WO2009098793A1 - Dispositif d'affichage électroluminescent organique et son procédé de fabrication - Google Patents

Dispositif d'affichage électroluminescent organique et son procédé de fabrication Download PDF

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Publication number
WO2009098793A1
WO2009098793A1 PCT/JP2008/064308 JP2008064308W WO2009098793A1 WO 2009098793 A1 WO2009098793 A1 WO 2009098793A1 JP 2008064308 W JP2008064308 W JP 2008064308W WO 2009098793 A1 WO2009098793 A1 WO 2009098793A1
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layer
organic
substrate
display
color conversion
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PCT/JP2008/064308
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English (en)
Japanese (ja)
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Kouki Kasai
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Fuji Electric Holdings Co., Ltd.
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Priority to TW098103684A priority Critical patent/TW201002123A/zh
Publication of WO2009098793A1 publication Critical patent/WO2009098793A1/fr

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    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05B—ELECTRIC HEATING; ELECTRIC LIGHT SOURCES NOT OTHERWISE PROVIDED FOR; CIRCUIT ARRANGEMENTS FOR ELECTRIC LIGHT SOURCES, IN GENERAL
    • H05B33/00—Electroluminescent light sources
    • H05B33/10—Apparatus or processes specially adapted to the manufacture of electroluminescent light sources
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K59/00—Integrated devices, or assemblies of multiple devices, comprising at least one organic light-emitting element covered by group H10K50/00
    • H10K59/30—Devices specially adapted for multicolour light emission
    • H10K59/38—Devices specially adapted for multicolour light emission comprising colour filters or colour changing media [CCM]

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  • the present invention relates to an organic electroluminescence display (hereinafter also referred to as “organic EL display”). More specifically, the organic EL display according to the present invention relates to an organic EL display in which light emitted from the organic EL element portion to the outside does not exhibit a different emission color depending on a viewing angle. The present invention relates to a method for manufacturing such an organic EL display.
  • display devices such as liquid crystal displays and organic EL displays are used as display units for electronic devices such as mobile phones, personal computers, digital copiers, and printers.
  • the light emitting form of the display device includes a self light emitting type and a non-light emitting type.
  • the self-luminous type is applied to an electroluminescence element (EL element), a field emission display (FED), a cathode ray tube (CRT), and the like.
  • the non-light emitting type is applied to a liquid crystal display element or the like.
  • the color display method of the display device includes a multi-color method or a full-color method that realizes light emission of three primary colors of red, green, and blue.
  • a means for interposing a color filter layer between the light exit surface of the light emitting element and the image surface is frequently used. According to this means, it is possible to selectively emit light of a specific wavelength from the light emitting element and improve the color purity of light emission of the three primary colors, thereby improving the image display quality.
  • Patent Document 1 discloses an organic EL element portion having an organic EL material portion and a fluorescent material portion that absorbs light emitted from the organic EL material portion and emits visible light fluorescence. This element is equipped with a color conversion filter containing a fluorescent material in the fluorescent material part, so that the light emitted from the organic EL material part is absorbed by the fluorescent material part to emit fluorescence in the visible light range, thereby realizing a color conversion method. To do.
  • the light emission color of the organic EL element portion is not limited to white.
  • an organic EL element part having higher luminance than conventional ones can be applied as a light source.
  • blue light is wavelength-converted into green light or red light by a color conversion method using a blue light emitting organic EL element part. Can do.
  • the color conversion layer (corresponding to the fluorescent material part) used in the color conversion method can be formed mainly by a wet process using a photoresist or a dry process using a vapor deposition method.
  • the material used for the color conversion layer has low heat resistance, it is difficult to completely dry the color conversion layer and the photoresist when a wet process is employed. For this reason, according to the wet process, moisture remaining after drying may move from the color conversion layer to the organic EL layer, and a non-luminous defect called a dark area may occur in the organic EL layer. Therefore, the color conversion layer is actively formed not by a wet process but by a dry process. For example, the following techniques have been proposed.
  • Patent Document 2 a color filter layer, a fluorescence conversion layer (corresponding to a color conversion layer), a barrier layer, a hole injection electrode, and an electron injection electrode are provided on a substrate, and an organic layer involved in a light emitting function is provided between the electrodes.
  • An organic EL display device having a color filter layer formed by a vapor deposition method is disclosed.
  • the color filter layer not only the color filter layer but also the color conversion layer is formed by a vapor deposition method (dry process). This is because the color conversion layer is weak against moisture and it is desired to suppress the occurrence of the dark area.
  • the color conversion layer is formed by a dry process and the color filter layer or the flattening layer that is the base of the color conversion layer is formed by a wet process, the color conversion is performed after these are completely dried at a high temperature. It is desirable to form a layer.
  • the color conversion layer can be selectively formed on the flattening layer according to the red, green, and blue subpixels. Since the refractive index of the planarization layer and the glass substrate is about 1.5, whereas the refractive index of the color conversion layer is about 2, the sub-pixel formed with the color conversion layer does not form the color conversion layer. Compared with sub-pixels, light directivity is low. For example, when the color conversion layer is formed only on the red sub-pixel, the red sub-pixel has lower light directivity than the green sub-pixel and the blue sub-pixel.
  • the refractive index between the color conversion layers of the respective colors is different, so that there is a difference in the light directivity between the sub-pixels on which the color conversion layers are formed. For example, when a color conversion layer is formed on a red subpixel and a green subpixel, a difference regarding the directivity of light occurs between these subpixels.
  • red, green, and blue light emitted from the display may have different directivities, and the emission color of the screen may be different depending on the viewing angle with respect to the display.
  • the refractive index of the planarization layer and / or the glass substrate In order to increase the amount of light extracted from the sub-pixel, it is important to reduce the refractive index of the planarization layer and / or the glass substrate. However, when the refractive index of the flattening layer or the like is reduced, the difference in refractive index between the flattening layer or the like and the color conversion layer increases. For this reason, the difference in the directivity of light between the subpixel in which the color conversion layer is formed and the subpixel in which the color conversion layer is not formed is further increased, and the emission color of the screen may be further different depending on the viewing angle.
