WO2017082173A1 - Procédé de fabrication de dispositif électroluminescent organique, et dispositif électroluminescent organique - Google Patents

Procédé de fabrication de dispositif électroluminescent organique, et dispositif électroluminescent organique Download PDF

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Publication number
WO2017082173A1
WO2017082173A1 PCT/JP2016/082820 JP2016082820W WO2017082173A1 WO 2017082173 A1 WO2017082173 A1 WO 2017082173A1 JP 2016082820 W JP2016082820 W JP 2016082820W WO 2017082173 A1 WO2017082173 A1 WO 2017082173A1
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Prior art keywords
organic
emitting layer
light emitting
organic light
flatness
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PCT/JP2016/082820
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English (en)
Japanese (ja)
Inventor
倉田　知己
山下　和貴
関口　泰広
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住友化学株式会社
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Priority to KR1020187015927A priority Critical patent/KR20180082497A/ko
Priority to JP2017550292A priority patent/JP6814742B2/ja
Priority to CN201680065207.4A priority patent/CN108353480B/zh
Publication of WO2017082173A1 publication Critical patent/WO2017082173A1/fr

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    • 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
    • H10K59/10—OLED displays
    • 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
    • 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
    • H05B33/12—Light sources with substantially two-dimensional radiating surfaces
    • 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
    • H05B33/12—Light sources with substantially two-dimensional radiating surfaces
    • H05B33/22—Light sources with substantially two-dimensional radiating surfaces characterised by the chemical or physical composition or the arrangement of auxiliary dielectric or reflective layers

Definitions

  • the present invention relates to an organic EL device manufacturing method and an organic EL device.
  • an organic EL device As an organic EL device, a device in which a plurality of pixels are defined by banks (partition walls) as in Patent Document 1 is known. In such an organic EL device, an organic light emitting layer is provided in each pixel, and light is emitted for each pixel.
  • the thickness of the organic light emitting layer in the pixel of the organic EL device is not uniform, the luminance characteristics (for example, luminance uniformity) in the pixel deteriorate.
  • the luminance characteristics for example, luminance uniformity
  • the desired luminance characteristics are required until the organic EL device is made to emit light after being manufactured once by forming an electrode on the organic light-emitting layer. I don't know if Therefore, when desired luminance characteristics are not obtained, it is necessary to form not only the organic light emitting layer but also an electrode to be provided on the organic light emitting layer, which reduces the productivity of the organic EL device.
  • an object of the present invention is to provide a method for manufacturing an organic EL device and an organic EL device capable of improving productivity.
  • a banked substrate includes a substrate, a bank provided on the substrate for defining a pixel, and a first region provided on a pixel region corresponding to the pixel on the substrate.
  • a step of forming an organic light emitting layer by a coating method on the first electrode of the banked substrate including electrodes, a step of calculating the flatness of the organic light emitting layer, and a flatness of the organic light emitting layer is desired.
  • the thickness of the organic light emitting layer is (d + predetermined value) nm or less when viewed from the thickness direction of the substrate, and the area of the organic light emitting layer is A1, the area of the pixel region is A2, and the flatness is where ⁇ is the flatness,
  • the inventors of the present application have a certain relationship between the flatness and the organic light emitting layer to the luminance state. I found.
  • an organic EL device having an organic light emitting layer having a flatness equal to or higher than a desired value in a pixel can be manufactured.
  • an organic EL device according to the knowledge found by the inventors of the present application, light can be emitted from the pixel in a luminance state substantially corresponding to the desired value.
  • an organic EL device capable of emitting light in a desired luminance state from the pixel can be manufactured. Therefore, the productivity of the organic EL device is improved.
  • the desired flatness is set based on the relationship between the flatness defined by the above formula (1) for the luminance distribution rate calculation pixel and the luminance distribution rate in the luminance distribution rate calculation pixel.
  • the luminance distribution rate may be a ratio of the area of a region having 70% or more of the maximum luminance of the area of the luminance distribution rate calculation pixel in the luminance distribution rate calculation pixel.
  • the desired luminance distribution rate can be realized by setting the flatness of the organic light emitting layer to a desired value or more based on the relationship between the flatness and the luminance distribution rate.
  • the desired flatness is 70%, preferably 80%.
  • a step of forming an organic structure including at least one organic layer on the first electrode of the banked substrate may be further provided.
  • the organic light emitting layer may be formed on the organic structure.
  • the thickness distribution of the organic light emitting layer is changed to the thickness distribution of the organic structure and the organic on the organic structure.
  • the flatness can be calculated on the basis of the thickness distribution of the organic light emitting layer by calculating the difference from the thickness distribution of the laminate formed with the light emitting layer.
  • An organic EL device includes (A) a substrate, a bank provided on the substrate for defining a pixel, and (B) a pixel region corresponding to the pixel on the substrate.
  • a banked substrate having a first electrode provided; (C) an organic light emitting layer provided on the first electrode; and (D) a second electrode provided on the organic light emitting layer.
  • the minimum thickness of the organic light emitting layer is d (nm), the area of the organic light emitting layer that is (d + predetermined value) nm or less when viewed from the thickness direction of the substrate is A1, and the area of the pixel region Is A2, and the flatness of the organic light emitting layer is (A1 / A2) ⁇ 100 [%], the flatness is 70% or more.
  • the organic EL device can realize a luminance distribution rate corresponding to a flatness of 70% or more. Since this organic EL device can be manufactured by the manufacturing method of the organic EL device, productivity can be improved.
  • the predetermined value may be 2 or more and 15 or less, for example.
  • the predetermined value may be 10.
  • FIG. 1 is a plan view of an organic EL device according to an embodiment as viewed from the banked substrate side.
  • FIG. 2 is a partially enlarged view of a cross section taken along line II-II in FIG.
  • FIG. 3 is a diagram illustrating a banked substrate included in the organic EL device of FIG.
  • FIG. 4 is a flowchart of an example of a method for manufacturing an organic EL device according to an embodiment.
