JPH11111456A - Multiple type multicolor-emitting organic electroluminescent element - Google Patents

Multiple type multicolor-emitting organic electroluminescent element

Info

Publication number
JPH11111456A
JPH11111456A JP9264504A JP26450497A JPH11111456A JP H11111456 A JPH11111456 A JP H11111456A JP 9264504 A JP9264504 A JP 9264504A JP 26450497 A JP26450497 A JP 26450497A JP H11111456 A JPH11111456 A JP H11111456A
Authority
JP
Japan
Prior art keywords
layer
organic electroluminescent
interlayer insulating
electrode
light
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.)
Granted
Application number
JP9264504A
Other languages
Japanese (ja)
Other versions
JP3887079B2 (en
Inventor
Koichi Yamashita
浩一 山下
Tatsuo Mori
竜雄 森
Terukichi Mizutani
照吉 水谷
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Nippon Steel Chemical and Materials Co Ltd
Original Assignee
Nippon Steel Chemical Co Ltd
Priority date (The priority date 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 date listed.)
Filing date
Publication date
Application filed by Nippon Steel Chemical Co Ltd filed Critical Nippon Steel Chemical Co Ltd
Priority to JP26450497A priority Critical patent/JP3887079B2/en
Publication of JPH11111456A publication Critical patent/JPH11111456A/en
Application granted granted Critical
Publication of JP3887079B2 publication Critical patent/JP3887079B2/en
Anticipated expiration legal-status Critical
Expired - Fee Related legal-status Critical Current

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Classifications

    • HELECTRICITY
    • H10SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10KORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K59/00Integrated devices, or assemblies of multiple devices, comprising at least one organic light-emitting element covered by group H10K50/00
    • H10K59/30Devices specially adapted for multicolour light emission
    • H10K59/32Stacked devices having two or more layers, each emitting at different wavelengths

Landscapes

  • Electroluminescent Light Sources (AREA)
  • Luminescent Compositions (AREA)

Abstract

PROBLEM TO BE SOLVED: To simultaneously drive respective elements and emit multi-color electroluminescence by forming a plurality of luminescent layers with different luminescent colors and forming interlayer insulating films between a back face electrode and a light transmissive electrode. SOLUTION: In this multiple type organic electroluminescent element, a light transmissive electrode 2, a luminescent layer 3 containing an organic phosphor substance, and a back face electrode 4 are successively formed on a transparent substrate 1 to give a first element layer A and a light transmissive electrode 2', a luminescent layer 3', and a back face electrode 4' are successively laminated further on the element layer A to give a second element layer B and two or more such element layers are laminated. The luminescent layers 3, 3' are so constituted as to emit respectively different colors and an interlayer insulating film 5 is formed between the back face electrode 4 of the first element layer A and the light transmissive electrode 2' of the second element layer B. The polyparaxylylene base polymer compound to be used for the interlayer insulating film 5 has excellent electric insulation property and sufficient to independently and respectively drive the organic electroluminescent elements formed in both sides of the films 5.

Description

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

【0001】[0001]

【発明の属する技術分野】本発明は、有機電界発光素子
に関し、さらに詳しくは透明基板上に透光性電極、発光
層及び背面電極を順次積層してなる多重型多色発光有機
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 electroluminescent device, and more particularly, to a multiplex type multicolor organic electroluminescent device in which a light-transmitting electrode, a light-emitting layer and a back electrode are sequentially laminated on a transparent substrate. .

【0002】[0002]

【従来の技術】従来のブラウン管に代わるフラットパネ
ルディスプレイの需要の急増に伴い、各種表示素子の開
発及び実用化が精力的に進められている。電界発光素子
もこうしたニーズに応えるものであり、特に全体が固体
の自発光素子であって他のディスプレイにはない高解像
度及び高視認性を有することから注目を集めている。そ
して現在実用化されているものとしては、発光層にZn
S/Mn系の無機材料を用いた無機電界発光素子が知ら
れている。しかしながら、この種の無機電界発光素子に
おいては、発光に必要な駆動電圧が100V以上と高
く、このために駆動方法が複雑になって製造コストが高
くなるという問題があるほか、青色発光の効率が低くて
フルカラー化が困難であるという問題もある。
2. Description of the Related Art With the rapid increase in demand for flat panel displays replacing conventional CRTs, various display elements have been developed and put into practical use. Electroluminescent devices also meet these needs, and are particularly attracting attention because they are solid self-luminous devices and have high resolution and high visibility that other displays do not have. Currently, the light emitting layer has been put into practical use.
An inorganic electroluminescent device using an S / Mn-based inorganic material is known. However, in this type of inorganic electroluminescent device, the driving voltage required for light emission is as high as 100 V or more, which causes a problem that the driving method is complicated and the manufacturing cost is increased. There is also a problem that it is difficult to achieve full color because of low cost.

