JP5730547B2 - See-through organic EL device and manufacturing method thereof - Google Patents
See-through organic EL device and manufacturing method thereof Download PDFInfo
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Description
本発明は、面光源として有機層を備えた発光部材、すなわち、主として照明を対象とした有機エレクトロルミネッセント（以下、「ＥＬ」と略することがある。）装置に関する。 The present invention relates to a light-emitting member having an organic layer as a surface light source, that is, an organic electroluminescent (hereinafter sometimes abbreviated as “EL”) device mainly for illumination.
有機ＥＬ装置は電気エネルギーを光エネルギーに変換する半導体素子である。近年、有機ＥＬ装置を用いた研究が加速的に行われるようになっており、すでに一部の照明分野では実用化が始まっている。 An organic EL device is a semiconductor element that converts electrical energy into light energy. In recent years, research using organic EL devices has been accelerated, and commercialization has already started in some lighting fields.
有機ＥＬ装置は、電力を投入するために少なくとも２つの電極を備えており、その電極に挟まれた有機層が光を発する。この有機ＥＬ装置を発光装置として利用するためには、その光を外部に取り出す必要があり、そのため、少なくとも一方の電極は透光性である必要がある。この透光性の電極材料として、ＡｇやＡｕ等の金属の極薄膜や、インジウム等をドープした酸化錫、アルミニウム等をドープした酸化亜鉛等の金属酸化物に代表される透光性の導電材料が用いられる。もう一方の電極は、電極の抵抗を下げるため、また有機層で発生した光を反射させ外部への光の取り出しの効率を上げるため、ＡｇやＡｌ等の金属膜が用いられる。ところが、金属膜は遮光性があるため有機ＥＬ装置には透光性がなく、外部の光を通すことができない。 The organic EL device includes at least two electrodes for supplying power, and an organic layer sandwiched between the electrodes emits light. In order to use this organic EL device as a light emitting device, it is necessary to extract the light to the outside, and therefore, at least one of the electrodes needs to be translucent. As this translucent electrode material, a translucent conductive material typified by a metal oxide such as an ultra-thin metal such as Ag or Au, tin oxide doped with indium or the like, zinc oxide doped with aluminum or the like Is used. The other electrode is made of a metal film such as Ag or Al in order to reduce the resistance of the electrode or to reflect light generated in the organic layer and increase the efficiency of extracting light to the outside. However, since the metal film has a light-shielding property, the organic EL device does not transmit light and cannot pass external light.
この有機ＥＬ装置に透光性がないということに起因して、その応用範囲は限定的にならざるを得ない。例えば、住宅用の照明に応用する場合を考える。天井や壁に有機ＥＬ装置を照明として使用する場合、もともと天井や壁には透光性はないことから有機ＥＬ装置にも透光性は不要であり、従ってそのまま応用が可能である。ところが、天窓や窓に応用を考える場合、天窓や窓は外光を取り込む必要があるため、透光性のない有機ＥＬ装置は使用することができない。逆に、もし有機ＥＬ装置に透光性があり、天窓や窓に使用すれば、図３に模式的に示すように、昼間は透光性を利用して外光を室内に取り込み、夜は照明として使用する、という応用が生まれる。 Due to the lack of translucency in this organic EL device, its application range must be limited. For example, consider the case of application to residential lighting. When the organic EL device is used for illumination on the ceiling or wall, the organic EL device is not required to transmit light because the ceiling or wall originally has no light transmitting property, and thus can be applied as it is. However, when considering application to skylights and windows, the skylights and windows need to take in external light, and thus organic EL devices that do not transmit light cannot be used. Conversely, if the organic EL device has translucency and is used for a skylight or a window, as shown schematically in FIG. 3, outside light is taken into the room using the translucency in the daytime, and at night. The application of using as lighting is born.
この有機ＥＬ装置に透光性がないという問題を解決する方法として、遮光性の電極材料の代わりに透光性の電極材料を用い、有機層に電力を供給する両側の電極を透光性の材料にする方法がある。これにより、有機ＥＬ装置は透光性を持ち、外部の光を通すことができる。しかし、発光装置とする場合、両側の電極に透光性があるため、有機層で発せられた光は必然的に両側の電極から放射されてしまい、原理的に片側だけに光を放射することはできない。これでは、前記のように天窓や窓へ有機ＥＬ装置を応用する例では、外部を照らすことになるという問題がある。 As a method for solving the problem that the organic EL device does not have translucency, a translucent electrode material is used instead of the light-shielding electrode material, and the electrodes on both sides for supplying power to the organic layer are made translucent. There is a way to make it a material. Thereby, the organic EL device has translucency and can transmit external light. However, in the case of a light emitting device, since the electrodes on both sides are translucent, the light emitted from the organic layer is inevitably emitted from the electrodes on both sides, and in principle, light is emitted only to one side. I can't. In this case, in the example in which the organic EL device is applied to the skylight or the window as described above, there is a problem that the outside is illuminated.
本発明は、外観上平均化して一様に透過して見える透光性を有し、かつ不要な方面への照射が抑制され、さらに、透光性の第１の導電性電極層の抵抗に起因する問題の発生が抑制された有機ＥＬ装置、並びに製造方法を提供することを目的とする。本発明は、所謂、透光性のある（以下「シースルー」と呼ぶこともある）有機ＥＬ装置の提供を目的とする。 The present invention has a light- transmitting property that is averaged in appearance and appears to be transmitted uniformly , and irradiation to unnecessary areas is suppressed , and further, the resistance of the light-transmitting first conductive electrode layer is reduced. An object of the present invention is to provide an organic EL device and a manufacturing method in which occurrence of problems due to the suppression is suppressed . An object of the present invention is to provide a so-called translucent (hereinafter also referred to as “see-through”) organic EL device.
本発明者らは上記課題に鑑み鋭意検討した結果、以下の構成により上記課題を解決できることを見出し、本発明を完成するに至った。 As a result of intensive studies in view of the above problems, the present inventors have found that the above problems can be solved by the following configuration, and have completed the present invention.
即ち、本発明は、透光性基板上に少なくとも透光性部材により構成される第１の導電性電極層、有機発光層を含む複数の化合物層からなる積層体層、遮光性部材により構成される第２の導電性電極層が順次積層され、外観上平均化して一様に透過して見えるように、均等に配置された透過領域であって、該第２の導電性電極層の部分的不在により構成された透過領域を含むシースルー有機ＥＬ装置であって、発光部分が複数の単位発光素子に分割され、かつ、複数の該単位発光素子が電気的に直列に接続されており、前記第２の導電性電極層の総面積のうち２乃至４０％の範囲に設けられた可視光を５０％以上透過する領域が該透過領域に相当し、かつ、前記第１の導電性電極層が連続して存在する領域が該透過領域に相当し、さらに、該単位発光素子の各領域内において、複数箇所に該第２の導電性電極の部分的不在による透過領域が形成されていることを特徴とするシースルー有機ＥＬ装置、即ち、本発明の発光部材に関する。 That is, the present invention includes a first conductive electrode layer composed of at least a translucent member on a translucent substrate, a laminate layer composed of a plurality of compound layers including an organic light emitting layer, and a light shielding member. The second conductive electrode layers are sequentially laminated, and are uniformly transmissive regions so that they can be seen through evenly after averaging in appearance, and a part of the second conductive electrode layers A see-through organic EL device including a transmissive region configured by absence , wherein a light emitting portion is divided into a plurality of unit light emitting elements, and the plurality of unit light emitting elements are electrically connected in series, A region that transmits 50% or more of visible light provided in a range of 2 to 40% of the total area of the two conductive electrode layers corresponds to the transmissive region, and the first conductive electrode layer is continuous. and regions present corresponds to the transparent over-region, further, the unit In each region of the light emitting elements, the see-through organic EL device, wherein the transmission region by partial absence of the second conductive electrode is formed at a plurality of locations, i.e., a light emitting member of the present invention.
好ましい実施態様は、前記可視光を５０％以上透過する領域の少なくとも一部が、直径１０μｍ以上１ｍｍ以下の複数の概略円であることを特徴とする前記の発光部材に関する。 In a preferred embodiment, the light-emitting member is characterized in that at least a part of the region that transmits 50% or more of visible light is a plurality of approximate circles having a diameter of 10 μm to 1 mm.
好ましい実施態様は、前記可視光を５０％以上透過する領域の少なくとも一部が、幅１０μｍ以上１ｍｍ以下の溝であることを特徴とする前記の発光部材に関する。 A preferred embodiment relates to the light-emitting member, wherein at least a part of the region that transmits 50% or more of visible light is a groove having a width of 10 μm or more and 1 mm or less.
好ましい実施態様は、前記第２の導電性電極層の積層体層とは反対側の面に接して、樹脂バインダーを含有する着色層を形成されてなる発光部材に関する。 A preferred embodiment relates to a light emitting member in which a colored layer containing a resin binder is formed in contact with the surface of the second conductive electrode layer opposite to the laminate layer.
好ましい実施態様は、前記透光性基板と透光性の封止板で、第１の導電性電極層、積層体層および第２の導電性電極層を挟み込み、少なくとも前記第２の導電性電極層と透光性の封止板の間に、透光性の樹脂が充填されていることを特徴とする前記の発光部材に関する。 In a preferred embodiment, the light-transmitting substrate and the light-transmitting sealing plate sandwich the first conductive electrode layer, the laminated body layer, and the second conductive electrode layer, and at least the second conductive electrode. The light-emitting member is characterized in that a light-transmitting resin is filled between the layer and the light-transmitting sealing plate.
好ましい実施態様は、発光部分が複数に分割され、かつ電気的に直列に接続されていることを特徴とする前記の発光部材に関する。 A preferred embodiment relates to the light-emitting member, wherein the light-emitting portion is divided into a plurality of parts and electrically connected in series.
