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JP2007115645A - Organic light emitting element and its manufacturing method - Google Patents

Organic light emitting element and its manufacturing method Download PDF

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JP2007115645A
JP2007115645A JP2005341222A JP2005341222A JP2007115645A JP 2007115645 A JP2007115645 A JP 2007115645A JP 2005341222 A JP2005341222 A JP 2005341222A JP 2005341222 A JP2005341222 A JP 2005341222A JP 2007115645 A JP2007115645 A JP 2007115645A
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JP4769068B2 (en
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Nobuhiro Ide
伸弘 井出
Takuya Komoda
卓哉 菰田
Junji Kido
淳二 城戸
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Panasonic Electric Works Co Ltd
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Matsushita Electric Works Ltd
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Abstract

<P>PROBLEM TO BE SOLVED: To provide an organic light emitting element capable of materializing high quality luminescence showing luminescence with a desired color tone without relying on angles since angle dependency of emission spectrum is not much, and also capable of adjusting the color tone. <P>SOLUTION: This organic light emitting element is formed by laminating a first light emitting part 4 formed by providing a luminescent layer 3 between a pair of electrodes 1, 2 and a second light emitting part 8 formed by providing a luminescent layer 7 between a pair of electrodes 5, 6. Among those four electrodes, one of the electrodes positioned on the outside is an electrode having light reflectivity, and all others electrodes are light-transmissive, and a light transmissive insulating layer 9 having such a thickness that light emitted in the luminescent layer 2 of the light emitting part 4 on the side having no light reflective electrode causes no interference and making light emitted in the luminescent layer 3 scatter is provided between the first light emitting part 4 and the second light emitting part 8. <P>COPYRIGHT: (C)2007,JPO&INPIT

Description

本発明は、フラットディスプレイパネル、液晶表示機用バックライト、照明用光源等に用いられる有機発光素子及びその製造方法に関するものである。   The present invention relates to an organic light-emitting device used for a flat display panel, a backlight for a liquid crystal display, a light source for illumination, and the like, and a method for manufacturing the same.

有機エレクトロルミネッセンス素子(有機EL素子)と称される有機発光素子は、陽極となる透明電極、ホール輸送層、有機発光層、電子注入層、陰極となる電極の順に、透明基板の片側の表面に積層した構成のものが、その一例として知られている。そして陽極と陰極の間に電圧を印加することによって、電子注入層を介して発光層に注入された電子と、ホール輸送層を介して発光層に注入されたホールとが、発光層内で再結合し、励起状態が生成して発光が起こり、発光層で発光したこの光は透明電極及び透明基板を通して取り出されるようになっている。   An organic light-emitting device called an organic electroluminescence device (organic EL device) is formed on the surface of one side of a transparent substrate in the order of a transparent electrode serving as an anode, a hole transport layer, an organic light-emitting layer, an electron injection layer, and an electrode serving as a cathode. A laminated structure is known as an example. By applying a voltage between the anode and the cathode, electrons injected into the light emitting layer through the electron injection layer and holes injected into the light emitting layer through the hole transport layer are regenerated in the light emitting layer. As a result, the excited state is generated to emit light, and the light emitted from the light emitting layer is extracted through the transparent electrode and the transparent substrate.

有機発光素子は、自発光であること、比較的高効率の発光特性を示すこと、各種の色調で発光可能であること等の特徴を有するものであり、表示装置、例えばフラットパネルディスプレイ等の発光体として、あるいは光源、例えば液晶表示機用バックライトや照明としての活用が期待されており、一部ではすでに実用化されている。しかし、有機発光素子は、その輝度と寿命とがトレードオフの関係にあり、より鮮明な画像、あるいは明るい照明光を得るために輝度を増大させると、寿命が短くなるという性質を有する。   Organic light-emitting elements are characterized by being self-luminous, exhibiting relatively high-efficiency light-emitting characteristics, and capable of emitting light in various colors, and can emit light from display devices such as flat panel displays. It is expected to be used as a body or as a light source, for example, a backlight for a liquid crystal display or illumination, and a part thereof has already been put into practical use. However, the organic light emitting element has a trade-off relationship between the luminance and the lifetime, and has a property that the lifetime is shortened when the luminance is increased in order to obtain a clearer image or bright illumination light.

この問題を解決するものとして、近年、陽極と陰極の間に発光層を複数備え、かつ各発光層間に等電位面を形成する層、もしくは電荷発生層を設けるようにした有機発光素子が提案されている(例えば、特許文献1参照)。   In order to solve this problem, in recent years, an organic light-emitting device has been proposed in which a plurality of light-emitting layers are provided between an anode and a cathode, and a layer for forming an equipotential surface between each light-emitting layer or a charge generation layer is provided. (For example, refer to Patent Document 1).

図16はこのような有機発光素子の構造の一例を示すものであり、陽極となる電極20と陰極となる電極21の間に複数の発光層22を、隣接する発光層22の間に等電位面を形成する層もしくは電荷発生層23を介在させた状態で積層し、これを透明基板24の表面に積層したものであり、電極20は光透過性の電極として、電極21は光反射性の電極として形成してある。尚、図16において、発光層22の両側にはホール輸送層と電子注入層が設けられているが、ホール輸送層と電子注入層の図示は省略してある。そしてこのように複数層の発光層22を等電位面形成層もしくは電荷発生層23で仕切ることによって、電極20,21間に電圧を印加したとき、複数の発光層22があたかも直列的に接続された状態で同時に発光し、各発光層22からの光が合算されるため、一定電流通電時には従来型の有機発光素子よりも高輝度で発光させることができ、上記のような輝度−寿命のトレードオフを回避することが可能になるものである。   FIG. 16 shows an example of the structure of such an organic light-emitting element. A plurality of light-emitting layers 22 are provided between an electrode 20 serving as an anode and an electrode 21 serving as a cathode, and an equipotential is provided between adjacent light-emitting layers 22. A layer that forms a surface or a charge generation layer 23 is laminated, and this is laminated on the surface of the transparent substrate 24. The electrode 20 is a light-transmissive electrode, and the electrode 21 is a light-reflective electrode. It is formed as an electrode. In FIG. 16, a hole transport layer and an electron injection layer are provided on both sides of the light emitting layer 22, but the hole transport layer and the electron injection layer are not shown. By dividing the plurality of light emitting layers 22 by the equipotential surface forming layer or the charge generation layer 23 in this way, when a voltage is applied between the electrodes 20 and 21, the plurality of light emitting layers 22 are connected in series. In this state, the light is emitted simultaneously and the light from each light emitting layer 22 is added. Therefore, when a constant current is applied, the light can be emitted with higher brightness than the conventional organic light emitting element, and the brightness-lifetime trade-off as described above can be achieved. It is possible to avoid turning off.

しかしながら、有機発光素子において知られている、発光輝度、発光スペクトルの視野角依存性、膜厚依存性、及び光利用効率の低下等の問題は、有機発光素子が光学波長オーダーの膜厚を有する薄膜デバイスであることや、素子内に屈折率段差もしくは金属面等からなる反射面を有することや、高屈折率媒体中で光が発生することなどに由来する、光干渉効果、全反射による有機膜の発光層、基板、電極等の高屈折率媒体内への光閉じ込めなどの現象によるものであるため、上記のような複数の発光層を備える有機発光素子では、これらの問題がより顕著に発生することになる。   However, problems such as emission luminance, viewing angle dependency of the emission spectrum, film thickness dependency, and decrease in light utilization efficiency, which are known in organic light emitting elements, have a film thickness on the order of optical wavelength. Optical interference effect, organic due to total reflection, derived from being a thin film device, having a reflective surface consisting of a refractive index step or a metal surface in the element, and generating light in a high refractive index medium These problems are more conspicuous in organic light-emitting devices having a plurality of light-emitting layers as described above, due to phenomena such as light confinement in a high-refractive index medium such as a light-emitting layer, a substrate, and an electrode. Will occur.

光干渉効果は、それを適切に利用すれば、色純度の向上、指向性の制御等を実現することが可能であり、特にフラットパネルディスプレイ等の用途に有用である。例えば引用文献2には、発光層−光反射性の電極間の光学距離を1/4波長の奇数倍に調整することや、発光位置−最大屈折率段差位置間の光学距離を1/4波長の偶数倍に調整することで、この波長を強調することが可能であることが記載されており、特に発光層−光反射性の電極間の光学距離が発光スペクトルに与える影響が大きいことが知られている。さらに特許文献3には、複数の発光層のそれぞれの発光位置から光反射性の電極までの光学膜厚をすべて1/4波長の奇数倍にすることで、最も高効率の発光が得られると共に、発光スペクトル形状が細くなることが記載されている。   If the light interference effect is appropriately used, it is possible to improve color purity, control directivity, etc., and is particularly useful for applications such as flat panel displays. For example, in cited document 2, the optical distance between the light emitting layer and the light reflective electrode is adjusted to an odd multiple of 1/4 wavelength, or the optical distance between the light emitting position and the maximum refractive index step position is set to 1/4 wavelength. It is described that it is possible to emphasize this wavelength by adjusting to an even number of times, and it is known that the optical distance between the light emitting layer and the light reflective electrode has a great influence on the light emission spectrum. It has been. Further, Patent Document 3 discloses that the most efficient light emission can be obtained by making all the optical film thicknesses from the respective light emitting positions of the plurality of light emitting layers to the light reflective electrodes an odd multiple of 1/4 wavelength. It is described that the emission spectrum shape becomes narrower.

しかし、上記のように発光層−光反射性の電極間の光学距離や、発光層−最大屈折率段差位置間の光学距離、つまり素子の膜厚の最適化によって色純度等の適正化を行なった有機発光素子では、膜厚が変化した際の発光輝度や発光色の変動が大きくなる。これはすなわち、有機発光素子の製造時の膜厚許容性が狭くなることを意味するものであり、生産性の問題に直結するものである。特に複数の発光層や等電位面形成層もしくは電荷発生層などを積層した構造の上記のような有機発光素子では、いずれかの層の光学特性のずれ(膜厚・屈折率の異常)が他の層の光学位置にさえも影響を及ぼすため、膜厚制御の精度や必然性がさらに増大することになる。   However, as described above, the optical distance between the light-emitting layer and the light-reflective electrode, the optical distance between the light-emitting layer and the maximum refractive index step position, that is, the color purity is optimized by optimizing the film thickness of the element. In the organic light-emitting element, fluctuations in emission luminance and emission color when the film thickness changes are large. This means that the film thickness tolerance at the time of manufacturing the organic light emitting device is narrowed, which directly leads to the problem of productivity. In particular, in the above organic light emitting device having a structure in which a plurality of light emitting layers, equipotential surface forming layers, or charge generation layers are laminated, the optical characteristic deviation (abnormal film thickness / refractive index) of any of the layers is other. Even the optical position of this layer is affected, so that the accuracy and necessity of film thickness control is further increased.

さらに上記の特許文献3のものでは、発光層−光反射性の電極間の光学距離を1/4波長の奇数(2n+1)[n=0,1,2…]倍に設定することが効率の観点で好ましいとされているが、実際にはnの値が大きくなるに伴なって、輝度やスペクトルの角度依存性が大きくなるという問題が新たに生じる。すなわち、発光層を一層のみ有する有機発光素子では、概ねn=0に相当する光学長で膜厚設計がなされることが多いために、膜厚変化に対する発光輝度、発光色の変動は必ずしも大きくないが、上記のような複数層の発光層を備える有機発光素子においては、各発光層が1/4波長の(2n+1)[n=0,1,2…]倍の位置に必然的に位置するため、層数の増大に伴なって特定の波長がより顕著に強調され、発光層が本来有するスペクトルとは大きく異なる発光スペクトルを与えると同時に角度依存性が大きくなる問題を有するものである。よって、上記のような複数層の発光層を備える有機発光素子は、確かに従来型の有機発光素子では実現不可能であった高い電流効率、量子効率を実現することができるが、その発光スペクトル及び視野角依存性に関しては必ずしも好ましい特性を有するものではない。   Further, in the above-mentioned Patent Document 3, it is efficient to set the optical distance between the light emitting layer and the light reflective electrode to an odd number (2n + 1) [n = 0, 1, 2,. Although it is preferable from the viewpoint, in reality, as the value of n increases, there arises a new problem that the angle dependency of luminance and spectrum increases. That is, in an organic light emitting device having only one light emitting layer, the film thickness is often designed with an optical length corresponding to n = 0 in many cases, and therefore, variations in light emission luminance and light emission color with respect to film thickness change are not necessarily large. However, in an organic light emitting device having a plurality of light emitting layers as described above, each light emitting layer is necessarily located at a position (2n + 1) [n = 0, 1, 2,. Therefore, as the number of layers increases, a specific wavelength is more remarkably emphasized, and an emission spectrum that is significantly different from the spectrum originally possessed by the light emitting layer is given, and at the same time, the angle dependency is increased. Therefore, an organic light emitting device having a plurality of light emitting layers as described above can surely achieve high current efficiency and quantum efficiency that cannot be achieved by conventional organic light emitting devices, but its emission spectrum. In addition, the viewing angle dependency does not necessarily have preferable characteristics.

一方、前記の図16の構造を有する有機発光素子は、複数の各発光層が直列接続されているため、各発光層に供給される電流値は常に同一であり、各発光層の発光色を駆動時に個別にコントロールすることは実質的に不可能である。有機発光素子を製造する際に、所定の発光色を呈するように各発光層を選定して設計することで、各発光層が種々の発光色で発光する有機発光素子を得ることは可能であるが、一度発光色が決まったものを変えることはできない。また例えばRGBそれぞれの発光色を呈する複数の発光層を積層した場合には、その発光色の合算によって白色発光を得ることが可能であるが、各発光色を呈する発光層の輝度に対する発光特性挙動が異なる場合、各輝度における発光色が変化することになるという問題が生じる。さらに複数の各発光層の寿命が異なる場合、駆動に伴って、先に劣化した発光層からの発光色が減少するため、色ずれを生じるという問題もある。例えば有機発光素子をディスプレイの発光光源として用いた場合には、表示される発光色の色バランスが狂い、また照明の光源として用いた場合には、劣化が色ずれとして視認されるために好ましくない。   On the other hand, in the organic light emitting device having the structure shown in FIG. 16, since a plurality of light emitting layers are connected in series, the current value supplied to each light emitting layer is always the same, and the light emission color of each light emitting layer is changed. Individual control during driving is virtually impossible. When manufacturing an organic light emitting device, it is possible to obtain an organic light emitting device in which each light emitting layer emits light in various light emission colors by selecting and designing each light emitting layer so as to exhibit a predetermined light emitting color. However, once the emission color is determined, it cannot be changed. In addition, for example, when a plurality of light emitting layers exhibiting RGB emission colors are stacked, white light emission can be obtained by adding the light emission colors, but the light emission characteristic behavior with respect to the luminance of the light emitting layer exhibiting each light emission color If they are different, there arises a problem that the emission color at each luminance changes. Further, when the life of each of the plurality of light emitting layers is different, the emission color from the previously deteriorated light emitting layer decreases with driving, which causes a problem of color shift. For example, when an organic light emitting element is used as a light emission source of a display, the color balance of the displayed emission color is out of order, and when used as a light source of illumination, deterioration is visually recognized as a color shift, which is not preferable. .