【0003】これに対して、有機材料を用いた薄膜有機
電界発光素子は、その発光に必要な駆動電圧を大幅に低
くすることができ、また各種の発光材料の適用によりフ
ルカラー化の可能性も充分にあり、近年その研究が活発
化している。中でも、フルカラー化に際し、色の同調方
法は素子応用への大きな研究課題となっている。
On the other hand, a thin film organic electroluminescent device using an organic material can drastically reduce the driving voltage required for its light emission, and the possibility of full color by applying various light emitting materials is also increased. There is enough, and the research has been active in recent years. Above all, the color tuning method has become a major research topic for device application in full color.

【0004】従来の有機電界発光素子は、一つの素子か
らは一色の光しか発光しない(特開平5−198378
号公報等)。このため、フルカラーディスプレイにおい
て、必要な色の3原色である赤、緑及び青を発光させる
ためには、それぞれの色の素子を微細にかつ規則正しく
並べることが必須になり、素子によっては、必要な色の
画素数分だけ微細にかつ規則正しく並べることは非常に
困難なことであった。
A conventional organic electroluminescent device emits only one color of light from one device (Japanese Patent Laid-Open No. 5-198338).
No.). For this reason, in a full-color display, in order to emit red, green, and blue, which are three primary colors of required colors, it is essential to arrange elements of each color finely and regularly. It has been very difficult to finely and regularly arrange the pixels by the number of color pixels.

【0005】[0005]

【発明が解決しようとする課題】したがって、本発明の
目的は、各々の素子を同時に駆動して多色発光可能な多
重型多色発光有機電界発光素子を提供することにある。
SUMMARY OF THE INVENTION Accordingly, an object of the present invention is to provide a multiplex type multicolor light emitting organic electroluminescent device capable of driving each device simultaneously to emit multicolor light.

【0006】[0006]

【課題を解決するための手段】本発明者らは、上記課題
を鋭意検討した結果、有機電界発光素子の層構成に特徴
を持たせることで、前記課題を解決しうることを見出
し、本発明を完成するに至った。
Means for Solving the Problems As a result of diligent studies on the above problems, the present inventors have found that the above problems can be solved by giving a characteristic to the layer structure of the organic electroluminescent device. Was completed.

【0007】すなわち、本発明は、透明基板上に透光性
電極、有機蛍光性物質を含有する発光層及び背面電極を
順次積層してなる有機電界発光素子において、発光色の
異なる少なくとも2層以上の発光層を有し、かつ背面電
極と透光性電極の間に層間絶縁膜を有してなる多重型多
色発光有機電界発光素子である。
That is, the present invention provides an organic electroluminescent device in which a light-transmitting electrode, a light-emitting layer containing an organic fluorescent substance, and a back electrode are sequentially laminated on a transparent substrate. Is a multiplex type multicolor light-emitting organic electroluminescent device having a light-emitting layer and an interlayer insulating film between a back electrode and a translucent electrode.

【0008】また、本発明は、上記の多重型多色発光有
機電界発光素子において、層間絶縁膜が、ポリパラキシ
リレン、ポリモノクロロパラキシリレン、ポリモノブロ
ムパラキシリレン、ポリシアノパラキシリレン、ポリジ
クロロパラキシリレン、ポリメチルパラキシリレン又は
ポリエチルパラキシリレンから選ばれた少なくとも1種
のポリパラキシリレン系高分子化合物を1層又は2層以
上積層してなる多重型多色発光有機電界発光素子であ
る。
Further, the present invention provides the multiplex type multicolor light emitting organic electroluminescent device, wherein the interlayer insulating film is made of polyparaxylylene, polymonochloroparaxylylene, polymonobromoparaxylylene, polycyanoparaxylylene. Multi-color light emission comprising one or more layers of at least one polyparaxylylene-based polymer compound selected from polydichloroparaxylylene, polymethylparaxylylene or polyethylparaxylylene An organic electroluminescent device.

【0009】[0009]