本発明は、透光性基板上に少なくとも透光性部材により構成される第１の導電性電極層、有機発光層を含む複数の化合物層からなる積層体層、遮光性部材により構成される第２の導電性電極層を順次積層され、外観上平均化して一様に透過して見えるように、均等に配置された透過領域であって、該第２の導電性電極層の部分的不在により構成された透過領域を含むシースルー有機ＥＬ装置の製造方法であって、発光部分が複数の単位発光素子に分割され、かつ、複数の該単位発光素子が電気的に直列に接続されており、前記第２の導電性電極層を積層する際に、その総面積のうち２乃至４０％の範囲に設けられた可視光を５０％以上透過する領域が該透過領域に相当し、かつ、前記第１の導電性電極層が連続して存在する領域が該透過領域に相当し、さらに、該単位発光素子の各領域内において、複数箇所に該第２の導電性電極の部分的不在による透過領域が形成されるように、第２の導電性電極層の一部の領域の膜形成を遮断することを特徴とするシースルー有機ＥＬ装置の製造方法に関する。 The present invention provides a first conductive electrode layer composed of at least a translucent member on a translucent substrate, a laminate layer composed of a plurality of compound layers including an organic light emitting layer, and a first composed of a light shielding member. Two conductive electrode layers are sequentially laminated, and are uniformly arranged so that they appear to be uniformly transmitted through averaging in appearance, due to the partial absence of the second conductive electrode layer. A method of manufacturing a see-through organic EL device including a configured transmission region , wherein a light emitting portion is divided into a plurality of unit light emitting elements, and the plurality of unit light emitting elements are electrically connected in series, When the second conductive electrode layer is stacked, a region that transmits 50% or more of visible light provided in a range of 2 to 40% of the total area corresponds to the transmission region, and the first The region where the conductive electrode layer continuously exists is the transmission region Corresponds to, further, in each region of the unit light-emitting element, a so that the transmission region by partial absence of the second conductive electrode is formed at a plurality of positions, a portion of the second conductive electrode layer The present invention relates to a method for manufacturing a see-through organic EL device, wherein the film formation in a region is blocked.
本発明は、透光性基板上に少なくとも透光性部材により構成される第１の導電性電極層、有機発光層を含む複数の化合物層からなる積層体層、遮光性部材により構成される第２の導電性電極層を順次積層され、外観上平均化して一様に透過して見えるように、均等に配置された透過領域であって、該第２の導電性電極層の部分的不在により構成された透過領域を含むシースルー有機ＥＬ装置の製造方法であって、発光部分が複数の単位発光素子に分割され、かつ、複数の該単位発光素子が電気的に直列に接続されており、前記第２の導電性電極層を積層した後に、その総面積のうち２乃至４０％の範囲に設けられた可視光を５０％以上透過する領域が該透過領域に相当し、かつ、前記第１の導電性電極層が連続して存在する領域が該透過領域に相当し、さらに、該単位発光素子の各領域内において、複数箇所に該第２の導電性電極の部分的不在による透過領域が形成されるように、前記第２の導電性電極層の一部を除去することを特徴とするシースルー有機ＥＬ装置の製造方法に関する。
The present invention provides a first conductive electrode layer composed of at least a translucent member on a translucent substrate, a laminate layer composed of a plurality of compound layers including an organic light emitting layer, and a first composed of a light shielding member. Two conductive electrode layers are sequentially laminated, and are uniformly arranged so that they appear to be uniformly transmitted through averaging in appearance, due to the partial absence of the second conductive electrode layer. A method of manufacturing a see-through organic EL device including a configured transmission region , wherein a light emitting portion is divided into a plurality of unit light emitting elements, and the plurality of unit light emitting elements are electrically connected in series, After laminating the second conductive electrode layer, a region that transmits 50% or more of visible light provided in a range of 2 to 40% of the total area corresponds to the transmission region, and the first The region where the conductive electrode layer continuously exists is the transmission region Corresponds to, further, in each region of the unit light-emitting element, a so that the transmission region by partial absence of the second conductive electrode is formed at a plurality of positions, a portion of the second conductive electrode layer The present invention relates to a method for manufacturing a see-through organic EL device, characterized by removing the light.
好ましい実施態様は、前記の第２の導電性電極層の一部を除去する手段が、透光性基板側からレーザービームを照射する手段であることを特徴とする前記の発光部材の製造方法に関する。 In a preferred embodiment, the means for removing a part of the second conductive electrode layer is a means for irradiating a laser beam from the translucent substrate side. .
好ましい実施態様は、前記第２の導電性電極層の一部を除去する手段を、複数のレーザービームを同時に照射する手段とすることに関する。 In a preferred embodiment, the means for removing a part of the second conductive electrode layer is a means for simultaneously irradiating a plurality of laser beams.
好ましい実施態様は、前記可視光を５０％以上透過する領域が、直径１０μｍ以上１ｍｍ以下の複数の概略円を含んで形成されることを特徴とする前記の発光部材の製造方法に関する。 A preferred embodiment relates to the method for manufacturing the light-emitting member, wherein the region that transmits 50% or more of visible light includes a plurality of approximate circles having a diameter of 10 μm to 1 mm.
好ましい実施態様は、前記可視光を５０％以上透過する領域が、幅１０μｍ以上１ｍｍ以下の溝を含んで形成されることを特徴とする前記の発光部材の製造方法に関する。 A preferred embodiment relates to the method for manufacturing a light emitting member, wherein the region that transmits 50% or more of visible light includes a groove having a width of 10 μm or more and 1 mm or less.
好ましい実施態様は、前記の方法により第２の導電性電極層を積層した後、透光性の樹脂と透光性の封止板を用いて、前記第１の導電性電極層、前記積層体層および前記第２の導電性電極層を封止することを特徴とする発光部材の製造方法に関する。 In a preferred embodiment, after the second conductive electrode layer is laminated by the above-described method, the first conductive electrode layer and the laminate are formed using a translucent resin and a translucent sealing plate. It is related with the manufacturing method of the light emitting member characterized by sealing a layer and said 2nd conductive electrode layer.
本発明により、外観上平均化して一様に透過して見える透光性を有し、かつ不要な方面への照射が抑制され、さらに、透光性の第１の導電性電極層の抵抗に起因する問題の発生が抑制された有機ＥＬ装置を提供することが可能となり、その応用範囲を広げることができる。 According to the present invention, it has a light- transmitting property that is averaged in appearance and appears to be transmitted uniformly , and irradiation to unnecessary areas is suppressed , and further, the resistance of the light-transmitting first conductive electrode layer is reduced. It is possible to provide an organic EL device in which the occurrence of problems due to the suppression is suppressed , and the application range can be expanded.
本発明が対象としているのは、例えばガラスや高分子フィルム等に代表される透光性基板上に、第１の電極となる透光性導電層が形成され、その上に発光層を含む複数の各種有機化合物層と、裏面（第２）電極となる遮光性の電極層が形成されたいわゆるボトムエミッション型の有機ＥＬ装置である。より具体的には、本発明は、透光性基板上に少なくとも透光性部材により構成される第１の導電性電極層、有機発光層を含む複数の化合物層からなる積層体層、遮光性部材により構成される第２の導電性電極層が順次積層された発光部材（有機ＥＬ装置）であって、前記第２の導電性電極層が、その総面積のうち２乃至４０％の範囲に可視光を５０％以上透過する領域を含むことを特徴とする発光部材（有機ＥＬ装置）である。以下、本発明について詳細に説明する。 The present invention is directed to a plurality of light-transmitting layers including a light-emitting layer formed on a light-transmitting conductive layer serving as a first electrode on a light-transmitting substrate typified by glass or a polymer film, for example. This is a so-called bottom emission type organic EL device in which a light-shielding electrode layer serving as a back (second) electrode is formed. More specifically, the present invention relates to a first conductive electrode layer composed of at least a light-transmitting member on a light-transmitting substrate, a laminate layer composed of a plurality of compound layers including an organic light-emitting layer, and a light shielding property. A light-emitting member (organic EL device) in which second conductive electrode layers composed of members are sequentially stacked, and the second conductive electrode layer is in a range of 2 to 40% of the total area. A light-emitting member (organic EL device) including a region that transmits 50% or more of visible light. Hereinafter, the present invention will be described in detail.
本発明において、透光性基板や透光性部材における「透光性」とは光を透過する性質を有することを意味し、具体的には、発光領域の可視光域（波長領域３８０〜７８０ｎｍ）における透過率が５０％以上であればよい。以下、特に断らない限り「透光性」は上記の意味として用いる。 In the present invention, “translucency” in a translucent substrate or translucent member means having a property of transmitting light, specifically, a visible light region (wavelength region of 380 to 780 nm) of a light emitting region. The transmittance | permeability in 50) should just be 50% or more. Hereinafter, unless otherwise specified, “translucency” is used as the above meaning.
前記透光性基板としては特に制限されず、公知のものを使用できる。例えば、アルカリガラス、ホウ珪酸ガラス、無アルカリガラスなどのガラス基板、サファイヤ基板、アクリル樹脂、ポリエステル樹脂、ポリカーボネート樹脂、ポリオレフィン樹脂、シクロオレフィンポリマーなどの透光性の高分子フィルム基板などを用いることができる。透光性基板の透過率は、発光する光のロスを減少する観点から、可視光域における透過率が８０％以上であることが好ましく、さらに好ましくは９５％以上である。 The translucent substrate is not particularly limited, and a known substrate can be used. For example, a glass substrate such as alkali glass, borosilicate glass or non-alkali glass, a sapphire substrate, a transparent polymer film substrate such as an acrylic resin, a polyester resin, a polycarbonate resin, a polyolefin resin, or a cycloolefin polymer may be used. it can. The transmittance of the translucent substrate is preferably 80% or more, more preferably 95% or more in the visible light region, from the viewpoint of reducing the loss of light emitted.
本発明の発光部材における第１の導電性電極層（以下、透光性導電層ともいう）は透光性部材により構成される。より具体的には、第１の導電性電極層は、ＩＴＯ（酸化インジウム錫）、ＳｎＯ２（酸化錫）、ＺｎＯ（酸化亜鉛）などに代表される透光性部材から構成された透光性導電層であることが好ましい。中でも、製膜およびパターニングの容易性の観点から、本発明の発光部材においてはＩＴＯがより好ましい。なお、導電性を補うために透光性導電層の下または上に遮光性の金属グリッド層を配してもよいが、このような部分透光性の第１の導電性電極層を用いる場合でも本発明を適用することができる。また、前記第1の導電性電極層中には、必要に応じて、例えばアルミニウム、ガリウム、ケイ素、ホウ素、ニオブなどの１種以上のドーパントがドーピングされていてもよい。前記第１の導電性電極層の透過率は、透明性の観点から、可視光域における透過率が７０％以上であることが好ましく、さらに好ましくは８０％以上であり、特に好ましくは９０％以上である。 The 1st electroconductive electrode layer (henceforth a translucent conductive layer) in the light emitting member of this invention is comprised by the translucent member. More specifically, the first conductive electrode layer is made of a translucent member represented by ITO (indium tin oxide), SnO 2 (tin oxide), ZnO (zinc oxide), or the like. A conductive layer is preferred. Among these, from the viewpoint of film formation and patterning ease, ITO is more preferable in the light emitting member of the present invention. In order to supplement conductivity, a light-shielding metal grid layer may be disposed under or on the light-transmitting conductive layer. However, when such a partially light-transmitting first conductive electrode layer is used. However, the present invention can be applied. The first conductive electrode layer may be doped with one or more dopants such as aluminum, gallium, silicon, boron, and niobium, if necessary. From the viewpoint of transparency, the transmittance of the first conductive electrode layer is preferably such that the transmittance in the visible light region is 70% or more, more preferably 80% or more, and particularly preferably 90% or more. It is.