また、特許文献4には、電極を有する発光層を複数積層した積層型有機発光素子が提案されている。この有機発光素子は、独立したもしくは一部を共通とした電極を備える複数の発光層を、必要に応じて絶縁層を介して積層したものであり、ディスプレイ用途に使用可能であるとされている。しかしこの構造の有機発光素子においても、発光層間の距離は、例え絶縁層が挿入されている場合にも小さいものであり、前記の光干渉の問題を回避することはできない。事実、光干渉があることを前提に、この特許文献4では、各発光層の位置をその発光波長に基づいて設定し、高色純度で発光する素子設計方針が提案されている。この提案内容は干渉設計を利用したものであり、その要点は前記の特許文献2の場合と同様に、発光層と光反射層との間の距離を所定の波長の光を強調する膜厚とすることであるため、発光波長の角度依存性の問題は依然として存在している。このように、この特許文献4の構造の有機発光素子は、駆動時に発光色を変更することが可能であるものの、それ以外の問題、特に発光層の積層数が増大した際の発光色の角度依存性に対する問題が解決されたものではない。
特開平11−329748号公報 特開2000−323277号公報 特開2003−272860号公報 特表2001−511296号公報
Patent Document 4 proposes a stacked organic light emitting device in which a plurality of light emitting layers having electrodes are stacked. This organic light-emitting element is formed by laminating a plurality of light-emitting layers having independent or partly shared electrodes through an insulating layer as necessary, and is said to be usable for display applications. . However, even in the organic light emitting device having this structure, the distance between the light emitting layers is small even when an insulating layer is inserted, and the above-described problem of optical interference cannot be avoided. In fact, on the premise that there is optical interference, Patent Document 4 proposes an element design policy in which the position of each light emitting layer is set based on the light emission wavelength to emit light with high color purity. This proposal uses interference design, and the main point is that, as in the case of Patent Document 2, the distance between the light emitting layer and the light reflecting layer is set to a film thickness that emphasizes light of a predetermined wavelength. Therefore, the problem of the angle dependence of the emission wavelength still exists. As described above, the organic light emitting device having the structure of Patent Document 4 can change the light emission color during driving, but other problems, in particular, the angle of the light emission color when the number of stacked light emitting layers is increased. The dependency problem is not solved.
Japanese Patent Laid-Open No. 11-329748 JP 2000-323277 A JP 2003-272860 A JP 2001-511296 A

本発明は上記の点に鑑みてなされたものであり、発光スペクトルの角度依存性が小さく、角度によらず所望の色調の発光を示す高品位発光を実現することができると共に、色調の調整が可能な有機発光素子を提供することを目的とするものである。   The present invention has been made in view of the above points, and the angle dependency of the emission spectrum is small, and high-quality light emission that exhibits light emission of a desired color tone can be realized regardless of the angle, and the color tone can be adjusted. An object of the present invention is to provide a possible organic light emitting device.

本発明の請求項1に係る有機発光素子は、一対の電極の間に発光層を備えて形成される第1の発光部と、一対の電極の間に発光層を備えて形成される第2の発光部とを積層して形成される有機発光素子であって、上記の4つの電極のうち、外側に位置する電極の一方が光反射性を有する電極であると共に、他の総ての電極は光透過性であり、且つ、第1の発光部と第2の発光部の間に、光反射性の電極を有しない側の発光部の発光層で発光した光が干渉を起こさない厚みの、あるいは、この発光層で発光した光を散乱させる、光透過性の絶縁層を備えて成ることを特徴とするものである。   The organic light-emitting device according to claim 1 of the present invention includes a first light-emitting portion formed with a light-emitting layer between a pair of electrodes, and a second light-emitting layer formed with a light-emitting layer between a pair of electrodes. An organic light-emitting element formed by laminating the light-emitting portion of the above-mentioned four electrodes, and one of the four electrodes located on the outside is a light-reflective electrode, and all the other electrodes Is light transmissive and has a thickness between the first light emitting part and the second light emitting part so that the light emitted from the light emitting layer of the light emitting part on the side having no light reflective electrode does not cause interference. Alternatively, a light-transmitting insulating layer that scatters light emitted from the light-emitting layer is provided.

本発明の請求項2に係る有機発光素子は、一対の電極の間に発光層を備えて形成される第1の発光部と、一対の電極の間に発光層を備えて形成される第2の発光部とを積層して形成される有機発光素子であって、上記の4つの総ての電極が光透過性であると共に、外側に位置する電極のうち一方の電極の外側に光反射性を有する光反射層を有し、且つ、第1の発光部と第2の発光部の間に、光反射層を有しない側の発光部の発光層で発光した光が干渉を起こさない厚みの、あるいは、この発光層で発光した光を散乱させる、光透過性の絶縁層を備えて成ることを特徴とするものである。   An organic light-emitting device according to claim 2 of the present invention includes a first light-emitting portion formed with a light-emitting layer between a pair of electrodes, and a second light-emitting layer formed with a light-emitting layer between a pair of electrodes. An organic light emitting device formed by laminating a light emitting portion of the above, wherein all the four electrodes described above are light transmissive and light reflective on the outside of one of the electrodes located outside. And a thickness of light emitted from the light emitting layer of the light emitting portion on the side not having the light reflecting layer between the first light emitting portion and the second light emitting portion. Alternatively, a light-transmitting insulating layer that scatters light emitted from the light-emitting layer is provided.

本発明の請求項3に係る有機発光素子は、一対の電極の間に発光層を備えて形成される第1の発光部と、一対の電極の間に発光層を備えて形成される第2の発光部とを積層して形成される有機発光素子であって、上記の4つの総ての電極が光透過性であり、且つ、外側に位置する電極のうち一方の電極の外側に、第1及び第2の発光部の発光層で発光した光が干渉を起こさない厚みの、あるいは、これらの発光層で発光した光を散乱させる、光透過性の絶縁層を介して、光反射性を有する光反射層を備えて成ることを特徴とするものである。   An organic light-emitting device according to claim 3 of the present invention is a first light-emitting portion formed with a light-emitting layer between a pair of electrodes, and a second light-emitting layer formed with a light-emitting layer between a pair of electrodes. An organic light-emitting element formed by laminating a light-emitting portion of the above-mentioned light-emitting section, wherein all the four electrodes are light-transmitting, and the first electrode out of one of the electrodes located outside is The light emitted from the light emitting layers of the first and second light emitting portions has a thickness that does not cause interference, or the light emitted from these light emitting layers is scattered through a light-transmitting insulating layer. The light reflecting layer is provided.

また請求項4の発明は、請求項1乃至3のいずれかにおいて、第1及び第2の発光部のうち少なくとも一方が、等電位面を形成する層もしくは電荷発生層を介して積層される複数の発光層を、電極間に備えて形成されていることを特徴とするものである。   According to a fourth aspect of the present invention, in any one of the first to third aspects, at least one of the first and second light emitting portions is a plurality of layers stacked via a layer forming an equipotential surface or a charge generation layer. The light emitting layer is provided between the electrodes.

また請求項5の発明は、請求項1乃至4のいずれかにおいて、発光層で発光した光が干渉を起こさない厚みの光透過性の絶縁層、発光層で発光した光を散乱させる光透過性の絶縁層が、ガラス板もしくはフィルムで形成されていることを特徴とするものである。   According to a fifth aspect of the present invention, in any one of the first to fourth aspects, the light-transmitting insulating layer has a thickness that prevents light emitted from the light-emitting layer from interfering, and the light-transmitting property that scatters the light emitted from the light-emitting layer. The insulating layer is formed of a glass plate or a film.

本発明の請求項6に係る有機発光素子の製造方法は、請求項1乃至5のいずれかに記載の有機発光素子を製造するにあたって、発光層で発光した光が干渉を起こさない厚みの、あるいは、発光層で発光した光を散乱させる、第1の光透過性基板の表面に、電極、発光層、電極をこの順に積層して第1と第2のいずれか一方の発光部を形成する工程と、第2の光透過性基板の表面に、電極、発光層、電極をこの順に積層して第1と第2のいずれか他方の発光部を形成する工程と、第1の光透過性基板に、第2の光透過性基板に形成した発光部を積層することによって、2つの発光部を第1の光透過性基板を介して積層する工程と、を備えることを特徴とするものである。   According to a sixth aspect of the present invention, there is provided a method for manufacturing an organic light-emitting device according to any one of the first to fifth aspects, wherein the light emitted from the light-emitting layer has a thickness that does not cause interference. The step of scattering the light emitted from the light emitting layer and forming the first or second light emitting portion by laminating the electrode, the light emitting layer, and the electrode in this order on the surface of the first light transmitting substrate A step of laminating an electrode, a light emitting layer, and an electrode in this order on the surface of the second light transmissive substrate to form one of the first and second light emitting portions, and the first light transmissive substrate. And a step of laminating the two light emitting portions through the first light transmissive substrate by laminating the light emitting portions formed on the second light transmissive substrate. .

本発明の請求項7に係る有機発光素子の製造方法は、請求項1乃至5のいずれかに記載の有機発光素子を製造するにあたって、発光層で発光した光が干渉を起こさない厚みの、あるいは、発光層で発光した光を散乱させる、光透過性基板の表面に、電極、発光層、電極をこの順に積層して第1と第2のいずれか一方の発光部を形成する工程と、上記光透過性基板の発光部を形成した反対側の表面に、電極、発光層、電極をこの順に積層して第1と第2のいずれか他方の発光部を形成する工程と、を備えることを特徴とするものである。   According to a seventh aspect of the present invention, there is provided a method for manufacturing an organic light emitting device according to any one of the first to fifth aspects, wherein the light emitted from the light emitting layer has a thickness that does not cause interference, or A step of scattering the light emitted from the light emitting layer, forming a first light emitting portion and a first light emitting portion by laminating an electrode, a light emitting layer, and an electrode in this order on the surface of the light-transmitting substrate; A step of laminating an electrode, a light emitting layer, and an electrode in this order on the opposite surface of the light transmissive substrate on which the light emitting part is formed, to form either the first or second light emitting part. It is a feature.

発光層で発光した光が干渉を起こさない厚みの、あるいは、これらの発光層で発光した光を散乱させる、光透過性の絶縁層を有するので、発光スペクトルの角度依存性が小さく、角度によらず所望の色調の発光を示す高品位発光を実現することができるものである。また、第1の発光部と第2の発光部の間に光透過性の絶縁層を有することによって、両発光部を電気的に切り離すことができ、各発光部を独立して駆動することができるものであり、必要に応じて各発光部の発光特性を変化させることができ、色調の調整が可能な有機発光素子を得ることができるものである。   The light emission layer has a thickness that does not cause interference, or a light-transmitting insulating layer that scatters the light emitted from these light emission layers. Therefore, high-quality light emission that exhibits light emission of a desired color tone can be realized. In addition, by having a light-transmitting insulating layer between the first light emitting unit and the second light emitting unit, both the light emitting units can be electrically separated, and each light emitting unit can be driven independently. It is possible to obtain an organic light emitting device capable of changing the light emission characteristics of each light emitting portion as required and capable of adjusting the color tone.

以下、本発明を実施するための最良の形態を説明する。   Hereinafter, the best mode for carrying out the present invention will be described.

図1(a)は請求項1の発明の実施の形態の一例を示すものであり、第1及び第2の二つの電極1,2の間に第1の発光層3を積層して形成される第1の発光部4と、第3及び第4の二つの電極5,6の間に第2の発光層7を積層して形成される第2の発光部8とを、光透過性の絶縁層9を介して積層した構造に形成されており、これらを基板26の上に設けて有機発光素子(有機EL発光素子)として形成するようにしてある。第1の発光部4において、第1及び第2の電極1,2のうち、一方が陽極、他方が陰極となるものであり、また第2の発光部8において、第3及び第4の電極5,6のうち、一方が陽極、他方が陰極となるものである。また第1〜第4の電極1,2,5,6のち、第1の発光部4の外側に位置する第1の電極1あるいは第2の発光部8の外側に位置する第4の電極6のいずれか一方が光反射性電極として形成されるものであり、他の総ては光透過性電極として形成されるものである。   FIG. 1A shows an example of an embodiment of the invention of claim 1, which is formed by laminating a first light emitting layer 3 between first and second electrodes 1 and 2. A first light-emitting portion 4 and a second light-emitting portion 8 formed by laminating a second light-emitting layer 7 between the third and fourth electrodes 5, 6. They are formed in a laminated structure with an insulating layer 9 interposed therebetween, and these are provided on the substrate 26 to form an organic light emitting device (organic EL light emitting device). In the first light emitting unit 4, one of the first and second electrodes 1 and 2 is an anode and the other is a cathode. In the second light emitting unit 8, the third and fourth electrodes are used. Among 5 and 6, one is an anode and the other is a cathode. Further, after the first to fourth electrodes 1, 2, 5, and 6, the first electrode 1 positioned outside the first light emitting unit 4 or the fourth electrode 6 positioned outside the second light emitting unit 8. Any one of these is formed as a light-reflective electrode, and all the others are formed as light-transmissive electrodes.

