JP2007335105A - Light-emitting element, and its manufacturing method - Google Patents

Light-emitting element, and its manufacturing method Download PDF

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JP2007335105A
JP2007335105A JP2006162251A JP2006162251A JP2007335105A JP 2007335105 A JP2007335105 A JP 2007335105A JP 2006162251 A JP2006162251 A JP 2006162251A JP 2006162251 A JP2006162251 A JP 2006162251A JP 2007335105 A JP2007335105 A JP 2007335105A
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organic material
material layer
conductive
recess
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Takeshi Fukuda
武司 福田
Kentaro Ichii
健太郎 市井
Yoshihiro Terada
佳弘 寺田
Munehisa Fujimaki
宗久 藤巻
Morio Taniguchi
彬雄 谷口
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Fujikura Ltd
Shinshu University NUC
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Shinshu University NUC
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Abstract

<P>PROBLEM TO BE SOLVED: To provide a light-emitting element with small distortion occurring at the interface with an organic material layer and a second conductive layer arranged on it, in which thickness of the light-emitting layer is maintained uniformly and loss of conductivity of the second conductive layer can be suppressed. <P>SOLUTION: The manufacturing method of a light-emitting element comprises a process in which a first jointing material is fabricated by forming a first conductive layer and an organic material layer in the order on a transparent first base material of flat-plate shape, a process in which a second jointing member is fabricated by coating a conductive paste so as to cover the inner face of a recessed part and a part of the peripheral part of the recessed part aperture on a second base material of a cap-shape which has the recessed part and in which at least the inner face has insulation property, a process in which the first jointing member and the second jointing member are superposed so that the recessed part may envelope the organic material layer, and a process in which heat treatment is applied on each jointing member superposed to cure the conductive paste, and by electrically connecting to the organic material layer, a light-emitting element is obtained. <P>COPYRIGHT: (C)2008,JPO&INPIT

Description

本発明は、有機エレクトロルミネッセンスを用いた発光素子に係り、詳しくは発光特性の優れた安定性を有する発光素子と、製造プロセスにおいて発光素子に及ぼす熱的あるいは機械的な影響を抑制できる製造方法に関する。   The present invention relates to a light emitting device using organic electroluminescence, and more particularly to a light emitting device having excellent stability of light emitting characteristics and a manufacturing method capable of suppressing thermal or mechanical influence on the light emitting device in the manufacturing process. .

有機エレクトロルミネッセンス素子(以下、有機EL素子と記す。)は、透明なガラスもしくは透明な基板の表面に、第一電極(陽極)、有機材料層、第二電極層(陰極)が、この順に積層された基本構成を有する。
通常、第一電極層としては、ITO(スズ添加インジウム)に代表される透明導電材料から構成される。有機材料層は、少なくとも有機材料の発光層から構成され、必要に応じて、第一導電層(陽極)と発光層の間には正孔(ホール)注入層や正孔(ホール)輸送層が、発光層と第二導電層(陰極)との間には電子輸送層と電子注入巣が、それぞれ設けられる。その際、第二導電層としては、マグネシウム(Mg)、銀(Ag)、アルミニウム(Al)等の金属材料またはこれら金属を主体とする合金材料が好適に用いられる。
An organic electroluminescence element (hereinafter referred to as an organic EL element) is formed by laminating a first electrode (anode), an organic material layer, and a second electrode layer (cathode) in this order on the surface of a transparent glass or transparent substrate. It has the basic composition made.
Usually, the first electrode layer is made of a transparent conductive material typified by ITO (tin-added indium). The organic material layer is composed of at least a light emitting layer of an organic material, and if necessary, a hole injection layer or a hole transport layer is provided between the first conductive layer (anode) and the light emitting layer. The electron transport layer and the electron injection hole are provided between the light emitting layer and the second conductive layer (cathode), respectively. At that time, as the second conductive layer, a metal material such as magnesium (Mg), silver (Ag), aluminum (Al) or an alloy material mainly composed of these metals is preferably used.

前述した構成とするためには、以下に説明する2通りの代表的な製法が知られている。
第一の製法は、第一導電層の上に有機材料層を形成した後、第二導電層を有機材料層の上に成膜する方法である。その際、第二導電層を構成する金属膜は、蒸着法やスパッタ法等の物理的成膜法により形成し、有機EL素子を製造する方法である(例えば、特許文献1参照。)。
In order to achieve the above-described configuration, two typical manufacturing methods described below are known.
The first manufacturing method is a method in which an organic material layer is formed on a first conductive layer, and then a second conductive layer is formed on the organic material layer. In that case, the metal film which comprises a 2nd conductive layer is the method of forming an organic EL element by forming by physical film-forming methods, such as a vapor deposition method and a sputtering method (for example, refer patent document 1).

第二の製法は、予め、第一基材上に第一電極層と正孔輸送層を順に積層してなる第一基板と、第二基材上に第二導電層と発光層を順に積層してなる第二基板とを用意し、発光層と正孔輸送層が接するように2つの基板を重ね、発光層もしくは正孔輸送層が軟化する温度下で圧着して両者を貼り合わせることにより、有機EL素子を製造する方法である(例えば、特許文献2参照。)。
特開2003−45674号公報 特許第2755216号公報
In the second manufacturing method, a first substrate in which a first electrode layer and a hole transport layer are sequentially laminated on a first substrate, and a second conductive layer and a light emitting layer are sequentially laminated on the second substrate. A second substrate is prepared, and the two substrates are stacked so that the light emitting layer and the hole transport layer are in contact with each other, and bonded together by pressure bonding at a temperature at which the light emitting layer or the hole transport layer is softened. This is a method for producing an organic EL element (for example, see Patent Document 2).
JP 2003-45674 A Japanese Patent No. 2755216

