JPH07192866A - Organic thin film type electroluminescent element - Google Patents

Organic thin film type electroluminescent element

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Publication number
JPH07192866A
JPH07192866A JP34821993A JP34821993A JPH07192866A JP H07192866 A JPH07192866 A JP H07192866A JP 34821993 A JP34821993 A JP 34821993A JP 34821993 A JP34821993 A JP 34821993A JP H07192866 A JPH07192866 A JP H07192866A
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Japan
Prior art keywords
layer
light emitting
thickness
organic compound
electroluminescent element
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JP34821993A
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Japanese (ja)
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JPH07192866K1 (en
Inventor
Chihaya Adachi
Kazukiyo Nagai
Hirota Sakon
Nozomi Tamoto
千波矢 安達
洋太 左近
一清 永井
望 田元
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Ricoh Co Ltd
株式会社リコー
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Priority to JP34821993A priority Critical patent/JPH07192866A/en
Publication of JPH07192866A publication Critical patent/JPH07192866A/en
Publication of JPH07192866K1 publication Critical patent/JPH07192866K1/ja
Application status is Pending legal-status Critical

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Abstract

PURPOSE: To prevent the intrusion of moisture, and to provide an electroluminescent element, in which the generation of dark spot is reduced and which has the excellent durability, by containing at least one kind of each organic compound layer structural component and inorganic oxide in a sealing protecting layer of a laminated product.
CONSTITUTION: A stripe positive electrode pattern 2 at 2mm of width made of ITO is formed on a glass substrate 1, and a hole transporting layer 3 at 500Å of thickness and a light emitting layer 4 at 500Å of thickness are laminated by the deposition. Next, a negative electrode 5a at 3000Å of film thickness is deposited with a pattern, which crosses the positive electrode 2. Finally, as a sealing protecting layer 6, the organic compound used for the light emitting layer 4 and GeO as the inorganic oxide are deposited together at 1:6 of ratio and laminated at 3500Å of thickness to form an electroluminescent element. In this element, the reduction of the light emitting area due to the generation of dark spot is not recognized after passing one month from the manufacture, and the durability is improved.
COPYRIGHT: (C)1995,JPO

Description

【発明の詳細な説明】 DETAILED DESCRIPTION OF THE INVENTION

【0001】 [0001]

【産業上の利用分野】本発明は電界の印加によって発光する、有機薄膜型電界発光素子に関する。 The present invention relates to light by application of an electric field, an organic thin film electroluminescent device.

【0002】 [0002]

【従来の技術】電気信号に応答して多色表示するカラー表示装置として、近年、完全固体型として高輝度の発光が得られる有機薄膜型電界発光素子が開発され、各種の表示装置における発光素子として注目されている。 As a color display device for multicolor display in response to the Prior Art Electrical signals, in recent years, full as solid-state light emission with high luminance it has been developed an organic thin film electroluminescent device obtained, luminescence of various display devices element It has been attracting attention as. この有機薄膜型電界発光素子は、有機物質を原料としているため、それを構成する材料も多種の材料から選択しうること、完全固体型であるため耐衝撃性に優れていること、低電圧の印加で発光しうること、高輝度高効率の発光が得られること、更に、多色表示が可能である等、優れた特性を有しており、それを構成する材料、構造等の研究が盛んに行なわれている。 The organic thin-film electroluminescent device, since the organic material as a raw material, the material also can be selected from a variety of materials, to be excellent in impact resistance because it is a complete solid type, a low voltage constituting the it can emit light by application, the emission of high luminance and high efficiency is obtained, further, etc. are possible multicolor display, has excellent characteristics, a material constituting it, flourishing study of structure, etc. It has been made to.

【0003】有機薄膜型電界発光素子としては、その構造として、陰極/発光層/正孔輸送層/陽極、陰極/電子輸送層/発光層/陽極、陰極/電子輸送層/発光層/ [0003] The organic thin-film electroluminescent device, as its structure, a cathode / light-emitting layer / hole transport layer / anode, cathode / electron transport layer / emitting layer / anode, cathode / electron transport layer / light emitting layer /
正孔輸送層/陽極、等の構成のものが開発されている。 Hole transport layer / anode, having a structure equal have been developed.
具体的には、例えば、透明基板上に、複数の透明陽極、 Specifically, for example, on a transparent substrate, a plurality of transparent anode,
必要により正孔輸送層、発光層、必要により電子輸送層、前記透明電極に交差する複数の背面陰極を、順に積層したものである。 A hole transport layer, if necessary, the light-emitting layer, an electron transporting layer as necessary, a plurality of rear cathode intersecting the transparent electrode, is laminated in this order.

