JPH09134787A - Organic electroluminescent element and its manufacture - Google Patents
Organic electroluminescent element and its manufactureInfo
- Publication number
- JPH09134787A JPH09134787A JP7289988A JP28998895A JPH09134787A JP H09134787 A JPH09134787 A JP H09134787A JP 7289988 A JP7289988 A JP 7289988A JP 28998895 A JP28998895 A JP 28998895A JP H09134787 A JPH09134787 A JP H09134787A
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- film
- organic
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- Prior art date
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Links
- 238000004519 manufacturing process Methods 0.000 title claims abstract description 18
- 239000000758 substrate Substances 0.000 claims abstract description 61
- 229920002396 Polyurea Polymers 0.000 claims abstract description 34
- 238000000059 patterning Methods 0.000 claims abstract description 15
- 239000010410 layer Substances 0.000 claims description 87
- 238000007740 vapor deposition Methods 0.000 claims description 22
- 239000012044 organic layer Substances 0.000 claims description 13
- 238000000034 method Methods 0.000 claims description 12
- 229910004298 SiO 2 Inorganic materials 0.000 claims description 6
- 238000005401 electroluminescence Methods 0.000 claims description 5
- 239000010408 film Substances 0.000 abstract description 111
- 229910052751 metal Inorganic materials 0.000 abstract description 15
- 239000002184 metal Substances 0.000 abstract description 15
- 230000005525 hole transport Effects 0.000 abstract description 13
- 239000010409 thin film Substances 0.000 abstract description 10
- 230000005684 electric field Effects 0.000 abstract description 6
- 239000012141 concentrate Substances 0.000 abstract description 2
- 238000009413 insulation Methods 0.000 abstract 4
- 230000020169 heat generation Effects 0.000 abstract 2
- 230000002411 adverse Effects 0.000 abstract 1
- 230000000694 effects Effects 0.000 abstract 1
- 238000001704 evaporation Methods 0.000 description 38
- 230000008020 evaporation Effects 0.000 description 34
- 230000001681 protective effect Effects 0.000 description 24
- 239000002994 raw material Substances 0.000 description 19
- RHZWSUVWRRXEJF-UHFFFAOYSA-N indium tin Chemical compound [In].[Sn] RHZWSUVWRRXEJF-UHFFFAOYSA-N 0.000 description 17
- 239000000178 monomer Substances 0.000 description 15
- 238000010438 heat treatment Methods 0.000 description 13
- 238000006116 polymerization reaction Methods 0.000 description 13
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 9
- 239000000975 dye Substances 0.000 description 9
- 229910052760 oxygen Inorganic materials 0.000 description 9
- 239000001301 oxygen Substances 0.000 description 9
- 150000002894 organic compounds Chemical class 0.000 description 7
- UPMLOUAZCHDJJD-UHFFFAOYSA-N 4,4'-Diphenylmethane Diisocyanate Chemical compound C1=CC(N=C=O)=CC=C1CC1=CC=C(N=C=O)C=C1 UPMLOUAZCHDJJD-UHFFFAOYSA-N 0.000 description 6
- 230000015572 biosynthetic process Effects 0.000 description 6
- 239000010406 cathode material Substances 0.000 description 5
- 238000000151 deposition Methods 0.000 description 5
- 239000011521 glass Substances 0.000 description 5
- 238000005192 partition Methods 0.000 description 5
- 229920006254 polymer film Polymers 0.000 description 5
- 230000008021 deposition Effects 0.000 description 4
- 238000009832 plasma treatment Methods 0.000 description 4
- 239000000126 substance Substances 0.000 description 4
- 239000013078 crystal Substances 0.000 description 3
- 150000004985 diamines Chemical class 0.000 description 3
- 238000010894 electron beam technology Methods 0.000 description 3
- 229920000343 polyazomethine Polymers 0.000 description 3
- YBRVSVVVWCFQMG-UHFFFAOYSA-N 4,4'-diaminodiphenylmethane Chemical compound C1=CC(N)=CC=C1CC1=CC=C(N)C=C1 YBRVSVVVWCFQMG-UHFFFAOYSA-N 0.000 description 2
- KFZMGEQAYNKOFK-UHFFFAOYSA-N Isopropanol Chemical compound CC(C)O KFZMGEQAYNKOFK-UHFFFAOYSA-N 0.000 description 2
- ZOKXTWBITQBERF-UHFFFAOYSA-N Molybdenum Chemical compound [Mo] ZOKXTWBITQBERF-UHFFFAOYSA-N 0.000 description 2
- 239000004642 Polyimide Substances 0.000 description 2
- PJANXHGTPQOBST-VAWYXSNFSA-N Stilbene Natural products C=1C=CC=CC=1/C=C/C1=CC=CC=C1 PJANXHGTPQOBST-VAWYXSNFSA-N 0.000 description 2
- 229910052782 aluminium Inorganic materials 0.000 description 2
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 2
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 2
- 238000010586 diagram Methods 0.000 description 2
- 125000005442 diisocyanate group Chemical group 0.000 description 2
- 230000001678 irradiating effect Effects 0.000 description 2
- 239000011777 magnesium Substances 0.000 description 2
- 229910052750 molybdenum Inorganic materials 0.000 description 2
- 239000011733 molybdenum Substances 0.000 description 2
- 239000005416 organic matter Substances 0.000 description 2
- 229920001721 polyimide Polymers 0.000 description 2
- 229920000642 polymer Polymers 0.000 description 2
- PJANXHGTPQOBST-UHFFFAOYSA-N stilbene Chemical compound C=1C=CC=CC=1C=CC1=CC=CC=C1 PJANXHGTPQOBST-UHFFFAOYSA-N 0.000 description 2
- 235000021286 stilbenes Nutrition 0.000 description 2
- CBCKQZAAMUWICA-UHFFFAOYSA-N 1,4-phenylenediamine Chemical compound NC1=CC=C(N)C=C1 CBCKQZAAMUWICA-UHFFFAOYSA-N 0.000 description 1
- XXKRKYCPIGXMAM-UHFFFAOYSA-N 1-methyl-3-(2-phenylphenyl)benzene Chemical group CC1=CC=CC(C=2C(=CC=CC=2)C=2C=CC=CC=2)=C1 XXKRKYCPIGXMAM-UHFFFAOYSA-N 0.000 description 1
- MVWPVABZQQJTPL-UHFFFAOYSA-N 2,3-diphenylcyclohexa-2,5-diene-1,4-dione Chemical class O=C1C=CC(=O)C(C=2C=CC=CC=2)=C1C1=CC=CC=C1 MVWPVABZQQJTPL-UHFFFAOYSA-N 0.000 description 1
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 1
- FYYHWMGAXLPEAU-UHFFFAOYSA-N Magnesium Chemical compound [Mg] FYYHWMGAXLPEAU-UHFFFAOYSA-N 0.000 description 1
- 239000004952 Polyamide Substances 0.000 description 1
- -1 Si 3 N 4 Inorganic materials 0.000 description 1
- 229910006404 SnO 2 Inorganic materials 0.000 description 1
- 238000009835 boiling Methods 0.000 description 1
- 238000010549 co-Evaporation Methods 0.000 description 1
- 239000011248 coating agent Substances 0.000 description 1
- 238000000576 coating method Methods 0.000 description 1
- 229910052802 copper Inorganic materials 0.000 description 1
- 239000010949 copper Substances 0.000 description 1
- 238000000354 decomposition reaction Methods 0.000 description 1
- 238000005530 etching Methods 0.000 description 1
- 239000007850 fluorescent dye Substances 0.000 description 1
- 229910052736 halogen Inorganic materials 0.000 description 1
- 150000002367 halogens Chemical class 0.000 description 1
- 150000002484 inorganic compounds Chemical class 0.000 description 1
- 229910010272 inorganic material Inorganic materials 0.000 description 1
- 125000000040 m-tolyl group Chemical group [H]C1=C([H])C(*)=C([H])C(=C1[H])C([H])([H])[H] 0.000 description 1
- 229910052749 magnesium Inorganic materials 0.000 description 1
- 239000000463 material Substances 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 239000003960 organic solvent Substances 0.000 description 1
- WCPAKWJPBJAGKN-UHFFFAOYSA-N oxadiazole Chemical compound C1=CON=N1 WCPAKWJPBJAGKN-UHFFFAOYSA-N 0.000 description 1
- 150000004866 oxadiazoles Chemical class 0.000 description 1
- 238000000206 photolithography Methods 0.000 description 1
- 229920002647 polyamide Polymers 0.000 description 1
- 229910052709 silver Inorganic materials 0.000 description 1
- 239000004332 silver Substances 0.000 description 1
- 239000002356 single layer Substances 0.000 description 1
- 239000007787 solid Substances 0.000 description 1
- 238000004544 sputter deposition Methods 0.000 description 1
- 229910001220 stainless steel Inorganic materials 0.000 description 1
- 239000010935 stainless steel Substances 0.000 description 1
- 229920003002 synthetic resin Polymers 0.000 description 1
- 239000000057 synthetic resin Substances 0.000 description 1
- 229910052715 tantalum Inorganic materials 0.000 description 1
- GUVRBAGPIYLISA-UHFFFAOYSA-N tantalum atom Chemical compound [Ta] GUVRBAGPIYLISA-UHFFFAOYSA-N 0.000 description 1
- KUCOHFSKRZZVRO-UHFFFAOYSA-N terephthalaldehyde Chemical compound O=CC1=CC=C(C=O)C=C1 KUCOHFSKRZZVRO-UHFFFAOYSA-N 0.000 description 1
- WFKWXMTUELFFGS-UHFFFAOYSA-N tungsten Chemical compound [W] WFKWXMTUELFFGS-UHFFFAOYSA-N 0.000 description 1
- 229910052721 tungsten Inorganic materials 0.000 description 1
- 239000010937 tungsten Substances 0.000 description 1
- 238000009281 ultraviolet germicidal irradiation Methods 0.000 description 1
- 238000011144 upstream manufacturing Methods 0.000 description 1
- 229910052720 vanadium Inorganic materials 0.000 description 1
- 229910052727 yttrium Inorganic materials 0.000 description 1
Landscapes
- Electroluminescent Light Sources (AREA)
- Polyurethanes Or Polyureas (AREA)
- Paints Or Removers (AREA)
Abstract
Description
【0001】[0001]
【発明の属する技術分野】本発明は、有機エレクトロル
ミネッセンス素子(以下、「有機EL素子」という)及
びその作製方法に関する。TECHNICAL FIELD The present invention relates to an organic electroluminescence device (hereinafter referred to as “organic EL device”) and a manufacturing method thereof.
