WO2021144993A1 - 自発光素子及び自発光素子の製造方法、並びに自発光表示パネル、自発光表示装置、電子機器 - Google Patents

自発光素子及び自発光素子の製造方法、並びに自発光表示パネル、自発光表示装置、電子機器 Download PDF

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WO2021144993A1
WO2021144993A1 PCT/JP2020/001615 JP2020001615W WO2021144993A1 WO 2021144993 A1 WO2021144993 A1 WO 2021144993A1 JP 2020001615 W JP2020001615 W JP 2020001615W WO 2021144993 A1 WO2021144993 A1 WO 2021144993A1
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layer
self
functional layer
luminous
light emitting
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PCT/JP2020/001615
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English (en)
French (fr)
Japanese (ja)
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孝介 三島
光洋 坂元
宗治 佐藤
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株式会社Ｊｏｌｅｄ
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Priority to PCT/JP2020/001615 priority Critical patent/WO2021144993A1/ja
Priority to CN202080091277.3A priority patent/CN114902805A/zh
Publication of WO2021144993A1 publication Critical patent/WO2021144993A1/ja

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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
    • H10K59/80—Constructional details
    • H10K59/805—Electrodes
    • H10K59/8052—Cathodes
    • 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

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  • the present invention relates to, for example, a self-luminous element such as an organic electroluminescent element (hereinafter referred to as "organic EL element”), a method for manufacturing the self-luminous element, and a self-luminous display panel in which the self-luminous element is arranged in a matrix on a substrate.
  • a self-luminous display device and an electronic device using the self-luminous display panel as an image display unit.
  • each organic EL element has a basic structure in which an organic light emitting layer containing an organic light emitting material (hereinafter, simply referred to as "light emitting layer”) is arranged between a pair of electrode pairs of an anode and a cathode, and a pair at the time of driving.
  • a current-driven self-luminous element that generates light by recombining holes injected into the light emitting layer from the anode and electrons injected into the light emitting layer from the cathode by applying a voltage between the electrode pairs. be.
  • Patent Document 1 discloses a structure in which an organic layer contains a compound of an alkali metal or an alkaline earth metal (hereinafter, referred to as "alkali metal or the like").
  • alkali metal or the like has a low work function and a high ability to inject and transport electrons from the cathode, so that the luminous efficiency of the organic EL element can be improved.
  • a buffer layer is provided between the electron transport layer and the light emitting layer so that alkali metals and the like in the electron transport layer do not diffuse to the light emitting layer due to high temperature and the light emitting characteristics are not deteriorated.
  • This buffer layer is composed of an organic compound such as Alq3, 4,4'-N, N'-dicarbazole-biphenyl (CBP), distyrylarylene (DSA), DPB, BAlq, or anthracene derivative compound Ir.
  • the functional layer including the light emitting layer, particularly the organic functional layer has a physical property that it easily absorbs and permeates water.
  • the alkali metal and the like contained in the electron transport layer have high activity and immediately react with the water contained in the functional layer to change their quality, resulting in deterioration of electron injection characteristics and shortening of the life of the organic EL display panel.
  • a solution in which a material having a specific function (functional material: not only an organic material but also an inorganic material) is dissolved or dispersed in a solvent hereinafter, simply referred to as a simple material).
  • a wet process in which (referred to as "ink") is applied by a printing device or the like to form a functional layer is often used.
  • the residual amount of water in the functional layer is vaporized. It is much more than the case of forming a film by a dry process (dry method) such as a method, and in the configuration of Patent Document 1 above, since the buffer layer is made of an organic compound, the water content in the organic layer below it is the buffer layer. It may permeate into the electron transport layer and react with an alkali metal or the like in the electron transport layer, resulting in deterioration of light emission characteristics.
  • a self-luminous element that can be converted into a self-luminous element a method for manufacturing the self-luminous element, a self-luminous display panel in which the self-luminous element is arranged in a matrix on a substrate, a self-luminous display device using the self-luminous display panel as an image display unit, and an electronic device.
  • the purpose is to provide equipment.
  • the self-luminous element is a self-luminous element in which a light emitting layer is arranged between an anode and a cathode, and is arranged between the light emitting layer and the cathode, and is made of an alkali metal or alkaline soil. It includes a first functional layer containing a fluoride of a metal selected from an earth metal or a rare earth metal, and a second functional layer arranged between the first functional layer and the cathode and containing a rare earth metal as a dope material. It is characterized by that.
  • the method for manufacturing a self-luminous element includes a first step of forming an anode, a second step of forming a light emitting layer above the anode, and an alkali metal on the light emitting layer.
  • the self-luminous element and the method for manufacturing the self-luminous element according to the above aspect by forming at least one functional layer by a wet process, the manufacturing cost is reduced, good luminous efficiency is ensured, and the life is extended. It is possible to provide a self-luminous element, a self-luminous display panel, a self-luminous display device, and an electronic device capable of the above.
  • FIG. 1 It is a block diagram which shows the whole structure of the organic EL display device which concerns on aspect of this disclosure. It is a schematic plan view which enlarged a part of the image display surface of the machine EL panel in the said organic EL display device.
  • (A) is a schematic cross-sectional view taken along the line AA of FIG. 2, and (b) is an enlarged view of the broken line circle C of (a).
  • (A) to (e) are partial cross-sectional views schematically showing a manufacturing process of an organic EL element.
  • (A) to (d) are partial cross-sectional views schematically showing the manufacturing process of the organic EL element following FIG.
  • FIG. 1 A) and (b) are partial cross-sectional views schematically showing the manufacturing process of the organic EL element following FIG.
  • FIG. 1 A to (d) are partial cross-sectional views schematically showing the manufacturing process of the organic EL element following FIG. It is a flowchart which shows the manufacturing process of an organic EL element. It is a figure which shows typically the laminated structure of the organic EL element which concerns on aspect of this disclosure. It is a table which shows the result of the comparative experiment for verifying the effect of the organic EL element which concerns on the aspect of this disclosure. It is a schematic diagram which shows the laminated structure which concerns on the 1st modification in the 2nd functional layer of an organic EL element. It is a schematic diagram which shows the laminated structure which concerns on the 2nd modification in the 2nd functional layer of an organic EL element.
  • FIG. 3 (b) of the organic EL display panel formed thereby. It is an enlarged view of a part.
  • (A) is a perspective view showing the state of the partition wall in the line bank system, and (b) is a perspective view showing the state of the partition wall in the pixel bank system.
  • each functional layer in an organic EL display panel is often formed by a dry process (dry method) such as vacuum deposition, but in recent years, with the progress of coating technology, especially printing equipment technology, wet Technology for forming each functional layer in a process is becoming widespread.
  • the wet process is a large display panel in which an ink in which an organic or inorganic functional material is dissolved or dispersed in a solvent is printed on a necessary place by a printing device or the like and then dried to form a functional layer.
  • the equipment cost can be suppressed and the material utilization rate is high, which is excellent in terms of cost.
  • the light emitting layer is formed by a printing process, it is partitioned by a partition wall so that inks of adjacent sub-pixels are not mixed, and the partition wall is also formed of a resin material by a wet process.
  • a cost advantage is achieved.
  • an electron transport layer in which an organic material is doped with an alkali metal having a low work function is formed between the cathode and the light emitting layer in order to facilitate the transfer of electrons to the light emitting layer.
  • this may be configured to maintain a good carrier balance and optimize the luminous efficiency in the light emitting layer.
  • each pixel arranged in a line is partitioned by a bank for each row, and the ink is applied in a band shape (line bank method). May be used.
  • the contact area with the functional layer that is the base of the light emitting layer becomes large, and the moisture in the functional layer moves to the electron transport layer, and the characteristics of the electron transport layer may be further deteriorated. Conceivable.
  • Such a problem is not limited to an organic EL display panel using an organic EL element as a light emitting element, but a quantum dot display panel in which the light emitting layer is composed of a quantum dot light emitting element (QLED: quantum dot-LED), etc. It can occur commonly for display panels that include elements and that form a functional layer by a wet process. Therefore, the inventors of the present application have diligently researched a configuration in which the luminous efficiency is good and the life is not shortened even when the line bank method is adopted while trying to reduce the cost by adopting the wet process. This is one aspect.
  • the self-luminous element according to one aspect of the present disclosure is a self-luminous element in which a light emitting layer is arranged between an anode and a cathode, and is arranged between the light emitting layer and the cathode, and is made of an alkali metal or alkaline soil. It includes a first functional layer containing a fluoride of a metal selected from an earth metal or a rare earth metal, and a second functional layer arranged between the first functional layer and the cathode and containing a rare earth metal as a dope material. ..
  • the manufacturing cost can be reduced, the luminous efficiency of the self-luminous element can be improved, and the life of the self-luminous element can be extended.
  • the film thickness of the first functional layer is 0.1 nm or more and 20 nm or less.
  • the metal fluoride while exhibiting the moisture blocking property of the metal fluoride in the first functional layer, the metal fluoride is partially reduced by the second functional layer containing a rare earth metal as a dope material, so that electron injectability is achieved. It is possible to obtain a self-luminous element having good luminous efficiency and not shortening its life. Further, in the self-luminous element according to another aspect of the present disclosure, in the above aspect, the film thickness of the second functional layer is 5 nm or more and 150 nm or less.
