JP2734464B2 - Electroluminescence device and method of manufacturing the same - Google Patents
Electroluminescence device and method of manufacturing the sameInfo
- Publication number
- JP2734464B2 JP2734464B2 JP2045717A JP4571790A JP2734464B2 JP 2734464 B2 JP2734464 B2 JP 2734464B2 JP 2045717 A JP2045717 A JP 2045717A JP 4571790 A JP4571790 A JP 4571790A JP 2734464 B2 JP2734464 B2 JP 2734464B2
- Authority
- JP
- Japan
- Prior art keywords
- light emitting
- insulating film
- light
- layer
- interlayer insulating
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Expired - Lifetime
Links
- 238000004519 manufacturing process Methods 0.000 title claims description 14
- 238000005401 electroluminescence Methods 0.000 title description 2
- 239000010410 layer Substances 0.000 claims description 118
- 238000000034 method Methods 0.000 claims description 41
- 239000011229 interlayer Substances 0.000 claims description 40
- 239000000758 substrate Substances 0.000 claims description 30
- 238000007740 vapor deposition Methods 0.000 claims description 30
- 229910004298 SiO 2 Inorganic materials 0.000 claims description 8
- 238000004544 sputter deposition Methods 0.000 claims description 8
- 238000005530 etching Methods 0.000 claims description 7
- 238000000059 patterning Methods 0.000 claims description 3
- 238000001020 plasma etching Methods 0.000 claims description 2
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 claims 1
- 229910052739 hydrogen Inorganic materials 0.000 claims 1
- 239000001257 hydrogen Substances 0.000 claims 1
- 238000002347 injection Methods 0.000 description 39
- 239000007924 injection Substances 0.000 description 39
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- 239000000203 mixture Substances 0.000 description 10
- 230000015572 biosynthetic process Effects 0.000 description 9
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- 230000005684 electric field Effects 0.000 description 7
- 238000000151 deposition Methods 0.000 description 6
- 229910052751 metal Inorganic materials 0.000 description 6
- 239000002184 metal Substances 0.000 description 6
- -1 SiO 2 Chemical class 0.000 description 5
- JHYLKGDXMUDNEO-UHFFFAOYSA-N [Mg].[In] Chemical compound [Mg].[In] JHYLKGDXMUDNEO-UHFFFAOYSA-N 0.000 description 5
- 238000010438 heat treatment Methods 0.000 description 5
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- 239000000956 alloy Substances 0.000 description 4
- 229910045601 alloy Inorganic materials 0.000 description 4
- 230000008021 deposition Effects 0.000 description 4
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- 239000011777 magnesium Substances 0.000 description 4
- 229910052749 magnesium Inorganic materials 0.000 description 4
- 239000012044 organic layer Substances 0.000 description 4
- 238000012545 processing Methods 0.000 description 4
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- 239000011248 coating agent Substances 0.000 description 3
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- KAKZBPTYRLMSJV-UHFFFAOYSA-N Butadiene Chemical compound C=CC=C KAKZBPTYRLMSJV-UHFFFAOYSA-N 0.000 description 2
- UFWIBTONFRDIAS-UHFFFAOYSA-N Naphthalene Chemical compound C1=CC=CC2=CC=CC=C21 UFWIBTONFRDIAS-UHFFFAOYSA-N 0.000 description 2
- 229910006404 SnO 2 Inorganic materials 0.000 description 2
- MWPLVEDNUUSJAV-UHFFFAOYSA-N anthracene Chemical compound C1=CC=CC2=CC3=CC=CC=C3C=C21 MWPLVEDNUUSJAV-UHFFFAOYSA-N 0.000 description 2
- 239000003795 chemical substances by application Substances 0.000 description 2
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- 239000007772 electrode material Substances 0.000 description 2
- 238000005516 engineering process Methods 0.000 description 2
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- 229910052738 indium Inorganic materials 0.000 description 2
- APFVFJFRJDLVQX-UHFFFAOYSA-N indium atom Chemical compound [In] APFVFJFRJDLVQX-UHFFFAOYSA-N 0.000 description 2
- 150000004866 oxadiazoles Chemical class 0.000 description 2
- YNPNZTXNASCQKK-UHFFFAOYSA-N phenanthrene Chemical compound C1=CC=C2C3=CC=CC=C3C=CC2=C1 YNPNZTXNASCQKK-UHFFFAOYSA-N 0.000 description 2
- 229920002120 photoresistant polymer Polymers 0.000 description 2
- 229920000642 polymer Polymers 0.000 description 2
- BBEAQIROQSPTKN-UHFFFAOYSA-N pyrene Chemical compound C1=CC=C2C=CC3=CC=CC4=CC=C1C2=C43 BBEAQIROQSPTKN-UHFFFAOYSA-N 0.000 description 2
- 238000007650 screen-printing Methods 0.000 description 2
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- JCXLYAWYOTYWKM-UHFFFAOYSA-N (2,3,4-triphenylcyclopenta-1,3-dien-1-yl)benzene Chemical compound C1C(C=2C=CC=CC=2)=C(C=2C=CC=CC=2)C(C=2C=CC=CC=2)=C1C1=CC=CC=C1 JCXLYAWYOTYWKM-UHFFFAOYSA-N 0.000 description 1
- VERMWGQSKPXSPZ-BUHFOSPRSA-N 1-[(e)-2-phenylethenyl]anthracene Chemical class C=1C=CC2=CC3=CC=CC=C3C=C2C=1\C=C\C1=CC=CC=C1 VERMWGQSKPXSPZ-BUHFOSPRSA-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
- KWIVRAVCZJXOQC-UHFFFAOYSA-N 3h-oxathiazole Chemical compound N1SOC=C1 KWIVRAVCZJXOQC-UHFFFAOYSA-N 0.000 description 1
- 229910017090 AlO 2 Inorganic materials 0.000 description 1
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 1
- 241000511976 Hoya Species 0.000 description 1
- CBENFWSGALASAD-UHFFFAOYSA-N Ozone Chemical compound [O-][O+]=O CBENFWSGALASAD-UHFFFAOYSA-N 0.000 description 1
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- 229910052802 copper Inorganic materials 0.000 description 1
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- 125000000332 coumarinyl group Chemical class O1C(=O)C(=CC2=CC=CC=C12)* 0.000 description 1
- 238000001035 drying Methods 0.000 description 1
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- 238000010292 electrical insulation Methods 0.000 description 1
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- 150000008376 fluorenones Chemical class 0.000 description 1
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 description 1
- 229910052737 gold Inorganic materials 0.000 description 1
- 239000010931 gold Substances 0.000 description 1
- 229940083761 high-ceiling diuretics pyrazolone derivative Drugs 0.000 description 1
- 150000007857 hydrazones Chemical class 0.000 description 1
- 150000002460 imidazoles Chemical class 0.000 description 1
- 230000001771 impaired effect Effects 0.000 description 1
- 229910003437 indium oxide Inorganic materials 0.000 description 1
- PJXISJQVUVHSOJ-UHFFFAOYSA-N indium(iii) oxide Chemical compound [O-2].[O-2].[O-2].[In+3].[In+3] PJXISJQVUVHSOJ-UHFFFAOYSA-N 0.000 description 1
- AMGQUBHHOARCQH-UHFFFAOYSA-N indium;oxotin Chemical compound [In].[Sn]=O AMGQUBHHOARCQH-UHFFFAOYSA-N 0.000 description 1
- 239000012212 insulator Substances 0.000 description 1
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- QSHDDOUJBYECFT-UHFFFAOYSA-N mercury Chemical compound [Hg] QSHDDOUJBYECFT-UHFFFAOYSA-N 0.000 description 1
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- 150000007978 oxazole derivatives Chemical class 0.000 description 1
- 125000002080 perylenyl group Chemical group C1(=CC=C2C=CC=C3C4=CC=CC5=CC=CC(C1=C23)=C45)* 0.000 description 1
- CSHWQDPOILHKBI-UHFFFAOYSA-N peryrene Natural products C1=CC(C2=CC=CC=3C2=C2C=CC=3)=C3C2=CC=CC3=C1 CSHWQDPOILHKBI-UHFFFAOYSA-N 0.000 description 1
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- JEXVQSWXXUJEMA-UHFFFAOYSA-N pyrazol-3-one Chemical class O=C1C=CN=N1 JEXVQSWXXUJEMA-UHFFFAOYSA-N 0.000 description 1
- 150000003219 pyrazolines Chemical class 0.000 description 1
- 239000010453 quartz Substances 0.000 description 1
- 238000005215 recombination Methods 0.000 description 1
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- 238000011160 research Methods 0.000 description 1
- 230000027756 respiratory electron transport chain Effects 0.000 description 1
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N silicon dioxide Inorganic materials O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 1
- 229910052709 silver Inorganic materials 0.000 description 1
- 239000004332 silver Substances 0.000 description 1
- 239000007787 solid Substances 0.000 description 1
- 239000000243 solution Substances 0.000 description 1
- 238000005507 spraying Methods 0.000 description 1
- PJANXHGTPQOBST-UHFFFAOYSA-N stilbene Chemical class C=1C=CC=CC=1C=CC1=CC=CC=C1 PJANXHGTPQOBST-UHFFFAOYSA-N 0.000 description 1
- 229940042055 systemic antimycotics triazole derivative Drugs 0.000 description 1
- 238000012360 testing method Methods 0.000 description 1
- JLZUZNKTTIRERF-UHFFFAOYSA-N tetraphenylethylene Chemical group C1=CC=CC=C1C(C=1C=CC=CC=1)=C(C=1C=CC=CC=1)C1=CC=CC=C1 JLZUZNKTTIRERF-UHFFFAOYSA-N 0.000 description 1
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- IBBLKSWSCDAPIF-UHFFFAOYSA-N thiopyran Chemical compound S1C=CC=C=C1 IBBLKSWSCDAPIF-UHFFFAOYSA-N 0.000 description 1
- XOLBLPGZBRYERU-UHFFFAOYSA-N tin dioxide Chemical compound O=[Sn]=O XOLBLPGZBRYERU-UHFFFAOYSA-N 0.000 description 1
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Description
【発明の詳細な説明】 〔産業上の利用分野〕 本発明はエレクトロルミネッセンス素子及びその製造
方法に関し、詳しくは層間に絶縁膜を存在させてなるパ
ターン精度が良好で発光面の均一性が高いエレクトロル
ミネッセンス素子、及びそれを簡易な工程で効率良く製
造する方法に関する。Description: BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to an electroluminescent device and a method for manufacturing the same, and more particularly, to an electroluminescent device having an insulating film between layers, which has good pattern accuracy and high uniformity of a light emitting surface. The present invention relates to a luminescent element and a method for efficiently manufacturing the luminescent element with simple steps.