  • FIG. 5 is a drawing for explaining the organic structure forming step.
  • FIG. 6 is a view for explaining an organic light emitting layer forming step.
  • FIG. 7 is a schematic diagram for explaining the relationship between the drying rate and the thickness distribution of the organic light emitting layer.
  • FIG. 1 is a plan view of an organic EL device according to an embodiment as viewed from the banked substrate side.
  • FIG. 2 is a partially enlarged view of a cross section taken along line II-II in FIG.
  • FIG. 3 is a diagram illustrating a bank
  • FIG. 8 is a drawing schematically showing the configuration of the organic EL device of the example, and FIG. 8A schematically shows the configuration of the organic EL device of Experimental Examples 1 to 4.
  • FIG. 8A schematically shows the configuration of the organic EL device of Experimental Examples 1 to 4.
  • FIG. 8 schematically shows the configurations of the organic EL devices of Experimental Examples 5 to 9, and
  • FIG. 8 (c) schematically shows the configurations of the organic EL devices of Experimental Examples 10 to 14. Yes.
  • FIG. 9 is a drawing showing the experimental results of Experimental Examples 1-14.
  • FIG. 10 is a drawing showing the thickness distribution of the organic light emitting layer in Experimental Examples 1 to 4.
  • FIG. 11 is a drawing showing the thickness distribution of the organic light emitting layer in Experimental Examples 5 to 9.
  • FIG. 12 is a drawing showing the thickness distribution of the organic light emitting layer in Experimental Examples 10 to 14.
  • the organic electroluminescence (organic EL) device 1 shown in FIG. 1 is an organic EL display panel, and has a plurality of pixels 2.
  • Each pixel 2 is an organic EL element part. That is, the organic EL device 1 has a configuration in which a plurality of organic EL element units are integrally connected.
  • “pixel” means a minimum unit (or minimum region) that emits light, and the pixel 2 has color information by light emission of the pixel 2.
  • the pixel 2 is schematically indicated by a broken line.
  • the organic EL device 1 includes three types of pixels 2, that is, a red pixel 2R that emits red light, a green pixel 2G that emits green light, and a blue pixel 2B that emits blue light.
  • the pixel 2 when distinguishing the colors emitted by the pixel 2, the pixel 2 may be referred to as a red pixel 2R, a green pixel 2G, and a blue pixel 2B as described above.
  • the plurality of pixels 2 are arranged in a two-dimensional array (or matrix). Two directions orthogonal to each other in the two-dimensional array are also referred to as an X direction (or row direction) and a Y direction (or column direction).
  • the three types of red pixel 2R, green pixel 2G, and blue pixel 2B constituting the plurality of pixels 2 are arranged in the order of the following columns (i), (ii), and (iii) in this order.
  • the arrangement is performed in an aligned manner.
  • (Ii) A column in which the green pixels 2G are arranged at predetermined intervals in the X direction.
  • the blue pixels 2B are arranged at predetermined intervals in the X direction.
  • the organic EL device 1 controls the red pixel 2R, the green pixel 2G, and the blue pixel 2B included in the display pixel unit by using the red pixel 2R, the green pixel 2G, and the blue pixel 2B arranged in parallel as one display pixel unit. Therefore, full color display can be performed.
  • the interval between the pixels 2 in each column, the interval between the pixels 2 in each row, the arrangement example of the pixels 2, the number of the pixels 2, and the like are appropriately set according to the specifications of the organic EL device 1 and the like.
  • the configuration of the organic EL device 1 will be described in detail.
  • the organic EL device 1 includes a banked substrate 10, a plurality of organic EL structure units 20, and a cathode (second electrode) 30.
  • the organic EL device 1 may be a top emission type device or a bottom emission type device.
  • a bottom emission type that is, a case where light is extracted from the banked substrate 10 side will be described.
  • the banked substrate 10 includes a substrate 11, a plurality of anodes (first electrodes) 12, and a bank 13. 3 corresponds to a partially enlarged view of the cross section of the banked substrate 10 taken along the line II-II in FIG. 1.
  • FIG. 2 corresponds to the drawing in which components other than the banked substrate 10 are omitted. To do.
  • the substrate 11 is a plate-like transparent member that is transparent to visible light (light having a wavelength of 400 nm to 800 nm).
  • the substrate 11 is a support that supports the anode 12 and the bank 13.
  • An example of the thickness of the substrate 11 is 30 ⁇ m or more and 1100 ⁇ m or less.
  • the substrate 11 may be a rigid substrate such as a glass substrate and a silicon substrate, or may be a flexible substrate such as a plastic substrate and a polymer film. By using a flexible substrate, the organic EL device 1 can have flexibility.
  • a circuit for driving each pixel 2 may be formed in advance on the substrate 11.
  • a TFT Thin Film Transistor
  • a capacitor may be formed in advance on the substrate 11.
  • the plurality of anodes 12 are provided on the pixel region 2 a corresponding to each pixel 2 on the surface 11 a of the substrate 11.
  • Examples of the shape of the anode 12 in plan view include a quadrangle such as a rectangle and a square, and other polygons.
  • the shape of the anode 12 in plan view may be circular or elliptical.
  • a thin film made of a metal oxide, a metal sulfide, a metal, or the like can be used for the anode 12.
  • indium oxide, zinc oxide, tin oxide, indium tin oxide Indium Tin Oxide: abbreviated as ITO
  • ITO Indium Tin Oxide
  • IZO Indium Zinc Oxide
  • gold, platinum, silver, copper, or the like is used.
  • an anode 12 exhibiting light transmittance is used.
  • the thickness of the anode 12 can be appropriately determined in consideration of light transmittance, electrical conductivity, and the like.
  • the thickness of the anode 12 is, for example, 10 nm to 10 ⁇ m, preferably 20 nm to 1 ⁇ m, and more preferably 50 nm to 500 nm.