【0002】[0002]
【従来の技術】従来、有機EL素子として、図5に示す
ように、基板1上に設けられた透明陽極2と金属陰極5
との間に正孔輸送層3と有機蛍光色素(発光層)4とが
積層されたものが知られている。また、図6に示すよう
に、基板1上に設けられた透明陽極2と金属陰極5との
間に正孔輸送層3、発光層4、電子輸送層6からなる3
層が積層された構造のものも知られている。2. Description of the Related Art Conventionally, as an organic EL element, as shown in FIG. 5, a transparent anode 2 and a metal cathode 5 provided on a substrate 1 are provided.
It is known that a hole transporting layer 3 and an organic fluorescent dye (light emitting layer) 4 are laminated between and. Further, as shown in FIG. 6, a hole transport layer 3, a light emitting layer 4, and an electron transport layer 6 are provided between the transparent anode 2 and the metal cathode 5 provided on the substrate 1.
A structure in which layers are laminated is also known.
【0003】有機EL素子は、通常、パターニングされ
た透明陽極2上へ蒸着マスクを介して正孔輸送層3、発
光層4、電子輸送層6、金属陰極5を、順次、成膜して
作製される。An organic EL device is usually manufactured by sequentially forming a hole transport layer 3, a light emitting layer 4, an electron transport layer 6 and a metal cathode 5 on a patterned transparent anode 2 through a vapor deposition mask. To be done.
【0004】[0004]
【発明が解決しようとする課題】有機EL素子の膜厚
は、通常、透明陽極2が100〜200nm、正孔輸送
層3、発光層4、電子輸送層6からなる有機層が全体で
100〜300nm、陰極5が100〜300nmであ
る。有機EL素子においては、透明陽極2と金属陰極5
との間に50〜100MV/mの高電界を印加して作動
させているため、主に電極の端面(エッジ部)に電界が
集中し易く、そのロスがジュール熱となり、有機薄膜と
金属陰極との間を剥離させ、非発光領域(ダークスポッ
ト)を生じるという不具合が起こる。The film thickness of the organic EL device is usually 100 to 200 nm for the transparent anode 2, 100 to 200 nm for the whole organic layer consisting of the hole transport layer 3, the light emitting layer 4, and the electron transport layer 6. 300 nm, and the cathode 5 is 100 to 300 nm. In the organic EL device, the transparent anode 2 and the metal cathode 5
Since a high electric field of 50 to 100 MV / m is applied between and to operate, the electric field tends to concentrate mainly on the end face (edge part) of the electrode, and the loss thereof becomes Joule heat, and the organic thin film and the metal cathode. There is a problem in that the non-luminous area (dark spot) is generated by peeling the gap between the areas.
【0005】上記有機層は、蒸着法で作製するために、
透明陽極の側部へ膜が成長しずらい。そのために、図7
中で○印で囲まれた部分における有機層7の膜厚が他の
部分と比べて薄くなり、電界がここへ集中し易いという
問題がある。図7中、1、2及び5は、図5及び6にお
けるものと同じものを示す。Since the above organic layer is produced by the vapor deposition method,
The film is hard to grow on the side of the transparent anode. To that end, FIG.
There is a problem that the film thickness of the organic layer 7 in the portion surrounded by a circle becomes thinner than that in other portions, and the electric field is easily concentrated here. In FIG. 7, 1, 2 and 5 indicate the same as those in FIGS.
【0006】また、金属陰極5は、蒸着マスクを介して
形成されるために、細かいパターンの発光面が得られに
くく、ディスプレイを作製する上で問題になっている。Further, since the metal cathode 5 is formed through the vapor deposition mask, it is difficult to obtain a light emitting surface having a fine pattern, which is a problem in manufacturing a display.
【0007】本発明は、透明陽極の端面の影響をなくし
て、素子の短絡、非発光領域の増加といった問題を解消
し、安定な発光面を有する有機EL素子及びその作製方
法を提供することを目的としている。The present invention provides an organic EL device having a stable light emitting surface by eliminating the influence of the end face of the transparent anode, solving the problems of short-circuiting of the device and increasing the non-light emitting area, and a method for manufacturing the same. Has an aim.
【0008】[0008]
【課題を解決するための手段】本発明の有機EL素子
は、基板上に陽極、有機層及び陰極を有する有機EL素
子において、該陽極上又は陽極間へパターニングにより
絶縁層が設けられ、その上に該有機層及び陰極が形成さ
れていることを特徴とする。The organic EL element of the present invention is an organic EL element having an anode, an organic layer and a cathode on a substrate, and an insulating layer is provided on the anode or between the anodes by patterning, and Is characterized in that the organic layer and the cathode are formed.
【0009】本発明の有機EL素子では、例えば、図1
に示すように、基板1上に設けられた透明陽極2上に絶
縁膜をパターニングして得た絶縁層8が設けられ、その
上に正孔輸送層3、発光層4、電子輸送層(図示せず)
及び金属陰極5が、成膜されている。また、図2に示す
ように、基板1上へ透明電極2がパターニングされてい
る場合は、透明電極間へ絶縁膜8を埋め込むように作製
する。In the organic EL device of the present invention, for example, as shown in FIG.
As shown in FIG. 3, an insulating layer 8 obtained by patterning an insulating film is provided on a transparent anode 2 provided on a substrate 1, and a hole transport layer 3, a light emitting layer 4, an electron transport layer (see FIG. (Not shown)
And the metal cathode 5 is formed into a film. Further, as shown in FIG. 2, when the transparent electrode 2 is patterned on the substrate 1, the insulating film 8 is formed so as to be embedded between the transparent electrodes.
【0010】前記絶縁層としては、例えば、蒸着せしめ
たポリ尿素膜を紫外線露光後、加熱現像によりパターニ
ングされた膜(例えば、特開平6−80968号及び特
開平7−209863号記載の膜)を用いることが望ま
しい。この現像工程では、紫外線露光後、光未照射部が
有機溶剤による除去又は加熱による分解で取り除かれ
る。また、絶縁層として、SiO2 、Si3N4、GeO
等の無機化合物の膜をレジストプロセス等を使って、パ
ターニングした構造を用いてもよい。As the insulating layer, for example, a film obtained by subjecting a vapor-deposited polyurea film to ultraviolet exposure and then patterning by heat development (for example, the films described in JP-A-6-80968 and JP-A-7-209863) is used. It is desirable to use. In this developing step, after the exposure to ultraviolet rays, the non-irradiated area is removed by removal with an organic solvent or decomposition by heating. Further, as an insulating layer, SiO 2 , Si 3 N 4 , GeO is used.
A structure in which a film of an inorganic compound such as is patterned using a resist process or the like may be used.
