JP2008181828A - Organic el element, and its manufacturing method - Google Patents

Organic el element, and its manufacturing method Download PDF

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JP2008181828A
JP2008181828A JP2007015840A JP2007015840A JP2008181828A JP 2008181828 A JP2008181828 A JP 2008181828A JP 2007015840 A JP2007015840 A JP 2007015840A JP 2007015840 A JP2007015840 A JP 2007015840A JP 2008181828 A JP2008181828 A JP 2008181828A
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film
inorganic film
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JP4776556B2 (en
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Mari Fukao
万里 深尾
Hiroshi Kikuchi
博 菊地
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Ulvac Inc
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Abstract

<P>PROBLEM TO BE SOLVED: To provide an organic EL element wherein a protective film having moisture permeability resistance and oxygen permeability resistance is formed, and its manufacturing method. <P>SOLUTION: A display part 20 is covered with the protective film 10 in which a first inorganic film 15, an organic film 16, and a second inorganic film 17 are laminated. Thanks to the first inorganic film 15, an organic thin film material is not brought into contact with the display part 20, and the second inorganic film 17 can be formed by a sputtering method of high deposition rate since it is formed on the organic film 16. <P>COPYRIGHT: (C)2008,JPO&INPIT

Description

本発明は有機ＥＬ素子とその製造方法に関するものである。   The present invention relates to an organic EL element and a method for manufacturing the same.

有機ＥＬ素子は、低消費電力、高輝度、自己発光素子という優れた特徴を有しており、薄型テレビ等の表示装置として注目されている。
しかしながら、有機ＥＬ素子中の有機薄膜は、外部から水分、酸素が侵入すると劣化し、有機ＥＬ素子の特性が低下するという問題がある。
このため、有機ＥＬ素子において、耐水分透過性・耐酸素透過性に優れた保護層を形成し、有機薄膜を水分から保護することは、有機ＥＬ素子の長寿命化を実現する為に重要である。 An organic EL element has excellent features such as low power consumption, high luminance, and a self-light-emitting element, and has attracted attention as a display device such as a thin television.
However, there is a problem that the organic thin film in the organic EL element is deteriorated when moisture and oxygen enter from the outside, and the characteristics of the organic EL element are deteriorated.
For this reason, in organic EL devices, it is important to form a protective layer with excellent moisture permeation resistance and oxygen permeation resistance and to protect the organic thin film from moisture in order to extend the life of the organic EL device. is there.

有機ＥＬ素子に必要とされる耐水分透過性・耐酸素透過性の保護膜を形成する方法は様々報告があり、ＣＶＤ法、スパッタ法などによる成膜が一般的であるが、いずれの処理方法でも、高パワーで保護膜を形成すると、下層の有機薄膜にダメージを与えてしまうため、高い成膜レートで形成することができない。
よって、低成膜レートで形成せざるを得ず、処理時間が長くなることが問題となる。 There have been various reports on the methods for forming a moisture-permeable and oxygen-resistant protective film required for organic EL elements, and film formation by CVD, sputtering, etc. is common. However, when the protective film is formed with high power, the underlying organic thin film is damaged, and therefore cannot be formed at a high film formation rate.
Therefore, it has to be formed at a low film formation rate, and there is a problem that the processing time becomes long.

また、成膜中に有機ＥＬ素子を加熱することもできないため、緻密な保護膜を形成できず、十分な耐水分透過性・耐酸素透過性が得られない。
そこで従来技術では、十分な耐水分透過性・耐酸素透過性を得るために、保護膜の膜厚を厚く形成しており、これもまた処理時間を長くする要因となっている。
特開２００４−０２２３９８号公報 In addition, since the organic EL element cannot be heated during the film formation, a dense protective film cannot be formed, and sufficient moisture permeation resistance and oxygen permeation resistance cannot be obtained.
Therefore, in the prior art, in order to obtain sufficient moisture permeation resistance and oxygen permeation resistance, the protective film is formed thick, which is also a factor for increasing the processing time.
JP 2004-022398 A

耐水分透過性・耐酸素透過性を持った保護膜が形成された有機ＥＬ素子とその製造方法を提供する。   Provided are an organic EL element on which a protective film having moisture permeation resistance and oxygen permeation resistance is formed, and a method for producing the same.