【発明の実施の形態】図1は、本発明の多重型多色発光
有機電界発光素子(以下、多重有機電界発光素子ともい
う)の基本概念の一例を示す側面断面図である。本発明
の多重有機電界発光素子は、透明基板1の上に、透光性
電極2、有機蛍光性物質を含有する発光層(以下、発光
層ともいう)3及び背面電極4を順次積層して第1素子
層Aとし、この上に更に、透光性電極2’、発光層3’
及び背面電極4’を順次積層して第2素子層Bとし、こ
のような素子層が2以上積層された構造とされている。
そして、発光層3、3’はそれぞれ異なる色を発光する
ように構成され、また第1素子層Aの背面電極4と第2
素子層Bの透光性電極2’との間には層間絶縁膜5が設
けられている。なお、図1には、第1素子層Aと第2素
子層Bの2層の素子層からなる二重型二色発光有機電界
発光素子の例を示したが、更にこれに層間絶縁膜を介し
て他の色を発光する第3素子層を設けるなど多重型多色
発光有機電界発光素子とすることもできる。
FIG. 1 is a side sectional view showing an example of a basic concept of a multiplex type multicolor light emitting organic electroluminescent device (hereinafter, also referred to as a multiplex organic electroluminescent device) of the present invention. In the multiple organic electroluminescent device of the present invention, a light-transmitting electrode 2, a light-emitting layer (hereinafter, also referred to as a light-emitting layer) 3 containing an organic fluorescent substance, and a back electrode 4 are sequentially laminated on a transparent substrate 1. The first element layer A was formed, and a light transmitting electrode 2 ′ and a light emitting layer 3 ′ were further formed thereon.
And the back electrode 4 ′ are sequentially laminated to form a second element layer B, and two or more such element layers are laminated.
The light emitting layers 3 and 3 ′ are configured to emit different colors, respectively, and the back electrode 4 of the first element layer A and the second
An interlayer insulating film 5 is provided between the element layer B and the translucent electrode 2 '. FIG. 1 shows an example of a double-type two-color light-emitting organic electroluminescent element composed of two element layers, a first element layer A and a second element layer B, which is further provided with an interlayer insulating film interposed therebetween. For example, a multiplex-type multicolor organic electroluminescent element can be provided by providing a third element layer that emits another color.

【0010】本発明の多重有機電界発光素子に用いられ
る透明基板は、透明性を有する基板であれば特に限定さ
れるものではないが、耐熱性の点からガラス基板が好ま
しい。
The transparent substrate used in the multiple organic electroluminescent device of the present invention is not particularly limited as long as it is a substrate having transparency, but a glass substrate is preferred from the viewpoint of heat resistance.

【0011】各素子層の透光性電極としては、例えば
金、ニッケル等の半透膜や、インジウムスズ酸化物(以
下、ITOという)、酸化スズ、酸化インジウム、酸化
亜鉛アルミニウム、ポリピロール等の透明導電膜などが
挙げられる。その形成方法としては、例えば抵抗加熱蒸
着法、電子ビーム蒸着法、スパッタリング法、電解重合
法などが挙げられる。
The light-transmitting electrode of each element layer is, for example, a semi-permeable film of gold, nickel or the like, or a transparent material of indium tin oxide (hereinafter referred to as ITO), tin oxide, indium oxide, zinc aluminum oxide, polypyrrole, or the like. A conductive film; Examples of the formation method include a resistance heating evaporation method, an electron beam evaporation method, a sputtering method, and an electrolytic polymerization method.

【0012】また、発光層は、有機蛍光性物質を含有す
るものであればよく、透光性電極、正孔注入層又は正孔
注入輸送層から注入された正孔と、背面電極、電子注入
層又は電子注入輸送層から注入された電子との高効率な
再結合により発光する有機蛍光性物質が用いられる。こ
のような有機蛍光性物質としては、例えば8−オキシキ
ノリンのアルミニウム錯体、芳香族化合物などが挙げら
れる。その形成方法としては、例えば抵抗加熱蒸着法、
電子ビーム蒸着法、スピンコート法、キャスティング
法、LB法、分子線エピタキシ法などがあげられる。
The light-emitting layer may be any one containing an organic fluorescent substance. The light-emitting layer includes a hole injected from a light-transmitting electrode, a hole injection layer or a hole injection transport layer, a back electrode, and an electron injection layer. An organic fluorescent substance that emits light by highly efficient recombination with electrons injected from the layer or the electron injection / transport layer is used. Examples of such an organic fluorescent substance include an aluminum complex of 8-oxyquinoline and an aromatic compound. As a forming method, for example, a resistance heating evaporation method,
Examples include an electron beam evaporation method, a spin coating method, a casting method, an LB method, and a molecular beam epitaxy method.

【0013】本発明の多重有機電界発光素子における発
光層は、有機蛍光性物質を含有するものであればよい
が、さらに正孔注入層、正孔注入輸送層、電子注入輸送
層などを設けてもよい。
The light emitting layer in the multiple organic electroluminescent device of the present invention may be any as long as it contains an organic fluorescent substance, and is further provided with a hole injection layer, a hole injection transport layer, an electron injection transport layer and the like. Is also good.

【0014】正孔注入層を設ける場合、透光性電極から
高効率で正孔を注入し、かつ発光した光の発光極大領域
においてできるだけ透明なものを用いることが好まし
い。正孔注入層に用いる材料としては、例えばアミン化
合物、ヒドラゾン化合物、ピラゾリン化合物、シラン化
合物、ポルフィリン化合物、フタロシアニン、ポリビニ
ルカルバゾール、その他の芳香族化合物や、無定形P型
シリコン、無定形P型炭化シリコンなどが挙げられる。
その形成方法としては、例えば抵抗加熱蒸着法、スピン
コート法、キャスティング法、LB法、電子ビーム蒸着
法、分子線エピタキシ法、化学気相蒸着法などが挙げら
れる。
When a hole injection layer is provided, it is preferable to inject holes with high efficiency from the translucent electrode and to use a layer as transparent as possible in the maximum region of emitted light. Materials used for the hole injection layer include, for example, amine compounds, hydrazone compounds, pyrazoline compounds, silane compounds, porphyrin compounds, phthalocyanine, polyvinylcarbazole, other aromatic compounds, amorphous P-type silicon, amorphous P-type silicon carbide And the like.
Examples of the formation method include a resistance heating evaporation method, a spin coating method, a casting method, an LB method, an electron beam evaporation method, a molecular beam epitaxy method, and a chemical vapor deposition method.