【0011】本発明の有機EL素子の作製方法は、基板
上に設けられた陽極上又は陽極間へパターニングにより
絶縁層を形成し、その上に有機層を形成し、次いでその
上に電極パターンのマスク蒸着をせずに陰極を形成し
て、該絶縁層で囲まれたパターンの中に発光面が形成さ
れるようにすることを特徴とする。According to the method for producing an organic EL device of the present invention, an insulating layer is formed by patterning on or between anodes provided on a substrate, an organic layer is formed thereon, and then an electrode pattern is formed thereon. It is characterized in that the cathode is formed without mask vapor deposition so that the light emitting surface is formed in the pattern surrounded by the insulating layer.
【0012】本発明では、上記したように、透明陽極上
又は陽極間にパターニングされた絶縁層を設けてあるの
で、発光は絶縁層が抜けた部分で起こる。このため、金
属陰極5は特にパターニングされた膜を用いなくてよ
い。従って、有機EL素子の作製プロセスにおいて、金
属陰極のパターニングプロセスを省略することができ
る。In the present invention, as described above, since the patterned insulating layer is provided on the transparent anode or between the anodes, light emission occurs at the portion where the insulating layer is removed. Therefore, the metal cathode 5 does not need to use a patterned film. Therefore, the patterning process of the metal cathode can be omitted in the manufacturing process of the organic EL element.
【0013】また、透明陽極の端部(エッジ部)の影響
がなくなるために、電圧を印加したときに電界の集中す
る部分がなくなり、膜全体に均一に電界が印加されるの
で、安定した発光を得ることができる。Further, since the influence of the end portion (edge portion) of the transparent anode is eliminated, there is no portion where the electric field is concentrated when a voltage is applied, and the electric field is uniformly applied to the entire film, so that stable light emission is achieved. Can be obtained.
【0014】上記絶縁膜は、微細加工することが可能な
ので、1画素あたりの面積を小さくすることができる。
従来の金属陰極のマスク蒸着においては、0.5mm×
0.5mmの面積が限界であり、それより小さい面積で
は微細加工が困難であった。Since the insulating film can be finely processed, the area per pixel can be reduced.
In conventional metal cathode mask vapor deposition, 0.5 mm ×
The area of 0.5 mm is the limit, and if the area is smaller than that, fine processing is difficult.
【0015】[0015]
【発明の実施の形態】以下、添付図面を参照して本発明
の実施の態様を説明する。BEST MODE FOR CARRYING OUT THE INVENTION Embodiments of the present invention will be described below with reference to the accompanying drawings.
【0016】まず、有機EL素子の構造について説明す
る。First, the structure of the organic EL element will be described.
【0017】該有機EL素子の構造としては、陽極/絶
縁層/発光層/陰極のような有機化合物膜が発光層(高
分子膜又はオリゴマー膜からなる)のみの単層構造の場
合、陽極/絶縁層/正孔輸送層/発光層/陰極又は陽極
/絶縁層/発光層/電子輸送層/陰極のような有機化合
物膜が正孔輸送層と発光層或いは発光層と電子輸送層の
2層構造の場合、陽極/絶縁層/正孔輸送層/発光層/
電子輸送層/陰極のような有機化合物膜が3層構造の場
合がある。As the structure of the organic EL element, when the organic compound film such as anode / insulating layer / light emitting layer / cathode is a single layer structure having only a light emitting layer (comprising a polymer film or an oligomer film), An organic compound film such as an insulating layer / hole transporting layer / light emitting layer / cathode or an anode / insulating layer / light emitting layer / electron transporting layer / cathode has two layers of a hole transporting layer and a light emitting layer or a light emitting layer and an electron transporting layer. In the case of structure, anode / insulating layer / hole transport layer / light emitting layer /
The electron transport layer / organic compound film such as the cathode may have a three-layer structure.
【0018】ここで、絶縁層としては、例えば、前記し
たような特開平6−80968号及び特開平7−209
863号に記載されたものがよい。Here, as the insulating layer, for example, the above-mentioned JP-A-6-80968 and JP-A-7-209 can be used.
The one described in No. 863 is preferable.
【0019】また、有機化合物膜の正孔輸送層として
は、例えば、N,N′−ジフェニル−N,N′−ビス
(3−メチルフェニル)1,1′−ビフェニル4,4′
−ジアミン(以下、TPDという)に代表される正孔輸
送能を持つ低分子色素を蒸着法により形成した薄膜や正
孔輸送性の分子構造を有する高分子膜(ポリアミド、ポ
リイミド、ポリアゾメチン等)を蒸着重合法により形成
した薄膜が用いられ、また正孔輸送性の低分子色素を高
分子薄膜中に蒸着分散させたものでもよい。The hole transport layer of the organic compound film is, for example, N, N'-diphenyl-N, N'-bis (3-methylphenyl) 1,1'-biphenyl 4,4 '.
A thin film formed by a vapor deposition method of a low molecular weight dye having a hole transporting property represented by diamine (hereinafter referred to as TPD) or a polymer film having a hole transporting molecular structure (polyamide, polyimide, polyazomethine, etc.) A thin film formed by a vapor deposition polymerization method is used, and a low molecular weight dye having a hole transporting property may be vapor-dispersed in a polymer thin film.
【0020】また、発光層としては、例えば、8−オキ
シキノリノアルミニウム錯体(以下、Alq3 という)
に代表される発光性色素を蒸着法により形成した薄膜や
スチルベン、オキサジアゾール等の共役系構造を有する
高分子膜(ポリ尿素、ポリイミド、ポリオキサジアゾー
ル等)を蒸着重合法により形成した薄膜が用いられ、ま
た発光性色素を高分子薄膜中に蒸着分散させたものでも
よい。As the light emitting layer, for example, 8-oxyquinolino aluminum complex (hereinafter referred to as Alq 3 )
Thin films formed by vapor deposition of luminescent dyes, such as stilbene, and thin films formed by vapor deposition polymerization of polymer films (polyurea, polyimide, polyoxadiazole, etc.) having a conjugated structure such as stilbene and oxadiazole. Alternatively, the luminescent dye may be dispersed in a polymer thin film by vapor deposition.
【0021】更に、電子輸送層としては、例えば、Al
q3 やオキサジアゾール誘導体の蒸着薄膜が用いられ、
またアントラキノジメタン誘導体、ジフェニルキノン誘
導体の薄膜も用いることができる。Further, as the electron transport layer, for example, Al
depositing a thin film of q 3 and an oxadiazole derivative is used,
Alternatively, a thin film of an anthraquinodimethane derivative or a diphenylquinone derivative can be used.
【0022】本発明において用いる絶縁層の成膜装置の
一例は、以下説明するように、真空中で感光性合成樹脂
の原料モノマーを蒸発させる蒸発源と、原料モノマーの
蒸着重合でポリ尿素膜のような絶縁膜が形成される基板
を互いに対向して配置した蒸着重合室と、基板上の該絶
縁膜に紫外線および/または電子線を照射する紫外線源
および/または電子線源と、該絶縁膜にパターンを形成
するために用いるフォトマスクを配置した露光室と、紫
外線および/または電子線の照射露光後の絶縁膜に加熱
処理を施す加熱装置を配置した現像室とからなる。An example of an insulating layer forming apparatus used in the present invention is, as described below, an evaporation source for evaporating a raw material monomer of a photosensitive synthetic resin in a vacuum and a polyurea film formed by vapor deposition polymerization of the raw material monomer. Vapor deposition polymerization chamber in which substrates on which an insulating film is formed are arranged to face each other, an ultraviolet ray source and / or an electron beam source for irradiating the insulating film on the substrate with ultraviolet rays and / or electron beams, and the insulating film And an exposure chamber in which a photomask used for forming a pattern is disposed, and a developing chamber in which a heating device for performing a heat treatment on the insulating film after exposure to irradiation with ultraviolet rays and / or electron beams is disposed.
【0023】まず、図3は、絶縁層、特にポリ尿素層の
パターン形成装置の1例を示すもので、ポリ尿素膜を形
成する蒸着重合室11、該ポリ尿素膜に紫外線を照射す
るための露光室12、紫外線を照射されたポリ尿素膜に
加熱処理を施す現像室13から構成されており、バルブ
14b、14cにより蒸着重合室11、露光室12、現
像室13の順で互いに連通されている。First, FIG. 3 shows an example of an apparatus for forming a pattern of an insulating layer, especially a polyurea layer. The vapor deposition polymerization chamber 11 for forming a polyurea film and the polyurea film for irradiating ultraviolet rays. It is composed of an exposure chamber 12 and a developing chamber 13 for heat-treating a polyurea film irradiated with ultraviolet rays. The vapor deposition polymerization chamber 11, the exposure chamber 12, and the developing chamber 13 are connected in this order by valves 14b and 14c. There is.
