WO2005002289A1 - 電界発光素子 - Google Patents
電界発光素子 Download PDFInfo
- Publication number
- WO2005002289A1 WO2005002289A1 PCT/JP2004/008799 JP2004008799W WO2005002289A1 WO 2005002289 A1 WO2005002289 A1 WO 2005002289A1 JP 2004008799 W JP2004008799 W JP 2004008799W WO 2005002289 A1 WO2005002289 A1 WO 2005002289A1
- Authority
- WO
- WIPO (PCT)
- Prior art keywords
- electroluminescent device
- inorganic compound
- light
- emitting layer
- metal
- Prior art date
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Classifications
-
- H—ELECTRICITY
- H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
- H05B—ELECTRIC HEATING; ELECTRIC LIGHT SOURCES NOT OTHERWISE PROVIDED FOR; CIRCUIT ARRANGEMENTS FOR ELECTRIC LIGHT SOURCES, IN GENERAL
- H05B33/00—Electroluminescent light sources
- H05B33/12—Light sources with substantially two-dimensional radiating surfaces
- H05B33/14—Light sources with substantially two-dimensional radiating surfaces characterised by the chemical or physical composition or the arrangement of the electroluminescent material, or by the simultaneous addition of the electroluminescent material in or onto the light source
-
- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09K—MATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
- C09K11/00—Luminescent, e.g. electroluminescent, chemiluminescent materials
- C09K11/08—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials
- C09K11/77—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials containing rare earth metals
- C09K11/7728—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials containing rare earth metals containing europium
- C09K11/7732—Halogenides
- C09K11/7733—Halogenides with alkali or alkaline earth metals
-
- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K50/00—Organic light-emitting devices
- H10K50/10—OLEDs or polymer light-emitting diodes [PLED]
- H10K50/11—OLEDs or polymer light-emitting diodes [PLED] characterised by the electroluminescent [EL] layers
-
- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K50/00—Organic light-emitting devices
- H10K50/10—OLEDs or polymer light-emitting diodes [PLED]
- H10K50/14—Carrier transporting layers
Definitions
- the present invention relates to a novel charge injection type electroluminescent device.
- the present invention relates to a novel charge injection type electroluminescent device which can be expected to improve internal light efficiency by improving internal quantum efficiency in addition to using a phosphorescent material as a light emitting layer. Also, the present invention relates to an electroluminescent device having good color purity, particularly suitable for blue color for full color display.
- an inorganic electroluminescent device using an inorganic compound for a light emitting layer has been mainly used.
- the inorganic electroluminescent device employs a method in which an inorganic compound is sandwiched between insulating layers and driven by applying an AC voltage.
- the intrinsic electric field in which high-speed electrons accelerated by a high electric field collide with each other and excite the emission center is used. It is a light emitting element. Due to their high durability, inorganic electroluminescent elements have been put to practical use in car audio and displays of factory automation (FA) equipment.
- FA factory automation
- the conventional inorganic electroluminescent device requires an AC power supply and a high voltage as high as 200 V to drive the device, and it is difficult to achieve full color display and insufficient brightness. Yes.
- This device is also called a charge injection type, and its light emission mechanism is based on the fact that holes (holes) injected from an anode and electrons injected from a cathode are recombined to generate a molecule in an excited state (hereinafter referred to as an excited state). It is said to emit energy by emitting energy when the exciton returns to the ground state.
- the light emission observed in the organic electroluminescent device is a light emission phenomenon when the exciton returns to the basal state as described above.
- the types of excitons formed by the organic compound include a singlet excited state and a triplet excited state.
- the ratio of exciton generation between the singlet excited state and the triplet excited state in the organic electroluminescent device is 1: 3.
- the ground state of the organic compound is usually a singlet ground state.
- the transition from the singlet excited state to the singlet ground state is a spin-allowed transition (the spin direction is opposite), but the transition from the triplet excited state to the singlet ground state is a strong spin-forbidden transition (spin Are the same direction).
