficiency, and driving durability.

  In addition, the content of the host compound is not particularly limited, but may be 15% by mass or more and 95% by mass or less with respect to the total compound mass forming the light emitting layer from the viewpoint of luminous efficiency and driving voltage. preferable.

----- Hole injection layer, hole transport layer ----
The hole injection layer and the hole transport layer are layers having a function of receiving holes from the anode or the anode side and transporting them to the cathode side. The hole injection material and the hole transport material used for these layers may be a low molecular compound or a high molecular compound.
Specifically, pyrrole derivatives, carbazole derivatives, triazole derivatives, oxazole derivatives, oxadiazole derivatives, imidazole derivatives, polyarylalkane derivatives, pyrazoline derivatives, pyrazolone derivatives, phenylenediamine derivatives, arylamine derivatives, amino-substituted chalcone derivatives, styryl Anthracene derivatives, fluorenone derivatives, hydrazone derivatives, stilbene derivatives, silazane derivatives, aromatic tertiary amine compounds, styrylamine compounds, aromatic dimethylidin compounds, phthalocyanine compounds, porphyrin compounds, thiophene derivatives, organosilane derivatives, carbon, And the like.

  An electron-accepting dopant can be contained in the hole injection layer or the hole transport layer of the organic electroluminescence element. As the electron-accepting dopant introduced into the hole-injecting layer or the hole-transporting layer, an inorganic compound or an organic compound can be used as long as it has an electron-accepting property and oxidizes an organic compound.

  Specific examples of the inorganic compound include metal halides such as ferric chloride, aluminum chloride, gallium chloride, indium chloride, and antimony pentachloride, and metal oxides such as vanadium pentoxide and molybdenum trioxide.

In the case of an organic compound, a compound having a nitro group, halogen, cyano group, trifluoromethyl group or the like as a substituent, a quinone compound, an acid anhydride compound, fullerene, or the like can be preferably used.
In addition, JP-A-6-212153, JP-A-11-111463, JP-A-11-251067, JP-A-2000-196140, JP-A-2000-286054, JP-A-2000-315580, JP-A-2001-102175, JP-A-2001-2001. -160493, JP2002-252085, JP2002-56985, JP2003-157981, JP2003-217862, JP2003-229278, JP2004-342614, JP2005-72012, JP20051666667 , And compounds described in JP-A-2005-209643 can be preferably used.

  Among these, hexacyanobutadiene, hexacyanobenzene, tetracyanoethylene, tetracyanoquinodimethane, tetrafluorotetracyanoquinodimethane, p-fluoranyl, p-chloranil, p-bromanyl, p-benzoquinone, 2,6-dichlorobenzoquinone, 2 , 5-dichlorobenzoquinone, 1,2,4,5-tetracyanobenzene, 1,4-dicyanotetrafluorobenzene, 2,3-dichloro-5,6-dicyanobenzoquinone, p-dinitrobenzene, m-dinitrobenzene, o-dinitrobenzene, 1,4-naphthoquinone, 2,3-dichloronaphthoquinone, 1,3-dinitronaphthalene, 1,5-dinitronaphthalene, 9,10-anthraquinone, 1,3,6,8-tetranitrocarbazole, 2,4,7-trinitro-9- Luenone, 2,3,5,6-tetracyanopyridine and fullerene C60 are preferred, hexacyanobutadiene, hexacyanobenzene, tetracyanoethylene, tetracyanoquinodimethane, tetrafluorotetracyanoquinodimethane, p-fluoranyl, p-chloranil. P-bromanyl, 2,6-dichlorobenzoquinone, 2,5-dichlorobenzoquinone, 2,3-dichloronaphthoquinone, 1,2,4,5-tetracyanobenzene, 2,3-dichloro-5,6-dicyanobenzoquinone 2,3,5,6-tetracyanopyridine is more preferable, and tetrafluorotetracyanoquinodimethane is particularly preferable.

  These electron-accepting dopants may be used alone or in combination of two or more. Although the usage-amount of an electron-accepting dopant changes with kinds of material, it is preferable that it is 0.01 mass%-50 mass% with respect to hole transport layer material, and it is 0.05 mass%-20 mass%. More preferably, it is especially preferable that it is 0.1 mass%-10 mass%.