  • Patent Document 3 includes a pixel having a light emitting functional layer sandwiched between a first electrode and a second electrode on a substrate and a unit pixel group including a plurality of the pixels, and is selected from the unit pixel group.
  • an organic electroluminescence device is disclosed in which each pixel is provided with a scattering portion that scatters light emitted from the light emitting functional layer.
  • Patent Document 3 since the unevenness in Patent Document 3 is formed under the same dimensional design in the blue subpixel and the green subpixel, the difference in the directivity of light between subpixels that generate light of different colors is finely adjusted. Therefore, it is impossible to prevent a change in emission color due to the viewing angle at a high level.
  • the change in the emission color depending on the viewing angle is caused by the occurrence of different directivities in the red, green, and blue light emitted by the color conversion layer.
  • the red directivity is small, while the green and blue directivities are large. Therefore, the above problem can be solved if the difference in directivity of light between red, green, and blue can be reduced.
  • the object of the present invention is to reduce the difference in the directivity of light between the sub-pixels of each color without adversely affecting the color purity and brightness of the light of each color generated from the color conversion layer, and depending on the viewing angle.
  • An object of the present invention is to provide an organic EL display that does not exhibit different emission colors.
  • the objective of this invention is providing the manufacturing method of the said organic EL display.
  • the present invention includes a substrate, a color conversion filter unit including a planarization layer and at least one color conversion layer, and an organic EL element unit having a plurality of light emitting units, and a plurality of subpixels by the plurality of light emitting units. And an interface having a concavo-convex shape between the substrate and the planarizing layer, and the concavo-convex shape relates to an organic EL display having a different concavo-convex density for each sub-pixel.
  • the organic EL display of the present invention can be used as a display unit of an electronic device such as a mobile phone.
  • the present invention also includes a substrate, a first laminate including a color conversion filter unit including a planarization layer and at least one color conversion layer, a base, and an organic EL element unit having a plurality of light emitting units.
  • a plurality of sub-pixels are defined by the plurality of light emitting portions, an interface having a concavo-convex shape between the substrate and the planarization layer, and the concavo-convex shape is
  • An organic EL display having different uneven density is included for each subpixel.
  • At least one color filter layer can be interposed between the substrate and the planarizing layer.
  • the interface between the substrate and the color filter layer has an uneven shape, and the uneven shape has a different uneven density for each sub-pixel.
  • the concavo-convex shape can be an array shape of a plurality of concave portions and convex portions having at least one period and smaller than the sub-pixel width.
  • corrugated shape can be made into the shape which has a different period for every said subpixel.
  • the present invention provides a step of forming a color conversion filter portion including a planarization layer and at least one color conversion layer on a substrate, and an organic EL element portion having a plurality of light emitting portions on the color conversion filter portion.
  • a concavo-convex shape is formed on a substrate surface in contact with the planarization layer, and the concavo-convex shape is formed for each sub-pixel.
  • corrugated density is included.
  • the present invention also includes a step of forming a color conversion filter portion including a planarization layer and at least one color conversion layer on a substrate to obtain a first laminate, and an organic having a plurality of light emitting portions on a substrate.
  • an organic EL display manufacturing method is provided in which an uneven shape is formed on a substrate surface in contact with the planarization layer, and the uneven shape is adjusted to a different uneven density for each subpixel. Include.
  • At least one color filter layer can be formed between the substrate and the planarization layer.
  • an uneven shape is formed on the substrate surface in contact with the color filter layer, and the uneven shape is adjusted to a different uneven density for each sub-pixel.
  • the concavo-convex shape can be adjusted to at least one cycle to form an array shape of a plurality of concave portions and convex portions smaller than the sub-pixel width.
  • corrugated shape can be adjusted to a different period for every said subpixel.
  • the organic EL display of the present invention finely adjusts the directivity of light between sub-pixels of different colors by forming the substrate surface into a predetermined shape for each sub-pixel defined by the light emitting unit of the organic EL element unit. In addition, it is possible to prevent a change in emission color due to the viewing angle at a high level.
  • FIG. 1 is a side sectional view showing an organic EL display of the present invention.
  • FIG. 2 is a side sectional view showing the organic EL display of the present invention.
  • FIG. 3 is a side sectional view showing the organic EL display of Comparative Example 1.
  • FIG. 4 is a side sectional view showing the organic EL display of Comparative Example 2.
  • uneven portions having different densities are formed for different subpixels.
  • the light of R, G, B emitted from the organic EL element part is allowed to pass through the uneven part.
  • the directivity of light of each color at the interface is controlled independently by the principle of light scattering, the difference in directivity of light of each color is reduced, and the emission color changes depending on the angle at which the organic EL display is viewed. Can solve the problem.
  • this inventor observed the organic EL display from the front and the diagonal direction, and measured the angular distribution of the emission spectrum. As a result, it has been concluded that the reduction of the directivity difference in the light of each color can be realized while maintaining the performance of the organic EL element part such as chromaticity and luminance.
  • the organic EL display (bottom emission type) of the present invention includes a transparent substrate 100, a color conversion filter unit 200 laminated on one surface of the transparent substrate 100, and light incident on the color conversion filter unit 200.
  • the organic EL element unit 300 having the light-emitting surface facing the surface, and a sealing material (not shown) that blocks the color conversion filter unit 200 and the organic EL element unit 300 from outside air.
  • the transparent substrate 100 is a layer for supporting each component of the organic EL display sequentially formed thereon.
  • the transparent substrate 100 is rich in light transmission, and the color filter layer 210 (R, G, B), the light shielding layer 220, a red conversion layer 240 described later, and the organic EL element unit 300 (electrode, organic light emitting layer, etc.) ) That can withstand the conditions (solvent, temperature, etc.) used in the formation of).
  • the transparent substrate 100 is preferably excellent in dimensional stability because it is exposed to repeated formation conditions of each layer in each subsequent forming step. Further, it is important to use a transparent substrate 100 that does not cause a decrease in the light emission performance of the multicolor light emitting display, and examples thereof include glass, various plastics, and various films.
  • the color conversion filter unit 200 is a color filter including red (R), green (G), and blue (B) color filter layers 210R, 210G, and 210B formed in a stripe shape on one surface of the transparent substrate 100.
