WO2014185025A1 - Élément électroluminescent organique - Google Patents
Élément électroluminescent organique Download PDFInfo
- Publication number
- WO2014185025A1 WO2014185025A1 PCT/JP2014/002359 JP2014002359W WO2014185025A1 WO 2014185025 A1 WO2014185025 A1 WO 2014185025A1 JP 2014002359 W JP2014002359 W JP 2014002359W WO 2014185025 A1 WO2014185025 A1 WO 2014185025A1
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- WIPO (PCT)
- Prior art keywords
- substrate
- moisture
- organic light
- sealing wall
- organic electroluminescent
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Images
Classifications
-
- 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
- H10K59/87—Passivation; Containers; Encapsulations
- H10K59/871—Self-supporting sealing arrangements
- H10K59/8722—Peripheral sealing arrangements, e.g. adhesives, sealants
-
- 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
- H10K59/87—Passivation; Containers; Encapsulations
- H10K59/874—Passivation; Containers; Encapsulations including getter material or desiccant
Definitions
- the present invention relates to an organic electroluminescent device.
- the light emission characteristic is easily deteriorated in the presence of water such as water vapor. Furthermore, when the organic electroluminescent element is operated for a long time, the place where it is deteriorated by the moisture does not emit light. Such non-luminescent portions are called dark spots. Dark spots grow over time. Therefore, various methods have been proposed to suppress the generation and growth of dark spots due to moisture.
- Patent Document 1 proposes that a photocurable resin layer having moisture resistance be formed to cover an organic EL layer.
- the present invention has been made in view of the above points, and provides an organic electroluminescent device having fastness and capable of prolonging the life by suppressing the penetration of moisture into the organic light-emitting body. To aim.
- the organic electroluminescent device is A first substrate, An organic light emitter provided on the first substrate; A second substrate disposed opposite to the first substrate via the organic light emitter; A sealing wall provided between the first substrate and the second substrate so as to surround the organic light emitter; A hygroscopic part which is hygroscopic and covers the organic luminescent material, A moisture diffusing portion having moisture diffusibility and interposed between at least the second substrate and the hygroscopic portion; And the like.
- the water diffusion portion is preferably formed of a porous hard resin.
- At least one of the interface between the first substrate and the sealing wall and the interface between the sealing wall and the second substrate is formed in an uneven shape.
- the width between the inner side surface of the sealing wall and the side surface of the hygroscopic member is narrower than the width between the side surface of the hygroscopic member and the side surface of the organic light emitter, It is preferable that the thickness of the water diffusion part is thicker than the thickness of the moisture absorption part.
- ADVANTAGE OF THE INVENTION According to this invention, it has toughness and can suppress permeation of a water
- FIG. 1 shows an example of the organic electroluminescent element 1 in the embodiment of the present invention.
- the organic electroluminescent device 1 includes a first substrate 11, an organic light emitting body 20, and a second substrate 12 in layers, and further includes a sealing wall 3, a hygroscopic portion 4, and a moisture diffusion portion 5. ing.
- the first substrate 11 preferably has optical transparency.
- the first substrate 11 may be colorless or colored.
- the first substrate 11 may be transparent or translucent.
- Examples of the first substrate 11 include a glass substrate, a plastic substrate, and the like.
- As a material of a glass substrate soda lime glass, an alkali free glass etc. can be mentioned, for example.
- Examples of the material of the plastic substrate include polyethylene terephthalate (PET), polyethylene naphthalate (PEN), acrylic resin, epoxy resin, polyamide resin, fluorine resin and the like.
- PET polyethylene terephthalate
- PEN polyethylene naphthalate
- acrylic resin epoxy resin
- polyamide resin polyamide resin
- fluorine resin fluorine resin and the like.
- the shape of the first substrate 11 may be a rectangular shape in plan view, or any other shape.
- planar view means the case where the organic electroluminescent element 1 is seen in the direction (thickness direction) in which the first substrate 11, the organic light emitting body 20, and the
- the organic light emitting body 20 is provided on the first substrate 11. Specifically, the organic light emitting body 20 is formed by sequentially stacking, from the first substrate 11, a first electrode 21 functioning as an anode, an organic light emitting layer 23, and a second electrode 22 functioning as a cathode.