  • the second functional layer is arranged on the first layer portion arranged on the first functional layer and the first layer portion.
  • the proportion of the rare earth metal contained in the second layer portion is larger than the proportion of the rare earth metal contained in the first layer portion.
  • the second functional layer has the first layer portion, the second layer portion and the third layer portion in order from the side closer to the first functional layer.
  • the concentration of the rare earth metal in the film thickness direction of the second functional layer is appropriately reduced while exhibiting the water blocking property, and electrons are injected into the light emitting layer.
  • the concentration of the rare earth metal in the third layer portion by increasing the concentration of the rare earth metal in the third layer portion, the electron injection property from the cathode side into the second functional layer is improved, and the infiltration of water from the outside is prevented to extend the life of the self-luminous element. It can be extended further.
  • the content of the rare earth metal in the second functional layer continuously increases as it approaches the cathode from the first functional layer.
  • the water blocking property of the metal fluoride of the first functional layer is exhibited, and the first functional layer is allowed to exert a weak reducing property.
  • the electron injectability it is possible to further suppress the invasion of water into the second functional layer, and it is also possible to prevent the light transmission from being lowered more than necessary due to the increase in the doping amount of the rare earth metal.
  • the electron injection property from the cathode side into the second functional layer is improved, and the infiltration of water from the outside is prevented, so that the life of the self-luminous element can be further extended. be able to.
  • a transparent conductive film is formed as a third functional layer between the second functional layer and the cathode.
  • the film thickness of the third functional layer is 15 nm or more. According to this aspect, by adjusting the film thickness of the third functional layer, it is possible to construct an optical resonator structure according to the wavelength of the emission color.
  • the self-luminous element according to another aspect of the present disclosure is a thin film having a film thickness of 0.1 nm or more and 3 nm or less containing a rare earth metal between the second functional layer and the third functional layer in the above embodiment. Is formed. Further, in the self-luminous element according to another aspect of the present disclosure, in the above aspect, a thin film having a film thickness of 0.1 nm or more and 3 nm or less containing a rare earth metal is formed between the third functional layer and the cathode. There is.
  • a thin film having a film thickness of 0.1 nm or more and 5 nm or less containing a rare earth metal is formed on the opposite side of the cathode from the light emitting layer.
  • the anode has light reflectivity and the cathode has semitransparency.
  • the light emitted by the light emitting layer is reflected between the first luminous flux directly emitted from the cathode and between the anode and the cathode.
  • the film thickness of at least one functional layer including the second luminous flux emitted from the cathode and intervening from the light emitting layer to the cathode so that the first luminous flux and the second luminous flux resonate with each other. , It is set according to the wavelength of the emission color to emit the light.
  • an optical resonator composed of an interface between the anode and the interface of the cathode can be constructed, and the luminous efficiency of the self-luminous element can be further improved.
  • at least one functional layer interposed between the anode and the cathode is a coating film.
  • the fluoride of a metal selected from the alkali metal, alkaline earth metal or rare earth metal is NaF.
  • the rare earth metal is Yb.
  • a plurality of self-luminous elements according to the above aspect are arranged in a matrix, and at least the light emitting layers in the self-luminous elements adjacent to each other in the row direction extend in the column direction. It is separated by existing partition walls.
  • the self-luminous display panel according to another aspect of the present disclosure is a top emission type.
  • the aperture ratio of each self-luminous element can be increased and the luminous efficiency is excellent.
  • the self-luminous display device includes a self-luminous display panel according to the above aspect and a driving unit that drives the self-luminous display panel to display an image.
  • the electronic device includes the self-luminous display device as an image display unit in the above aspect. Such a self-luminous display device and an electronic device are excellent in luminous efficiency of the display panel and can extend the life.
  • the method for manufacturing a self-luminous element includes a first step of forming an anode, a second step of forming a light emitting layer above the anode, and an alkali metal on the light emitting layer. , A third step of forming a first functional layer containing a fluoride of a metal selected from an alkaline earth metal or a rare earth metal, and a second functional layer using a rare earth metal as a dope material on the first functional layer. The fourth step of forming and the fifth step of forming a cathode above the second functional layer are included.
  • the layer of the organic material is doped with a rare earth metal. It forms a second functional layer.
  • the fourth step an organic material and the rare earth metal are co-deposited on the first functional layer to form a second functional layer. Further, the step of forming a hole migration facilitating layer having a hole injecting property and / or a hole transporting function is further included between the first step and the second step, and the hole migration facilitating layer is further included. At least one of the second step, the third step, and the fourth step is executed by the wet process. This facilitates the reduction of manufacturing costs.
  • upper does not mean an upward direction (vertically upward) in absolute spatial recognition, but a relative positional relationship based on the stacking order in the laminated structure of the self-luminous element. Is specified by. Specifically, in the self-luminous element, the direction perpendicular to the main surface of the substrate and the direction from the substrate toward the laminate side is the upward direction. Further, for example, the expression “on the substrate” does not mean only the region directly in contact with the substrate, but also includes the region above the substrate via the laminate. Further, for example, when the expression “above the substrate” is used, it does not mean only the upper region separated from the substrate, but also includes the region on the substrate.
  • FIG. 1 is a block diagram showing an overall configuration of the organic EL display device 1.
  • the organic EL display device 1 is a display device used for, for example, a television, a personal computer, a mobile terminal, a commercial display (electronic signboard, a large screen for commercial facilities), and the like.
  • the organic EL display device 1 includes an organic EL display panel 10 and a drive control unit 200 electrically connected to the organic EL display panel 10.
  • the organic EL display panel 10 is a top emission type display panel having a rectangular image display surface on the upper surface.
  • a plurality of organic EL elements (not shown) are arranged along the image display surface, and the light emission of each organic EL element is combined to display an image.
  • the organic EL display panel 10 adopts an active matrix method as an example.
  • the drive control unit 200 has a drive circuit 210 connected to the organic EL display panel 10 and a control circuit 220 connected to an external device such as a computer or a receiving device such as an antenna.
  • the drive circuit 210 is a power supply circuit that supplies electric power to each organic EL element, a signal circuit that applies a voltage signal that controls the electric power supplied to each organic EL element, and a scan that switches a location where a voltage signal is applied at regular intervals. It has a circuit and so on.
  • the control circuit 220 controls the operation of the drive circuit 210 according to data including image information input from an external device or a receiving device.
  • four drive circuits 210 are arranged around the organic EL display panel 10 as an example, but the configuration of the drive control unit 200 is not limited to this, and the number of drive circuits 210 is not limited to this. And the position can be changed as appropriate. Further, for the sake of explanation below, as shown in FIG. 1, the direction along the long side of the upper surface of the organic EL display panel 10 is defined as the X direction, and the direction along the short side of the upper surface of the organic EL display panel 10 is defined as the Y direction. ..
  • FIG. 2 is a schematic plan view in which a part of the image display surface of the organic EL display panel 10 is enlarged.
  • the organic EL display panel 10 as an example, sub-pixels 100R, 100G, and 100B that emit light to R (red), G (green), and B (blue) (hereinafter, also simply referred to as R, G, and B) are arranged in a matrix. They are arranged in a shape.
  • the sub-pixels 100R, 100G, and 100B are arranged alternately in the X direction, and a set of sub-pixels 100R, 100G, and 100B arranged in the X direction constitute one pixel P.
  • the pixel P it is possible to express full color by combining the emission luminance of the sub-pixels 100R, 100G, and 100B whose gradation is controlled.
  • the sub-pixel row CR, the sub-pixel row CG, and the sub-pixel row CB are configured by arranging only one of the sub-pixel 100R, the sub-pixel 100G, and the sub-pixel 100B, respectively.
  • the pixels P of the organic EL display panel 10 as a whole are arranged in a matrix along the X and Y directions, and the image is displayed on the image display surface by combining the coloring of the pixels P arranged in the matrix. ..
  • Organic EL elements 2 (R), 2 (G), and 2 (B) (see FIG. 3) that emit light in the colors R, G, and B are arranged in the sub-pixels 100R, 100G, and 100B, respectively.
  • the organic EL display panel 10 employs a so-called line bank method. That is, a plurality of partition walls (banks) 14 for partitioning the sub-pixel rows CR, CG, and CB for each row are arranged at intervals in the X direction, and in each sub-pixel row CR, CG, and CB, the sub-pixels 100R, 100G, 100B shares a light emitting layer.
  • a plurality of pixel regulation layers 141 that insulate the sub-pixels 100R, 100G, and 100B are arranged at intervals in the Y direction, and the sub-pixels 100R, 100G, and 100B are arranged. It can emit light independently.
  • the height of the pixel regulation layer 141 is lower than the height of the liquid level when the light emitting layer is coated with ink.
  • the partition wall 14 and the pixel regulation layer 141 are represented by dotted lines, which is because the pixel regulation layer 141 and the partition wall 14 are not exposed on the surface of the image display surface and are inside the image display surface. Because it is arranged.
  • FIG. 3 (a) is a schematic cross-sectional view taken along the line AA of FIG.