図1(a)の実施の形態では、基板26の片面に、第1の電極1、第1の発光層3、第2の電極2、光透過性の絶縁層9、第3の電極5、第2の発光層7、第4の電極6をこの順に積層した構造に形成してあり、図1(a)の矢印のように発光層3,7で発光した光を基板26の側から取り出す場合には、基板26を透明樹脂板や透明樹脂シートなどで光透過性基板として形成すると共に、第1の電極1、第2の電極2、第3の電極5をそれぞれ光透過性の電極で形成し、また第4の電極6は光反射性を有する電極として形成してある。   In the embodiment of FIG. 1A, the first electrode 1, the first light emitting layer 3, the second electrode 2, the light-transmissive insulating layer 9, the third electrode 5, The second light emitting layer 7 and the fourth electrode 6 are stacked in this order, and light emitted from the light emitting layers 3 and 7 is extracted from the substrate 26 side as indicated by arrows in FIG. In this case, the substrate 26 is formed as a light transmissive substrate with a transparent resin plate or a transparent resin sheet, and the first electrode 1, the second electrode 2, and the third electrode 5 are respectively light transmissive electrodes. The fourth electrode 6 is formed as an electrode having light reflectivity.

第1及び第2の発光部4,8を構成する第1及び第2の発光層3,7は、公知の任意の構造・組成のものを用いることができるものであり、例えば、単一の材料で発光する発光層、いわゆるホスト材料中にドーパントを導入したドープ型発光層、異なる組成からなる二層以上の発光層を積層もしくは併置した構造の発光層等として形成することができる。ここで、各発光層3,7と電極1,2,5,6の間には、必要に応じて、ホール輸送層、ホール注入層、電子輸送層、電子注入層、キャリアブロック層等が積層されるが、図1(後述の各図においても同じ)にはこれらの各層の図示は省略してある。   The first and second light-emitting layers 3 and 7 constituting the first and second light-emitting portions 4 and 8 can be of any known structure and composition. It can be formed as a light emitting layer that emits light from a material, a doped light emitting layer in which a dopant is introduced into a so-called host material, a light emitting layer having a structure in which two or more light emitting layers having different compositions are stacked or juxtaposed. Here, a hole transport layer, a hole injection layer, an electron transport layer, an electron injection layer, a carrier block layer, and the like are laminated between the light emitting layers 3 and 7 and the electrodes 1, 2, 5, and 6 as necessary. However, these layers are not shown in FIG. 1 (the same applies to each of the drawings described later).

第1〜第4の電極1,2,5,6のうち、光透過性の電極の材料としては、有機発光素子の機能を損ねない限り特に限定されるものではないが、ITO、IZO、AZO、GZO、ATO、SnO等の透明導電膜、Ag、Au、Al等の金属薄膜、導電性有機材料や、あるいはこれらを組み合わせたものを好適に用いることができる。光透過性の電極はその透過率が高いことが好ましい。また、光透過性の電極と隣接する層との界面および/または電極そのものの反射率が低い場合に、本発明の効果をより有効に得ることができる。光透過性の電極と隣接する層との界面に於ける反射率は、例えば、光透過性の電極と、光透過性の電極に隣接する層(空気層の場合も含む)との間に、いわゆる反射防止膜を形成することによって低減することが可能である。あるいは単純に両者の屈折率の間に位置する屈折率の層を設けてもよい。 Of the first to fourth electrodes 1, 2, 5, 6, the material of the light transmissive electrode is not particularly limited as long as it does not impair the function of the organic light emitting device, but ITO, IZO, AZO , GZO, ATO, SnO 2 and other transparent conductive films, Ag, Au, Al and other metal thin films, conductive organic materials, or combinations thereof can be suitably used. The light transmissive electrode preferably has a high transmittance. In addition, the effect of the present invention can be obtained more effectively when the interface between the light transmissive electrode and the adjacent layer and / or the reflectivity of the electrode itself is low. The reflectance at the interface between the light transmissive electrode and the adjacent layer is, for example, between the light transmissive electrode and the layer adjacent to the light transmissive electrode (including the case of an air layer). It can be reduced by forming a so-called antireflection film. Or you may provide the layer of the refractive index located between both refractive indexes simply.

また光反射性の電極の材料としては、有機発光素子の機能を損ねずまた十分な光反射率を有していればよく、特に限定されるものではないが、Al、Ag、Au、Ni、Crその他の金属電極、もしくは前記の透明導電膜とこれらの金属電極もしくは誘電体多層膜等任意の反射層、導電性有機材料との組み合わせからなるものを好適に用いることができる。   Further, the material of the light reflective electrode is not particularly limited as long as it does not impair the function of the organic light emitting device and has sufficient light reflectivity, but is not limited to Al, Ag, Au, Ni, It is possible to suitably use Cr or another metal electrode, or a combination of the transparent conductive film and any reflective layer such as the metal electrode or dielectric multilayer film, or a conductive organic material.

第1の発光部4と第2の発光部8の間に積層される光透過性の絶縁層9は、光反射性の電極6を有しない側の発光部4、すなわち光を取り出す側の発光部4の発光層3で発光した光が干渉を起こさない厚みの層、あるいは、この発光層3で発光した光を散乱させる層として形成されるものである。   The light-transmissive insulating layer 9 stacked between the first light-emitting unit 4 and the second light-emitting unit 8 is a light-emitting unit 4 on the side that does not have the light-reflecting electrode 6, that is, light emission on the side from which light is extracted. The light emitted from the light emitting layer 3 of the portion 4 is formed as a layer having a thickness that does not cause interference, or a layer that scatters the light emitted from the light emitting layer 3.

このような光を取り出す側の発光部4の発光層3で発光した光が干渉を起こさない厚みの光透過性の絶縁層9としては、本発明の趣旨に反しない限り特に限定されるものではないが、例えばSiO、SiO、SiN、LiF、MgF等の蒸着、スパッタ、CVD等の手段で成膜が可能な光透過性材料や、無機系樹脂、有機系樹脂等のスピンコート、ディップコート、塗布、インクジェット、グラビア、スクリーンなど任意の印刷法・コート法で形成される光透過性の膜や、さらに有機材料や無機材料からなるシート、フィルム、ゲル、シール、板など貼付や配置することによって用いることができる材料で、形成することができるものである。また有機発光素子を保持する基板自体で形成することも可能である。ここで、光が干渉を起こさない厚みとは、一般に発光波長の数倍以上のオーダーであれば特に限定されるものではなく、例えば1μm〜3mm程度の厚みである。 The light-transmitting insulating layer 9 having such a thickness that the light emitted from the light-emitting layer 3 of the light-emitting portion 4 on the light extraction side 4 does not cause interference is not particularly limited as long as it does not contradict the gist of the present invention. There is no light transmission material that can be formed by means such as vapor deposition, sputtering, CVD, etc., such as SiO 2 , SiO, SiN, LiF, MgF 2 , spin coating, dip of inorganic resin, organic resin, etc. Light-transmitting film formed by any printing method / coating method such as coating, coating, inkjet, gravure, screen, etc., and sheets, films, gels, seals, plates, etc. made of organic or inorganic materials It can be formed by a material that can be used depending on the situation. It is also possible to form the substrate itself holding the organic light emitting element. Here, the thickness at which light does not cause interference is not particularly limited as long as it is generally on the order of several times the emission wavelength, and is, for example, a thickness of about 1 μm to 3 mm.

また光を取り出す側の発光部4の発光層3で発光した光を散乱させる光透過性の絶縁層9としては、上記の層中に光散乱成分、例えば層を形成する周辺材料とは屈折率の異なる粒子、箔などを含有するものや、異なる屈折率を有する界面を内部に備える組み合わせの、例えば凹凸を有する材料上に別の材料を積層したもの、周辺材料と相分離を起こすことによって散乱性を発現する材料の組み合わせからなるものや、層中に反射性を有する粒子、箔、面などを含むものなどで形成することができるものである。この光を散乱させる光透過性の絶縁層9の膜厚は特に限定されるものではなく、必要に応じて任意に設定することができるものである。   The light-transmitting insulating layer 9 that scatters the light emitted from the light-emitting layer 3 of the light-emitting portion 4 on the light extraction side is a light-scattering component in the above-described layer, for example, a peripheral material that forms the layer and a refractive index. Scattering due to phase separation from surrounding materials, such as those containing different particles, foils, etc., or combinations with internal interfaces with different refractive indexes, for example, other materials laminated on uneven materials It can be formed of a combination of materials exhibiting properties, or a layer containing reflective particles, foil, surface, etc. in the layer. The film thickness of the light-transmissive insulating layer 9 that scatters the light is not particularly limited, and can be arbitrarily set as required.

また、光が干渉を起こさない厚みの光透過性の絶縁層9や、光を散乱させる光透過性の絶縁層9としては、ガラス板あるいはフィルムおよびこれに準じるもの、例えば樹脂板、プラスチックシート、ガラスとプラスチックの複合体、光透過性セラミック板、樹脂硬化体、有機・無機ハイブリッド材料からなるシート・フィルムなど、光透過性を有する基材を用いることもできる。この場合、ガラス板やフィルムの表面に電極1,2,5,6や発光層3,7を積層することによって、ガラス板やフィルムで絶縁層9を形成することができるものである。そしてガラス板やフィルムは基板としての機能も有するので、後述の図4や図5の製造方法で有機発光素子を製造する際に用いる光透過性基板12を、このガラス板やフィルムで形成することができるものである。   Further, as the light-transmissive insulating layer 9 having a thickness that does not cause interference of light, and the light-transmissive insulating layer 9 that scatters light, a glass plate or a film and the like, such as a resin plate, a plastic sheet, It is also possible to use a light-transmitting substrate such as a glass / plastic composite, a light-transmitting ceramic plate, a cured resin, and a sheet / film made of an organic / inorganic hybrid material. In this case, the insulating layer 9 can be formed of a glass plate or film by laminating the electrodes 1, 2, 5, 6 and the light emitting layers 3, 7 on the surface of the glass plate or film. And since a glass plate and a film also have a function as a substrate, a light-transmitting substrate 12 used when manufacturing an organic light-emitting element by the manufacturing method shown in FIGS. 4 and 5 to be described later is formed from this glass plate or film. It is something that can be done.

図2(a)は請求項2の発明の実施の形態の一例を示すものであり、積層構成は図1(a)のものとほぼ共通するが、第1〜第4の電極1,2,5,6は総て光透過性の電極として形成してある。そして第1の発光部4の外側に位置する第1の電極1あるいは第2の発光部8の外側に位置する第4の電極6のいずれか一方の外側に、光反射性を有する光反射層10を積層して設けてある。図2(a)の矢印のように発光層3,7で発光した光を基板26の側から取り出す場合には、第4の電極6の外面に光反射層10が形成されるものである。   FIG. 2 (a) shows an example of the embodiment of the invention of claim 2, and the laminated structure is substantially the same as that of FIG. 1 (a), but the first to fourth electrodes 1, 2, 5 and 6 are all formed as light transmissive electrodes. A light reflecting layer having light reflectivity is provided outside either the first electrode 1 located outside the first light emitting unit 4 or the fourth electrode 6 located outside the second light emitting unit 8. 10 are stacked. When the light emitted from the light emitting layers 3 and 7 is extracted from the substrate 26 side as indicated by the arrows in FIG. 2A, the light reflecting layer 10 is formed on the outer surface of the fourth electrode 6.

この電極6の外側に形成される光反射層10は、いわゆる鏡面反射性を有するものであってもよいし、光散乱性・拡散反射性を有するものであってもよい。鏡面反射性を有するものとしては、例えば、Al、Ag等の金属膜、誘電体多層膜からなる反射膜など、実質的に鏡面反射を示す任意の反射体を用いることができる。また光散乱性・拡散反射性を有するものとしては、例えば、酸化バリウム、酸化チタン等の粒子の層からなる反射面や、凹凸形状を有する面の上に形成した金属膜や誘電体多層膜からなる反射膜や、鏡面反射性を有する層の上に、光散乱性、光拡散性、回折性を有する光透過性の層を設けたものなどで形成することができる。   The light reflection layer 10 formed on the outside of the electrode 6 may have a so-called specular reflection property, or may have a light scattering property and a diffuse reflection property. As a material having specular reflectivity, for example, any reflector that substantially exhibits specular reflection, such as a metal film of Al, Ag, or the like, or a reflection film made of a dielectric multilayer film can be used. Examples of the light scattering / diffuse reflecting properties include a reflective surface composed of a layer of particles such as barium oxide and titanium oxide, and a metal film or dielectric multilayer film formed on a surface having an uneven shape. Or a layer having a light-transmitting layer having a light scattering property, a light diffusing property, or a diffractive property on a reflecting film or a layer having a specular reflection property.

図3(a)は請求項3の発明の実施の形態の一例を示すものであり、第1及び第2の二つの電極1,2の間に第1の発光層3を積層して形成される第1の発光部4と、第3及び第4の二つの電極5,6の間に第2の発光層7を積層して形成される第2の発光部8とを積層した構造に形成されており、これらを基板26の上に設けて有機発光素子(有機EL発光素子)として形成するようにしてある。第1の発光部4において、第1及び第2の電極1,2のうち、一方が陽極、他方が陰極となるものであり、また第2の発光部8において、第3及び第4の電極5,6のうち、一方が陽極、他方が陰極となるものである。第1〜第4の電極1,2,5,6は総て光透過性の電極として形成してあり、そして第1の発光部4の外側に位置する第1の電極1あるいは第2の発光部8の外側に位置する第4の電極6のいずれか一方の外側に、第1及び第2の発光層3,4で発光した光が干渉を起こさない厚みの光透過性の絶縁層9、あるいは、第1及び第2の発光層3,4で発光した光を散乱させる光透過性の絶縁層9を介して、光反射性を有する光反射層10を積層して設けてある。図3(a)の矢印のように発光層3,7で発光した光を基板26の側から取り出す場合には、第4の電極6の外面に光透過性の絶縁層9を介して、光反射性を有する光反射層10が形成されるものである。また図3(a)の実施の形態では、第1の発光部4と第2の発光部5の間に光透過性の絶縁層14が設けてあるが、この光透過性の絶縁層14は必要に応じて設けられるものであり、必ずしも必要なものではない。   FIG. 3A shows an example of an embodiment of the invention of claim 3, which is formed by laminating a first light emitting layer 3 between first and second electrodes 1 and 2. The first light-emitting portion 4 and the second light-emitting portion 8 formed by laminating the second light-emitting layer 7 between the third and fourth electrodes 5 and 6 are laminated. These are provided on the substrate 26 to form an organic light emitting device (organic EL light emitting device). In the first light emitting unit 4, one of the first and second electrodes 1 and 2 is an anode and the other is a cathode. In the second light emitting unit 8, the third and fourth electrodes are used. Among 5 and 6, one is an anode and the other is a cathode. The first to fourth electrodes 1, 2, 5, 6 are all formed as light-transmitting electrodes, and the first electrode 1 or the second light emission located outside the first light-emitting portion 4. A light-transmissive insulating layer 9 having a thickness that does not cause interference of light emitted from the first and second light-emitting layers 3 and 4 on the outer side of one of the fourth electrodes 6 positioned outside the portion 8; Alternatively, a light reflecting layer 10 having light reflectivity is laminated and provided through a light-transmitting insulating layer 9 that scatters light emitted from the first and second light emitting layers 3 and 4. When the light emitted from the light emitting layers 3 and 7 is extracted from the substrate 26 side as indicated by the arrows in FIG. 3A, the light is transmitted through the light transmissive insulating layer 9 on the outer surface of the fourth electrode 6. The light reflecting layer 10 having reflectivity is formed. In the embodiment of FIG. 3A, a light-transmissive insulating layer 14 is provided between the first light-emitting portion 4 and the second light-emitting portion 5, and this light-transmissive insulating layer 14 is It is provided as necessary and is not necessarily required.