本発明において、透光性基板上に透光性の第１の導電性電極層を積層する方法については特に制限されず、例えば、スパッタ法や熱ＣＶＤ法等により形成することができる。 In the present invention, the method for laminating the translucent first conductive electrode layer on the translucent substrate is not particularly limited, and can be formed by, for example, a sputtering method or a thermal CVD method.
次に、上記透光性の第１の導電性電極層の上に、有機発光層を含む複数の化合物層からなる積層体層が形成される。当該積層体層は、例えば、複数の有機化合物層から構成されており、いわゆる発光層のほかに、電子注入層、電子輸送層、正孔注入層、正孔輸送層等が含まれてもよい。また、これらの層は多くは接合を成すが、これら有機化合物層には複数の接合が含まれていてもよいし、これら多接合で良好な性能を得るために電荷発生層等を含んでいてもよい。より具体的には、これらの有機化合物層の中に一部薄膜のアルカリ金属層を含んでもよいし、無機層を含むこともできる。 Next, a laminate layer composed of a plurality of compound layers including an organic light emitting layer is formed on the translucent first conductive electrode layer. The laminate layer is composed of, for example, a plurality of organic compound layers, and may include an electron injection layer, an electron transport layer, a hole injection layer, a hole transport layer, and the like in addition to a so-called light emitting layer. . In addition, many of these layers form a bond, but these organic compound layers may include a plurality of bonds, or include a charge generation layer or the like in order to obtain good performance with these multiple bonds. Also good. More specifically, these organic compound layers may partially include a thin alkali metal layer or an inorganic layer.
上記有機発光層については公知の有機発光層を適用でき、例えば、ホール輸送層として真空蒸着法により形成された４，４’−ビス［Ｎ−（２−ナフチル）−Ｎ−フェニル−アミノ］ビフェニル上に、電子輸送層を兼ねて、真空蒸着法により７０ｎｍの厚みで形成される［トリス（８−ハイドロキシキノリナート）］アルミニウム(ＩＩＩ)などがあげられる。 As the organic light emitting layer, a known organic light emitting layer can be applied. For example, 4,4′-bis [N- (2-naphthyl) -N-phenyl-amino] biphenyl formed by a vacuum deposition method as a hole transport layer. In addition, [tris (8-hydroxyquinolinato)] aluminum (III), which is also used as an electron transport layer and is formed with a thickness of 70 nm by a vacuum deposition method, can be given.
前記の複数の化合物層からなる積層体層を形成する方法は公知の方法を用いることができる。例えば、低分子有機化合物等を蒸着法で形成してもよいし、高分子有機化合物の場合は印刷等で形成することも可能である。さらに金属層や金属酸化物層を形成する場合は、スパッタ、化学気相堆積法（ＣＶＤ）等の方法で形成することも可能である。適宜それぞれの層に適切な形成法を選択すればよい。 A known method can be used as a method of forming the laminate layer composed of the plurality of compound layers. For example, a low molecular organic compound or the like may be formed by an evaporation method, and in the case of a high molecular organic compound, it may be formed by printing or the like. Further, when a metal layer or a metal oxide layer is formed, it can be formed by a method such as sputtering or chemical vapor deposition (CVD). An appropriate formation method may be selected for each layer as appropriate.
本発明の発光部材（有機ＥＬ装置）においては、前記の有機発光層を含む複数の化合物層からなる積層体層の上に、遮光性部材により構成される第２の導電性電極層が積層される。有機ＥＬ装置は、電力を投入するために少なくとも２つの電極を備えており、その電極に挟まれた有機層が光を発する装置である。この有機ＥＬ装置を発光装置として利用するためには、その光を外部に取り出す必要があり、そのため、少なくとも一方の電極は前述のごとく透光性である必要がある。しかしながら、もう一方（裏面）の電極は電力を投入するためには必要であるが、必ずしも透光性である必要はない。そのため、透光性導電層として先に例示したＩＴＯ等を用いることも可能であれば、遮光性を有する導電層としてＡｇに代表される金属層を用いることも可能である。 In the light-emitting member (organic EL device) of the present invention, a second conductive electrode layer composed of a light-shielding member is laminated on a laminate layer composed of a plurality of compound layers including the organic light-emitting layer. The An organic EL device includes at least two electrodes for supplying power, and an organic layer sandwiched between the electrodes emits light. In order to use this organic EL device as a light-emitting device, it is necessary to extract the light to the outside. Therefore, at least one of the electrodes needs to be translucent as described above. However, the other electrode (rear surface) is necessary for supplying power, but is not necessarily translucent. Therefore, if it is possible to use ITO or the like exemplified above as the light-transmitting conductive layer, it is also possible to use a metal layer typified by Ag as the conductive layer having a light shielding property.
ところが、一般的に透光性の導電層は、金属層に比べて電気抵抗が高く、この抵抗による発熱によって発光効率の低下や、素子劣化、輝度分布の拡大等の問題が顕在化しやすい傾向がある。また、裏面にも透光性導電層を用いた場合は発光層で生じた光は両側に放出されるため、例えば片側のみを照らしたい場合には、反対側に無駄な光が放出されることになる。加えて、金属膜のような光の反射が起きないため、発光効率が極めて悪くなる傾向がある。以上より、本発明において第２の導電性電極層には、電気抵抗が低く、光の反射がよい、金属膜のような、遮光性部材により構成される導電性電極層が望ましい。なお、本発明において「遮光性」とは、光を透過する性質を有しない、又は非常に小さいことを意味し、具体的には、発光領域の可視光域における透過率が１０％以下、好ましくは２％以下であればよい。 However, a translucent conductive layer generally has a higher electrical resistance than a metal layer, and heat generated by this resistance tends to cause problems such as a decrease in light emission efficiency, element degradation, and an increase in luminance distribution. is there. In addition, when a translucent conductive layer is used on the back side, light generated in the light emitting layer is emitted on both sides. For example, if only one side is illuminated, useless light is emitted on the opposite side. become. In addition, since light reflection does not occur like a metal film, the luminous efficiency tends to be extremely poor. As described above, in the present invention, the second conductive electrode layer is preferably a conductive electrode layer made of a light-shielding member such as a metal film that has low electrical resistance and good light reflection. In the present invention, the “light-shielding property” means that the light-transmitting property does not have or is very small, and specifically, the transmittance in the visible light region of the light-emitting region is preferably 10% or less, preferably May be 2% or less.
前記の遮光性部材により構成される第２の導電性電極層は、例えば、Ａｇ、Ａｌ、Ｃｒなどの金属単体層や、ＭｇＡｇなどの金属の合金層、あるいはこれらの複数層でも構わない。例えば、一部にアルカリ金属を含んでもよいし、金属酸化物を含んでもよい。また、本発明においては、これらの層を形成する方法は特に制限されず、例えば、低融点金属は抵抗加熱による蒸着法による形成でもよいし、高融点金属はＥＢ（電子ビーム）蒸着法でもよいし、スパッタ等による方法で形成することも可能である。 The second conductive electrode layer formed of the light shielding member may be, for example, a single metal layer such as Ag, Al, or Cr, an alloy layer of metal such as MgAg, or a plurality of these layers. For example, an alkali metal may be included in part, or a metal oxide may be included. In the present invention, the method for forming these layers is not particularly limited. For example, the low melting point metal may be formed by vapor deposition using resistance heating, and the high melting point metal may be formed by EB (electron beam) vapor deposition. However, it can also be formed by a method such as sputtering.
本発明の発光部材においては、前記第２の導電性電極層が、その総面積のうち２乃至４０％の範囲に可視光を５０％以上透過する領域（以下、透過領域ともいう）を含むことを特徴とする。ここで第２の導電性電極層の「総面積」とは、遮光性の第２の導電性電極層の外周部に囲まれた範囲の面積を意味し、「その総面積のうち２乃至４０％の範囲に可視光を５０％以上透過する領域を含む」とは、上記総面積を１００％とした場合に対する、可視光を５０％以上透過する領域の面積の比率、いわゆる開口率が２乃至４０％の範囲であることを意味する。 In the light emitting member of the present invention, the second conductive electrode layer includes a region (hereinafter also referred to as a transmission region) that transmits 50% or more of visible light in a range of 2 to 40% of the total area. It is characterized by. Here, the “total area” of the second conductive electrode layer means an area in a range surrounded by the outer periphery of the light-shielding second conductive electrode layer, and “2 to 40 out of the total area”. % Includes a region that transmits 50% or more of visible light ”is a ratio of the area of a region that transmits 50% or more of visible light to the case where the total area is 100%, that is, an aperture ratio of 2 to 2 It means the range of 40%.
前記開口率が２％未満の場合には、シースルー有機ＥＬ装置として用いる場合の透光性が不十分であり、逆に開口率が４０％を超える場合には、有機ＥＬ照明装置として用いる場合の光量出力が不十分である。これに対し、遮光性の第２の導電性電極層が上記範囲の開口率を有する場合は、透過領域以外は、電力を与えられない状態では遮光領域として機能し、電力を与えられた状態では光を反射する発光領域として機能し、一方、透過領域は電力の付与にかかわらず透光領域として機能する、というシースルーの有機ＥＬ装置を実現できる。上記観点から、開口率の好ましい範囲は５乃至３０％の範囲である。開口率が５％以上であれば、例えば、本発明の発光部材を窓ガラスとして利用する場合に、晴天時に直射日光をカットしつつ屋内に十分な採光が可能であり、また、３０％以下であれば、十分に照明装置として光量を確保できる。 When the aperture ratio is less than 2%, the translucency when used as a see-through organic EL device is insufficient, and conversely when the aperture ratio exceeds 40%, it is used as an organic EL lighting device. The light output is insufficient. On the other hand, when the light-shielding second conductive electrode layer has an aperture ratio in the above range, except for the transmission region, it functions as a light-shielding region in a state where power is not applied, and in a state where power is applied. A see-through organic EL device that functions as a light-emitting region that reflects light, while the transmissive region functions as a light-transmitting region regardless of application of electric power can be realized. From the above viewpoint, the preferable range of the aperture ratio is 5 to 30%. If the aperture ratio is 5% or more, for example, when the light-emitting member of the present invention is used as a window glass, sufficient sunlight can be taken indoors while cutting direct sunlight in fine weather, and 30% or less. If so, the amount of light can be sufficiently secured as a lighting device.