  • one pixel is composed of three sub-pixels that emit light of R, G, and B, and each sub-pixel emits the corresponding color of the organic EL elements 2 (R) and 2 (G). ), 2 (B).
  • the organic EL elements 2 (R), 2 (G), and 2 (B) of each emission color basically have substantially the same configuration, they will be described as the organic EL element 2 when they are not distinguished.
  • the organic EL element 2 includes a substrate 11, an interlayer insulating layer 12, a pixel electrode (anode) 13, a partition wall 14, a hole injection layer 15, a hole transport layer 16, and a light emitting layer 17. It is composed of a first functional layer 18, a second functional layer 19, a counter electrode (cathode) 20, and a sealing layer 21.
  • the substrate 11, the interlayer insulating layer 12, the first functional layer 18, the second functional layer 19, the counter electrode 20, and the sealing layer 21 are not formed for each pixel, but are provided in the organic EL display panel 10. It is commonly formed in a plurality of organic EL elements 2.
  • the substrate 11 includes a base material 111 which is an insulating material and a TFT (Thin Film Transistor) layer 112. A drive circuit is formed in the TFT layer 112 for each sub-pixel.
  • the base material 111 includes, for example, a glass substrate, a quartz substrate, a silicon substrate, molybdenum sulfide, copper, zinc, aluminum, stainless steel, magnesium, iron, nickel, gold, silver and other metal substrates, gallium arsenic and other semiconductor substrates, and plastic substrates. Etc. can be adopted.
  • thermoplastic resin either a thermoplastic resin or a thermosetting resin may be used.
  • a laminated body in which one type or two or more types are laminated can be used.
  • the interlayer insulation layer 12 is formed on the substrate 11.
  • the interlayer insulating layer 12 is made of a resin material and is for flattening a step on the upper surface of the TFT layer 112.
  • the resin material include a positive type photosensitive material.
  • a photosensitive material an acrylic resin, a polyimide resin, a siloxane resin, and a phenol resin can be mentioned.
  • contact holes are formed in the interlayer insulating layer 12 for each sub-pixel.
  • the pixel electrode 13 includes a metal layer made of a light-reflecting metal material and is formed on the interlayer insulating layer 12.
  • the pixel electrode 13 is provided for each sub-pixel and is electrically connected to the TFT layer 112 through a contact hole (not shown). In this embodiment, the pixel electrode 13 functions as an anode.
  • the metal material having light reflectivity include Ag (silver), Al (aluminum), aluminum alloy, Mo (molybdenum), APC (alloy of silver, palladium and copper), ARA (silver, rubidium, gold). , MoCr (alloy of molybdenum and chromium), MoW (alloy of molybdenum and tungsten), NiCr (alloy of nickel and chromium) and the like.
  • the pixel electrode 13 may be composed of a metal layer alone, but as a laminated structure in which a layer made of a metal oxide such as ITO (indium tin oxide) or IZO (indium tin oxide) is laminated on the metal layer. May be good.
  • the partition 14 partitions a plurality of pixel electrodes 13 arranged for each sub-pixel above the substrate 11 for each row in the X direction (see FIG. 2), and is in the X direction. It is a line bank shape extending in the Y direction between the sub-pixel rows CR, CG, and CB arranged in the same direction.
  • An electrically insulating material is used for the partition wall 14.
  • an electrically insulating material for example, an insulating organic material (for example, acrylic resin, polyimide resin, novolak resin, phenol resin, etc.) is used.
  • the partition wall 14 functions as a structure for preventing the applied inks of each color from overflowing and mixing when the light emitting layer 17 is formed by the coating method.
  • the partition wall 14 preferably has resistance to an organic solvent and heat. Further, in order to suppress the outflow of ink, it is preferable that the surface of the partition wall 14 has a predetermined liquid repellency. In the portion where the pixel electrode 13 is not formed, the bottom surface of the partition wall 14 is in contact with the upper surface of the interlayer insulating layer 12.
  • the pixel regulation layer 141 is made of an electrically insulating material, covers the ends of the pixel electrodes 13 adjacent to the Y direction (FIG. 2) in each sub-pixel row, and partitions the pixel electrodes 13 adjacent to the Y direction. ..
  • the height of the pixel regulation layer 141 is slightly larger than the film thickness of the pixel electrode 13, but is lower than the position of the liquid surface when the ink of the light emitting layer is dropped on the opening 14a. Further, the height is higher than the height of the light emitting layer 17 after drying, and the insulating property between the light emitting layers 17 is ensured. As a result, the flow of ink when forming the light emitting layer 17 is not hindered by the pixel regulation layer 141. Therefore, it is easy to make the thickness of the light emitting layer 17 in each sub-pixel row uniform.
  • the pixel regulation layer 141 improves the electrical insulation of the pixel electrodes 13 adjacent to each other in the Y direction, suppresses the step breakage of the light emitting layer 17 in each of the sub-pixel rows CR, CG, and CB, and faces the pixel electrodes 13. It has a role of improving the electrical insulation between the electrode 20 and the like.
  • Specific examples of the electrically insulating material used for the pixel regulation layer 141 include a resin material and an inorganic material exemplified as the material of the partition wall 14. Further, when the light emitting layer 17 to be the upper layer is formed, it is preferable that the surface of the pixel regulation layer 141 has a liquid property to the ink so that the ink can be easily wetted and spread.
  • the hole injection layer 15 is provided on the pixel electrode 13 for the purpose of promoting the injection of holes from the pixel electrode 13 into the light emitting layer 17.
  • the hole injection layer 15 is formed by, for example, an oxide such as Ag (silver), Mo (molybdenum), Cr (chromium), V (vanadium), W (tungsten), Ni (nickel), Ir (iridium), or A layer made of a conductive polymeric material such as PEDOT (a mixture of polythiophene and polystyrene sulfonic acid). For example, it may be formed by a sputtering process or a wet process.
  • the hole injection layer 15 made of a metal oxide has a large work function and stably injects holes into the light emitting layer 17.
  • the hole transport layer 16 has a function of transporting holes injected from the hole injection layer 15 to the light emitting layer 17.
  • the hole transport layer 16 is formed by a wet process using, for example, polyfluorene or a derivative thereof, or a polymer compound such as polyarylamine or a derivative thereof, which does not have a hydrophilic group.
  • Light-emitting layer 17 is formed in the opening 14a and has a function of emitting light of each color of R, G, and B by recombination of holes and electrons. In particular, when it is necessary to specify and explain the emission color, the emission layers 17 (R), 17 (G), and 17 (B) are described.
  • an oxinoid compound for example, an oxinoid compound, a perylene compound, a coumarin compound, an azacumine compound, an oxazole compound, an oxadiazole compound, a perinone compound, a pyrolopyrrole compound, a naphthalene compound, an anthracene compound, a fluorene compound, Fluorantene compounds, tetracene compounds, pyrene compounds, coronene compounds, quinolones and azaquinolones, pyrazoline derivatives and pyrazolone derivatives, rhodamine compounds, chrysene compounds, phenanthrene compounds, cyclopentadiene compounds, styrubene compounds, diphenylquinone compounds, styryl compounds, butadiene compounds, Dicyanomethylenepyran compound, dicyanomethylenethiopyran compound, fluorescein compound, pyririum
  • the first functional layer 18 has a function of suppressing the movement of water from the lower organic layer to the second functional layer 19 and transporting electrons from the counter electrode 20 to the light emitting layer 17.
  • the first functional layer 18 contains a fluoride of a metal selected from an alkali metal, an alkaline earth metal, or a rare earth metal (hereinafter, referred to as “fluoride such as alkali metal”).
  • fluoride such as alkali metal have a dense crystal structure, low moisture permeability and excellent moisture blocking properties, and some alkali metals and the like are liberated by depositing a reducing material on the upper layer. It has the advantage of being excellent in electron injection.
  • NaF sodium fluoride
  • the first functional layer 18 is also configured to contain NaF in this embodiment.
  • ytterbium fluoride (YbF 3 ), lithium fluoride (LiF), and barium fluoride (BaF 2 ) are suitable.
  • alkali metal fluoride cerium fluoride (CeF 3 ), lithium fluoride (LiF), sodium fluoride (NaF), as alkaline earth metal fluoride, calcium fluoride (CaF 2 ), magnesium fluoride (MgF 2 ), barium fluoride (BaF 2 ), as rare earth metal fluoride, lanthanum fluoride (LaF 3 ), neodium fluoride (NdF 3 ), samarium fluoride (SmF 3 ), yttrium fluoride (YbF 3 ) , Yttrium fluoride (YF 3 ), gadolinium fluoride (GdF 3 ) and the like may be used.
  • the second functional layer 19 has a function of injecting and transporting electrons supplied from the counter electrode 20 toward the light emitting layer 17.
  • the second functional layer 19 is formed by using an organic material, particularly an organic material having electron transport property, as a host material and a rare earth metal as a dope material.
  • Rare earth metals generally have a low work function, excellent electron injection properties, and reducing properties, and thus have an action of dissociating fluorides such as alkali metals in the first functional layer 18.