【0024】また、蒸着重合室11の上流側にバルブ1
4aを介して外部の真空ポンプその他の真空排気系15
aに接続された真空室16を配置し、また、現像室13
の下流側にバルブ14dを介して外部の真空ポンプその
他の真空排気系15bに接続された真空室17を配置
し、真空排気系15a及び15bのいずれか一方、また
は両方の真空排気系の作動により蒸着重合室11内、露
光室12内、現像室13内をそれぞれ所定の圧力に設定
できるようにしてある。A valve 1 is provided upstream of the vapor deposition polymerization chamber 11.
An external vacuum pump or other vacuum exhaust system 15 via 4a
a vacuum chamber 16 connected to a, and also the developing chamber 13
A vacuum chamber 17 connected to an external vacuum pump or other vacuum exhaust system 15b via a valve 14d is disposed downstream of the vacuum exhaust system 15a and 15b, or both vacuum exhaust systems are operated. The inside of the vapor deposition polymerization chamber 11, the inside of the exposure chamber 12, and the inside of the developing chamber 13 can be set to predetermined pressures.
【0025】前記蒸着重合室11内に、ポリ尿素膜のよ
うな蒸着重合膜を形成させるための基板1を保持する基
板ホルダー18を配置すると共に、該蒸着重合室11の
下方に前記基板1に対向させてポリ尿素膜の一方の原料
モノマー(a)としてジアミン、他方の原料モノマー
(b)としてジイソシアナートをそれぞれ蒸発させるた
めのガラス製の蒸発源19a、19bを設け、該各蒸発
源19a、19bをその近傍に設けられた水晶振動の蒸
発モニター20a、20bと、ヒーター21a、21b
とによって、前記原料モノマー(a)及び(b)の蒸発
量を常に一定化させる所定温度にコントロールできるよ
うにした。A substrate holder 18 for holding a substrate 1 for forming a vapor-deposited polymerized film such as a polyurea film is arranged in the vapor-deposited polymerization chamber 11, and the substrate 1 is provided below the vapor-deposition polymerization chamber 11. Evaporating sources 19a and 19b made of glass for facing each other and evaporating diamine as one raw material monomer (a) of the polyurea film and diisocyanate as the other raw material monomer (b), respectively, are provided. , 19b provided in the vicinity thereof, and evaporation monitors 20a and 20b for crystal vibration, and heaters 21a and 21b.
Thus, the evaporation amount of the raw material monomers (a) and (b) can be controlled to a predetermined temperature that always keeps the same.
【0026】また、基板1と両蒸発源19a、19bと
の間にシャッター22を配置し、また、両蒸発源19
a、19bの間に仕切板23を設けた。A shutter 22 is arranged between the substrate 1 and both evaporation sources 19a and 19b.
A partition plate 23 was provided between a and 19b.
【0027】前記露光室12内の下方に基板ホルダー1
8に保持された基板1に対向させて紫外線源24を設
け、基板1の前方に所定形状のパターンを備えるフォト
マスク25を設けて、前記蒸着重合室11内で基板1の
表面に形成されたポリ尿素膜に紫外線源24より紫外線
を照射してパターン状に露光させるようにした。The substrate holder 1 is provided below the inside of the exposure chamber 12.
The ultraviolet light source 24 is provided so as to face the substrate 1 held on the substrate 8, and a photomask 25 having a pattern of a predetermined shape is provided in front of the substrate 1 to be formed on the surface of the substrate 1 in the vapor deposition polymerization chamber 11. The polyurea film was irradiated with ultraviolet rays from an ultraviolet ray source 24 so as to be exposed in a pattern.
【0028】前記現像室13内に、基板ホルダー18に
保持された基板1の背面側にハロゲンランプからなる加
熱装置26を設けて、前記露光室12内で紫外線に照射
されて架橋したポリ尿素膜を所定温度に加熱して非露光
部分のポリ尿素膜を解重合させて除去するようにした。In the developing chamber 13, a heating device 26 comprising a halogen lamp is provided on the back side of the substrate 1 held by the substrate holder 18, and a polyurea film crosslinked by being irradiated with ultraviolet rays in the exposing chamber 12 is provided. Was heated to a predetermined temperature to depolymerize and remove the polyurea film in the unexposed portion.
【0029】図3に示したような絶縁層の成膜装置を用
いて、まず、透明電極として例えばITO(Indium-Tin
-Oxide)を成膜した基板1を真空室16へ仕込み、蒸着
重合室11へ搬送して基板ホルダー18上に配置された
基板1上にポリ尿素膜のような絶縁膜を成膜する。次い
で、基板1を真空室(現像室)12へ搬出して紫外線源
24によりフォトマスク25を介して露光する。その
後、真空室13へ搬送して、加熱装置26により紫外線
未照射部を分解、蒸発させて取り除き、絶縁膜のパター
ニングを完了する。First, as a transparent electrode, for example, ITO (Indium-Tin) is used by using the insulating layer forming apparatus as shown in FIG.
The substrate 1 on which -Oxide) has been formed is charged into the vacuum chamber 16 and conveyed to the vapor deposition polymerization chamber 11 to form an insulating film such as a polyurea film on the substrate 1 placed on the substrate holder 18. Next, the substrate 1 is carried out to the vacuum chamber (developing chamber) 12 and exposed by the ultraviolet ray source 24 through the photomask 25. Then, it is conveyed to the vacuum chamber 13, and the ultraviolet ray non-irradiated portion is decomposed and evaporated by the heating device 26 to be removed, and the patterning of the insulating film is completed.
【0030】図4は、本発明の有機EL素子を製造する
ために用いる装置の一例を示すものであるが、ここでは
陽極形成装置、絶縁層成膜装置は示されていない。図
中、27は酸素プラズマ処理室、28は正孔輸送層、発
光層、電子輸送層などの有機化合物膜の成膜室、29は
陰極形成室、30は保護膜形成室、31は紫外線処理室
を示す。そして酸素プラズマ処理室27、成膜室28、
陰極形成室29、保護膜形成室30、紫外線処理室31
の各室間をそれぞれ開閉自在のゲートバルブ32a、3
2b、32c及び32dで仕切るようにすると共に、各
室内に基板1を搬送するトレー式搬送系33を配設し
た。FIG. 4 shows an example of an apparatus used for manufacturing the organic EL element of the present invention, but here, an anode forming apparatus and an insulating layer forming apparatus are not shown. In the figure, 27 is an oxygen plasma treatment chamber, 28 is a deposition chamber for an organic compound film such as a hole transport layer, a light emitting layer, an electron transport layer, 29 is a cathode formation chamber, 30 is a protective film formation chamber, and 31 is ultraviolet treatment. Indicates a room. Then, the oxygen plasma processing chamber 27, the film forming chamber 28,
Cathode forming chamber 29, protective film forming chamber 30, ultraviolet treatment chamber 31
Gate valves 32a, 3 that can be opened and closed between the chambers
It is partitioned by 2b, 32c and 32d, and a tray type transfer system 33 for transferring the substrate 1 is arranged in each chamber.
【0031】酸素プラズマ処理室27内を真空ポンプ等
の真空排気系34に接続すると共に、酸素プラズマ処理
室27内にはITO膜のような陽極にプラズマ処理を施
す銅製のRF電極35を配設した。The inside of the oxygen plasma processing chamber 27 is connected to a vacuum exhaust system 34 such as a vacuum pump, and the inside of the oxygen plasma processing chamber 27 is provided with a copper RF electrode 35 for performing plasma processing on an anode such as an ITO film. did.
【0032】成膜室28内を真空ポンプ等の真空排気系
36に接続し、成膜室28内の下方の一方にTPD、A
lq3 等の色素原料Tをその周囲に巻回したヒーター3
7a、37bで所定温度に加熱し、蒸発させるアルミナ
製又はガラス製の色素蒸発源38a、38bを2個並設
すると共に、成膜室28内の下方の他方に蒸着重合高分
子膜の原料モノマーU、Vを赤外線ランプ39a及び3
9bで所定温度に加熱し、蒸発させるガラス製又は金属
製の有機物蒸発源40a及び40bを配設した。成膜室
28内の上方に色素蒸発源38a及び38b並びに有機
物蒸発源40a及び40bに対向させて有機化合物膜を
成膜すべき基板1を配設すると共に、基板1の裏面に基
板1上に成膜された高分子膜を加熱するシースヒーター
41を配設した。The inside of the film forming chamber 28 is connected to a vacuum exhaust system 36 such as a vacuum pump, and TPD, A
A heater 3 around which a dye material T such as lq 3 is wound.