  • a red conversion layer 240 formed at a position corresponding to the color filter layer 210R, and a gas barrier layer 250 formed on the planarization layer 230 so as to wrap the red conversion layer 240.
  • the organic EL element unit 300 is formed on the gas barrier layer 250 and formed on the gas barrier layer 250 so as to wrap around the transparent electrode 310 formed at a position corresponding to the color filter layer 210. And an organic EL layer 320 and a reflective electrode 330 formed on the organic EL layer 320.
  • At least one color filter layer (green color filter layer 210G and blue color filter layer 210B in the example shown in FIG. 1) selected from the color filter layers 210R, 210G, and 210B of each color,
  • the interface with the transparent substrate 100 in contact has an uneven shape.
  • the uneven shape of the interface (interface 1) between the green color filter layer 210G and the transparent substrate 100 and the uneven shape of the interface (interface 2) between the blue color filter layer 210B and the transparent substrate 100 are reflected at the interface of incident external light. And a shape that can enhance the amount of light outside the incident to the organic EL element unit 300 due to refraction.
  • the uneven shape is a shape that allows the emitted light from the organic EL element unit 300 to be sufficiently scattered and emitted to the image plane.
  • the average depth of the valley is 0.4 to 0.625 ⁇ m.
  • the average depth of the valley is the vertical direction of the paper surface of the concave portion adjacent to the position of the vertical direction of the paper surface in each interface shape between each color filter layer 210 (G, B) and the transparent substrate 100 in FIG.
  • the difference from the position means an average value obtained by measuring one representative position in the entire horizontal region of each color filter layer 210 (G, B).
  • the depth is preferably 0.525 to 0.625 ⁇ m.
  • the uneven shape of the interfaces 1 and 2 has an uneven density of 0.83 to 1.99 / ⁇ m 2 .
  • the uneven density is the number of protrusions per 1 ⁇ m 2 in the shape of the interface between the green color filter layer 210G or the blue color filter layer 210B and the transparent substrate 100 (horizontal direction in FIG. 1 ⁇ vertical direction in FIG. 1). It means number.
  • the uneven density is preferably 0.83 to 1.18 / ⁇ m 2 .
  • the uneven shape of the interfaces 1 and 2 can be a regular or irregular shape having such an average depth of the valley and uneven density. By not excessively increasing the average depth or average density of the valleys, it is possible to suppress excessive irregular reflection of incident external light and to prevent luminance loss of the light emitting surface.
  • Such a concavo-convex shape has a different concavo-convex density for each sub-pixel (in the example shown in FIG. 1, for each of the green color filter layer 210G and the blue color filter layer 210B). This is to prevent a change in emission color due to the viewing angle at a high level by utilizing the directivity of light based on the principle of scattering.
  • the concave / convex shape is determined with a period of 1 ⁇ 2 or more of the wavelength of the light to be changed, thereby adjusting the concave / convex density, and changing the refractive index for each sub-pixel to direct the light emitted from each sub-pixel. Adjust gender.
  • FIG. 1 1 ⁇ 2 or more of the wavelength of the light to be changed
  • the period of the concavo-convex shape refers to a horizontal distance in the drawing between adjacent convex portions in each color filter layer 210 (G, B).
  • the unevenness density of the uneven shape of the interface 1 is 0.83 to 0.91 piece / ⁇ m 2
  • the uneven density of the uneven shape of the interface 2 is 1.01 to 1.18 piece / ⁇ m 2. Is preferred.
  • the sub-pixel means a part corresponding to the light emitting part of the organic EL element part, that is, a part having the width of the transparent electrode 310 in the pixel (the whole of FIG. 1) as shown in FIG. .
  • corrugation is not attached
  • such a concavo-convex shape can be an array shape of a plurality of concave portions and convex portions having at least one period and smaller than the sub-pixel width.
  • a specific means for making the uneven density of the uneven shapes of the interfaces 1 and 2 different there is a means for attaching uneven shapes having different periods to each sub-pixel (for each of the interfaces 1 and 2).
  • the unevenness is formed on the surface of the transparent substrate 100 corresponding to the pattern of the color filter layers 210G and 210B.
  • the selected color filter layers 210G and 210B are stacked on the pattern.
  • a method generally used for surface roughening treatment for example, a method of etching with a chemical agent, plasma or the like using a resist pattern as a mask can be used.
  • a sandblasting method for example, a mechanical method of scratching the surface using comb teeth, or the like, using a mask and an abrasive.
  • a suitable irregularity is formed on the surface of the glass substrate by using an abrasive having an average particle size of 5 ⁇ m by sandblasting and treating for 2 to 8 seconds, preferably 3 to 7.5 seconds. Can be formed.
  • the interface between the red color filter layer 210 ⁇ / b> R and the transparent substrate 100 is not provided with an uneven shape.
  • the red color filter layer 210R can be laminated on the transparent substrate 100 by various known methods. For example, it can be formed by applying a known red color filter material by spin coating and performing patterning by photolithography.
  • the color filter layer 210 is a layer for improving the color purity of light having a certain region of the incident light incident on the layer by blocking a specific wavelength.
  • the color filter layer 210 (R, G, B) can be formed on the transparent substrate 100 using a material for a flat panel display.
  • the color filter layer 210 has a structure in which a blue color filter layer that transmits a wavelength of 400 to 550 nm, a green color filter layer that transmits a wavelength of 500 to 600 nm, and a red color filter layer that transmits a wavelength of 600 nm or more are arranged. be able to.
  • These color filter layers are composed of a photosensitive resin layer in which a dye or pigment, preferably a pigment is dispersed.
  • a dye or pigment preferably a pigment is dispersed.
  • azo lake insoluble azo, condensed azo, phthalocyanine, quinacridone, dioxazine, Indolinone, anthraquinone, berylone, thioin, berylene, and mixtures thereof are preferably used.
  • the color filter layer 210 has a stripe pattern composed of red (R), green (G), and blue (B) repetitions. Each pattern is transparent with a pattern width of 60 to 100 ⁇ m and a pattern interval of 70 to 90 ⁇ m. It is provided on one surface of the substrate 100.
  • a coating method can be used, and it is particularly preferable to use a photo process.