The thicknesses of the hole injection layer and the hole transport layer are each preferably 500 nm or less from the viewpoint of lowering the driving voltage.
The thickness of the hole transport layer is preferably 1 nm to 500 nm, more preferably 5 nm to 200 nm, and even more preferably 10 nm to 100 nm. In addition, the thickness of the hole injection layer is preferably 0.1 nm to 200 nm, more preferably 0.5 nm to 100 nm, and further preferably 1 nm to 100 nm.
The hole injection layer and the hole transport layer may have a single-layer structure composed of one or more of the materials described above, or may have a multilayer structure composed of a plurality of layers having the same composition or different compositions. .

----- Electron injection layer, electron transport layer ----
The electron injection layer and the electron transport layer are layers having a function of receiving electrons from the cathode or the cathode side and transporting them to the anode side. The electron injection material and the electron transport material used for these layers may be a low molecular compound or a high molecular compound.
Specifically, pyridine derivatives, quinoline derivatives, pyrimidine derivatives, pyrazine derivatives, phthalazine derivatives, phenanthroline derivatives, triazine derivatives, triazole derivatives, oxazole derivatives, oxadiazole derivatives, imidazole derivatives, fluorenone derivatives, anthraquinodimethane derivatives, anthrone Derivatives, diphenylquinone derivatives, thiopyran dioxide derivatives, carbodiimide derivatives, fluorenylidenemethane derivatives, distyrylpyrazine derivatives, naphthalene, perylene and other aromatic ring tetracarboxylic acid anhydrides, phthalocyanine derivatives, 8-quinolinol derivative metal complexes, Metal phthalocyanines, various metal complexes represented by metal complexes with benzoxazole and benzothiazole as ligands, organosilane derivatives represented by siloles Body, it is preferably a layer containing such.

The electron injection layer or the electron transport layer of the organic electroluminescence device of the present invention can contain an electron donating dopant. The electron donating dopant introduced into the electron injecting layer or the electron transporting layer only needs to have an electron donating property and a property of reducing an organic compound, such as an alkali metal such as Li or an alkaline earth metal such as Mg. Transition metals including rare earth metals and reducing organic compounds are preferably used. As the metal, a metal having a work function of 4.2 eV or less can be preferably used. Specifically, Li, Na, K, Be, Mg, Ca, Sr, Ba, Y, Cs, La, Sm, Gd , Yb, and the like. Examples of the reducing organic compound include nitrogen-containing compounds, sulfur-containing compounds, and phosphorus-containing compounds.
In addition, materials described in JP-A-6-212153, JP-A-2000-196140, JP-A-2003-68468, JP-A-2003-229278, JP-A-2004-342614, and the like can be used.

  These electron donating dopants may be used alone or in combination of two or more. The amount of the electron donating dopant varies depending on the type of material, but is preferably 0.1% by mass to 99% by mass, and 1.0% by mass to 80% by mass with respect to the electron transport layer material. Is more preferable, and 2.0 mass% to 70 mass% is particularly preferable.

The thicknesses of the electron injection layer and the electron transport layer are each preferably 500 nm or less from the viewpoint of lowering the driving voltage.
The thickness of the electron transport layer is preferably 1 nm to 500 nm, more preferably 5 nm to 200 nm, and particularly preferably 10 nm to 100 nm. In addition, the thickness of the electron injection layer is preferably 0.1 nm to 200 nm, more preferably 0.2 nm to 100 nm, and particularly preferably 0.5 nm to 50 nm.
The electron injection layer and the electron transport layer may have a single layer structure composed of one or more of the above-described materials, or may have a multilayer structure composed of a plurality of layers having the same composition or different compositions.

---- Hole blocking layer ----
The hole blocking layer is a layer having a function of preventing holes transported from the anode side to the light emitting layer from passing through to the cathode side. As the organic compound layer adjacent to the light emitting layer on the cathode side, a hole blocking layer can be provided.
Examples of the compound constituting the hole blocking layer include aluminum complexes such as BAlq, triazole derivatives, phenanthroline derivatives such as BCP, and the like.
The thickness of the hole blocking layer is preferably 1 nm to 500 nm, more preferably 5 nm to 200 nm, and particularly preferably 10 nm to 100 nm.
The hole blocking layer may have a single layer structure composed of one or more of the above-described materials, or may have a multilayer structure composed of a plurality of layers having the same composition or different compositions.