エレクトロルミネッセンス素子（以下EL素子という）
は、自己発光のため視認性が高く、また完全固体素子で
あるため耐衝撃性に優れるという特徴を有しており、各
種の表示装置における発光素子等の利用が試みられてい
る。特に有機EL素子は陰極／発光層／正孔注入層／陽
極，陰極／電子注入層／発光層／陽極，陰極／電子注入
層／発光層／正孔注入層／陽極，陽極／発光層／電子注
入層／陰極／等の構成のものが開発されている。これら
は、（１）低電圧の印加するだけで発光する、（２）高
輝度高効率の発光が得られる、（３）多色表示が可能で
あるなどの優れた特性を有しており、発光材料，電荷注
入層，電極材料等の研究が盛んに行われている（「アプ
ライド・フィズィクス・レターズ」第51巻,913頁（1987
年）；「アプライド・フィズィクス・レターズ」第55
巻,1489頁（1989年）；「ジャーナル・オブ・アプライ
ド・フィズィクス」第65巻,3610頁（1989年））。Electroluminescence device (hereinafter referred to as EL device)
Has a feature that it has high visibility due to self-emission and is excellent in impact resistance because it is a completely solid element, and attempts have been made to use light emitting elements and the like in various display devices. In particular, organic EL devices include cathode / light-emitting layer / hole injection layer / anode, cathode / electron injection layer / light-emitting layer / anode, cathode / electron injection layer / light-emitting layer / hole injection layer / anode, anode / light-emitting layer / electron. An injection layer / cathode / etc. Configuration has been developed. These have excellent characteristics such as (1) light emission only by applying a low voltage, (2) high-luminance and high-efficiency light emission, and (3) multicolor display is possible. Research on luminescent materials, charge injection layers, electrode materials, etc. has been actively conducted ("Applied Fixix Letters", Vol. 51, p. 913 (1987).
Year); “Applied Fizzix Letters” No. 55
Volume, 1489 (1989); Journal of Applied Fidics, 65, 3610 (1989)).
従来、有機EL素子を作製するにあたっては、素子の対
向電極はマスクを基板上にかけ発光素子形成部分に電極
を蒸着する方法により製造されているが、蒸着の廻り込
みにより対向電極のパターン精度が悪くなるという問題
があった。また、有機層を形成する際のマスクと、対向
電極を形成する際のマスクが異なるため、マスク交換機
構を持たない通常の蒸着装置においては、対向電極形成
前に一度真空を破り、真空槽を開けマスク交換を行った
り、マスクを設置する必要があり、工程が複雑である。
この場合、有機層と対向電極の界面が汚染され、均一性
等の良好なEL素子を得ることが困難であった。Conventionally, when manufacturing an organic EL element, the opposing electrode of the element is manufactured by a method in which a mask is placed on a substrate and an electrode is vapor-deposited on a light-emitting element formation portion, but the pattern accuracy of the opposing electrode is poor due to the evaporation. There was a problem of becoming. In addition, since the mask for forming the organic layer and the mask for forming the counter electrode are different, in a normal vapor deposition apparatus without a mask exchange mechanism, the vacuum is once broken before forming the counter electrode, and the vacuum chamber is opened. It is necessary to open the mask and replace it, or to install a mask, and the process is complicated.
In this case, the interface between the organic layer and the counter electrode was contaminated, and it was difficult to obtain an EL device having good uniformity and the like.
さらに、有機EL素子において、陰極にマグネシウムと
第二金属系の合金または混合物の電極を二元蒸着法によ
り形成し使用することが多いが、これらを対向電極に使
用した場合電極を蒸着させる際、廻り込みによるダレ部
分を生じる。そのため、マグネシウムと第二金属系の廻
り込みの程度が異なることから、この部分の組成が対向
電極面内とずれるため、発光の均一性が損なわれるとい
う問題があった。Furthermore, in the organic EL element, an electrode of an alloy or a mixture of magnesium and a second metal system is often formed and used for a cathode by a binary vapor deposition method, but when these are used for a counter electrode, when depositing an electrode, A dripping portion occurs due to wraparound. For this reason, since the degree of wraparound between magnesium and the second metal system is different, the composition of this portion is shifted from the surface of the counter electrode, and there is a problem that the uniformity of light emission is impaired.
そこで、本発明者らは、上記の従来の技術の問題点を
解決し、パターン精度の優れた発光面の均一なEL素子
を、マスク交換等の操作を最小限度でしか必要としない
工程で製造する方法を開発すべく鋭意研究を重ねた。そ
の結果、層間絶縁膜を設けたEL素子が、上記目的が達成
できることを見出した。本発明はかかる知見に基いて完
成したものである。Therefore, the present inventors have solved the above-mentioned problems of the conventional technology and manufactured an EL element having a uniform light emitting surface with excellent pattern accuracy in a process that requires only minimal operations such as mask replacement. We have been working hard to develop ways to do this. As a result, they have found that an EL element provided with an interlayer insulating film can achieve the above object. The present invention has been completed based on such findings.
すなわち本発明は、基板に設けられた下部電極、発光
層を含む有機多層部及び対向電極からなる発光素子部分
を含むEL素子において、下部電極と対向電極との間に、
パターン加工された層間絶縁膜を存在させた非発光素子
部分を保有し、且つ該層間絶縁膜の開口部には発光層を
含む有機多層部と対向電極が設けられているとともに、
実質的に正孔または電子の注入ができるように有機多層
部と対向電極が接合され配置されていることを特徴とす
るEL素子を提供するものである。また本発明は、基板に
設けられた下部電極上に層間絶縁膜をパターン加工にて
膜付けした後、形成された層間絶縁膜の開口部に発光層
を含む有機多層部および対向電極を形成する工程を行う
ことを特徴とするEL素子の製造方法をも提供するもので
ある。That is, the present invention provides a lower electrode provided on a substrate, an EL element including a light emitting element portion including an organic multilayer portion including a light emitting layer and a counter electrode, between the lower electrode and the counter electrode,
Having a non-light emitting element portion in which a patterned interlayer insulating film is present, and an organic multilayer portion including a light emitting layer and a counter electrode are provided in an opening of the interlayer insulating film,
It is an object of the present invention to provide an EL device characterized in that an organic multilayer portion and a counter electrode are joined and arranged so that holes or electrons can be substantially injected. Further, according to the present invention, after an interlayer insulating film is formed on a lower electrode provided on a substrate by pattern processing, an organic multilayer portion including a light emitting layer and a counter electrode are formed in openings of the formed interlayer insulating film. Another object of the present invention is to provide a method for manufacturing an EL device, which comprises performing a step.