上記課題を解決するため、本発明は、下部電極と、前記下部電極上に配置された有機ＥＬ層と、前記有機ＥＬ層上に配置された上部電極とから成る表示部と、前記表示部を覆う保護層とを有する有機ＥＬ素子であって、前記保護層は、前記表示部上に設けられた第一の無機膜と、前記第一の無機膜上に設けられた有機膜と、前記有機膜上に設けられた第二の無機膜とを有する有機ＥＬ素子である。
また、本発明は、前記第二の無機膜は、スパッタリング法によって形成された有機ＥＬ素子である。
また、本発明は、前記いずれかの有機ＥＬ素子を製造する有機ＥＬ素子の製造方法であって、前記表示部上に前記第一の無機膜を形成した後、有機膜材料を前記第一の無機膜表面に塗布し、表面が平坦な有機膜材料層を形成した後、前記有機膜材料層を硬化させ、前記有機膜を形成する有機ＥＬ素子の製造方法である。
また、本発明は、前記第一の無機膜はＣＶＤ方法によって形成する有機ＥＬ素子の製造方法である。 In order to solve the above problems, the present invention provides a display unit including a lower electrode, an organic EL layer disposed on the lower electrode, an upper electrode disposed on the organic EL layer, and the display unit. An organic EL element having a protective layer for covering, wherein the protective layer includes a first inorganic film provided on the display portion, an organic film provided on the first inorganic film, and the organic An organic EL element having a second inorganic film provided on the film.
In the present invention, the second inorganic film is an organic EL element formed by a sputtering method.
In addition, the present invention provides a method for manufacturing an organic EL element that manufactures any one of the above organic EL elements, wherein the first inorganic film is formed on the display unit, and then the organic film material is used as the first organic film material. This is an organic EL device manufacturing method in which an organic film material layer is applied by applying to an inorganic film surface to form a flat organic film material layer and then curing the organic film material layer to form the organic film.
Moreover, this invention is a manufacturing method of the organic EL element in which said 1st inorganic film is formed by CVD method.

表示部と有機膜の間に第一の無機膜が配置されているので、有機膜材料が表示部に接触せず、有機ＥＬ層に溶剤などが侵入しない。
有機膜を塗布や滴下によって形成すると、段差が平坦化され、平坦な表面に第二の無機膜を形成することができる。従って、第二の無機膜は、カバレッジ性が低いスパッタリング法で形成することができる。
有機膜上に、第二の無機膜を形成するので、高成膜レートで第二の無機膜を形成することができる。 Since the first inorganic film is disposed between the display portion and the organic film, the organic film material does not contact the display portion, and a solvent or the like does not enter the organic EL layer.
When the organic film is formed by coating or dropping, the step is flattened, and the second inorganic film can be formed on a flat surface. Therefore, the second inorganic film can be formed by a sputtering method with low coverage.
Since the second inorganic film is formed on the organic film, the second inorganic film can be formed at a high film formation rate.

図１(ｆ)の符号１１は、有機ＥＬ素子を示している。
この有機ＥＬ素子１１は、下部基板２１と、表示部２０と、保護層１０とを有している。
表示部２０は、下部基板２１上に形成された下部電極２２と、下部電極２２上に形成された有機ＥＬ層２３と、有機ＥＬ層２３上に形成された上部電極２４とを有しており、保護層１０は、表示部２０を覆っており、上部基板２５は、保護層１０上に配置されている。アクティブ型の素子の場合、保護層１０の下層の表示部２０内にトランジスタが設けられている。 The code | symbol 11 of FIG.1 (f) has shown the organic EL element.
The organic EL element 11 includes a lower substrate 21, a display unit 20, and a protective layer 10.
The display unit 20 includes a lower electrode 22 formed on the lower substrate 21, an organic EL layer 23 formed on the lower electrode 22, and an upper electrode 24 formed on the organic EL layer 23. The protective layer 10 covers the display unit 20, and the upper substrate 25 is disposed on the protective layer 10. In the case of an active element, a transistor is provided in the display unit 20 below the protective layer 10.

保護層１０は、リング状の封止部材２８で取り囲まれており、封止部材２８上には、上部基板２５が乗せられ、有機ＥＬ層２３と、下部及び上部電極２２、２４は、保護層１０で保護された状態で、下部及び上部基板２１、２５と封止部材２８とで、大気に触れないように密閉されている。   The protective layer 10 is surrounded by a ring-shaped sealing member 28, an upper substrate 25 is placed on the sealing member 28, and the organic EL layer 23 and the lower and upper electrodes 22, 24 are formed of a protective layer. 10, the lower and upper substrates 21 and 25 and the sealing member 28 are hermetically sealed so as not to be exposed to the atmosphere.