本発明においては、前記可視光を５０％以上透過する領域の少なくとも一部が、直径１０μｍ以上１ｍｍ以下の複数の概略円で構成されることが好ましい。透過領域における概略円の直径は、先述の開口率とも関係するが、１０μｍ未満では、有機発光装置に実質的に透光性を付与できない傾向がある。また、逆に直径が１ｍｍを超える場合は、透光性は十分得られるが透過領域が目立ち過ぎることとなり、また発光面積が実質的に小さくなることから、照明装置としては光量不足となる傾向がある。前記透過領域における概略円の直径の好ましい範囲は１０μｍ乃至５００μｍの範囲であり、この範囲であれば、例えば窓ガラスとして本発明の発光部材を利用する場合に、晴天時に直射日光をカットしつつ屋内に十分な採光が可能である。 In the present invention, it is preferable that at least a part of the region that transmits 50% or more of the visible light is composed of a plurality of approximate circles having a diameter of 10 μm or more and 1 mm or less. The diameter of the approximate circle in the transmission region is related to the aperture ratio described above, but if it is less than 10 μm, there is a tendency that the organic light-emitting device cannot be substantially imparted with translucency. On the other hand, when the diameter exceeds 1 mm, sufficient translucency can be obtained, but the transmission region is too conspicuous, and the light emission area is substantially reduced, so that the light quantity tends to be insufficient as a lighting device. is there. A preferable range of the diameter of the approximate circle in the transmission region is in the range of 10 μm to 500 μm. In this range, for example, when the light-emitting member of the present invention is used as a window glass, indoors while cutting direct sunlight in clear weather Enough lighting.
本発明においては、前記可視光を５０％以上透過する領域の少なくとも一部が、平均幅１０μｍ以上１ｍｍ以下の溝で構成されることが好ましく、更には平均幅１０μｍ以上５００μｍ以下の範囲であることがより好ましい。上述の開口率および透過領域の直径とも関係するが、透光性を十分得るためには、透過領域を大きくする必要があるが、逆に大きくし過ぎると透過領域が目立ってしまう。これを防ぐために、目立たない程度の小さな透過領域を連続的に配置して、隣接する開口部同士の一部を重なり合わせて溝にし、実質的な透過領域の面積を大きくして、透光性を得ることで実現できる。ここで溝とは、図１における２のように透過領域が重なり合って連続的に配置されていればよく、必ずしも直線溝でなくてもよい。 In the present invention, it is preferable that at least a part of the region that transmits 50% or more of the visible light is composed of grooves having an average width of 10 μm or more and 1 mm or less, and further, an average width of 10 μm or more and 500 μm or less. Is more preferable. Although it is also related to the aperture ratio and the diameter of the transmissive region, it is necessary to enlarge the transmissive region in order to obtain sufficient translucency, but conversely, if it is too large, the transmissive region becomes conspicuous. In order to prevent this, a small transparent region that is inconspicuous is continuously arranged, a part of adjacent openings are overlapped to form a groove, and a substantial area of the transparent region is increased, thereby translucent. It can be realized by obtaining. Here, the groove is not limited to a linear groove as long as the transmission regions overlap and are continuously arranged as indicated by 2 in FIG.
前記の遮光性の第２の導電性電極層における透過領域は、第２の導電性電極層を積層する際に、その総面積のうち２乃至４０％の範囲に可視光を５０％以上透過する領域が含まれるように、第２の導電性電極層の一部の領域の膜形成を遮断する方法により製造することが好ましい。「第２の導電性電極層の一部の領域の膜形成を遮断する」方法の好適な例としては、マスクを用いて第２の導電性電極層を蒸着する方法があげられる。前記透過領域に必要な要件は、第２の遮光性の導電性電極層に可視光の５０％以上が透過する領域があり、また第１の透光性電極層に損傷はなく、第２の電極層と第１の電極層は電気的に絶縁されていることであり、これらに加えて、透過領域の大きさや前述の開口率があげられる。上記要件を踏まえた上で、加工精度や、生産性、コストを勘案して、「第２の導電性電極層の一部の領域の膜形成を遮断する」方法は適宜選択すればよい。 The transmissive region in the light-shielding second conductive electrode layer transmits 50% or more of visible light in a range of 2 to 40% of the total area when the second conductive electrode layer is laminated. It is preferable to manufacture by the method of interrupting | blocking film formation of the one part area | region of a 2nd electroconductive electrode layer so that an area | region may be included. A preferred example of the method of “blocking film formation in a partial region of the second conductive electrode layer” is a method of depositing the second conductive electrode layer using a mask. The requirement for the transmissive region is that the second light-shielding conductive electrode layer has a region through which 50% or more of visible light is transmitted, the first light-transmissive electrode layer is not damaged, The electrode layer and the first electrode layer are electrically insulated, and in addition to these, the size of the transmission region and the above-described aperture ratio can be raised. In consideration of the above requirements, a method of “blocking film formation in a part of the second conductive electrode layer” may be selected as appropriate in consideration of processing accuracy, productivity, and cost.
一方、前記透過領域の少なくとも一部が、前記第２の導電性電極層を積層した後に、その総面積のうち２乃至４０％の範囲に可視光を５０％以上透過する領域が含まれるように、前記第２の導電性電極層の一部を除去する方法により製造することが好ましい。上記の第２の導電性電極層を積層後に、この一部を除去して透過領域を作る方法として、例えば、フォトリソグラフィー、ＲＩＥ（リアクティブイオンエッチング）、ウォータージェット、レーザービーム照射などの方法、およびこれらの組み合わせがあげられる。透過領域に必要な要件は先述した通りであるが、これらの要件を踏まえた上で、加工精度や、生産性、コストを勘案して適宜選択すればよい。 On the other hand, at least a part of the transmissive region includes a region that transmits 50% or more of visible light in a range of 2 to 40% of the total area after the second conductive electrode layer is stacked. Preferably, the second conductive electrode layer is manufactured by a method of removing a part of the second conductive electrode layer. After laminating the second conductive electrode layer, as a method of removing a part of this and creating a transmission region, for example, a method such as photolithography, RIE (reactive ion etching), water jet, laser beam irradiation, And combinations thereof. The requirements necessary for the transmission region are as described above, and may be selected as appropriate in consideration of processing accuracy, productivity, and cost in consideration of these requirements.
中でも、前記の「第２の導電性電極層を積層後に、この一部を除去して透過領域を作る方法」として、透光性基板側からレーザービームを照射することによって前記積層体層と第２の導電性電極層の一部を適宜除去する手段がより好ましい。レーザービームを照射する方法では、レーザービームは、任意のレーザーパワー（結果的には主として焦点位置）で照射できるので、第１の透光性電極層に損傷を与えず、また第２の遮光性電極層と第１の透光性電極層の間に電気的短絡を起こさない条件を容易に見出すことができる。加えて、透過領域の大きさの調整も、レーザーパワーを調整することにより可能である。レーザーザービームは、任意の加工速度でレーザー光源と前記透光性基板の位置を相対的にずらしながら照射されるため、透過領域の間隔や開口率も加工速度を調整することで容易に設計可能である。 Among them, as the above-mentioned “method for removing a part of the second conductive electrode layer after laminating and forming a transmission region”, the laser beam is irradiated from the translucent substrate side to form the first layer layer and the second layer. A means for appropriately removing a part of the conductive electrode layer 2 is more preferable. In the method of irradiating the laser beam, the laser beam can be irradiated with an arbitrary laser power (as a result, mainly the focal position), so that the first light transmitting electrode layer is not damaged and the second light shielding property is obtained. Conditions that do not cause an electrical short circuit between the electrode layer and the first translucent electrode layer can be easily found. In addition, the size of the transmissive region can be adjusted by adjusting the laser power. The laser beam is irradiated at an arbitrary processing speed while relatively shifting the position of the laser light source and the translucent substrate, so the interval between the transmission areas and the aperture ratio can be easily designed by adjusting the processing speed. It is.
このレーザービームの照射は、透光性基板側から入射されることが好ましい。透過領域に求められる要件は、先述のように第２の遮光性の電極層に可視光を５０％以上透過する領域があり、第１の透光性電極層に損傷はなく、第２の遮光性電極層と第１の透光性電極層は電気的に絶縁されていることであるが、有機発光層を含む複数の化合物層からなる積層体層には、損傷があっても、透過領域が生じても構わない。 The laser beam is preferably incident from the side of the translucent substrate. The requirement for the transmissive region is that the second light-shielding electrode layer has a region that transmits 50% or more of visible light as described above, the first light-transmissive electrode layer is not damaged, and the second light-shielding electrode layer is not damaged. The conductive electrode layer and the first translucent electrode layer are electrically insulated. However, even if the laminated body layer composed of a plurality of compound layers including the organic light emitting layer is damaged, the transmission region May occur.
第２の導電性電極層は、遮光性のある反射率の高い金属薄膜またはそれを含む多層膜が用いられるが、レーザービームを第２の電極層側から照射した場合、エネルギー密度が小さい場合は大部分のレーザービームは反射されてしまい電極層の加熱に有効に働かないため電極層を除去することができない。さらにビーム強度を高めていくと第２の電極層である金属層が溶解することによって反射率が小さくなり大きなエネルギーを急激に吸収することになる。この場合には、第２の電極層や透光性の第１の導電性電極層までがレーザービームのエネルギーによって損傷を受け、所望のパターニングができなくなり、また第２の電極層と第１の電極層の電気的絶縁を保てなくなる傾向がある。すなわち、入射するレーザービームのエネルギー密度を適切に制御することが難しく、事実上適切な加工条件が見出せなくなる場合が多い。 For the second conductive electrode layer, a light-shielding highly reflective metal thin film or a multilayer film including the same is used. When the laser beam is irradiated from the second electrode layer side, the energy density is low. Since most of the laser beam is reflected and does not work effectively for heating the electrode layer, the electrode layer cannot be removed. When the beam intensity is further increased, the metal layer as the second electrode layer is dissolved, so that the reflectance is reduced and a large amount of energy is absorbed rapidly. In this case, even the second electrode layer and the light-transmitting first conductive electrode layer are damaged by the energy of the laser beam, and the desired patterning cannot be performed. There is a tendency that the electrical insulation of the electrode layer cannot be maintained. That is, it is difficult to appropriately control the energy density of the incident laser beam, and it is often impossible to find an appropriate processing condition in practice.