  • the light shielding layer 220 is formed for the purpose of improving the contrast by preventing the visible region from being transmitted between the color filter layers.
  • the light shielding layer 220 is formed using a material for a normal flat panel display.
  • a coating method can be used, and it is particularly preferable to use a photo process.
  • planarization layer 230 is a layer formed for the purpose of protecting the color filter layer 210 (R, G, B). Further, the planarizing layer 230 is formed so that a step generated by the color filter layer 210 and the light shielding layer 220 does not adversely affect the dimensional accuracy of each layer formed above the layers 210 and 220. Layer. For this reason, the planarization layer 230 needs to be formed by selecting a material and a process that are rich in light transmittance and do not deteriorate the color filter layer 210 (R, G, B).
  • a photocurable or photothermal combination type curable resin is subjected to light and / or heat treatment to generate radical species and ionic species to be polymerized or crosslinked to be insoluble and infusible. Is common.
  • the photocurable or photothermal combination type curable resin is preferably soluble in an organic solvent or an alkaline solution before curing in order to perform patterning.
  • photocurable or photothermal combination type curable resin (1) A composition film composed of an acrylic polyfunctional monomer or oligomer having a plurality of acroyl groups and methacryloyl groups, and light or a thermal polymerization initiator is subjected to light or heat treatment to generate photo radicals or heat radicals for polymerization.
  • a composition comprising a polyvinyl cinnamate ester and a sensitizer, which is dimerized by light or heat treatment and crosslinked.
  • composition film composed of a chain or cyclic olefin and a bisazide generated by nitrene generation by light or heat treatment to be crosslinked with the olefin, and (4) a monomer having an epoxy group and a photoacid generator And a composition film obtained by polymerizing an acid (cation) by light or heat treatment.
  • photocurable or photothermal combination type curable resins include polycarbonate (PC), polyethylene terephthalate (PET), polyethersulfone, polyvinyl butyral, polyphenylene ether, polyamide, polyetherimide, norbornene resin, and methacrylic resin. , Isobutylene maleic anhydride copolymer resin, cyclic olefin thermoplastic resin, epoxy resin, phenol resin, urethane resin, acrylic resin, vinyl ester resin, imide resin, urethane resin, urea resin, melamine resin, etc. Examples thereof include a curable resin, or a polymer hybrid containing a trifunctional or tetrafunctional alkoxysilane with polystyrene, polyacrylonitrile, polycarbonate, or the like.
  • a coating method can be used, and it is particularly preferable to use a photo process.
  • FIG. 1 is an example including the color filter layer 210, but when the color filter layer 210 is not included at all, an uneven shape is formed at the interface between the transparent substrate 100 and the planarization layer 230. Also in this case, a coating method can be used, and it is particularly preferable to use a photo process.
  • the color conversion layer is a photosensitive material in which a fluorescent dye having a function of causing the fluorescent dye to absorb incident light having a wavelength in the near ultraviolet region or visible region and emitting fluorescent light in a visible light region having a wavelength different from that of the incident light is dispersed. It consists of a functional resin layer. In the example shown in FIG. 1, only the red color conversion layer 240 is used among the red color conversion layer, the green color conversion layer, and the blue color conversion layer.
  • Examples of the fluorescent dye used in the red conversion layer 240 that absorbs light in the blue or blue-green region emitted from the organic EL element unit 300 and emits fluorescence in the red region include, for example, rhodamine B, rhodamine 6G, rhodamine 3B, Rhodamine 101, rhodamine 110, sulforhodamine, basic violet 11, basic red 2 and other rhodamine dyes, cyanine dyes, 1-ethyl-2- [4- (p-dimethylaminophenyl) -1,3-butadienyl]- Examples thereof include pyridine dyes such as pyridinium perchlorate (pyridine 1), and oxazine dyes. Various dyes such as direct dyes, acid dyes, basic dyes, and disperse dyes can be used as long as they exhibit fluorescence.
  • a fluorescent dye used for a green conversion layer that absorbs light in a blue to blue-green region emitted from the organic EL element unit 300 and emits fluorescence in a green region
  • a fluorescent dye used for a green conversion layer that absorbs light in a blue to blue-green region emitted from the organic EL element unit 300 and emits fluorescence in a green region
  • a coumarin dye such as diethylamino-coumarin (coumarin 30), 2,3,5,6-1H, 4H-tetrahydro-8-trifluoromethylquinolidine (9,9a, 1-gh) coumarin (coumarin 153), Coumarin dyes such as Basic Yellow 51, phthalimide colors such as Solvent Yellow
  • the blue conversion layer is usually omitted because the light emitted from the organic EL element unit 300 has substantially the same wavelength region as the wavelength region selected by the blue color filter layer 210B, and is not used in the example shown in FIG. .
  • a transparent photosensitive resin layer can be formed as a dummy.
  • the color conversion layer (red conversion layer 240 in the example shown in FIG. 1) can be formed by various dry processes, and is preferably formed by vacuum deposition because it can be formed without decomposing the organic material.
  • a heating method of the vacuum evaporation method either a direct heating method or an indirect heating method can be used, and specifically, resistance heating, electron beam heating, infrared heating, or the like can be used.
  • a preliminary mixture prepared by mixing a plurality of types of color conversion dyes in a predetermined ratio is prepared in advance, and co-evaporation is performed using the preliminary mixture. Can do.
  • the film thickness of the color conversion layer is preferably 1 ⁇ m or less from the viewpoint of exhibiting the function of the color conversion layer, and is preferably 200 nm to 1 ⁇ m. It is more preferable at the point which can utilize a layer effectively.
  • the gas barrier layer 250 is a layer formed to prevent moisture and / or oxygen from entering the color conversion layer (the red conversion layer 240 in the case shown in the figure) from the outside. This is because the color conversion dye is an organic substance and thus is vulnerable to moisture and oxygen.
  • the purpose of forming the gas barrier layer 250 is to protect the red color conversion layer 240, but in the example shown in FIG. 1, not only the red color conversion layer 240 but also the planarization layer 230 is protected.
  • This structure is also effective for protecting the organic EL layer 320, which will be described later, since it is necessary to prevent moisture from being emitted from the color conversion filter unit 200.