  • it since it has high chemical stability as compared with alkaline earth metals such as Ba, it is difficult to react with moisture (high water resistance), and a long life can be expected.
  • Yb ytterbium
  • Yb is used as a dope material.
  • the rare earth metal other than Yb La (lantern), Nd (neodymium), Sm (samarium), Eu (europium), Gd (gadolinium), Ce (cerium), Lu (lutetium) and the like may be used. ..
  • organic material (host material) having electron transportability for example, a ⁇ -electron low molecular weight organic material such as an oxadiazole derivative (OXD), a triazole derivative (TAZ), and a phenanthroline derivative (BCP, Bphen) can be used. These include, but are not limited to.
  • OXD oxadiazole derivative
  • TEZ triazole derivative
  • BCP, Bphen phenanthroline derivative
  • the counter electrode 20 is made of a translucent conductive material and is formed on the second functional layer 19.
  • the counter electrode 20 functions as a cathode.
  • a metal thin film or a transparent conductive film such as ITO or IZO can be used.
  • a metal thin film made of at least one of aluminum, magnesium, silver, aluminum-lithium alloy, magnesium-silver alloy and the like is formed as the material of the counter electrode 20. Is desirable. In this case, the film thickness of the metal thin film is preferably 5 nm or more and 30 nm or less.
  • a transparent conductive film such as ITO or IZO is formed between the second functional layer 19 and the counter electrode 20 with a desired film thickness to face the light emitting layer 17. It is desirable to adjust the optical distance between the electrodes 20 to an appropriate size (for details, see the modified example (2) described later).
  • the sealing layer 21 prevents organic layers such as the hole transport layer 16, the light emitting layer 17, and the second functional layer 19 from being exposed to moisture or air and deteriorating. It is provided to do so.
  • the sealing layer 21 is formed by using a translucent material such as silicon nitride (SiN) or silicon oxynitride (SiON).
  • FIG. 3A is an enlarged view of a portion surrounded by a broken line circle C in FIG. 3A. Since the hole transport layer 16 and the light emitting layer 17 are formed by the wet process as described above, the pinnings (contact positions with the partition wall 14) P1 and P2 are higher than those of the central flat portion, respectively. Therefore, by observing the surface shape of each layer, it can be easily determined whether or not the layer is a coating film formed by the wet process.
  • FIGS. 4 (a) to (e), FIGS. 5 (a) to 5 (d), FIGS. 6 (a) and 6 (b) and FIGS. 7 (a) to 7 (d) are shown in the manufacture of the organic EL display panel 10. It is a schematic cross-sectional view which shows the state in a process. Further, FIG. 8 is a flowchart showing a manufacturing process of the organic EL display panel 10.
  • a TFT layer 112 is formed on the substrate 111 to prepare the substrate 11 (step S1 in FIG. 8).
  • the TFT layer 112 can be formed by a known method for manufacturing a TFT.
  • the interlayer insulation layer 12 is formed on the substrate 11 (step S2 in FIG. 8).
  • a resin material having a certain fluidity is applied, for example, by a die coating method so as to fill the unevenness on the substrate 11 by the TFT layer 112 along the upper surface of the substrate 11.
  • the upper surface of the interlayer insulating layer 12 has a flattened shape along the upper surface of the base material 111.
  • a contact hole (not shown) is formed in the interlayer insulating layer 12 by performing a dry etching method on a portion of the TFT element, for example, on the source electrode.
  • the contact hole is formed by patterning or the like so that the surface of the source electrode is exposed at the bottom thereof.
  • connection electrode layer is formed along the inner wall of the contact hole.
  • a part of the upper part of the connection electrode layer is arranged on the interlayer insulating layer 12.
  • a sputtering method can be used, and after forming a metal film, patterning may be performed using a photolithography method and a wet etching method.
  • the pixel electrode material layer 130 is formed on the interlayer insulating layer 12.
  • the pixel electrode material layer 130 can be formed by, for example, a vacuum vapor deposition method, a sputtering method, or the like.
  • the hole injection material layer 150 is formed on the pixel electrode material layer 130 (FIG. 4 (d)).
  • the hole injection material layer 150 can be formed by, for example, a reactive sputtering method or the like. Then, as shown in FIG. 4E, the pixel electrode material layer 130 and the hole injection material layer 150 are patterned by etching, and a plurality of pixel electrodes 13 and hole injection layers 15 partitioned for each sub-pixel are formed. And are formed (step S3 in FIG. 8).
  • the method of forming the pixel electrode 13 and the hole injection layer 15 is not limited to the above method.
  • the pixel electrode material layer 130 is patterned to form the pixel electrode 13, and then the hole injection layer 15 is formed. You may.
  • the partition 14 and the pixel regulation layer 141 are formed (step S4 in FIG. 8).
  • the pixel regulation layer 141 and the partition wall 14 are formed in separate steps.
  • a photosensitive resin material used as a material for the pixel regulation layer 141 is uniformly applied onto the interlayer insulating layer 12 on which the pixel electrode 13 and the hole injection layer 15 are formed.
  • the pixel regulation layer material layer 1410 having a thickness equal to the height of the pixel regulation layer 141 to be formed is formed.
  • a specific coating method for example, a wet process such as a die coating method, a slit coating method, or a spin coating method can be used. After application, for example, vacuum drying and 60 ° C. It is preferable that unnecessary solvent is removed by low-temperature heat drying (pre-baking) at about 120 ° C., and the pixel-regulating layer material layer 1410 is fixed to the interlayer insulating layer 12.
  • the pixel regulation layer material layer 1410 is patterned by using a photolithography method. For example, when the pixel regulation layer material layer 1410 has positive photosensitivity, the portion to be left as the pixel regulation layer 141 is shielded from light, and the portion to be removed is transparent through a photomask (not shown). 1410 is exposed.
  • the pixel regulation layer 141 can be formed by developing and removing the exposed region of the pixel regulation layer material layer 1410.
  • a developing solution such as an organic solvent or an alkaline solution that dissolves a portion exposed by exposure of the pixel regulation layer material layer 1410, and then a rinsing solution such as pure water is used.
  • the substrate 11 may be washed with.
  • firing (post-baking) at a predetermined temperature a pixel regulation layer 141 extending in the X direction can be formed on the interlayer insulating layer 12 (FIG. 5 (b)).
  • a partition wall 14 extending in the Y direction is formed in the same manner as the pixel regulation layer 141. That is, the partition wall 14 to be formed by applying a resin material for a partition wall on the interlayer insulating layer 12 on which the pixel electrode 13, the hole injection layer 15, and the pixel regulation layer 141 are formed by using a die coating method or the like.
  • a partition wall material layer 140 having a thickness equal to the height of the partition wall material 140 is formed (FIG. 5 (c)), and the partition wall 14 extending in the Y direction is patterned on the partition wall material layer 140 by a photolithography method, and then fired at a predetermined temperature.
  • the partition wall 14 is formed (FIG. 5 (d)).
  • the material layers of the pixel regulation layer 141 and the partition wall 14 are formed by a wet process and then patterned, but one or both of the material layers are formed by a dry process and a photolithography method is performed. The patterning may be performed by the etching method.
  • an ink containing the constituent material of the hole transport layer 16 is applied to the opening 14a defined by the partition wall 14 in a printing apparatus. It is discharged from the nozzle 3011 of the head 301 and applied onto the hole injection layer 15 in the opening 14a. At this time, the ink of the hole transport layer 16 is applied so as to extend along the Y direction (FIG. 2) above the pixel electrode row. Then, it is dried to form the hole transport layer 16 (step S5 in FIG. 8).
  • the light-emitting layer 17 is formed above the hole transport layer 16 (step S6 in FIG. 8). Specifically, as shown in FIG. 6B, ink containing a luminescent material having a luminescent color corresponding to each opening 14a is sequentially ejected from the nozzle 3011 of the coating head 301 of the printing apparatus into the opening 14a. Is applied on the hole transport layer 16. At this time, the ink is applied so as to be continuous even above the pixel regulation layer 141. As a result, the ink can flow along the Y direction, the uneven coating of the ink can be reduced, and the film thickness of the light emitting layer 17 in the same sub-pixel row can be made uniform.
  • the substrate 11 after the ink is applied is carried into a vacuum drying chamber and heated in a vacuum environment to evaporate the organic solvent in the ink.
  • the light emitting layer 17 can be formed.
  • the first functional layer 18 is formed on the light emitting layer 17 and the partition wall 14 (step S7 in FIG. 8).
  • the first functional layer 18 is formed by forming NaF in common with each sub-pixel by a vapor deposition method.
  • a second functional layer 19 is formed on the first functional layer 18 (step S8 in FIG. 8).
  • the second functional layer 19 is formed, for example, by forming an electron-transporting organic material and Yb, which is a dope metal, in common with each sub-pixel by a co-evaporation method. Further, Yb may be doped by a sputtering method or the like after first forming a film of an electron-transporting organic material.
  • Counter electrode forming step As shown in FIG. 7 (c), the counter electrode 20 is formed on the second functional layer 19 (step S9 in FIG. 8). In the present embodiment, the counter electrode 20 is formed by forming a film of silver, aluminum, or the like by a sputtering method or a vacuum vapor deposition method.