- Non-Patent Document 2 Hijikawa Hosokawa, Tadashi Kusumoto, (Junji Kido) "Organic EL Materials and Displays", 2001, p.321
- the inventors of the present invention have conducted intensive research and development based on the idea that there is an effective means for increasing the internal quantum efficiency other than using a phosphorescent material as the light emitting layer.
- a new charge injection type electroluminescent device formed by the above was completed.
- the internal quantum efficiency of 25% of the conventional organic electroluminescent device is due to the exciton generation ratio (1: 3) between the singlet excited state and the triplet excited state. If an inorganic compound that is not affected by the generation ratio of GaN is used for the light emitting layer, it is expected that the internal quantum efficiency will be improved and the luminous efficiency will be increased.
- the light emitting layer is formed of an inorganic compound, useful research results of inorganic electroluminescent elements that have been conventionally stacked (what kind of light emitting characteristics should be used when using an inorganic compound for the light emitting layer). Can be referred to, and the degree of freedom in selecting a light emitting material is increased.
- An object of the present invention is to provide a novel charge injection type electroluminescent device which can be expected to improve internal light efficiency by improving internal quantum efficiency, in addition to using a phosphorescent material as a light emitting layer.
- Another object of the present invention is to provide an electroluminescent device having good color purity, particularly suitable for blue color for full color display.
- a charge injection type electroluminescent element that emits light by recombination of holes injected from an anode and electrons injected from a cathode is formed of an organic compound.
- An electroluminescent device comprising a light emitting layer formed only of an inorganic compound between a hole transport layer and an electron transport layer.
- the inorganic compound includes a metal compound that emits light by an emission transition composed of a spin-allowed transition or a spin-forbidden transition, or that emits light by an emission transition caused by an inner-shell transition of a metal ion.
- An electroluminescent device according to the first invention characterized in that:
- the inorganic compound is a combination of a luminescent metal compound and an inorganic compound capable of forming a solid solution with the metal compound. Or an electroluminescent device according to the second invention.
- a fourth invention is the electroluminescent device according to the first, second or third invention, wherein the inorganic compound is a metal halide.
- the fifth invention is characterized in that the inorganic compound is a combination of a rare earth element halide and an alkali metal or alkaline earth metal halide.
- the inorganic compound comprises a divalent europium halide
- the electroluminescent device according to the first, second or third invention characterized in that it is a combination of a halide of a alkali metal or an alkaline earth metal.
- the inorganic compound is a combination of europium bromide ( ⁇ ) and cesium iodide, wherein the inorganic compound is a combination of europium bromide ( ⁇ ) and cesium iodide. This is the electroluminescent device.
- an organic compound formed of an inorganic compound alone is provided between a hole transport layer and an electron transport layer formed of an organic compound.
- a novel charge injection type electroluminescent device can be formed which is not affected by a limit value where the upper limit of the internal quantum efficiency is 25%.
- a novel charge injection type electroluminescent device that can be expected to improve luminous efficiency by improving internal quantum efficiency can be obtained.
- the light-emitting layer can be deposited at a relatively low temperature, and thus there is an advantage that the organic layer is not easily damaged by heat.
- FIG. 1 is an explanatory view showing an element configuration of an electroluminescent device according to Example 1 of the present invention.
- Garden 2 FIG. It is a characteristic diagram.
- FIG. 3 is a characteristic diagram showing a relationship between luminance and current of the electroluminescent device according to Example 1.
- Garden 4 FIG. 4 is a characteristic diagram of the emission spectrum of the electroluminescent devices according to Example 1 and Example 5. is there.
- FIG. 5 is a characteristic diagram showing a relationship between luminance and current of the electroluminescent devices according to Example 1 and Example 5.
- FIG. 6 is a characteristic diagram of an emission spectrum of the electroluminescent devices according to Example 1 and Example 6.
- FIG. 7 is a characteristic diagram showing a relationship between luminance and current of the electroluminescent elements according to Example 1 and Example 6.
- FIG. 8 is a characteristic diagram showing a luminance-voltage relationship of the electroluminescent devices according to Example 1 and Example 6.
- the electroluminescent device according to the present invention is formed, for example, by the following device configuration.