Two dye evaporation sources 38a, 38b made of alumina or glass, which are heated to a predetermined temperature by 7a, 37b to evaporate, are arranged in parallel, and a raw material monomer for the vapor-deposited polymer film is provided on the other lower side in the film forming chamber 28. U and V are infrared lamps 39a and 3
Glass or metal organic evaporation sources 40a and 40b, which are heated to a predetermined temperature by 9b and evaporated, are provided. A substrate 1 on which an organic compound film is to be formed is disposed facing the dye evaporation sources 38a and 38b and the organic substance evaporation sources 40a and 40b above the film forming chamber 28, and the back surface of the substrate 1 is provided on the substrate 1. A sheath heater 41 for heating the formed polymer film was provided.
【0033】また、基板1と色素蒸発源38a及び38
bとの間にシャッター42a及び42bを、また基板1
と有機物蒸発源40a及び40bとの間にシャッター4
3をそれぞれ配設した。また、有機物蒸発源40a及び
40b内にそれぞれ熱電対44a及び44bを配設し
た。Further, the substrate 1 and the dye evaporation sources 38a and 38
b between the shutters 42a and 42b, and the substrate 1
Between the organic substance evaporation sources 40a and 40b and the shutter 4
3 were arranged respectively. Further, thermocouples 44a and 44b are arranged in the organic substance evaporation sources 40a and 40b, respectively.
【0034】陰極形成室29内を真空ポンプ等の真空排
気系45に接続し、陰極形成室29内の下方の一方に陰
極の一方の原料W(原料Wは、例えば、Mg)をその周
囲を巻回したヒーター46で所定温度に加熱し、蒸発さ
せるアルミナ製の陰極材料蒸発源47を配設すると共
に、陰極形成室29内の下方の他方に陰極の他方の原料
X(原料Xは、例えば、Ag)を所定温度に加熱し、蒸
発させるタングステン製又はモリブデン製のボートから
なる陰極材料蒸発源48を配設した。The inside of the cathode forming chamber 29 is connected to a vacuum exhaust system 45 such as a vacuum pump, and one raw material W of the cathode (raw material W is, for example, Mg) is provided in the lower one inside the cathode forming chamber 29 around the periphery thereof. A cathode material evaporation source 47 made of alumina, which is heated to a predetermined temperature by a wound heater 46 to evaporate, is provided, and the other raw material X of the cathode is provided on the other lower side in the cathode forming chamber 29 (the raw material X is, for example, , Ag) is provided with a cathode material evaporation source 48 consisting of a boat made of tungsten or molybdenum for evaporating by heating it to a predetermined temperature.
【0035】また、基板1と陰極材料蒸発源47との間
にシャッター49を、また基板1と陰極材料蒸発源48
との間にシャッター50をそれぞれ配設した。A shutter 49 is provided between the substrate 1 and the cathode material evaporation source 47, and a substrate 1 and the cathode material evaporation source 48 are provided.
A shutter 50 is provided between each of them.
【0036】保護膜形成室30内を真空ポンプ等の真空
排気系51に接続し、保護膜形成室30内の下方にポリ
尿素膜のような保護膜の原料モノマーY、Z(例えば、
原料Yはジアミンモノマー、原料モノマーZはジイソシ
アナートモノマー)を赤外線ヒーター52a及び52b
で所定温度に加熱し、蒸発させるガラス製または金属製
の保護膜蒸発源53a及び53bをそれぞれ配設した。The inside of the protective film forming chamber 30 is connected to a vacuum exhaust system 51 such as a vacuum pump, and the raw material monomers Y and Z (for example, polyurea film) of a protective film such as a polyurea film are provided below the inside of the protective film forming chamber 30.
The raw material Y is a diamine monomer, and the raw material monomer Z is a diisocyanate monomer).
The protective film evaporation sources 53a and 53b made of glass or metal, which are heated to a predetermined temperature and vaporized, are provided.
【0037】また、基板1と保護膜蒸発源53a及び5
3bとの間にシャッター54を配設し、基板1近傍に保
護膜の水晶振動式膜厚モニター55を配設した。さら
に、保護膜蒸発源53a及び53b内にそれぞれ熱電対
56a及び56bを配設した。The substrate 1 and the protective film evaporation sources 53a and 5
A shutter 54 was provided between the substrate 3 and 3b, and a crystal vibration type film thickness monitor 55 of a protective film was provided near the substrate 1. Further, thermocouples 56a and 56b are arranged in the protective film evaporation sources 53a and 53b, respectively.
【0038】紫外線処理室31内を真空ポンプ等の真空
排気系57に接続し、紫外線処理室31内に紫外線を照
射して低分子のポリ尿素を架橋し、高分子化させてポリ
尿素保護膜とするための紫外線ランプ58を配設した。The inside of the ultraviolet treatment chamber 31 is connected to a vacuum exhaust system 57 such as a vacuum pump, and the inside of the ultraviolet treatment chamber 31 is irradiated with ultraviolet rays to cross-link low molecular weight polyurea and polymerize it to form a polyurea protective film. An ultraviolet lamp 58 is provided for this purpose.
【0039】なお、図4中、59は有機物蒸発源40a
と40bとの間に設けた仕切板、60は保護膜蒸発源5
3aと53bとの間に設けた仕切板をそれぞれ示す。In FIG. 4, 59 is an organic matter evaporation source 40a.
And a partition plate provided between 40b and 40b, 60 is a protective film evaporation source 5
The partition plates provided between 3a and 53b are shown respectively.
【0040】図4に示されたような有機EL素子製造装
置を用いて、ポリ尿素膜等のような絶縁膜をパターニン
グして得た前記基板を図4の真空室27へ仕込み、酸素
プラズマ処理を行う。この場合の処理は、透明陽極上に
残存する絶縁膜の除去と透明陽極上の平坦化を兼ねる。
次いで、成膜室28で正孔輸送層3、発光層4、電子輸
送層6等からなる有機層7を成膜する。その後、陰極形
成室29で陰極を形成し、保護膜形成室30で保護膜を
形成し、EL素子が完成される。Using the organic EL device manufacturing apparatus as shown in FIG. 4, the substrate obtained by patterning an insulating film such as a polyurea film is placed in the vacuum chamber 27 of FIG. 4 and subjected to oxygen plasma treatment. I do. The treatment in this case serves to remove the insulating film remaining on the transparent anode and flatten the transparent anode.
Then, the organic layer 7 including the hole transport layer 3, the light emitting layer 4, the electron transport layer 6 and the like is deposited in the deposition chamber 28. Then, a cathode is formed in the cathode forming chamber 29 and a protective film is formed in the protective film forming chamber 30 to complete the EL element.
【0041】上記図3と図4とに示された装置はまた、
基板が、仕込み室から、一体化された絶縁膜形成室を経
て、図4に示された酸素プラズマ処理室、有機層の成膜
室、陰極形成室、随時保護膜形成室へそして次いで取り
出し室へ搬送されるように構成されていてもよい。The apparatus shown in FIGS. 3 and 4 above also includes
The substrate is transferred from the charging chamber through the integrated insulating film forming chamber to the oxygen plasma processing chamber, the organic layer forming chamber, the cathode forming chamber, the occasional protective film forming chamber, and then the take-out chamber shown in FIG. It may be configured to be transported to.
【0042】なお、図2に示したような、絶縁層8がパ
ターン化された陽極(ITO)2の間に埋め込まれて平
坦化されている構造を有する有機EL素子の場合には、
例えば、基板1上にITOをパターニングにより形成
し、その上に絶縁膜を成膜し、次いで、絶縁膜がポリ尿
素からなる時には、(1)紫外線照射(ITO上)し、
(2)加熱現像することにより、又、絶縁膜がSiO2
又はSi3N4からなる時には、フォトリソ工程、(1)
レジスト塗布、(2)露光、(3)エッチング、(4)
レジスト除去により、ITO上の絶縁膜を除去し、残り
の絶縁膜がITO間に埋め込まれて平坦化されるように
し、その後、前記したように、正孔輸送層3、発光層
4、電子輸送層(図示せず)等からなる有機層を成膜
し、次いで陰極5を形成し、保護膜(図示せず)を形成
して、該EL素子を作製してもよい。In the case of an organic EL element having a structure in which the insulating layer 8 is embedded between the patterned anodes (ITO) 2 and planarized as shown in FIG.
For example, ITO is formed on the substrate 1 by patterning, an insulating film is formed thereon, and then, when the insulating film is made of polyurea, (1) UV irradiation (on ITO),
(2) By heat development, the insulating film also has SiO 2
Alternatively, when it is made of Si 3 N 4 , the photolithography process, (1)
Resist coating, (2) exposure, (3) etching, (4)
By removing the resist, the insulating film on the ITO is removed so that the remaining insulating film is embedded between the ITO so as to be planarized, and then, as described above, the hole transport layer 3, the light emitting layer 4, and the electron transport layer. The EL element may be manufactured by forming an organic layer including a layer (not shown) and the like, then forming the cathode 5 and forming a protective film (not shown).