光透過性の電極1,2,5,6、発光層3、干渉を起こさない厚みのあるいは光散乱性の光透過性の絶縁層9の材料は、上記で用いたものと同じものを使用することが可能である。また第1の発光部4と第2の発光部5の間の光透過性の絶縁層14の厚みは特に限定されるものではなく、光散乱性の有無も特に問うものではない。この光透過性の絶縁層14を設けない場合、第1の発光部4と第2の発光部8の電極2,5を共用した一つの電極で形成することが可能になる。例えば、第1の発光部4のための陽極/第1の発光層3/第1の発光部4のための陰極兼第2の発光部8のための陰極/第2の発光層7/第2の発光部8のための陽極、というように、電極を形成することができるものである。   The same materials as those used above are used for the light transmissive electrodes 1, 2, 5, 6 and the light emitting layer 3, and the light transmissive insulating layer 9 having a thickness that does not cause interference or a light scattering property. It is possible. Further, the thickness of the light-transmitting insulating layer 14 between the first light-emitting portion 4 and the second light-emitting portion 5 is not particularly limited, and the presence or absence of light scattering is not particularly questioned. When this light-transmissive insulating layer 14 is not provided, it is possible to form the first light-emitting portion 4 and the second light-emitting portion 8 with a single electrode that shares the electrodes 2 and 5. For example, the anode for the first light emitting unit 4 / the first light emitting layer 3 / the cathode for the first light emitting unit 4 and the cathode for the second light emitting unit 8 / the second light emitting layer 7 / the first. An electrode can be formed such as an anode for the second light emitting portion 8.

尚、上記の各実施の形態にあって、発光部は第1の発光部4と第2の発光部8の2つの例を挙げているが、3つ以上の発光部の場合にも、こられの発光部のうち少なくとも隣合う2つの発光部が、上記のような第1の発光部4と第2の発光部8の構成を満たすものであればよい。   In each of the embodiments described above, two examples of the light emitting unit, that is, the first light emitting unit 4 and the second light emitting unit 8, are given. Of these light emitting units, at least two adjacent light emitting units may satisfy the configuration of the first light emitting unit 4 and the second light emitting unit 8 as described above.

図1(b)、図2(b)、図3(b)の各実施の形態は、等電位面を形成する層11もしくは電荷発生層11を介して積層した複数の発光層3,7で発光部4,8を形成し、いわゆる積層型、タンデム型、マルチフォトン型の発光部として形成するようにしたものである。第1及び第2の発光部4,8の両方をこのような複数の発光層3,7で形成するようにしてもよく、第1及び第2の発光部4,8のいずれか一方をこのような複数の発光層3,7で形成するようにしてもよい。等電位面形成層11もしくは電荷発生層11の材料としては、例えばAg、Au、Al等の金属薄膜、酸化バナジウム、酸化モリブデン、酸化レニウム、酸化タングステン等の金属酸化物、ITO、IZO、AZO、GZO、ATO、SnO等の透明導電膜、いわゆるn型半導体とp型半導体の積層体、金属薄膜もしくは透明導電膜とn型半導体及び/またはp型半導体との積層体、n型半導体とp型半導体の混合物、n型半導体及び/またはp型半導体と金属との混合物、などを挙げることができる。n型半導体やp型半導体としては、無機材料であっても、有機材料であってもよく、あるいは有機材料と金属との混合物や、有機材料と金属酸化物や、有機材料と有機系アクセプタ/ドナー材料や、無機系アクセプタ/ドナー材料等の組合わせによって得られるものであってもよく、特に制限されることなく必要に応じて選定して使用することができる。 Each of the embodiments of FIG. 1B, FIG. 2B, and FIG. 3B includes a plurality of light-emitting layers 3 and 7 stacked via the layer 11 forming the equipotential surface or the charge generation layer 11. The light emitting portions 4 and 8 are formed to form so-called stacked, tandem, and multiphoton light emitting portions. Both the first and second light-emitting portions 4 and 8 may be formed of the plurality of light-emitting layers 3 and 7, and either one of the first and second light-emitting portions 4 and 8 may be formed in this manner. A plurality of such light emitting layers 3 and 7 may be formed. Examples of the material of the equipotential surface forming layer 11 or the charge generation layer 11 include metal thin films such as Ag, Au, and Al, metal oxides such as vanadium oxide, molybdenum oxide, rhenium oxide, and tungsten oxide, ITO, IZO, AZO, Transparent conductive film such as GZO, ATO, SnO 2 , so-called n-type semiconductor and p-type semiconductor laminate, metal thin film or transparent conductive film and n-type semiconductor and / or p-type semiconductor laminate, n-type semiconductor and p And a mixture of a n-type semiconductor and / or a p-type semiconductor and a metal. The n-type semiconductor or p-type semiconductor may be an inorganic material or an organic material, or a mixture of an organic material and a metal, an organic material and a metal oxide, an organic material and an organic acceptor / It may be obtained by a combination of a donor material, an inorganic acceptor / donor material, etc., and can be selected and used as needed without any particular limitation.

上記のように形成される図1、図2、図3の有機発光素子にあって、第1の発光部4の発光層3や、第2の発光部8の発光層7で発光した光は、光透過性の基板26を通して取り出される。第1の発光部4の発光層3や、第2の発光部8の発光層7で発光した光の一部は、図1の実施の形態では光反射性を有する電極6で反射して、図2の実施の形態では光反射層10で反射して、図3の実施の形態では光反射層10で反射して、光透過性の基板26を通して取り出される。   1, 2, and 3 formed as described above, the light emitted from the light emitting layer 3 of the first light emitting unit 4 and the light emitting layer 7 of the second light emitting unit 8 is And is taken out through the light-transmitting substrate 26. A part of the light emitted from the light emitting layer 3 of the first light emitting unit 4 or the light emitting layer 7 of the second light emitting unit 8 is reflected by the electrode 6 having light reflectivity in the embodiment of FIG. In the embodiment of FIG. 2, the light is reflected by the light reflecting layer 10. In the embodiment of FIG. 3, the light is reflected by the light reflecting layer 10, and is taken out through the light-transmitting substrate 26.

そして本発明のこれらの有機発光素子には、光が干渉を起こさない厚みの、あるいは光散乱性を有する光透過性の絶縁層9が設けられているので、発光スペクトルの角度依存性を低減することができるものである。発光スペクトルの角度依存性は、発光位置から発生した光と、その光が反射面で反射された光の干渉によって生じるものであるが、光の取り出し側に近い位置に存在する発光部と光反射面との距離を光学干渉が発生しない距離に設定することにより、角度依存性を低減することができるものである。光学干渉抑制効果は、図1や図2の実施の形態の場合には、第1及び第2の発光部4,8の間に設けられた、実質的に光学干渉が発生しない光学長に相当する厚みの光透過性絶縁層9あるいは光散乱性の光透過性絶縁層9によって発現し、図3の実施の形態の場合には、光の取り出し側から最も遠い位置にある光透過性の電極6の外側に設けられた、実質的に光学干渉が発生しない光学長に相当する厚みの光透過性絶縁層9あるいは光散乱性の光透過性絶縁層9によって発現するものである。尚、最も光反射面に近い発光部8の発光層7はその光学的設計によって、例えば、その発光部位と反射面との光学的距離が1/4波長の奇数倍の距離になるように設定することで、より好ましくは、発光部位と、発光部位に対して反射面とは反対側に位置する反射率段差が最も大きな界面との距離を1/4波長の整数倍に設定することで、好ましくない干渉効果をほぼ抑制することが可能であるため、必要に応じて、このような膜厚設計による光干渉効果の抑制方法を併用するようにしてもよい。また光の取り出し側に近い側の、すなわち反射面から遠い側の発光部4の発光層3に関しても、同様の膜厚設計をすることによって、好ましくない干渉効果を調整することが可能であるが、その効果は比較的低いことを認識して適用することが必要である。   These organic light emitting devices of the present invention are provided with a light-transmitting insulating layer 9 having a thickness that does not cause interference of light or having light scattering properties, thereby reducing the angle dependency of the emission spectrum. It is something that can be done. The angle dependence of the emission spectrum is caused by the interference between the light generated from the light emission position and the light reflected by the reflection surface. By setting the distance from the surface to a distance that does not cause optical interference, the angle dependency can be reduced. The optical interference suppression effect corresponds to an optical length that is provided between the first and second light emitting units 4 and 8 and that does not substantially cause optical interference in the embodiment of FIGS. The light-transmitting electrode 9 is expressed by the light-transmitting insulating layer 9 or the light-scattering light-transmitting insulating layer 9 having the thickness to be used, and in the case of the embodiment of FIG. 6 is exhibited by the light-transmitting insulating layer 9 or the light-scattering light-transmitting insulating layer 9 having a thickness corresponding to the optical length substantially free of optical interference. The light emitting layer 7 of the light emitting unit 8 closest to the light reflecting surface is set by optical design such that, for example, the optical distance between the light emitting portion and the reflecting surface is an odd multiple of 1/4 wavelength. More preferably, by setting the distance between the light emitting part and the interface having the largest reflectance step located on the opposite side of the reflecting surface with respect to the light emitting part to an integral multiple of ¼ wavelength, Since an undesirable interference effect can be substantially suppressed, a method for suppressing the optical interference effect by such a film thickness design may be used in combination as necessary. Further, with respect to the light emitting layer 3 of the light emitting unit 4 on the side close to the light extraction side, that is, on the side far from the reflecting surface, it is possible to adjust an undesirable interference effect by designing the film thickness in the same manner. It is necessary to recognize and apply that the effect is relatively low.

また、本発明に係る有機発光素子は、第1及び第2の複数の発光部4,8を有し、これらが異なる電極1,2及び5,6間に形成された構造を有するものである。そして図1、図2、図3のように第1の発光部4と第2の発光部8の間に光透過性の絶縁層9,14が介在していることによって、両発光部4,8は電気的に切り離されており、各発光部4,8をそれぞれ個別に駆動して発光させることが可能である。また図3において絶縁層14を備えない構造の場合、既述のように第1及び第2の発光部4,8に電極を共有させるようにしてもよい。このような電気的構造を有することで、第1の発光部4と第2の発光部8には必要に応じて異なる電界を印加して駆動し、必要に応じて発光特性を変化させることが可能である。   The organic light emitting device according to the present invention has a structure in which the first and second light emitting portions 4 and 8 are formed between the different electrodes 1, 2, 5 and 6. . As shown in FIGS. 1, 2, and 3, the light-transmitting insulating layers 9 and 14 are interposed between the first light-emitting portion 4 and the second light-emitting portion 8, whereby both the light-emitting portions 4 and 4. 8 is electrically disconnected, and each of the light emitting units 4 and 8 can be individually driven to emit light. In the case where the structure does not include the insulating layer 14 in FIG. 3, the electrodes may be shared by the first and second light emitting units 4 and 8 as described above. By having such an electrical structure, the first light emitting unit 4 and the second light emitting unit 8 can be driven by applying different electric fields as necessary, and the light emission characteristics can be changed as necessary. Is possible.

例えば、本発明の有機発光素子で白色有機発光素子を形成してカラーフィルターと組み合わせて用いたディスプレイの場合、基本発光色である白の色ずれを、予め劣化の速い色調の光を発する発光部を白色の発光部以外に備えた素子構造としておくことによって、使用途中でも補正することが可能である。もしくは、同一の発光色を有する発光部を積層している場合、発光強度の低下に伴って、新たな発光部を発光させることで、強度補正も可能である。一方、照明用途では、上記のディスプレイの場合に挙げたように発光色の色ずれ、発光強度の低下の補正用に用いることも可能であるし、あるいは、例えば白色の発光部と赤色の発光部を用意しておくことによって、白色発光から赤色発光の範囲の光を調色することのできる光源を得るといった用途にも使用可能である。また必要に応じて、調整するための色調を用意しておき、2つの発光部での出力比で調色することも可能であるし、また発光部を3つ以上設け、各発光部の出力を調整することで、黒体軌跡に沿った調色も可能である。各発光部の発光色及び発光部の数は、上記のような用途・目的・必要性に応じて任意に設定することが可能である。   For example, in the case of a display in which a white organic light-emitting element is formed with the organic light-emitting element of the present invention and used in combination with a color filter, a light emitting unit that emits light of a color tone that is quickly deteriorated with respect to a white color shift that is a basic emission color It is possible to correct even during use by providing an element structure provided with other than the white light emitting portion. Alternatively, when light emitting units having the same emission color are stacked, intensity correction can be performed by causing a new light emitting unit to emit light as the light emission intensity decreases. On the other hand, in lighting applications, as mentioned in the case of the above-mentioned display, it can be used for correction of emission color misregistration and decrease in emission intensity, or, for example, a white light emitting portion and a red light emitting portion. Can be used for the purpose of obtaining a light source capable of toning light in the range of white light emission to red light emission. In addition, if necessary, it is possible to prepare a color tone to be adjusted and to adjust the color with the output ratio of the two light emitting units, or to provide three or more light emitting units and output each light emitting unit. By adjusting, color matching along the black body locus is also possible. The light emission color and the number of light emission parts of each light emission part can be arbitrarily set according to the above uses, purposes, and necessity.