- a substrate an anode, a single layer or a plurality of organic layers having a hole transporting property, A light-emitting layer formed of a single layer, a single layer or a plurality of organic layers having an electron-transporting property, and a cathode sequentially laminated.
- hole blocking layer hole blocking layer
- electron injection layer an electron injection layer
- Examples of the substrate include, but are not limited to, glass, plastic, and a metal thin film.
- anode transparent electrode
- examples of the anode include indium tin oxide (IT ⁇ ), titanium oxide, tin oxide, and the like formed into a thin film by a vacuum evaporation method, a sputtering method, or a sol-gel method. It is not limited to these.
- Examples of the organic material layer having a hole transporting property include polybutyral rubazole (PVK) and fueurenediamine derivatives (for example, ⁇ , ⁇ '-bis (3-methylphenyl) - ⁇ , ⁇ '-bis (phenyl)- Benzidine (TPD, etc.), triphenylamine derivative, sorbazole derivative, phenylstyrene derivative and the like are not limited thereto.
- PVK polybutyral rubazole
- fueurenediamine derivatives for example, ⁇ , ⁇ '-bis (3-methylphenyl) - ⁇ , ⁇ '-bis (phenyl)- Benzidine (TPD, etc.
- triphenylamine derivative sorbazole derivative
- phenylstyrene derivative and the like are not limited thereto.
- the organic material layer having an electron-transporting property is not limited to these, and may be an oxaziazole derivative, a triazole derivative, a phenantophorin derivative, an aluminum quinolinol complex, or the like.
- the organic layer having a hole transporting property and the organic layer having an electron transporting property can be formed by a vacuum evaporation method, a spin coating method, or the like.
- Examples of the cathode (back electrode) include lithium, aluminum, magnesium, and silver, but are not limited thereto.
- the light-emitting layer formed only of an inorganic compound is not limited to the above-described forces that can be formed by, for example, a vacuum evaporation method or a spin coating method.
- a vacuum deposition method is preferable.
- the inorganic compound a combination of a luminescent metal compound and an inorganic compound capable of forming a solid solution with the metal compound is preferable.
- concentration quenching can be suppressed by increasing the distance between metal ions involved in luminescence, and as a result, the luminous efficiency of the electroluminescent device is increased. That can be S.
- the inorganic compound is preferably a metal halide that can be deposited at a relatively low temperature so that the organic layer is not damaged by heat.
- Examples of the inorganic compound include a rare earth element halide described below, an alkali metal or alkaline earth metal halide, manganese, copper, antimony, platinum, silver, gold, mercury, molybdenum, and tungsten. And luminescent metal compounds using iridium, ruthenium, cobalt and the like.
- the light emitting layer can be used alone or in combination of two or more kinds.
- halide examples include fluoride, chloride, bromide, and iodide. More specifically, as the metal halide, for example, a halide of a rare earth element, an alkali metal or an alkaline earth metal And a combination of the above halogen compounds.
- Examples of the rare earth element include cerium, praseodymium, neodymium, samarium, europium, gadolinium, terbium, dysprosium, honolemium, erbium, thulium, ytterbium and the like.
- alkali metal examples include lithium, sodium, potassium, rubidium, and cesium.
- alkaline earth metal examples include magnesium, calcium, strontium, barium and the like.
- the light-emitting layer can be formed of a halide of an alkali metal or a halide of an alkaline earth metal alone or in combination of two or more.
- the level (ground level) of Eu 2+ is the spin octet, In the light emission from each of these excited states, the octet excited state ⁇ the octet ground state The transition is a spin-allowed transition, and the transition from the sixt excited state to the octet ground state is a spin-forbidden transition. Moreover, unlike the light emitting layer of the organic electroluminescent device, Eu 2+ is said to emit light from both spin-allowed transition and spin-forbidden transition.
- the internal quantum efficiency is usually 25. /. It can be expected to have an internal quantum efficiency of 100%, which is 4 times that of an organic electroluminescent device with an upper limit of 100%.