しかしながら、第1の製法においては、第二導電層の成膜に伴い、有機材料層上に粒子が高いエネルギーを持って衝突し堆積するプロセスを利用するため、発光層を含む有機材料層にダメージを与え、有機材料層を熱的にあるいは機械的に破壊し、ひいては有機EL素子の発光品質を著しく低下させる虞があった。
また、物理的成膜法により第二導電層を有機材料層上に形成すると、材料の性質が異なるゆえに、両者の界面には内部応力が残存しやすい。ゆえに、有機EL素子がその後に受ける熱履歴によっては、界面に起因した歪みが発生し、この歪みは有機EL素子の発光品質に悪い影響を及ぼしてしまう虞もあった。
However, the first manufacturing method uses a process in which particles collide and deposit on the organic material layer with high energy as the second conductive layer is formed, so that the organic material layer including the light emitting layer is damaged. And the organic material layer is thermally or mechanically destroyed, and as a result, the light emission quality of the organic EL element may be significantly reduced.
Further, when the second conductive layer is formed on the organic material layer by a physical film formation method, the internal stress tends to remain at the interface between the two because the properties of the materials are different. Therefore, depending on the thermal history that the organic EL element subsequently receives, distortion due to the interface occurs, and this distortion may adversely affect the light emission quality of the organic EL element.

また、第二の製法においては、第二導電層の形成において、有機材料層が軟化する温度まで加熱して圧着する必要があるため、有機材料層は熱的かつ機械的な影響を受け、その厚みに偏りが生じてしまう。ゆえに、有機EL素子において均一に優れた発光特性を著しく低下させてしまう虞があった。   Further, in the second production method, in the formation of the second conductive layer, it is necessary to heat and pressure-bond the organic material layer to a temperature at which the organic material layer is softened. The thickness will be biased. Therefore, there is a possibility that the light emission characteristics that are uniformly excellent in the organic EL element are remarkably deteriorated.

また、有機EL素子の陰極には、有機材料に対して効率よく電子を注入できる材料が望ましいため、前述したような、仕事関数が小さく、活性の高い金属を含む合金材料が好適に用いられる。しかしながら、これらの合金材料は、酸素に触れると酸化して導電性が損なわれ易いという性質をもっている。そのため、このような合金材料からなる陰極は、酸化の影響を受け、その導電性が損失し、発光素子の輝度が低下したり、あるいは陰極層と有機材料層との間が部分的に剥離して、発光素子に非発光部分が生じたりするといった虞があった。   In addition, since a material capable of efficiently injecting electrons into an organic material is desirable for the cathode of the organic EL element, an alloy material containing a metal having a low work function and high activity as described above is preferably used. However, these alloy materials have the property that when exposed to oxygen, they are oxidized and their conductivity is easily impaired. Therefore, a cathode made of such an alloy material is affected by oxidation, and its conductivity is lost, the luminance of the light emitting element is lowered, or the cathode layer and the organic material layer are partially separated. As a result, a non-light emitting portion may occur in the light emitting element.

本発明は、前記事情に鑑みてなされ、有機材料層とその上に配される第二導電層との界面に生じる歪みが小さく、発光層の厚みが均一に保持されるとともに、第二導電層が有する導電性の損失も抑制することが可能な発光素子の提供を目的とする。   The present invention has been made in view of the above circumstances, the strain generated at the interface between the organic material layer and the second conductive layer disposed thereon is small, the thickness of the light emitting layer is kept uniform, and the second conductive layer An object of the present invention is to provide a light-emitting element capable of suppressing the loss of conductivity of the.

前記目的を達成するため、本発明は、平板状の透明な第一基材、該第一基材上に設けられた第一導電層、及び該第一導電層上に設けられた有機材料層から構成される第一接合部材と、凹部を有し、少なくとも該凹部内面が絶縁性を有しているキャップ形状の第二基材及び該第二基材の凹部内面と凹部開口周縁部の一部を覆うように設けられた第二導電層から構成される第二接合部材とを備え、前記凹部が前記有機材料層を包み込むように前記第一接合部材と前記第二接合部材とを重ね合わせてなる発光素子であって、前記第二導電層が、導電性ペーストを硬化させた導電体からなることを特徴とする発光素子を提供する。   In order to achieve the above object, the present invention provides a flat transparent first base material, a first conductive layer provided on the first base material, and an organic material layer provided on the first conductive layer. A cap-shaped second base material having a concave portion, and at least the inner surface of the concave portion is insulative, and the inner surface of the concave portion and the peripheral edge of the concave portion of the second base material. And a second bonding member composed of a second conductive layer provided so as to cover the portion, and the first bonding member and the second bonding member are overlapped so that the concave portion wraps the organic material layer The light-emitting element is characterized in that the second conductive layer is made of a conductor obtained by curing a conductive paste.

また本発明は、平板状の透明な第一基材上に、第一導電層と有機材料層とを順に成膜して第一接合部材を作製する工程、凹部を有し、少なくとも該凹部内面が絶縁性を有しているキャップ形状の第二基材に、該凹部内面及び凹部開口周縁部の一部を覆うように導電性ペーストを塗布して第二接合部材を作製する工程、前記凹部が前記有機材料層を包み込むように前記第一接合部材と前記第二接合部材とを重ね合わせる工程、及び、重ね合わせた各接合部材に熱処理を施して前記導電性ペーストを硬化させて前記有機材料層と電気的に接続させ、発光素子を得る工程、を含むことを特徴とする発光素子の製造方法を提供する。   The present invention also includes a step of forming a first joining member by sequentially forming a first conductive layer and an organic material layer on a flat transparent first base material, having a recess, and at least the inner surface of the recess A step of applying a conductive paste to the cap-shaped second base material having an insulating property so as to cover a part of the inner surface of the concave portion and the peripheral edge of the concave portion, thereby producing a second bonding member, the concave portion Wrapping the first bonding member and the second bonding member so as to wrap the organic material layer, and applying heat treatment to the stacked bonding members to cure the conductive paste, thereby the organic material There is provided a method for manufacturing a light-emitting element, including a step of electrically connecting a layer to obtain a light-emitting element.