【0015】また、正孔注入輸送層には、正孔を効率よ
く注入及び輸送し、かつ発光した光の発光極大領域にお
いてできるだけ透明なものを用いることが好ましい。正
孔注入輸送層に用いる材料としては、正孔注入層と同
様、例えばアミン化合物、ヒドラゾン化合物、ピラゾリ
ン化合物、シラン化合物、ポルフィリン化合物、フタロ
シアニン、ポリビニルカルバゾール、その他の芳香族化
合物や、無定形P型シリコン、無定形P型炭化シリコン
などが挙げられる。その形成方法としては、例えば抵抗
加熱蒸着法、スピンコート法、キャスティング法、LB
法、電子ビーム蒸着法、分子線エピタキシ法、化学気相
蒸着法などが挙げられる。
It is preferable that the hole injecting / transporting layer be one that efficiently injects and transports holes, and that is as transparent as possible in the maximum region of emitted light. As the material used for the hole injection transport layer, similar to the hole injection layer, for example, an amine compound, a hydrazone compound, a pyrazoline compound, a silane compound, a porphyrin compound, phthalocyanine, polyvinyl carbazole, other aromatic compounds, and amorphous P-type Silicon and amorphous P-type silicon carbide can be used. Examples of the formation method include resistance heating evaporation, spin coating, casting, and LB.
Method, an electron beam evaporation method, a molecular beam epitaxy method, a chemical vapor deposition method, and the like.

【0016】さらに、電子注入輸送層を設ける場合、電
子を効率よく注入輸送できるものであればよい。電子注
入輸送層に用いる材料としては、例えば8−オキシキノ
リンのアルミニウム錯体、ニトロ置換フルオレノン誘導
体、アントラキノン誘導体、ジオキサゾール誘導体、チ
オピランジオキシド誘導体、フルオレニリデンメタン誘
導体、アントロン誘導体、ペリレン誘導体、ジオキサン
誘導体、オキサジアゾール化合物、オキサトリアゾール
化合物、その他の有機化合物や、無定形n型シリコン、
無機半導体などが挙げられる。その形成方法としては、
抵抗加熱蒸着法、電子ビーム蒸着法、スピンコート法、
キャスティング法、LB法、分子線エピタキシ法などが
挙げられる。
Further, when an electron injecting and transporting layer is provided, any layer can be used as long as it can inject and transport electrons efficiently. Materials used for the electron injecting and transporting layer include, for example, aluminum complexes of 8-oxyquinoline, nitro-substituted fluorenone derivatives, anthraquinone derivatives, dioxazole derivatives, thiopyran dioxide derivatives, fluorenylidenemethane derivatives, anthrone derivatives, perylene derivatives, dioxane Derivatives, oxadiazole compounds, oxatriazole compounds, other organic compounds, amorphous n-type silicon,
Inorganic semiconductors and the like can be mentioned. The formation method is
Resistance heating evaporation, electron beam evaporation, spin coating,
A casting method, an LB method, a molecular beam epitaxy method, and the like can be given.

【0017】背面電極は、電子を効率よく有機層(発光
層、電子注入層、電子注入輸送層等)に注入できるもの
であればよく、一般的には、仕事関数の小さいLi、N
a、Mg、Sr、Ag、In、Sn、Zn、Zr、C
a、Al、Mo、Bi等の単独金属の薄膜や、これらの
2成分、3成分等の積層、共蒸着、合金等の複合化合物
の薄膜などが用いられる。この背面電極の形成方法とし
ては、例えば抵抗加熱蒸着法、電子ビーム蒸着法、スパ
ッタリング法、イオンプレーティング法などが挙げられ
る。
The back electrode may be any material that can efficiently inject electrons into an organic layer (emission layer, electron injection layer, electron injection transport layer, etc.).
a, Mg, Sr, Ag, In, Sn, Zn, Zr, C
A thin film of a single metal such as a, Al, Mo, Bi or the like, or a thin film of a composite compound such as lamination, co-evaporation, alloy or the like of these two components and three components is used. Examples of the method for forming the back electrode include a resistance heating evaporation method, an electron beam evaporation method, a sputtering method, and an ion plating method.