保護層１０は三層構造であり、保護層１０を形成して有機ＥＬ素子１１を製造する工程を説明すると、図１(ａ)の下部基板２１上には、下部電極２２と、有機ＥＬ層２３と、上部電極２４が形成されており、この状態の下部基板２１を真空成膜装置内に搬入し、同図(ｂ)に示すように、第一の無機膜１５を形成する。   The protective layer 10 has a three-layer structure, and a process of forming the protective layer 10 to manufacture the organic EL element 11 will be described. A lower electrode 22 and an organic EL layer are formed on the lower substrate 21 in FIG. 23 and an upper electrode 24 are formed. The lower substrate 21 in this state is carried into a vacuum film forming apparatus, and a first inorganic film 15 is formed as shown in FIG.

ここでは、第一の無機膜１５には、シリコン酸化膜が用いられている。
第一の無機膜１５は、後述する有機膜１６を形成するための有機膜材料が有機ＥＬ層２３と接触し、有機ＥＬ層２３中に、有機膜材料の成分が浸透することを防止するための薄膜であり、耐水分透過性や、耐酸素透過性は必要がない。従って、第一の無機膜１５は、ＣＶＤ方法、スパッタリング方法、真空蒸着方法等の成膜方法で形成することができるが、表示部２０には段差が存在するので、ステップカバレッジのためにはＣＶＤ法による成膜が望ましい。また、膜厚は１００ｎｍ〜３００ｎｍが望ましい。 Here, a silicon oxide film is used for the first inorganic film 15.
The first inorganic film 15 prevents an organic film material for forming the organic film 16 to be described later from coming into contact with the organic EL layer 23 and the organic film material component from penetrating into the organic EL layer 23. It is a thin film and does not need moisture permeation resistance or oxygen permeation resistance. Accordingly, the first inorganic film 15 can be formed by a film forming method such as a CVD method, a sputtering method, or a vacuum vapor deposition method. However, since there is a step in the display unit 20, a CVD is used for step coverage. Film formation by the method is desirable. The film thickness is preferably 100 nm to 300 nm.

下部基板２１の表面のうち、封止部材２８の外部になる外周付近には、接続端子が配置されており、下部及び上部電極２２、２４は、接続配線によって接続端子に接続されており、第一の無機膜１５は、接続配線が表示部２０から外周方向に導出された状態で、下部電極２２と有機ＥＬ層２３と上部電極２４の側面や表面を覆っている。   Of the surface of the lower substrate 21, connection terminals are arranged near the outer periphery that is outside the sealing member 28, and the lower and upper electrodes 22, 24 are connected to the connection terminals by connection wiring, One inorganic film 15 covers the side surfaces and surfaces of the lower electrode 22, the organic EL layer 23, and the upper electrode 24 in a state where the connection wiring is led out from the display unit 20 in the outer peripheral direction.

第一の無機膜１５の表面には、表示部２０の段差が反映され、段差が生じており、第一の無機膜１５が形成された下部基板２１を、スクリーン印刷装置内に搬入し、第一の無機膜１５の表面に光硬化型の有機膜材料を塗布し、表面の凹部内に有機膜材料が充填された有機膜材料層を形成する。このとき、第一の無機膜１５の平坦な部分との距離を一定にして下部基板２１上にブレードを配置し、その状態でブレードを移動させて余分な有機膜材料を除去し、有機膜材料層の表面を平坦にする(スクリーン印刷法)。   The step of the display unit 20 is reflected on the surface of the first inorganic film 15, and a step is generated. The lower substrate 21 on which the first inorganic film 15 is formed is carried into the screen printing apparatus, and A photocurable organic film material is applied to the surface of one inorganic film 15 to form an organic film material layer in which the organic film material is filled in the recesses on the surface. At this time, a blade is disposed on the lower substrate 21 with a constant distance from the flat portion of the first inorganic film 15, and the blade is moved in this state to remove excess organic film material. The surface of the layer is flattened (screen printing method).