  • a layer composed of an insulating layer or the like may be provided between the anode 12 and the substrate 11.
  • a layer such as an insulating layer can also be regarded as a part of the substrate 11.
  • the bank 13 is provided around each anode 12.
  • the bank 13 is also provided between the adjacent anodes 12.
  • a part of the bank 13 may cover the peripheral edge of the anode 12.
  • the bank 13 is a partition that partitions the pixel 2 or the pixel region 2a. That is, the bank 13 is provided on the substrate 11 in such a pattern as having an opening that partitions the pixel area 2 a set in advance on the surface 11 a of the substrate 11.
  • a lattice bank 13 is provided on the substrate 11.
  • the bank 13 is a cured product of a photosensitive resin composition containing a liquid repellent, for example.
  • An example of the liquid repellent is a liquid repellent containing a fluororesin.
  • an organic layer such as an organic light emitting layer 23 is formed on the pixel region 2a defined by the bank 13 by a coating method. Therefore, the bank 13 usually has characteristics (for example, wettability) that can suitably form the organic layer when the organic layer is formed on the pixel region 2a defined by the bank 13 using a coating method. It is formed as follows.
  • the shape of the bank 13 and its arrangement are appropriately set according to the specifications of the organic EL device 1 such as the number of pixels 2 and the resolution, the ease of manufacturing, and the like.
  • the side surface 13 a facing the pixel region 2 a of the bank 13 is substantially orthogonal to the surface 11 a of the substrate 11.
  • the side surface 13a may be inclined to form an acute angle with respect to the surface 11a, or may be inclined to form an obtuse angle.
  • the shape of the bank 13 is known as a forward taper type
  • the shape of the bank 13 has a reverse taper type.
  • An example of the thickness (height) of the bank 13 is about 0.3 ⁇ m to 5 ⁇ m.
  • the banked substrate 10 can be manufactured, for example, by forming the banks 13 after forming the anodes 12 on the plurality of pixel regions 2 a set in advance on the substrate 11.
  • the anode 12 can be formed by a vapor deposition method or a coating method.
  • the layer may be patterned into a pattern of a plurality of anodes 12.
  • the coating liquid containing the material of the anode 12 can be formed on the substrate 11 in a pattern corresponding to the plurality of anodes 12 and then dried.
  • a coating film made of a material to be the anode 12 may be formed on the substrate 11 and dried, and then patterned into the pattern of the anode 12.
  • examples of the coating method include an inkjet printing method, but other known coating methods such as a slit coating method, a micro gravure coating method, a gravure coating method, a bar coating method, and the like.
  • a coating method, a roll coating method, a wire bar coating method, a spray coating method, a screen printing method, a flexographic printing method, an offset printing method, a nozzle printing method, and the like may be used.
  • the solvent of the coating solution containing the material of the anode 12 may be any solvent that can dissolve the material of the anode 12.
  • the bank 13 is formed using, for example, a coating method. Specifically, it is formed by drying a coating film formed by coating a coating solution containing the material of the bank 13 on the substrate 11 on which the anode 12 is formed, and then patterning the coating film into a predetermined pattern. obtain.
  • the coating method may include a spin coating method and a slit coating method.
  • the solvent of the coating solution containing the bank 13 may be any solvent that can dissolve the material of the bank 13.
  • the plurality of organic EL structure portions 20 are provided in a recess 14 (see FIGS. 2 and 3) formed by the bank 13 and the anode 12 in the banked substrate 10.
  • the organic EL structure unit 20 includes a hole injection layer 21, a hole transport layer 22, and an organic light emitting layer 23.
  • the hole injection layer 21 is an organic layer having a function of improving the hole injection efficiency from the anode 12 to the organic light emitting layer 23.
  • a known hole injection material can be used as the material of the hole injection layer 21.
  • hole injection materials include oxides such as vanadium oxide, molybdenum oxide, ruthenium oxide, and aluminum oxide, phenylamine compounds, starburst amine compounds, phthalocyanine compounds, amorphous carbon, polyaniline, and polyethylenedioxy Mention may be made of polythiophene derivatives such as thiophene (PEDOT).
  • the thickness of the hole injection layer 21 varies depending on the material used, and is appropriately determined in consideration of the required characteristics and the ease of forming the layer.
  • the thickness of the hole injection layer 21 is, for example, 1 nm to 1 ⁇ m, preferably 2 nm to 500 nm, and more preferably 5 nm to 200 nm.
  • the hole injection layer 21 is provided with a different material or thickness for each type of pixel 2, that is, for each of the red pixel 2R, the green pixel 2G, and the blue pixel 2B, as necessary. From the viewpoint of simplicity of the formation process of the hole injection layer 21, all the hole injection layers 21 may be formed with the same material and the same thickness.
  • the hole transport layer 22 is a layer having a function of improving hole injection from the anode 12, the hole injection layer 21, or the hole transport layer 22 closer to the anode 12 to the organic light emitting layer 23.
  • a known hole transport material can be used as the material of the hole transport layer 22 .
  • the material of the hole transport layer 22 include: polyvinyl carbazole or a derivative thereof, polysilane or a derivative thereof, polysiloxane having an aromatic amine in a side chain or a main chain, or a derivative thereof, pyrazoline or a derivative thereof.
  • Arylamine or derivative thereof, stilbene or derivative thereof, triphenyldiamine or derivative thereof, polyaniline or derivative thereof, polythiophene or derivative thereof, polyarylamine or derivative thereof, polypyrrole or derivative thereof, poly (p-phenylene vinylene) or derivative thereof Derivatives, or poly (2,5-thienylene vinylene) or derivatives thereof may be mentioned.
  • hole transport layer materials disclosed in JP 2012-144722 A can be mentioned.
  • the thickness of the hole transport layer 22 varies depending on the material used, and is appropriately set so that the drive voltage and the light emission efficiency are appropriate.
  • the thickness of the hole transport layer 22 is, for example, 1 nm to 1 ⁇ m, preferably 2 nm to 500 nm, and more preferably 5 nm to 200 nm.