- the first electrode 21 may function as a cathode and the second electrode 22 may function as an anode.
- a portion where all of the first electrode 21, the organic light emitting layer 23 and the second electrode 22 overlap in a plan view is a light emitting area E (display area), and the other area is a non-light emitting area (non-display area). is there.
- the shape of the light emitting region E may be a rectangular shape in plan view, or any other shape.
- the organic light emitting body 20 refers to a stacked body of the first electrode 21, the organic light emitting layer 23, and the second electrode 22 in the light emitting region E.
- the 1st electrode 21 has light transmittance.
- the first substrate 11 is also light transmissive, it becomes a bottom emission type light extraction system, and light emitted from the organic light emitting layer 23 is transmitted through the first electrode 21 and the first substrate 11. It can be taken out outside.
- the material of the first electrode 21 include an electrode material composed of a metal having a large work function, an alloy, an electrically conductive compound, or a mixture thereof. As such a material, for example, CuI, ITO (Indium Tin Oxide), IZO (Indium Zinc Oxide), etc. can be mentioned.
- the second electrode 22 preferably has light reflectivity.
- the first substrate 11 and the first electrode 21 have light transmissivity, it becomes a bottom emission type light extraction system, and the light emitted from the organic light emitting layer 23 and directed to the second electrode 22 is transmitted.
- the first electrode 21 and the first substrate 11 can be transmitted and taken out to the outside.
- the material of the second electrode 22 include an electrode material made of a metal having a low work function, an alloy, an electrically conductive compound, or a mixture thereof. As such a material, sodium, lithium, magnesium, aluminum etc. can be mentioned, for example.
- the first electrode 21 may have light reflectivity, and the second electrode 22 may have light transparency.
- the moisture absorption part 4, the water diffusion part 5, and the second substrate 12 have light transmittance.
- each of the first electrode 21 and the second electrode 22 may have light transmittance.
- the first substrate 11, the moisture absorption unit 4, the moisture diffusion unit 5, and the second substrate 12 have light transmittance.
- a double-sided light emission type light extraction system is realized, and light emitted from the organic light emitting layer 23 can be extracted from both the first substrate 11 and the second substrate 12 to the outside.
- the organic light emitting layer 23 can be formed with the well-known material known as a material for organic electroluminescent elements.
- materials include, for example, anthracene, naphthalene, pyrene, tetracene, coronene, perylene, phthaloperylene, naphthaloperylene, diphenylbutadiene, tetraphenylbutadiene, coumarin, oxadiazole, bisbenzoxazoline, bisstyryl, cyclopentadiene, quinoline metal.
- Tri- (p-terphenyl-4-yl) amine Tri- (p-terphenyl-4-yl) amine, 1-aryl-2,5-di (2-thienyl) pyrrole derivative, pyran, quinacridone, rubrene, distyrylbenzene derivative, distyryl Arylene derivatives, and distyrylamine derivatives, various fluorescent dyes. Two or more of these materials may be used in combination.
- the organic light emitting layer 23 may be formed by a dry process such as a vapor deposition method or a transfer method, or may be formed by a wet process such as a coating method.
- one or more layers selected from a hole injection layer, a hole transport layer, an electron transport layer, and an electron injection layer may be interposed between the first electrode 21 and the second electrode 22. It can form by a well-known method using the well-known material known as a material for organic electroluminescent elements. As described above, since at least the organic light emitting layer 23 is interposed between the first electrode 21 and the second electrode 22, the first electrode 21 and the second electrode 22 are unlikely to be in direct contact with each other, and electrical Will be isolated. As shown in FIG. 1, an insulating layer 6 is formed of a known material on a part or all of the periphery of the organic light emitting layer 23, and the insulating properties of the first electrode 21 and the second electrode 22 are further increased by this insulating layer 6. It may be enhanced.
- the second substrate 12 is disposed to face the first substrate 11 via the organic light emitter 20.
- the second substrate 12 is also preferably light transmissive, but if the first substrate 11 is light transmissive, the second substrate 12 has light reflectivity. It may be In this case, as described above, the bottom emission type light extraction system is used.