第1と第2の各発光部4,8の駆動方法は、既存の任意の方法を組み合わせて行なうことができるものであり、各発光部4,8の発光出力の関係は適宜設定することができるものである。各発光部4,8の出力は、電圧、電流、電力のいずれによって制御してもよいし、あるいはパルスなど任意の電流/電圧波形で通電することによって調整してもかまわない。また各発光部4,8の出力は、各種の方法を用いて制御可能であり、各発光部4,8を独立に制御してもよく、あるいは、例えば黒体軌跡上を発光色が移動するように各発光部4,8の出力を所定の関係に従って制御するようにしてもよい。   The driving method of each of the first and second light emitting units 4 and 8 can be performed by combining existing arbitrary methods, and the relationship between the light emitting outputs of the light emitting units 4 and 8 can be set as appropriate. It can be done. The outputs of the light emitting units 4 and 8 may be controlled by any of voltage, current, and power, or may be adjusted by energizing with an arbitrary current / voltage waveform such as a pulse. The outputs of the light emitting units 4 and 8 can be controlled using various methods, and the light emitting units 4 and 8 may be controlled independently, or, for example, the emission color moves on a black body locus. As described above, the outputs of the light emitting units 4 and 8 may be controlled in accordance with a predetermined relationship.

本発明の有機発光素子の製造は、任意の方法で行なうことができるが、例えば、透明基板26上に形成された透明導電膜を光透過性の第1の電極1とし、この上に第1の発光層3、次いで光透過性の第2の電極2を積層して第1の発光部4を形成し、この上に上記の光透過性の絶縁層9を積層した後、この上に光透過性の第3の電極5、第2の発光層7を積層し、さらにこの上に光反射性を有する第4の電極6を積層して第2の発光部8を形成することによって、図1のような有機発光素子を製造することができる。また光反射性を有する第4の電極6の代りに、光透過性の第4の電極6を形成すると共にその上に光反射層10を積層することによって、図2のような有機発光素子を製造することができる。また、透明基板26上に形成された透明導電膜を光透過性の第1の電極1とし、この上に第1の発光層3、次いで光透過性の第2の電極2を積層して第1の発光部4を形成し、必要に応じて上記の光透過性の絶縁層14を積層した後、この上に光透過性の第3の電極5、第2の発光層7、光透過性の第4の電極6を積層して第2の発光部8を形成し、さらにこの上に上記の光透過性の絶縁層9を積層した後、この上に光反射性層10を積層することによって、図3のような有機発光素子を製造することができる。   The organic light-emitting device of the present invention can be manufactured by any method. For example, the transparent conductive film formed on the transparent substrate 26 is used as the light-transmitting first electrode 1, and the first electrode is formed thereon. The light-emitting layer 3 and then the light-transmissive second electrode 2 are laminated to form the first light-emitting portion 4, and the light-transmissive insulating layer 9 is laminated on the light-emitting layer 4. By laminating the transmissive third electrode 5 and the second light emitting layer 7 and further laminating the fourth electrode 6 having light reflectivity thereon, the second light emitting portion 8 is formed. 1 can be produced. Also, instead of the light-reflecting fourth electrode 6, a light-transmitting fourth electrode 6 is formed and a light-reflecting layer 10 is laminated thereon, whereby an organic light-emitting device as shown in FIG. Can be manufactured. The transparent conductive film formed on the transparent substrate 26 is used as the light transmissive first electrode 1, and the first light emitting layer 3 and then the light transmissive second electrode 2 are stacked thereon to form the first electrode 1. 1 light-emitting portion 4 is formed, and the light-transmitting insulating layer 14 is laminated as necessary. Then, the light-transmitting third electrode 5, the second light-emitting layer 7, and the light-transmitting property are formed thereon. 4th electrode 6 is laminated | stacked, the 2nd light emission part 8 is formed, Furthermore, after laminating | stacking said light-transmissive insulating layer 9 on this, laminating | stacking the light reflection layer 10 on this. Thus, an organic light emitting device as shown in FIG. 3 can be manufactured.

図4は請求項6の製造方法の実施の形態の一例を示すものであり、図4(a)のように、光が干渉を起こさない厚みの、あるいは光散乱性の第1の光透過性基板12を用い、この第1の光透過性基板12の表面に、電極28、発光層29、電極30をこの順に積層して発光部31を形成する。また図4(b)のように、第2の光透過性基板13の表面に、電極32、発光層33、電極34をこの順に積層して発光部35を形成する。そして図4(c)のように、第1の光透過性基板12の発光部31を形成した面と反対側の表面に、第2の光透過性基板13に形成した発光部35の電極34を積層することによって、2つの発光部31,35を第1の光透過性基板12を介して積層した有機発光素子を得ることができるものである。   FIG. 4 shows an example of an embodiment of the manufacturing method according to claim 6. As shown in FIG. 4 (a), the first light transmittance having a thickness that does not cause interference of light or a light scattering property. Using the substrate 12, the light emitting portion 31 is formed by laminating the electrode 28, the light emitting layer 29, and the electrode 30 in this order on the surface of the first light transmitting substrate 12. Further, as shown in FIG. 4B, the light emitting portion 35 is formed by laminating the electrode 32, the light emitting layer 33, and the electrode 34 in this order on the surface of the second light transmissive substrate 13. Then, as shown in FIG. 4C, the electrode 34 of the light emitting unit 35 formed on the second light transmitting substrate 13 is provided on the surface opposite to the surface on which the light emitting unit 31 of the first light transmitting substrate 12 is formed. By laminating the organic light emitting device, it is possible to obtain an organic light emitting element in which the two light emitting portions 31 and 35 are laminated via the first light transmitting substrate 12.

ここで、電極28,32,34を光透過性の電極で形成すると共に電極30を光反射性を有する電極で形成することによって、電極32で第1の電極1、電極34で第2の電極2、発光層33で第1の発光層3、発光部35で第1の発光部4、電極28で第3の電極5、電極30で第4の電極6、発光層29で第2の発光層7、発光部31で第2の発光部8、第1の光透過性基板12で光透過性の絶縁層9、第2の光透過性基板13で基板26がそれぞれ形成される、図1の構成の有機発光素子を得ることができるものである。また、電極28,30,32,34をそれぞれ光透過性の電極で形成すると共に電極30の外側に光反射層10を形成することによって、同様に図2の構成の有機発光素子を得ることができるものである。   Here, the electrodes 28, 32, and 34 are formed of light-transmitting electrodes, and the electrode 30 is formed of a light-reflecting electrode, whereby the electrode 32 is the first electrode 1 and the electrode 34 is the second electrode. 2, the light emitting layer 33 is the first light emitting layer 3, the light emitting portion 35 is the first light emitting portion 4, the electrode 28 is the third electrode 5, the electrode 30 is the fourth electrode 6, and the light emitting layer 29 is the second light emitting. The layer 7, the light emitting unit 31 form the second light emitting unit 8, the first light transmitting substrate 12 forms the light transmitting insulating layer 9, and the second light transmitting substrate 13 forms the substrate 26, respectively. Thus, an organic light emitting device having the following structure can be obtained. Further, by forming the electrodes 28, 30, 32, and 34 as light transmissive electrodes and forming the light reflecting layer 10 on the outer side of the electrode 30, the organic light emitting device having the configuration shown in FIG. It can be done.

図5は請求項7の製造方法の実施の形態の一例を示すものであり、図5(a)のように、光が干渉を起こさない厚みの、あるいは光散乱性の光透過性基板12を用い、この光透過性基板12の表面に、電極28、発光層29、電極30をこの順に積層して発光部31を形成する。次に、図5(b)のように、この光透過性基板12の発光部31を形成した側と反対側の表面に、電極32、発光層33、電極34をこの順に積層して発光部35を形成することによって、2つの発光部31,35を光透過性基板12を介して積層した有機発光素子を得ることができるものである。   FIG. 5 shows an example of an embodiment of the manufacturing method of claim 7. As shown in FIG. 5A, a light-transmitting substrate 12 having a thickness that does not cause interference of light or a light scattering property is shown. The light emitting section 31 is formed by laminating the electrode 28, the light emitting layer 29, and the electrode 30 in this order on the surface of the light transmissive substrate 12. Next, as shown in FIG. 5B, an electrode 32, a light emitting layer 33, and an electrode 34 are laminated in this order on the surface of the light transmissive substrate 12 opposite to the side where the light emitting part 31 is formed. By forming 35, an organic light emitting element in which two light emitting portions 31 and 35 are laminated via the light transmissive substrate 12 can be obtained.

ここで、電極28,32,34を光透過性の電極で形成すると共に電極30を光反射性を有する電極で形成することによって、電極34で第1の電極1、電極32で第2の電極2、発光層33で第1の発光層3、発光部35で第1の発光部4、電極28で第3の電極5、電極30で第4の電極6、発光層29で第2の発光層7、発光部31で第2の発光部8、光透過性基板12で光透過性の絶縁層9がそれぞれ形成される、図1の構成の有機発光素子を得ることができるものである。また、電極28,30,32,34をそれぞれ光透過性の電極で形成すると共に電極30の外側に光反射層10を形成することによって、同様に図2の構成の有機発光素子を得ることができるものである。   Here, the electrodes 28, 32, and 34 are formed of light-transmitting electrodes, and the electrode 30 is formed of a light-reflecting electrode, whereby the electrode 34 is the first electrode 1, and the electrode 32 is the second electrode. 2, the light emitting layer 33 is the first light emitting layer 3, the light emitting portion 35 is the first light emitting portion 4, the electrode 28 is the third electrode 5, the electrode 30 is the fourth electrode 6, and the light emitting layer 29 is the second light emitting. The organic light-emitting device having the structure of FIG. 1 can be obtained in which the second light-emitting portion 8 is formed by the layer 7 and the light-emitting portion 31, and the light-transmitting insulating layer 9 is formed by the light-transmitting substrate 12. Further, by forming the electrodes 28, 30, 32, and 34 as light transmissive electrodes and forming the light reflecting layer 10 on the outer side of the electrode 30, the organic light emitting device having the configuration shown in FIG. It can be done.

上記の図4や図5の実施の形態のように、光が干渉を起こさない厚みの、あるいは光散乱性の光透過性基板12を用い、この光透過性基板12に第1の発光部4や第2の発光部8を形成することによって、光が干渉を起こさない厚みの、あるいは光散乱性の光透過性の絶縁層9を別途特別に形成するような必要がなくなり、製造の工数を低減することができるものである。   As in the embodiments of FIGS. 4 and 5 described above, a light-transmitting substrate 12 having a thickness that does not cause interference of light or a light-scattering property is used, and the first light emitting unit 4 is provided on the light-transmitting substrate 12. By forming the second light-emitting portion 8, it is not necessary to separately form a separate light-transmitting insulating layer 9 having a thickness that does not cause light interference or light scattering. It can be reduced.

上記の図5の実施の形態では、一枚の光透過性基板12の両面に発光部31と発光部35をそれぞれ形成するようにした例を示したが、例えば,図6(a)のように、光透過性基板12aの上に発光部31を形成し、また図6(b)のように別の光透過性基板12bの上に発光部35を形成し、そして図6(c)のように光透過性基板12aの発光部31を形成した面と反対側の表面に、光透過性基板12bの発光部35を形成した面と反対側の表面を接触させることによって、有機発光素子を製造することもできる。このものでは、2枚の光透過性基板12a,12bで光透過性基板12が形成されるものであり、図5のものと光学的に類似のものと見なせるものである。この図6の場合、2つの光透過性基板12a,12bの発光部31,35と反対の面同士を近接して配設するようにしてもよい。この場合、光透過性基板12a,12bの間は、光透過性基板12a,12bと同等の屈折率を有する媒体で満たすかまたは接着するか、もしくは散乱性を有する媒体で満たすかまたは接着するのが好ましい。場合によっては、光透過性基板12a,12b同士を近接させるのみでもかまわない。この図6の方法によれば、一枚の光透過性基板12の両面にそれぞれ発光部31,35を形成するという、操作上困難なプロセスを採用するような必要がなくなり、光透過性基板12a,12bの各片面に発光部31,35をそれぞれ形成するという、操作が容易で一般的なプロセスを採用することが可能になるものである。   In the embodiment of FIG. 5 described above, an example in which the light emitting unit 31 and the light emitting unit 35 are respectively formed on both surfaces of one light transmissive substrate 12 has been shown. For example, as shown in FIG. In addition, the light emitting part 31 is formed on the light transmissive substrate 12a, and the light emitting part 35 is formed on another light transmissive substrate 12b as shown in FIG. 6B. As described above, the surface of the light transmissive substrate 12a opposite to the surface on which the light emitting portion 31 is formed is brought into contact with the surface on the opposite side of the surface on which the light emitting portion 35 of the light transmissive substrate 12b is formed. It can also be manufactured. In this case, the light transmissive substrate 12 is formed by two light transmissive substrates 12a and 12b, and can be regarded as optically similar to that of FIG. In the case of FIG. 6, the surfaces opposite to the light emitting portions 31 and 35 of the two light transmissive substrates 12a and 12b may be disposed close to each other. In this case, the space between the light transmissive substrates 12a and 12b is filled or adhered with a medium having a refractive index equivalent to that of the light transmissive substrates 12a and 12b, or is filled or adhered with a medium having scattering properties. Is preferred. In some cases, the light transmissive substrates 12a and 12b may be brought close to each other. According to the method of FIG. 6, it is not necessary to employ a process that is difficult to operate, such as forming the light emitting portions 31 and 35 on both surfaces of one light transmissive substrate 12, respectively, and the light transmissive substrate 12a. , 12b, the light emitting portions 31 and 35 are formed on one side, respectively, and an easy operation and a general process can be adopted.

次に、本発明を実施例によって具体的に説明する。   Next, the present invention will be specifically described with reference to examples.

(青色発光素子Aの作製)
厚み0.7mmのガラス基板の片面に1100Å厚のITO(シート抵抗12Ω/□)が形成されたITO付きガラス基板を用意した。このITO付きガラス基板40を、図7(a)の寸法で、ITO41をエッチングして残すと共に切断した。次いで、このITO付きガラス基板を純水、アセトン、イソプロピルアルコールで各10分間超音波洗浄した後、イソプロピルアルコール蒸気で2分間蒸気洗浄して、乾燥し、さらに10分間UVオゾン洗浄した。
(Preparation of blue light-emitting element A)
A glass substrate with ITO in which 1100 mm thick ITO (sheet resistance 12Ω / □) was formed on one surface of a 0.7 mm thick glass substrate was prepared. The glass substrate 40 with ITO was cut to the size shown in FIG. Next, this ITO-attached glass substrate was subjected to ultrasonic cleaning with pure water, acetone, and isopropyl alcohol for 10 minutes each, followed by vapor cleaning with isopropyl alcohol vapor for 2 minutes, drying, and UV ozone cleaning for further 10 minutes.