本発明のEL素子は、素子の基板上に形成される下部電
極（陽極あるいは陰極）、発光層を含む有機多層部及び
その上に形成される対向電極（下部電極が陽極である場
合は陰極であり、陰極である場合は陽極である。）から
なる構成を発光素子部分に持ち、非発光素子部分には、
下部電極と対向電極の間にパターン加工された層間絶縁
膜を設けたことを特徴である。ここで、パターン加工さ
れた層間絶縁膜とは、発光素子を形成する部分（発光素
子部分）を開口部として発光素子を形成しない部分（非
発光素子部分）に施される下部電極と対向電極の間にあ
る絶縁膜である。この膜の上にさらに発光材料層及び対
向電極を形成すると、パターン加工された開口部のみに
通電可能となり、その部分にのみパターン精度の良い発
光が得られる。尚、層間絶縁膜は下部電極と対向電極の
間に発光層を含む有機多層部が存在しない場合にも、こ
れら下部電極と対向電極の短絡を防ぎ電気的に絶縁を防
ぐ層である場合もある。The EL device of the present invention comprises a lower electrode (anode or cathode) formed on a substrate of the device, an organic multilayer portion including a light-emitting layer, and a counter electrode formed thereon (a cathode when the lower electrode is an anode). The light emitting element portion, and the non-light emitting element portion has
It is characterized in that a patterned interlayer insulating film is provided between the lower electrode and the counter electrode. Here, the patterned interlayer insulating film refers to a lower electrode and a counter electrode which are formed on a portion where a light emitting element is formed (a light emitting element portion) and a portion where a light emitting element is not formed (a non light emitting element portion). This is the insulating film between them. If a light emitting material layer and a counter electrode are further formed on this film, it is possible to conduct electricity only to the patterned openings, and light emission with high pattern accuracy can be obtained only at those portions. Note that the interlayer insulating film may be a layer that prevents short circuit between the lower electrode and the counter electrode and prevents electrical insulation even when the organic multilayer portion including the light emitting layer does not exist between the lower electrode and the counter electrode. .
この層間絶縁膜としては、絶縁体である材料からなる
膜であれば、特に制限はなく種々のものが使用できる。
具体的には無機物としては、SiO2,Si3N4,AlO2等の酸化
物、窒化物などが挙げられ、有機物としてはポリイミド
等の高分子が挙げられる。これらの材料を用いて製膜す
るには、通常無機物の場合、蒸着法，スパッタリング
法，プラズマCVD法などの方法で行われ、また有機物の
場合、スピンコート法，キャスト法,LB法などの方法で
行われる。The interlayer insulating film is not particularly limited as long as it is made of a material that is an insulator, and various types can be used.
Specifically, examples of the inorganic substance include oxides and nitrides such as SiO 2 , Si 3 N 4 and AlO 2 , and examples of the organic substance include polymers such as polyimide. Film formation using these materials is usually performed by methods such as vapor deposition, sputtering, and plasma CVD for inorganic substances, and methods such as spin coating, casting, and LB for organic substances. Done in
さらに本発明において、この層間絶縁膜は開口部すな
わち発光素子形成部分を設けるパターン加工を施された
ものである。ここで、パターン加工は種々の方法で行う
ことができ、特に制限はないが、フォトレジストを用い
たエッチング法（ウエットエッチングまたはドライエッ
チング）が好適である。エッチングにあたっては、膜の
材料，厚さ，工程等より適宜ウエットエッチング剤ある
いはドライエッチングガス（例えばSiO2のエッチングの
ときにはCHF3）を選択すればよい。このエッチングにお
いて、感光性ポリイミドコーテング剤を用いるとフォト
レジスト剤を使用する必要がなく工程が簡便で好まし
い。Further, in the present invention, this interlayer insulating film is subjected to pattern processing for providing an opening, that is, a light emitting element forming portion. Here, the pattern processing can be performed by various methods, and there is no particular limitation, but an etching method using a photoresist (wet etching or dry etching) is preferable. In etching, a wet etching agent or a dry etching gas (for example, CHF 3 when etching SiO 2 ) may be appropriately selected depending on the material, thickness, process and the like of the film. In this etching, use of a photosensitive polyimide coating agent does not require the use of a photoresist agent, and the process is simple and preferable.
また、本発明において層間絶縁膜は、少なくとも1MV/
cmの電界強度に耐えうるものであることが好ましい。1M
V/cmより耐圧の低い材料を用いた場合、リーク電流によ
り素子の配線が破断するなどの問題を生じることがあ
る。通常、スパッタリング法又はCVD法により形成され
るSiO2層,Y2O3層，スピンコート法で形成されたポリイ
ミド層などは充分な電界強度を有しており、好適に利用
できる。In the present invention, the interlayer insulating film has at least 1 MV /
Preferably, it can withstand an electric field strength of cm. 1M
When a material having a withstand voltage lower than V / cm is used, a problem such as breakage of element wiring due to a leak current may occur. Usually, a SiO 2 layer, a Y 2 O 3 layer formed by a sputtering method or a CVD method, a polyimide layer formed by a spin coating method, and the like have a sufficient electric field strength and can be suitably used.
また、膜の厚さは特に制限はないが、通常は1000Å〜
５μｍである。1000Å未満であると、通常有機EL素子に
使用される駆動電圧３〜20Vで下部電極と対向電極間の
絶縁破壊，リーク電流等の好ましくない事態が生じる。
膜の厚さが５μｍを越えると絶縁膜開口部端の断差部分
で対向電極の断線が生じ好ましくない。膜厚を厚くする
場合、断線を防ぐためには、断差部分を斜めにする、い
わゆるテーパー加工を行うと良い。Further, the thickness of the film is not particularly limited, but is usually 1000Å
5 μm. If it is less than 1000 °, undesired situations such as a dielectric breakdown between the lower electrode and the counter electrode and a leak current occur at a drive voltage of 3 to 20 V normally used for an organic EL device.
If the thickness of the film exceeds 5 μm, disconnection of the opposing electrode occurs at the difference between the openings of the insulating film, which is not preferable. When the film thickness is increased, in order to prevent disconnection, it is preferable to perform so-called taper processing in which the difference portion is inclined.
本発明のEL素子において、層間絶縁膜として黒色のも
のまたは濃色のものを使用すると、より発光素子のコン
トラストが上昇して好ましい。このような例には黒色色
素（カーボンブラック等）を混入したポリイミド等があ
る。In the EL device of the present invention, it is preferable to use a black or dark color as the interlayer insulating film because the contrast of the light emitting device is further increased. Examples of such a material include polyimide mixed with a black pigment (such as carbon black).
ちなみに、この層間絶縁膜は、従来から、対向電極上
に素子を封止するために形成される封止膜とは、根本的
に機能の異なるものであるとを付言しておく。Incidentally, it is added that the interlayer insulating film has a fundamentally different function from the sealing film formed for sealing the element on the counter electrode.
本発明のEL素子の構成は、また、ZnS:Mnなどの無機蛍
光材を発光層として用いた電極／絶縁膜／発光層／絶縁
膜／電極等の無機EL素子に用いられる絶縁膜とも異なる
ものである。つまり本発明の層間絶縁膜は、非発光素子
部分を形成するためのものであるからである。発光素子
部分においては、下部電極／発光層を含む有機多層部／
対向電極の構成であり、非発光素子部分においては、下
部電極／層間絶縁膜／発光層を含む有機多層部／対向電
極、または下部電極／層間絶縁膜／対向電極、または下
部電極／層間絶縁膜の構成になっている。The structure of the EL device of the present invention is also different from an insulating film used for an inorganic EL device such as an electrode / insulating film / light emitting layer / insulating film / electrode using an inorganic fluorescent material such as ZnS: Mn as a light emitting layer. It is. That is, the interlayer insulating film of the present invention is for forming a non-light emitting element portion. In the light emitting element portion, a lower electrode / an organic multilayer portion including a light emitting layer /
In the non-light emitting element portion, the lower electrode / interlayer insulating film / organic multilayer portion including light emitting layer / counter electrode, or lower electrode / interlayer insulating film / counter electrode, or lower electrode / interlayer insulating film It has a configuration.
本発明においてEL素子の基板としては、透明性を有す
るものが好ましく、一般にガラス，透明プラスチック，
石英等が充当される。厚さについては素子の使用目的な
どにより適宜選定される。また、電極（陽極，陰極）と
しては、金，アルミニウム，インジウム，マグネシウ
ム，銅，銀などの金属，これらの合金，混合物、特開昭
63−295695号公報に開示されている合金または混合物電
極、インジウムチンオキサイド（酸化インジウムと酸化
錫の混合酸化物;ITO）,SnO2,ZnO等の透明電極等が挙げ
られる。これらの中で素子の駆動電圧を低くできるた
め、特開昭63−295695号公報に開示されている合金また
は混合物電極、ITO,SnO2,ZnO等の透明電極が好ましい。
なお陽極には、仕事関数の大きい金属または電気伝導性
化合物が好適であり、また陰極には、仕事関数の小さい
金属または電気伝導性化合物が好適である。これらの電
極は、少なくとも一方が透明あるいは半透明であると、
発光を透過し取り出す効率が良いため好ましい。電極の
厚さは通常、EL素子において行われる範囲で適宜決定さ
れるが、一般に10nm〜１μｍ、特に200nm以下が発光の
透過率を高める場合は好ましい。In the present invention, the substrate of the EL device is preferably a substrate having transparency, and is generally glass, transparent plastic,
Quartz or the like is applied. The thickness is appropriately selected according to the purpose of use of the element. As the electrodes (anode, cathode), metals such as gold, aluminum, indium, magnesium, copper, silver, alloys and mixtures thereof,
63-295695 discloses an alloy or mixture electrode, a transparent electrode such as indium tin oxide (a mixed oxide of indium oxide and tin oxide; ITO), SnO 2 , and ZnO. Among these, the alloy or mixture electrodes disclosed in JP-A-63-295695, and transparent electrodes such as ITO, SnO 2 , and ZnO are preferable because the driving voltage of the element can be lowered.