- a glass substrate, a metal substrate, a resin substrate or the like can be used as the second substrate 12.
- soda lime glass, an alkali free glass etc. can be mentioned, for example.
- a material of a metal substrate aluminum, stainless steel, etc. can be mentioned, for example.
- the material of the resin substrate examples include polyethylene terephthalate (PET) and polyethylene naphthalate (PEN).
- PET polyethylene terephthalate
- PEN polyethylene naphthalate
- the second substrate 12 is formed of a resin substrate, a SiON film or a SiN film may be formed on the surface of the second substrate 12 to suppress the permeation of moisture.
- the second substrate 12 may have a rectangular shape in a plan view, or another shape.
- the sealing wall 3 is provided between the first substrate 11 and the second substrate 12 so as to surround the organic light emitting body 20.
- the sealing wall 3 can prevent moisture outside the organic electroluminescent element 1 from intruding into the organic light emitter 20.
- the sealing wall 3 is preferably formed of a material having a moisture permeability of 60 g / m 2 ⁇ 24 hours or less.
- the moisture permeability can be measured by the moisture permeability test method (cup method) of the moisture-proof packaging material defined in JIS Z0208.
- an ultraviolet curable resin etc. can be mentioned, for example. Specific examples thereof include resin materials such as epoxy resin and acrylic resin, wax materials such as paraffin wax and microcrystalline wax, and frit materials such as glass frit.
- the sealing wall 3 may contain an inorganic filler such as alumina, or a hygroscopic agent such as calcium oxide, strontium oxide, barium oxide or silica.
- the sealing wall 3 can be formed by, for example, a dispensing method, a printing method, an inkjet method, or the like.
- a first electrode lead-out portion 211 is formed at an end portion of the first substrate 11 outside the sealing wall 3.
- the first electrode lead portion 211 is formed by drawing the first electrode 21 inside the sealing wall 3 to the outside.
- a second electrode lead-out portion 222 is formed at the other end of the first substrate 11 outside the sealing wall 3.
- the second electrode lead-out portion 222 is formed by pulling out the second electrode 22 inside the sealing wall 3 to the outside. Electric power is supplied through the first electrode lead-out portion 211 and the second electrode lead-out portion 222 to apply a voltage between the first electrode 21 and the second electrode 22 of the organic light emitting body 20 to cause the organic light emitting layer 23 to emit light. be able to.
- the hygroscopic part 4 has hygroscopicity, preferably further has light transparency, and covers the whole of the organic light emitting body 20.
- the moisture absorption part 4 is solid. In this case, even if the moisture passes through the sealing wall 3 and enters inside, the moisture absorption part 4 can further suppress the moisture from entering the organic light emitting body 20.
- the moisture absorption part 4 can be formed with the resin material containing a moisture absorption agent (drying agent).
- the hygroscopic agent may be one that chemically adsorbs moisture or one that physically adsorbs it, and examples thereof include alkali metals such as calcium oxide, strontium oxide, barium oxide, sodium oxide, potassium oxide, sodium sulfate, calcium sulfate, etc.
- alkali metals such as calcium oxide, strontium oxide, barium oxide, sodium oxide, potassium oxide, sodium sulfate, calcium sulfate, etc.
- the powder particle containing an alkaline-earth metal, a zeolite, etc. can be mentioned.
- the resin material include thermosetting resins that cure by heating at a temperature of 100 ° C. or less and ultraviolet curable resins.
- Such a resin material is preferably one that is hard to permeate moisture, and examples thereof include epoxy resin, alkali resin, silicone resin and the like.
- the hygroscopic agent is preferably contained in an amount of 30% by mass or more and less than 95% by mass with respect to the total amount of materials constituting the hygroscopic portion 4.
- the moisture absorbent portion 4 can be formed, for example, by a dispensing method, a printing method, a sputtering method, a spin coating method, a dipping method, a spraying method, or the like.
- a moisture diffusing portion 5 having moisture diffusibility, preferably further having light permeability is interposed between the second substrate 12 and the moisture absorbing portion 4. I have to. Then, the moisture which has passed through the sealing wall 3 can be diffused and moved to the inside of the light emitting area E by the water diffusing unit 5, and the moisture absorbing part 4 inside the light emitting area E can be effectively used. Can. As a result, moisture is less likely to enter the organic light emitting body 20, and the lifetime of the organic electroluminescent device 1 can be extended.