続いてこのITO付きガラス基板を真空蒸着装置にセットし、図7(b)の寸法の開口部42を設けたマスク43を用いて、5×10−5Paの減圧下、4,4′−ビス[N−(ナフチル)−N−フェニル−アミノ]ビフェニル(e−Ray社製「α−NPD」)と酸化モリブデン(MoO)を3:1の成膜速度比で、合計成膜速度を1.3Å/sとして100Å厚に蒸着し、陽極となるITOの上にホール注入層を形成した。次いで、ホール注入層の上に「α−NPD」を1Å/sの蒸着速度で700Å厚に蒸着して、ホール輸送層を形成した。次いでホール輸送層の上に、ジナフチルアントラセン誘導体(コダック社製「BH−2」)にジスチリルアリーレン誘導体([化1])を4質量%ドープした層を500Å厚積層することによって、青色に発光する発光層を設けた。次にこの発光層の上に、バソクプロイン((株)同仁化学研究所製「BCP」)を100Å厚、「BCP」とCsをモル比1:1で100Å厚に共蒸着して電子注入層を設けた。さらにこの上に、「α−NPD」と酸化モリブデン(MoO)を3:1の成膜速度比で、合計成膜速度を1.3Å/sとして100Å厚に蒸着し、電荷発生層を形成した。この後、この上に、上記と同様にしてホール輸送層を700Å厚、発光層を500Å厚、電子輸送層を100Å厚、電子注入層を100Å厚で積層した。さらにこの上に、図7(c)の寸法の開口部44を設けたマスク45を用いて、アルミニウムを4Å/sの成膜速度で100Å厚積層して、光透過性の陰極を形成することによって、2層の青色に発光する発光層を電荷発生層を挟んで設けた、青色発光素子Aを得た。 Subsequently, the ITO-attached glass substrate was set in a vacuum deposition apparatus, and 4,4′- under a reduced pressure of 5 × 10 −5 Pa using a mask 43 provided with an opening 42 having the dimensions shown in FIG. Bis [N- (naphthyl) -N-phenyl-amino] biphenyl (“α-NPD” manufactured by e-Ray) and molybdenum oxide (MoO 3 ) at a film formation rate ratio of 3: 1 and the total film formation rate Evaporation was performed to a thickness of 100 Å as 1.3 Å / s, and a hole injection layer was formed on ITO serving as an anode. Next, “α-NPD” was deposited on the hole injection layer at a deposition rate of 1 Å / s to a thickness of 700 、 to form a hole transport layer. Next, on the hole transport layer, a layer obtained by doping a dinaphthyl anthracene derivative (“BH-2” manufactured by Kodak Co., Ltd.) with 4% by mass of a distyrylarylene derivative ([Chemical Formula 1]) to a thickness of 500 mm is laminated. A light emitting layer for emitting light was provided. Next, on the light-emitting layer, bathocuproin (“BCP” manufactured by Dojindo Laboratories Co., Ltd.) is 100 Å thick, and “BCP” and Cs are co-deposited at a molar ratio of 100 Å to form an electron injection layer. Provided. Furthermore, “α-NPD” and molybdenum oxide (MoO 3 ) are vapor-deposited to a thickness of 100 μm at a film formation rate ratio of 3: 1 and a total film formation rate of 1.3 μm / s to form a charge generation layer. did. Thereafter, in the same manner as described above, a hole transport layer having a thickness of 700 mm, a light emitting layer having a thickness of 500 mm, an electron transport layer having a thickness of 100 mm, and an electron injection layer having a thickness of 100 mm were stacked thereon. Further thereon, a mask 45 having an opening 44 having the dimensions shown in FIG. 7C is used to form a light-transmitting cathode by laminating aluminum with a thickness of 100 mm at a film forming rate of 4 mm / s. As a result, a blue light-emitting element A in which two light-emitting layers emitting blue light were provided with a charge generation layer interposed therebetween was obtained.

Figure 2007115645
Figure 2007115645

(黄色発光素子Bの作製)
150μm厚みのガラス板の片面に、厚み1100ÅのITO41を図7(a)の寸法で成膜した。
(Preparation of yellow light-emitting element B)
An ITO 41 having a thickness of 1100 mm was formed on one side of a 150 μm thick glass plate with the dimensions shown in FIG.

このITO付きガラス板を真空蒸着装置にセットし、図7(b)のマスクを用いて、上記と同様にして、陰極となるITOの上に、電子注入層として「BCP」とCsのモル比1:1の共蒸着層を150Å厚、電子輸送層として「BCP」を50Å厚、発光層として「BH−2」に[化2]に示す材料を4質量%ドープしたものを500Å厚、ホール輸送層として「α−NPD」を400Å厚、ホール注入層として「α−NPD」と酸化モリブデンを3:1の割合で共蒸着した層を200Å厚、それぞれこの順に形成し、最後に図7(c)のマスクを用いて、アルミニウムを4Å/sの成膜速度で800Å厚積層して、光反射性の陽極を形成することによって、黄色に発光する発光層を設けた黄色発光素子Bを得た。   This ITO-attached glass plate is set in a vacuum deposition apparatus, and using the mask of FIG. 7B, a molar ratio of “BCP” and Cs as an electron injection layer is formed on the ITO serving as the cathode in the same manner as described above. A 1: 1 co-deposited layer is 150 Å thick, “BCP” is 50 Å thick as an electron transport layer, and “BH-2” as a light emitting layer is 500 Å thick doped with 4% by mass of the material shown in [Chemical Formula 2]. As the transport layer, “α-NPD” was formed to a thickness of 400 mm, and as the hole injection layer, a layer in which “α-NPD” and molybdenum oxide were co-evaporated at a ratio of 3: 1 was formed to a thickness of 200 mm, and finally, FIG. Using the mask of c), aluminum is laminated at a thickness of 800 mm at a film forming rate of 4 mm / s to form a light-reflective anode, thereby obtaining a yellow light-emitting element B provided with a light-emitting layer that emits yellow light. It was.

Figure 2007115645
Figure 2007115645

(白色発光素子Cの作製)
上記の(青色発光素子Aの作製)において、2層目の発光層を、「BH−2」に[化2]の化合物を1質量%ドープした50Å厚の層と、「BH−2」に[化1]の化合物を4質量%ドープした450Å厚の層とを積層したものに変更する他は、上記の(青色発光素子Aの作製)と同様にして、白色に発光する白色発光素子Cを得た。この白色発光素子Cの発光色度は(0.28,0.37)であった。
(Preparation of white light emitting element C)
In the above (production of blue light-emitting element A), the second light-emitting layer is formed as a 50-thick layer in which “BH-2” is doped with 1% by mass of the compound of [Chemical Formula 2] and “BH-2”. A white light-emitting element C that emits white light in the same manner as in the above (Preparation of blue light-emitting element A), except that the compound of [Chemical formula 1] is laminated with a layer having a thickness of 450 mm doped with 4% by mass of the compound Got. The emission chromaticity of this white light emitting element C was (0.28, 0.37).

(赤色発光素子Dの作製)
上記の(黄色発光素子Bの作製)において、発光層を、トリス(8−ヒドロキシキノリナート)アルミニウム(Alq)にDCJTBを2質量%ドープしたものを500Å厚に蒸着して形成するようにした他は、上記の(黄色発光素子Bの作製)と同様にして、赤色に発光する赤色発光素子Dを得た。
(Preparation of red light emitting element D)
In the above (production of yellow light-emitting element B), the light-emitting layer is formed by vapor-depositing tris (8-hydroxyquinolinato) aluminum (Alq) with 2% by mass of DCJTB to a thickness of 500 mm. Otherwise, a red light-emitting element D that emits red light was obtained in the same manner as described above (production of yellow light-emitting element B).

(白色発光素子Eの作製)
上記の青色発光素子Aの作製で用いたのと同じITO付きガラス基板40の上に、図7(b)の寸法の開口部42を設けたマスク43を用いて、電子注入層としてBCPとCsのモル比1:1の共蒸着層を50Å厚、電子輸送層としてAlqを150Å厚、発光層としてBH−2に[化1]に示す材料を4質量%ドープしたものを500Å厚、ホール輸送層としてα−NPDを600Å厚、ホール注入層としてα−NPDと酸化モリブデンを3:1の割合で共蒸着した層を150Å厚蒸着し、青色発光部を設けた。次いで、電子注入層としてBCPとCsのモル比1:1の共蒸着層を50Å厚、電子輸送層としてAlqを250Å厚、発光層としてBH−2に化2に示す材料を1.5質量%ドープしたものを500Å厚、ホール輸送層としてα−NPDを600Å厚、ホール注入層としてα−NPDと酸化モリブデンを3:1の割合で共蒸着した層を150Å厚蒸着し、黄色発光部を設けた。さらに電子注入層としてBCPとCsのモル比1:1の共蒸着層を50Å厚、電子輸送層としてAlqを150Å厚、発光層としてBH−2に[化1]に示す材料を4質量%ドープしたものを500Å厚、ホール輸送層としてα−NPDを600Å厚、ホール注入層としてα−NPDと酸化モリブデンを3:1の割合で共蒸着した層を200Å厚蒸着し、青色発光部を設けた。最後に図7(c)の寸法の開口部44を設けたマスク45を用いて厚み100Åの金を蒸着して陽極を形成し、また、厚み600ÅのLiFを保護層および電極と空気との中間的な屈折率を有する層として蒸着して、白色発光素子Eを得た。
(Preparation of white light emitting element E)
On the same glass substrate 40 with ITO as that used in the production of the blue light emitting element A, a mask 43 having an opening 42 having the dimensions shown in FIG. 7B is used, and BCP and Cs are used as electron injection layers. The co-deposited layer with a molar ratio of 1: 1 is 50 mm thick, the electron transport layer is 150 mm thick with Alq, the light emitting layer is BH-2 doped with 4% by mass of the material shown in [Chemical Formula 1], and the thickness is 500 mm thick. As a layer, α-NPD was deposited with a thickness of 600 mm, and as a hole injection layer, a layer in which α-NPD and molybdenum oxide were co-deposited at a ratio of 3: 1 was deposited with a thickness of 150 mm to provide a blue light emitting portion. Next, a co-deposited layer with a molar ratio of 1: 1 BCP and Cs as the electron injection layer is 50 mm thick, Alq is 250 mm thick as the electron transport layer, and BH-2 is used as the light emitting layer. The doped layer is 500 mm thick, α-NPD is 600 mm thick as the hole transport layer, and α-NPD and molybdenum oxide are co-deposited at a ratio of 3: 1 as the hole injection layer to 150 mm thick to provide a yellow light emitting part. It was. Furthermore, as the electron injection layer, a co-deposited layer with a 1: 1 molar ratio of BCP and Cs is 50 mm thick, Alq is 150 mm thick as the electron transport layer, and BH-2 is doped with 4% by mass of the material shown in [Chemical Formula 1] as the light emitting layer. The thickness was 500 mm thick, α-NPD was 600 mm thick as a hole transport layer, and a layer in which α-NPD and molybdenum oxide were co-deposited at a ratio of 3: 1 was vapor deposited as a hole injection layer to a thickness of 200 mm to provide a blue light emitting portion. . Finally, gold having a thickness of 100 mm is vapor-deposited using a mask 45 having an opening 44 having the dimensions shown in FIG. 7C to form an anode, and LiF having a thickness of 600 mm is formed between the protective layer, the electrode and air. The white light emitting device E was obtained by vapor deposition as a layer having a specific refractive index.

(白色発光素子Fの作製)
白色発光素子Eと同様に3種の発光層を形成し、最後の金電極の代わりに厚み800ÅのAlを蒸着して陽極を形成し、白色発光素子Fを得た。
(Preparation of white light emitting element F)
Three kinds of light emitting layers were formed in the same manner as the white light emitting element E, and an anode was formed by vapor-depositing Al having a thickness of 800 mm instead of the last gold electrode, whereby a white light emitting element F was obtained.

(実施例1)
上記の青色発光素子Aを真空蒸着装置にセットし、この青色発光素子Aの陰極の上に、図8(a)の寸法の開口部47を設けたマスク48を用いて、LiFを20μmの厚みで真空蒸着することによって、光が干渉を起こさない厚みの光透過性の絶縁層を形成した。次に、この絶縁層の上に、図8(b)の寸法の開口部49を設けたマスク50を用いて金を100Åの厚みで成膜して透明の陽極を形成し、さらにこの上に、図7(b)の寸法の開口部42を設けたマスク43を用いて、ホール注入層として「α−NPD」と酸化モリブデンを3:1の割合で共蒸着した層を1200Å厚、ホール輸送層として「α−NPD」を500Å厚、黄色発光の発光層として「BH−2」に[化2]に示す材料を4質量%ドープしたものを500Å厚、電子輸送層として「BCP」を50Å厚、電子注入層として「BCP」とCsのモル比1:1の共蒸着層を150Å厚、それぞれこの順に形成し、最後に図8(c)の寸法の開口部69を設けたマスク70を用いて、アルミニウムを800Å厚積層し、光反射性を有する陰極を形成することによって、青色発光素子Aの上に、光が干渉を起こさない厚みの光透過性の絶縁層を介して、黄色発光の黄色発光素子Gを積層した構造の、有機発光素子を得た(図1の構造参照)。
Example 1
The blue light-emitting element A is set in a vacuum vapor deposition apparatus, and LiF is formed to a thickness of 20 μm using a mask 48 provided with an opening 47 having the dimensions shown in FIG. 8A on the cathode of the blue light-emitting element A. A light-transmitting insulating layer having a thickness that does not cause interference of light was formed by vacuum deposition. Next, on this insulating layer, a transparent anode is formed by forming a gold film with a thickness of 100 mm using a mask 50 provided with an opening 49 having the dimensions shown in FIG. Using a mask 43 provided with an opening 42 having the dimensions shown in FIG. 7B, a layer in which “α-NPD” and molybdenum oxide are co-deposited at a ratio of 3: 1 is used as a hole injection layer in a thickness of 1200 mm, and the hole is transported. “Α-NPD” is 500 Å thick as a yellow light emitting layer, “BH-2” is doped with 4% by mass of the material shown in [Chemical Formula 2] as a yellow luminescent layer, and 500 Å is thick as “BCP” as an electron transport layer. As a thickness and electron injection layer, a co-deposited layer having a molar ratio of “BCP” and Cs of 1: 1 was formed in a thickness of 150 mm in this order, and finally a mask 70 provided with an opening 69 having the dimensions shown in FIG. Using aluminum, it has a thickness of 800 mm and has light reflectivity. An organic light emitting device having a structure in which a yellow light emitting device G emitting yellow light is laminated on a blue light emitting device A through a light-transmitting insulating layer having a thickness that does not cause interference. (See the structure in FIG. 1).