  • the sealing layer 21 is formed on the counter electrode 20 (step S10 in FIG. 8).
  • the sealing layer 21 can be formed by forming a film of SiON, SiN, or the like by a sputtering method, a CVD method, or the like. As a result, the organic EL display panel 10 is completed.
  • FIG. 9 is a diagram schematically showing a laminated structure of a main part (from a pixel electrode (anode) 13 to a counter electrode (cathode) 20) in the organic EL element 2.
  • an Al alloy is vapor-deposited on a glass substrate to form a pixel electrode (anode) 13, a hole injection layer 15, a hole transport layer 16, a light emitting layer 17, and a first.
  • the functional layer 18, the second functional layer 19, and the counter electrode (cathode) 20 are laminated in this order.
  • the first functional layer 18 was a NaF thin film having a film thickness of 2 nm, and was formed by a vacuum deposition method.
  • the second functional layer 19 was formed by co-depositing an organic material and Yb so as to have a film thickness of 15 nm.
  • the doping concentration of the doping metal Yb is 20 wt%.
  • the doping metal of the second functional layer 19 was Ba as the first functional layer 18 in FIG. 9 was not formed.
  • This Ba is an alkaline earth metal, has a sufficiently low work function, and has been widely used as an n-type dopant.
  • the doping metal of the second functional layer 19 was Yb without forming the first functional layer 18 in FIG.
  • the organic EL device according to Comparative Product 3 formed a first functional layer 18 made of NaF, and the doping metal of the second functional layer 19 was Ba.
  • the film thickness of the second functional layer of Comparative Products 1 to 3 and the doping concentration of the doping metal were set to 15 nm and 20 wt%, which are the same as those of the present product, respectively. Further, the film thickness of the first functional layer 18 in the comparative product 3 is 2 nm, which is the same as that of the implemented product.
  • FIG. 10 is a comparison table showing the results of the luminous efficiency, drive voltage, life, and comprehensive evaluation of the present product and the comparative products 1 to 3.
  • the luminous efficiency column shows the luminous efficiency at the initial stage of luminous flux (total luminous flux lm / W per unit power (lumen per watt)) as a comparative value when the luminous efficiency of the product is 100. There is.
  • the reciprocal of the drive voltage when a constant current is applied is shown as a comparative value when the implemented product is 100. Since the comparison is made by reciprocal, the higher the value in this column, the lower the drive voltage.
  • the life column shows the result of the acceleration experiment. Here, for example, it is determined that the life has been reached when the luminous efficiency becomes 80% or less of the initial value. In this case as well, it is shown as a comparison value when the life of the actual product is 100.
  • the doping metal of the second functional layer is Ba, but since it has the first functional layer made of NaF, the electron transport property is complemented, and the evaluation values in terms of luminous efficiency and drive voltage are obtained. Is higher, but slightly less than the examples. However, regarding the lifespan, there is still a difference of 30 points from the actual product. And, only this product was evaluated as " ⁇ " as a comprehensive evaluation.
  • the doping metal is Yb in terms of emission efficiency and drive voltage.
  • the evaluation is slightly higher in the case where the doping metal is Ba. This is because Yb, which is a rare earth, has lower activity than Ba, which is an alkaline earth metal, reacts with moisture in the process of manufacturing a light emitting device, is less likely to deteriorate, has a low voltage, and suppresses a decrease in the amount of electron current. It is considered that the decrease in efficiency is suppressed by this.
  • Yb which is a rare earth metal, has lower activity than Ba, which is an alkaline earth metal, and is less likely to be altered by reacting with moisture. Therefore, Yb is considerably superior to the doping metal from the viewpoint of life.
  • C When there is no first functional layer (comparative product 1, comparative product 2), the difference in life is 18% regardless of whether the doping metal of the second functional layer is Ba or Yb.
  • the first functional layer of NaF is provided (Comparative Product 3, Implemented Product)
  • the difference in life is up to 30% depending on whether the doping metal of the second functional layer is Ba or Yb. It is presumed that this is because the combination of NaF and Yb is compatible, and the synergistic effect thereof forms a long-life organic EL device having better resistance to moisture.
  • the film thickness of the first functional layer NaF forming the first functional layer 18 is transferred to the light emitting layer 17 as described above. It has electron injecting property and moisture blocking property, and its film thickness is preferably 0.1 nm or more and 20 nm or less. If the film thickness is less than 0.1 nm, it is too thin to sufficiently exert the effects of electron injection from the second functional layer 19 to the light emitting layer 17 and moisture blocking property to the second functional layer 19. If the film thickness exceeds 20 nm, the reducing action of the second functional layer does not sufficiently act on the first functional layer, and the electron injection property is deteriorated.
  • Film thickness of the second functional layer Yb which is a doping metal of the second functional layer 19, has excellent electron injection property from the counter electrode 20 which is a cathode, and has higher transparency than conventional Ba or the like.
  • the film thickness can be in the range of 5 nm or more and 150 nm or less. If the film thickness is less than 5 nm, it is too thin to sufficiently reduce NaF, which is the first functional layer, and sufficient electrons cannot be injected from the cathode. If the film thickness exceeds 150 nm, optical adjustment is performed. This is because it is difficult to take out light, the efficiency of light extraction is deteriorated, and the efficiency of light emission may be hindered.
  • the thickness of the second functional layer 19 is individually set for each of the emission colors of R, G, and B within this film thickness range by the optical design. It is also possible to set to to construct an optical resonance structure. Since the first functional layer 18 simultaneously has two functions of blocking the movement of water from the lower organic layer to the second functional layer 19 and injecting electrons into the light emitting layer 17, the first function is achieved. It is effective that the layer 18 is directly laminated on the light emitting layer 17 and the second functional layer 19 is directly formed on the first functional layer 18. As a result, it is not necessary to intervene an extra intermediate layer, so that the process load can be reduced.
  • Doping concentration of Yb in the second functional layer Yb has a low work function and excellent electron injection property, and its reactivity with water is considerably lower than that of alkali metals and the like. Therefore, the doping concentration of Yb is 1 wt% or more. , 90 wt% or less. If it is less than 1 wt%, the required electron injection property cannot be obtained, and if it exceeds 90 wt%, lumps of Yb are likely to be generated at the time of vapor deposition or the like, and it becomes difficult to evenly disperse it in the organic layer which is the host material. Is.
  • the first functional layer 18 made of NaF is formed on the light emitting layer 17, and the second functional layer 19 doped with Yb is formed on the first functional layer 18. is doing.
  • the NaF of the first functional layer 18 has a high water blocking ability and can increase the electron injectability by the reducing action of Yb. Therefore, while fulfilling the function of the electron transport layer, the light emitting layer 17 and the partition wall 14 under the first functional layer 18 have a high ability to block water. It is possible to suppress the infiltration of water from the organic layer of the pixel regulation layer 141 into the second functional layer 19.
  • Fluoride of a metal selected from an alkali metal other than NaF, an alkaline earth metal, or a rare earth metal can also be used because it has similar characteristics.
  • Yb which is a doping metal of the second functional layer 19, is a rare earth element and has a low work function, so that the electron injection property is good, the luminous efficiency is improved, and the drive voltage can be suppressed to a low level.
  • the first functional layer 18 suppresses the infiltration of water from the organic layer in the lower layer, and Yb itself has lower reactivity with water than alkali metals and the like, so that it is difficult to deteriorate. If it is a rare earth metal, the same effect can be obtained even if a metal other than Yb is doped. This is because rare earth metals have a low work function and have a reducing property, and mainly have chemical stability as a common property.
  • At least one organic layer of the organic EL element 2 is formed by a wet process to reduce the manufacturing cost, and the deterioration of the electron injection property of the second functional layer 19 due to the water content of the organic layer is suppressed to be organic.
  • the life of the EL element can be extended.
  • FIG. 11 is a schematic view showing a laminated structure of the organic EL element 2 according to the first modification. In the figure, only the laminated structure of the main part (from the pixel electrode 13 to the counter electrode 20) of the organic EL element 2 according to this modification is shown (FIGS. 19, FIG. 20, FIG. 24, and FIG. 25). Except, the same applies to the laminated structure diagram in other modified examples.)
  • the side of the second functional layer 19 in which the Yb doping concentration is in contact with the counter electrode 20 is X2 wt%, and the doping concentration decreases as the first functional layer 18 approaches the first functional layer.
  • the portion in contact with 18 is configured so that X1 wt% (1 ⁇ X1 ⁇ X2 ⁇ 90).
  • the temperature of the electric furnace for heating Yb and the temperature of the electric furnace for heating the organic material are controlled, respectively, to reduce the vapor deposition rate of Yb. This can be achieved by making the deposition rate of the organic material relatively slow.
  • FIG. 12 is a schematic view showing a laminated structure of the organic EL element 2 according to the second modification.
  • the second functional layer 19 has a two-layer structure of the first layer portion 191 and the second layer portion 192, and the Yb dope concentration (X2 wt%) of the second layer portion 192 is the first layer portion. It is higher than the Yb dope concentration (X1 wt%) of 191 (1 ⁇ X1 ⁇ X2 ⁇ 90).