これに対して、透光性基板側からレーザービームを照射した場合は、透光性基板や第１の透光性電極層での吸収がほとんどないため、エネルギー密度が低い場合でも積層体層でエネルギーが吸収される。先述のように、積層体層は損傷を受けてもよく、この吸収したエネルギーにより、ビーム照射周辺の温度を上昇させ、積層体層はガス化し、昇華成分によって第２の導電性電極層まで剥離され、これにより第２の電極層を除去することができる。また、この積層体層のガス化は、低エネルギー密度でできるため、微細なパターニングが可能であり、また第２の電極層と第１の電極層の電気的短絡を抑えることができる。 On the other hand, when the laser beam is irradiated from the translucent substrate side, there is almost no absorption in the translucent substrate or the first translucent electrode layer. Energy is absorbed. As described above, the laminate layer may be damaged, and the absorbed energy increases the temperature around the beam irradiation, the laminate layer is gasified, and is peeled off to the second conductive electrode layer by the sublimation component. Thus, the second electrode layer can be removed. In addition, since gasification of the stacked body layer can be performed at a low energy density, fine patterning is possible, and electrical short-circuiting between the second electrode layer and the first electrode layer can be suppressed.
このレーザーレーザーの照射に用いられるレーザー光源は、ネオジウム添加のＹＡＧパルスレーザーの高調波であることが好ましい。本発明では、第２の導電性電極層に透過領域を設ける際には、なるべく第１の透光性導電層に損傷を与えないことが望ましい。このため、照射するレーザー光としては積層体層に大きな吸収をもち、第１の透光性導電層での吸収は小さいことが求められる。ネオジウム添加のＹＡＧパルスレーザーは、広く産業界に普及しており入手が容易であるばかりでなく、パルス状発振によって短時間ではあるが非常に大きなパワー密度を得ることができ、加工性の高いレーザーである。基本波の波長は１０６４ｎｍであり、その高調波（５３２ｎｍ、３５５ｎｍ）は、ＩＴＯ等の透光性導電材料にほとんど吸収がない。このため、第１の透光性導電層に損傷を与えることなく積層体層や第２の遮光性導電層電極層を除去することに適している。とくに第２高調波は、比較的レーザー光源として広く普及しており製造装置に用いることは好適といえる。 The laser light source used for the laser laser irradiation is preferably a harmonic of a neodymium-added YAG pulse laser. In the present invention, when providing the transmissive region in the second conductive electrode layer, it is desirable that the first light transmissive conductive layer is not damaged as much as possible. For this reason, it is required that the laser beam to be irradiated has a large absorption in the laminate layer and a small absorption in the first light-transmitting conductive layer. Neodymium-added YAG pulse lasers are not only widely available and easily available in the industry, but also can be obtained in a short time but with a very high power density by pulsed oscillation, and have high processability. It is. The wavelength of the fundamental wave is 1064 nm, and its harmonics (532 nm, 355 nm) are hardly absorbed by the light-transmitting conductive material such as ITO. For this reason, it is suitable for removing the laminated body layer and the second light-shielding conductive layer electrode layer without damaging the first light-transmitting conductive layer. In particular, the second harmonic is relatively widespread as a laser light source, and it can be said that it is preferable to use it in a manufacturing apparatus.
本発明においては、前記の方法により第２の導電性電極層を積層した後、透光性の樹脂と透光性の封止板を用いて、前記第１の導電性電極層、前記積層体層および前記第２の導電性電極層を封止することが好ましい。すなわち、この場合の発光部材は、透光性基板と透光性の封止板で、第１の導電性電極層、積層体層、および第２の導電性電極層が挟み込まれており、少なくとも前記第２の導電性電極層と透光性の封止板の間に、透光性の樹脂が充填されていることになる。 In the present invention, after laminating the second conductive electrode layer by the above method, the first conductive electrode layer and the laminate are formed using a translucent resin and a translucent sealing plate. It is preferable to seal the layer and the second conductive electrode layer. That is, the light-emitting member in this case includes the first conductive electrode layer, the laminate layer, and the second conductive electrode layer sandwiched between the light-transmitting substrate and the light-transmitting sealing plate, and at least A translucent resin is filled between the second conductive electrode layer and the translucent sealing plate.
有機ＥＬ装置の封止方法として、第１の導電性電極層、有機発光層を含む複数の化合物層からなる積層体層、および第２の導電性電極層に接触しないように、一部を凹型に成形したガラス板や金属板を、透光性基板に覆い被せることが一般的である。ところが、金属板を用いた場合は、有機ＥＬ装置全体の透光性はなくなってしまう。また、ガラス板を用いた場合は、その凹型の内部は空間である場合が一般的であり、有機ＥＬ装置自体の機械的強度に問題があり、例えば、窓ガラスに応用した場合、問題となってしまう。本発明のように、透光性の樹脂を用いて、透光性基板と透光性の封止板で、第１の導電性電極層、積層体層、および第２の導電性電極層を挟み込めば、有機ＥＬ装置全体の透光性は確保でき、また機械的強度も得ることができる。加えて、凹型の板で覆い被せた場合はその中が空間であるため熱の伝導が悪いのに対して、樹脂で挟み込んだ場合は固体であるため熱の伝導がよく、有機ＥＬ装置で一般に問題となる均熱性の問題も解決でき、引いては素子の劣化を抑えることが可能となる。 As a sealing method of the organic EL device, a part of the first conductive electrode layer, a laminate layer composed of a plurality of compound layers including an organic light emitting layer, and a part of the second conductive electrode layer are recessed. In general, a glass plate or a metal plate molded into a glass substrate is covered with a translucent substrate. However, when a metal plate is used, the translucency of the entire organic EL device is lost. In addition, when a glass plate is used, the inside of the concave mold is generally a space, and there is a problem with the mechanical strength of the organic EL device itself. For example, it becomes a problem when applied to a window glass. End up. As in the present invention, the first conductive electrode layer, the laminate body layer, and the second conductive electrode layer are formed using a light-transmitting resin and a light-transmitting substrate and a light-transmitting sealing plate. If sandwiched, the translucency of the whole organic EL device can be secured, and the mechanical strength can also be obtained. In addition, when it is covered with a concave plate, it is a space, so heat conduction is poor, whereas when it is sandwiched between resins, it is solid, so heat conduction is good. It is possible to solve the problem of thermal uniformity, which is a problem, and to suppress deterioration of the element.
ここで、前記の透光性の樹脂としては、例えば、ＵＶ硬化型や熱硬化型のエポキシ樹脂を用いることができる。また、透光性の封止板としては、前述の透光性基板と同様のものが使用可能であり、例えば、アルカリガラスなどガラス基板やアクリル樹脂などの高分子フィルム基板を用いることができる。 Here, as the translucent resin, for example, a UV curable or thermosetting epoxy resin can be used. Moreover, as a translucent sealing board, the thing similar to the above-mentioned translucent board | substrate can be used, For example, polymer film substrates, such as glass substrates, such as alkali glass, and an acrylic resin, can be used.
本発明の発光部材（有機ＥＬ装置）おいては、発光部分が複数に分割され、かつそれらが電気的に直列に接続されていることが好ましい。有機ＥＬ装置の面積を拡大すると透光性の第１の導電性電極層の電気抵抗が問題となって、発熱による発光効率低下や、素子劣化、輝度分布の拡大等の問題が顕在化する傾向がある。これを防ぐために、発光部分を複数に分割し、電気的に直列に接続して、透光性の第１の導電性電極層の実質的な電気抵抗を下げることが可能である。このような直列接続された有機ＥＬ装置においても本発明は適用でき、然るに大面積のシースルー有機ＥＬ装置（以下、大面積有機ＥＬ発光部材）が実現でき、窓や天窓にも応用ができることとなる。 In the light emitting member (organic EL device) of the present invention, it is preferable that the light emitting part is divided into a plurality of parts and they are electrically connected in series. When the area of the organic EL device is enlarged, the electric resistance of the first conductive electrode layer having a light-transmitting property becomes a problem, and problems such as a decrease in light emission efficiency due to heat generation, element deterioration, and an increase in luminance distribution tend to become apparent. There is. In order to prevent this, the light emitting portion can be divided into a plurality of parts and electrically connected in series to reduce the substantial electrical resistance of the light-transmitting first conductive electrode layer. The present invention can also be applied to such organic EL devices connected in series. However, a large-area see-through organic EL device (hereinafter referred to as a large-area organic EL light emitting member) can be realized, and can be applied to windows and skylights. .
（大面積化への対応）
しかしながら、このような大面積有機ＥＬ発光部材において、十分な透光性を得るためには、透過領域の発光面に対する面積比率を一定以上確保する必要があり、本発明の好ましい実施態様の如くレーザー光を照射しつつ走査することで、遮光性電極層等を除去する方法で透過領域、即ち、透光性開口を曲線、又は直線等の線に沿って形成する場合、レーザー光の照射及び走査を行ういわゆるレーザスクライブ工程の負荷つまり装置コストや加工時間が製造工程上過大となるという問題がある。
(Corresponding to large area)
However, in such a large area organic EL light emitting member, in order to obtain sufficient translucency, it is necessary to ensure a certain ratio of the area of the transmissive region to the light emitting surface, and the laser as in the preferred embodiment of the present invention. When a light-transmitting region, that is, a light-transmitting aperture is formed along a curve or a straight line by a method of removing a light-shielding electrode layer by scanning while irradiating light, laser light irradiation and scanning There is a problem that the load of the so-called laser scribing process, that is, the apparatus cost and processing time becomes excessive in the manufacturing process.
この問題を解決する方法としては、透過領域の形成を、同時に複数のレーザー光を基板上のそれぞれ異なる部分に照射する方法が効果的であり、レーザスクライブ工程の負荷を大幅に低下することができる。同時に複数のレーザー光を基板上のそれぞれ異なる部分に照射することにより、複数の透過領域が同時に形成され、透過領域の面積比率が大きい大面積有機ＥＬ発光部材を、低価格の装置で短時間に形成することができる。 As a method for solving this problem, a method of irradiating a plurality of laser beams to different portions on the substrate at the same time for the formation of the transmission region is effective, and the load of the laser scribing process can be greatly reduced. . By simultaneously irradiating different portions on the substrate with a plurality of laser beams at the same time, a plurality of transmission regions are formed at the same time, and a large area organic EL light emitting member having a large area ratio of the transmission regions can be obtained in a short time with a low-cost apparatus Can be formed.
ところで、各透過領域は、夫々を形成したレーザー光の状態を反映し、個々異なる形態を有する。そして、レーザー光の状態はレーザー光出射ヘッドが同じなら若干の時間変動を除き一定である。従って、上記のように同時に複数のレーザー光を照射し複数の透光性開口を線上に形成する場合には、同一のレーザー光出射ヘッドから出射されたレーザー光により形成された透過領域が隣接している面領域は、異なるレーザー出射ヘッドから出射されたレーザー光により形成された周囲の面領域とは異なった外観に見えるという問題がある。 By the way, each transmissive region reflects the state of the laser beam that formed each, and has a different form. The state of the laser light is constant except for some time fluctuation if the laser light emitting head is the same. Therefore, when a plurality of laser beams are simultaneously irradiated as described above to form a plurality of light-transmitting apertures on a line, transmission regions formed by laser beams emitted from the same laser beam emission head are adjacent to each other. There is a problem that the surface area that is present looks different from the surrounding surface area formed by the laser light emitted from the different laser emission heads.