---- Electron blocking layer ----
The electron blocking layer is a layer having a function of preventing electrons transported from the cathode side to the light emitting layer from passing through to the anode side. In the present invention, an electron blocking layer can be provided as the organic compound layer adjacent to the light emitting layer on the anode side.
As examples of the compound constituting the electron blocking layer, for example, those mentioned as the hole transport material described above can be applied.
The thickness of the electron blocking layer is preferably 1 nm to 500 nm, more preferably 5 nm to 200 nm, and particularly preferably 10 nm to 100 nm.
The hole blocking layer may have a single layer structure composed of one or more of the above-described materials, or may have a multilayer structure composed of a plurality of layers having the same composition or different compositions.

-Diffraction grating structure formation process-
The diffraction grating structure forming step is a step of forming a diffraction grating structure by forming a diffraction grating on a transparent substrate.

--Diffraction grating structure--
The diffraction grating structure includes at least a transparent substrate and a diffraction grating, and further includes other members as necessary.

---- Transparent substrate ---
The transparent substrate is not particularly limited as long as it is a substrate capable of transmitting visible light, and can be appropriately selected according to the purpose.
There is no restriction | limiting in particular about the shape of the said transparent base material, a structure, a magnitude | size, According to the objective, it can select suitably. In general, the shape of the transparent substrate is preferably a plate shape. The structure of the transparent substrate may be a single layer structure or a laminated structure, may be formed of a single member, or may be formed of two or more members. Also good.
The material of the transparent substrate is not particularly limited and may be appropriately selected depending on the purpose. For example, a transparent inorganic material such as silicon oxide, a transparent resin such as an acrylic resin, a novolac resin, or a polyimide resin. Is mentioned.
There is no restriction | limiting in particular as thickness of the said transparent base material, Although it can select suitably according to the objective, It is necessary to have the thickness which has sufficient barrier property.
There is no restriction | limiting in particular as a refractive index of the said transparent base material, According to the objective, it can select suitably.

---- Diffraction grating ---
The diffraction grating is not particularly limited as long as it functions as a diffraction grating, and can be appropriately selected depending on the purpose. For example, the concavo-convex pattern formed on the transparent substrate, formed on the transparent substrate. And a diffraction grating film.
The pitch P of the convex portions in the concave / convex pattern (the distance from the central point of the convex portion to the central point of the adjacent convex portion (P in FIG. 1)) is not particularly limited and is appropriately selected according to the purpose. However, it is preferably 200 nm to 2,000 nm.
If the pitch P is less than 200 nm, it may not function as a diffraction grating. If the pitch P exceeds 2,000 nm, a sufficient diffraction angle cannot be obtained, and diffracted light is taken out of the organic electroluminescence element. May not contribute to improving the light extraction efficiency.
There is no restriction | limiting in particular as the height H of the convex part in the said uneven | corrugated pattern, Although it can select suitably according to the objective, 100 nm or more is preferable.
If the height H of the convex portion is less than 100 nm, sufficient diffraction efficiency may not be obtained.
There is no restriction | limiting in particular as a formation method of the said uneven | corrugated pattern, According to the objective, it can select suitably, For example, the method of patterning the said transparent base material etc. are mentioned.
The patterning can be performed, for example, by forming a mask pattern on the transparent substrate and etching the transparent substrate using the mask pattern as an etching mask. The mask pattern can be formed using, for example, photolithography, nanoimprint, or the like.
The refractive index of the diffraction grating is not particularly limited and may be appropriately selected depending on the purpose. It is preferable that the refractive difference between the diffraction grating surface and the refractive index of the adjacent adhesive is 0.1 or more. .
If the refractive index difference between the diffraction grating and the adjacent adhesive is less than 0.1, sufficient diffraction efficiency may not be obtained.

-Adhesion process-
The bonding step is a step in which the organic electroluminescence element and the diffraction grating structure are opposed to each other and the organic electroluminescence element and the diffraction grating structure are bonded by an adhesive layer.
Thus, the organic electroluminescence element and the diffraction grating structure are separately manufactured, and then the organic electroluminescence element is damaged by bonding the organic electroluminescence element and the diffraction grating structure. The diffraction gratings can be arranged close to each other without giving them.