A metal with a high work function or an electrically conductive compound is suitable for the anode, and a metal or an electrically conductive compound with a small work function is suitable for the cathode. If at least one of these electrodes is transparent or translucent,
This is preferable because the efficiency of transmitting and extracting light emission is high. The thickness of the electrode is usually appropriately determined within a range performed in the EL element, but is preferably from 10 nm to 1 μm, particularly preferably 200 nm or less, in order to increase the transmittance of light emission.
なお、下部電極及び対向電極はいずれが陽極であって
も陰極であってもよい。また、下部電極は通常スパッタ
リング法，蒸着法，スクリーン印刷法などにより、対向
電極はスパッタリング法，蒸着法等により形成される。
また、下部電極がパターンニングされたものであっても
よい。Note that either the lower electrode or the counter electrode may be an anode or a cathode. The lower electrode is usually formed by a sputtering method, a vapor deposition method, a screen printing method or the like, and the counter electrode is formed by a sputtering method, a vapor deposition method or the like.
Further, the lower electrode may be patterned.
さらに発光層を含む有機多層部とは、EL素子の発光に
必要な有機層であって、具体的には発光層，発光層／正
孔注入層，電子注入層／発光層，電子注入層／発光層／
正孔注入層等の構成のものが挙げられる。ここで発光層
は、以下の三つの機能を併せ持つものである。即ち、 注入機能 電界印加時に、陽極又は正孔注入輸送層より正孔を注
入することができ、陰極又は電子注入輸送層より電子を
注入することができる機能 輸送機能 注入した電荷（電子と正孔）を電界の力で移動させる
機能 発光機能 電子と正孔の再結合の場を提供し、これを発光につな
げる機能 但し、正孔の注入されやすさと電子の注入されやすさ
に違いがあってもよく、また正孔と電子の移動度で表わ
される輸送能に大小があってもよいが、どちらか一方の
電荷を移動することが好ましい。Further, the organic multilayer portion including the light emitting layer is an organic layer necessary for light emission of the EL element, and specifically, a light emitting layer, a light emitting layer / hole injection layer, an electron injection layer / light emitting layer, an electron injection layer / Emitting layer /
One having a configuration such as a hole injection layer is exemplified. Here, the light emitting layer has the following three functions. Injection function When an electric field is applied, holes can be injected from the anode or the hole injection / transport layer, and electrons can be injected from the cathode or the electron injection / transport layer. Transport function Injected charges (electrons and holes) ) The function of moving the) by the force of an electric field. Light-emitting function Provides a field for recombination of electrons and holes, and connects it to light emission. However, there is a difference between the ease of hole injection and the ease of electron injection. Although the transport ability represented by the mobility of holes and electrons may be large or small, it is preferable to transfer either one of the charges.
このような条件を満たす材料であって、所望の発光が
得られるものを適宜使用することができる。その膜厚
は、特に制限はなく適宜状況に応じて選定すればよい
が、通常は5nm〜５μｍ程度とすればよい。また、各種
のフィルター層を素子発光面に面して設けることもでき
る。A material that satisfies such a condition and can obtain desired light emission can be used as appropriate. The film thickness is not particularly limited and may be appropriately selected according to the situation, but is usually about 5 nm to 5 μm. Also, various filter layers can be provided facing the element light emitting surface.
また、多色のEL素子の場合は発光層の発光材料は一種
類には限定されず、発光素子形成部分に各々異なる所望
の発光色を発光する発光材料を使用することができる。
ここで、発光材料としては公知の様々なものを充当でき
るが、例えばペリレン，アントラセン，ナフタレン，フ
ェナンスレン，ピレン，骨格を含む縮合環発光材料，特
開昭59−194393号公報に記載のオキサジアゾール，オキ
サチアゾール系蛍光増白剤，特開昭63−295695号公報記
載の金属キレート化オキサノイド化合物，特願平１−00
9995号明細書にあるクマリン系化合物等の蛍光材料，特
願昭63−313932号明細書，特願平１−029681号明細書，
同１−054957号明細書，同１−068387号明細書，同１−
068388号明細書，同１−067448号明細書，同１−075035
号明細書にあるスチルベン系発光材料、アプライド フ
ィズィクスレターズ第55巻1487頁（1989年）等に記載の
あるスチリルアミン系化合物、テトラフィニルブタジェ
ン，テトラフェニルシクロペンタジエン，テトラフェニ
ルエチレン及びポルフィリン等々である。In the case of a multicolor EL element, the light-emitting material of the light-emitting layer is not limited to one kind, and a light-emitting material that emits a different desired light-emitting color can be used for a light-emitting element formation portion.
Here, as the light emitting material, various known materials can be used. For example, perylene, anthracene, naphthalene, phenanthrene, pyrene, a condensed ring light emitting material having a skeleton, and an oxadiazole described in JP-A-59-194393. Oxathiazole fluorescent brighteners; metal chelated oxanoid compounds described in JP-A-63-295695;
Fluorescent materials such as coumarin compounds described in Japanese Patent Application No. 9995, Japanese Patent Application No. 63-313932, Japanese Patent Application No. 1-029681,
Nos. 1-054957, 1-068387, 1-
068388, 1-067448, 1-075035
No. 55, p. 1487 (1989) and the like, tetrafinyl butadiene, tetraphenylcyclopentadiene, tetraphenylethylene, porphyrin and the like. It is.
また、本発明のEL素子では、発光層を含む有機多層に
正孔注入層や電子注入層は必ずしも必要ではないが、こ
れらの層があると、発光性能が一段と向上する。ここ
で、正孔注入層は、正孔伝達化合物（正孔注入材料）よ
りなり、陽極より注入された正孔を、発光層に伝達する
機能を持つ。この層をEL素子の陽極と発光層間に挟むこ
とにより低電圧でより多くの正孔が発光層に注入され、
素子の輝度は向上する。In the EL device of the present invention, a hole injection layer and an electron injection layer are not necessarily required in the organic multilayer including the light emitting layer, but the presence of these layers further enhances the light emission performance. Here, the hole injection layer is made of a hole transport compound (hole injection material) and has a function of transmitting holes injected from the anode to the light emitting layer. By sandwiching this layer between the anode of the EL element and the light emitting layer, more holes are injected into the light emitting layer at a low voltage,
The brightness of the device is improved.
ここで用いられる正孔注入層の正孔伝達化合物は、電
場を与えられた二個の電極間に配置されて陽極から正孔
が注入された場合、正孔を適切に発光層へ伝達すること
ができる化合物である。正孔注入輸送層を陽極と発光層
との間に挟むことにより、より低い電界で多くの正孔が
発光層に注入される。さらに、陰極や電子注入層から発
光層に注入された電子は、発光層と正孔層の界面に存在
する電子の障壁により、この発光層内の界面付近に蓄積
され発光効率が向上する。ここで好ましい正孔伝達化合
物は、104〜106ボルト/cmの電場を与えられた電極間に
層が配置された場合、少なくとも10-6cm2/ボルト・秒の
正孔移動度をもつ。従って好ましい例としては、光導電
材料において正孔の電荷輸送材として用いられている各
種化合物があげられる。The hole transport compound of the hole injection layer used here is disposed between two electrodes to which an electric field is applied, and when holes are injected from the anode, the holes are appropriately transmitted to the light emitting layer. Is a compound that can be By interposing the hole injection transport layer between the anode and the light emitting layer, many holes are injected into the light emitting layer with a lower electric field. Furthermore, electrons injected into the light emitting layer from the cathode or the electron injection layer are accumulated near the interface in the light emitting layer due to the electron barrier existing at the interface between the light emitting layer and the hole layer, and the light emission efficiency is improved. Preferred hole transport compounds here have a hole mobility of at least 10 -6 cm 2 / volt-second when the layer is placed between electrodes exposed to an electric field of 10 4 to 10 6 volts / cm. . Therefore, preferred examples include various compounds used as a hole charge transporting material in a photoconductive material.