この問題を解決する方法としては、隣り合う前記透過領域、即ち、線上の透光性開口が同一のレーザー光出射ヘッドからのレーザー光により形成された基板上の面領域の数を、前記複数のレーザー光の数よりも大きくすることが有効である。このようにすると、同一のレーザー光出射ヘッドから出射されたレーザー光により形成された線上の透光性開口が隣接している面領域の数を、一枚の基板内で少なくとも２面領域以上、間隔をもって、つまり別面領域を挟んで離れて存在させることができ、外観上平均化して一様に見える効果がある。ここで、別面領域とは、上記の同一のレーザー光出射ヘッドから出射されたレーザー光とは異なる、同一のレーザー光出射ヘッドから出射されたレーザー光により形成された線上の透光性開口が隣接している面領域のことである。 As a method for solving this problem, the number of the adjacent transmission regions, that is, the surface regions on the substrate formed by the laser light from the laser light emitting head having the same translucent opening on the line, is set to the plurality of the plurality of the transmission regions. It is effective to make it larger than the number of laser beams. In this case, the number of surface areas adjacent to the transparent aperture on the line formed by the laser light emitted from the same laser light emitting head is at least two surface areas in one substrate, They can be present with a space, that is, with a different surface area between them, and have the effect of appearing uniform in appearance. Here, the different surface area is different from the laser beam emitted from the same laser beam emitting head described above, and is a translucent aperture on a line formed by the laser beam emitted from the same laser beam emitting head. It is an adjacent surface area.
さらに、隣り合う前記線上の透光性開口が異なるレーザー光出射ヘッドからのレーザー光により形成されるようにすることが効果的である。このようにすると、同一のレーザー光出射ヘッドから出射されたレーザー光により形成された線上の透光性開口が隣接している領域自体が存在しないようにできるので、基板内で線上の透光性開口形成に伴う領域としての外観ムラを皆無にすることができる。 Furthermore, it is effective that the transparent apertures on the adjacent lines are formed by laser beams from different laser beam emitting heads. By doing so, it is possible to prevent the region itself adjacent to the transparent aperture on the line formed by the laser beam emitted from the same laser beam emitting head, so that the transparent property on the line in the substrate is present. It is possible to eliminate the appearance unevenness as a region associated with the opening formation.
また、前記透光性開口が直線上に形成されてなる大面積有機ＥＬ発光部材とすると、同時に複数のレーザー光を基板上のそれぞれ異なる部分に照射するレーザスクライブ工程により、高い生産性が得られ、また外観上も好ましいものとなる。 Further, when the light-transmitting opening is a large-area organic EL light-emitting member formed on a straight line, high productivity can be obtained by a laser scribing process in which a plurality of laser beams are simultaneously irradiated onto different portions on the substrate. Also, the appearance is preferable.
さらに、隣り合う前記線上の透光性開口間の間隔が実質的に等間隔である大面積有機ＥＬ発光部材とすると、外観に優れた大面積有機ＥＬ発光部材となり好ましい。 Further, a large-area organic EL light-emitting member having a substantially uniform interval between the translucent openings on the adjacent lines is preferable because it provides a large-area organic EL light-emitting member with excellent appearance.
特に、好ましい実施態様として集積化発光素子とした場合には、その直列接続の方向に平行に前記線上の透光性開口を形成することが、外観上また実生産上さらには施工上好ましい。 In particular, when an integrated light-emitting device is used as a preferred embodiment, it is preferable in terms of appearance, actual production, and construction to form a translucent opening on the line parallel to the direction of the series connection.
（着色層）
本発明の発光部材は、窓として用いた場合の室外側防眩性および室外側外観を向上させる観点から、好ましくは、遮光性電極層の積層体層の反対側の面、即ち、遮光性電極層の非発光側面に接して樹脂バインダーを含有する着色層が形成される。前記防眩とは、屋外に面する金属光沢面やガラス表面のような良く光を反射する面に、太陽光が直達した場合に周囲に眩さを感じさせないようにすることをいう。
(Colored layer)
The light-emitting member of the present invention is preferably a surface opposite to the laminate layer of the light-shielding electrode layer, that is, the light-shielding electrode, from the viewpoint of improving outdoor anti-glare property and outdoor appearance when used as a window. A colored layer containing a resin binder is formed in contact with the non-light emitting side surface of the layer. The term “antiglare” refers to preventing glare from being felt when sunlight reaches a surface that reflects light well, such as a metallic glossy surface facing the outdoors or a glass surface.
前記樹脂バインダーを含有する着色層の形成は、遮光性電極層成膜後で、透過領域形成前であれば、後述する遮光性電極層分離溝形成前後どちらでも良いが、後述する着色層形成液による有機化合物層への悪影響の発生を防止する観点から、遮光性電極層分離溝形成前の方が好ましい。遮光性電極層成膜前に着色層を形成した場合には発光せず、また、透過領域形成後に着色層を形成した場合には本発明に係る発光部材の透光性は得られない。 The colored layer containing the resin binder may be formed either after the formation of the light-shielding electrode layer or before the formation of the transmission region, either before or after the formation of the light-shielding electrode layer separation groove described later. From the viewpoint of preventing the occurrence of adverse effects on the organic compound layer due to the formation of the light-shielding electrode layer separation groove, it is preferable. When the colored layer is formed before the light-shielding electrode layer is formed, no light is emitted, and when the colored layer is formed after the transmissive region is formed, the light-transmitting property of the light-emitting member according to the present invention cannot be obtained.
前記樹脂バインダーを含有する着色層を形成する方法としては、塗装後には揮発する有機溶剤に、主成分として超微粒子が分散されてなり、バインダーとしてアクリル系樹脂やアクリルウレタン系樹脂が溶解されてなる着色層形成液をスプレー塗装する方法が好ましい。 As a method of forming a colored layer containing the resin binder, ultrafine particles are dispersed as a main component in an organic solvent that volatilizes after coating, and an acrylic resin or an acrylic urethane resin is dissolved as a binder. A method of spray coating the colored layer forming liquid is preferred.
前記着色層の厚みとしてはレーザー加工の安定性の観点から０．５μｍ〜５μｍが好ましく、より好ましくは０．５μｍ〜３μｍ、さらに好ましくは１μｍ〜２μｍである。 The thickness of the colored layer is preferably 0.5 μm to 5 μm, more preferably 0.5 μm to 3 μm, still more preferably 1 μm to 2 μm from the viewpoint of laser processing stability.
前記超微粒子としては、レーザー加工が可能な２μｍ程度の着色層の厚みで十分に着色された層を形成する観点、及び、スプレー塗装を可能とする観点から、個数平均粒径が１〜１００ｎｍの超微粒子が好ましく、その材料としてはグラファイト超微粒子が好ましく、黒色又は青色に着色することができる。 As the ultrafine particles, the number average particle diameter is 1 to 100 nm from the viewpoint of forming a sufficiently colored layer with a thickness of a colored layer of about 2 μm capable of laser processing and enabling spray coating. Ultrafine particles are preferred, and the material is preferably graphite ultrafine particles, which can be colored black or blue.
次に、本発明の具体的な実施例およびこれらの実施例に対する比較例の有機ＥＬ装置の詳細な製造方法と、これらの評価結果を説明する。 Next, specific examples of the present invention and a detailed manufacturing method of an organic EL device of a comparative example with respect to these examples and evaluation results thereof will be described.
（実施例１）
平均膜厚１５０ｎｍのＩＴＯ膜を片面全体にコーティングした厚さ０．７ｍｍの無アルカリガラスを基板として用いた。この基板（サイズ２００ｍｍ×２００ｍｍ）をＩＴＯ膜が上になるようにＸＹステージ上に設置し、ＹＡＧレーザーの基本波を用いて上面からレーザービームを照射することにより、極力ガラスに損傷がないようにしてＩＴＯ膜の一部を除去した。レーザーの発振周波数は１５ｋＨｚ、出力１４Ｗ、ビーム径は約２５μｍ、加工速度は５０ｍｍ／秒であった。
Example 1
A non-alkali glass having a thickness of 0.7 mm in which an entire surface of an ITO film having an average thickness of 150 nm was coated was used as a substrate. This substrate (size 200mm x 200mm) is placed on the XY stage with the ITO film on top, and the laser beam is irradiated from the top using the fundamental wave of the YAG laser so that the glass is not damaged as much as possible. Then, a part of the ITO film was removed. The laser oscillation frequency was 15 kHz, the output was 14 W, the beam diameter was about 25 μm, and the processing speed was 50 mm / second.
この基板を中性洗剤で洗浄し、１５０℃で２０分加熱乾燥させた後、短冊状の各ＩＴＯ部分間の抵抗値が概ね２０ＭΩ以上であることを確認した。その後、真空蒸着装置を用いてパターニングされた陽極電極上に低分子有機化合物を主成分とする積層体層を形成した。すなわち、ＩＴＯ上の一層目には発光ユニットを形成するホール注入層として、酸化モリブデンと下記一般式１の４，４’−ビス［Ｎ−（２−ナフチル）−Ｎ−フェニル−アミノ］ビフェニル（以下α−ＮＰＤと略す）を、各蒸着速度０．０１５ｎｍ／秒と０．１３５ｎｍ／秒で真空共蒸着法により、１０ｎｍの膜厚で形成した。 This substrate was washed with a neutral detergent, dried by heating at 150 ° C. for 20 minutes, and then it was confirmed that the resistance value between the strip-like ITO portions was approximately 20 MΩ or more. Then, the laminated body layer which has a low molecular organic compound as a main component was formed on the anode electrode patterned using the vacuum evaporation system. That is, as a hole injection layer forming a light emitting unit on the first layer on ITO, molybdenum oxide and 4,4′-bis [N- (2-naphthyl) -N-phenyl-amino] biphenyl of the following general formula 1 ( (Hereinafter abbreviated as α-NPD) was formed to a thickness of 10 nm by vacuum co-evaporation at a deposition rate of 0.015 nm / second and 0.135 nm / second.
次いでホール輸送層として、α−ＮＰＤを真空蒸着法により５０ｎｍ（蒸着速度０．０８ｎｍ〜０．１２ｎｍ／秒）の膜厚で形成した。 Next, α-NPD was formed as a hole transport layer with a film thickness of 50 nm (deposition rate: 0.08 nm to 0.12 nm / second) by a vacuum evaporation method.