-Adhesive layer-
The adhesive layer includes at least an adhesive, inorganic fine particles, and, if necessary, other components.
The adhesive is not particularly limited as long as the organic electroluminescence element and the diffraction grating structure can be bonded, and can be appropriately selected according to the purpose. For example, an acrylic resin, a novolac resin, Examples thereof include a polyimide resin.
The inorganic fine particles are not particularly limited as long as the refractive index of the adhesive layer can be improved, and can be appropriately selected according to the purpose. For example, titanium oxide (TiOx), zirconium oxide (ZrOx) , Silicon nitride, ITO (indium tin oxide), IZO (indium zinc oxide), and the like.
The thickness of the adhesive layer is preferably as thin as possible because the light extraction efficiency can be improved by reducing the distance between the diffraction grating and the organic electroluminescence element, and specifically, 1 μm or less. preferable.
The refractive index of the adhesive layer is not particularly limited as long as it is different from the refractive index of the diffraction grating, and can be appropriately selected according to the purpose, but the refractive index difference from the diffraction grating is 0.1 or more. Preferably there is.
If the difference in refractive index between the adhesive layer and the diffraction grating is less than 0.1, sufficient diffraction efficiency may not be obtained.

-Sealing layer lamination process-
The sealing layer stacking step is a step of stacking a sealing layer on the organic electroluminescence element.
The sealing layer is not particularly limited as long as it protects the organic electroluminescence element, and can be appropriately selected according to the purpose.
The material contained in the sealing layer may be any material that has a function of suppressing the entry of elements that promote element deterioration such as moisture and oxygen into the element. Specific examples thereof include In , Sn, Pb, Au, Cu , Ag, Al, Ti, a metal such as _{Ni, MgO, SiO, SiO 2,} Al 2 O 3, GeO, NiO, CaO, BaO, Fe 2 O 3, Y 2 O 3, Metal oxides such as TiO ₂ , metal nitrides such as SiNx, SiNxOy, metal fluorides such as MgF ₂ , LiF, AlF ₃ , CaF ₂ , polyethylene, polypropylene, polymethyl methacrylate, polyimide, polyurea, polytetrafluoroethylene, Polychlorotrifluoroethylene, polydichlorodifluoroethylene, chlorotrifluoroethylene and dichlorodifluoroethylene Polymer, copolymer obtained by copolymerizing monomer mixture containing tetrafluoroethylene and at least one comonomer, fluorine-containing copolymer having a cyclic structure in the copolymer main chain, water absorption of 1% or more And a moisture-proof substance having a water absorption rate of 0.1% or less.

  There is no restriction | limiting in particular about the formation method of the said sealing layer, According to the objective, it can select suitably, For example, a vacuum evaporation method, sputtering method, reactive sputtering method, MBE (molecular beam epitaxy) method, cluster ion Beam method, ion plating method, plasma polymerization method (high frequency excitation ion plating method), plasma CVD method, laser CVD method, thermal CVD method, gas source CVD method, coating method, printing method, transfer method, etc. .

There is no restriction | limiting in particular as thickness of the said sealing layer, According to the objective, it can select suitably.
There is no restriction | limiting in particular as a refractive index of the said sealing layer, According to the objective, it can select suitably.

-Circularly polarizing member formation process-
The circularly polarizing member forming step is a step of forming or adhering a circularly polarizing member between the transparent substrate and the diffraction grating, or on the surface of the transparent substrate opposite to the surface on which the diffraction grating is formed. .
The circularly polarizing member can be formed by bonding, adhering, or laminating a polarizing plate and a quarter wavelength plate.
There is no restriction | limiting in particular as thickness of the said circularly-polarizing member, According to the objective, it can select suitably.
There is no restriction | limiting in particular as a refractive index of the said circularly-polarizing member, According to the objective, it can select suitably.
In addition, when the transparent base material is a barrier film, forming the circularly polarizing member impairs the function of the circularly polarizing member. Therefore, when the transparent base material is other than the barrier film, the circularly polarized light is used. Form a member.

-Color filter member formation process-
The color filter member forming step is a step of forming a color filter member between the transparent substrate and the diffraction grating, or on the surface of the transparent substrate opposite to the surface on which the diffraction grating is formed.
There is no restriction | limiting in particular as said color filter member, According to the objective, it can select suitably, For example, a pigment-type color filter, a dye-type color filter, etc. are mentioned.
There is no restriction | limiting in particular about the formation method of the said color filter member, According to the objective, it can select suitably, For example, the inkjet method, the printing method, the laser transfer method etc. are mentioned.
There is no restriction | limiting in particular as thickness of the said color filter member, According to the objective, it can select suitably.
There is no restriction | limiting in particular as a refractive index of the said color filter member, According to the objective, it can select suitably.
Further, a black matrix may be formed on both side surfaces of the color filter member.