- spin-allowed transition or spin-forbidden transition may include either a spin-allowed transition or a spin-forbidden transition, or a spin-allowed transition and a spin-forbidden transition. In some cases.
- the excited state of cerium ion is (5C1) 1 level
- the ground state is (4 is a level and both have only spin doublets. Since it is said that the transition between the excited state and the ground state is only a spin-allowed transition, a luminous efficiency with an internal quantum efficiency of 100% can be expected as in Eu 2+ .
- the inorganic compounds there are compounds in which excitons in a triplet excited state intersecting from a singlet excited state participate in 100% emission.
- the types of the light emission pathways are more diverse than those of the organic compounds. Therefore, if an inorganic compound suitable for the light emitting layer is selected, a device having higher internal quantum efficiency can be expected.
- the Br dope concentration is preferably 0.01-40% by weight, more preferably 0.1-10% by weight.
- the content is less than 0.01% by weight, carriers having a low emission center density are likely to emit light in the hole transporting layer or the electron transporting layer. Therefore, if the content exceeds 40% by weight, concentration quenching becomes strong and the luminance is significantly reduced. It is not preferable because the possibility is high.
- the thickness of the light emitting layer is preferably 0.120 nm, more preferably 0.310 nm. . If the thickness of the light-emitting layer is less than 0.1 nm, carriers escape from the hole-transporting layer to the electron-transporting layer or vice versa to the hole-transporting layer and recombine outside the light-emitting layer It is not preferable because there is a possibility that the resistance value increases and the current becomes difficult to flow if it exceeds 20 bandages.
- the thickness of the light emitting layer is preferably 5 nm or less. Exceeding 5 waking is not preferable because the driving voltage is no longer high and the brightness is reduced, and the element is liable to be damaged.
- the hole blocking layer includes, for example, bathocuproine (BCP), a triazole derivative (TAZ), and an oxadiazole derivative.
- BCP bathocuproine
- TEZ triazole derivative
- oxadiazole derivative an oxadiazole derivative
- Examples of the electron injecting layer include, but are not limited to, lithium fluoride and magnesium fluoride.
- FIG. 1 is an explanatory diagram showing an element configuration of an electroluminescent element according to Example 1 of the present invention.
- EuBr (europium (II) bromide), which is a halide of a rare earth element, and an alkali metal
- An electroluminescent device 1 shown in FIG. 1 was produced by co-evaporating Csl (cesium iodide), which is a halide, to form a light emitting layer 5.
- Csl cesium iodide
- Transparent electrode 2 I ⁇
- Hole transport layer 4 TPD
- Emitting layer 5 CsI + EuBr
- Hole block layer 6 BCP
- Electron transport layer 7 Alq
- Cathode 8 LiF / Al
- TPD T, ⁇ ′-bis (3-methylphenyl) - ⁇ , ⁇ ′-bis (phenyl) -benzidine
- a glass substrate 3 having a transparent electrode 2 (100 nm) made of ITO.
- a vacuum deposition method to form a hole transport layer 4.
- Vacuum is 2.0 X 10- 4 Pa (Example 2 hereinafter same), the thickness of the hole transport layer 4 is 55 nm.
- a hole block layer 6 having a thickness of 25 nm is formed thereon by vapor deposition using BCP (batasoproin), and further, using Alq (tris (8-hydroxyquinoline) aluminum). Evaporation
- a LiF-Al electrode as a cathode was set to 100.7 nm (LiF 0.7 nm, Al 100 nm
- reference numeral 9 denotes an electrode.
- Example 2 using Rbl, Example 3 using KI, and Example 4 using CsBr (cesium bromide).
- FIG. 2 shows a light emitting spectrum of the electroluminescent device according to Examples 14 to 14.
- the emission spectrum was measured with a multi-channel detector (Hamamatsu Photonitas PMA-11).
- Example 1 in which Csl was used as the alkali metal halide (host material), a sharp emission peak of 466 nm, which is a wavelength region showing blue, and a half-value width of 67 nm was obtained. The coordinates (0.15,0.11) were obtained. This is high-purity blue light emission exceeding the CIE1931 chromaticity coordinates (0.15, 0.16) of the blue light-emitting material reported in Non-Patent Document 2.