- the moisture diffusion unit 5 may be interposed at least between the second substrate 12 and the moisture absorption unit 4, for example, as shown in FIG. 2, the inner side surface of the sealing wall 3 and the side surface of the moisture absorption unit 4 There may be a gap 7 between them.
- the moisture that has passed through the sealing wall 3 and entered the air gap 7 is absorbed as it is by the moisture absorption part 4 outside the light emission area E or is diffused and moved to the inside of the light emission area E by the water diffusion part 5 once. After that, the moisture is absorbed by the moisture absorbing portion 4 inside the light emitting region E or the like.
- the water diffusion portion 5 is interposed between the second substrate 12 and the moisture absorption portion 4, the second substrate 12 is less likely to be dented on the first substrate 11 side, and the fastness of the organic electroluminescent element 1 is obtained. You can also get it.
- the robustness in this case is a concept including pressure resistance. More specifically, the water diffusion portion 5 is preferably a solid, and such a solid water diffusion portion 5 is between the second substrate 12 and the moisture absorption portion 4 in the thickness direction of the organic electroluminescent element 1. Is preferably filled without gaps. In this case, even if the pressure is applied to the organic electroluminescent element 1 from both sides in the thickness direction, the second substrate 12 contacts the organic light emitting layer 20 and the organic light emitting layer 20 is damaged.
- the solid water diffusion unit 5 inhibits the contact between the second substrate 12 and the organic light emitting layer 20.
- the solid water diffusion unit 5 absorbs moisture with at least the second substrate 12 in the thickness direction of the organic electroluminescent element 1. It may be filled without a gap between the part 4 and, as shown in FIG. 2, the void 7 may be present between the inner side surface of the sealing wall 3 and the side surface of the hygroscopic part 4 .
- the second substrate 12 may be dented on the side of the first substrate 11 and may be in contact with the organic light emitting layer 20, and the organic light emitting layer 20 may be damaged.
- the water diffusion portion 5 is preferably formed of a porous hard resin.
- a water diffusion unit 5 coats, for example, particles having an average particle diameter of 10 to 100 ⁇ m with an ultraviolet curable resin such as an ultraviolet curable epoxy resin, and the coated particles are dispersed on the surface of the moisture absorbent 4 It can be formed.
- the particles described above are preferably materials that do not easily adsorb moisture, such as metals and silica. In this manner, when the water diffusion portion 5 is formed, a large number of fine holes included in the hard resin serve as a passage of water, so that the water does not easily stay, and the water diffusibility can be further improved. Moreover, since the water diffusion portion 5 is hard, the fastness can be further improved.
- an average particle diameter means the particle size in 50% of the integration value in the particle size distribution calculated
- the moisture diffusion part 5 may be formed using a porous sheet formed by sintering polyethylene particles etc. to a thickness of 1000 ⁇ m or less .
- the solid moisture diffusion portion 5 in the thickness direction of the organic electroluminescent element 1 It is preferable to be filled without gaps with the hygroscopic member 4.
- the gap in this case does not mean the large number of fine holes possessed by the hard resin. These holes are secured as a water passage without being blocked.
- the interface between the first substrate 11 and the sealing wall 3 and the interface between the sealing wall 3 and the second substrate 12 may be formed flat, but these interfaces It is preferable to form in the uneven
- the interface between the first substrate 11 and the sealing wall 3 and the interface between the sealing wall 3 and the second substrate 12 are formed in a concavo-convex shape, moisture hardly passes through these interfaces, Infiltration of the inside of the sealing wall 3 can be suppressed. It is more preferable that both of the above interfaces be formed in a concavo-convex shape, but at least one of the interfaces may be formed in a concavo-convex shape.
- a glass frit is previously applied to a portion where the sealing wall 3 of the first substrate 11 and the second substrate 12 is provided and then fired to have a height of 10 to 200 ⁇ m.
- a bank-like protrusion 8 may be formed.