【0004】正孔輸送層は、陽極からの正孔を注入させ易くする機能と、電子をブロックする機能とを有し、一方電子輸送層は陰極からの電子を注入させ易くする機能を有している。 [0004] The hole transport layer has a function of facilitating to inject holes from the anode and a function of blocking electrons, whereas the electron transporting layer has a function to easier to inject electrons from the cathode ing. 発光層において、一対の電極から注入された電子と正孔との再結合によって励起子が生じ、この励起子が放射失活する過程で光を放ち、この光が透明電極及び透明基板を介して外部に放出され、表示が可能となる。 In the light-emitting layer, excitons generated by recombination of electrons and holes injected from a pair of electrodes, emits light in the course of this exciton radiative deactivation, the light through the transparent electrode and the transparent substrate is released to the outside, it is possible to display.

【0005】このような有機薄膜型電界発光素子において、素子の高精細化のために電極パターンを微細化することが望まれており、電極間に層間絶縁膜を形成し、発光の均一性を保持し、パターン精度を向上させたものが提案されている(特開平3−250583号)。 [0005] In such an organic thin film electroluminescent elements, and it is desired to miniaturize the electrode pattern for the high definition of elements, an interlayer insulating film between the electrodes, the uniformity of light emission held, it has been proposed with improved pattern accuracy (JP 3-250583). また有機化合物層と電極間に絶縁層を形成し、パターン精度及び表示品質を向上させたものも提案されている(特開平3−274694号)。 The formation of the insulating layer between the organic compound layer and the electrode, has also been proposed that improves pattern accuracy and display quality (JP-A-3-274694). 更にまた、電極の縁部に絶縁層を形成し、クロストークや発光のにじみを減少させたものも提案されている(特開平4−51494号)。 Furthermore, an insulating layer on the edge portion of the electrode, crosstalk and light emitting be proposals (Japanese Patent Laid-Open No. 4-51494) that reduces bleeding.

【0006】更に、これらの有機薄膜型電界発光素子は外界からの水分の侵入等によって、耐久性低下の原因となるダークスポットと呼ばれる非発光部が多発するため、その表面に封止保護層を設けることが数多く提案されている(例えば、特開平4−233192号、特開平4−206386号、特開平4−79194号、特開平4−212284号)。 Furthermore, due to moisture penetration etc. from these organic thin-film electroluminescent device outside, since the non-luminous portion called dark spots causing degradation in durability frequently, a sealing protective layer on the surface it has been proposed to provide (e.g., JP-a-4-233192, JP-a-4-206386, JP-a-4-79194, JP-a-4-212284). しかしながら、未だ満足するものが得られていないのが現状である。 However, it has not yet been obtained which satisfies yet.

【0007】 [0007]

【発明が解決しようとする課題】本発明は、かかる事情に鑑み、外界からの水分等の侵入を防止し、ダークスポットの発生が少なく、耐久性に優れた電界発光素子を提供することを目的とする。 [0008] The present invention has been made in view of such circumstances, aims to prevent the penetration of moisture from the outside, the generation of dark spots is small, to provide an electroluminescent device having excellent durability to.

【0008】 [0008]

【課題を解決するための手段】本発明によれば、第1 According to the present invention, in order to solve the problems], first
に、基板上に陽極及び陰極とこれらの間に挟持された一層又は複数層の有機化合物層より構成される積層体を配置した有機薄膜型電界発光素子において、該積層体を保護するように封止保護層が設けられ、その封止保護層が構成成分として有機化合物層構成成分の少なくとも1種と無機酸化物を少なくとも1種含有することを特徴とする有機薄膜型電界発光素子が提供され、第2に、封止保護層構成成分である無機酸化物が一酸化ゲルマニウムであることを特徴とする上記有機薄膜型電界発光素子が提供される。 , As in the anode and cathode and the organic thin film electroluminescent elements arranged an configured laminate of an organic compound layer one or more layers interposed between these substrates, to protect the laminate seal provided stop protective layer, the sealing protective layer is an organic thin film electroluminescent device of at least one inorganic oxide of the organic compound layer constituent, characterized in that it contains at least one is provided as a component, second, the organic thin film electroluminescent elements, wherein the inorganic oxide is a sealing protective layer constituents monoxide germanium is provided.