  A first embodiment of an organic electroluminescent light emitting device manufactured by the method of manufacturing an organic electroluminescent light emitting device of the present invention includes, for example, a glass substrate 1 (refractive index: about 1.5) as shown in FIG. And a passivation layer 2 made of SiNx, SiON or the like, disposed on the glass substrate 1, disposed on the passivation layer 2, and on the planarization layer 3 and on the passivation layer 2 and adjacent to the planarization layer 3. An organic thin film transistor (TFT) 4 disposed, an ITO layer 5 disposed on the planarizing layer 3, a reflective electrode (anode) 6 made of Al, Ag, etc., and a reflective electrode (anode) 6 are disposed, An organic compound layer 7 (refractive index: about 1.8) including a light emitting layer, a counter electrode (semi-transmissive cathode) 8 made of Ag, Mg—Ag, etc., disposed on the organic compound layer 7; A bank 9 made of an acrylic resin and the like, and disposed opposite the reflective electrode (anode) 6, the organic compound layer 7 and the counter electrode (semi-transmissive cathode) 8. A sealing layer 10 (refractive index: about 1.75) disposed on the cathode 8 and made of SiNx, SiON, or the like; and an adhesive layer 11 (refractive index) made of epoxy resin or the like disposed on the sealing layer 10. : About 1.72), a transparent substrate 12 (refractive index: about 1.5) disposed on the adhesive layer 11 and made of glass or the like, and a diffraction grating provided on the adhesive layer 11 side of the transparent substrate 12 As a plurality of convex portions 13 (refractive index: about 1.5) and a circularly polarizing member 14 disposed on the surface of the transparent substrate 12 opposite to the surface on which the convex portions 13 are formed.

  A second embodiment of the organic electroluminescence light-emitting device manufactured by the method for manufacturing an organic electroluminescence light-emitting device of the present invention includes, for example, a glass substrate 1 (refractive index: about 1.5) as shown in FIG. And a passivation layer 2 made of SiNx, SiON, etc., a planarizing layer 3 arranged on the passivation layer 2, and a position on the passivation layer 2 adjacent to the planarizing layer 3. An organic thin film transistor (TFT) 4 disposed, an ITO layer 5 disposed on the planarizing layer 3, a reflective electrode (anode) 6 made of Al, Ag, etc., and a reflective electrode (anode) 6 are disposed, An organic compound layer 7 (refractive index: about 1.8) including a light emitting layer, a counter electrode (semi-transmissive cathode) 8 made of Ag, Mg—Ag, etc., disposed on the organic compound layer 7; A bank 9 made of an acrylic resin and the like, and disposed opposite the reflective electrode (anode) 6, the organic compound layer 7 and the counter electrode (semi-transmissive cathode) 8. A sealing layer 10 (refractive index: about 1.75) disposed on the cathode 8 and made of SiNx, SiON, or the like; and an adhesive layer 11 (refractive index) made of epoxy resin or the like disposed on the sealing layer 10. : About 1.72), disposed on the adhesive layer 11, provided on the transparent substrate 12 (refractive index: about 1.5) made of glass, a barrier film, and the like on the adhesive layer 11 side of the transparent substrate 12. A plurality of convex portions 13 (refractive index: about 1.5) as a diffraction grating, a color filter 15 (refractive index: about 1.5) disposed between the convex portion 13 and the transparent substrate 12, and a color Black matrix formed on both sides of filter 15 And a 16.

Examples of the present invention will be described below, but the present invention is not limited to the following examples.
Example 1

