JPH07192866A - Organic thin film electroluminescent device - Google Patents
Organic thin film electroluminescent deviceInfo
- Publication number
- JPH07192866A JPH07192866A JP5348219A JP34821993A JPH07192866A JP H07192866 A JPH07192866 A JP H07192866A JP 5348219 A JP5348219 A JP 5348219A JP 34821993 A JP34821993 A JP 34821993A JP H07192866 A JPH07192866 A JP H07192866A
- Authority
- JP
- Japan
- Prior art keywords
- electroluminescent device
- protective layer
- layer
- sealing protective
- organic thin
- Prior art date
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Abstract
(57)【要約】
【構成】 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。
【効果】 本発明の電界発光素子は、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から、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。
(57) [Summary] [Structure] An organic thin-film electroluminescent device comprising a substrate, and an anode and a cathode, and a laminate composed of one or a plurality of organic compound layers sandwiched between the anode and the cathode. An organic thin-film electroluminescent device, characterized in that a sealing protective layer is provided so as to protect the film, and the sealing protective layer contains at least one organic compound layer constituent component and an inorganic oxide as constituent components. . EFFECTS OF THE INVENTION The electroluminescent device of the present invention is provided with a unique sealing protective layer, and therefore, the electroluminescent device can be well shielded and protected from moisture in the external environment, so that it is durable without deterioration such as dark spots. It is extremely excellent in sex.
Description
【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。BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to an organic thin film type electroluminescent device which emits light when an electric field is applied.
【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。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。2. Description of the Related Art In recent years, as a color display device for displaying multicolor in response to an electric signal, an organic thin film type electroluminescent device which is a completely solid type and can obtain high-luminance light emission has been developed, and a light emitting device in various display devices. Is being watched as. Since this organic thin film type electroluminescent device is made of an organic material as a raw material, the material constituting it can be selected from various materials, and since it is a completely solid type, it has excellent impact resistance and low voltage. It has excellent properties such as being able to emit light by applying voltage, being able to obtain high-luminance and high-efficiency light emission, and being capable of multicolor display. Research on the materials and structures that make it up is active. Has been done 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／
正孔輸送層／陽極、等の構成のものが開発されている。
具体的には、例えば、透明基板上に、複数の透明陽極、
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。The organic thin film electroluminescent device has a structure such as cathode / light emitting layer / hole transport layer / anode, cathode / electron transport layer / light emitting layer / anode, cathode / electron transport layer / light emitting layer /
A structure such as a hole transport layer / anode has been developed.
Specifically, for example, on a transparent substrate, a plurality of transparent anodes,
A hole transport layer, a light emitting layer, if necessary, an electron transport layer, and a plurality of back cathodes intersecting with the transparent electrode are 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。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。The hole transport layer has a function of facilitating injection of holes from the anode and a function of blocking electrons, while the electron transport layer has a function of facilitating injection of electrons from the cathode. ing. In the light-emitting layer, excitons are generated by recombination of electrons and holes injected from the pair of electrodes, and the excitons emit light in the process of radiation deactivation, and the light passes through the transparent electrode and the transparent substrate. It is released to the outside and can be displayed.
【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）。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）。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）。In such an organic thin film type electroluminescent device, it is desired to miniaturize the electrode pattern in order to make the device finer, and an interlayer insulating film is formed between the electrodes to improve the uniformity of light emission. There has been proposed a device which holds and improves pattern accuracy (Japanese Patent Laid-Open No. 3-250583). In addition, there is also proposed a structure in which an insulating layer is formed between an organic compound layer and an electrode to improve pattern accuracy and display quality (JP-A-3-274694). Furthermore, there has been proposed a structure in which an insulating layer is formed on the edge of the electrode to reduce crosstalk and bleeding of light emission (Japanese Patent Laid-Open No. 4-51494).
【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）。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。Further, in these organic thin film type electroluminescent devices, non-luminous portions called dark spots, which cause deterioration of durability, frequently occur due to invasion of moisture from the outside, and therefore, a sealing protective layer is formed on the surface thereof. Many proposals have been made to provide them (for example, JP-A-4-233192, JP-A-4-206386, JP-A-4-79194, and JP-A-4-212284). However, the current situation is that the one that satisfies us has not been obtained 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。SUMMARY OF THE INVENTION In view of such circumstances, an object of the present invention is to provide an electroluminescent device which prevents moisture and the like from entering from the outside world, has few dark spots, and is excellent in durability. And
【０００８】[0008]
【課題を解決するための手段】本発明によれば、第１
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。According to the present invention, a first
In an organic thin-film electroluminescent device in which a laminate composed of an anode and a cathode and one or a plurality of organic compound layers sandwiched therebetween is arranged on a substrate, a seal is provided to protect the laminate. An organic thin film type electroluminescent device is provided, which is provided with a stop protective layer, and the sealing protective layer contains at least one organic compound layer constituent component and at least one inorganic oxide as constituent components, Secondly, there is provided the organic thin film type electroluminescent device as described above, wherein the inorganic oxide which is a constituent component of the sealing protective layer is germanium monoxide.