  • a material applicable to the gas barrier layer 250 a material having electrical insulating properties and a barrier property against a gas and an organic solvent and having high transparency in the visible region (transmittance in a range of 400 to 700 nm). 50% or more) can be used. Further, it is preferable to use a material having a film hardness (pencil hardness) of 2H or more, which is a hardness that can withstand the formation of a transparent electrode 310 and the like, which will be described later, formed on the gas barrier layer 250.
  • the film hardness (pencil hardness) conforms to JIS K5600-5-4.
  • an inorganic oxide such as SiOx, SiNx, SiNxOy, AlOx, TiOx, TaOx, ZnOx, or an inorganic nitride can be used.
  • the formation method of the gas barrier layer 250 is not particularly limited, and a sputtering method, a CVD method, a vacuum deposition method, or the like can be used.
  • the gas barrier layer 250 can be a single layer or a laminate including a plurality of layers.
  • the color conversion filter unit 200 is formed on the transparent substrate 100.
  • Transparent electrode 310 Materials applicable to the transparent electrode 310 include ITO, tin oxide, indium oxide, IZO, zinc oxide, zinc-aluminum oxide, zinc-gallium oxide, or a dopant such as F or Sb added to these oxides. Conductive transparent metal oxides can be used.
  • the transparent electrode 310 can be obtained by forming using a vapor deposition method, a sputtering method, or a chemical vapor deposition (CVD) method and then patterning using a photolithographic method or the like. Among such formation methods, it is particularly preferable to use a sputtering method.
  • the transparent electrode 310 can be either an anode or a cathode.
  • a cathode buffer layer (not shown) between the transparent electrode 310 and the organic EL layer 320 to improve the electron injection efficiency for the organic EL layer 320.
  • an alkali metal such as Li, Na, K or Cs, an alkaline earth metal such as Ba or Sr, an alloy containing them, a rare earth metal, or a fluoride of these metals is used. be able to.
  • the thickness of the cathode buffer layer is preferably 10 nm or less from the viewpoint of ensuring transparency.
  • a conductive transparent metal oxide layer is provided between the transparent electrode 310 and the organic EL layer 320 to increase the hole injection efficiency for the organic EL layer 320. It is preferable to improve.
  • materials applicable as the conductive transparent metal oxide include ITO, tin oxide, indium oxide, IZO, zinc oxide, zinc-aluminum oxide, zinc-gallium oxide, and oxides such as F or Sb. A material to which a dopant is added can be used.
  • the organic EL layer 320 includes at least an organic light emitting layer, and has a structure in which a hole injection layer, a hole transport layer, an electron transport layer and / or an electron injection layer are interposed as required.
  • a specific layer structure of the organic EL element portion the following structure can be adopted.
  • anode / organic light emitting layer / cathode (2) Anode / hole injection layer / organic light emitting layer / cathode (3) Anode / organic light emitting layer / electron injection layer / cathode (4) Anode / hole injection layer / organic light emitting layer / electron injection layer / cathode (5) Anode / hole transport layer / organic light emitting layer / electron injection layer / cathode (6) Anode / hole injection layer / hole transport layer / organic light emitting layer / electron injection layer / cathode (7) Anode / hole injection layer / hole transport layer / organic light emitting layer / electron transport layer / electron injection layer / cathode In the layer structures (1) to (7), the anode and the cathode are either the transparent electrode 310 or the reflective electrode 330.
  • each layer constituting the organic EL layer 320 As a material of each layer constituting the organic EL layer 320, a known material can be used. Moreover, each layer which comprises the organic EL layer 320 can be formed using arbitrary methods well-known in the said techniques, such as a vapor deposition method.
  • the organic EL layer 320 realizes light emission from blue to blue-green.
  • materials applicable to the organic light emitting layer for obtaining blue to blue-green light emission include fluorescent brighteners such as benzothiazole, benzimidazole, or benzoxazole, metal chelated oxonium compounds, and styrylbenzene. It is preferable to use a compound or an aromatic dimethylidin compound.
  • the light emission of the organic light emitting layer can be white light as necessary. In this case, it is important to use a known red dopant.
  • Reflective electrode 330 As a material applicable to the reflective electrode 330, it is preferable to use a metal with high reflectivity, an amorphous alloy with high reflectivity, or a microcrystalline alloy with high reflectivity.
  • the highly reflective metal include Al, Ag, Mo, W, Ni, and Cr.
  • the highly reflective amorphous alloy include NiP, NiB, CrP, and CrB.
  • An example of the highly reflective microcrystalline alloy is NiAl.
  • the reflective electrode 330 can be either a cathode or an anode.
  • a cathode buffer layer (not shown) between the reflective electrode 330 and the organic EL layer 320 to improve the electron injection efficiency for the organic EL layer 320.
  • a conductive transparent metal oxide layer is provided between the reflective electrode 330 and the organic EL layer 320 to increase the hole injection efficiency for the organic EL layer 320. It is preferable to improve.
  • materials applicable as the conductive transparent metal oxide include ITO, tin oxide, indium oxide, IZO, zinc oxide, zinc-aluminum oxide, zinc-gallium oxide, and oxides such as F or Sb. A material to which a dopant is added can be used.
  • the reflective electrode 330 As a method for forming the reflective electrode 330, any means known in the technical field such as vacuum deposition, sputtering, ion plating, or laser ablation can be used depending on the material to be used. Unlike the example shown in FIG. 1, when the reflective electrode 330 made up of a plurality of partial electrodes is required, the reflective electrode 330 made up of the plurality of partial electrodes is formed using a mask that gives a desired shape. You can also.
  • the reflective electrode 330 has a striped pattern that intersects the pattern of the transparent electrode 310, and this intersecting region forms a light emitting subpixel.
  • the organic EL display obtained as described above is bonded to a sealing glass (not shown) by UV curing in a dry nitrogen atmosphere in the glove box (an atmosphere in which both O 2 concentration and H 2 O concentration are 10 ppm or less). It seals using the contact bonding layer which consists of an agent.
  • the organic EL display (top emission type) of the present invention As shown in FIG. 2, the first laminate X in which the color conversion filter unit 200 is formed on the substrate 100 and the organic EL element unit 300 on the base 400 are formed.