<Preparation of organic electroluminescence element>
A buffer layer 32 made of a SiO ₂ film is formed on a glass substrate as the insulating substrate 31 by a CVD method, and then a polycrystalline silicon layer is deposited by the CVD method, and then island-shaped using a normal photoetching process. A polycrystalline silicon layer 33 was formed (FIG. 3A).
Next, after depositing a SiO ₂ film on the entire surface by CVD, an AlNd film is deposited by sputtering, and then the SiO ₂ film and AlNd film are patterned using a normal photoetching process to form the gate insulating film 34 and A gate electrode 35 was formed (FIG. 3B).
Next, using the gate electrode 35 as a mask, for example, phosphorus ions are ion-implanted by an ion implantation method to form the source region 36 and the drain region 37 in the island-like polycrystalline silicon layer 33 on both sides of the gate electrode 35, and the rest This portion was used as the channel layer 38 (FIG. 3C).
Next, an interlayer insulating film 39 made of a SiN film is deposited on the entire surface by using the CVD method, and then contact holes 40 and 41 reaching the source region 36 and the drain region 37 are formed by using a normal photoetching process (see FIG. FIG. 3D).
Next, after depositing an Al / Ti / Al multilayer conductive layer on the entire surface, patterning is performed using a normal photoetching process to form the source electrode 42 and the drain electrode 45, and the TFT substrate for organic electroluminescence is formed. It produced (FIG. 4). The prepared polyimide solution is applied on the produced TFT substrate for organic electroluminescence to form a planarization layer, and a contact hole (for connecting an organic thin film transistor (TFT) and an ITO layer to be described later) is connected to the planarization layer. After that, ITO was vapor-deposited to form an ITO layer with a thickness of 100 nm, and a reflective electrode with a thickness of 100 nm made of Al was formed on the ITO layer.
Further, an organic compound layer (a hole injection layer, a hole transport layer, a light emitting layer, and an electron injection layer) was sequentially formed on the reflective electrode. First, as a hole injection layer, 2-TNATA [4,4 ′, 4 ″ -tris (2-naphthylphenylamino) triphenylamine] was formed by vapor deposition to a thickness of 50 nm. Furthermore, α-NPD [N, N ′-(dinaphthylphenylamino) pyrene] was formed by vapor deposition as a hole transport layer to a thickness of 50 nm. Furthermore, Alq3 [8-quinolinol aluminum complex] was formed as a light emitting layer by vapor deposition to a thickness of 50 nm. Finally, as an electron injection layer, a pyridine derivative was formed by vapor deposition to a thickness of 25 nm.
Thereafter, a semi-transmissive cathode (Al electrode, Ag electrode) was sequentially formed by vapor deposition.
First, as an Al electrode, aluminum was formed by vapor deposition to a thickness of 100 nm. Furthermore, silver was formed by vapor deposition to a thickness of 100 nm.
Furthermore, SiON was formed into a film by vapor deposition to form a 25 μm-thick sealing layer, and an organic electroluminescence element was produced.

<Production of diffraction grating structure>
By performing the following operations, an uneven pattern (convex pitch P: 700 nm, convex height H: 400 nm, refractive index: about 1.5) is formed on one surface of the glass substrate, and the diffraction grating structure is formed. Produced.

<< Formation of uneven pattern >>
For the concave / convex pattern, first, an Al film was formed by sputtering on a glass substrate, and a photoresist was applied on the formed Al film, followed by drying, pattern exposure, development, washing, and drying to form a glass etching pattern. Thereafter, the glass substrate on which the etching pattern by the Al film was formed was subjected to reactive ion etching to form a diffraction grating corresponding to the etching pattern on the glass substrate.

<Production of organic electroluminescence light emitting device>
An adhesive layer composition for acrylate optical path coupling (manufactured by NTT Advanced Technology) is applied on the sealing layer in the produced organic electroluminescence element so that the concavo-convex pattern is on the organic electroluminescence element side. And an adhesive layer (refractive index: about 1.72) was formed by irradiating with UV light for 10 minutes, and the diffraction grating structure and the organic electroluminescence element were adhered.

(Example 2)
In Example 1, instead of forming a concavo-convex pattern on one surface of a glass substrate and producing a diffraction grating structure, a concavo-convex pattern is formed on one surface of the glass substrate, and the other surface of the glass substrate is formed. An organic electroluminescence light-emitting device was produced in the same manner as in Example 1 except that the circularly polarizing plate was bonded with a UV curable resin to produce a diffraction grating structure.

(Example 3)
In Example 1, instead of forming a concavo-convex pattern on one surface of a glass substrate to produce a diffraction grating structure, a color filter is formed at the center of one surface of the glass substrate, and both sides of the color filter are formed. A black matrix is formed on the surface, and a concavo-convex pattern (protrusion pitch P: 700 nm, convex height H: 400 nm, refractive index: about 1.5) is formed on the color filter as follows. An organic electroluminescence light-emitting device was produced in the same manner as in Example 1 except that the diffraction grating structure was produced.
<< Formation of uneven pattern >>
A transparent resin having a refractive index of 1.5 was applied on the color filter, and further a photoresist was applied, dried, pattern sensitive, developed, washed with water, and dried to form an uneven pattern.