- Fig. 3 is a characteristic diagram showing the relationship between the luminance and the current.
- the light emitting layer is formed by changing the doping concentration of EuBr to Csl, and the light emitting layer of the device is formed.
- Example 5 An electroluminescent device was produced in the same manner as in Example 1, and this was designated as Example 5.
- the emission spectrum of the electroluminescent device according to Example 5 is shown in FIG. In the fifth embodiment, even if the doping concentration of EuBr is set to 5% by weight, which is five times that of the first embodiment, the luminescence of the phosphor is not increased.
- FIG. 5 is a characteristic diagram showing the relationship between the luminance and the current.
- FIG. 5 shows Example 1 (EuBr doping concentration was Csl
- Example 1 (1% by weight) has about 2.5 times higher brightness per current. Therefore, doping of EuBr
- the light emitting layer was formed by changing the thickness of the light emitting layer, and the light emission spectrum and light emission luminance of the device were measured.
- Example 6 an electroluminescent device was produced in the same manner as in Example 1 except that the thickness of the light emitting layer was changed to 5 nm, and this was designated as Example 6.
- Example 6 The emission spectrum of the electroluminescent device according to Example 6 is shown in FIG. As shown in FIG. 6, in Example 6 in which the thickness of the light-emitting layer was set to 5 nm, the emission at the bottom was reduced, High-purity blue luminescence with CIE 1931 chromaticity coordinates (0.16, 0.09) was obtained. This is considered to be due to the fact that the crystal was grown and the defects were reduced by increasing the thickness of the light emitting layer.
- FIG. 7 shows the relationship between the luminance and the current.
- FIG. 7 also shows the relationship between the luminance and the current of the electroluminescent device according to Example 1 (film thickness: 2 nm).
- FIG. 8 is a characteristic diagram showing a relationship between luminance and voltage of the electroluminescent elements according to Example 1 and Example 6.
- Example 6 in which the light emitting layer was thickened to 5 nm, the luminance per current was reduced.
- the maximum luminance in Example 6 was about 5 cd / m 2 . This is considered to be due to the fact that the drive voltage was increased by increasing the thickness of the light emitting layer.
- an inorganic compound is provided between a hole transport layer and an electron transport layer formed of an organic compound.
- a novel charge-injection-type electroluminescent element which is not affected by a limit value where the upper limit of the internal quantum efficiency is 25% can be formed. This makes it possible to obtain a novel charge injection type electroluminescent device that can be expected to improve luminous efficiency by improving internal quantum efficiency.
- the light emitting layer can be deposited at a relatively low temperature, there is an advantage that the organic layer is not easily damaged by heat.
- the light emitting element described in Non-Patent Document 2 has a higher chromaticity coordinate (0.15, 0.16) and higher color purity. A blue light-emitting element can be formed.
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- Chemical & Material Sciences (AREA)
- Inorganic Chemistry (AREA)
- Engineering & Computer Science (AREA)
- Materials Engineering (AREA)
- Organic Chemistry (AREA)
- Electroluminescent Light Sources (AREA)
- Luminescent Compositions (AREA)
Abstract
Description
Claims
Priority Applications (1)
Application Number | Priority Date | Filing Date | Title |
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US10/563,168 US20070108895A1 (en) | 2003-06-30 | 2004-06-23 | Electroluminescent device |