このような電荷輸送材として以下のような例があげら
れる。Examples of such charge transport materials include the following.
米国特許第3112197号明細書等に記載されているトリ
アゾール誘導体、 米国特許第3189447号明細書等に記載されているオキ
サジアゾール誘導体、 特公昭37−16096号公報等に記載されているイミダゾ
ール誘導体、 米国特許第3615402号，同3820989号，同3542544号明
細書や特公昭45−555号，同51−10983号公報さらには特
開昭51−93224号，同55−17105号，同56−4148号，同55
−108667号，同55−156953号，同56−36656号公報等に
記載されているポリアールアルカン誘導体、 米国特許第3180729号，同4278746号明細書や特開昭55
−88064号，同55−88065号，同49−105537号，同55−51
086号，同56−80051号，同56−88141号，同57−45545
号，同54−112637号，同57−7546号公報等に記載されて
いるピラゾリン誘導体およびピラゾロン誘導体、 米国特許第3615404号明細書や特公昭51−10105号，同
46−3712号，同47−25336号公報さらには特開昭54−534
35号，同54−110536号，同54−119925号公報等に記載さ
れているフェニレンジアミン誘導体、 米国特許第3567450号，同3180703号，同3240597号，
同3658520号，同4232103号，同4175961号，同4012376号
明細書や特公昭49−35702号，同39−27577号公報さらに
は特開昭55−144250号，同56−119132号，同56−22437
号公報、西独特許第1110518号明細書等に記載されてい
るアリールアミン誘導体、 米国特許第3526501号明細書等に記載されているアミ
ノ置換カルコン誘導体、 米国特許第3257203号明細書等に記載されているオキ
サゾール誘導体、 特開昭56−46234号公報等に記載されているスチリル
アントラセン誘導体、 特開昭54−110837号公報等に記載されている 特開昭54−110837号公報等に記載されているフルオレ
ノン誘導体、 米国特許第3717462号明細書や特開昭54−59143号，同
55−52063号，同55−52064号，同55−46760号，同55−8
5495号，同57−11350号，同57−148749号公報等に記載
されているヒドラゾン誘導体、 特開昭61−210363号，同61−228451号，同61−14642
号，同61−72255号，同62−47646号，同62−36674号，
同62−10652号，同62−30255号，同60−93445号，同60
−94462号，同60−174749号，同60−175052号公報等に
記載されているスチルベン誘導体などを列挙することが
できる。Triazole derivatives described in U.S. Patent No. 3,112,197, etc., oxadiazole derivatives described in U.S. Patent No. 3,189,447, etc., imidazole derivatives described in JP-B-37-1696, etc. U.S. Patent Nos. 3615402, 3820989, 3542544, JP-B Nos. 45-555, 51-10983, and JP-A-51-93224, 55-17105, 56-4148. , Id 55
Polyalalkane derivatives described in JP-A-108667, JP-A-55-156953, JP-A-56-36656 and the like; U.S. Pat. Nos. 3,180,729 and 4,278,746;
-88064, 55-88065, 49-105537, 55-51
Nos. 086, 56-80051, 56-88141, 57-45545
Pyrazoline derivatives and pyrazolone derivatives described in U.S. Pat. Nos. 6,115,105, 54-112637 and 57-7546, and U.S. Pat.
46-3712, 47-25336 and JP-A-54-534.
Phenylenediamine derivatives described in JP-A Nos. 35, 54-110536 and 54-119925; U.S. Pat. Nos. 3,567,450, 3,180,703, 3,240,597;
Nos. 3,658,520, 4,322,103, 4,117,961 and 4,012,376, and JP-B-49-35702, JP-A-39-27577, and JP-A-55-144250, JP-A-56-119132, and JP-A-56-119. 22437
JP-A No. 1110518, an arylamine derivative described in U.S. Pat.No. 3,235,501, an amino-substituted chalcone derivative described in U.S. Pat. Oxazole derivatives, styryl anthracene derivatives described in JP-A-56-46234, etc., and JP-A 54-110837 described in JP-A-54-110837, etc. Fluorenone derivatives, described in U.S. Pat. No. 3,717,462 and JP-A-54-59143,
55-52063, 55-52064, 55-46760, 55-8
Hydrazone derivatives described in JP-A-5495, JP-A-57-11350, JP-A-57-148749, etc., and JP-A-61-210363, JP-A-61-228451, JP-A-61-14642.
Nos. 61-72255, 62-47646, 62-36674,
No. 62-10652, No. 62-30255, No. 60-93445, No. 60
Stilbene derivatives and the like described in JP-A-94462, JP-A-60-174749, JP-A-60-175052 and the like can be listed.
さらに特に好ましい例としては、特開昭63−295695号
公報に開示されているホール輸送層としての化合物（芳
香族三級アミン）や正孔注入帯としての化合物（ポリフ
ィリン化合物）をあげることができる。More particularly preferred examples include a compound (aromatic tertiary amine) as a hole transport layer and a compound (porphyrin compound) as a hole injection zone disclosed in JP-A-63-295695. .
さらに特に正孔伝達化合物として好ましい例は、特開
昭53−27033号公報，同54−58445号公報，同54−149634
号公報，同54−64299号公報，同55−79450号公報，同55
−144250号公報，同56−119132号公報，同61−295558号
公報，同61−98353号公報及び米国特許第4127412号明細
書等に開示されているものがある。それらの例を示せば
次の如くである。Further preferred examples of the hole transport compound are described in JP-A-53-27033, JP-A-54-58445, and JP-A-54-149634.
JP-A-54-64299, JP-A-55-79450, and 55
Japanese Patent Nos. 144244, 56-119132, 61-295558, 61-98353, and U.S. Pat. No. 4,127,412. Examples of these are as follows.
これらの正孔伝達化合物から正孔注入層を形成する
が、この正孔注入層は一層からなってもよく、あるいは
上記一層と別種の化合物を用いた正孔注入層を積層して
もよい。 The hole injecting layer is formed from these hole transporting compounds. The hole injecting layer may be composed of one layer, or a hole injecting layer using a compound different from the above one layer may be laminated.
一方、電子注入層は電子を伝達する化合物よりなる。
電子注入層を形成する電子伝達化合物（電子注入材料）
の好ましい例としては、 などのニトロ置換フルオレノン誘導体、 特開昭57−149259号，同58−55450号，同63−104061
号公報等に記載されているアントラキノジメタン誘導
体、 Polymer Prerpints,Japan Vol.37,No.3（1988）,p.68
1等に記載されている などのジフェニルキノン誘導体、 などのチオピランジオキシド誘導体、 J.J.APPl.Phys.,27,L 269（1988）等に記載されてい
る で表わされる化合物、 特開昭60−69657号，同61−143764号，同61−148159
号公報等に記載されているフレオレニリデンメタン誘導
体、 特開昭61−225151号，同61−233750号公報等に記載さ
れているアントラキノジメタン誘導体及びアントロン誘
導体、 アプライド フィズィクスレターズ第55巻1489頁（19
89年）で開示されている 一般式 で表わされる化合物及び類似のオキサジアゾール誘導体
などをあげることができる。On the other hand, the electron injection layer is made of a compound that transmits electrons.
Electron transfer compound that forms the electron injection layer (electron injection material)
As a preferred example of Nitro-substituted fluorenone derivatives such as JP-A-57-149259, JP-A-58-55450 and JP-A-63-104061.
No. 3, anthraquinodimethane derivatives, Polymer Prerpints, Japan Vol. 37, No. 3 (1988), p. 68
Listed in 1 etc. Diphenylquinone derivatives such as, Thiopyran dioxide derivatives such as those described in JJAPPl. Phys., 27, L269 (1988). Compounds represented by the following formulas: JP-A-60-69657, JP-A-61-143764, JP-A-61-148159
No. 55, and anthraquinodimethane derivatives and anthrone derivatives described in JP-A-61-225151 and JP-A-61-233750. Applied Physics Letters Vol. 55 1489 (19
(1989) And similar oxadiazole derivatives.
本発明のEL素子の発光層を含む有機多層部は上述の如
き層からなるものであり、その機能から正孔注入層は陽
極と発光層の間に、電子注入層は陰極と発光層の間に設
けるものである。The organic multilayer portion including the light-emitting layer of the EL device of the present invention is composed of the above-mentioned layers, and the hole injection layer is between the anode and the light-emitting layer, and the electron injection layer is between the cathode and the light-emitting layer. It is provided in.
以上の構成よりなる本発明のEL素子は直流を加える場
合、陽極を＋，陰極を−の極性として、電圧３〜40Vを
印加すれば絶縁膜が形成されていない部分のみが精度良
く発光する。逆の極性で電圧を印加しても電流は流れず
発光しない。また、交流や任意のパルス電圧を印加する
こともでき、この場合陽極に＋，陰極に−のバイアスの
状態のときのみ発光する。When a direct current is applied to the EL device of the present invention having the above-described configuration, if a voltage of 3 to 40 V is applied with the anode having a positive polarity and the cathode having a negative polarity, only the portion where the insulating film is not formed emits light with high accuracy. Even if a voltage is applied with the opposite polarity, no current flows and no light is emitted. Alternatively, an AC or an arbitrary pulse voltage can be applied. In this case, light is emitted only when the anode has a positive bias and the cathode has a negative bias.