  • the second laminated body Y is bonded to the light incident surface of the color conversion filter unit 200 with the light emitting surface of the organic EL element unit 300 by a thermosetting adhesive layer 500. is there.
  • the organic EL display shown in FIG. 2 includes a sealing material (not shown) that blocks the color conversion filter unit 200 and the organic EL element unit 300 from the outside air.
  • the transparent substrate 100 supports the components (the color filter layer 210, the light shielding layer 220, the planarization layer 230, the red color conversion layer 240, and the gas barrier layer 250) of the color conversion filter unit 200 that are sequentially formed thereon. Is a layer.
  • the transparent substrate 100 is one that can withstand the conditions (solvent, temperature, etc.) used for forming these components. Other conditions for the transparent substrate 100 are the same as those of the transparent substrate 100 shown in FIG.
  • the substrate 400 is a component for supporting the organic EL element 300.
  • a substrate that can withstand the conditions (solvent, temperature, etc.) used for forming the organic EL element 300 is used.
  • Other conditions for the substrate 400 are the same as those of the transparent substrate 100.
  • the adhesive layer 500 is a component used for bonding the first laminate X and the second laminate Y together.
  • the adhesive layer 500 is not particularly limited as long as it has visible light transparency and can be formed without causing adverse effects such as damage to the red color conversion layer 240 and the organic EL layer 320.
  • a general thermoplastic resin, a thermosetting resin that can be cured by heat at room temperature to 120 ° C., a resin that can be cured by visible light, or a combination of heat and light can be used.
  • the reflective electrode 330, the organic EL layer 320, and the transparent electrode 310 are sequentially formed on the substrate 400 to obtain the second stacked body Y.
  • the formation mode of the reflective electrode 330 and the like on the substrate 400 is performed in accordance with the formation mode of the corresponding component in the organic EL display (type 1) shown in FIG.
  • first stacked body X and the second stacked body Y are interposed through the thermosetting adhesive layer 500 in a state where the light incident surface of the color conversion filter unit 200 faces the light emitting surface of the organic EL element unit 300. to paste together.
  • the obtained organic EL display was subjected to a sealing layer made of a UV curable sealing agent (not shown) under a dry nitrogen atmosphere (an atmosphere in which both O 2 concentration and H 2 O concentration were 10 ppm or less) in the glove box. Is used to seal the color conversion filter unit 200 and the organic EL element unit 300.
  • examples and comparative examples all relate to an organic EL display in which 160 pixels including R, G, and B subpixels are formed at a pitch of 0.33 mm in the vertical direction and 120 in the horizontal direction.
  • Example 1 The organic EL display of Example 1 was a display of the type shown in FIG. A glass substrate of 200 mm ⁇ 200 mm ⁇ 0.7 mm was prepared. A dry etching method (C 4 F 8 : 16 msccm, CH 2 F 2 : 16 sccm, gas pressure 0.8 Pa, and power 2 kW) is used with a Cr film (film thickness 100 nm) first patterned at a predetermined pitch as a mask.
  • C 4 F 8 16 msccm
  • CH 2 F 2 16 sccm
  • gas pressure 0.8 Pa gas pressure 0.8 Pa
  • power 2 kW power 2 kW
  • the blue subpixel area on the color filter layer side of the substrate is formed into a right-cone-shaped irregularity with a depth of 0.6 ⁇ m and a pitch of 0.2 ⁇ m, and then the green subpixel area is formed with a depth of 0.4 ⁇ m and a pitch of 0.
  • a substrate 100 having a 3 ⁇ m right conical unevenness was obtained.
  • a light-shielding layer coating solution (CK8400L manufactured by Fuji Film ARCH) was applied to the entire surface by a spin coating method, and dried at 80 ° C. by heating. Thereafter, a pattern having a sub-pixel size (vertical direction of 80 ⁇ m ⁇ horizontal direction of 300 ⁇ m, thickness direction of 1 ⁇ m) was formed at a pitch of 330 ⁇ m by using a photolithography method, and the light shielding layer 220 was laminated on the substrate 100.
  • CK8400L manufactured by Fuji Film ARCH
  • the blue color filter layer 210B a blue color filter material (manufactured by Fuji Film ARCH: Color Mosaic CB-7001) was applied on the substrate 100 by spin coating, and patterning was performed by photolithography. Specifically, the substrate 100 formed into a conical unevenness having a depth of 0.6 ⁇ m and a pitch of 0.2 ⁇ m was traced. As a result, the substrate side of the blue color filter layer 210B has an area size of 80 ⁇ m ⁇ 300 ⁇ m and a thickness of 0.6 ⁇ m in depth, a pitch of 0.2 ⁇ m, and an average density of 0.88 pieces / ⁇ m 2 formed into a right cone shape. A 2 ⁇ m line pattern was obtained.
  • the green color filter layer 210G For the formation of the green color filter layer 210G, a green color filter material (manufactured by Fuji Film ARCH: Color Mosaic CG-7001) was applied on the substrate 100 by spin coating, and patterning was performed by photolithography. Specifically, the substrate 100 formed into a conical unevenness having a depth of 0.4 ⁇ m and a pitch of 0.3 ⁇ m was traced. As a result, the substrate side of the green color filter layer 210G is an area size of 80 ⁇ m ⁇ 300 ⁇ m, formed into a conical unevenness having a depth of 0.4 ⁇ m, a pitch of 0.3 ⁇ m, and an average density of 1.99 / ⁇ m 2 A 2 ⁇ m line pattern was obtained.
  • a green color filter material manufactured by Fuji Film ARCH: Color Mosaic CG-7001
  • the substrate side of the green color filter layer 210G is an area size of 80 ⁇ m ⁇ 300 ⁇ m, formed into a conical unevenness having
  • red color filter layer 210R For the formation of the red color filter layer 210R, a red color filter material (manufactured by Fuji Film ARCH: Color Mosaic CR-7001) was applied on the substrate 100 by spin coating, and patterning was performed by photolithography. Specifically, a line pattern having an area size of 80 ⁇ m ⁇ 300 ⁇ m and a film thickness of 2 ⁇ m was obtained.