【0009】以下、本発明を図面に沿って説明する。 [0009] The present invention will now be described with reference to the drawings. 図において、1はガラス基板、2は陽極、3は正孔輸送層、4は発光層、5は陰極、6は封止保護層である。 In FIG, 1 is a glass substrate, 2 anode, 3 hole-transporting layer, the fourth light emitting layer, 5 is the cathode, 6 is a sealing protective layer.

【0010】本発明に係る封止保護層6は前記したように、有機化合物層構成成分の少なくとも1種と無機酸化物を少なくとも1種を主成分とする。 [0010] As sealing protective layer 6 according to the present invention described above, as a main component at least one at least one inorganic oxide of the organic compound layer constituents.

【0011】有機化合物層の構成成分の少なくとも1種としては、後記する発光層、正孔輸送層、電子輸送層等の主成分となる有機化合物がそのまま使用できるが、電極をはさんで封止保護層に最も近い層の有機化合物層の構成成分がより好ましく、これらを用いることにより、 [0011] The at least one component of the organic compound layer, the light emitting layer to be described later, a hole transport layer, although the organic compound as a main component such as an electron transport layer can be used as it is, sealed across the electrodes constituents of the organic compound layer of the layer closest to the protective layer, more preferably, by using these,
耐久性が更に向上した電界発光素子が得られる。 Electroluminescent device durability was further improved can be obtained.

【0012】無機酸化物としては、CeO 2 、Cr [0012] Examples of the inorganic oxide, CeO 2, Cr
23 、MgO、MoO 3 、SiO、SiO 2 、TiO、T 2 O 3, MgO, MoO 3 , SiO, SiO 2, TiO, T
iO 2 、GeO等が挙げられるが、好ましいのはGeO iO 2, but GeO and the like, preferred are GeO
(一酸化ゲルマニウム)である。 It is a monoxide (germanium).

【0013】封止保護層の作成は蒸着法、溶液塗布法等の良好な膜形成法であれば任意の形成法を利用できる。 [0013] Creating a sealing protective layer may utilize any forming method if evaporation method, a good film-forming method such as a solution coating method.
例えば蒸着法の場合には多元蒸着法により所望の形態で作製が可能であり、溶液塗布法では所望の割合で塗布液を調整して成膜することができる。 For example in the case of the deposition method is capable of producing a desired form by multi-source deposition method, a solution coating method can be formed by adjusting the coating solution in the desired proportions. 封止保護層の緻密性や素子作製時の積層容易性等から蒸着法が好ましく、また抵抗加熱による蒸発が困難な無機酸化物を用いる場合には電子ビーム蒸着法等を利用するのが好ましい。 Preferably denseness and elements deposition of a laminated easiness during manufacturing of the sealing protective layer, also preferred to utilize an electron beam evaporation method or the like in the case of evaporation by resistance heating using a hard inorganic oxides. 封止保護層の膜厚は任意であるが、保護層の機能の発現性からみて500Å以上好ましくは1000Å以上であることがより好ましい。 The thickness of the sealing protective layer is optional, it is more preferable than 500Å preferably 1000Å or more viewed from the expression of function of the protective layer.

【0014】本発明による封止保護層が優れている理由としては、次のようなことが考えられる。 [0014] The reason for sealing the protective layer is excellent according to the present invention is considered to be as follows. 素子に封止保護層を設ける場合、封止保護層は金属である陰極と、陰極の形成されていない部分では有機化合物層と接することになり、2種類の性質の異なる物質と接する。 If element providing a sealing protective layer, sealing the protective layer and the cathode is a metal, it will be in contact with the organic compound layer in a portion not formed with the cathode, in contact with two different substances properties. 本発明による封止保護層は、無機酸化物と有機化合物層構成成分の両方を成分として含有している為、陰極と有機化合物層の双方との接着性、密着性が良好な状態となっていると考えられ、結果的にダークスポットの抑制等に効果を有する封止保護層が得られたものと推定される。 Sealing the protective layer according to the present invention, because they contain both inorganic oxide and an organic compound layer component as a component, adhesion to the both the cathode and the organic compound layer, adhesion becomes excellent condition considered are, sealing protective layer has an effect to suppress such a result, the dark spot is assumed obtained.

【0015】次に、本発明の他の構成要素について説明する。 Next, a description will be given other components of the present invention. 有機化合物を構成成分とする層としては、例えば発光層、正孔輸送性化合物と電子輸送性化合物との組合せになる発光層、正孔輸送層、電子輸送層等が挙げられ、有機化合物としては従来公知のものがいずれも使用できる。 The layer which includes an organic compound as a constituent component, for example, a light emitting layer, hole transporting compound and a light emitting layer made of a combination of the electron transport compound, a hole transport layer, an electron transporting layer and the like, and organic compounds both the conventionally known can be used. 以下、その具体例を示す。 Hereinafter, a specific example.