本発明の発光素子は、有機材料層を有する第一接合部材と、凹部内に第二電極層を有する第二接合部材とを、凹部が前記有機材料層を包み込むように前記第一接合部材と前記第二接合部材とを重ね合わせてなり、導電性ペーストを硬化させた導電体からなる第二導電層を有するものなので、導電性ペーストが未硬化の状態で第一接合部材と前記第二接合部材とを重ね合わせることによって、有機材料層の外面に導電性ペーストが十分に接着し、次に、この導電性ペーストを硬化させることによって、有機材料層にダメージを与えることなく有機材料層と第二電極層とを電気的に接続でき、有機材料層の膜厚が均一な発光素子を提供することができる。
また、有機材料層と第二電極層との界面の電気的、機械的接合特性が向上し、発光効率、寿命などの特性に優れた発光素子を提供することができる。
The light-emitting element of the present invention includes a first bonding member having an organic material layer, a second bonding member having a second electrode layer in the recess, and the first bonding member so that the recess wraps the organic material layer. The second bonding member is overlaid and has a second conductive layer made of a conductive material obtained by curing the conductive paste, so that the first bonding member and the second bonding are in an uncured state of the conductive paste. By superimposing the members, the conductive paste is sufficiently adhered to the outer surface of the organic material layer, and then the conductive paste is cured, so that the organic material layer and the first layer are not damaged without damaging the organic material layer. A light-emitting element in which the two electrode layers can be electrically connected and the organic material layer has a uniform thickness can be provided.
In addition, the electrical and mechanical bonding characteristics of the interface between the organic material layer and the second electrode layer are improved, and a light emitting element having excellent characteristics such as luminous efficiency and lifetime can be provided.

本発明の発光素子の製造方法は、有機材料層を有する第一接合部材と、凹部内に第二電極層となる導電性ペーストを塗布した第二接合部材とを、凹部が前記有機材料層を包み込むように前記第一接合部材と前記第二接合部材とを重ね合わせ、次いで導電性ペーストを硬化させて第二導電層を形成するものなので、導電性ペーストが未硬化の状態で第一接合部材と前記第二接合部材とを重ね合わせることによって、有機材料層の外面に導電性ペーストが十分に接着し、次に、この導電性ペーストを硬化させることによって、有機材料層にダメージを与えることなく有機材料層と第二電極層とを電気的に接続でき、有機材料層の膜厚が均一な発光素子を歩留まりよく製造することができる。
また、有機材料層と第二電極層との界面の電気的、機械的接合特性が向上し、発光効率、寿命などの特性に優れた発光素子を製造することができる。
The method for manufacturing a light-emitting element of the present invention includes a first bonding member having an organic material layer and a second bonding member in which a conductive paste serving as a second electrode layer is applied in the recess, and the recess has the organic material layer. Since the first bonding member and the second bonding member are overlapped so as to wrap, and then the conductive paste is cured to form the second conductive layer, the first bonding member is in an uncured state. And the second bonding member are superposed on each other so that the conductive paste is sufficiently adhered to the outer surface of the organic material layer, and then the conductive paste is cured without damaging the organic material layer. A light-emitting element in which the organic material layer and the second electrode layer can be electrically connected and the thickness of the organic material layer is uniform can be manufactured with high yield.
In addition, the electrical and mechanical joining characteristics of the interface between the organic material layer and the second electrode layer are improved, and a light emitting element having excellent characteristics such as luminous efficiency and lifetime can be manufactured.

以下、本発明の一実施形態として、発光素子を構成する有機材料層が有機EL素子として機能する場合について、図面を参照して説明する。
図1は、本発明の発光素子の製造方法における第一接合部材と前記第二接合部材とを重ね合わせる工程を示す模式的な断面図、図2は本発明の発光素子の一例を示す模式的な断面図である。これらの図中、符号1は有機材料層、2は第一基材、3は第一導電層、4は導電性ペースト、5は第二基材、6は第一接合部材、7は第二接合部材、8は絶縁層、9は第二導電層、10は発光素子である。
Hereinafter, as an embodiment of the present invention, a case where an organic material layer constituting a light emitting element functions as an organic EL element will be described with reference to the drawings.
FIG. 1 is a schematic cross-sectional view showing a process of superimposing the first joining member and the second joining member in the method for producing a light-emitting element of the present invention, and FIG. 2 is a schematic view showing an example of the light-emitting element of the present invention. FIG. In these drawings, reference numeral 1 is an organic material layer, 2 is a first substrate, 3 is a first conductive layer, 4 is a conductive paste, 5 is a second substrate, 6 is a first bonding member, and 7 is a second member. A joining member, 8 is an insulating layer, 9 is a second conductive layer, and 10 is a light emitting element.