  • the planarization layer 230 was formed by applying a planarization layer material (Nippon Steel Chemical Co., Ltd .: V-259PA) on the color filter layer 210 and the light shielding layer 220 by spin coating.
  • the thickness of the planarizing layer 230 in the region in contact with the light shielding layer 220 was 2.5 ⁇ m.
  • a planarization film was separately formed under the same conditions on a glass substrate and the refractive index was measured, it was found that the planarization layer of this example had a refractive index of 1.5.
  • the layered product having the flattening layer 230 or less obtained as described above is heated to 200 ° C. for 20 minutes under a dry nitrogen atmosphere (moisture concentration of 1 ppm or less) to remove residual moisture. Removed.
  • This laminate was attached to a vacuum deposition apparatus, and DCM-R was deposited at a deposition rate of 0.3 ⁇ / s under a pressure of 1 ⁇ 10 ⁇ 4 Pa to form a red conversion layer 240 having a thickness of 500 nm. .
  • a DCM-R film was separately formed on a glass substrate under the same conditions and the refractive index was measured, it was found that the red conversion layer of this example had a refractive index of 1.9.
  • a 300 nm-thick SiNH film was laminated by using a plasma CVD method to obtain a gas barrier layer 250.
  • 100 SCCM SiH 4 , 500 SCCM NH 3 , and 2000 SCCM N 2 were used as source gases, and the gas pressure was set to 80 Pa.
  • 0.5 kW of 27 MHz RF power was applied as plasma generation power.
  • the gas barrier layer of this example had a refractive index of 1.95.
  • the transparent electrode 310 / organic EL layer 320 (hole injection layer / hole transport layer / organic light emitting layer / electron transport layer) / reflection electrode 330
  • the organic EL element part 300 which consists of was formed.
  • the transparent electrode 310 formed an In—Zn oxide pattern.
  • An In—Zn oxide film having a thickness of 200 nm was formed at room temperature by DC sputtering.
  • An In—Zn oxide target was used as the sputtering target, and Ar and oxygen were used as the sputtering gas.
  • patterning was performed using oxalic acid as an etchant to form a pattern with a wiring width of 100 ⁇ m.
  • drying treatment 150 ° C.
  • UV treatment room temperature and 150 ° C.
  • the laminate is mounted in a resistance heating vapor deposition apparatus, and a hole injection layer, a hole transport layer, an organic light emitting layer, and an electron injection layer are sequentially formed without breaking the vacuum to form an organic EL layer 320. did.
  • the internal pressure of the vacuum chamber was reduced to 1 ⁇ 10 ⁇ 5 Pa.
  • As the hole injection layer copper phthalocyanine (CuPc) was laminated to a thickness of 100 nm.
  • As the hole transport layer 4,4′-bis [N- (1-naphthyl) -N-phenylamino] biphenyl ( ⁇ -NPD) was laminated to a thickness of 20 nm.
  • DPVBi 4,4′-bis (2,2′-diphenylvinyl) biphenyl
  • a reflection made of a Mg / Ag (10: 1 weight ratio) layer having a thickness of 200 nm is used by using a mask capable of obtaining a stripe pattern having a width of 0.30 mm and a gap of 0.03 mm perpendicular to the line of the transparent electrode 310.
  • the electrode 330 was formed without breaking the vacuum.
  • a UV curable adhesive (trade name 30Y-437, manufactured by ThreeBond Co., Ltd.) in which beads having a diameter of 6 ⁇ m were dispersed was placed on the outer periphery of the laminate thus obtained using a dispenser robot in a dry nitrogen atmosphere inside the glove box.
  • the organic EL display of Example 1 was obtained by bonding using the sealing glass applied to the substrate and irradiating with 100 mW / cm 2 ultraviolet rays for 30 seconds to cure the outer peripheral sealing layer.
  • Example 2 The organic EL display of Example 2 was a display of the type shown in FIG. The formation of the substrate 100 and the sequential formation of the light shielding layer 220, the color filter layer 210, the planarization layer 230, the red color conversion layer 240, and the gas barrier layer 250 on the substrate 100 are performed in the same manner as in Example 1. 1 laminate X was obtained.
  • a glass substrate as a substrate 400 was separately prepared, and a reflective electrode 330 made of indium / tin oxide (ITO) having a thickness of 200 nm was formed by sputtering and photolithography.
  • the shape of the reflective electrode 330 was a stripe pattern with a wiring width of 100 ⁇ m extending in the vertical direction.
  • the laminated body in which the reflective electrode 330 is formed on the substrate 400 is mounted in a resistance heating vapor deposition apparatus, and the electron injection layer, the organic EL light emitting layer, the hole transport layer, and the hole injection layer are set in a vacuum chamber.
  • a passivation layer (not shown) made of SiN having a thickness of 500 nm was formed so as to cover the stacked body from the base body 400 to the transparent electrode 310, and a second stacked body Y was obtained.
  • the first laminated body X and the second laminated body Y obtained in this manner were carried into a bonding apparatus managed with a moisture concentration of 1 ppm and an oxygen concentration of 1 ppm.
  • a UV curable adhesive (trade name 30Y-437, manufactured by ThreeBond Co., Ltd.) in which beads having a diameter of 6 ⁇ m are dispersed is applied to the first laminate X as an outer peripheral sealing layer, and at the center.
  • a predetermined amount of a thermosetting adhesive was dropped, and the atmosphere was removed with a vacuum of 1 Pa in a bonding apparatus.
  • the gas barrier layer 250 and a passivation layer (not shown) were opposed to each other, the laminated body Y was placed on the upper surface of the passivation layer, and the laminated bodies X and Y were bonded together by pressure bonding.
  • 100 mW / cm 2 ultraviolet ray was irradiated for 30 seconds to cure, then heating at 100 ° C. for 1 hour to heat the outer periphery sealing part and the thermosetting adhesive Curing was performed to obtain an organic EL display of Example 2.
  • Comparative Example 1 The organic EL display of Comparative Example 1 was a display of the type shown in FIG. A glass substrate of 200 mm ⁇ 200 mm ⁇ 0.7 mm was prepared. First, a light shielding layer coating solution (CK8400L manufactured by Fuji Film ARCH) was applied on the entire surface of the substrate 100 by a spin coat method and dried by heating at 80 ° C. Then, using a photolithographic method, at a pitch of 330 ⁇ m, A pattern with a subpixel size (vertical direction 80 ⁇ m ⁇ horizontal direction 300 ⁇ m, thickness direction 1 ⁇ m) was formed, and a light shielding layer 220 was laminated on the substrate 100.