Example 4
In Example 1, instead of forming a concavo-convex pattern on one surface of the glass substrate to produce a diffraction grating structure, a circularly polarizing plate is adhered to one surface of the glass substrate with a UV curable resin, Except that a concavo-convex pattern (protrusion pitch P: 700 nm, convex height H: 400 nm, refractive index: about 1.5) was formed as follows on the polarizing plate to produce a diffraction grating structure. In the same manner as in Example 1, an organic electroluminescence light emitting device was produced.
<< Formation of uneven pattern >>
For the concave / convex pattern, first, an Al film was formed by sputtering on a circularly polarizing plate, and a photoresist was applied on the formed Al film, followed by drying, pattern exposure, development, washing, and drying to form a glass etching pattern. Thereafter, the circularly polarizing plate on which the etching pattern of the Al film was formed was reactive ion etched to form a diffraction grating corresponding to the etching pattern on the circularly polarizing plate.

(Example 5)
In Example 1, instead of forming a concavo-convex pattern on one surface of a glass substrate and producing a diffraction grating structure, a concavo-convex pattern is formed on one surface of the glass substrate, and the other surface of the glass substrate is formed. An organic electroluminescence light-emitting device was produced in the same manner as in Example 1 except that a color filter was formed and a black matrix was formed on both sides of the color filter to produce a diffraction grating structure.

  The organic electroluminescent light emitting device of the present invention is an organic electroluminescent light emitting device in which a diffraction grating is disposed in the vicinity of an organic electroluminescent element to improve light extraction efficiency. In the organic electroluminescent light emitting device, any chemical process or physical process is provided in the vicinity of the organic light emitting layer. Therefore, the reliability of the organic electroluminescent element can be improved by arranging the diffraction grating in the vicinity of the organic light emitting layer only by adhesion without causing any damage to the element. Is suitably used as a light emitting device.

1 Glass substrate 2 Passivation layer 3 Flattening layer 4 Organic thin film transistor (TFT)
5 ITO layer 6 Reflective electrode (anode)
7 Organic compound layer 8 Counter electrode (semi-transmissive cathode)
9 Bank 10 Sealing layer 11 Adhesive layer 12 Transparent substrate 13 Protruding portion 14 Circular polarization member 15 Color filter 16 Black matrix 31 Insulating substrate 32 Buffer layer 33 Island-like polycrystalline silicon layer 34 Gate insulating film 35 Gate electrode 36 Source region 37 Drain region 38 Channel layer 39 Interlayer insulating film 40 Contact hole 41 Contact hole 42 Source electrode 45 Drain electrode

Claims (8)

On the substrate, a reflective electrode, an organic light emitting layer, and an electrode are laminated in this order to form an organic electroluminescent element, and an organic electroluminescent element forming step;
Forming a diffraction grating on a transparent substrate, and forming a diffraction grating structure; and
An adhesion step in which the organic electroluminescence element and the diffraction grating structure are opposed to each other and the organic electroluminescence element and the diffraction grating structure are adhered by an adhesive layer having a refractive index different from that of the diffraction grating. A method for manufacturing an organic electroluminescence light-emitting device.   The method for producing an organic electroluminescence light-emitting device according to claim 1, wherein the refractive index of the adhesive layer is larger than the refractive index of the diffraction grating.   The method for producing an organic electroluminescence light-emitting device according to claim 2, wherein inorganic fine particles are dispersed in the adhesive layer.   The manufacturing method of the organic electroluminescent light-emitting device in any one of Claim 1 to 3 which further includes the sealing layer lamination process which laminates | stacks a sealing layer on an organic electroluminescent element.   The manufacturing method of the organic electroluminescent light-emitting device in any one of Claim 1 to 4 which further includes the circularly-polarizing member formation process which forms a circularly-polarizing member between a transparent base material and a diffraction grating.   The organic electroluminescence light-emitting device according to any one of claims 1 to 4, further comprising a circularly polarizing member forming step of forming a circularly polarizing member on a surface opposite to the surface on which the diffraction grating of the transparent substrate is formed. Manufacturing method.   The manufacturing method of the organic electroluminescent light-emitting device according to any one of claims 1 to 6, further comprising a color filter member forming step of forming a color filter member between the transparent substrate and the diffraction grating. The organic electroluminescence light-emitting device according to claim 1, further comprising a color filter member forming step of forming a color filter member on a surface opposite to the surface on which the diffraction grating of the transparent substrate is formed. Manufacturing method.