  • the hole transport layer 22 is provided with a different material or thickness for each type of pixel 2, that is, for each of the red pixel 2R, the green pixel 2G, and the blue pixel 2B, as necessary. From the viewpoint of simplicity of the formation process of the hole transport layer 22, all the hole injection layers 21 may be formed with the same material and the same thickness.
  • the organic light emitting layer 23 is provided on the hole transport layer 22.
  • the organic light emitting layer 23 is an organic layer having a function of emitting light of a predetermined wavelength.
  • the organic light emitting layer 23 is usually formed of an organic substance that mainly emits fluorescence and / or phosphorescence, or an organic substance and a dopant that assists the organic substance.
  • the dopant is added, for example, in order to improve the luminous efficiency and change the emission wavelength.
  • the organic substance contained in the organic light emitting layer 23 may be a low molecular compound or a high molecular compound. Examples of the light emitting material constituting the organic light emitting layer 23 may include the following dye materials, metal complex materials, polymer materials, and dopant materials.
  • dye-based luminescent materials include cyclopentamine or derivatives thereof, tetraphenylbutadiene or derivatives thereof, triphenylamine or derivatives thereof, oxadiazole or derivatives thereof, pyrazoloquinoline or derivatives thereof, distyrylbenzene or derivatives thereof.
  • the metal complex-based light emitting material examples include rare earth metals such as Tb, Eu, and Dy, or Al, Zn, Be, Pt, Ir, and the like as a central metal, and oxadiazole, thiadiazole, phenylpyridine, and phenylbenzimidazole. And a metal complex having a quinoline structure or the like as a ligand.
  • metal complexes include metal complexes having light emission from triplet excited states such as iridium complexes and platinum complexes, aluminum quinolinol complexes, benzoquinolinol beryllium complexes, benzoxazolyl zinc complexes, benzothiazole zinc complexes, azomethyl zinc complexes, A porphyrin zinc complex, a phenanthroline europium complex, etc. may be mentioned.
  • polymer light-emitting material examples include polyparaphenylene vinylene or derivatives thereof, polythiophene or derivatives thereof, polyparaphenylene or derivatives thereof, polysilane or derivatives thereof, polyacetylene or derivatives thereof, polyfluorene or derivatives thereof, polyvinylcarbazole or derivatives thereof. Derivatives, dye materials, materials obtained by polymerizing metal complex materials, and the like can be given.
  • red light emitting materials materials emitting red light
  • materials emitting red light include coumarin or derivatives thereof, thiophene ring compounds, and polymers thereof, polyparaphenylene vinylene or derivatives thereof, polythiophene or A derivative thereof, polyfluorene or a derivative thereof, and the like can be given.
  • polymer materials such as polyparaphenylene vinylene or derivatives thereof, polythiophene or derivatives thereof, and polyfluorene or derivatives thereof are preferable.
  • examples of the red light emitting material include materials disclosed in JP 2011-105701 A.
  • green light-emitting materials examples include quinacridone or derivatives thereof, coumarin or derivatives thereof, and polymers thereof, polyparaphenylene vinylene or derivatives thereof, polyfluorene or derivatives thereof, and the like. May be mentioned. Among them, polymer materials such as polyparaphenylene vinylene or a derivative thereof, polyfluorene or a derivative thereof are preferable. Examples of the green light emitting material include materials disclosed in JP2012-036388.
  • blue light-emitting materials include distyrylarylene or derivatives thereof, oxadiazole or derivatives thereof, polymers thereof, polyvinylcarbazole or derivatives thereof, polyparaphenylene or derivatives thereof. Derivatives, polyfluorene or derivatives thereof, and the like can be given. Among these, polyvinylcarbazole or a derivative thereof, polyparaphenylene or a derivative thereof, and polyfluorene or a derivative thereof are preferable. Examples of the blue light emitting material include materials disclosed in JP2012-144722A.
  • dopant materials include perylene or derivatives thereof, coumarin or derivatives thereof, rubrene or derivatives thereof, quinacridone or derivatives thereof, squalium or derivatives thereof, porphyrin or derivatives thereof, styryl dyes, tetracene or derivatives thereof, pyrazolone or derivatives thereof, decacyclene Alternatively, derivatives thereof, phenoxazone or derivatives thereof, and the like can be mentioned.
  • the organic light emitting layer 23 is provided according to the type of the pixel 2, that is, the red pixel 2R, the green pixel 2G, and the blue pixel 2B.
  • An organic light-emitting layer 23 that emits red light is provided on the hole transport layer 22 of the recess 14 corresponding to the red pixel 2R, and green is displayed on the hole injection layer 21 of the recess 14 corresponding to the green pixel 2G.
  • An organic light emitting layer 23 that emits light is provided, and an organic light emitting layer 23 that emits blue light is provided on the hole transport layer 22 of the recess 14 corresponding to the blue pixel 2B.
  • the organic light emitting layer 23 included in the red pixel 2R, the green pixel 2G, and the blue pixel 2B may be referred to as a red light emitting layer 23R, a green light emitting layer 23G, and a blue light emitting layer 23B.
  • the cathode 30 is provided on the organic light emitting layer 23.
  • the material of the cathode 30 is preferably a material having a low work function, easy electron injection into the organic light emitting layer 23, and high electrical conductivity. Further, as described in the present embodiment, when the organic EL device 1 takes out light from the anode 12 side, the light emitted from the organic light emitting layer 23 is reflected by the cathode 30 toward the anode 12 side.
  • the material of the cathode 30 is preferably a material having a high visible light reflectance.
  • an alkali metal, an alkaline earth metal, a transition metal, a Group 13 metal of the periodic table, or the like can be used.
  • a transparent conductive cathode made of a conductive metal oxide, a conductive organic material, or the like can be used.
  • the thickness of the cathode 30 is appropriately set in consideration of electric conductivity and durability.