  • the second layer portion 192 which is the region on the counter electrode 20 side of the second functional layer 19, has a higher Yb doping concentration than the first layer portion 191 which is the region on the first functional layer 18 side.
  • FIG. 13 is a schematic view showing a laminated structure of the organic EL element 2 according to the second modification.
  • the second functional layer 19 has a three-layer structure of the first layer portion 191 and the second layer portion 192, and the third layer portion 193, and the Yb of the first to third layer portions 191 to 193.
  • the dope concentrations are X1 wt%, X2 wt%, and X3 wt%, respectively, they are formed so as to satisfy the relationships of X2 ⁇ X1 ⁇ X3 and 1 ⁇ X1 ⁇ X3 ⁇ 90, 0 ⁇ X2.
  • the doping concentration of the second layer portion 192 between the first and third layer portions 191 and 193 is set to be the lowest, the amount of Yb doping of the entire second functional layer 19 is increased. It is possible to prevent the light transmission from being lowered more than necessary due to the increase. Since the doping concentration of the first layer portion 191 is high, it is possible to reduce the NaF of the first functional layer 18 while exhibiting the water blocking property, and improve the electron injection property into the light emitting layer. Further, by increasing the concentration of Yb in the third layer portion 193, the electron injection property from the cathode side into the second functional layer is improved, and the infiltration of water from the outside is prevented to extend the life of the organic EL element. The effect that it can be further extended can be obtained.
  • FIG. 14 is a schematic view showing a laminated structure according to another aspect of the organic EL element 2. As shown in the figure, a transparent conductive film 23 having a predetermined film thickness is formed between the second functional layer 19 and the counter electrode 20. The transparent conductive film 23 forms ITO, IZO, or the like by a magnetron sputtering method or the like.
  • the pair of the counter electrode 20 and the transparent conductive film 23 functions as a cathode, the combined sheet resistance is lowered, and it contributes to the prevention of the decrease in brightness due to the voltage drop. Since ITO and IZO have high transparency, a relatively large film thickness can be obtained, so that they can be used for adjusting the optical path length in the optical resonator structure.
  • the film thickness of the transparent conductive film 23 is preferably 15 nm or more. 40 nm or more is more desirable. By setting the film thickness of the transparent conductive film to 15 nm or more, cavity adjustment (film thickness adjustment for the optical resonator structure) can be effectively used, and high efficiency can be realized.
  • FIG. 15 is a diagram illustrating light interference in the optical resonator structure of the organic EL element 2 according to this modification.
  • the optical resonator structure is formed between the interface of the pixel electrode 13 with the hole injection layer 15 and the interface of the counter electrode 20 with the transparent conductive film 23.
  • FIG. 15 shows the main optical paths of the light emitted from the light emitting layer 17.
  • the optical path C1 is an optical path in which light emitted from the light emitting layer 17 toward the counter electrode 20 passes through the counter electrode 20 without being reflected.
  • the optical path C2 is an optical path in which light emitted from the light emitting layer 17 toward the pixel electrode 13 is reflected by the pixel electrode 13 and passes through the counter electrode 20 via the light emitting layer 17.
  • the counter electrode 20 has a semitransparent property that partially reflects the light coming from below.
  • such a counter electrode 20 can be achieved by forming a film thickness of 5 nm or more and 30 nm or less by a vapor deposition method using Ag or Al, an alloy thereof or the like as a material.
  • the optical path C3 is an optical path in which light emitted from the light emitting layer 17 toward the counter electrode 20 is reflected by the counter electrode 20, further reflected by the pixel electrode 13, and transmitted through the counter electrode 20 via the light emitting layer 17.
  • the difference in optical distance (optical path difference) ⁇ C1 between the optical path C1 and the optical path C2 corresponds to twice the length of the optical film thickness L1 shown in FIG.
  • the optical film thickness L1 is the total optical distance between the hole injection layer 15 and the hole transport layer 16 from the light emitting layer 17 to the interface with the hole injection layer 15 of the pixel electrode 13 (the thickness and refractive index of each layer). The total value of the products of).
  • the optical distance difference ⁇ C2 between the optical path C2 and the optical path C3 corresponds to twice the optical film thickness L2 shown in FIG.
  • the optical film thickness L2 is the optical distance between the first functional layer 18, the second functional layer 19, and the transparent conductive film 23 from the light emitting layer 17 to the interface of the counter electrode 20 with the transparent conductive film 23 (thickness and refraction in each layer). The total value of the product with the rate).
  • it is necessary to adjust so that the light passing through each of the optical paths C1, the optical path C2, and the optical path C3 is emitted from the organic EL element 2 in the same phase. Therefore, assuming that the target wavelength of the light emitted in FIG. 15 is ⁇ , it is reflected once in the optical path C2 and is deviated by half a wavelength. It is desirable that the optical path difference ⁇ C1 an integral multiple of ⁇ + ⁇ / 2.
  • the optical path difference ⁇ C1 is determined by the thickness of the hole injection layer 15 or the hole transport layer 16 and their refractive indexes.
  • the optical path difference ⁇ C2 is determined by the thickness and refractive index of the transparent conductive film 23 in FIG. It is desirable to be adjusted by. As described above, since the transparent conductive film 23 has high transparency, even if there is a slight difference in the film thickness of the thin film, the influence is small. Since the wavelength of each emission color is different, the hole injection layer 15, the hole transport layer 16, and the light emission in the organic EL element 2 corresponding to each emission color are changed in order to change the optical path differences ⁇ C1 and ⁇ C2 according to the wavelength. The film thickness of the layer 17 and the film thickness of the transparent conductive film 23 are determined.
  • the film thickness may be set so that the optical path difference ⁇ C2 satisfies the above-mentioned resonance condition instead of the transparent conductive film 23 or in combination with the transparent conductive film 23. Further, even when ITO or IZO is formed as a third functional layer on the second functional layer 19 by a sputtering method, the second functional layer 19 can alleviate the sputtering damage, so that the light emitting layer is protected.
  • FIG. 16 shows an example of the organic EL display panel 10 reflecting this optical resonator structure.
  • the hole injection layer 15 of the organic EL element 2 is positive in the order of red (R), green (G), and blue (B) according to the wavelength of the emission color so as to satisfy the above-mentioned optical resonance condition.
  • the total thickness of the hole transport layer 16 and the light emitting layer 17 is reduced.
  • FIG. 17 is a schematic view showing a laminated structure according to still another aspect of the organic EL element 2. The difference from the configuration of FIG. 14 is that an intermediate layer (Yb layer) 24 made of Yb is formed between the second functional layer 19 and the transparent conductive film 23.
  • Yb layer intermediate layer
  • the electron injection property from the counter electrode 20 is further improved, and the overall sheet resistance is reduced when the Yb layer 24, the transparent conductive film 23, and the counter electrode 20 are regarded as a set of cathodes. Even if the panel 10 is enlarged, the voltage drop in the center of the screen can be suppressed and better image quality can be obtained. Further, since Yb has a certain degree of water resistance, it prevents the infiltration of water from the upper layer (transparent conductive film 23, counter electrode 20, sealing layer 21), and causes the lower second functional layer 19 and the like. Deterioration of the light emitting layer 17 can be suppressed and the life can be extended.
  • the film thickness of the Yb layer 24 is preferably in the range of 0.1 nm or more and 3 nm or less. If it is less than 0.1 nm, the effects of reducing water resistance and sheet resistance cannot be expected so much, and if it exceeds 3 nm, it may affect the light transmission and rather reduce the luminous efficiency of the organic EL element 2. Because there is.
  • FIG. 17 is a schematic view showing a laminated structure according to still another aspect of the organic EL element 2.
  • the Yb layer 24 is formed between the transparent conductive film 23 and the counter electrode 20. Even with this configuration, the sheet resistance composed of the pair of the counter electrode 20 and the Yb layer 24 is reduced, so that the voltage drop is reduced, and even if the organic EL display panel 10 is enlarged, the voltage drop at the center of the screen is suppressed. , Better image quality can be obtained.
  • the water resistance of Yb prevents the infiltration of moisture from the upper layer (counter electrode 20, sealing layer 21), and suppresses deterioration of the transparent conductive film 23, the second functional layer 19, and the light emitting layer 17 of the lower layer. , The life can be extended. According to this configuration, the transparent conductive film 23 can also be protected from external moisture.
  • the film thickness of the Yb layer 24 in this modification is also preferably in the range of 0.1 nm or more and 3 nm or less for the same reason as in (3-1) above.
  • FIG. 19 is a schematic view showing a laminated structure according to still another aspect of the organic EL element 2.
  • the Yb layer 24 is formed on the outside of the counter electrode 20 (on the side opposite to the light emitting layer 17) and between the sealing layer 21 and the sealing layer 21.
  • the voltage drop due to the sheet resistance of the counter electrode 20 can be reduced, and even if the organic EL display panel 10 becomes large, the voltage drop at the center of the screen can be suppressed and better image quality can be obtained.
  • the Yb layer 24 is provided outside the counter electrode 20, it does not have the effect of reinforcing the electron injection property.