図2に示した発光素子10(有機EL素子)は、平板状の透明な第一基材2、該第一基材2上に設けられた第一導電層3(陽極)、及び該第一導電層3上に設けられた有機材料層1から構成される第一接合部材6と、凹部を備えたキャップ形状の第二基材5、該第二基材5の凹部内の底面及び側面と凹部開口周縁部の一部を覆うように設けられた絶縁層8、及び該絶縁層8の一部を覆うように設けられた第二導電層9(陰極)から構成される第二接合部材7とを備え、凹部が有機材料層1を包み込むように第一接合部材6と第二接合部材7とを重ね合わせてなり、第二導電層9が、導電性ペースト4を硬化させた導電体からなることを特徴としている。   The light-emitting element 10 (organic EL element) shown in FIG. 2 includes a flat plate-like transparent first base material 2, a first conductive layer 3 (anode) provided on the first base material 2, and the first A first joining member 6 comprising an organic material layer 1 provided on the conductive layer 3; a cap-shaped second base material 5 having a recess; a bottom surface and side surfaces in the recess of the second base material 5; A second bonding member 7 comprising an insulating layer 8 provided so as to cover a part of the peripheral edge of the recess opening, and a second conductive layer 9 (cathode) provided so as to cover a part of the insulating layer 8. And the second conductive layer 9 is made of a conductor obtained by curing the conductive paste 4 so that the concave portion wraps the organic material layer 1. It is characterized by becoming.

第一基材2としては、平板状の透明な、ガラスもしくは樹脂からなる基板(以下、それぞれ「ガラス基板」、「樹脂基板」と記す。)を用いることができる。ガラス基板の例としては、石英ガラス、BK7,ソーダライムガラス等が挙げられる。また、樹脂基板の例としては、ポリカーボネート、ポリイミド、ポリエチレンテレフタレート等が挙げられる。前記第一接合部材6は、この第一基材2の上に、第一導電層3、有機材料層1を順に積層した構造となっている。   As the first base material 2, a plate-like transparent glass or resin substrate (hereinafter referred to as “glass substrate” or “resin substrate”, respectively) can be used. Examples of the glass substrate include quartz glass, BK7, and soda lime glass. Examples of the resin substrate include polycarbonate, polyimide, polyethylene terephthalate, and the like. The first joining member 6 has a structure in which a first conductive layer 3 and an organic material layer 1 are sequentially laminated on the first base material 2.

また、第一基材2として樹脂基板を用いた場合、樹脂基板は水分を透過してしまうため、第一基材2と第一導電層3との間に、該第一基材2の一面を全て覆うようにガスバリア層を設ける必要がある。このガスバリア層としては、例えば、Au,Ag,Cu,Al,Pt等の金属、またはこれらの合金の他に、SiO,Si等の酸化物や窒化物を用いることができる。また、ガスバリア層は、有機材料層24から外部へ出射される光(以下、「発光」とも呼ぶ。)の透過率が高いことが求められる。発光の透過率は85%以上であることが望ましい。 In addition, when a resin substrate is used as the first base material 2, since the resin substrate transmits moisture, one surface of the first base material 2 is interposed between the first base material 2 and the first conductive layer 3. It is necessary to provide a gas barrier layer so as to cover all of the above. As this gas barrier layer, for example, in addition to metals such as Au, Ag, Cu, Al, and Pt, or alloys thereof, oxides and nitrides such as SiO 2 and Si 3 N 4 can be used. Further, the gas barrier layer is required to have a high transmittance for light emitted from the organic material layer 24 to the outside (hereinafter also referred to as “light emission”). The light transmittance is desirably 85% or more.

このようなガスバリア層の形成方法としては特に限定されないが、例えば真空蒸着法、スパッタ法、スクリーン印刷法、スリットコーティング法等が挙げられる。ガスバリア層に金属等の導電性物質を用いた場合、ガスバリア層と第一導電層3の間に絶縁層を設ける必要があるので、SiO,Si等の絶縁材料を用いることが望ましい。 A method for forming such a gas barrier layer is not particularly limited, and examples thereof include a vacuum deposition method, a sputtering method, a screen printing method, and a slit coating method. When a conductive material such as a metal is used for the gas barrier layer, it is necessary to provide an insulating layer between the gas barrier layer and the first conductive layer 3, so it is desirable to use an insulating material such as SiO 2 or Si 3 N 4. .

第一導電層3は、高導電性と高透過性を有する材料からなり、一般に第一基材2上に互いに離間して複数設けられる。この第一導電層3としては、例えば、スズ添加酸化インジウム(ITO:Tin doped Indium Oxide)、亜鉛添加酸化インジウム(IZO:Indium Zinc Oxide)、アルミニウム添加酸化亜鉛(AZO:Al doped Zinc Oxide)等の材料を用いることができる。   The first conductive layer 3 is made of a material having high conductivity and high permeability, and generally, a plurality of first conductive layers 3 are provided on the first base material 2 so as to be separated from each other. Examples of the first conductive layer 3 include tin-doped indium oxide (ITO), zinc-doped indium oxide (IZO), and aluminum-doped zinc oxide (AZO). Materials can be used.

第一導電層3の形成方法としては特に制限されないが、例えばスパッタ法、インクジェット法、スピンコート法等を用いることができる。インクジェット法、スピンコート法では、第一導電材料の微粒子をバインダーに分散し、塗布後に加熱して脱脂することで透明な導電層(陽極)を形成することができる。また、例えばITO膜を形成する場合、塩化インジウムと塩化スズのエタノール溶液を塗布し、加熱する手法を用いてもよい。その際、第一導電層3の厚さは、50nm〜400nm程度が好ましい。   A method for forming the first conductive layer 3 is not particularly limited, and for example, a sputtering method, an inkjet method, a spin coating method, or the like can be used. In the ink jet method and the spin coating method, a transparent conductive layer (anode) can be formed by dispersing fine particles of the first conductive material in a binder and heating and degreasing after coating. For example, when forming an ITO film, an ethanol solution of indium chloride and tin chloride may be applied and heated. At that time, the thickness of the first conductive layer 3 is preferably about 50 nm to 400 nm.