  • CK8400L manufactured by Fuji Film ARCH
  • a blue color filter material manufactured by Fuji Film ARCH: Color Mosaic CB-7001 was applied on the substrate 100 by spin coating, and patterning was performed by photolithography. Specifically, a line pattern having an area size of 80 ⁇ m ⁇ 300 ⁇ m and a film thickness of 2 ⁇ m was obtained.
  • the green color filter layer 210G For the formation of the green color filter layer 210G, a green color filter material (manufactured by Fuji Film ARCH: Color Mosaic CG-7001) was applied on the substrate 100 by a spin coating method, and patterning was performed by a photolithographic method. Specifically, a line pattern having an area size of 80 ⁇ m ⁇ 300 ⁇ m and a film thickness of 2 ⁇ m was obtained.
  • the red color filter layer 210R the flattening layer 230, the red color conversion layer 240, the gas barrier layer 250, the transparent electrode 310, the organic EL layer 320, and the reflective electrode 330 are formed and sealed in the same manner as in the example.
  • the organic EL display of Comparative Example 1 was obtained.
  • Comparative Example 2 The organic EL display of Comparative Example 2 was a display of the type shown in FIG.
  • a glass substrate of 200 mm ⁇ 200 mm ⁇ 0.7 mm was prepared.
  • a dry etching method (C 4 F 8 : 16 msccm, CH 2 F 2 : 16 sccm, gas pressure 0.8 Pa, and power 2 kW) is used with a Cr film (film thickness 100 nm) first patterned at a predetermined pitch as a mask.
  • a substrate 100 was obtained in which the blue subpixel area and the green subpixel area on the color filter layer side of the substrate were formed in a conical irregularity having a depth of 0.6 ⁇ m and a pitch of 0.2 ⁇ m.
  • a light-shielding layer coating solution (CK8400L manufactured by Fuji Film ARCH) was applied to the entire surface by a spin coating method, and dried at 80 ° C. by heating. Thereafter, a pattern having a sub-pixel size (vertical direction of 80 ⁇ m ⁇ horizontal direction of 300 ⁇ m, thickness direction of 1 ⁇ m) was formed at a pitch of 330 ⁇ m by using a photolithography method, and the light shielding layer 220 was laminated on the substrate 100.
  • CK8400L manufactured by Fuji Film ARCH
  • the blue color filter layer 210B a blue color filter material (manufactured by Fuji Film ARCH: Color Mosaic CB-7001) was applied on the substrate 100 by spin coating, and patterning was performed by photolithography. Specifically, the substrate 100 formed into a conical unevenness with a depth of 0.6 ⁇ m and a pitch of 0.2 ⁇ m was traced. As a result, the substrate side of the blue color filter layer 210B has an area size of 80 ⁇ m ⁇ 300 ⁇ m and a thickness of 0.6 ⁇ m in depth, a pitch of 0.2 ⁇ m, and an average density of 0.88 pieces / ⁇ m 2 formed into a right cone shape. A 2 ⁇ m line pattern was obtained.
  • the green color filter layer 210G For the formation of the green color filter layer 210G, a green color filter material (manufactured by Fuji Film ARCH: Color Mosaic CG-7001) was applied on the substrate 100 by spin coating, and patterning was performed by photolithography. Specifically, the substrate 100 formed into a conical unevenness having a depth of 0.6 ⁇ m and a pitch of 0.2 ⁇ m was traced. As a result, the substrate side of the green color filter layer 210G is an area size of 80 ⁇ m ⁇ 300 ⁇ m formed in a right-cone-shaped unevenness with a depth of 0.6 ⁇ m, a pitch of 0.2 ⁇ m, and an average density of 0.88 / ⁇ m 2. A 2 ⁇ m line pattern was obtained.
  • the red color filter layer 210R the flattening layer 230, the red color conversion layer 240, the gas barrier layer 250, the transparent electrode 310, the organic EL layer 320, and the reflective electrode 330 are formed and sealed in the same manner as in the example.
  • the organic EL display of Comparative Example 2 was obtained.
  • Comparative Example 1 where the interface between the substrate 100 and the blue and green color filter layers 210B and 210G is not uneven, it was found that the change in the emission color of the screen depending on the observation angle was significant.
  • the organic EL displays of Examples 1 and 2 have a structure in which the unevenness density is adjusted for each of R, G, and B at the interface between the substrate and the color filter, so that the luminance and chromaticity are maintained. It has been found that the difference in directivity of light between G, B and B can be reduced.
  • the present invention has a predetermined shape at the interface between the substrate and the color filter or the flattening layer, thereby finely adjusting the difference in directivity of light between different-colored subpixels and increasing the change in emission color depending on the viewing angle. Can be prevented by level. Therefore, the present invention is promising in that it can provide various electronic devices such as a mobile phone having a display unit that does not change the emission color depending on the viewing angle.

Abstract

L'invention porte sur un dispositif d'affichage électroluminescent organique qui a un substrat ; une section de filtre de conversion de couleur comprenant une couche planarisée et au moins un type de couche de conversion de couleur ; une section d'élément électroluminescent organique ayant une pluralité de sections luminescentes, qui définissent une pluralité de sous-pixels ; et une interface dans la forme irrégulière entre le substrat et la couche planarisée, la forme irrégulière ayant une densité irrégulière différente pour chacun des sous-pixels. Dans un tel agencement, la surface supérieure du substrat a une forme prédéterminée pour chacun des sous-pixels définis par les sections luminescentes sur la section d'élément électroluminescent organique pour effectuer un ajustement fin de la directivité de lumière parmi différents sous-pixels de couleur, empêchant ainsi une variation des couleurs luminescentes en fonction des angles de champ de vison à des niveaux élevés.
PCT/JP2008/064308 2008-02-07 2008-08-08 Dispositif d'affichage électroluminescent organique et son procédé de fabrication WO2009098793A1 (fr)

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