【0016】正孔輸送能を有する電子供与性有機化合物としては、ポリビニルカルバゾールのような正孔輸送能に優れた高分子化合物や正孔輸送能に優れた低分子化合物が挙げられる。 [0016] As the electron-donating organic compound having a hole transporting ability, low molecular compounds having excellent polymer compound or the hole transport property excellent in the hole transport ability such as polyvinyl carbazole. 低分子化合物の例としては、トリフェニルアミン類、スチルベン誘導体類、オキサジアゾール類等が挙げられ、その具体例としては、例えば以下のようなものが例示される。 Examples of low-molecular compounds, triphenylamine, stilbene derivatives, oxadiazoles and the like, Specific examples thereof include the following exemplified.

【0017】 [0017]

【表1】 [Table 1]

【0018】発光性有機化合物としては、電子輸送性または正孔輸送性を持ち、固体状態で強い蛍光を発する物質を用いる。 [0018] The luminous organic compound has an electron transporting property or hole transport property, a substance which emits strong fluorescence in the solid state. 電子輸送性の物質としては例えば、ペリノン誘導体、、キノリン錯体誘導体が挙げられるが、その具体例としては次のような物質等を挙げることができる。 As the electron transporting material for example, there may be mentioned perinone derivatives ,, quinoline complex derivatives, and following materials etc. As specific examples.

【0019】 [0019]

【表2】 [Table 2]

【0020】正孔輸送性の物質としては例えば、トリフェニルアミン誘導体、オキサジアゾール誘導体、トリフェニルアミン誘導体が挙げられるが、その具体例としては次のような物質等を挙げることができる。 [0020] As the hole-transporting materials such as triphenylamine derivatives, oxadiazole derivatives, triphenylamine derivatives, mention may be made of the following substances, and specific examples thereof.

【0021】 [0021]

【表3】 [Table 3]

【0022】発光層は、正孔輸送性、電子輸送性、発光特性を有する化合物を各々単独で用いた単層、あるいは正孔輸送性化合物、発光性化合物あるいは電子輸送性化合物の組合せによりなる多層で形成されていてもよい。 The light emitting layer, hole transporting, electron transporting, monolayer using the compound either singly with luminescent properties, or the hole transporting compound, multi-layer comprising a combination of a luminescent compound or electron transport compound in may be formed.

【0023】陽極2としては金、白金、パラジウムなどの金属の蒸着、スパッタ膜あるいはスズ、インジウム− The gold as the anode 2, platinum, deposition of a metal such as palladium, sputtered film or tin, indium -
スズの酸化薄膜(ITO)等で形成され、発光を取り出すため、400nm以上の波長領域で透明であることが望ましい。 Is formed by oxidizing a thin film (ITO) or the like of tin, for taking out light emission, it is desirable that transparent at least in the wavelength region 400 nm.

【0024】陽極4は、金属の真空蒸着により前記発光層上に形成されるが、その材質としては真空蒸着可能なあらゆる金属が使用され得るが、仕事関数が小さい金属、特にMg、Al、Ag、In、Sn、Pb、Mn、 The anode 4 is by vacuum deposition of a metal is formed on the light emitting layer, but any metal that can vacuum deposition may be used as its material, a metal having a low work function, in particular Mg, Al, Ag , In, Sn, Pb, Mn,
あるいはこれらの合金を用いることが望ましい。 Alternatively it is desirable to use these alloys.

【0025】 [0025]

【実施例】つぎに、本発明を実施例により更に詳細に説明する。 EXAMPLES Next, further detailed explanation of the present invention embodiment.

【0026】実施例1 ITOより成る2mm幅のストライプ状陽極パターンを形成したガラス基板を用い、図1に示すように正孔輸送層500Å、発光層500Åを蒸着して積層した。 [0026] using a glass substrate with the stripe anode pattern of 2mm width consisting Example 1 ITO, laminated by depositing a hole transport layer 500Å, light-emitting layer 500Å as shown in FIG. なお、正孔輸送層、発光層に用いた有機化合物は各々下記に示す〔化1〕、〔化2〕である。 The hole transport layer, an organic compound used for a light-emitting layer are each shown in the following general formula [1], a [Formula 2]. 次にMgCu合金(Mg:Cu=10:1)より成る陰極を2mm幅でI Then MgCu alloy I a cathode consisting of (Mg:: Cu = 10 1) with 2mm wide
TO陽極パターンと交差するように膜厚3000Åで蒸着した。 It was deposited in a thickness of 3000Å ​​to intersect TO anode pattern. 最後に封止保護層として〔化2〕とGeOを1:6(成膜速度比)で共蒸着により膜厚3500Åで積層し電界発光素子を作製した。 Finally as a sealing protective layer and [Formula 2] a GeO 1: by co-evaporation with 6 (deposition rate ratio) was prepared by laminating a film thickness of 3500Å electroluminescent device. 以上のようにして作製した素子は、素子作製1カ月後においても、ダークスポットによる発光領域の減少は認められず耐久性に優れた素子であった。 Element manufactured as described above, even after the device fabrication 1 month, reduction of the light emitting region due to dark spots was excellent device durability was not observed.