有機材料層1は、複数配された前記第一導電層3の一つと部分的に重なるように配置されており、有機材料からなる発光層を少なくとも含んでいる。また、有機材料層1は、必要に応じて、発光層の上下に、電子注入層、電子輸送層、正孔(ホール)輸送層、正孔(ホール)注入層といった各機能層を備えて構成される。
したがって、有機材料層1は、第一導電層3に重ねて、正孔(ホール)輸送層、発光層、電子輸送層が順に配された構成としたり、第一導電層3に重ねて、正孔(ホール)注入層、正孔(ホール)輸送層、発光層が順に配された構成とすることができる。これにより、発光素子の発光効率を向上させたり、発光波長をコントロールする等、発光素子の諸特性を設計・制御することができる。
The organic material layer 1 is disposed so as to partially overlap with one of the plurality of first conductive layers 3 arranged, and includes at least a light emitting layer made of an organic material. Moreover, the organic material layer 1 includes a functional layer such as an electron injection layer, an electron transport layer, a hole transport layer, and a hole injection layer above and below the light emitting layer as necessary. Is done.
Therefore, the organic material layer 1 has a structure in which a hole transport layer, a light-emitting layer, and an electron transport layer are sequentially arranged on the first conductive layer 3, or on the first conductive layer 3. A hole injection layer, a hole transport layer, and a light emitting layer may be arranged in this order. This makes it possible to design and control various characteristics of the light emitting element, such as improving the light emission efficiency of the light emitting element and controlling the emission wavelength.

この有機材料層1の各層を形成する方法は特に限定されず、例えば真空蒸着法、スパッタ法、インクジェット法、グラビア印刷法、スリットコーティング法、転写法等が挙げられる。その際、インクジェット法を用いれば、材料の利用効率が高く、また、高価な真空プロセスが不必要になるため、工業的に有利である。   A method for forming each layer of the organic material layer 1 is not particularly limited, and examples thereof include a vacuum deposition method, a sputtering method, an ink jet method, a gravure printing method, a slit coating method, and a transfer method. In that case, if the inkjet method is used, the utilization efficiency of the material is high, and an expensive vacuum process is unnecessary, which is industrially advantageous.

本発明において、有機材料層1の表面には、未硬化の導電性ペースト4を接着させ、その後、導電性ペースト4を硬化させて第二導電層9を形成するので、この有機材料層1の表面は、平坦であっても、凹凸面であってもよい。このように本発明によれば、有機材料層1の表面粗さの影響を緩和することができ、有機材料層1−第二導電層9間の電気的接合不良に起因するダークスポットの発生を大幅に低下させることができる。   In the present invention, the uncured conductive paste 4 is adhered to the surface of the organic material layer 1 and then the conductive paste 4 is cured to form the second conductive layer 9. The surface may be flat or an uneven surface. As described above, according to the present invention, the influence of the surface roughness of the organic material layer 1 can be alleviated, and the generation of dark spots due to poor electrical connection between the organic material layer 1 and the second conductive layer 9 can be prevented. It can be greatly reduced.

一方、第二接合部材7の第二基材5としては、凹部を備えたキャップ形状をなしており、腐食に強く、ガスバリア性に優れる部材が好ましく、例えば、ステンレス鋼やガラスからなる缶体(封止缶)を用いることができる。ただし、第二基材5はこれに限定されるものではなく、例えば、柔軟性のあるシート体や薄体(膜も含む)を用いても構わない。   On the other hand, the second base member 5 of the second bonding member 7 is preferably a member having a cap shape with a recess, strong against corrosion, and excellent in gas barrier properties. For example, a can body made of stainless steel or glass ( Sealing cans) can be used. However, the 2nd base material 5 is not limited to this, For example, you may use a flexible sheet | seat body and a thin body (a film | membrane is also included).

第二基材5をステンレス鋼等の導電性を有する部材で構成した場合、第二基材5と第二導電層9との間は、電気的に絶縁されている形態が望ましい。その際、例えばAl,Si,Ti等の酸化物または窒化物を第二基材5の一面に絶縁層8として成膜することにより、電気的な絶縁を図る方法が好適である。   When the 2nd base material 5 is comprised with members which have electroconductivity, such as stainless steel, the form with which the 2nd base material 5 and the 2nd conductive layer 9 are electrically insulated is desirable. In that case, for example, a method of electrically insulating by forming an oxide or nitride such as Al, Si, Ti or the like as the insulating layer 8 on one surface of the second substrate 5 is suitable.

絶縁層8は、前述した第二基材5の凹部内の底面及び側面と凹部開口周縁部を全て覆うように配される。酸化物または窒化物よりなる絶縁層8を成膜する方法としては、例えばエアロゾルデポジション法、スパッタ法、CVD法等を挙げることができる。また、絶縁層8の厚さは、十分な絶縁が確保できる厚さならば制限されないが、素子全体の厚さを低減できるようにするため、10〜1000nmの範囲であることが望ましい。   The insulating layer 8 is disposed so as to cover all the bottom and side surfaces in the recess of the second base material 5 and the peripheral edge of the recess opening. Examples of the method for forming the insulating layer 8 made of oxide or nitride include an aerosol deposition method, a sputtering method, a CVD method, and the like. Further, the thickness of the insulating layer 8 is not limited as long as sufficient insulation can be ensured, but is desirably in the range of 10 to 1000 nm in order to reduce the thickness of the entire device.