【0043】[0043]
【実施例】以下、本発明の実施例を添付図面を参照して
説明する。Embodiments of the present invention will be described below with reference to the accompanying drawings.
【0044】(実施例1)図1に示す構造の有機EL素
子の作製について説明する。Example 1 Production of an organic EL device having the structure shown in FIG. 1 will be described.
【0045】イソプロパノール中で煮沸洗浄したガラス
基板1へスパッタリング法によりITO(In2O3−1
0%SnO2 )膜2を1000Å成膜した。この基板を
図3に示すポリ尿素膜のような絶縁膜のパターニング装
置の真空室16へ仕込み、1.0×10-3Paに達した
後、バルブ14aを開いて蒸着重合室11へ搬送した。
5.3×10-3Paの圧力下で、4, 4′−ジアミノジ
フェニルメタン(MDA)aと4, 4′−ジフェニルメ
タンジイソシアナート(MDI)bとを蒸発源19a、
19bからそれぞれ蒸発させて、ITO膜2の付いた基
板1へオリゴマー状態のポリ尿素を6000Å堆積させ
た。バルブ14bを開いて、基板を真空室12へ搬送し
て紫外線源24によりフォトマスク25を介して中心波
長254nmの光を30分照射した。次いで、バルブ1
4cを開いて、基板を真空室13へ搬送して、1.33
×10-3Paの圧力下、加熱装置26で基板を200℃
〜300℃の範囲内に加熱し、未露光部の膜を分解、蒸
発させて取り除いた。こうしてITO膜2上へパターニ
ングされたポリ尿素膜8が完成された。この時露光部の
膜厚は2000Åになった。真空室17を経て基板を取
り出し、これを図4に示す有機EL素子製造装置の真空
室(酸素プラズマ処理室)27へ仕込んだ。この処理室
を1.33×10-3Paまで排気した後、酸素を導入
し、6.65Paの圧力で、RF電源により50Wのパ
ワーでプラズマ処理を5分間行った。ゲートバルブ32
aを開いて、この基板を成膜室28へ搬送し、6.65
×10-4Paの真空度でN, N′−ジフェニル−N,
N′−ビス(3−メチルフェニル)−1, 1′−ジフェ
ニル−4, 4′−ジアミン(TPD)を蒸発源38aよ
り蒸発させ、基板1上へ正孔輸送層3を500Å堆積さ
せた。次に、8−オキシキノリノアルミニウム錯体(A
lq3 )を蒸発源38bより蒸発させ、発光層4を50
0Å成膜した。その後、ゲートバルブ32bを開いて、
基板を陰極形成室29へ搬送し、1.33×10-4Pa
の真空度でマグネシウムと銀とを蒸発源47、48より
10:1の原子比で蒸発させ、MgAg陰電極5を20
00Å成膜して有機EL素子を完成した。ITO (In 2 O 3 −1) was formed on the glass substrate 1 washed by boiling in isopropanol by a sputtering method.
A 0% SnO 2 ) film 2 was formed at 1000 Å. This substrate was charged into a vacuum chamber 16 of a patterning device for an insulating film such as a polyurea film shown in FIG. 3, and after reaching 1.0 × 10 −3 Pa, the valve 14a was opened and the substrate was transferred to the vapor deposition polymerization chamber 11. .
Under a pressure of 5.3 × 10 −3 Pa, 4,4′-diaminodiphenylmethane (MDA) a and 4,4′-diphenylmethane diisocyanate (MDI) b were evaporated as a source 19a,
From each of 19b, 6000Å of polyurea in an oligomer state was deposited on the substrate 1 having the ITO film 2 by evaporation. The valve 14b was opened, the substrate was transferred to the vacuum chamber 12, and light having a central wavelength of 254 nm was irradiated by the ultraviolet source 24 through the photomask 25 for 30 minutes. Then valve 1
4c is opened, the substrate is transferred to the vacuum chamber 13, and 1.33
The substrate is heated to 200 ° C. with a heating device 26 under a pressure of × 10 −3 Pa.
The film in the unexposed portion was decomposed and evaporated to remove by heating within a range of up to 300 ° C. Thus, the patterned polyurea film 8 was completed on the ITO film 2. At this time, the film thickness of the exposed portion became 2000 liters. The substrate was taken out through the vacuum chamber 17 and loaded into the vacuum chamber (oxygen plasma processing chamber) 27 of the organic EL element manufacturing apparatus shown in FIG. After evacuating the processing chamber to 1.33 × 10 −3 Pa, oxygen was introduced, and plasma treatment was performed for 5 minutes at a pressure of 6.65 Pa and an RF power source at a power of 50 W. Gate valve 32
a is opened, and this substrate is transferred to the film forming chamber 28.
N, N'-diphenyl-N, at a vacuum degree of × 10 -4 Pa
N'-bis (3-methylphenyl) -1,1'-diphenyl-4,4'-diamine (TPD) was evaporated from the evaporation source 38a, and the hole transport layer 3 was deposited on the substrate 1 by 500Å. Next, an 8-oxyquinolino aluminum complex (A
1q 3 ) is evaporated from the evaporation source 38b, and the light emitting layer 4 is heated to 50
0 ° was formed. After that, open the gate valve 32b,
The substrate is transferred to the cathode formation chamber 29 and 1.33 × 10 −4 Pa
With a vacuum degree of, magnesium and silver are evaporated from the evaporation sources 47 and 48 at an atomic ratio of 10: 1, and the MgAg negative electrode 5 is heated to 20%.
An organic EL device was completed by forming a film of 00Å.
【0046】このようにして得られた絶縁パターンを用
いた素子へDC電圧を印加して輝度と電流値とを測定し
たところ、11Vで10500cd/m2 (130mA
/cm2 )の輝度が得られた。発光開始電圧は3Vであ
った。一方、絶縁パターンを用いない場合は、1000
0cd/m2 の電流密度は500mA/cm2 であっ
た。従って、絶縁パターンを用いることにより、同一輝
度での電流密度が減少したことがわかる。A luminance and a current value were measured by applying a DC voltage to the element using the insulating pattern thus obtained. It was 10500 cd / m 2 (130 mA at 11 V).
A luminance of / cm 2 ) was obtained. The light emission starting voltage was 3V. On the other hand, when the insulating pattern is not used, 1000
The current density at 0 cd / m 2 was 500 mA / cm 2 . Therefore, it can be seen that the use of the insulating pattern reduced the current density at the same brightness.
【0047】(実施例2)実施例1で作製した有機EL
素子を、ゲートバルブ21cを開いて、保護膜形成室3
0へ搬送し、該素子上へポリ尿素保護膜を1μm堆積さ
せた。即ち、保護膜形成室30を真空排気系51により
1.33×10-3Paまで排気した後、蒸発源53a内
の原料モノマーY(4,4’−ジアミノジフェニルメタ
ン:以下MDAという)の温度を熱電対56aで測定し
ながらヒーター52aで100℃に加熱すると共に、蒸
発源53b内の原料モノマーZ(4,4’−ジフェニル
メタンジイソシアナート:以下MDIという)の温度を
熱電対56bで測定しながらヒーター52bで70℃に
加熱し、MDA:MDIのモノマー組成比が1:1にな
るようにそれぞれの蒸発レートを設定後、シャッター5
4の開閉操作によりMDAとMDIとを蒸発させて、膜
厚モニター55により陰極上に膜厚1μmに堆積させた
後、陰極上で重合させてポリ尿素膜を形成した。(Example 2) Organic EL prepared in Example 1
Open the gate valve 21c to open the protective film forming chamber 3
Then, the polyurea protective film was deposited on the device to a thickness of 1 μm. That is, after the protective film forming chamber 30 is evacuated to 1.33 × 10 −3 Pa by the vacuum exhaust system 51, the temperature of the raw material monomer Y (4,4′-diaminodiphenylmethane: hereinafter referred to as MDA) in the evaporation source 53a is changed. While heating with the heater 52a to 100 ° C. while measuring with the thermocouple 56a, while measuring the temperature of the raw material monomer Z (4,4′-diphenylmethane diisocyanate: hereinafter referred to as MDI) in the evaporation source 53b with the thermocouple 56b. After heating to 70 ° C. by the heater 52b and setting each evaporation rate so that the monomer composition ratio of MDA: MDI becomes 1: 1, the shutter 5
MDA and MDI were evaporated by the opening / closing operation of No. 4 and deposited to a film thickness of 1 μm on the cathode by the film thickness monitor 55, and then polymerized on the cathode to form a polyurea film.