【0018】本発明の多重有機電界発光素子には、積層
した素子と素子の層間に層間絶縁膜を設ける必要があ
る。例えば、図1において、第1素子層Aの背面電極4
と第2素子層Bの透光性電極2’との間に層間絶縁膜5
を設けることが必要である。この層間絶縁膜5は背面電
極4の外表面側に設ける。この際、層間絶縁膜5は、背
面電極4のみを被覆してもよいが、発光層3を含む有機
層全体を被覆することが好ましい。また、最外層の背面
電極4’は、層間絶縁膜で被覆してもしなくてもよい
が、被覆する場合は、背面電極4’のみを被覆してもよ
く、発光層3’を含む有機層全体を被覆してもよい。有
機電界発光素子の寿命の観点からは、発光層3’を含む
有機層全体を被覆することが好ましい。なお、素子層が
3層以上が存在する場合は、同様に各層間に層間絶縁膜
を設ける必要がある。
In the multiple organic electroluminescent device of the present invention, it is necessary to provide an interlayer insulating film between the stacked devices and between the devices. For example, in FIG. 1, the back electrode 4 of the first element layer A
Between the transparent electrode 2 ′ of the second element layer B and the interlayer insulating film 5
It is necessary to provide. This interlayer insulating film 5 is provided on the outer surface side of the back electrode 4. At this time, the interlayer insulating film 5 may cover only the back electrode 4, but preferably covers the entire organic layer including the light emitting layer 3. The outermost back electrode 4 ′ may or may not be covered with an interlayer insulating film. If covered, the back electrode 4 ′ may be covered only with the back electrode 4 ′. The whole may be covered. From the viewpoint of the life of the organic electroluminescent element, it is preferable to cover the entire organic layer including the light emitting layer 3 '. When there are three or more element layers, it is necessary to similarly provide an interlayer insulating film between the respective layers.

【0019】このような層間絶縁膜は、耐熱性がよく透
明であり、製膜する際に発光素子に悪影響を与えないも
のであれば特に限定されるものではない。本発明に用い
る層間絶縁膜の材料としては、特にポリパラキシリレン
系高分子化合物が好ましい。ポリパラキシリレン系高分
子化合物は、電気絶縁性が優れ、層の両側に形成された
有機電界発光素子の駆動時に電気的相互作用を全く与え
ることなく、各々独立に駆動させることが可能となる。
また、酸素と水分透過性が著しく低く、有機電界発光素
子への劣化原因である酸素と水分を接触抑制することも
でき、有機電界発光素子のよりいっそうの長寿命化を図
ることができる。
Such an interlayer insulating film is not particularly limited as long as it has good heat resistance and is transparent, and does not adversely affect the light-emitting element when the film is formed. As a material of the interlayer insulating film used in the present invention, a polyparaxylylene-based polymer compound is particularly preferable. The polyparaxylylene-based polymer compound has excellent electrical insulation properties, and can be independently driven without giving any electric interaction when driving the organic electroluminescent elements formed on both sides of the layer. .
In addition, oxygen and moisture permeability are remarkably low, so that contact between oxygen and moisture, which is a cause of deterioration of the organic electroluminescent element, can be suppressed, and the life of the organic electroluminescent element can be further extended.

【0020】このポリパラキシリレン系高分子化合物と
しては、例えばポリパラキシリレン(ユニオン・カーバ
イト社製 商品名 パリレンN)、ポリモノクロロパラ
キシリレン(同パリレンC)、ポリジクロロパラキシリ
レン(同パリレンD)などの他、ポリモノブロムパラキ
シリレン、ポリシアノパラキシリレン、ポリメチルパラ
キシリレン、ポリエチルパラキシリレンなどが挙げられ
る。
Examples of the polyparaxylylene-based polymer compound include polyparaxylylene (trade name: Parylene N, manufactured by Union Carbide Co., Ltd.), polymonochloroparaxylylene (parylene C), polydichloroparaxylylene ( Other than the above parylene D), polymonobromoparaxylylene, polycyanoparaxylylene, polymethylparaxylylene, polyethylparaxylylene and the like can be mentioned.

【0021】これらのポリパラキシリレン系高分子化合
物は、単独で用いてもよいし、2種類以上を組み合わせ
て2層以上の積層構造をもつ層間絶縁膜を形成してもよ
い。また、これらの層間絶縁膜の総膜厚を1.0μm以
上とすると、水分やガスとの接触を抑制できるので好ま
しい。
These polyparaxylylene polymer compounds may be used alone or in combination of two or more to form an interlayer insulating film having a laminated structure of two or more layers. Further, it is preferable that the total thickness of these interlayer insulating films is 1.0 μm or more, because contact with moisture or gas can be suppressed.

【0022】この層間絶縁膜は、熱CVD法により形成
することが好ましい。熱CVD法は、原料となるジパラ
キシリレン系低分子化合物を気相重合し、有機電界発光
素子の背面電極側へ製膜する、重合・製膜を真空を破ら
ずに進行する連続プロセスであり、酸素、水分の接触を
抑制できる方法である。この熱CVD法は、製膜する際
の有機電界発光素子の温度が室温程度に抑えることがで
き、発光特性に悪影響を及ぼさずに製膜できる。
This interlayer insulating film is preferably formed by a thermal CVD method. The thermal CVD method is a continuous process in which gas-phase polymerization of a diparaxylylene-based low-molecular compound as a raw material is performed to form a film on the back electrode side of an organic electroluminescent element, and the polymerization and film formation proceed without breaking vacuum. This is a method that can suppress contact with moisture. According to this thermal CVD method, the temperature of the organic electroluminescent element at the time of film formation can be suppressed to about room temperature, and the film can be formed without adversely affecting the light emission characteristics.