本発明におけるEL素子は、次の如き方法にて効率良く
製造される。The EL device of the present invention is efficiently manufactured by the following method.
まず、基板上に下部電極を通常行われている方法によ
り形成し、その上に上記の如き層間絶縁膜を形成する。
下部電極はスパッタリング法，蒸着法，スクリーン印刷
法などで行われ、また、下部電極をパターンニングして
おいてもよい。絶縁膜形成はその材料等により種々の方
法を選択できるが、蒸着法，スパッタリング法，スピン
コート法などが挙げれる。この場合、膜形成時に発光素
子を形成する部分すなわち開口部を有するパターンの膜
を形成してもよいが、膜形成後にエッチングなどの方法
により開口部を形成する方法がパターン精度が向上し好
ましい。First, a lower electrode is formed on a substrate by an ordinary method, and an interlayer insulating film as described above is formed thereon.
The lower electrode is formed by a sputtering method, a vapor deposition method, a screen printing method, or the like, and the lower electrode may be patterned. Various methods can be selected for the formation of the insulating film depending on the material and the like, and examples thereof include a vapor deposition method, a sputtering method, and a spin coating method. In this case, a film having a pattern in which a light emitting element is formed, that is, a pattern having an opening may be formed at the time of film formation.
次いで、本発明の方法では、上記の如き下部電極上に
パターン加工をした層間絶縁膜を形成したものにさらに
発光層を含む有機多層部を形成する。ここで発光層を含
む有機多層部は、蒸着法により通常形成されるが、下部
電極の取り出し位置を確保するため蒸着マスクなどのマ
スクを用い、下部電極上にかけて蒸着を行う。したがっ
て、上記開口部の上に有機多層部が形成される。有機多
層部中に正孔注入層，電子注入層を形成する場合、下部
電極が陽極の場合には正孔注入層／発光層，正孔注入層
／発光層／電子注入層の構成とし、下部電極が陰極の場
合には電子注入層／発光層，電子注入層／発光層／正孔
注入層の構成とすべきである。なお、蒸着にあたっての
条件は、使用する発光層の有機化合物の種類，膜厚等に
より異なるが、一般にボート加熱温度50〜400℃、真空
度10-5〜10-3Pa,蒸着速度0.01〜50nm/秒、基板温度−50
〜300℃、膜厚5nmないし５μｍの範囲で適宜選択するこ
とが好ましい。Next, in the method of the present invention, an organic multilayer portion including a light-emitting layer is further formed on the patterned interlayer insulating film formed on the lower electrode as described above. Here, the organic multilayer portion including the light emitting layer is usually formed by a vapor deposition method, but vapor deposition is performed over the lower electrode using a mask such as a vapor deposition mask in order to secure a position for taking out the lower electrode. Therefore, an organic multilayer part is formed on the opening. When a hole injection layer and an electron injection layer are formed in the organic multilayer portion, when the lower electrode is an anode, the structure is a hole injection layer / light-emitting layer, and a hole injection layer / light-emitting layer / electron injection layer. When the electrode is a cathode, the structure should be electron injection layer / light emitting layer, or electron injection layer / light emitting layer / hole injection layer. The conditions for vapor deposition vary depending on the type and thickness of the organic compound of the light emitting layer to be used, but generally the boat heating temperature is 50 to 400 ° C., the degree of vacuum is 10 −5 to 10 −3 Pa, and the vapor deposition rate is 0.01 to 50 nm. / Sec, substrate temperature -50
It is preferable to appropriately select a temperature within a range of from about 300 ° C. and a thickness of 5 nm to 5 μm.
次いで、本発明においてこの発光層を含む有機多層部
を形成した上に対向電極を形成し、EL素子が得られる。
通常対向電極の形成は蒸着法で行われ、発光層含む有機
多層部を形成した際の真空度で、また同様の蒸着マスク
を使用して行うことができる。従来法においては、発光
材料層の形成に使用される蒸着マスクと対向電極の形成
に使用される蒸着マスクは異なるため、この工程でマス
クの交換が必要で作成面の汚染が問題であったが、本発
明の方法ではこのような問題がなく、良質の素子を製造
することができる。Next, in the present invention, a counter electrode is formed on the organic multilayer portion including the light emitting layer, and an EL element is obtained.
Usually, the formation of the counter electrode is performed by a vapor deposition method, and can be performed at a degree of vacuum at the time of forming the organic multilayer portion including the light emitting layer, and using a similar vapor deposition mask. In the conventional method, the vapor deposition mask used for forming the light emitting material layer and the vapor deposition mask used for forming the counter electrode are different. According to the method of the present invention, there is no such problem, and a high-quality device can be manufactured.
次に、本発明のEL素子の製造方法を第１図に従って説
明する。第１図（ａ）は基板１の上に下部電極２を蒸着
により形成し、さらにその上に発光素子形成部分が開口
部９となるようパターンニングした層間絶縁膜３を形成
したものの断面図である。このように形成されたもの
に、下部電極取り出し位置（第１図（ｂ）の11）を確保
するため、蒸着マスク６を開口部分及びその周辺を除い
た下部電極上にかけて、発光層を含む有機多層部４を蒸
着により形成する。このとき第１図ではマスク６と絶縁
膜３が離れているが、これは理解を助けるための便宜的
なものであり、実際には密着させる方がより好ましい。
得られたものの断面図を第１図（ｂ）に示す。続いて、
同一の蒸着マスク６を設置したまま発光層を含む有機多
層部４の上に対向電極５を蒸着することにより、本発明
のEL素子が製造される。このEL素子の断面図を第１図
（ｃ）に示す。本発明のEL素子は、第１図（ａ）におけ
る開口部９に、第１図（ｃ）における発光素子部分10が
パターン精度が良く形成される。Next, a method for manufacturing an EL device of the present invention will be described with reference to FIG. FIG. 1 (a) is a cross-sectional view of a structure in which a lower electrode 2 is formed on a substrate 1 by vapor deposition, and an interlayer insulating film 3 patterned thereon such that a light emitting element forming portion becomes an opening 9 is formed thereon. is there. In order to secure a lower electrode take-out position (11 in FIG. 1 (b)), a deposition mask 6 is applied over the lower electrode excluding the opening and its periphery to form an organic layer including a light emitting layer. The multilayer part 4 is formed by vapor deposition. At this time, the mask 6 and the insulating film 3 are separated from each other in FIG. 1, but this is for the sake of convenience for understanding, and actually, it is more preferable to make close contact.
FIG. 1 (b) shows a cross-sectional view of the obtained one. continue,
The EL element of the present invention is manufactured by depositing the counter electrode 5 on the organic multilayer portion 4 including the light emitting layer while the same deposition mask 6 is provided. FIG. 1C shows a cross-sectional view of the EL device. In the EL device of the present invention, the light emitting element portion 10 in FIG. 1C is formed with high pattern accuracy in the opening 9 in FIG.
なお、多色EL素子を製造する場合は、層間絶縁膜にお
いて形成される各開口部に、所望する発光色を発光可能
な材料を使用した発光層を各々形成すればよい。具体的
には、第２図に従って説明する。まず、基板１の上に下
部電極２を蒸着により形成する。ここで、多色EL素子形
成のため下部電極２は電気的に独立して形成する。この
上に発光素子形成部を開口部としたパターンニングした
層間絶縁膜３を、蒸着により開口部9a及び開口部9bを形
成する。このようにして形成されたものの断面図を第２
図（ａ）に示す。次いで、蒸着マスク７を開口部9a及び
その周辺を除いた部分にかけて発光層を含む有機多層部
４を蒸着にて形成し、さらに続いて対向電極５を蒸着に
て形成する。このようにして形成されたものの断面図を
第２図（ｂ）に示す。さらに、蒸着マスク８を開口部9b
を除いた部分にかけて発光層を含む有機多層部４と異な
る発光材料を用いた発光層を含む有機多層部４′を蒸着
にて形成し、さらに続いて対向電極５′を蒸着にて形成
する。このようにして形成されたものの断面図を第２図
（ｃ）に示す。このようにして得られたEL素子は開口部
9a及び開口部9bに各々異なる発光材料を使用した発光層
が形成されているため、異なる発光色を発光できる素子
となる。なお、同様の方法でさらに三色以上の発光色の
発光が得られるEL素子を製造することができる。In the case of manufacturing a multicolor EL element, a light emitting layer using a material capable of emitting a desired light emission color may be formed in each opening formed in the interlayer insulating film. Specifically, description will be given with reference to FIG. First, a lower electrode 2 is formed on a substrate 1 by vapor deposition. Here, the lower electrode 2 is formed electrically independently for forming a multicolor EL element. An opening 9a and an opening 9b are formed on the interlayer insulating film 3 patterned by using the light emitting element forming portion as an opening by vapor deposition. The cross-sectional view of the thus formed one is shown in FIG.