【0048】かくして得られた素子について、電流密度
10mA/cm2 (初期輝度500cd/m2 )で、大
気中で連続駆動させたところ、輝度半減時間は730時
間であった。非発光領域は300時間後ぐらいから出現
するが、その径は100μmより大きくはならなかっ
た。The device thus obtained was continuously driven in the atmosphere at a current density of 10 mA / cm 2 (initial brightness of 500 cd / m 2 ) and the brightness half-life was 730 hours. The non-emission region appeared after about 300 hours, but its diameter did not become larger than 100 μm.
【0049】(実施例3)ITO/ポリ尿素パターン/
TPD(正孔輸送層)500Å/Alq3 (発光層)1
00Å/ポリアゾメチン(電子輸送層)300Å/Mg
Ag(陰極)2000Å)/ポリ尿素保護膜10000
Åのような構造を有する有機EL素子を作製した。(Example 3) ITO / polyurea pattern /
TPD (hole transport layer) 500Å / Alq 3 (light emitting layer) 1
00Å / polyazomethine (electron transport layer) 300Å / Mg
Ag (cathode) 2000Å) / polyurea protective film 10000
An organic EL device having a structure like Å was produced.
【0050】Alq3 の成膜までは実施例1と同じプロ
セスを繰り返した。図4の成膜室28の有機物蒸発源4
0aへテレフタルアルデヒド、有機物蒸発源40bへパ
ラフェニレンジアミンをそれぞれ充填し、共蒸着を行
い、ポリアゾメチン膜を300Å成膜した。MgAg電
極以降の作製プロセスは実施例1及び2記載と同じプロ
セスを繰り返した。The same process as in Example 1 was repeated until the film formation of Alq 3 . Organic substance evaporation source 4 in the film forming chamber 28 of FIG.
0a was filled with terephthalaldehyde, and organic source 40b was filled with para-phenylenediamine, and co-evaporation was performed to form a polyazomethine film having a thickness of 300Å. The manufacturing process after the MgAg electrode was the same as that described in Examples 1 and 2.
【0051】かくして得られた有機EL素子を、電流密
度10mA/cm2 、700cd/m2 で、大気中で連
続駆動させたところ、輝度半減時間は1000時間であ
った。非発光領域は300時間後ぐらいから出現する
が、その径は100μmより大きくはならなかった。The organic EL device thus obtained was continuously driven in the atmosphere at a current density of 10 mA / cm 2 and 700 cd / m 2 , and the luminance half-life was 1000 hours. The non-emission region appeared after about 300 hours, but its diameter did not become larger than 100 μm.
【0052】(実施例4)絶縁層8としてポリ尿素膜の
代わりにSiO2 膜を用いた例を示す。(Embodiment 4) An example in which a SiO 2 film is used as the insulating layer 8 instead of the polyurea film is shown.
【0053】ITO成膜した基板を既存のプラズマCV
D装置へセットし、20SCCMのSiH4 、30SC
CMのO2 を流し、基板温度200℃、0.6Pa、2
00Wの条件でSiO2 膜を3000Å堆積させた。こ
の基板をレジストプロセスによりエッチングを行い、絶
縁層(SiO2 膜)8のパターニングを行った。その
後、TPD、Alq3 、MgAg、ポリ尿素保護膜の順
に成膜を行い有機EL素子を作製した。The substrate on which the ITO film is formed is converted into the existing plasma CV.
Set it in the D device, and 20 SCCM of SiH 4 , 30 SC
O 2 of CM is flowed, the substrate temperature is 200 ° C., 0.6 Pa, 2
A SiO 2 film of 3000 Å was deposited under the condition of 00W. This substrate was etched by a resist process to pattern the insulating layer (SiO 2 film) 8. Then, TPD, Alq 3 , MgAg, and a polyurea protective film were formed in this order to manufacture an organic EL device.
【0054】かくして得られた素子を、電流密度10m
A/cm2 、初期輝度500cd/m2 で、大気中で連
続駆動させたところ、輝度半減時間は500時間であっ
た。非発光領域は300時間後ぐらいから出現するが、
その径は100μmより大きくはならなかった。The element thus obtained was applied with a current density of 10 m.
When continuously driven in the atmosphere at A / cm 2 and an initial luminance of 500 cd / m 2 , the luminance half time was 500 hours. The non-emissive area appears after about 300 hours,
Its diameter did not become larger than 100 μm.
【0055】(実施例5)絶縁層8としてGeO膜を用
いた例を示す。Example 5 An example in which a GeO film is used as the insulating layer 8 will be shown.
【0056】ITO成膜した基板にステンレス製のパタ
ーニングされた金属マスクを密着させ、GeO膜の成膜
装置へセットした。GeOは、タンタル又はモリブデン
製のポートによる抵抗加熱法により蒸発させ、2000
Å堆積させた。このようなマスク蒸着によりGeOのパ
ターンを形成した。その後、TPD、Alq3 、MgA
g、ポリ尿素保護膜の順に成膜を行い、有機EL素子を
作製した。A patterned metal mask made of stainless steel was brought into close contact with the substrate on which the ITO film was formed, and the substrate was set in a GeO film forming apparatus. GeO is evaporated by a resistance heating method using a port made of tantalum or molybdenum to obtain 2000
た Deposited. A GeO pattern was formed by such mask deposition. After that, TPD, Alq 3 , MgA
g and a polyurea protective film were formed in this order to manufacture an organic EL device.
【0057】かくして得られた素子を、電流密度10m
A/cm2 、初期輝度500cd/m2 で、大気中で連
続駆動させたところ、輝度半減時間は700時間であっ
た。非発光領域は300時間後ぐらいから出現するが、
その径は100μmより大きくはならなかった。The device thus obtained was applied with a current density of 10 m.
When continuously driven in the atmosphere at A / cm 2 and an initial luminance of 500 cd / m 2 , the luminance half time was 700 hours. The non-emissive area appears after about 300 hours,
Its diameter did not become larger than 100 μm.
【0058】(実施例6)絶縁層8としてSi3N4膜を
用いた例を示す。Example 6 An example using a Si 3 N 4 film as the insulating layer 8 will be described.
【0059】ITO成膜した基板を既存のプラズマCV
D装置へセットし、20SCCMのSiH4 、30SC
CMのN2 を流し、基板温度250℃、0.6Pa、2
00Wの条件でSi3N4膜を3000Å堆積させた。こ
の基板をレジストプロセスによりエッチングを行い、絶
縁層(Si3N4膜)8のパターニングを行った。その
後、TPD、Alq3 、MgAg、ポリ尿素保護膜の順
に成膜を行い有機EL素子を作製した。The existing plasma CV is applied to the substrate on which the ITO film is formed.
Set it in the D device, and 20 SCCM of SiH 4 , 30 SC
Pour N 2 of CM, substrate temperature 250 ° C., 0.6 Pa, 2
A Si 3 N 4 film was deposited at 3000 W under the condition of 00W. This substrate was etched by a resist process to pattern the insulating layer (Si 3 N 4 film) 8. Then, TPD, Alq 3 , MgAg, and a polyurea protective film were formed in this order to manufacture an organic EL device.
【0060】かくして得られた素子を、電流密度10m
A/cm2 、初期輝度500cd/m2 で、大気中で連
続駆動させたところ、輝度半減時間は500時間であっ
た。非発光領域は300時間後ぐらいから出現するが、
その径は100μmより大きくはならなかった。The element thus obtained was applied with a current density of 10 m.
When continuously driven in the atmosphere at A / cm 2 and an initial luminance of 500 cd / m 2 , the luminance half time was 500 hours. The non-emissive area appears after about 300 hours,
Its diameter did not become larger than 100 μm.
【0061】なお、図2に示すような、絶縁膜8がパタ
ーン化された陽極(ITO)2の間に設けられている構
造を有する有機EL素子の場合も、上記実施例と同様の
結果が得られる。In the case of the organic EL element having a structure in which the insulating film 8 is provided between the patterned anodes (ITO) 2 as shown in FIG. can get.
【0062】[0062]
【発明の効果】本発明の有機EL素子によれば、平坦な
透明陽極上又は陽極間へ絶縁層のパターンが形成されて
いるために、陽極のエッジの影響がなくなるので、素子
の短絡、非発光部の増加といった問題がなくなる。According to the organic EL element of the present invention, since the pattern of the insulating layer is formed on the flat transparent anode or between the anodes, the influence of the edge of the anode is eliminated, so that the element is not short-circuited or non-exposed. The problem of increasing the number of light emitting parts is eliminated.