  • the water resistance of Yb prevents the infiltration of moisture from the upper layer (sealing layer 21), suppresses deterioration of the transparent conductive film 23, the second functional layer 19, and the light emitting layer 17 of the lower layer, and prolongs the service life. Can be planned.
  • the film thickness of the Yb layer 24 in this modification is preferably in the range of 0.1 nm or more and 5 nm or less. If it is less than 0.1 nm, the effects of reducing water resistance and sheet resistance cannot be expected so much, and if it exceeds 5 nm, it may affect the light transmission and rather reduce the luminous efficiency of the organic EL element 2. Because there is.
  • FIG. 20 is a schematic view showing a laminated structure according to still another aspect of the organic EL element 2.
  • the transparent conductive film 23 is formed on the outside of the counter electrode 20 (on the side opposite to the light emitting layer 17) and between the sealing layer 21 and the sealing layer 21.
  • the counter electrode 20 is formed of Ag (refractive index 0.05)
  • the transparent conductive film 23 is formed of IZO (refractive index 2.05)
  • the sealing layer 21 is SiN (refractive index).
  • the interface 23a between the counter electrode 20 and the transparent conductive film 23 and the interface 21a between the transparent conductive film 23 and the sealing layer 21 can serve as reflective surfaces.
  • each cavity has a spectrum having a different peak wavelength.
  • Light is generated, and light having a spectrum having a peak wavelength formed by synthesizing those spectra is output from the organic EL element 2. Therefore, by appropriately setting the refractive index and the film thickness of the counter electrode 20 and the transparent conductive film 23, it is possible to obtain the effect that the chromaticity of the output light can be finely adjusted.
  • the transparent conductive film 23 is made of an IZO film which is a transparent conductive film and is formed in direct contact with the counter electrode 20, the voltage drop due to the sheet resistance of the counter electrode 20 is reduced, and the organic EL display panel 10 is large. Even if the image quality is changed, the voltage drop in the center of the screen can be suppressed and better image quality can be obtained.
  • the transparent conductive film 23 may be another transparent conductive film, for example, an ITO film.
  • a single layer or a multi-layer rare earth metal layer containing another rare earth metal may be used.
  • the partition wall 14 and the pixel regulation layer 141 are formed in different steps, but the partition wall 14 and the pixels are formed by using a halftone mask.
  • the regulation layer 141 may be formed at the same time.
  • a resin material is applied on the interlayer insulating layer 12 on which the pixel electrode 13 and the hole injection layer 15 are formed by a wet process such as a die coating method to form a partition wall material layer 140 (see FIG. 5C). do.
  • the coating it is preferable that, for example, vacuum drying and low-temperature heat drying (pre-baking) at about 60 ° C. to 120 ° C. are performed to remove unnecessary solvents and the partition wall material layer is fixed to the interlayer insulating layer 12.
  • pre-baking vacuum drying and low-temperature heat drying
  • the partition material layer 140 is exposed through a photomask (not shown). For example, when the partition wall material layer 140 has positive photosensitivity, the portion where the partition wall material layer 140 is left is shielded from light, and the portion to be removed is exposed.
  • the pixel regulation layer 141 Since the pixel regulation layer 141 has a smaller film thickness than the partition wall 14, it is necessary to semi-expose the partition wall material layer 140 on the portion of the pixel regulation layer 141. Therefore, as a photomask used in the exposure process, a light-shielding portion arranged at a position corresponding to the partition wall 14 to completely block light, a translucent portion arranged at a position corresponding to the pixel regulation layer 141, and other parts. A halftone mask having a translucent portion arranged at a position corresponding to an exposed portion of the pixel electrode 13 of the above is used.
  • the translucency of the translucent portion is determined so that when exposed for a predetermined time, the partition wall material layer 140 on the pixel electrode 13 is fully exposed, and the pixel restricting layer 141 remains unexposed by the height thereof. NS.
  • a specific developing method for example, the entire substrate 11 is immersed in a developing solution such as an organic solvent or an alkaline solution that dissolves the exposed portion of the partition wall material layer 140, and then the substrate is rinsed with a rinsing solution such as pure water. 11 may be washed. Then, it is fired at a predetermined temperature.
  • the partition wall 14 extending in the Y direction and the pixel restricting layer 141 extending in the X direction can be formed on the interlayer insulating layer 12 in the same process. Since the number can be reduced, it contributes to cost reduction in manufacturing organic EL display panels.
  • the first functional layer 18, the second functional layer 19, the hole injection layer 15 and the hole transport layer 16 are provided as the laminated structure of the organic EL element. Although it is said that it has a configuration, it is not limited to this. For example, it may be an organic EL device that does not have the hole transport layer 16. Further, for example, a single hole injection transport layer may be provided instead of the hole injection layer 15 and the hole transport layer 16.
  • the stretching direction of the pixel regulation layer 141 is the long axis X direction of the organic EL display panel 10
  • the stretching direction of the partition wall 14 is the organic EL.
  • the stretching directions of the pixel regulation layer 141 and the partition wall 14 may be opposite to each other. Further, the stretching direction of the pixel regulation layer and the partition wall may be a direction irrelevant to the shape of the organic EL display panel 10.
  • the image display surface is rectangular as an example, but the shape of the image display surface is not limited and can be changed as appropriate.
  • the pixel electrode 13 is a rectangular flat plate-shaped member, but the present invention is not limited to this.
  • the hole injection layer 15 is formed by a dry process, but after the pixel electrode 13 is formed, the pixel regulation layer 141 and the partition wall 14 are formed, and then shown in FIG. 21 (a).
  • the hole injection layer 15 may be formed in the openings 14a between the adjacent partition walls 14 by a wet process.
  • the film shape of the hole injection layer 15 is also wet because the position P3 in contact with the partition wall 14 is located above the central flat portion. It can be easily known that the coating film is formed of.
  • sub-pixels 100R, 100G, and 100B that emit light in R, G, and B colors are arranged, but the emission color of the sub-pixels is not limited to this.
  • the emission color of the sub-pixels is not limited to this.
  • four colors of yellow (Y) may be used.
  • the number of sub-pixels is not limited to one per color, and a plurality of sub-pixels may be arranged.
  • the arrangement of the sub-pixels in the pixel P is not limited to the order of red, green, and blue as shown in FIG. 2, and may be in the order in which these are interchanged.
  • FIG. 22A shows a schematic partial perspective view at the stage where the pixel regulation layer 141 and the partition wall 14 are formed in the line bank type organic EL display panel 10. Since the pixel regulation layer 141 that defines the range of sub-pixels in the Y direction is lower in height than the partition wall 14, when ink is continuously applied to the opening 14a, the ink flows in the Y direction to increase the film thickness by leveling. It has the advantage of being easy to make uniform, but on the other hand, it also has the disadvantage that the area of contact between the light emitting layer 17 and the first functional layer 18 formed by the wet process becomes large, and moisture easily penetrates into the upper layer.
  • FIG. 22B is a partial perspective view schematically showing the shape of the partition wall 14 in the pixel bank system.
  • the light emitting layer 17 cannot be further expanded, and the contact area between the first functional layer 18 and the light emitting layer 17 is a line. Since it is limited as compared with the bank method, there is an advantage that the amount of water that may infiltrate into the first functional layer 18 is reduced, and deterioration of the first functional layer 18 and the second functional layer 19 is further suppressed. In this respect, it can be said to be superior to the line bank method.
  • FIG. 23 is a schematic cross-sectional view showing a laminated structure of a bottom emission type organic EL display panel. It differs from the top-emission type organic EL display panel 10 described with reference to FIG. 3 in the following points.
  • the counter electrode 20 does not have to be transparent, and may have reflectivity. As a result, the film thickness of the counter electrode 20 can be increased, a material having high conductivity can be used, and the sheet resistance can be reduced, so that the variation in brightness due to the voltage drop of the counter electrode 20 can be eliminated. In addition, the thicker film thickness can be expected to have a sealing effect by the counter electrode 20.
  • the pixel electrode 13 is formed of a transparent conductive film such as IZO or ITO, and the interlayer insulating layer 12 is formed of a transparent resin material.
  • a drive circuit for a light emitting element using a TFT is formed in a first region 1121 that overlaps with a partition wall 14 (or a pixel regulation layer 141) in a plan view, and a second region 1122 between them has translucency. In this way, it is configured so as not to block the emitted light.
  • the base material 111 is also formed of a translucent resin sheet or a glass sheet.
  • the counter electrode 20 may be a light-reflecting anode
  • the pixel electrode 13 may be made of a light-transmitting (including semi-light-transmitting) material to serve as a cathode.
  • the stacking order of the other hole injection layer 15, the hole transport layer 16, the first functional layer 18, and the second functional layer 19 is also the reverse of that shown in FIG. Since the material 111 is thick, there is an advantage that the sealing property is very high and the second functional layer 19 is less likely to deteriorate.
  • a color filter substrate or a polarizing plate is provided, if they are attached to the substrate 11 or the substrate 11 itself is also used as the color filter substrate or the polarizing plate, the configuration can be simplified and the cost can be reduced. Can be planned.
  • this bottom emission type organic EL display panel by making the counter electrode 20 also transparent, it is possible to provide a transmission type organic EL display panel.