【化1】 [Formula 1]

【化2】 ## STR2 ##

【0027】実施例2 発光層に使用する有機化合物を下記〔化3〕に示す化合物とし、封止保護層を〔化3〕で示される化合物とSi [0027] The organic compounds used in Example 2 emission layer and compound shown in the following [Chemical Formula 3], a compound represented sealing protective layer in [Formula 3] and Si
Oを1:4(成膜速度比)で共蒸着した以外は実施例1 O 1: 4 except that the co-depositing (deposition rate ratio) Example 1
と同様にして作製した。 It was prepared in the same manner as. この素子は、素子作製1カ月後においても、ダークスポットによる発光領域の減少は認められず耐久性に優れた素子であった。 This device, even after device fabrication 1 month, reduction of the light emitting region due to dark spots was excellent device durability was not observed.

【化3】 [Formula 3]

【0028】比較例 封止保護層をSiOのみで構成した以外は実施例2と同様にして電界発光素子を作製した。 [0028] except that the comparative example sealing protective layer was constituted of only the SiO was fabricated EL device in the same manner as in Example 2. 以上のようにして作製した素子は、素子作製1カ月後において、ダークスポットによる発光領域の減少率は50%以上ともなり、陰極端部での劣化が著しいものであった。 Element manufactured as described above, after the device fabrication 1 month, the reduction rate of the light emitting region due to dark spots becomes even 50% or more, degradation in the cathode end was a remarkable.

【0029】 [0029]

【発明の効果】本発明の電界発光素子は、前記したように特有な封止保護層を設けたことから、電界発光素子を外界の水分等から良好に遮断保護することができるので、ダークスポット等の劣化のない耐久性の著しく優れたものである。 Electroluminescent device of the present invention according to the present invention, since the provision of the specific sealing protective layer as described above, it is possible to satisfactorily cut off protecting the light emitting element from the outside such as water, dark spots it is obtained significantly better degradation without the durability and the like.

【0030】 [0030]

【図面の簡単な説明】 BRIEF DESCRIPTION OF THE DRAWINGS

【図1】 本発明に係る電界発光素子の模式断面図。 Schematic cross-sectional view of an electroluminescent device according to the invention; FIG.

───────────────────────────────────────────────────── フロントページの続き (72)発明者 田元 望 東京都大田区中馬込1丁目3番6号 株式 会社リコー内 ────────────────────────────────────────────────── ─── of the front page continued (72) inventor the foot Nozomu Ota-ku, Tokyo Nakamagome 1-chome No. 3 No. 6 stock company in the Ricoh

Claims (2)

    【特許請求の範囲】 [The claims]
  1. 【請求項1】 基板上に陽極及び陰極とこれらの間に挟持された一層又は複数層の有機化合物層より構成される積層体を配置した有機薄膜型電界発光素子において、該積層体を保護するように封止保護層が設けられ、その封止保護層が構成成分として有機化合物層構成成分の少なくとも1種と無機酸化物を少なくとも含有することを特徴とする有機薄膜型電界発光素子。 1. A anode and cathode and the organic thin film electroluminescent elements arranged an configured laminate of an organic compound layer one or more layers interposed between these substrates, to protect the laminate sealing the protective layer is provided so as, organic thin film electroluminescent element characterized in that the sealing protective layer is at least contains at least one inorganic oxide of the organic compound layer component as a constituent component.
  2. 【請求項2】 封止保護層構成成分である無機酸化物が一酸化ゲルマニウムであることを特徴とする請求項1の有機薄膜型電界発光素子。 Wherein the organic thin-film electroluminescent device of claim 1, wherein the inorganic oxide is a sealing protective layer constituents monoxide germanium.
JP34821993A 1993-12-26 1993-12-26 Organic thin film type electroluminescent element Pending JPH07192866A (en)

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