そしてこの有機発光素子において、図9のように、下の青色発光素子Aの陽極52と陰極53に電源54を接続し、また上の黄色発光素子Gの陽極55と陰極56に電源57を接続することによって、各素子A,Gの発光部にそれぞれ通電できるようにした。   In this organic light emitting device, as shown in FIG. 9, a power source 54 is connected to the anode 52 and the cathode 53 of the lower blue light emitting device A, and a power source 57 is connected to the anode 55 and the cathode 56 of the upper yellow light emitting device G. By doing so, the light emitting portions of the elements A and G can be energized.

(実施例2)
図10(a)に示すように、青色発光素子Aの発光部59の上に、黄色発光素子Bのガラス板60を、その発光部61と反対側の面で重ねることによって、150μm厚みのガラス板60で形成される光が干渉を起こさない厚みの光透過性の絶縁層を介して、青色発光素子Aと黄色発光素子Bを積層した構造の、有機発光素子を得た(図1の構造参照)。
(Example 2)
As shown in FIG. 10 (a), a glass plate 60 of yellow light-emitting element B is laminated on the light-emitting part 59 of the blue light-emitting element A on the surface opposite to the light-emitting part 61, whereby a glass having a thickness of 150 μm is obtained. An organic light-emitting element having a structure in which the blue light-emitting element A and the yellow light-emitting element B are stacked through a light-transmitting insulating layer having a thickness that does not cause interference with the light formed by the plate 60 was obtained (structure in FIG. 1). reference).

そしてこの有機発光素子において、図10(b)のように、青色発光素子Aの陽極52と陰極53に電源54を接続し、また黄色発光素子Bの陽極62と陰極63に電源64を接続することによって、各素子A,Bの発光部にそれぞれ通電できるようにした。   In this organic light emitting device, as shown in FIG. 10B, the power source 54 is connected to the anode 52 and the cathode 53 of the blue light emitting device A, and the power source 64 is connected to the anode 62 and the cathode 63 of the yellow light emitting device B. As a result, the light emitting portions of the elements A and B can be energized.

(実施例3)
青色発光素子AのITO付きガラス板40の、ITO形成面と反対側の面(発光部59を形成しなかった側の面)に、実施例1における透明電極である金の蒸着以降を、実施例1と同様にして行ない、黄色の発光素子Hを形成し、0.7mm厚のガラス板で形成される光が干渉を起こさない厚みの光透過性の絶縁層を介して、青色発光素子Aと黄色発光素子Hを積層した図11の構造の、有機発光素子を得た(図1の構造参照)。
(Example 3)
On the surface opposite to the ITO formation surface of the glass plate 40 with ITO of the blue light emitting element A (the surface on the side where the light emitting portion 59 was not formed), the deposition after gold deposition as a transparent electrode in Example 1 was performed. In the same manner as in Example 1, a yellow light-emitting element H is formed, and a blue light-emitting element A is formed through a light-transmitting insulating layer having a thickness that does not cause interference of light formed by a 0.7 mm-thick glass plate. An organic light emitting device having the structure of FIG. 11 in which the yellow light emitting device H and the yellow light emitting device H were stacked was obtained (see the structure of FIG. 1).

(実施例4)
白色発光素子Cと赤色発光素子Dを、実施例2と同様にして重ねることによって、150μm厚みのガラス板で形成される光が干渉を起こさない厚みの光透過性の絶縁層を介して、白色発光素子Cと赤色発光素子Dを積層した構造の、有機発光素子を得た(図1の構造参照)。
Example 4
By overlapping the white light emitting element C and the red light emitting element D in the same manner as in Example 2, the light formed by the glass plate having a thickness of 150 μm passes through a light-transmitting insulating layer having a thickness that does not cause interference. An organic light emitting device having a structure in which the light emitting device C and the red light emitting device D were laminated was obtained (see the structure in FIG. 1).

(実施例5)
実施例1において、LiFの絶縁層の代りに、CVDで形成した1000Å厚のSiON膜の上に、スリーボンド社製光硬化性樹脂「30Y−431」に粒径2μmと粒径4μmを1:1の重量比で混合した酸化チタン粒子を50質量%加えたものを、12μm厚でコートすると共に紫外線照射して硬化させて光散乱層を設けることによって、光散乱性の絶縁層を形成した。後は実施例1と同様にして、青色発光素子Aの上に、光散乱性の絶縁層を介して、黄色発光の発光素子Gを積層した構造の、有機発光素子を得た(図1の構造参照)。
(Example 5)
In Example 1, in place of the LiF insulating layer, a 3 μm-thick SiON film formed by CVD has a particle size of 2 μm and a particle size of 4 μm on a three-bond photocurable resin “30Y-431” of 1: 1. A light scattering insulating layer was formed by coating 50 wt% of titanium oxide particles mixed at a weight ratio of 12 wt. Thereafter, in the same manner as in Example 1, an organic light emitting device having a structure in which a yellow light emitting device G was laminated on a blue light emitting device A through a light scattering insulating layer was obtained (FIG. 1). See structure).

(実施例6)
青色発光素子Aを真空蒸着装置にセットし、図7(b)のマスクを用いて、青色発光素子Aの陰極の上に、電子注入層として「BCP」とCsのモル比1:1の共蒸着層を150Å厚、電子輸送層として「BCP」を50Å厚、発光層として「BH−2」に[化2]に示す材料を4質量%ドープしたものを500Å厚、ホール輸送層として「α−NPD」を400Å厚、ホール注入層として「α−NPD」と酸化モリブデンを3:1の割合で共蒸着した層を200Å厚、それぞれこの順に形成し、次いで図7(c)のマスクを用いて、800Å厚のIZOを光透過性の陽極として形成し、さらにこの上に500ÅのSiON膜をスパッタして光が干渉しない厚みの光透過性の絶縁層を形成すると共に、この上にスリーボンド社製光硬化性樹脂「30Y−431」を20μm厚でコートして硬化させ、最後に1000Å厚のAlを光反射層として設けることによって、青色発光素子Aと黄色発光素子Iを積層した、有機発光素子を得た(図3の絶縁層を設けていない構造参照)。尚、この有機発光素子において、青色発光素子Aと黄色発光素子Iの陰極は共通電極として用い、各素子の陽極にそれぞれ電源を接続した。
(Example 6)
The blue light-emitting element A is set in a vacuum deposition apparatus, and using the mask of FIG. 7B, the BCP and Cs molar ratio of 1: 1 is formed on the cathode of the blue light-emitting element A as an electron injection layer. The deposited layer is 150 mm thick, the electron transport layer is “BCP” is 50 mm thick, the light emitting layer is “BH-2” doped with 4% by mass of the material shown in [Chemical Formula 2], and the hole transport layer is “α” -NPD "has a thickness of 400 mm, and a layer in which" α-NPD "and molybdenum oxide are co-evaporated at a ratio of 3: 1 is formed as a hole injection layer in a thickness of 200 mm, and each is formed in this order, and then the mask of FIG. Then, 800 mm thick IZO is formed as a light transmissive anode, and further a 500 mm thick SiON film is sputtered thereon to form a light transmissive insulating layer having a thickness that does not interfere with light. Photo curable resin 30Y-431 "was coated with a thickness of 20 μm and cured, and finally 1000 mm thick Al was provided as a light reflecting layer to obtain an organic light emitting device in which the blue light emitting device A and the yellow light emitting device I were laminated (see FIG. 3 (see the structure in which the insulating layer is not provided). In this organic light emitting device, the cathodes of the blue light emitting device A and the yellow light emitting device I were used as a common electrode, and a power source was connected to the anode of each device.

(実施例7)
白色発光素子Eと赤色発光素子Dを、それぞれの基板面同士を屈折率1.5の接着剤を用いて発光面が重なる位置関係で積層して、有機発光素子を得た。
(Example 7)
The white light emitting element E and the red light emitting element D were laminated | stacked by the positional relationship with which the light emitting surface overlaps each substrate surface using the adhesive agent of refractive index 1.5, and the organic light emitting element was obtained.

そしてこの有機発光素子において、図12のように、赤色発光素子Dの陰極66と陽極67に電源68を接続し、また白色発光素子Eの陰極69と陽極70に電源71を接続することによって、各素子D,Eの発光部にそれぞれ通電できるようにした。なおこの時、発光は白色発光素子Eの陽極70である金電極を透過して得られる。   In this organic light emitting device, as shown in FIG. 12, a power source 68 is connected to the cathode 66 and the anode 67 of the red light emitting device D, and a power source 71 is connected to the cathode 69 and the anode 70 of the white light emitting device E. The light emitting portions of the elements D and E can be energized. At this time, light emission is obtained through the gold electrode which is the anode 70 of the white light-emitting element E.

(比較例1)
実施例1において、絶縁層であるLiFの膜厚を1000Åに設定するようにした他は、実施例1と同様にして有機発光素子を得た。
(Comparative Example 1)
In Example 1, an organic light emitting device was obtained in the same manner as in Example 1 except that the film thickness of LiF as an insulating layer was set to 1000 mm.

(比較例2)
実施例1において、LiFの絶縁層を形成しないようにした他は、実施例1と同様にして有機発光素子を得た。この有機発光素子では、青色発光素子Aの陰極と黄色発光の発光素子Gの陽極は電気的に結合されるため、電源の結線は青色発光素子Aの陽極と黄色発光の発光素子Gの陰極に行なった。
(Comparative Example 2)
In Example 1, an organic light emitting device was obtained in the same manner as in Example 1 except that the LiF insulating layer was not formed. In this organic light emitting device, since the cathode of the blue light emitting device A and the anode of the yellow light emitting device G are electrically coupled, the power source is connected to the anode of the blue light emitting device A and the cathode of the yellow light emitting device G. I did it.

(比較例3)
白色発光素子Fを単独で用いて、白色発光を得た。
(Comparative Example 3)
White light emitting element F was used alone to obtain white light emission.

上記のように実施例1〜7及び比較例1〜3で得た有機発光素子を、電源(KEITHLEY モデル2400)に接続して、定電流駆動を行ない、CIE色度をマルチチャンネルアナライザー(浜松ホトニクス社製「PMA−11」:測定距離25cm)を用いて測定した。実施例1〜6及び比較例1〜2においては、有機発光素子の正面からと、正面に対して45度の方向から、実施例7及び比較例3においては、有機発光素子の正面からと、正面に対して、20度、40度、60度の方向からスペクトル評価を行った。   As described above, the organic light-emitting devices obtained in Examples 1 to 7 and Comparative Examples 1 to 3 were connected to a power source (KEITHLEY model 2400), driven at a constant current, and CIE chromaticity was measured using a multichannel analyzer (Hamamatsu Photonics). It was measured using “PMA-11” manufactured by company: measuring distance 25 cm). In Examples 1 to 6 and Comparative Examples 1 and 2, from the front of the organic light emitting element, from the direction of 45 degrees with respect to the front, in Example 7 and Comparative Example 3, from the front of the organic light emitting element, Spectrum evaluation was performed from the direction of 20 degrees, 40 degrees, and 60 degrees with respect to the front.

そして、実施例1で得た有機発光素子について、正面から観測した際の色度座標のX値が0.30となるように通電したときの発光スペクトルを、正面方向から観察したものと45度の角度から観察したものを併せて図13(a)に示す。また発光強度比を種々変更した際の正面発光スペクトルの変化を図13(b)に示す。正面と45度の角度から観察したスペクトルの差は比較的小さく、正面からの色度は(0.30,0.39)、45度からの色度は(0.31,0.40)であった。また図13(c)のように発光強度比を変化させることによって、青色発光素子Aの発光色と黄色発光素子Gの発光色を結ぶ線上の任意の色調での発光が可能であることがわかる。尚、実施例4の有機発光素子では、発光色は白色と赤色を結ぶ線上の任意のものとすることが可能であった。   And about the organic light emitting element obtained in Example 1, the emission spectrum when energized so that the X value of the chromaticity coordinates when viewed from the front is 0.30 and 45 degrees observed from the front direction What was observed from the angle is shown in FIG. FIG. 13B shows changes in the front emission spectrum when various emission intensity ratios are changed. The difference in spectrum observed from the front and 45 degrees is relatively small, the chromaticity from the front is (0.30, 0.39), and the chromaticity from 45 degrees is (0.31, 0.40). there were. Further, by changing the emission intensity ratio as shown in FIG. 13C, it can be seen that light emission in an arbitrary color tone on the line connecting the emission color of the blue light emitting element A and the emission color of the yellow light emitting element G is possible. . In the organic light emitting device of Example 4, the emission color could be any on the line connecting white and red.

次に実施例7で得た有機発光素子において、白色発光素子Eのみを発光させたときの発光スペクトルを、正面、20度、40度、60度の方向から観測したものを図14(a)に示す。図14(a)にみられるように発光スペクトルの角度依存性が小さいことがわかる。また図14(b)に白色発光素子Eと赤色発光素子Dを任意の電流比で駆動した際の発光スペクトルの変化を示す。図14(b)にみられるように両者のスペクトルが任意に混合されたブロードな発光スペクトルが得られることがわかる。この時の発光色のCIE色度座標上での変化を図14(c)に示す。図14(c)にみられるように、発光色は、白色発光素子Eのそれと、赤色発光素子Dのそれとを結ぶ線近傍の任意のものを得ることが可能であった。   Next, in the organic light-emitting device obtained in Example 7, the emission spectrum observed when only the white light-emitting device E emits light is observed from the front, 20 degrees, 40 degrees, and 60 degrees directions as shown in FIG. Shown in As can be seen from FIG. 14A, the angle dependence of the emission spectrum is small. FIG. 14B shows a change in emission spectrum when the white light emitting element E and the red light emitting element D are driven at an arbitrary current ratio. As shown in FIG. 14B, it can be seen that a broad emission spectrum in which both spectra are arbitrarily mixed is obtained. FIG. 14C shows the change of the emission color on the CIE chromaticity coordinates at this time. As can be seen in FIG. 14 (c), it was possible to obtain any emission color in the vicinity of the line connecting that of the white light emitting element E and that of the red light emitting element D.