- the gap between the tip of the protrusion 8 formed on the first substrate 11 and the second substrate 12 and the gap between the first substrate 11 and the tip of the protrusion 8 formed on the second substrate 12 are 20 ⁇ m or less Is preferred.
- the gap between the first substrate 11 and the second substrate 12 is preferably 200 ⁇ m or less.
- the first substrate 11 and the sealing wall 3 in addition to the case where the first substrate 11 and the sealing wall 3 are in direct contact, the first substrate 11 and the sealing wall 3
- the case where the first electrode 21 is interposed is also included.
- the width W 1 between the inner side surface of the sealing wall 3 and the side surface of the hygroscopic member 4 is the side surface of the hygroscopic member 4 and the side surface of the organic light emitting body 20 it is preferably narrower than the width W 2 between.
- W 1 ⁇ W 2 it is possible to promote the diffusion of water to the inside of the light emitting area E by the water diffusing unit 5 while sufficiently securing the moisture absorbing part 4 outside the light emitting area E. it can.
- the thickness T 1 of the moisture diffusion portion 5 be thicker than the thickness T 2 of the moisture absorption portion 4.
- the thickness T 1 of the water diffusion portion 5 is preferably 20 to 200 ⁇ m, and the thickness T 2 of the moisture absorption portion 4 is preferably 10 to 100 ⁇ m.
- a transparent conductive film such as ITO is formed on the surface of the first substrate 11 such as a glass substrate and patterned by photolithography to form the first electrode 21 and the first electrode lead-out portion 211.
- an organic light emitting layer 23 is formed on the surface of the first electrode 21 by vapor deposition or the like using a predetermined material.
- one or more layers selected from a hole injection layer, a hole transport layer, an electron transport layer, and an electron injection layer may be appropriately formed, or the insulating layer 6 may be formed.
- a second electrode 22 and a second electrode lead-out portion 222 are formed by depositing a metal film of aluminum or the like on the surface of the organic light emitting layer 23 by a vapor deposition method or the like.
- the organic light emitting body 20 can be formed on the surface of the first substrate 11.
- a resin material containing a hygroscopic agent is applied by a screen printing method or the like so as to cover the whole of the organic light emitting body 20, and then the resin material is cured by heating or ultraviolet irradiation to form the hygroscopic portion 4. .
- the thickness T 2 of the moisture absorption part 4 formed in this manner is preferably 10 to 100 ⁇ m as described above.
- the uncured moisture diffusion portion 5 is formed by spraying the particles coated with the ultraviolet curable resin so as to cover the entire cured moisture absorbing portion 4. Spraying the particles is preferably carried out to a thickness T 1 shown in FIG 1 is about 100 ⁇ 1000 .mu.m.
- the ultraviolet curable resin which is a material of the sealing wall 3 is apply
- the first substrate 11 and the second substrate 12 having the same size as above are placed in a vacuum chamber whose pressure is reduced to about 1 Pa, and the first substrate 11 and the second substrate are separated via the organic light emitter 20. 12 is placed in close contact with each other.
- the ultraviolet curable resin which is the material of the sealing wall 3
- the uncured water diffusion portion 5 can be sealed.
- the water diffusion portion 5 is crushed by both the moisture absorption portion 4 and the second substrate 12, but the thickness T 1 of the water diffusion portion 5 after being crushed is greater than the thickness T 2 of the moisture absorption portion 4. It is preferably thick, and specifically, the thickness T 1 is preferably 20 to 200 ⁇ m.
- the entire cured moisture absorption part 4 is covered with a porous sheet.
- a porous sheet a sheet formed by sintering polyethylene particles or the like and having a thickness of 1000 ⁇ m or less can be used.
- the porous sheet may be adhered to the moisture absorbent portion 4 with an adhesive material so that the position of the porous sheet does not shift.
- an ultraviolet curable resin which is a material of the sealing wall 3 is applied to the outer periphery of the porous sheet in plan view.
- the first substrate 11 and the second substrate 12 are disposed so as to face each other via the organic light emitting body 20 so as to be in close contact with each other.
- the ultraviolet curable resin which is the material of the sealing wall 3 is crushed by both the first substrate 11 and the second substrate 12.