  • the thickness of the cathode 30 is, for example, 10 nm to 10 ⁇ m, preferably 20 nm to 1 ⁇ m, and more preferably 50 nm to 500 nm.
  • the cathode 30 is formed on the entire display area where the plurality of pixels 2 are provided. That is, the cathode 30 is formed not only on the organic light emitting layer 23 but also on the bank 13 and is provided as the anode 12 common to the plurality of pixels 2.
  • the cathode 30 is provided on the organic light emitting layer 23.
  • a predetermined inorganic layer may be provided between the organic light emitting layer 23 and the cathode 30 provided thereon.
  • a sealing substrate is usually provided on the cathode 30 of the organic EL device 1.
  • the organic EL device 1 may have a known configuration provided in, for example, an organic EL panel display panel.
  • the organic EL device 1 having the above configuration, the structure in each pixel 2, that is, the pixel region 2a portion of the substrate 11, the anode 12, the organic EL structure portion 20, and the pixel region 2a portion of the cathode 30 constitute an organic EL element portion. is doing. Therefore, the organic EL device 1 has a configuration in which a plurality of organic EL element portions partitioned by the bank 13 are integrally connected with the substrate 11 and the anode 12 in common.
  • the minimum thickness of the organic light emitting layer 23 in the pixel 2, that is, the organic light emitting layer 23 in the recess 14 is d (nm), and the thickness direction of the substrate 11 is
  • the area of the organic light emitting layer 23 that is equal to or less than (d + predetermined value) [nm] is A1
  • the pixel area is A2
  • the flatness ⁇ (%) of the organic light emitting layer 23 is expressed by the following formula (I).
  • the flatness ⁇ is 70% or more.
  • ⁇ (A1 / A2) ⁇ 100 (I)
  • the pixel area is the area of the pixel region 2a, and is also the area of the region defined by the end 13b (see FIGS.
  • the predetermined value (nm) is preferably 2 or more and 15 or less. If it is this range, it will be easy to evaluate flatness more appropriately.
  • the predetermined value is more preferably 5 or more and 12 or less, and may be 10, for example.
  • the minimum thickness d (nm) of each of the red light emitting layer 23R, the green light emitting layer 23G, and the blue light emitting layer 23B may be different.
  • the flatness ⁇ of each of the red light emitting layer 23R, the green light emitting layer 23G, and the blue light emitting layer 23B is 70% or more.
  • the manufacturing method of the organic EL device 1 includes a step of forming the organic structure 40 (organic structure forming step) S10 and a step of forming the organic light emitting layer 23 (organic light emitting layer forming step). S12, a step of calculating the flatness ⁇ of the organic light emitting layer 23 (flatness calculation step) S14, a step of determining whether the flatness ⁇ is equal to or higher than a desired value (determination step) S16, and the cathode 30 are formed. Step (cathode formation step) S18.
  • an organic structure forming step S10 is performed.
  • the hole injection layer 21 and the hole transport layer 22 are provided on the anode 12 provided in the pixel region 2a, in other words, provided in the recess 14.
  • An organic structure 40 that is a laminate of the hole injection layer 21 and the hole transport layer 22 is formed in this order by a coating method.
  • a coating liquid containing a hole injection material is dropped on the anode 12 in the recess 14 to form a coating film, and then the coating film is dried to form the hole injection layer 21.
  • the coating method examples include an inkjet printing method.
  • other known coating methods such as a micro gravure coating method, a gravure coating method, a bar coating method, a roll coating method, a wire bar coating method, and a spray coating method are used.
  • the screen printing method, the flexographic printing method, the offset printing method, and the nozzle printing method may be used.
  • the screen printing method, the flexographic printing method, the offset printing method, and the nozzle printing method may be used.
  • the solvent used in the coating solution is not limited as long as the hole injection material can be dissolved.
  • a chloride solvent such as chloroform, methylene chloride, and dichloroethane
  • an ether solvent such as tetrahydrofuran
  • an aromatic hydrocarbon solvent such as toluene and xylene.
  • Ketone solvents such as acetone and methyl ethyl ketone
  • ester solvents such as ethyl acetate, butyl acetate, and ethyl cellosolve acetate.
  • the drying method of the coating film is not limited as long as the coating film can be dried, and examples thereof include vacuum drying and heat drying.
  • a coating liquid containing a hole transport material is dropped on the hole injection layer 21 in the recess 14 to form a coating film, and then the coating film is dried to form the hole transport layer 22.
  • the solvent and the drying method may be the same as those for the hole injection layer 21.
  • the structure obtained through the organic structure forming step S10 that is, the structure including the banked substrate 10 and the organic structure 40 formed in the recess 14 is referred to as an intermediate structure 3.
  • an intermediate structure 3 In the organic structure forming step S ⁇ b> 10, two intermediate structures 3 are prepared, and the thickness distribution of the organic structure 40 included in one of the intermediate structures 3 is measured in order to obtain the thickness of the organic light emitting layer 23. Keep it.
  • the organic light emitting layer forming step S12 is performed.
  • the organic light emitting layer 23 is formed on the organic structure 40 by a coating method. Specifically, a coating liquid containing a light emitting material to be the organic light emitting layer 23 is dropped into the recess 14 to form a coating film (coating film forming process), and then the coating film is dried (drying process). Then, the organic light emitting layer 23 is formed.
  • a red light emitting layer 23R and a green light emitting layer are respectively formed using a coating liquid containing a red light emitting material, a green light emitting material, and a blue light emitting material. 23G and the blue light emitting layer 23B are formed.
  • the coating method an inkjet printing method is exemplified, but other known coating methods exemplified in the case of the hole injection layer 21 can also be used.
  • the solvent used in the coating solution is not limited as long as it can dissolve the light emitting material, and may be the same as the solvent exemplified in the formation of the hole injection layer 21.
  • the drying method of the coating film is not limited as long as the coating film can be dried as in the case of the hole injection layer 21, and examples thereof include vacuum drying and heat drying.