また、実施例7の有機発光素子を0度から80度の範囲で回転させた際の各角度に於ける発光色のCIE色度座標上での変化を、比較のために、比較例3で用いた白色発光素子Fの発光色のCIE色度座標上での変化と併せて、図15に示す。図15において「▲」「△」は、実施例7の素子を各条件で駆動させた場合に観測角度0〜80度の範囲で示す色度範囲をそれぞれ示したものである。また、「◇」は、比較例3の白色発光素子が0〜80度の範囲で示す色度範囲を示したものである。図15にみられるように実施例7の有機発光素子の発光色の観測角度による変化は、どの発光色に於いても非常に小さいことがわかる。これに対して、比較例3の白色発光素子は発光色の観測角度による変化は非常に大きいものである。   For comparison, the change in the CIE chromaticity coordinates of the emission color at each angle when the organic light-emitting device of Example 7 was rotated in the range of 0 to 80 degrees was compared with Comparative Example 3. Along with the change in the CIE chromaticity coordinates of the emission color of the white light emitting element F used, it is shown in FIG. In FIG. 15, “▲” and “Δ” indicate the chromaticity range indicated by the observation angle range of 0 to 80 degrees when the element of Example 7 is driven under each condition. Further, “◇” indicates the chromaticity range indicated by the white light emitting element of Comparative Example 3 in the range of 0 to 80 degrees. As can be seen from FIG. 15, the change of the emission color of the organic light emitting device of Example 7 according to the observation angle is very small in any emission color. On the other hand, the white light emitting element of Comparative Example 3 has a very large change in the emission color depending on the observation angle.

また、各実施例及び各比較例について、正面方向の色度と45度方向の色度の測定結果を表1にまとめて示す。尚、実施例7と比較例3については上記のように詳細に評価したので、表1には記載していない。   Moreover, about each Example and each comparative example, the measurement result of the chromaticity of a front direction and the chromaticity of a 45 degree direction is put together in Table 1, and is shown. Since Example 7 and Comparative Example 3 were evaluated in detail as described above, they are not described in Table 1.

Figure 2007115645
Figure 2007115645

表1の「色度の角度依存性」に評価を記すように、各実施例のものは発光色度の角度依存性は小さいが、各比較例のものは色度の角度依存性が大きいものであった。また表1の「色調調整」に評価を記すように、各実施例のものは積層された素子をそれぞれ駆動することができ、色調調整が可能であるが、比較例2のものは、2つの素子が電気的に接続されてしまうためにそれぞれの素子を駆動することができず、色調調整は不可能であった。   As shown in the evaluation in “Angle Dependency of Chromaticity” in Table 1, each example has a small angle dependency of emission chromaticity, but each comparative example has a large angle dependency of chromaticity. Met. In addition, as described in “Color tone adjustment” in Table 1, each of the examples can drive the stacked elements, and the color tone can be adjusted. Since the elements are electrically connected, each element cannot be driven, and color tone adjustment is impossible.

本発明に係る有機発光素子の層構成の一例を示すものであり、(a),(b)はそれぞれ概略図である。An example of the layer structure of the organic light emitting element which concerns on this invention is shown, (a), (b) is a schematic diagram, respectively. 本発明に係る有機発光素子の層構成の一例を示すものであり、(a),(b)はそれぞれ概略図である。An example of the layer structure of the organic light emitting element which concerns on this invention is shown, (a), (b) is a schematic diagram, respectively. 本発明に係る有機発光素子の層構成の一例を示すものであり、(a),(b)はそれぞれ概略図である。An example of the layer structure of the organic light emitting element which concerns on this invention is shown, (a), (b) is a schematic diagram, respectively. 本発明に係る有機発光素子の製造方法の一例を示すものであり、(a)〜(c)はそれぞれ概略図である。An example of the manufacturing method of the organic light emitting element which concerns on this invention is shown, (a)-(c) is schematic. 本発明に係る有機発光素子の製造方法の一例を示すものであり、(a),(b)はそれぞれ概略図である。An example of the manufacturing method of the organic light emitting element which concerns on this invention is shown, (a), (b) is schematic, respectively. 本発明に係る有機発光素子の製造方法の一例を示すものであり、(a)〜(c)はそれぞれ概略図である。An example of the manufacturing method of the organic light emitting element which concerns on this invention is shown, (a)-(c) is schematic. (a)は実施例に用いられるITO付きガラス基板の平面図、(b),(c)は実施例に用いられるマスクの平面図である。(A) is a top view of the glass substrate with ITO used for an Example, (b), (c) is a top view of the mask used for an Example. (a),(b),(c)は実施例に用いられるマスクの平面図である。(A), (b), (c) is a top view of the mask used for an Example. 実施例の有機発光素子の概略平面図である。It is a schematic plan view of the organic light emitting element of an Example. 実施例の有機発光素子を示すものであり、(a)は正面図、(b)は平面図である。The organic light emitting element of an Example is shown, (a) is a front view, (b) is a top view. 実施例の有機発光素子を示す正面図である。It is a front view which shows the organic light emitting element of an Example. 実施例の有機発光素子の概略平面図である。It is a schematic plan view of the organic light emitting element of an Example. (a)は実施例1の有機発光素子の発光スペクトルを示すグラフ、(b)は同上の発光強度比を種々変更した際の正面発光スペクトルの変化を示すグラフ、(c)は同上の発光強度比と色調の関係を示すグラフである。(A) is a graph showing the emission spectrum of the organic light emitting device of Example 1, (b) is a graph showing changes in the front emission spectrum when the emission intensity ratio is variously changed, and (c) is the emission intensity of the above. It is a graph which shows the relationship between a ratio and a color tone. (a)は実施例7の有機発光素子の発光スペクトルを示すグラフ、(b)は同上の白色発光素子と赤色発光素子を任意の電流比で発光させた際の発光スペクトルの変化を示すグラフ、(c)は同上の発光色のCIE色度座標上での変化を示すグラフである。(A) is a graph showing the emission spectrum of the organic light emitting device of Example 7, (b) is a graph showing the change in the emission spectrum when the white light emitting device and the red light emitting device are made to emit light at an arbitrary current ratio, (C) is a graph which shows the change in the CIE chromaticity coordinate of the luminescent color same as the above. 実施例7と比較例3の有機発光素子を0度から80度の範囲で回転させた際の各角度に於ける発光色のCIE色度座標上での変化を示すグラフである。It is a graph which shows the change on the CIE chromaticity coordinate of the luminescent color in each angle when the organic light emitting element of Example 7 and Comparative Example 3 is rotated in the range of 0 degree to 80 degrees. 従来例を示す概略図である。It is the schematic which shows a prior art example.

符号の説明Explanation of symbols

1 第1の電極
2 第2の電極
3 第1の発光層
4 第1の発光部
5 第3の電極
6 第4の電極
7 第2の発光層
8 第2の発光部
9 光透過性の絶縁層
10 光反射層
11 等電位面形成層・電荷発生層
12 第1の光透過性基板
13 第2の光透過性基板
14 光透過性の絶縁層
DESCRIPTION OF SYMBOLS 1 1st electrode 2 2nd electrode 3 1st light emitting layer 4 1st light emitting part 5 3rd electrode 6 4th electrode 7 2nd light emitting layer 8 2nd light emitting part 9 Light transmission insulation Layer 10 Light reflecting layer 11 Equipotential surface forming layer / charge generation layer 12 First light transmitting substrate 13 Second light transmitting substrate 14 Light transmitting insulating layer

Claims (7)

一対の電極の間に発光層を備えて形成される第1の発光部と、一対の電極の間に発光層を備えて形成される第2の発光部とを積層して形成される有機発光素子であって、上記の4つの電極のうち、外側に位置する電極の一方が光反射性を有する電極であると共に、他の総ての電極は光透過性であり、且つ、第1の発光部と第2の発光部の間に、光反射性の電極を有しない側の発光部の発光層で発光した光が干渉を起こさない厚みの、あるいは、この発光層で発光した光を散乱させる、光透過性の絶縁層を備えて成ることを特徴とする有機発光素子。   Organic light emission formed by laminating a first light emitting part formed with a light emitting layer between a pair of electrodes and a second light emitting part formed with a light emitting layer between a pair of electrodes Among the above four electrodes, one of the electrodes located outside is an electrode having light reflectivity, and all the other electrodes are light transmissive, and the first light emission The light emitted from the light emitting layer of the light emitting part on the side not having the light-reflecting electrode is scattered between the light emitting part and the second light emitting part, or the light emitted from this light emitting layer is scattered. An organic light emitting device comprising a light transmissive insulating layer. 一対の電極の間に発光層を備えて形成される第1の発光部と、一対の電極の間に発光層を備えて形成される第2の発光部とを積層して形成される有機発光素子であって、上記の4つの総ての電極が光透過性であると共に、外側に位置する電極のうち一方の電極の外側に光反射性を有する光反射層を有し、且つ、第1の発光部と第2の発光部の間に、光反射層を有しない側の発光部の発光層で発光した光が干渉を起こさない厚みの、あるいは、この発光層で発光した光を散乱させる、光透過性の絶縁層を備えて成ることを特徴とする有機発光素子。   Organic light emission formed by laminating a first light emitting part formed with a light emitting layer between a pair of electrodes and a second light emitting part formed with a light emitting layer between a pair of electrodes An element having a light reflecting layer on the outside of one of the electrodes located on the outside, and having a light reflecting layer having a light reflecting property; The light emitted from the light emitting layer of the light emitting part on the side not having the light reflecting layer is scattered between the light emitting part and the second light emitting part, or the light emitted from the light emitting layer is scattered. An organic light emitting device comprising a light transmissive insulating layer. 一対の電極の間に発光層を備えて形成される第1の発光部と、一対の電極の間に発光層を備えて形成される第2の発光部とを積層して形成される有機発光素子であって、上記の4つの総ての電極が光透過性であり、且つ、外側に位置する電極のうち一方の電極の外側に、第1及び第2の発光部の発光層で発光した光が干渉を起こさない厚みの、あるいは、これらの発光層で発光した光を散乱させる、光透過性の絶縁層を介して、光反射性を有する光反射層を備えて成ることを特徴とする有機発光素子。   Organic light emission formed by laminating a first light emitting part formed with a light emitting layer between a pair of electrodes and a second light emitting part formed with a light emitting layer between a pair of electrodes All four electrodes described above are light transmissive, and light is emitted from the light emitting layers of the first and second light emitting portions outside one of the electrodes located outside. It is characterized by comprising a light reflecting layer having a light reflecting property through a light-transmitting insulating layer that scatters light emitted from these light emitting layers or has a thickness that does not cause interference with light. Organic light emitting device. 第1及び第2の発光部のうち少なくとも一方が、等電位面を形成する層もしくは電荷発生層を介して積層される複数の発光層を、電極間に備えて形成されていることを特徴とする請求項1乃至3のいずれかに記載の有機発光素子。   It is characterized in that at least one of the first and second light emitting portions is formed with a plurality of light emitting layers that are stacked via a layer that forms an equipotential surface or a charge generation layer between electrodes. The organic light emitting device according to any one of claims 1 to 3. 発光層で発光した光が干渉を起こさない厚みの光透過性の絶縁層、発光層で発光した光を散乱させる光透過性の絶縁層が、ガラス板もしくはフィルムで形成されていることを特徴とする請求項1乃至4のいずれかに記載の有機発光素子。   A light-transmitting insulating layer having a thickness that does not cause interference of light emitted from the light-emitting layer and a light-transmitting insulating layer that scatters light emitted from the light-emitting layer are formed of a glass plate or a film. The organic light emitting element according to any one of claims 1 to 4. 請求項1乃至5のいずれかに記載の有機発光素子を製造するにあたって、発光層で発光した光が干渉を起こさない厚みの、あるいは、発光層で発光した光を散乱させる、第1の光透過性基板の表面に、電極、発光層、電極をこの順に積層して第1と第2のいずれか一方の発光部を形成する工程と、第2の光透過性基板の表面に、電極、発光層、電極をこの順に積層して第1と第2のいずれか他方の発光部を形成する工程と、第1の光透過性基板に、第2の光透過性基板に形成した発光部を積層することによって、2つの発光部を第1の光透過性基板を介して積層する工程と、を備えることを特徴とする有機発光素子の製造方法。   In manufacturing the organic light-emitting device according to any one of claims 1 to 5, the first light transmission that scatters the light emitted from the light-emitting layer with a thickness that does not cause interference or the light emitted from the light-emitting layer. A step of laminating an electrode, a light emitting layer, and an electrode in this order on the surface of the transparent substrate to form one of the first and second light emitting portions, and an electrode, light emission on the surface of the second light transmissive substrate A layer and an electrode are laminated in this order to form either the first or second light emitting part, and the light emitting part formed on the second light transmissive substrate is laminated on the first light transmissive substrate. And a step of laminating the two light emitting portions via the first light transmissive substrate. A method for manufacturing an organic light emitting element, comprising: 請求項1乃至5のいずれかに記載の有機発光素子を製造するにあたって、発光層で発光した光が干渉を起こさない厚みの、あるいは、発光層で発光した光を散乱させる、光透過性基板の表面に、電極、発光層、電極をこの順に積層して第1と第2のいずれか一方の発光部を形成する工程と、上記光透過性基板の発光部を形成した反対側の表面に、電極、発光層、電極をこの順に積層して第1と第2のいずれか他方の発光部を形成する工程と、を備えることを特徴とする有機発光素子の製造方法。   In manufacturing the organic light emitting device according to any one of claims 1 to 5, a light transmissive substrate having a thickness that does not cause interference with light emitted from the light emitting layer or scatters light emitted from the light emitting layer. On the surface, an electrode, a light emitting layer, and an electrode are laminated in this order to form one of the first and second light emitting portions, and on the opposite surface on which the light emitting portion of the light transmitting substrate is formed, And a step of laminating an electrode, a light emitting layer, and an electrode in this order to form either the first or the second light emitting portion, and a method for producing an organic light emitting element.
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