【0023】なお、前記の発光層、正孔注入層、正孔注
入輸送層、電子注入層、電子注入輸送層の各有機層の耐
熱性を上げるために、各層を構成する有機化合物に重合
性置換基を導入し、製膜前、製膜中又は製膜後に高分子
化させてもよい。
In order to increase the heat resistance of each of the light emitting layer, the hole injection layer, the hole injection / transport layer, the electron injection layer, and the electron injection / transport layer, the organic compound constituting each layer is polymerizable. A substituent may be introduced to polymerize before, during or after film formation.

【0024】次に、本発明の多重型多色発光有機電界発
光素子の具体的構成例を図2に基づいて説明する。図2
は、二重型二色発光有機電界発光素子(以下、二重有機
電界発光素子ともいう)の一例を示す側面断面図であ
る。透明基板11の上に透光性電極12aと、正孔注入
輸送層12b、正孔輸送層12c及び発光層兼電子注入
輸送層12d(図中、12b〜12dで示す)と背面電
極12eとで構成された第1素子層Aが積層され、発光
層兼電子注入輸送層12dの上にポリモノクロロパラキ
シリレン層間絶縁膜13a及びポリパラキシリレン層間
絶縁膜13bが積層され、更にその上に透光性電極12
a’と、正孔注入輸送層12b’、正孔輸送層12c’
及び発光層兼電子注入輸送層12d’(図中、12b’
〜12d’で示す)と背面電極12e’とで構成された
第2素子層Bが積層されて、二重有機電界発光素子を形
成する。なお、上記の具体的構成例には、二重有機電界
発光素子の例を示したが、三重以上の多重型多色発光有
機電界発光素子であってもよく、また層間絶縁膜が一層
のみでもよく、三層以上の多層であってもよく、さらに
他のポリパラキシリレン系高分子化合物を用いたもので
あってもよい。
Next, a specific configuration example of the multiplex type multicolor light emitting organic electroluminescent device of the present invention will be described with reference to FIG. FIG.
FIG. 1 is a side cross-sectional view illustrating an example of a double type two-color light emitting organic electroluminescent device (hereinafter, also referred to as a double organic electroluminescent device). A transparent electrode 12a, a hole injecting and transporting layer 12b, a hole transporting layer 12c, a light emitting layer and electron injecting and transporting layer 12d (indicated by 12b to 12d in the figure) and a back electrode 12e are formed on a transparent substrate 11. The first element layer A thus formed is stacked, a polymonochloroparaxylylene interlayer insulating film 13a and a polyparaxylylene interlayer insulating film 13b are stacked on the light emitting layer / electron injection / transport layer 12d, and a transparent layer is further formed thereon. Light electrode 12
a ′, the hole injection / transport layer 12b ′, and the hole transport layer 12c ′
And a light emitting layer / electron injection / transport layer 12d '(12b' in the figure).
To 12d ') and the back electrode 12e' are stacked to form a double organic electroluminescent device. Note that, in the above specific configuration example, an example of a double organic electroluminescent element has been described, but a triple or more multiplex type multicolor organic electroluminescent element may be used, or the interlayer insulating film may have only one layer. It may have a multi-layer structure of three or more layers, or may use another polyparaxylylene-based polymer compound.

【0025】[0025]

【実施例】以下、実施例及び比較例に基づいて、本発明
を具体的に説明する。
The present invention will be specifically described below based on examples and comparative examples.

【0026】実施例1 以下の方法により、図2に示す二重有機電界発光素子を
製作した。まず、透明基板11としてガラス基板を用
い、この上に透光性電極12aとして電子ビーム蒸着法
によりITOを積層した抵抗率15Ω/□及び電極面積
2mm×2mmのITO付ガラス基板(ミクロ技研製)を用
いた。ターボ分子ポンプによる真空蒸着装置と昇華金属
用のモリブデンボード抵抗加熱方式により、蒸着速度を
アルバック製の水晶振動子型膜厚コントローラーで制御
しながら、蒸着中の真空度2〜3×10-7torrで上記I
TO付ガラス基板のITO層の上に、有機薄膜群(正孔
注入輸送層12b、正孔輸送層12c、発光色素にクマ
リンを用いた発光層兼電子注入輸送層12d)を積層
し、更にその上に真空蒸着法によりアルミニウムとリチ
ウムの合金を積層して背面電極12eを設け、第1素子
層Aを構成した。
Example 1 A double organic electroluminescent device shown in FIG. 2 was manufactured by the following method. First, a glass substrate was used as the transparent substrate 11, and ITO was laminated thereon as the translucent electrode 12a by electron beam evaporation. A glass substrate with ITO having a resistivity of 15Ω / □ and an electrode area of 2 mm × 2 mm (manufactured by Micro Giken) Was used. With a vacuum evaporation system using a turbo molecular pump and a molybdenum board resistance heating system for sublimation metal, the degree of vacuum during evaporation is controlled at 2-3 × 10 -7 torr while controlling the evaporation rate with a quartz crystal type thickness controller made by ULVAC. The above I
On the ITO layer of the glass substrate with TO, an organic thin film group (a hole injection / transport layer 12b, a hole transport layer 12c, a light-emitting layer / electron injection / transport layer 12 using coumarin as a light-emitting dye) is laminated, and furthermore, An aluminum-lithium alloy was laminated thereon by a vacuum evaporation method to provide a back electrode 12e, thereby forming a first element layer A.