  • a laminated body 41 composed of the organic structure 40 and the organic light emitting layer 23 is formed on the anode 12 in the recess.
  • the organic light emitting layer 23 is formed on the organic structure 40 included in each of the two intermediate structures 3 prepared in the organic structure forming step S10.
  • the thickness of the laminate 41 formed in the intermediate structure 3 used for the measurement of the thickness of the organic structure 40 is measured, and the thickness distribution of the laminate 41 is acquired.
  • the flatness calculating step S14 is performed.
  • the thickness distribution of the organic light emitting layer 23 is calculated. Specifically, the thickness of the organic light emitting layer 23 is based on the thickness distribution of the organic structure 40 acquired in the organic structure forming step S10 and the thickness distribution of the stacked body 41 acquired in the organic light emitting layer forming step S12. The distribution is calculated. That is, when viewed from the thickness direction of the substrate 11, the thickness of the organic light emitting layer 23 is calculated by calculating the difference in the thickness of the organic structure 40 from the thickness of the stacked body 41 at each position in the recess 14. Get the distribution. Next, the flatness ⁇ is calculated using the calculated thickness distribution of the organic light emitting layer 23 and the formula (I).
  • the determination step S16 is performed.
  • the determination step S16 it is determined whether or not the flatness ⁇ is greater than or equal to a desired value.
  • the “desired value” is 70%.
  • the flatness ⁇ is different in the red light emitting layer 23R, the green light emitting layer 23G, and the blue light emitting layer 23B, the flatness that is the smallest of the flatness ⁇ in the red light emitting layer 23R, the green light emitting layer 23G, and the blue light emitting layer 23B.
  • the flatness ⁇ is different in the red light emitting layer 23R, the green light emitting layer 23G, and the blue light emitting layer 23B.
  • the flatness ⁇ of the plurality of organic light emitting layers 23 corresponding to the same color can be regarded as the same flatness ⁇ because the formation conditions of the material of the coating liquid are the same. Therefore, for example, for one color, the flatness ⁇ of one organic light emitting layer 23 may be calculated. However, as in the case of different colors, a plurality of organic light emitting layers 23 may be sampled and the smallest flatness ⁇ among them may be used for the determination.
  • the step of forming the cathode 30 on the organic light emitting layer 23 (cathode formation step) S18 To implement.
  • the method for forming the cathode 30 include vapor deposition methods and coating methods similar to those for the anode 12.
  • the cathode 30 is formed over the organic light emitting layer 23 formed in the plurality of recesses 14. Thereby, the organic EL device 1 shown in FIGS. 1 and 2 is obtained.
  • the step of changing the formation condition of the organic light emitting layer 23 is the drying speed in the step of drying the coating film formed by dropping the light emitting material onto the recesses 14 by the coating method in the organic light emitting layer forming step S12.
  • FIG. 7 schematically shows the relationship between the drying rate and the thickness distribution of the organic light emitting layer.
  • the horizontal axis indicates the position of the recess 14 in the cross section
  • x1 and x2 indicate the positions of the side surfaces 13a and 13a of the bank 13 that define the recess 14, respectively.
  • the vertical axis indicates the thickness.
  • the thickness of the central portion of the organic light emitting layer 23 becomes thin and concave as shown schematically in the thickness distribution on the left side in FIG.
  • the organic light emitting layer 23 schematically shown in the thickness distribution on the right side in FIG. 7 tends to be convex due to the thick central portion. Therefore, the thickness distribution of the organic light emitting layer 23 can be adjusted by adjusting the drying speed based on the thickness distribution of the organic light emitting layer 23 used in the determination step S16.
  • the thickness shown in the center in FIG. The organic light emitting layer 23 having a flat thickness distribution like the thickness distribution can be realized.
  • composition ratio of the coating solution Other parameters that can be changed in the formation conditions of the organic light emitting layer 23 include, for example, the composition ratio of the coating solution.
  • the organic light emitting layer 23 is formed again under the changed forming conditions.
  • FIG. 4 the case where it returns to organic light emitting layer formation process S12 after formation condition change process S20 is illustrated as an example. If it is such a flowchart, in the organic structure formation process S10, the some intermediate structure 3 is produced, and it returns to the organic light emitting layer formation process S12, and the intermediate structure which has not formed the organic light emitting layer 23 What is necessary is just to form the organic light emitting layer 23 on the organic structure 40 which 3 has. Or you may return to organic structure formation process S10 after formation condition change process S20.
  • the inventors of the present application have conducted intensive studies and found that there is a certain relationship between the flatness ⁇ of the organic light emitting layer and the luminance distribution rate ⁇ .
  • the luminance distribution ratio beta, luminance distribution rate for calculating (or test) organic EL devices of the pixels (luminance distribution ratio calculation pixels) of when light is emitted, the maximum brightness of the pixel is I MAX, (I MAX ⁇ When an area having a luminance of 0.7) or higher is A3 and a pixel area is A4, the area is defined by the following formula (II). ⁇ (A3 / A4) ⁇ 100 (II)
  • the definition of the pixel area A4 is the same as the pixel area A3 in the organic EL device 1 used for calculating the luminance distribution rate ⁇ .
  • the hole injection layer 21, the hole transport layer 22, and the organic light emitting layer 23 were formed by forming a coating film using a coating solution corresponding to each layer by an ink jet printing method and vacuum drying.
  • a blue light emitting layer 23 ⁇ / b> B was used as the organic light emitting layer 23 in each recess 14. Therefore, the organic EL devices E1 to E4 are organic EL devices 1 that emit blue light.
  • the same hole injection material, hole transport material and blue light emitting material were used for the hole injection layer 21, hole transport layer 22 and organic light emitting layer 23 in the organic EL devices E1 to E4.
  • the composition ratio of the coating solution when forming the corresponding hole injection layer 21, hole transport layer 22, and organic light emitting layer 23 is different.
  • the temperature in the vacuum chamber was 13 ° C to 30 ° C.