次いで、紫外線を照射して有機膜材料層を硬化させ、同図(ｃ)に示すように、第一の無機膜１５上に有機膜１６を形成する。有機膜材料には、光硬化性のエポキシ樹脂を用い、エポキシ樹脂の有機膜１６を形成することができる。   Next, the organic film material layer is cured by irradiating ultraviolet rays, and an organic film 16 is formed on the first inorganic film 15 as shown in FIG. As the organic film material, a photocurable epoxy resin is used, and the organic film 16 of the epoxy resin can be formed.

有機膜材料は塗布可能な２０ｃｐ(２０センチポアズ)以下の粘度であることが好ましい。また、有機ＥＬ層２３を放熱させるために、有機膜１６は、０．２Ｗ／ｍ・Ｋ以上の高熱伝導性が望ましい。
表面の凹部を充填し、表面が平坦な有機膜１６を得るためには、塗布法に限定されるものではなく、より低粘度の有機膜材料を滴下し、凹部内に流入させ、硬化させてもよい。 The organic film material preferably has a viscosity of 20 cp (20 centipoise) or less that can be applied. In order to dissipate the heat from the organic EL layer 23, the organic film 16 desirably has a high thermal conductivity of 0.2 W / m · K or more.
In order to fill the concave portion on the surface and obtain the organic film 16 having a flat surface, the coating method is not limited to the coating method, and a lower viscosity organic film material is dropped, allowed to flow into the concave portion, and cured. Also good.

次に、有機膜１６が形成された下部基板２１を成膜装置内に搬入し、有機膜１６の表面に第二の無機膜１７を形成すると、第一の無機膜１５と有機膜１６と第二の無機膜１７から成り、表示部２０を覆う三層構造の保護層１０が得られる。
有機膜１６は、第一の無機膜１５の表面と側面を覆っており、有機膜１６は表示部２０と接触していない。 Next, when the lower substrate 21 on which the organic film 16 is formed is carried into the film forming apparatus and the second inorganic film 17 is formed on the surface of the organic film 16, the first inorganic film 15, the organic film 16, The protective layer 10 having a three-layer structure that includes the two inorganic films 17 and covers the display unit 20 is obtained.
The organic film 16 covers the surface and side surfaces of the first inorganic film 15, and the organic film 16 is not in contact with the display unit 20.

有機ＥＬ層２３と第二の無機膜１７の間には、第一の無機膜１５と有機膜１６が配置されており、有機膜１６が第二の無機膜１７を形成するときのダメージを受けても有機ＥＬ層２３はダメージを受けないから、第二の無機膜１７をスパッタリング法によって高成膜レートで形成することができる。
水分や酸素の透過は第二の無機膜１７によって防止するため、第二の無機膜１７には、膜厚２μｍ以上のシリコン窒化膜やシリコン酸化膜が好ましい。 Between the organic EL layer 23 and the second inorganic film 17, the first inorganic film 15 and the organic film 16 are disposed, and the organic film 16 receives damage when the second inorganic film 17 is formed. However, since the organic EL layer 23 is not damaged, the second inorganic film 17 can be formed at a high film formation rate by the sputtering method.
Since the second inorganic film 17 prevents permeation of moisture and oxygen, the second inorganic film 17 is preferably a silicon nitride film or silicon oxide film having a thickness of 2 μm or more.

次に、下部基板２１の表面の外周付近に封着材料２９を配置し、表示部２０を封着材料２９によって取り囲む。有機膜１６は、封着材料２９が取り囲む領域内に配置されている。
真空雰囲気中で上部基板２５を封着材料２９上に乗せる。ここでは封着材料２９は低融点ガラスであり、加熱によって溶融させ、固化させると、同図(ｆ)に示すように、硬化した封着材料２９によってリング状の封止部材２８が形成され、有機ＥＬ素子１１が得られる。 Next, the sealing material 29 is disposed near the outer periphery of the surface of the lower substrate 21, and the display unit 20 is surrounded by the sealing material 29. The organic film 16 is disposed in a region surrounded by the sealing material 29.
The upper substrate 25 is placed on the sealing material 29 in a vacuum atmosphere. Here, the sealing material 29 is a low-melting glass, and when melted by heating and solidified, as shown in FIG. 5F, a ring-shaped sealing member 28 is formed by the cured sealing material 29, The organic EL element 11 is obtained.