また、絶縁層8を構成する部材として吸湿性の材料を用いることもできる。具体的な材料としては、例えばCa,Sr,Ba,Ra,Be,Mgといったアルカリ土類金属の酸化物や、アルミニウムオキサイドオクチレート等の有機金属化合物を用いることができる。このようなアルカリ土類金属の酸化物を成膜する方法としては、例えば、酸化物をターゲットとしたスパッタ法や電子ビーム蒸着法を用いることができる。また、アルミニウムオキサイドオクチレート等の有機金属化合物を成膜する方法としては、例えば、有機金属化合物をトルエンやキシレン等の有機溶媒に溶解した溶液を印刷する方法を用いることができる。前述した吸湿性を有する層は、絶縁層8と同一である形態の他に、別途、中間層として積層された形態としてもよい。
したがって、第二接合部材7は、第二基材5の一面に、絶縁層8、中間層(図示せず)、第二導電層9を順に積層した構造とすることもできる。
Further, a hygroscopic material can be used as a member constituting the insulating layer 8. As specific materials, for example, oxides of alkaline earth metals such as Ca, Sr, Ba, Ra, Be, and Mg, and organometallic compounds such as aluminum oxide octylate can be used. As a method for forming such an alkaline earth metal oxide film, for example, a sputtering method or an electron beam evaporation method using an oxide as a target can be used. In addition, as a method of forming an organic metal compound such as aluminum oxide octylate, for example, a method of printing a solution in which an organic metal compound is dissolved in an organic solvent such as toluene or xylene can be used. The hygroscopic layer described above may be separately laminated as an intermediate layer in addition to the same form as the insulating layer 8.
Therefore, the second bonding member 7 may have a structure in which the insulating layer 8, the intermediate layer (not shown), and the second conductive layer 9 are sequentially laminated on one surface of the second base material 5.

第二導電層9は、絶縁層8の一部を覆うように配される。ここで、一部とは、凹部の底面を被覆する絶縁層8の上面全域と、この上面から連続する、凹部の内側面と凹部開口周縁部とを被覆する絶縁層8の一部領域を意味する。   The second conductive layer 9 is disposed so as to cover a part of the insulating layer 8. Here, “part” means a partial region of the insulating layer 8 covering the entire upper surface of the insulating layer 8 covering the bottom surface of the recess and the inner surface of the recess and the peripheral edge of the recess opening, which is continuous from the upper surface. To do.

本発明の発光素子において、この第二導電層9としては、導電性ペースト4を硬化させた材料からなっている。
第二導電層9を形成するために用いる導電性ペースト4としては、例えば、Agペースト、Cuペースト、カーボン含有ペーストなどが用いられ、その中でもAgペーストが好ましい。このAgペーストは、未硬化の状態では、該ペーストを基材表面に塗布するのに十分な流動性を持ち、一方、基材表面に塗布したAgペーストを低温で熱処理することにより硬化させることができ、硬化後は十分な導電性を有しているものが望ましく、例えば銀ペースト、ドータイトなどの市販品を例示することができる。導電性ペーストを絶縁層8の一部に塗布する方法は特に限定されず、スクリーン印刷、スピンコート、インクジェット法などが挙げられる。
In the light emitting device of the present invention, the second conductive layer 9 is made of a material obtained by curing the conductive paste 4.
As the conductive paste 4 used for forming the second conductive layer 9, for example, an Ag paste, a Cu paste, a carbon-containing paste, or the like is used, and among these, an Ag paste is preferable. In the uncured state, this Ag paste has sufficient fluidity to apply the paste to the substrate surface, while the Ag paste applied to the substrate surface can be cured by heat treatment at a low temperature. It is desirable to have sufficient conductivity after curing, and examples include commercially available products such as silver paste and dotite. The method for applying the conductive paste to a part of the insulating layer 8 is not particularly limited, and examples thereof include screen printing, spin coating, and inkjet method.

第二導電層9の厚さは、50nm〜400nm程度とすることが望ましい。第二導電層9の厚さが前記範囲未満であると、導電層がショートする可能性が高くなるので好ましくなく、第二導電層9の厚さが前記範囲を超えると、塗布が困難となり、コストが増加するので好ましくない。   The thickness of the second conductive layer 9 is desirably about 50 nm to 400 nm. If the thickness of the second conductive layer 9 is less than the above range, it is not preferable because the possibility that the conductive layer is short-circuited is high, and if the thickness of the second conductive layer 9 exceeds the above range, coating becomes difficult. This is not preferable because the cost increases.

本発明の発光素子は、有機材料層1を有する第一接合部材6と、凹部内に第二電極層4を有する第二接合部材7とを、凹部が有機材料層1を包み込むように第一接合部材6と第二接合部材7とを重ね合わせてなり、導電性ペーストを硬化させた導電体からなる第二導電層9を有するものなので、導電性ペーストが未硬化の状態で第一接合部材6と前記第二接合部材7とを重ね合わせることによって、有機材料層1の外面に導電性ペースト4が十分に接着し、次に、この導電性ペースト4を硬化させることによって、有機材料層1にダメージを与えることなく有機材料層1と第二電極層4とを電気的に接続でき、有機材料層1の膜厚が均一な発光素子を提供することができる。
また、有機材料層1と第二電極層4との界面の電気的、機械的接合特性が向上し、発光効率、寿命などの特性に優れた発光素子を提供することができる。
The light emitting device of the present invention includes a first bonding member 6 having the organic material layer 1 and a second bonding member 7 having the second electrode layer 4 in the recess, and the first so that the recess wraps the organic material layer 1. Since the joining member 6 and the second joining member 7 are overlapped and have the second conductive layer 9 made of a conductor obtained by curing the conductive paste, the first joining member is in an uncured state. The conductive paste 4 is sufficiently adhered to the outer surface of the organic material layer 1 by superimposing the second bonding member 7 and the second bonding member 7, and then the conductive paste 4 is cured to thereby cure the organic material layer 1. The organic material layer 1 and the second electrode layer 4 can be electrically connected without causing damage to the light-emitting element, and a light-emitting element having a uniform film thickness of the organic material layer 1 can be provided.
In addition, the electrical and mechanical joining characteristics of the interface between the organic material layer 1 and the second electrode layer 4 are improved, and a light emitting element having excellent characteristics such as luminous efficiency and lifetime can be provided.