  • the drying speed of the coating film was slow in the order of the organic EL device E1, the organic EL device E2, the organic EL device E3, and the organic EL device E4.
  • the flatness ⁇ of the organic light emitting layer 23 included in the organic EL devices E1 to E4 is as shown in Table 1.
  • the luminance distribution ratio ⁇ when the organic EL devices E1 to E4 are caused to emit light under the same conditions is as shown in Table 1.
  • the pixel areas A2 and A4 used in the calculation of the flatness ⁇ and the luminance distribution rate ⁇ were the same.
  • organic EL devices E5 to E9 shown in FIG. 8B were manufactured.
  • the configurations of the organic EL devices E5 to E9 are the same as those of the organic EL devices E1 to E4, except that the green light emitting layer 23G is used as the organic light emitting layer 23 instead of the blue light emitting layer 23B.
  • the organic EL devices E5 to E9 are organic EL devices 1 that emit green light.
  • the hole injection layer 21, the hole transport layer 22, and the organic light emitting layer 23 were formed by forming a coating film using a coating liquid corresponding to each layer by an ink jet printing method and vacuum drying. In the vacuum drying performed when forming the organic light emitting layer 23, the temperature in the vacuum chamber was 13 ° C to 30 ° C.
  • the same hole injection material and hole transport material as in the organic EL devices E1 to E4 were used.
  • the composition ratio of the coating liquid when forming the hole injection layer 21, the hole transport layer 22, and the organic light emitting layer 23 is different.
  • the organic EL device E5, the organic EL device E6, the organic EL device E7, the organic EL device E8, and the organic EL device E9 are sequentially formed. The drying speed was fast.
  • the flatness ⁇ of the organic light emitting layer 23 included in the organic EL devices E5 to E9 is as shown in Table 2.
  • Table 2 shows the luminance distribution ratio ⁇ when the organic EL devices E5 to E9 emit light under the same conditions as the organic EL devices E1 to E4.
  • the pixel areas A2 and A4 used in the calculation of the flatness ⁇ and the luminance distribution rate ⁇ were the same.
  • organic EL devices E10 to E14 shown in FIG. 8C were manufactured.
  • the configuration of the organic EL devices E10 to E14 is the same as that of the organic EL devices E1 to E5 except that the red light emitting layer 23R is used as the organic light emitting layer 23 instead of the blue light emitting layer 23B.
  • the organic EL devices E10 to E14 are organic EL devices that emit red light.
  • the hole injection layer 21, the hole transport layer 22, and the organic light emitting layer 23 (red light emitting layer 23R) are coated using a coating liquid corresponding to each layer by the ink jet printing method as in the case of the organic EL devices E1 to E4. After the film was formed, it was formed by vacuum drying. In the vacuum drying performed when forming the organic light emitting layer 23, the temperature in the vacuum chamber was 13 ° C to 30 ° C.
  • the same hole injection material and hole transport material as in the organic EL devices E1 to E4 were used.
  • the composition ratios of the coating liquids when forming the hole injection layer 21, the hole transport layer 22, and the organic light emitting layer 23 are different.
  • the coating film is formed in the order of the organic EL device E10, the organic EL device E11, the organic EL device E12, the organic EL device E13, and the organic EL device E14. The drying rate was slow.
  • the flatness ⁇ of the organic light emitting layer 23 included in the organic EL devices E10 to E14 is as shown in Table 3.
  • Table 3 shows the luminance distribution ratio ⁇ when the organic EL devices E10 to E14 emit light under the same conditions as the organic EL devices E1 to E4.
  • the pixel areas A2 and A4 used in the calculation of the flatness ⁇ and the luminance distribution rate ⁇ were the same.
  • FIG. 9 is a graph showing the relationship between the flatness ⁇ (%) and the luminance distribution rate ⁇ (%) shown in Tables 1 to 3.
  • the horizontal axis indicates the flatness (%)
  • the vertical axis indicates the luminance distribution rate (%).
  • the same symbols rectangles, triangles, etc.
  • subjected to each symbol has shown the number of the experiment example.
  • FIG. 10 is a drawing showing the thickness distribution of the organic light emitting layer 23 (blue light emitting layer 23B) in the organic EL devices E1 to E4.
  • FIG. 11 is a drawing showing the thickness distribution in the recess 14 of the organic light emitting layer 23 (green light emitting layer 23G) in the organic EL devices E5 to E9.
  • FIG. 12 is a drawing showing the thickness distribution in the recess 14 of the organic light emitting layer 23 (red light emitting layer 23R) in the organic EL devices E10 to E14. 10 to 12, the horizontal axis indicates the position of the recess 14 in the cross section, and the positions of x1 and x2 indicate the positions of the side surfaces 13a and 13a of the bank 13 that define the recess 14, respectively.
  • FIGS. 10 to 12 the positions of x1 and x2 vary due to experimental errors and plots, but in FIGS. 10 to 12, x1 and x2 are roughly arranged near the positions corresponding to the side surfaces 13a and 13a. Yes.
  • the vertical axis in FIGS. 10 to 12 represents the thickness of the organic light emitting layer 23.
  • the flatness ⁇ and the luminance distribution rate ⁇ are substantially linear, that is, one-to-one for each of blue, green, and red. Therefore, the luminance distribution rate ⁇ can be adjusted by determining the flatness ⁇ .
  • the materials of the blue light emitting layer 23B, the green light emitting layer 23G, and the red light emitting layer 23R are different. Therefore, the relationship between the flatness ⁇ and the luminance distribution rate ⁇ is satisfied without depending on the material of the organic light emitting layer 23.
  • the luminance distribution can be obtained by adjusting the flatness ⁇ of the organic light emitting layer 23 as described in the method of manufacturing the organic EL device 1.
  • a certain value or more can be realized as the rate ⁇ .