It is shown in FIG. Next, the organic multilayer portion 4 including the light emitting layer is formed by vapor deposition using the vapor deposition mask 7 over the portion excluding the opening 9a and its periphery, and subsequently, the counter electrode 5 is formed by vapor deposition. FIG. 2 (b) is a cross-sectional view of the thus formed one. Further, the deposition mask 8 is placed in the opening 9b.
Then, the organic multilayer portion 4 'including the light emitting layer and the organic multilayer portion 4' using the light emitting material different from the organic multilayer portion 4 including the light emitting layer are formed by vapor deposition, and subsequently, the counter electrode 5 'is formed by vapor deposition. FIG. 2 (c) shows a cross-sectional view of the thus formed one. The EL element thus obtained has an opening
Since the light-emitting layers using different light-emitting materials are formed in the opening 9a and the opening 9b, the element can emit different emission colors. Note that an EL element capable of further emitting light of three or more colors can be manufactured by the same method.
このような方法により前述の如き高性能のEL素子が製
造できる。但しこの場合、マスク交換が必要であるがマ
スクの枚数は従来方法よりも少なくすることができる。By such a method, a high-performance EL device as described above can be manufactured. In this case, it is necessary to replace the mask, but the number of masks can be made smaller than in the conventional method.
次に本発明を実施例よりさらに詳しく説明する。 Next, the present invention will be described in more detail with reference to examples.
実施例１ （１）層間絶縁膜の形成 75mm×25mm×1mmのガラス基板上にITOを蒸着法にて10
00Åの厚さで製膜したものを下部電極を有する基板とし
た（HOYA（株）製）。この下部電極上に感光性ポリイミ
ドコーテイング剤（TORAY社製,UR3140）をスピンコート
にて、スピンナー回転数4000rpmで30秒間かけて塗布し
た。次いで、オーブンにて80℃,60分間の乾燥（プリベ
ーク）を行い、発光パターンのフォトマスクを通して超
高圧水銀灯（10mW/cm2）にて８秒間、フォトマスクとプ
リベークしたポリイミドコーテイング面を密着させてコ
ンタクト露光を行った。この後現像液（TORAY社製,DV−
140）にて35〜40秒間浸け、さらにイソプロパノール液
に浸けてから15秒間超音波処理を行った。露光された部
分のポリイミドコーテイング剤は基板よりとれて、層間
絶縁膜であるポリイミドのパターニングが得られた。Example 1 (1) Formation of interlayer insulating film ITO was deposited on a 75 mm × 25 mm × 1 mm glass substrate by vapor deposition.
A substrate having a thickness of 00 mm was used as a substrate having a lower electrode (HOYA Corporation). On this lower electrode, a photosensitive polyimide coating agent (UR3140, manufactured by TORAY) was applied by spin coating at a spinner rotation speed of 4000 rpm for 30 seconds. Next, drying (prebaking) is performed in an oven at 80 ° C. for 60 minutes, and the photomask and the prebaked polyimide-coated surface are brought into close contact with each other with an ultrahigh-pressure mercury lamp (10 mW / cm 2 ) for 8 seconds through a photomask having a light emitting pattern. Contact exposure was performed. Thereafter, the developer (TORAY, DV-
After immersion in 140) for 35 to 40 seconds, and further immersion in an isopropanol solution, ultrasonic treatment was performed for 15 seconds. The exposed portion of the polyimide coating agent was removed from the substrate, and a pattern of the polyimide as an interlayer insulating film was obtained.
続いて、窒素ガス雰囲気下のオーブン中で180℃にて3
0分、さらに300℃にて30分キュアして、ガラス基板/ITO
/層間絶縁膜を形成した。層間絶縁膜の膜厚を触針膜厚
計にて測定したところ、1.2μｍであった。Subsequently, in an oven under a nitrogen gas atmosphere at 180 ° C.
Cure for 30 minutes at 300 ° C for 0 minutes, then glass substrate / ITO
/ An interlayer insulating film was formed. When the film thickness of the interlayer insulating film was measured with a stylus film thickness meter, it was 1.2 μm.
（２）有機EL素子の製造 上記（１）で得られたガラス基板/ITO/層間絶縁膜
を、イソプロパノールにて10分間超音波洗浄を行い、そ
の後窒素ガスにて吹きつけ乾燥を行った。さらにUVオゾ
ン洗浄装置（サムコインターナショナル社製,UV−300）
にて、120秒間クリーニングを行った。さらにこれを真
空蒸着装置（日本真空技術社製）の基板ホルダーに装着
した。このときの基板ホルダーは第１図（ｂ）の６のマ
スクの役割もする。真空蒸着装置の抵抗加熱ボートＡに
TPD（下記に構造式を示す）を入れ、さらに別の抵抗加
熱ボートＢにDTVX（下記に構造式を示す）を入れた。ま
ず、ボートＡに通電し、これを加熱しTPD層を600Å蒸着
して正孔注入層を形成した。次にボートＢに通電し、DT
VXを600Å蒸着して発光層を形成した。さらに、予め用
意したマグネシウムを入れておいた抵抗加熱ボートＣと
インジウムを入れておいた抵抗加熱ボートＤに通電し
て、マグネシウム−インジウムの混合物電極を形成し
た。この際の蒸着レート比は9:1であった。(2) Production of Organic EL Element The glass substrate / ITO / interlayer insulating film obtained in the above (1) was subjected to ultrasonic cleaning with isopropanol for 10 minutes, and then dried by spraying with nitrogen gas. In addition, UV ozone cleaning equipment (Samco International, UV-300)
Cleaning was performed for 120 seconds. Further, this was mounted on a substrate holder of a vacuum evaporation apparatus (manufactured by Nippon Vacuum Engineering Co., Ltd.). At this time, the substrate holder also functions as the mask 6 in FIG. 1 (b). For resistance heating boat A of vacuum evaporation equipment
TPD (shown by the following structural formula) was put therein, and DTVX (shown below by a structural formula) was put into another resistance heating boat B. First, a current was applied to the boat A, which was heated, and a TPD layer was deposited by 600 ° to form a hole injection layer. Next, energize boat B, DT
VX was deposited at 600 ° to form a light emitting layer. Further, electricity was supplied to the resistance heating boat C containing magnesium and the resistance heating boat D containing indium, thereby forming a magnesium-indium mixture electrode. The deposition rate ratio at this time was 9: 1.
このようにして、ガラス基板/ITO/層間絶縁膜／正孔
注入層／発光層／マグネシウム−インジウムの混合物電
極からなる有機EL素子を得た。In this way, an organic EL device comprising a glass substrate / ITO / interlayer insulating film / hole injection layer / light emitting layer / mixture electrode of magnesium-indium was obtained.
得られた有機EL素子にマグネシウム−インジウムの混
合物電極を陰極、ITOを陽極として直流5Vを印加し、発
光させた。このときの発光パターンはフォトマスクと同
一のパターンであった。パターン精度を調べるため、光
学顕微鏡上で素子の発光のオン，オフを行ったところ、
層間絶縁膜のある部分は発光しないことが確認され、層
間絶縁膜の機能が確認されるとともにパターン精度が10
μｍと良好であることが判明した。また、このパターン
に従う発光面は端部，面中央部の区別なく均一であっ
た。以上の実施例は、有機多層部に使用する材料及び電
極材料の種類によらず、良好なパターン精度，発光面の
均一製を保証する。A 5 V DC was applied to the obtained organic EL device using a magnesium-indium mixture electrode as a cathode and ITO as an anode to emit light. The light emission pattern at this time was the same pattern as the photomask. The light emission of the device was turned on and off on an optical microscope to check the pattern accuracy.
It was confirmed that there was no light emission in a part of the interlayer insulating film, and the function of the interlayer insulating film was confirmed and the pattern accuracy was 10
It was found to be as good as μm. The light emitting surface according to this pattern was uniform without distinction between the end and the center of the surface. The above embodiment guarantees good pattern accuracy and uniform production of the light emitting surface irrespective of the type of the material and the electrode material used for the organic multilayer portion.