【０００９】以下、本発明を図面に沿って説明する。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。The present invention will be described below with reference to the drawings. In the figure, 1 is a glass substrate, 2 is an anode, 3 is a hole transport layer, 4 is a light emitting layer, 5 is a cathode, and 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。As described above, the sealing protective layer 6 according to the present invention contains at least one organic compound layer constituent component and at least one inorganic oxide as a main component.
【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、
耐久性が更に向上した電界発光素子が得られる。As at least one of the constituent components of the organic compound layer, an organic compound as a main component of a light emitting layer, a hole transporting layer, an electron transporting layer, etc., which will be described later, can be used as it is, but it is sealed by sandwiching the electrodes. The constituent components of the organic compound layer closest to the protective layer are more preferable, and by using these,
An electroluminescent device having further improved durability can be obtained.
【００１２】無機酸化物としては、ＣｅＯ2、Ｃｒ
2Ｏ3、ＭｇＯ、ＭｏＯ3、ＳｉＯ、ＳｉＯ2、ＴｉＯ、Ｔ
ｉＯ2、ＧｅＯ等が挙げられるが、好ましいのはＧｅＯ
（一酸化ゲルマニウム）である。Inorganic oxides include CeO 2 , Cr
2 O 3 , MgO, MoO 3 , SiO, SiO 2 , TiO, T
Examples thereof include iO 2 and GeO, and GeO is preferable.
(Germanium monoxide).
【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。
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。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。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。Any method can be used to form the sealing protective layer as long as it is a good film forming method such as a vapor deposition method or a solution coating method.
For example, in the case of the vapor deposition method, the desired form can be produced by the multi-source vapor deposition method, and in the solution coating method, the coating liquid can be adjusted at a desired ratio to form a film. The vapor deposition method is preferable from the viewpoint of the denseness of the sealing protective layer and the ease of stacking at the time of manufacturing the element, and when using an inorganic oxide that is difficult to evaporate by resistance heating, the electron beam vapor deposition method or the like is preferably used. Although the film thickness of the sealing protective layer is arbitrary, it is preferably 500 Å or more, and more preferably 1000 Å or more, from the viewpoint of the 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。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。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。The reason why the sealing protective layer according to the present invention is excellent is considered as follows. When a sealing protective layer is provided on the device, the sealing protective layer comes into contact with the metal cathode and the organic compound layer in the portion where the cathode is not formed, and thus comes into contact with two different substances. Since the sealing protective layer according to the present invention contains both the inorganic oxide and the organic compound layer constituent components as components, the adhesiveness and the adhesiveness with both the cathode and the organic compound layer are in a good state. It is presumed that a sealing protective layer having an effect of suppressing dark spots was obtained as a result.
【００１５】次に、本発明の他の構成要素について説明
する。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。以下、その具体例を示す。Next, other components of the present invention will be described. Examples of the layer containing an organic compound as a constituent component include a light emitting layer, a light emitting layer which is a combination of a hole transporting compound and an electron transporting compound, a hole transporting layer, an electron transporting layer, and the like. Any conventionally known one can be used. The specific examples are shown below.
【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。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 the electron-donating organic compound having a hole-transporting ability include a polymer compound having an excellent hole-transporting ability such as polyvinylcarbazole and a low-molecular compound having an excellent hole-transporting ability. Examples of low molecular weight compounds include triphenylamines, stilbene derivatives, oxadiazoles and the like, and specific examples thereof include the following.
【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。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 light emitting organic compound, a substance having an electron transporting property or a hole transporting property and emitting strong fluorescence in a solid state is used. Examples of the electron-transporting substance include a perinone derivative and a quinoline complex derivative, and specific examples thereof include the following substances.
【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。Examples of the hole-transporting substance include triphenylamine derivatives, oxadiazole derivatives and triphenylamine derivatives. Specific examples thereof include the following substances.