次いで、発光層は電子輸送層を兼ねた下記一般式２の［トリス（８−ハイドロキシキノリナート）］アルミニウム(ＩＩＩ)（以下Ａｌｑ３と略す）を真空蒸着法により７０ｎｍ（蒸着速度０．２５ｎｍ〜０．３０ｎｍ／秒）の膜厚で形成した。 Next, the light-emitting layer was prepared by vacuum evaporation of [tris (8-hydroxyquinolinato)] aluminum (III) (hereinafter abbreviated as Alq 3 ) of the following general formula 2 which also served as an electron transport layer (deposition rate: 0.25 nm). (-0.30 nm / sec).
次に、陰極にＬｉＦを真空蒸着法により１ｎｍ（蒸着速度０．０１ｎｍ〜０．０５ｎｍ／秒）の膜厚で積層し、その上に陰極電極Ａｌを真空蒸着法により１５０ｎｍ（蒸着速度０．３０ｎｍ〜０．３５ｎｍ／秒）の膜厚で製膜した。 Next, LiF was deposited on the cathode at a film thickness of 1 nm (deposition rate 0.01 nm to 0.05 nm / second) by vacuum deposition, and a cathode electrode Al was deposited thereon by 150 nm (deposition rate 0.30 nm). The film was formed at a film thickness of ˜0.35 nm / sec.
その後、この複数の有機化合物層が積層されたガラス基板を、有機化合物層が下面になるようにＸＹステージに設置した。その際、端部４個所でガラス基板を固定し、ガラス基板がＸＹステージから平行に７ｍｍ隔離され、有機化合物層が直接ＸＹステージに接触することのないように配置した。この状態で、ＹＡＧレーザーの第２高調波を用いて上面からレーザービームを照射することにより、極力ガラス基板およびＩＴＯ層に損傷がないようにして有機化合物層の一部を、ＩＴＯ層を除去した溝に平行に連続して除去した。レーザーの発振周波数は５kＨｚ、出力０．４Ｗ、ビーム径は約２５μｍ、加工速度は５０ｍｍ／秒であり、ＩＴＯを除去した溝との距離は１００μｍであった。 Thereafter, the glass substrate on which the plurality of organic compound layers were laminated was placed on an XY stage so that the organic compound layer was on the lower surface. At that time, the glass substrate was fixed at four end portions, and the glass substrate was arranged 7 mm in parallel with the XY stage so that the organic compound layer did not directly contact the XY stage. In this state, the ITO layer was removed from the organic compound layer by irradiating the laser beam from the upper surface using the second harmonic of the YAG laser so that the glass substrate and the ITO layer were not damaged as much as possible. It was continuously removed parallel to the grooves. The oscillation frequency of the laser was 5 kHz, the output was 0.4 W, the beam diameter was about 25 μm, the processing speed was 50 mm / second, and the distance from the groove from which ITO was removed was 100 μm.
有機化合物層の一部除去後に、再度ガラス基板を真空蒸着機に設置して、最表面のＡｌ層上に第２の電極層としてＡｌを真空蒸着法によりさらに１５０ｎｍ（蒸着速度０．３０ｎｍ〜０．３５ｎｍ／秒）の膜厚で製膜した。 After partial removal of the organic compound layer, the glass substrate is placed again in a vacuum deposition machine, and Al is further deposited on the outermost Al layer as a second electrode layer by 150 nm (deposition rate: 0.30 nm to 0 nm) by a vacuum deposition method. .35 nm / sec).
この有機化合物層が積層されたガラス基板を、Ａｌ層が下面になるようにＸＹステージに設置した。有機化合物層の除去の場合と同様に、端部４個所でガラス基板を固定し、ガラス基板がＸＹステージから平行に７ｍｍ隔離され、有機化合物層が直接ＸＹステージに接触することのないように配置した。ＹＡＧレーザーの第２高調波を用いて上面からレーザービームを照射することにより、極力ガラス基板およびＩＴＯ層に損傷がないようにしてＡｌ層の一部を、有機化合物層を除去した溝に平行に連続して除去した。レーザーの発振周波数は５kＨｚ、出力０．４Ｗ、ビーム径は約２５μｍ、加工速度は２００ｍｍ／秒であり、有機化合物層を除去した溝との距離は１００μｍであった。 The glass substrate on which the organic compound layer was laminated was placed on an XY stage so that the Al layer was on the lower surface. As in the case of the removal of the organic compound layer, the glass substrate is fixed at the four end portions, and the glass substrate is separated from the XY stage by 7 mm in parallel, so that the organic compound layer is not in direct contact with the XY stage. did. By irradiating a laser beam from the upper surface using the second harmonic of the YAG laser, a part of the Al layer is made parallel to the groove from which the organic compound layer has been removed so that the glass substrate and the ITO layer are not damaged as much as possible. Removed continuously. The oscillation frequency of the laser was 5 kHz, the output was 0.4 W, the beam diameter was about 25 μm, the processing speed was 200 mm / second, and the distance from the groove from which the organic compound layer was removed was 100 μm.
次に、外周部との絶縁のために、ＩＴＯの除去線等と垂直方向にＹＡＧレーザーの第２高調波を照射することにより、ＩＴＯと有機化合物層、第２の電極層を除去した。レーザーの発振周波数は５kＨｚ、出力０．４Ｗ、ビーム径は約２５μｍ、加工速度は５０ｍｍ／秒であった。 Next, in order to insulate from the outer peripheral portion, the second harmonic of the YAG laser was irradiated in a direction perpendicular to the ITO removal line or the like, thereby removing the ITO, the organic compound layer, and the second electrode layer. The oscillation frequency of the laser was 5 kHz, the output was 0.4 W, the beam diameter was about 25 μm, and the processing speed was 50 mm / second.
次に、第２の導電性電極層に可視光を５０％以上透過する領域を形成するために、この第２の電極層が積層されたガラス基板を、Ａｌ層が下面になるようにＸＹステージに設置した。端部４個所でガラス基板を固定し、ガラス基板がＸＹステージから平行に７ｍｍ隔離され、第２の電極層が直接ＸＹステージに接触することのないように配置した。ＹＡＧレーザーの第２高調波を用いて上面からレーザービームを照射することにより、極力ガラス基板およびＩＴＯ層に損傷がないようにして第２の電極層を、有機化合物層を除去した溝に垂直に繰り返し除去し、シースルー有機ＥＬ装置を完成した。レーザーの発振周波数は５kＨｚ、出力０．４Ｗ、ビーム径は約１００μｍ、加工速度は２００ｍｍ／秒であり、透過領域は約１００μｍ幅の溝とした。また、その溝の間隔は０．５ｍｍであり、開口率は２０％であった。 Next, in order to form a region that transmits 50% or more of visible light in the second conductive electrode layer, the glass substrate on which the second electrode layer is laminated is placed on an XY stage with the Al layer on the bottom surface. Installed. The glass substrate was fixed at four end portions, and the glass substrate was disposed 7 mm in parallel with the XY stage so that the second electrode layer did not directly contact the XY stage. By irradiating a laser beam from the upper surface using the second harmonic of the YAG laser, the second electrode layer is perpendicular to the groove from which the organic compound layer has been removed so that the glass substrate and the ITO layer are not damaged as much as possible. It was removed repeatedly to complete a see-through organic EL device. The oscillation frequency of the laser was 5 kHz, the output was 0.4 W, the beam diameter was about 100 μm, the processing speed was 200 mm / second, and the transmission region was a groove having a width of about 100 μm. The interval between the grooves was 0.5 mm, and the aperture ratio was 20%.
このようにして作製したシースルー有機ＥＬ装置、即ち、本発明の発光部材を昼間に室内窓際に置いたところ、窓に取り付けた通常のブラインドと同じ効果があり、外光を室内に取り込むことが出来た。また、夜間電力を与えると、室内を照らすことができ、照明として利用できた。 The see-through organic EL device thus produced, that is, when the light emitting member of the present invention is placed near the indoor window in the daytime, has the same effect as a normal blind attached to the window, and can take outside light into the room. It was. In addition, when night electricity was applied, the room could be illuminated and used as lighting.
（比較例）
実施例１と同様に、第２の電極層まで有機ＥＬ装置を作製したが、透過領域は形成しなかった。昼間、当該装置を室内窓際に置いたところ、壁と同じで、外光を室内に取り込むことは出来なかった。また、昼間に室外側からこの有機ＥＬ装置を観察したところ、金属光沢表面となっており眩く感じる場合があった。
(Comparative example)
Similar to Example 1, an organic EL device was manufactured up to the second electrode layer, but no transmissive region was formed. When the device was placed near the indoor window in the daytime, it was the same as the wall and outside light could not be taken into the room. In addition, when this organic EL device was observed from the outdoor side in the daytime, it sometimes became dazzling due to the metallic luster surface.
（実施例２）
実施例１において、第２の電極層の成膜後、即ち、遮光性電極層の成膜後であってレーザーにより遮光性電極層を除去する前、即ち、遮光性電極層分離溝形成前に、遮光性電極層の全面に着色層を形成したこと以外は、実施例１と同様にして、外周部との絶縁のための第２の電極層を除去までを実施して集積化発光素子を作製した。
(Example 2)
In Example 1, after the second electrode layer is formed, that is, after the light shielding electrode layer is formed, before the light shielding electrode layer is removed by the laser, that is, before the light shielding electrode layer separation groove is formed. The integrated light-emitting element is obtained by carrying out the steps up to the removal of the second electrode layer for insulation from the outer peripheral portion in the same manner as in Example 1 except that the colored layer is formed on the entire surface of the light-shielding electrode layer. Produced.
即ち、遮光性電極層分離溝形成後に、外周部との絶縁のために、ＩＴＯの除去線等と垂直方向に、その方向に平行な基板の辺の縁から１０ｍｍの位置に、その方向に垂直な基板の辺の一方の縁から他方の縁に連続して、ＹＡＧレーザーの第２高調波を照射することにより、ＩＴＯと有機化合物層、第２の電極層、及び着色層を連続する溝形状に除去することで集積化発光素子を作製した。レーザーの発振周波数は５kＨｚ、出力０．４Ｗ、ビーム径は約２５μｍ、加工速度は５０ｍｍ／秒であった。 That is, after the formation of the light-shielding electrode layer separation groove, in order to insulate from the outer periphery, in the direction perpendicular to the ITO removal line and the like, perpendicular to the direction at a position 10 mm from the edge of the side of the substrate parallel to that direction A groove shape in which ITO and the organic compound layer, the second electrode layer, and the colored layer are continuously formed by irradiating the second harmonic of the YAG laser continuously from one edge of the side of the substrate to the other edge. Then, an integrated light emitting device was manufactured. The oscillation frequency of the laser was 5 kHz, the output was 0.4 W, the beam diameter was about 25 μm, and the processing speed was 50 mm / second.