本発明の発光素子の製造方法は、まず、平板状の透明な第一基材2上に、第一導電層3と有機材料層1とを順に成膜して第一接合部材6を作製する工程、及び凹部を有し、少なくとも該凹部内面が絶縁性を有しているキャップ形状の第二基材5に、該凹部内面及び凹部開口周縁部の一部を覆うように導電性ペースト4を塗布して第二接合部材7を作製する工程を行う。これらの第一接合部材6と第二接合部材7とを作製する工程は、前述した各構成要素について説明した材料と作製方法を用いて行うことができる。   In the method for producing a light-emitting element of the present invention, first, a first bonding member 6 is produced by sequentially forming a first conductive layer 3 and an organic material layer 1 on a flat transparent first substrate 2. The conductive paste 4 is applied to the cap-shaped second base material 5 having a process and a recess, and at least the inner surface of the recess has an insulating property so as to cover a part of the inner surface of the recess and the peripheral edge of the recess. The process of apply | coating and producing the 2nd joining member 7 is performed. The process of manufacturing the first bonding member 6 and the second bonding member 7 can be performed by using the materials and manufacturing methods described for each component described above.

次に、図1に示すように、第二接合部材7の凹部が第一接合部材6の有機材料層1を包み込むように、第一接合部材6と第二接合部材7とを重ね合わせる工程を行う。
第二接合部材7の凹部内面側に塗布された導電性ペースト4は、第二接合部材7の押圧に従って、第一接合部材6の有機材料層1を包み込むように流動し、有機材料層1表面に接着する。また、第二接合部材7の凹部開口周縁部の一部に塗布されていた導電性ペースト4は、第一基材2上の図示していない陰極側配線に接着される。
Next, as shown in FIG. 1, a step of overlapping the first bonding member 6 and the second bonding member 7 so that the concave portion of the second bonding member 7 wraps the organic material layer 1 of the first bonding member 6. Do.
The conductive paste 4 applied to the inner surface of the concave portion of the second bonding member 7 flows so as to wrap around the organic material layer 1 of the first bonding member 6 according to the pressure of the second bonding member 7, and the surface of the organic material layer 1 Adhere to. In addition, the conductive paste 4 applied to a part of the peripheral edge of the recess opening of the second bonding member 7 is bonded to a cathode-side wiring (not shown) on the first substrate 2.

次に、重ね合わせた各接合部材に熱処理を施し、導電性ペースト4を硬化させて有機材料層1と電気的に接続させ、発光素子10を得る工程を行う。この熱処理の温度は、使用する導電性ペースト4の硬化する温度とされ、できるだけ低温とすることが好ましい。   Next, a process of obtaining a light-emitting element 10 is performed by performing heat treatment on the overlapped bonding members to cure the conductive paste 4 to be electrically connected to the organic material layer 1. The temperature of this heat treatment is a temperature at which the conductive paste 4 to be used is cured, and is preferably as low as possible.

この光学素子の製造方法は、有機材料層1を有する第一接合部材6と、凹部内に第二電極層9となる導電性ペースト4を塗布した第二接合部材7とを、凹部が有機材料層1を包み込むように第一接合部材6と第二接合部材7とを重ね合わせてなり、次いで導電性ペースト4を硬化させて第二導電層9を形成するものなので、導電性ペースト4が未硬化の状態で第一接合部材6と第二接合部材7とを重ね合わせることによって、有機材料層1の外面に導電性ペースト4が十分に接着し、次に、この導電性ペースト4を硬化させることによって、有機材料層1にダメージを与えることなく有機材料層1と第二電極層9とを電気的に接続でき、有機材料層1の膜厚が均一な発光素子を歩留まりよく製造することができる。
また、有機材料層1と第二電極層9との界面の電気的、機械的接合特性が向上し、発光効率、寿命などの特性に優れた発光素子を製造することができる。
In this method of manufacturing an optical element, a first bonding member 6 having an organic material layer 1 and a second bonding member 7 in which a conductive paste 4 to be a second electrode layer 9 is applied in a concave portion, the concave portion is an organic material. Since the first bonding member 6 and the second bonding member 7 are overlapped so as to wrap the layer 1, and then the conductive paste 4 is cured to form the second conductive layer 9, the conductive paste 4 is not yet formed. By overlapping the first bonding member 6 and the second bonding member 7 in a cured state, the conductive paste 4 is sufficiently adhered to the outer surface of the organic material layer 1, and then the conductive paste 4 is cured. Accordingly, the organic material layer 1 and the second electrode layer 9 can be electrically connected without damaging the organic material layer 1, and a light-emitting element having a uniform thickness of the organic material layer 1 can be manufactured with high yield. it can.
In addition, the electrical and mechanical bonding characteristics of the interface between the organic material layer 1 and the second electrode layer 9 are improved, and a light emitting element having excellent characteristics such as luminous efficiency and lifetime can be manufactured.

[実施例]
まずガラス基板上に第一導電層(ITO 150nm/a−NPD 130nm/Coumarin6:Alq 20nm/Alq 40nmを蒸着法で成膜して第一接合部材を作製した。
また、別のガラス基板上にAgペーストを塗布して第二接合部材とした。これらの接合部材を重ね合わせた後に、熱処理してAgペーストを硬化させ、有機EL素子を製造した。
[Example]
First, a first conductive layer (ITO 150 nm / a-NPD 130 nm / Coumarin 6: Alq 3 20 nm / Alq 3 40 nm) was formed on the glass substrate by a vapor deposition method to produce a first bonding member.
Moreover, Ag paste was apply | coated on another glass substrate, and it was set as the 2nd joining member. After superimposing these joining members, the Ag paste was cured by heat treatment to produce an organic EL device.