【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 is a single layer in which a compound having a hole transporting property, an electron transporting property, and a light emitting property is used alone, or a multi-layer comprising a combination of a hole transporting compound, a light emitting compound or an electron transporting compound. It may be formed of.
【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−
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。As the anode 2, a metal such as gold, platinum or palladium is vapor-deposited, a sputtered film, tin or indium.
Since it is formed of tin oxide thin film (ITO) or the like and emits light, it is desirable that it is transparent in the wavelength region of 400 nm or more.
【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、
あるいはこれらの合金を用いることが望ましい。The anode 4 is formed on the light emitting layer by vacuum vapor deposition of a metal. As the material thereof, any metal capable of being vacuum vapor deposited can be used, but a metal having a small work function, particularly Mg, Al, Ag. , In, Sn, Pb, Mn,
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, the present invention will be described in more detail with reference to Examples.
【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。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。次にＭｇＣｕ合金
（Ｍｇ：Ｃｕ＝１０：１）より成る陰極を２ｍｍ幅でＩ
ＴＯ陽極パターンと交差するように膜厚３０００Åで蒸
着した。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。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。Example 1 A glass substrate having a stripe-shaped anode pattern made of ITO and having a width of 2 mm was used to deposit a hole transport layer 500Å and a light emitting layer 500Å as shown in FIG. The organic compounds used for the hole transport layer and the light emitting layer are the following [Chemical formula 1] and [Chemical formula 2], respectively. Next, a cathode made of a MgCu alloy (Mg: Cu = 10: 1) was used with a width of 2 mm.
Deposition was performed with a film thickness of 3000Å so as to intersect with the TO anode pattern. Finally, as a sealing protective layer, [Chemical Formula 2] and GeO were laminated by co-evaporation at a film thickness of 3500Å at a ratio of 1: 6 (film formation rate ratio) to manufacture an electroluminescent device. The element produced as described above was an element having excellent durability without a decrease in the light emitting region due to dark spots even one month after the element was produced.
【化１】 [Chemical 1]
【化２】 [Chemical 2]
【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
Ｏを１：４（成膜速度比）で共蒸着した以外は実施例１
と同様にして作製した。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。Example 2 The organic compound used in the light emitting layer was the compound represented by the following [Chemical formula 3], and the sealing protective layer was the compound represented by the [Chemical formula 3] and Si.
Example 1 except that O was co-deposited at a ratio of 1: 4 (deposition rate).
Was prepared in the same manner as in. This device was excellent in durability, even after 1 month from the production of the device, with no reduction in the light emitting region due to dark spots.
【化３】 [Chemical 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。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。Comparative Example An electroluminescent device was manufactured in the same manner as in Example 2 except that the sealing protective layer was composed of only SiO 2. In the device manufactured as described above, the reduction rate of the light emitting region due to the dark spot was as high as 50% or more one month after the device was manufactured, and the deterioration at the cathode end was 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。Since the electroluminescent device of the present invention is provided with the peculiar sealing protective layer as described above, the electroluminescent device can be well shielded and protected from moisture in the external environment, so that the dark spot It has excellent durability without deterioration.
【００３０】[0030]
【図１】 本発明に係る電界発光素子の模式断面図。FIG. 1 is a schematic cross-sectional view of an electroluminescent device according to the present invention.
───────────────────────────────────────────────────── 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 ─────────────────────────────────────────────────── ─── Continuation of the front page (72) Inventor Nozomi Tamoto 1-3-3 Nakamagome, Ota-ku, Tokyo Inside Ricoh Co., Ltd.
Claims (2)
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. An organic thin-film electroluminescent device in which an anode, a cathode, and a laminated body composed of one or a plurality of organic compound layers sandwiched therebetween are arranged on a substrate, and the laminated body is protected. Thus, an organic thin film type electroluminescent device characterized in that the sealing protective layer is provided, and the sealing protective layer contains at least one organic compound layer constituent component and an inorganic oxide as constituent components.
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。2. The organic thin film type electroluminescent device according to claim 1, wherein the inorganic oxide which is a constituent component of the sealing protective layer is germanium monoxide.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP5348219A JPH07192866A (en) | 1993-12-26 | 1993-12-26 | Organic thin film electroluminescent device |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP5348219A JPH07192866A (en) | 1993-12-26 | 1993-12-26 | Organic thin film electroluminescent device |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| JPH07192866A true JPH07192866A (en) | 1995-07-28 |
Family
ID=18395552
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP5348219A Pending JPH07192866A (en) | 1993-12-26 | 1993-12-26 | Organic thin film electroluminescent device |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPH07192866A (en) |
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