【0027】次に、第1素子層Aの背面電極12e側の
表面にポリモノクロロパラキシリレン層間絶縁膜13a
を熱CVD法により1μmの厚さで積層し、更にその上
にポリパラキシリレン層間絶縁膜13bを熱CVD法に
より0.3μmの厚さで積層して2種類のポリパラキシ
リレン系高分子化合物による2層の層間絶縁膜を形成し
た。
Next, a polymonochloroparaxylylene interlayer insulating film 13a is formed on the surface of the first element layer A on the side of the back electrode 12e.
Are laminated at a thickness of 1 μm by thermal CVD, and a polyparaxylylene interlayer insulating film 13b is laminated thereon at a thickness of 0.3 μm by thermal CVD to form two types of polyparaxylylene-based polymers. A two-layered interlayer insulating film made of a compound was formed.

【0028】更に、この層間絶縁膜13bの表面に透光
性電極12a’として金を蒸着し、発光色素にDCMを
用いた以外は、第1素子層Aと全く同様の方法で第2素
子層Bを構成することによって、二重有機電界発光素子
を製作した。
Further, the second element layer is formed in exactly the same manner as the first element layer A except that gold is vapor-deposited on the surface of the interlayer insulating film 13b as the light-transmitting electrode 12a 'and DCM is used as a luminescent dye. By constructing B, a double organic electroluminescent device was manufactured.

【0029】このようにして製作した二重有機電界発光
素子の各々の素子に10Vの電圧を印加したところ、両
素子間の電気的相互作用は全くなく、独立に橙色と緑色
の光が放射された。この発光スペクトルを浜松ホトニク
ス社製Phtonic Multi−Channel
Analyzer−10(PMA−10)により測定し
た。図3に発光スペクトルのグラフを示す。
When a voltage of 10 V was applied to each of the thus manufactured dual organic electroluminescent elements, there was no electrical interaction between the two elements, and orange and green light were independently emitted. Was. This emission spectrum was measured using a photonic multi-channel manufactured by Hamamatsu Photonics.
It was measured by Analyzer-10 (PMA-10). FIG. 3 shows a graph of the emission spectrum.

【0030】実施例2 第2素子Bの透光性電極12a’をスパッタリング法に
よるITO電極とした以外は、実施例1と全く同様の方
法で二重有機電界発光素子を製作した。このようにして
製作した二重有機電界発光素子の各々の素子に10Vの
電圧を印加したところ、両素子間の電気的相互作用は全
くなく、独立に橙色と緑色の光が放射された。
Example 2 A double organic electroluminescent device was manufactured in exactly the same manner as in Example 1 except that the light-transmitting electrode 12a 'of the second device B was changed to an ITO electrode by a sputtering method. When a voltage of 10 V was applied to each of the dual organic electroluminescent devices manufactured in this manner, there was no electrical interaction between the two devices, and orange and green light were independently emitted.

【0031】比較例1 実施例1と同様にして二重有機電界発光素子を製作した
が、ポリパラキシリレン系高分子化合物からなる層間絶
縁膜13a及び13bを形成することなく、第1素子層
Aの表面にスッパッタリング法によるITO陽極電極を
形成して、二重有機電界発光素子とした。このようにし
て製作した二重有機電界発光素子の各々の素子に10V
の電圧を印加したところ、一時的に橙色の発光が確認さ
れたが、第1層発光素子Aからは全く発光が確認されな
かった。また、一時的に発光した橙色の光はその後消失
した。
COMPARATIVE EXAMPLE 1 A double organic electroluminescent device was manufactured in the same manner as in Example 1, but without forming the interlayer insulating films 13a and 13b made of a polyparaxylylene-based polymer compound, the first device layer was formed. An ITO anode electrode was formed on the surface of A by a sputtering method to obtain a double organic electroluminescent device. 10V is applied to each of the dual organic electroluminescent devices manufactured in this manner.
When the voltage was applied, orange light emission was temporarily confirmed, but no light emission was confirmed from the first layer light emitting element A at all. Further, the orange light temporarily emitted disappeared thereafter.