  • the flatness ⁇ is 70% or more
  • a luminance distribution rate ⁇ of 70% or more can be realized. Accordingly, the thickness of the layers below the organic light emitting layer 23 (in the example shown in FIG. 2, the hole injection layer 21 and the hole transport layer 22) is measured, and the layers made of different materials are made flat.
  • the productivity of the organic EL device 1 is significantly improved as compared with the case where the manufacturing conditions are adjusted every time.
  • the luminance distribution rate ⁇ of the manufactured organic EL device 1 can be estimated by evaluating the flatness ⁇ . Therefore, the manufacturing cost of the organic EL device 1 can also be reduced. This point will be described in comparison with a case where an organic EL device is manufactured once by forming a cathode on the organic light emitting layer, and then a luminance distribution rate is measured and fed back to the formation conditions of the organic light emitting layer.
  • the cathode In order to manufacture an organic EL device once by forming a cathode on the organic light emitting layer, the cathode must be formed at least on the organic light emitting layer. Therefore, after manufacturing, the luminance distribution ratio ⁇ of the organic EL device is calculated. As a result, if it is necessary to change the formation conditions of the organic light emitting layer, it is necessary to form a cathode again.
  • the luminance distribution rate ⁇ of the organic EL device 1 is estimated based on the relationship between the flatness ⁇ and the luminance distribution rate ⁇ at the stage where the organic light emitting layer 23 is formed. it can. As a result, unnecessary cathode formation can be omitted, and as a result, the manufacturing cost can be reduced.
  • the organic EL device 1 shown in FIG. 1 can be manufactured by the manufacturing method shown in FIG. Therefore, the configuration of the organic EL device 1 can be a configuration that contributes to an improvement in productivity. Further, since the flatness ⁇ of the organic light emitting layer 23 included in the organic EL device 1 is 70% or more, the organic EL device 1 can realize 70% or more as the luminance distribution ratio ⁇ .
  • the drying rate of the coating film was slow in the order of the organic EL devices E1 to E4.
  • the drying rate of the coating film was faster in the order of the organic EL devices E5 to E9.
  • the red light emitting layer 23R of the organic EL devices E10 to E14 was formed, the drying rate of the coating film was slower in the order of the organic EL devices E110 to E14. From FIG. 10 to FIG. 12, as shown in FIG.
  • the organic light emitting layer 23 tends to be formed so that the central portion is concave. It can be seen that the organic light-emitting layer 23 tends to be formed so that the central portion becomes convex as the drying speed of the coating film decreases. Therefore, for example, the flatness ⁇ of the organic light emitting layer 23 can be adjusted by adjusting the drying speed.
  • the hole injection layer and the hole transport layer are formed between the organic light emitting layer and the electrode of the banked substrate, they may not be formed.
  • the organic light emitting layer may be formed adjacent to the electrode of the substrate with bank.
  • the hole transport layer may not be formed, and the organic light emitting layer may be formed adjacent to the hole injection layer.
  • An electron injection layer may be provided between the organic light emitting layer and the cathode.
  • the electron injection layer is a layer having a function of improving electron injection efficiency from the cathode to the organic light emitting layer.
  • a known electron injection material can be used for the electron injection layer.
  • an electron carrying layer may be provided between an electron injection layer and an organic light emitting layer.
  • the electron transport layer is a layer having a function of improving electron injection from the cathode, the electron injection layer, or the electron transport layer closer to the cathode.
  • a known electron transport material can be used for the electron transport layer.
  • the first electrode of the banked substrate is the anode
  • the second electrode is the cathode
  • the first electrode may be a cathode
  • the second electrode may be an anode
  • the organic EL device has three types of pixels, that is, the red pixel 2R, the green pixel 2G, and the blue pixel 2B.
  • the color type is not particularly limited, and all the pixels The same color may be emitted.
  • the desired value in the determination step S16 has been described as 70%, the desired value is not limited to 70%. What is necessary is just to set according to the performance requested
  • the desired value is preferably 70% or more, and the desired value exceeding 70% is preferably 80%.
  • Examples of organic EL devices are not limited to organic display panels, and may be organic light emitting devices.
  • SYMBOLS 1 ... Organic EL device, 2 ... Pixel, 2a ... Pixel region, 10 ... Substrate with bank, 11 ... Substrate, 11a ... Surface, 12 ... Anode (first electrode), 13 ... Bank, 20 ... Organic EL structure DESCRIPTION OF SYMBOLS 21 ... Hole injection layer, 22 ... Hole transport layer, 23 ... Organic light emitting layer, 30 ... Cathode, 40 ... Organic structure, 41 ... Laminated body.

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  • Electroluminescent Light Sources (AREA)

Abstract

L'invention concerne un dispositif électroluminescent (EL) organique (1) qui est fabriqué par un procédé comprenant : une étape consistant à former une couche électroluminescente organique (23) par un procédé de revêtement sur une première électrode (12) disposée sur un substrat (10) pourvu de digues et disposée dans une région de pixel (2a) délimitée par les digues (13); une étape consistant à calculer le degré de planéité de la couche électroluminescente organique; une étape consistant à déterminer si le degré de planéité est supérieur ou égal à un degré de planéité souhaité; et une étape consistant à former une seconde électrode (30), le degré de planéité étant représenté par (A1/A2) × 100, où d (nm) est l'épaisseur minimale de la couche électroluminescente organique, A1 est l'aire d'une couche électroluminescente organique qui mesure (d + valeur prédéterminée) nm ou moins, et A2 est l'aire de la région de pixel, l'étape de formation de la seconde électrode étant effectuée quand le degré de planéité est supérieur ou égal à la valeur souhaitée à l'étape de détermination, et les conditions de formation de la couche électroluminescente organique étant modifiées pour former la couche électroluminescente organique quand le degré de planéité est inférieur à la valeur souhaitée à l'étape de détermination.
PCT/JP2016/082820 2015-11-13 2016-11-04 Procédé de fabrication de dispositif électroluminescent organique, et dispositif électroluminescent organique WO2017082173A1 (fr)

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