比較例１ 実施例１において、ガラス基板/ITOに層間絶縁膜を形
成することなく、下部電極取り出し口を確保するためマ
スクをかけTPD層,DTVX層を同様にして蒸着，積層した。
さらにここで真空槽をあけ、パターンニングされた別の
蒸着用マスクをガラス基板/ITO/TPD層/DTVX層の上に設
置し、これを基板ホルダーに取りつけた。次いで、実施
例１と同様にしてマグネシウム−インジウムの混合物電
極を形成した。このようにしてガラス基板/ITO/正孔注
入層／発光層／マグネシウム−インジウムの混合物電極
からなる有機EL素子を得た。 Comparative Example 1 In Example 1, without forming an interlayer insulating film on the glass substrate / ITO, a TPD layer and a DTVX layer were deposited and laminated in the same manner by using a mask to secure a lower electrode outlet.
Then, the vacuum chamber was opened, another patterned mask for vapor deposition was set on the glass substrate / ITO / TPD layer / DTVX layer, and this was attached to the substrate holder. Subsequently, a magnesium-indium mixture electrode was formed in the same manner as in Example 1. In this way, an organic EL device comprising a glass substrate / ITO / hole injection layer / light-emitting layer / magnesium-indium mixture electrode was obtained.
得られた有機EL素子を実施例１（２）と同様に方法に
て、パターン精度を測定したところ、最高50μｍ、場所
により100〜200μｍ程度であった。また、発光面端部が
著しく発光面中央部と強度が異なる箇所が存在し、不均
一であった。When the pattern accuracy of the obtained organic EL device was measured by the same method as in Example 1 (2), it was 50 μm at the maximum and about 100 to 200 μm depending on the place. In addition, there were places where the edge of the light-emitting surface was significantly different from the center of the light-emitting surface, which was uneven.
実施例２ （１）SiO2膜による層間絶縁膜の形成 スパッタリング法により前述のITO付ガラス基板上にS
iO2を5000Å膜付けした。このときの基板温度は200℃で
あった。さらにマスクを前述の基板/ITO/SiO2にかけ、
サムコインターナショナル社製リアクティブイオンエッ
チング装置RIE−10Nにて、CHF3をエッチングガスとして
毎分1000Å/minの速度でエッチングした。このときのガ
ス容量は15SCCM,圧力0.04Torr,高周波出力300Wであっ
た。上述のマスクの開口部のSiO2は、エッチングされ、
ITO面が露出した。以上によりSiO2層のパターン加工が
完了した。Example 2 (1) Formation of interlayer insulating film by SiO 2 film The above-mentioned glass substrate with ITO was sputtered by sputtering method.
5,000 Å of iO 2 was applied. At this time, the substrate temperature was 200 ° C. Further by masking the substrate / ITO / SiO 2 described above,
Using a reactive ion etching apparatus RIE-10N manufactured by Samco International Co., etching was performed at a rate of 1000 ° / min / min using CHF 3 as an etching gas. The gas capacity at this time was 15 SCCM, the pressure was 0.04 Torr, and the high frequency output was 300 W. The SiO 2 in the opening of the mask described above is etched,
The ITO surface was exposed. Thus, the patterning of the SiO 2 layer was completed.
（２）EL素子の作製 実施例１（２）と同様に有機EL素子を作製し同様な試
験を行ったところ、パターン精度は20μｍと良好である
ことが判明した。また、やはり発光面は均一であり良好
であった。(2) Production of EL Element An organic EL element was produced in the same manner as in Example 1 (2), and a similar test was conducted. As a result, it was found that the pattern accuracy was as good as 20 μm. Also, the light emitting surface was uniform and good.
以上の如く、本発明のEL素子は、パターン加工された
層間絶縁膜を設けたことにより、パターン精度が極めて
良好なものとなり、さらに従来法にて問題となった蒸着
だれは生じないので発光面の均一性が高い。また、本発
明の方法で、EL素子を製造する場合、従来必要であった
発光層の蒸着マスクと対向電極の蒸着マスクの交換を必
要とせず、この際に問題となった形成面の汚染がなく良
品質の素子が製造できる。As described above, the EL element of the present invention has an extremely good pattern accuracy by providing a patterned interlayer insulating film, and furthermore, the evaporation surface which is a problem in the conventional method does not occur, so that the light emitting surface High uniformity. In addition, in the case of manufacturing an EL element by the method of the present invention, it is not necessary to replace the evaporation mask of the light emitting layer and the evaporation mask of the counter electrode, which was conventionally required, and contamination of the formation surface which has become a problem at this time is eliminated. And a high quality device can be manufactured.
従って、本発明のEL素子は、各種表示装置の発光素
子，デスプレイ素子等に幅広く利用することができる。Therefore, the EL element of the present invention can be widely used as a light emitting element, a display element and the like of various display devices.
第１図（ａ），（ｂ），（ｃ）は、本発明の単色のEL素
子の製造過程の各段階における断面図を示し、第２図
（ａ），（ｂ），（ｃ）は、本発明の二色のEL素子の製
造過程の各段階における断面図を示す。 １……基板,2……下部電極,3……層間絶縁膜,4及び４′
……発光層を含む有機多層部， ５及び５′……対向電極,6,7,8……蒸着マスク,9,9a,9b
……開口部， 10……発光素子部分,11……下部電極取り出し位置1 (a), 1 (b) and 1 (c) are cross-sectional views at each stage of the process of manufacturing a monochromatic EL device of the present invention, and FIGS. 2 (a), 2 (b) and 2 (c) are cross-sectional views. 1 is a cross-sectional view at each stage of a manufacturing process of a two-color EL element of the present invention. DESCRIPTION OF SYMBOLS 1 ... Substrate, 2 ... Lower electrode, 3 ... Interlayer insulating film, 4 and 4 '
...... Organic multilayer part including light emitting layer, 5 and 5 '... Counter electrode, 6, 7, 8 ... Vapor deposition mask, 9, 9a, 9b
...... Opening, 10 ... Light emitting element, 11 ... Bottom electrode extraction position
Claims (6)
有機多層部及び対向電極からなる素子を発光素子部分と
して含むエレクトロルミネッセンス素子において、下部
電極と対向電極との間に、パターン加工された層間絶縁
膜を存在させた非発光素子部分を保有し、且つ該層間絶
縁膜の開口部には発光層を含む有機多層部と対向電極が
設けられているとともに、実質的に正孔または電子の注
入ができるように有機多層部と対向電極が接合され配置
されていることを特徴とするエレクトロルミネッセンス
素子。1. An electroluminescent device comprising, as a light emitting element portion, an element comprising a lower electrode, an organic multilayer portion including a light emitting layer, and a counter electrode provided on a substrate, wherein a pattern is formed between the lower electrode and the counter electrode. A non-light-emitting element portion in which an interlayer insulating film is present, and an opening in the interlayer insulating film is provided with an organic multilayer portion including a light-emitting layer and a counter electrode, and substantially has holes or electrons. An organic electroluminescent device characterized in that an organic multilayer portion and a counter electrode are joined and arranged so as to be capable of injecting hydrogen.
けられた下部電極、発光層を含む有機多層部と対向電極
からなる発光素子部分の構成が、各々電気的に独立した
構成からなる請求項１記載のエレクトロルミネッセンス
素子。2. A light-emitting element comprising a plurality of openings in an interlayer insulating film, a lower electrode provided on a substrate, an organic multilayer portion including a light-emitting layer, and a counter electrode, each of which has an electrically independent structure. The electroluminescent device according to claim 1.
をパターン加工にて膜付けした後、形成された層間絶縁
膜の開口部に発光層を含む有機多層部および対向電極を
形成する工程を行うことを特徴とするエレクトロルミネ
ッセンス素子の製造方法。3. An interlayer insulating film is formed on a lower electrode provided on a substrate by patterning, and an organic multilayer portion including a light emitting layer and a counter electrode are formed in openings of the formed interlayer insulating film. A method for manufacturing an electroluminescent element, comprising performing a step.
形成する請求項３の製造方法。4. The method according to claim 3, wherein the organic multilayer portion including the light emitting layer is formed by a vapor deposition method.
グ法により形成する請求項３の製造方法。5. The method according to claim 3, wherein the counter electrode is formed by a vapor deposition method or a sputtering method.
によるパターン加工の際、反応性イオンエッチング方法
を用いることを特徴とする請求項３の製造方法。6. The method according to claim 3, wherein a reactive ion etching method is used during patterning of the SiO 2 layer as an interlayer insulating film by etching.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP2045717A JP2734464B2 (en) | 1990-02-28 | 1990-02-28 | Electroluminescence device and method of manufacturing the same |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP2045717A JP2734464B2 (en) | 1990-02-28 | 1990-02-28 | Electroluminescence device and method of manufacturing the same |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPH03250583A JPH03250583A (en) | 1991-11-08 |
| JP2734464B2 true JP2734464B2 (en) | 1998-03-30 |
Family
ID=12727104
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP2045717A Expired - Lifetime JP2734464B2 (en) | 1990-02-28 | 1990-02-28 | Electroluminescence device and method of manufacturing the same |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JP2734464B2 (en) |
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| Publication number | Publication date |
|---|---|
| JPH03250583A (en) | 1991-11-08 |
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