【0032】[0032]

【発明の効果】本発明によれば、各層の発光層に使用す
る発光色素に異なる化合物を用い、かつ発光素子層と発
光素子層との間に層間絶縁膜を形成することにより、異
なる色を安定的に発光させることができる多重型多色発
光有機電界発光素子を製作することができた。
According to the present invention, different colors can be obtained by using different compounds for the luminescent dyes used in the luminescent layers of each layer and forming an interlayer insulating film between the luminescent element layers. A multiplex type multicolor organic electroluminescent device capable of stably emitting light was manufactured.

【図面の簡単な説明】[Brief description of the drawings]

【図1】本発明の多重型多色発光有機電界発光素子の基
本概念の一例を示す側面断面図である。
FIG. 1 is a side sectional view showing an example of a basic concept of a multiplex type multicolor light emitting organic electroluminescent device of the present invention.

【図2】本発明の多重型多色発光有機電界発光素子の具
体的構成例を示す側面断面図である。
FIG. 2 is a side sectional view showing a specific configuration example of a multiplex type multicolor light emitting organic electroluminescent device of the present invention.

【図3】実施例1の二重型二色発光有機電界発光素子の
発光スペクトルを示すグラフである。
FIG. 3 is a graph showing an emission spectrum of the double-type two-color organic electroluminescent device of Example 1.

【符号の説明】[Explanation of symbols]

1 透明基板 2、2’ 透光性電極 3、3’ 発光層 4、4’ 背面電極 5 層間絶縁膜 A 第1素子層 B 第2素子層 11 透明基板 12a、12a’ 透光性電極 12b、12b’ 正孔注入輸送層 12c、12c’ 正孔輸送層 12d、12d’ 発光層兼電子注入輸送層 12e、12e’ 背面電極 13a、13a’ ポリモノクロロパラキシリレン層
間絶縁膜 13b、13b’ ポリパラキシリレン層間絶縁膜
DESCRIPTION OF SYMBOLS 1 Transparent substrate 2, 2 'translucent electrode 3, 3' light emitting layer 4, 4 'back electrode 5 Interlayer insulating film A 1st element layer B 2nd element layer 11 Transparent substrate 12a, 12a' Translucent electrode 12b, 12b ′ hole injection / transport layer 12c, 12c ′ hole transport layer 12d, 12d ′ light emitting layer / electron injection / transport layer 12e, 12e ′ back electrode 13a, 13a ′ polymonochloroparaxylylene interlayer insulating film 13b, 13b ′ polypara Xylylene interlayer insulating film

フロントページの続き (72)発明者 森 竜雄 愛知県名古屋市中川区西日置1−5−6 (72)発明者 水谷 照吉 愛知県名古屋市千種区北千種2−1−43Continued on the front page (72) Inventor Tatsuo Mori 1-5-6, Nishihioki, Nakagawa-ku, Nagoya-shi, Aichi Prefecture

Claims (2)

【特許請求の範囲】[Claims] 【請求項1】 透明基板上に透光性電極、有機蛍光性物
質を含有する発光層及び背面電極を順次積層してなる有
機電界発光素子において、発光色の異なる少なくとも2
層の発光層を有し、かつ背面電極と透光性電極との間に
層間絶縁膜を有することを特徴とする多重型多色発光有
機電界発光素子。
An organic electroluminescent device comprising a transparent substrate, a light-transmitting electrode, a light-emitting layer containing an organic fluorescent substance, and a back electrode sequentially laminated on a transparent substrate.
1. A multiplex type multicolor light-emitting organic electroluminescent device, comprising: a light-emitting layer; and an interlayer insulating film between the back electrode and the translucent electrode.
【請求項2】 層間絶縁膜が、ポリパラキシリレン、ポ
リモノクロロパラキシリレン、ポリモノブロムパラキシ
リレン、ポリシアノパラキシリレン、ポリジクロロパラ
キシリレン、ポリメチルパラキシリレン又はポリエチル
パラキシリレンから選ばれた少なくとも1種のポリパラ
キシリレン系高分子化合物を1層又は2層以上積層して
なる請求項1記載の多重型多色発光有機電界発光素子。
2. The method according to claim 1, wherein the interlayer insulating film is made of polyparaxylylene, polymonochloroparaxylylene, polymonobromoparaxylylene, polycyanoparaxylylene, polydichloroparaxylylene, polymethylparaxylylene or polyethylparaxylylene. 2. The multiplex type multicolor light emitting organic electroluminescent device according to claim 1, wherein one or more layers of at least one kind of polyparaxylylene-based polymer selected from len are laminated.
JP26450497A 1997-09-29 1997-09-29 Multiple-type multicolor organic electroluminescence device Expired - Fee Related JP3887079B2 (en)

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WO2018083974A1 (en) * 2016-11-04 2018-05-11 コニカミノルタ株式会社 Organic electroluminescent element and light emitting device

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