Applications Claiming Priority (2)
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JP2003-188158 | 2003-06-30 | ||
JP2003188158A JP3651801B2 (ja) | 2003-06-30 | 2003-06-30 | 電界発光素子 |
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WO2005002289A1 true WO2005002289A1 (ja) | 2005-01-06 |
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PCT/JP2004/008799 WO2005002289A1 (ja) | 2003-06-30 | 2004-06-23 | 電界発光素子 |
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US (1) | US20070108895A1 (ja) |
JP (1) | JP3651801B2 (ja) |
WO (1) | WO2005002289A1 (ja) |
Cited By (1)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
EP1821579A3 (en) * | 2006-02-17 | 2008-04-02 | Semiconductor Energy Laboratory Co., Ltd. | Light emitting element, light emitting device, and electronic appliance |
Families Citing this family (7)
Publication number | Priority date | Publication date | Assignee | Title |
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US20070194321A1 (en) * | 2006-02-17 | 2007-08-23 | Semiconductor Energy Laboratory Co., Ltd. | Light emitting element, light emitting device, and electronic device |
GB2458443A (en) * | 2008-02-29 | 2009-09-23 | Univ Dublin City | Electroluminescent device |
KR101652789B1 (ko) | 2009-02-23 | 2016-09-01 | 삼성전자주식회사 | 다중 양자점층을 가지는 양자점 발광소자 |
TW201110423A (en) * | 2009-09-11 | 2011-03-16 | Power Light Tech Co Ltd | Light-emitting diode illumination device capable of adjusting color temperature |
CN103855310A (zh) * | 2012-11-30 | 2014-06-11 | 海洋王照明科技股份有限公司 | 有机电致发光装置及其制备方法 |
WO2021244801A1 (en) | 2020-06-04 | 2021-12-09 | Beeoled Gmbh | Metal-organic coordination compound and method for producing the same |
CN117157302A (zh) | 2021-04-16 | 2023-12-01 | 蜜蜂Oled股份有限公司 | 金属有机配位化合物及其制备方法 |
Citations (3)
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JP2000223264A (ja) * | 1999-01-29 | 2000-08-11 | Pioneer Electronic Corp | 有機el素子およびその製造方法 |
JP2001043977A (ja) * | 1999-05-27 | 2001-02-16 | Tdk Corp | 発光ダイオード |
JP2003059665A (ja) * | 2001-02-19 | 2003-02-28 | Kyushu Electric Power Co Inc | 電界発光素子 |
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FR2259435B1 (ja) * | 1974-01-29 | 1978-06-16 | Thomson Csf | |
DE3482869D1 (de) * | 1983-11-07 | 1990-09-06 | Fuji Photo Film Co Ltd | Phosphor, verfahren zum speichern und zum reproduzieren eines strahlungsbildes und schirm zum speichern eines strahlungsbildes mittels dieses verfahrens. |
JPH0696862A (ja) * | 1992-09-14 | 1994-04-08 | Fuji Xerox Co Ltd | 無機薄膜el素子 |
EP0745657B1 (en) * | 1995-06-01 | 1998-09-30 | Agfa-Gevaert N.V. | A novel class of stabilizing compounds for phosphor screens |
JP3933591B2 (ja) * | 2002-03-26 | 2007-06-20 | 淳二 城戸 | 有機エレクトロルミネッセント素子 |
DE10242006B4 (de) * | 2002-09-11 | 2006-04-27 | Siemens Ag | Leuchtstoffplatte |
US6833202B2 (en) * | 2003-03-13 | 2004-12-21 | City University Of Hong Kong | Electroluminescent devices |
-
2003
- 2003-06-30 JP JP2003188158A patent/JP3651801B2/ja not_active Expired - Fee Related
-
2004
- 2004-06-23 US US10/563,168 patent/US20070108895A1/en not_active Abandoned
- 2004-06-23 WO PCT/JP2004/008799 patent/WO2005002289A1/ja active Application Filing
Patent Citations (3)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
JP2000223264A (ja) * | 1999-01-29 | 2000-08-11 | Pioneer Electronic Corp | 有機el素子およびその製造方法 |
JP2001043977A (ja) * | 1999-05-27 | 2001-02-16 | Tdk Corp | 発光ダイオード |
JP2003059665A (ja) * | 2001-02-19 | 2003-02-28 | Kyushu Electric Power Co Inc | 電界発光素子 |
Cited By (1)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
EP1821579A3 (en) * | 2006-02-17 | 2008-04-02 | Semiconductor Energy Laboratory Co., Ltd. | Light emitting element, light emitting device, and electronic appliance |
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JP3651801B2 (ja) | 2005-05-25 |
JP2005025998A (ja) | 2005-01-27 |
US20070108895A1 (en) | 2007-05-17 |
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