[比較例]
ガラス基板上にITO 150nm/a−NPD 130nm/Coumarin6:Alq 20nm/Alq 40nm/Ag 200nmを全て蒸着法で成膜し、有機EL素子を製造した。
[Comparative example]
On the glass substrate, ITO 150 nm / a-NPD 130 nm / Coumarin 6: Alq 3 20 nm / Alq 3 40 nm / Ag 200 nm were formed by vapor deposition to produce an organic EL device.

実施例と比較例のそれぞれの有機EL素子に、10Vの電圧を印加して発光させ、その輝度を測定した。結果を表1に示す。   A voltage of 10 V was applied to each of the organic EL elements of Examples and Comparative Examples to emit light, and the luminance was measured. The results are shown in Table 1.

Figure 2007335105
Figure 2007335105

表1の結果より、本発明に係る実施例の有機EL素子は、比較例と比べて格段に優れた発光性能を有していることが実証された。   From the results shown in Table 1, it was demonstrated that the organic EL elements of the examples according to the present invention have significantly superior light emission performance as compared with the comparative examples.

本発明の発光素子の製造方法における第一接合部材と前記第二接合部材とを重ね合わせる工程を示す模式的な断面図である。It is typical sectional drawing which shows the process of superimposing the 1st joining member and said 2nd joining member in the manufacturing method of the light emitting element of this invention. 本発明の発光素子の一例を示す模式的な断面図である。It is typical sectional drawing which shows an example of the light emitting element of this invention.

符号の説明Explanation of symbols

1…有機材料層、2…第一基材、3…第一導電層、4…導電性ペースト、5…第二基材、6…第一接合部材、7…第二接合部材、8…絶縁層、9…第二導電層、10…発光素子。
DESCRIPTION OF SYMBOLS 1 ... Organic material layer, 2 ... 1st base material, 3 ... 1st electroconductive layer, 4 ... Conductive paste, 5 ... 2nd base material, 6 ... 1st joining member, 7 ... 2nd joining member, 8 ... Insulation Layer, 9 ... second conductive layer, 10 ... light emitting element.

Claims (2)

平板状の透明な第一基材、該第一基材上に設けられた第一導電層、及び該第一導電層上に設けられた有機材料層から構成される第一接合部材と、
凹部を有し、少なくとも該凹部内面が絶縁性を有しているキャップ形状の第二基材及び該第二基材の凹部内面と凹部開口周縁部の一部を覆うように設けられた第二導電層から構成される第二接合部材とを備え、前記凹部が前記有機材料層を包み込むように前記第一接合部材と前記第二接合部材とを重ね合わせてなる発光素子であって、
前記第二導電層が、導電性ペーストを硬化させた導電体からなることを特徴とする発光素子。
A first joining member comprising a flat transparent first base material, a first conductive layer provided on the first base material, and an organic material layer provided on the first conductive layer;
A cap-shaped second base material having a recess, and at least the inner surface of the recess has an insulating property, and a second base provided so as to cover the inner surface of the recess and a part of the peripheral edge of the recess opening. A light emitting device comprising a second bonding member composed of a conductive layer, wherein the first bonding member and the second bonding member are overlapped so that the concave portion wraps the organic material layer,
The light emitting device, wherein the second conductive layer is made of a conductor obtained by curing a conductive paste.
平板状の透明な第一基材上に、第一導電層と有機材料層とを順に成膜して第一接合部材を作製する工程、
凹部を有し、少なくとも該凹部内面が絶縁性を有しているキャップ形状の第二基材に、該凹部内面及び凹部開口周縁部の一部を覆うように導電性ペーストを塗布して第二接合部材を作製する工程、
前記凹部が前記有機材料層を包み込むように前記第一接合部材と前記第二接合部材とを重ね合わせる工程、及び
重ね合わせた各接合部材に熱処理を施して前記導電性ペーストを硬化させて前記有機材料層と電気的に接続させ、発光素子を得る工程、を含むことを特徴とする発光素子の製造方法。

A step of forming a first conductive layer and an organic material layer in order on a flat transparent first substrate to produce a first joining member,
A conductive paste is applied to a cap-shaped second base material having a recess and at least the inner surface of the recess having an insulating property so as to cover the inner surface of the recess and a part of the periphery of the opening of the recess. Producing a joining member;
A step of superimposing the first joining member and the second joining member so that the concave portion wraps the organic material layer, and heat-treating each superposed joining member to cure the conductive paste to form the organic And a step of obtaining a light emitting element by electrically connecting to a material layer.

JP2006162251A 2006-06-12 2006-06-12 Light-emitting element, and its manufacturing method Withdrawn JP2007335105A (en)

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Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US8471467B2 (en) 2009-02-05 2013-06-25 Koninklijke Philips Electronics N.V. Encapsulated electroluminescent device
US8536783B2 (en) 2009-02-05 2013-09-17 Koninklijke Philips N.V. Electroluminescent device with protective means for contact areas
CN103606549A (en) * 2009-04-23 2014-02-26 群创光电股份有限公司 Display panel and image display system using same
WO2017104399A1 (en) * 2015-12-16 2017-06-22 住友化学株式会社 Method for manufacturing organic el element, and organic el element

Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US8471467B2 (en) 2009-02-05 2013-06-25 Koninklijke Philips Electronics N.V. Encapsulated electroluminescent device
US8536783B2 (en) 2009-02-05 2013-09-17 Koninklijke Philips N.V. Electroluminescent device with protective means for contact areas
CN103606549A (en) * 2009-04-23 2014-02-26 群创光电股份有限公司 Display panel and image display system using same
WO2017104399A1 (en) * 2015-12-16 2017-06-22 住友化学株式会社 Method for manufacturing organic el element, and organic el element

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