前記着色層の形成は、着色層形成液として黒染めスプレー（有）トビカのトップガードを用いてスプレー塗装により、その厚みが１．５μｍとなるように形成した。 The colored layer was formed to a thickness of 1.5 μm by spray coating using a black guard sprayed tobica top guard as a colored layer forming liquid.
この集積化発光素子は、以下の記載する順に積層されてなり、かつ、複数の単位発光素子が直列接続されてなる。また、この単位発光素子は、透光性電極層／積層体層／遮光性電極層から構成されてなり、隣り合う一方の発光素子の遮光性電極層が他方の発光素子の透光性電極層に接続されることで、電気的に直列接続されている。本明細書において積層体層のことを、この層で主に機能する材料が有機化合物であることから、有機化合物層と記載することがある。上述の実施例１と同様に実施例２において、積層体層は、厚さ１５０ｎｍのＡｌ層を陰極電極層として含む。 The integrated light emitting elements are stacked in the order described below, and a plurality of unit light emitting elements are connected in series. The unit light-emitting element is composed of a light-transmitting electrode layer / laminate layer / light-shielding electrode layer, and the light-shielding electrode layer of one adjacent light-emitting element is the light-transmitting electrode layer of the other light-emitting element. Are connected in series. In this specification, a layered body layer is sometimes referred to as an organic compound layer because a material mainly functioning in this layer is an organic compound. Similar to Example 1 described above, in Example 2, the stacked body layer includes an Al layer having a thickness of 150 nm as the cathode electrode layer.
基板：無アルカリガラス、厚さ０．７ｍｍ
透光性電極層：ＩＴＯ、厚さ１５０ｎｍ
積層体層、厚さ合計２８１ｎｍ
ホール注入層：ＭｏＯ３、α−ＮＰＤ共蒸着膜、厚さ１０ｎｍ
ホール輸送層：α−ＮＰＤ、厚さ５０ｎｍ
発光・電子輸送層：Ａｌｑ３、厚さ７０ｎｍ
電子注入層：ＬｉＦ、厚さ１ｎｍ
陰極電極層：Ａｌ、厚さ１５０ｎｍ
遮光性電極層：Ａｌ、厚さ１５０ｎｍ
着色層：グラファイト超微粒子分散バインダー樹脂、厚さ１．５μｍ
この集積化発光素子に、実施例１と同様にして、第２の導電性電極層、即ち、遮光性電極層に可視光を５０％以上透過する領域（透過領域）を形成することで本発明の発光部材を作製した。
Substrate: alkali-free glass, thickness 0.7mm
Translucent electrode layer: ITO, thickness 150 nm
Laminate layer, total thickness 281 nm
Hole injection layer: MoO 3 , α-NPD co-deposited film, thickness 10 nm
Hole transport layer: α-NPD, thickness 50 nm
Light emitting / electron transport layer: Alq 3 , thickness 70 nm
Electron injection layer: LiF, thickness 1 nm
Cathode electrode layer: Al, thickness 150 nm
Light-shielding electrode layer: Al, thickness 150 nm
Colored layer: Graphite ultrafine particle dispersed binder resin, thickness 1.5 μm
In the integrated light-emitting device, in the same manner as in Example 1, the second conductive electrode layer, that is, the light-shielding electrode layer is formed with a region (transmissive region) that transmits 50% or more of visible light. A light emitting member was prepared.
実施例２においては、発光素子への水分の侵入による悪影響を防止するため、特に、透過領域を形成したことによる信頼性の低下を防止するために、この発光部材の素子面にさらにプラズマＣＶＤで膜厚０．５μｍの窒化珪素膜を第一保護膜として形成し、さらに、その窒化珪素膜の上にポリシラザン液を塗布した後乾燥させることで厚さ０．５μｍの第二保護膜を形成した。このようにして実施例２の本発明の発光部材を作製した。 In Example 2, in order to prevent an adverse effect due to the intrusion of moisture into the light emitting element, in particular, in order to prevent a decrease in reliability due to the formation of the transmission region, the element surface of the light emitting member is further subjected to plasma CVD. A silicon nitride film having a thickness of 0.5 μm was formed as a first protective film, and a polysilazane liquid was applied on the silicon nitride film and then dried to form a second protective film having a thickness of 0.5 μm. . Thus, the light emitting member of the present invention of Example 2 was produced.
このようにして作製した実施例２の本発明の発光部材を昼間に室内窓際に置いたところ、窓に取り付けた通常のブラインドと同じ効果があり、外光を室内に取り込むことが出来た。また、窓の外から観察したところ、黒色であり室内は観察されず、防眩性および外観に優れていた。さらに、夜間電力を与えると、室内を照らすことができ、照明として利用できた。 When the light emitting member of the present invention of Example 2 produced in this way was placed near the indoor window in the daytime, it had the same effect as a normal blind attached to the window, and external light could be taken into the room. Moreover, when observed from the outside of the window, it was black and the room was not observed, and the antiglare property and the appearance were excellent. Furthermore, when night power was applied, the room could be illuminated and used as lighting.
１ シースルー有機発光装置
２ 可視光の５０％以上が透過する領域
３ 接続領域
１１ 透光性基板
１２ 第１の透光性電極層
１３ 発光層を含む積層体層
１４ 第２の遮光性電極層
２１ 透光性の封止板
２２ 透光性の樹脂
DESCRIPTION OF SYMBOLS 1 See-through organic light-emitting device 2 Area | region which 50% or more of visible light permeate | transmits 3 Connection area | region 11 Translucent board | substrate 12 1st translucent electrode layer 13 Laminated body layer 14 containing a light emitting layer 2nd light-shielding electrode layer 21 Translucent sealing plate 22 Translucent resin
Claims (10)
発光部分が複数の単位発光素子に分割され、かつ、複数の該単位発光素子が電気的に直列に接続されており、
前記第２の導電性電極層の総面積のうち２乃至４０％の範囲に設けられた可視光を５０％以上透過する領域が該透過領域に相当し、かつ、前記第１の導電性電極層が連続して存在する領域が該透過領域に相当し、さらに、
該単位発光素子の各領域内において、複数箇所に該第２の導電性電極の部分的不在による透過領域が形成されていることを特徴とするシースルー有機ＥＬ装置。 A first conductive electrode layer composed of at least a translucent member on a translucent substrate, a laminate layer composed of a plurality of compound layers including an organic light emitting layer, and a second electroconductivity composed of a light shielding member The electrode layers are sequentially stacked, and are uniformly arranged so that the appearance is averaged and seen uniformly. The transmission region is configured by the partial absence of the second conductive electrode layer. A see-through organic EL device including a region ,
The light emitting portion is divided into a plurality of unit light emitting elements, and the plurality of unit light emitting elements are electrically connected in series,
A region that transmits 50% or more of visible light provided in a range of 2 to 40% of the total area of the second conductive electrode layer corresponds to the transmissive region, and the first conductive electrode layer Corresponds to the transmission region, and further,
A see-through organic EL device , wherein a transmission region due to partial absence of the second conductive electrode is formed at a plurality of locations in each region of the unit light emitting element .
前記透過領域において、該着色層も不在とされていることを特徴とする請求項１又は２に記載のシースルー有機ＥＬ装置。 Furthermore, a colored layer containing a resin binder is formed on the surface of the second conductive electrode layer opposite to the laminate layer,
The see-through organic EL device according to claim 1, wherein the colored layer is also absent in the transmission region.
発光部分が複数の単位発光素子に分割され、かつ、複数の該単位発光素子が電気的に直列に接続されており、
前記第２の導電性電極層を積層する際に、その総面積のうち２乃至４０％の範囲に設けられた可視光を５０％以上透過する領域が該透過領域に相当し、かつ、前記第１の導電性電極層が連続して存在する領域が該透過領域に相当し、さらに、該単位発光素子の各領域内において、複数箇所に該第２の導電性電極の部分的不在による透過領域が形成されるように、第２の導電性電極層の一部の領域の膜形成を遮断することを特徴とするシースルー有機ＥＬ装置の製造方法。 A first conductive electrode layer composed of at least a translucent member on a translucent substrate, a laminate layer composed of a plurality of compound layers including an organic light emitting layer, and a second electroconductivity composed of a light shielding member The electrode layers are sequentially laminated, and are uniformly arranged so as to appear to be uniformly transmitted through the appearance, and the transmission region is constituted by the partial absence of the second conductive electrode layer. A method of manufacturing a see-through organic EL device including a region ,
The light emitting portion is divided into a plurality of unit light emitting elements, and the plurality of unit light emitting elements are electrically connected in series,
When laminating the second conductive electrode layer, a region transmitting 50% or more of visible light provided in a range of 2 to 40% of the total area corresponds to the transmission region, and A region where one conductive electrode layer continuously exists corresponds to the transmission region, and further, a transmission region due to partial absence of the second conductive electrode in a plurality of locations in each region of the unit light emitting element. in so that but is formed, the manufacturing method of the see-through organic EL device, characterized in that to block the film formation of a partial region of the second conductive electrode layer.
発光部分が複数の単位発光素子に分割され、かつ、複数の該単位発光素子が電気的に直列に接続されており、
前記第２の導電性電極層を積層した後に、その総面積のうち２乃至４０％の範囲に設けられた可視光を５０％以上透過する領域が該透過領域に相当し、かつ、前記第１の導電性電極層が連続して存在する領域が該透過領域に相当し、さらに、該単位発光素子の各領域内において、複数箇所に該第２の導電性電極の部分的不在による透過領域が形成されるように、前記第２の導電性電極層の一部を除去することを特徴とするシースルー有機ＥＬ装置の製造方法。 A first conductive electrode layer composed of at least a translucent member on a translucent substrate, a laminate layer composed of a plurality of compound layers including an organic light emitting layer, and a second electroconductivity composed of a light shielding member The electrode layers are sequentially laminated, and are uniformly arranged so as to appear to be uniformly transmitted through the appearance, and the transmission region is constituted by the partial absence of the second conductive electrode layer. A method of manufacturing a see-through organic EL device including a region ,
The light emitting portion is divided into a plurality of unit light emitting elements, and the plurality of unit light emitting elements are electrically connected in series,
After laminating the second conductive electrode layer, a region that transmits 50% or more of visible light in a range of 2 to 40% of the total area corresponds to the transmissive region, and the first A region where the conductive electrode layer continuously exists corresponds to the transmissive region, and further, in each region of the unit light emitting element, a transmissive region due to partial absence of the second conductive electrode is present at a plurality of locations. to so that is formed, the manufacturing method of the see-through organic EL device, which comprises removing a portion of the second conductive electrode layer.
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| KR100600883B1 (en) * | 2004-11-11 | 2006-07-18 | 삼성에스디아이 주식회사 | Organic electroluminescence device and method for fabricating thereof |
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