  • a transmission type organic EL display panel For example, by arranging the transmissive organic EL display panel 10 on the windshield of a car, a car navigation guidance screen, a speedometer of the car, etc. can be displayed without obstructing the front view until driving is hindered. This makes it possible to further expand the fields of use of the organic EL display panel 10.
  • the sealing layer 21 is formed as a single layer using a translucent inorganic material such as silicon nitride (SiN) or silicon oxynitride (SiON), but these inorganic materials are sealed. Although it has excellent properties, it has the disadvantage that it is easily cracked by external force and is vulnerable to bending action. If the film thickness of the sealing layer of the inorganic material is increased in order to prevent the occurrence of cracks, the rigidity is increased and the flexibility is greatly impaired. Therefore, recently, a device has been made to reduce the film thickness of the inorganic material layer in the sealing layer and to absorb the impact due to the external force by stacking the resin material layers to ensure flexibility and prevent cracks from occurring. There is.
  • FIG. 24 is a schematic view showing an example of a laminated structure of an organic EL display panel (flexible display panel) 400 having excellent flexibility according to this modification.
  • the flexible display panel 400 includes a substrate 411, an interlayer insulating layer 412, a light emitting main portion 430, and a sealing layer 421.
  • the substrate 411 has a UC (undercoat) layer 4112 formed on the resin film 4111 which is a base material, and a TFT layer 4113 formed on the UC layer 4112.
  • the resin film 4111 is made of a resin material having flexibility and excellent heat resistance.
  • PET polyethylene terephthalate
  • a thin UC layer 4112 made of an inorganic material such as SiN or SiON is laminated on the resin film 4111 below. The infiltration of water from the water is blocked to protect the TFT layer 4113 from deterioration due to water.
  • a light emitting main portion 430 is arranged on the substrate 411 via an interlayer insulating layer 412.
  • the light emitting main part 430 has a laminated structure similar to that of the light emitting main part in the embodiment (see FIG. 9), and the hole injection layer 415 and the hole transport layer 416 are placed on the pixel electrode 413.
  • the light emitting layer 417, the first functional layer 418, the second functional layer 419, and the counter electrode 420 are laminated in this order. Since each of these components has the same contents as those described in the embodiments, detailed description thereof will be omitted.
  • a sealing layer 421 is formed on the counter electrode 420 of the light emitting main portion 430.
  • the sealing layer 421 has a three-layer structure of a first sealing layer 4211, a second sealing layer 4212, and a third sealing layer 4213.
  • the first sealing layer 4211 is formed by a dry process such as a sputtering method or a CVD method using a translucent inorganic material such as SiN or SiON
  • the second sealing layer 4212 is formed by, for example, a fluorine-based material or a fluorine-based material.
  • a translucent resin material such as an acrylic material or an epoxy material is formed on the first sealing layer 4211 by a wet process such as a coating method.
  • a third sealing layer 4213 is formed on the third sealing layer 4213 in the same manner as the first sealing layer 4211.
  • the base material of the substrate is formed of a resin film, and the sealing layer is flexible by sandwiching a film (organic material layer) made of a resin material between two thin films (inorganic material layer) made of an inorganic material.
  • the display panel having a structure for ensuring the property and the sealing property by adopting Yb as the dope metal of the second functional layer 419 as in the above embodiment, the water resistance is increased, so that the sealing layer 421 is also used, for example. Sufficient durability can be obtained by stacking the inorganic film and the organic film one by one. This makes it possible to simplify the sealing structure of the flexible display panel 400.
  • such a flexible display panel makes it easy to install in an automobile with many curves.
  • the temperature inside the vehicle may become high, but rare earth metals such as Yb generally have a standard reduction potential as compared with Ba (barium), which has been conventionally used as a dope metal. Since it is high, it is chemically stable even if the temperature rises a little, and it does not easily react with impurities such as moisture, so high temperature durability can be increased accordingly, and it can be used for a long time in a harsh temperature environment. It becomes.
  • a known resin film polarizing plate (more specifically, a circular polarizing plate formed by combining a linear polarizing plate and a quarter wave plate) may be further attached onto the sealing layer 421. do not have. As a result, the light incident on the inside of the flexible display panel 400 from the outside can be prevented from being reflected internally and emitted to the outside, and in particular, the visibility of the display image of the flexible display panel 400 outdoors can be improved. can. It also has the advantage of being able to suppress the intrusion of impurities such as moisture from the outside.
  • OCCF on-chip color filter
  • the light emitting main portion 430 in the flexible display panel 400 according to the present modification is not limited to the configuration shown in FIG. 9, and can be widely applied to all the configurations described in the modification.
  • FIG. 25 is a schematic view showing a laminated structure of a main part of a tandem type organic EL element 500, and the substrate and the sealing layer are not shown.
  • the organic EL element includes an anode (pixel electrode) 501, a hole injection transport layer 502, a light emitting layer 503, a NaF layer (first functional layer) 504, and a Yb-doped layer (second).
  • Functional layer) 505 charge generation layer 506, hole injection transport layer 507, light emitting layer 508, NaF layer (first functional layer) 509, Yb-doped layer (second functional layer) 510, and cathode (opposite electrode) 511. It is laminated in this order.
  • the charge generation layer 506 in the middle is formed of, for example, MoO 3 as an inorganic P-type oxide, supplies holes to the hole injection transport layer 507, and supplies holes to the Yb-doped layer 505. It has a function of supplying electrons.
  • the light emitting layer 503 emits B color (blue) light
  • the light emitting layer 508 emits Y color (yellow) light. Since blue and yellow are almost complementary colors, they are combined and finally light of a color close to white is emitted.
  • the combination of emission colors is not limited to this, and other emission colors may be freely combined to output light of a desired color. Even in the case of such a tandem type organic EL element 500, the combination of the Yb-doped layer and the NaF layer improves the electron injection property and durability, and can contribute to the improvement of luminous efficiency and the extension of life.
  • the organic EL display panel shown in the above embodiment can be used as a display panel for various electronic devices such as a display unit 601 of a television device 600 and other personal computers, mobile terminals, and commercial displays. Can be used.
  • the organic EL display panel 10 according to the above embodiment adopts an active matrix method, but the present invention is not limited to this, and a passive matrix method may be adopted.
  • QLED Quantum dot Light Emitting Diode
  • the present invention can be applied when the coating method is adopted for forming the light emitting layer and other functional layers.
  • the present invention can be applied when the coating method is adopted for forming the light emitting layer and other functional layers.
  • the self-luminous element according to the present disclosure can be widely used in a display panel used in various electronic devices.
  • Organic EL display device 2 Organic EL display panel 10
  • Organic EL display panel 11 Organic EL display panel 11
  • Organic EL display panel 12 Organic EL display panel 11
  • 411 Substrate 12 412 Thin film transistor 13, 413 Pixel electrode 14
  • 415 Hole injection layer 16, 416 Hole transport layer 17, 417
  • Sealing layer 4211 1st sealing layer 4212 2nd sealing layer 4213 3rd sealing layer 23 Transparent thin film transistor 24 Yb layer 100B, 100G, 100R Sub-pixel 111, 4111 Base material 112, 4113 TFT layer 4112 UC layer 140 Partition material layer 141 Pixel regulation layer 191 First layer part 192 Second layer part 193 Third layer part

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PCT/JP2020/001615 2020-01-17 2020-01-17 自発光素子及び自発光素子の製造方法、並びに自発光表示パネル、自発光表示装置、電子機器 WO2021144993A1 (ja)

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CN202080091277.3A CN114902805A (zh) 2020-01-17 2020-01-17 自发光元件及自发光元件的制造方法、以及自发光显示面板、自发光显示装置、电子设备

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Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2010278003A (ja) * 2009-06-01 2010-12-09 Samsung Mobile Display Co Ltd 有機発光素子
US20150318507A1 (en) * 2014-04-30 2015-11-05 Lg Display Co., Ltd. Organic light emitting display device
JP2019080027A (ja) * 2017-10-27 2019-05-23 株式会社Ｊｏｌｅｄ 有機電界発光素子、有機電界発光装置および電子機器
JP6633716B1 (ja) * 2018-10-26 2020-01-22 株式会社Ｊｏｌｅｄ 有機ｅｌ素子及び有機ｅｌ素子の製造方法、並びに有機ｅｌパネル、有機ｅｌパネルの製造方法、有機ｅｌ表示装置、電子機器

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Publication number Priority date Publication date Assignee Title
JP2010278003A (ja) * 2009-06-01 2010-12-09 Samsung Mobile Display Co Ltd 有機発光素子
US20150318507A1 (en) * 2014-04-30 2015-11-05 Lg Display Co., Ltd. Organic light emitting display device
JP2019080027A (ja) * 2017-10-27 2019-05-23 株式会社Ｊｏｌｅｄ 有機電界発光素子、有機電界発光装置および電子機器
JP6633716B1 (ja) * 2018-10-26 2020-01-22 株式会社Ｊｏｌｅｄ 有機ｅｌ素子及び有機ｅｌ素子の製造方法、並びに有機ｅｌパネル、有機ｅｌパネルの製造方法、有機ｅｌ表示装置、電子機器

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