- the porous sheet which is the material of the water diffusion portion 5 is crushed in both the moisture absorption portion 4 and the second substrate 12.
- the thickness T 1 of the water diffusion section 5 (porous sheet) thick is preferred than the thickness T 2 of the moisture absorption portion 4, the thickness T 1 is specifically is 20 ⁇ 200 [mu] m after being crushed Is preferred.
- a glass frit is applied by screen printing or the like to a place where the sealing wall 3 of the first substrate 11 is to be provided. Thereafter, this is fired at a temperature of 800 ° C. or higher to form a bank-like protrusion 8 having a height of about 10 to 200 ⁇ m. Similarly to this, the projection 8 is formed on the second substrate 12 in advance.
- an organic electroluminescent device 1 as shown in FIG. 3 can be obtained.
Landscapes
- Electroluminescent Light Sources (AREA)
Abstract
L'élément électroluminescent organique de l'invention est équipé : d'un premier substrat (11); d'un corps luminescent organique (20) agencé sur ce premier substrat (11); d'un second substrat (12) disposé en vis-à-vis par rapport au premier substrat (11) avec le corps luminescent organique (20) pour intermédiaire; d'une paroi de scellement (3) agencée entre le premier et le second substrat (11, 12) de manière à entourer le corps luminescent organique (20); d'une partie absorption d'humidité (4) possédant des propriétés d'absorption d'humidité, et revêtant le corps luminescent organique (20); et d'une partie diffusion d'humidité (5) possédant des propriétés de diffusion d'humidité, et s'intercalant au moins entre le second substrat (12) et la partie absorption d'humidité (4).
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JP2013-101204 | 2013-05-13 | ||
JP2013101204 | 2013-05-13 |
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WO2014185025A1 true WO2014185025A1 (fr) | 2014-11-20 |
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PCT/JP2014/002359 WO2014185025A1 (fr) | 2013-05-13 | 2014-04-28 | Élément électroluminescent organique |
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Cited By (1)
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CN107425136A (zh) * | 2017-05-11 | 2017-12-01 | 京东方科技集团股份有限公司 | 一种oled显示面板及其制备方法 |
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JP2005038842A (ja) * | 2003-06-27 | 2005-02-10 | Semiconductor Energy Lab Co Ltd | 表示装置及び表示装置の作製方法 |
JP2005209430A (ja) * | 2004-01-21 | 2005-08-04 | Pioneer Electronic Corp | 半導体装置 |
JP2006338946A (ja) * | 2005-05-31 | 2006-12-14 | Sanyo Electric Co Ltd | 表示パネル |
WO2009096537A1 (fr) * | 2008-01-31 | 2009-08-06 | Japan Gore-Tex Inc. | Élément d'adsorption de gaz et dispositif luminescent organique utilisant cet élément d'adsorption de gaz |
WO2011161586A1 (fr) * | 2010-06-22 | 2011-12-29 | Koninklijke Philips Electronics N.V. | Dispositif électroluminescent organique avec feuille de séparation |
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JP2005038842A (ja) * | 2003-06-27 | 2005-02-10 | Semiconductor Energy Lab Co Ltd | 表示装置及び表示装置の作製方法 |
JP2005209430A (ja) * | 2004-01-21 | 2005-08-04 | Pioneer Electronic Corp | 半導体装置 |
JP2006338946A (ja) * | 2005-05-31 | 2006-12-14 | Sanyo Electric Co Ltd | 表示パネル |
WO2009096537A1 (fr) * | 2008-01-31 | 2009-08-06 | Japan Gore-Tex Inc. | Élément d'adsorption de gaz et dispositif luminescent organique utilisant cet élément d'adsorption de gaz |
WO2011161586A1 (fr) * | 2010-06-22 | 2011-12-29 | Koninklijke Philips Electronics N.V. | Dispositif électroluminescent organique avec feuille de séparation |
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CN107425136A (zh) * | 2017-05-11 | 2017-12-01 | 京东方科技集团股份有限公司 | 一种oled显示面板及其制备方法 |
US11380865B2 (en) | 2017-05-11 | 2022-07-05 | Boe Technology Group Co., Ltd. | Package structure, electroluminescent display substrate, and fabrication method thereof |
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