上述したように、下部電極２２や上部電極２４に接続された接続配線は、封止部材２８と下部基板２１の間から封止部材２８の外部に導出されており、封止部材２８の外部で下部基板２１上の接続端子に接続されているが、その部分の図示は省略する。アクティブ型の素子の場合、トランジスタを制御するための接続配線も、封止部材２８の外部に導出される。
下部電極２２と上部電極２４によって有機ＥＬ層２３に電圧を印加すると、印加された部分の有機ＥＬ層２３が発光し、発光光が有機ＥＬ層２３の外部に放出される。 As described above, the connection wiring connected to the lower electrode 22 and the upper electrode 24 is led to the outside of the sealing member 28 from between the sealing member 28 and the lower substrate 21, and outside the sealing member 28. Although connected to the connection terminal on the lower substrate 21, the illustration of that portion is omitted. In the case of an active element, connection wiring for controlling the transistor is also led out of the sealing member 28.
When a voltage is applied to the organic EL layer 23 by the lower electrode 22 and the upper electrode 24, the applied portion of the organic EL layer 23 emits light, and emitted light is emitted to the outside of the organic EL layer 23.

トップエミッション型デバイスの場合は、上部基板２５が表示面になるから、上部基板２５から発光光を放出させるために、上部基板２５には、ガラス等の透明な材料を用い、保護層１０は９０％以上の光透過率が必要である。
また、トップエミッション型のデバイスの場合、上部基板２５にカラーフィルタを配置しておくと、カラー表示が可能である。 In the case of a top emission type device, since the upper substrate 25 becomes a display surface, a transparent material such as glass is used for the upper substrate 25 in order to emit emitted light from the upper substrate 25, and the protective layer 10 is 90. % Light transmittance is required.
In the case of a top emission type device, color display is possible if a color filter is arranged on the upper substrate 25.

(ａ)〜(ｆ)：本発明の有機ＥＬ素子の製造工程図(a)-(f): Manufacturing process diagram of organic EL device of the present invention

符号の説明Explanation of symbols

１０……保護層
１１……有機ＥＬ素子
１５……第一の無機膜
１６……有機膜
１７……第二の無機膜
２０……表示部
２１……下部基板
２２……下部電極
２３……有機ＥＬ層
２４……上部電極
２５……上部基板 DESCRIPTION OF SYMBOLS 10 ... Protective layer 11 ... Organic EL element 15 ... 1st inorganic film 16 ... Organic film 17 ... 2nd inorganic film 20 ... Display part 21 ... Lower substrate 22 ... Lower electrode 23 ... Organic EL layer 24 …… Upper electrode 25 …… Upper substrate

Claims (4)

下部電極と、前記下部電極上に配置された有機ＥＬ層と、前記有機ＥＬ層上に配置された上部電極とから成る表示部と、
前記表示部を覆う保護層とを有する有機ＥＬ素子であって、
前記保護層は、前記表示部上に設けられた第一の無機膜と、前記第一の無機膜上に設けられた有機膜と、前記有機膜上に設けられた第二の無機膜とを有する有機ＥＬ素子。 A display unit comprising a lower electrode, an organic EL layer disposed on the lower electrode, and an upper electrode disposed on the organic EL layer;
An organic EL element having a protective layer covering the display unit,
The protective layer includes a first inorganic film provided on the display unit, an organic film provided on the first inorganic film, and a second inorganic film provided on the organic film. Organic EL element having 前記第二の無機膜は、スパッタリング法によって形成された請求項１記載の有機ＥＬ素子。   The organic EL element according to claim 1, wherein the second inorganic film is formed by a sputtering method. 請求項１又は請求項２のいずれか１項記載の有機ＥＬ素子を製造する有機ＥＬ素子の製造方法であって、
前記表示部上に前記第一の無機膜を形成した後、有機膜材料を前記第一の無機膜表面に塗布し、表面が平坦な有機膜材料層を形成した後、前記有機膜材料層を硬化させ、前記有機膜を形成する有機ＥＬ素子の製造方法。 It is a manufacturing method of the organic EL element which manufactures the organic EL element of any one of Claim 1 or Claim 2,
After forming the first inorganic film on the display unit, an organic film material is applied to the surface of the first inorganic film to form an organic film material layer having a flat surface, and then the organic film material layer is formed. A method for producing an organic EL device, which is cured to form the organic film. 前記第一の無機膜はＣＶＤ方法によって形成する請求項３記載の有機ＥＬ素子の製造方法。   The method of manufacturing an organic EL element according to claim 3, wherein the first inorganic film is formed by a CVD method.
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