【0063】また、絶縁層を細かくパターニングでき、
陰極はベタ付けでよいので、小さな面積の発光面を得る
ことができる。そのため、ディスプレイを作製する上で
有利である。Further, the insulating layer can be finely patterned,
Since the cathode may be solid, a light emitting surface with a small area can be obtained. Therefore, it is advantageous in manufacturing a display.
【0064】さらに、絶縁層パターンがポリ尿素を用い
て形成される場合、耐電圧が1000MV/m以上ある
ので、絶縁層の厚さを薄くでき、1000Åぐらいまで
は可能である。このため、素子全体を平坦化できる。Further, when the insulating layer pattern is formed by using polyurea, the withstand voltage is 1000 MV / m or more, so that the thickness of the insulating layer can be reduced to about 1000 Å. Therefore, the entire element can be flattened.
【図1】本発明の有機EL素子の一実施例の構造を示す
模式的部分断面図である。FIG. 1 is a schematic partial cross-sectional view showing the structure of an embodiment of an organic EL device of the present invention.
【図2】本発明の有機EL素子の他の実施例の構造を示
す模式的部分断面図である。FIG. 2 is a schematic partial cross-sectional view showing the structure of another embodiment of the organic EL element of the present invention.
【図3】本発明における絶縁層の成膜装置の一例の説明
線図である。FIG. 3 is an explanatory diagram of an example of an insulating layer forming apparatus according to the present invention.
【図4】本発明の有機EL素子製造装置の一例の説明線
図である。FIG. 4 is an explanatory diagram of an example of an organic EL element manufacturing apparatus of the present invention.
【図5】従来技術の有機EL素子の一例の構造を示す模
式的部分断面図である。FIG. 5 is a schematic partial cross-sectional view showing the structure of an example of a conventional organic EL element.
【図6】従来技術の3層構造の有機EL素子の一例の構
造を示す模式的部分断面図である。FIG. 6 is a schematic partial cross-sectional view showing a structure of an example of a conventional organic EL device having a three-layer structure.
【図7】従来技術の有機EL素子の問題点を説明するた
めに該素子の一例の構造を示す模式的部分断面図であ
る。FIG. 7 is a schematic partial cross-sectional view showing the structure of an example of a conventional organic EL device for explaining the problems.
1 基板 2 透明陽極 3 正孔輸送層 4 発光層 5 金属陰極 6 電子輸送層 7 有機層 8 絶縁層 11 蒸着重合室 12 露光室 13 現像室(真空室) 14a、14b、
14c、14d バルブ 15a、15b 真空排気系 16、17 真空
室 18 基板ホルダー 19a、19b
蒸発源 20a、20b 蒸発モニター 21a、21b
ヒーター 22 シャッター 23 仕切板 24 紫外線源 25 フォトマス
ク 26 加熱装置 27 酸素プラズ
マ処理室 28 有機化合物膜の成膜室 29 陰極形成室 30 保護膜形成室 31 紫外線処理
室 32a、32b、32c、32d ゲートバルブ 33 トレー式搬送系 34 真空排気系 35 RF電極 36 真空排気系 37a、37b ヒーター 38a、38b
色素蒸発源 39a、39b 赤外線ランプ 40a、40b
有機物蒸発源 41 シースヒーター 42a、42b
シャッター 43 シャッター 44a、44b
熱電対 45 真空排気系 46 ヒーター 47、48 陰極材料蒸発源 49、50 シャ
ッター 51 真空排気系 52a、52b
赤外線ヒーター 53a、53b 保護膜蒸発源 54 シャッター 55 水晶振動式膜厚モニター 56a、56b
熱電対 57 真空排気系 58 紫外線ラン
プ 59、60 仕切板 a、b 原料モノマ T 色素原料 U、V、Y、Z 原料モノマー W、X 陰極原料1 Substrate 2 Transparent Anode 3 Hole Transport Layer 4 Light Emitting Layer 5 Metal Cathode 6 Electron Transport Layer 7 Organic Layer 8 Insulating Layer 11 Vapor Deposition Room 12 Exposure Room 13 Development Room (Vacuum Room) 14a, 14b,
14c, 14d Valves 15a, 15b Vacuum exhaust system 16, 17 Vacuum chamber 18 Substrate holder 19a, 19b
Evaporation source 20a, 20b Evaporation monitor 21a, 21b
Heater 22 Shutter 23 Partition plate 24 Ultraviolet source 25 Photomask 26 Heating device 27 Oxygen plasma treatment chamber 28 Organic compound film deposition chamber 29 Cathode formation chamber 30 Protective film formation chamber 31 Ultraviolet treatment chamber 32a, 32b, 32c, 32d Gate valve 33 tray type transfer system 34 vacuum exhaust system 35 RF electrode 36 vacuum exhaust system 37a, 37b heater 38a, 38b
Dye evaporation source 39a, 39b Infrared lamp 40a, 40b
Organic matter evaporation source 41 Sheath heater 42a, 42b
Shutter 43 Shutter 44a, 44b
Thermocouple 45 Vacuum exhaust system 46 Heater 47, 48 Cathode material evaporation source 49, 50 Shutter 51 Vacuum exhaust system 52a, 52b
Infrared heater 53a, 53b Protective film evaporation source 54 Shutter 55 Crystal vibration type film thickness monitor 56a, 56b
Thermocouple 57 Vacuum exhaust system 58 Ultraviolet lamp 59, 60 Partition plate a, b Raw material monomer T Dye raw material U, V, Y, Z Raw material monomer W, X Cathode raw material
Claims (4)
有機エレクトロルミネッセンス素子において、該陽極上
又は陽極間へパターニングにより絶縁層が設けられ、そ
の上に該有機層及び陰極が形成されていることを特徴と
する有機エレクトロルミネッセンス素子。1. In an organic electroluminescence device having an anode, an organic layer and a cathode on a substrate, an insulating layer is provided on the anode or between the anodes by patterning, and the organic layer and the cathode are formed thereon. An organic electroluminescence device characterized by the above.
露光後、加熱現像によりパターニングした構造を用いた
請求項1記載の有機エレクトロルミネッセンス素子。2. The organic electroluminescent device according to claim 1, wherein the insulating layer has a structure in which a polyurea film is exposed to ultraviolet rays and then patterned by heat development.
N4膜又はGeO膜をパターニングした構造を用いた請
求項1記載の有機エレクトロルミネッセンス素子。3. The insulating layer is a SiO 2 film or a Si 3 film.
The organic electroluminescence device according to claim 1, which has a structure obtained by patterning an N 4 film or a GeO film.
パターニングにより絶縁層を形成し、その上に有機層を
形成し、次いでその上に電極パターンのマスク蒸着をせ
ずに陰極を形成して、該絶縁層で囲まれたパターンの中
に発光面が形成されるようにすることを特徴とする有機
エレクトロルミネッセンス素子の作製方法。4. An insulating layer is formed by patterning on an anode provided on a substrate or between the anodes, an organic layer is formed thereon, and then a cathode is formed thereon without mask vapor deposition of an electrode pattern. Then, a light emitting surface is formed in a pattern surrounded by the insulating layer, and a method for manufacturing an organic electroluminescence element.
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|---|---|---|---|
| JP28998895A JP3865807B2 (en) | 1995-11-08 | 1995-11-08 | Organic electroluminescence device |
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| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP28998895A JP3865807B2 (en) | 1995-11-08 | 1995-11-08 | Organic electroluminescence device |
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| Publication Number | Publication Date |
|---|---|
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| JP3865807B2 JP3865807B2 (en) | 2007-01-10 |
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| WO1998003043A1 (en) * | 1996-07-16 | 1998-01-22 | Hewlett-Packard Company | Electroluminescent display device |
| JPH1154274A (en) * | 1997-07-29 | 1999-02-26 | Ulvac Japan Ltd | Organic el element |
| WO1999053725A1 (en) * | 1998-04-15 | 1999-10-21 | Tdk Corporation | Organic el display and method of manufacturing the same |
| WO1999053726A1 (en) * | 1996-12-10 | 1999-10-21 | Tdk Corporation | Organic electroluminescence element and manufacturing method therefor |
| JP2003092188A (en) * | 2001-09-19 | 2003-03-28 | Ulvac Japan Ltd | Organic electroluminescent element and method for manufacturing the same |
| US6798132B2 (en) | 2001-04-23 | 2004-09-28 | Semiconductor Energy Laboratory Co., Ltd. | Display device and method of manufacturing the same |
| JP2006339049A (en) * | 2005-06-02 | 2006-12-14 | Tokki Corp | Sealing film forming device |
| JP2007234526A (en) * | 2006-03-03 | 2007-09-13 | Showa Denko Kk | Display element |
| JP2008235280A (en) * | 2008-04-21 | 2008-10-02 | Dainippon Printing Co Ltd | Method for manufacturing electroluminescence element |
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