201002128 六、發明說明： 【發明所屬之技術領域】 本發明係主要關於有機電激發光顯示器。 【先前技術】 有機電激發光顯示器中，稱爲底發射構造方式，乃於 玻璃基板上形成彩色濾光片層及CCM層，爲使該階差被 f 埋藏’經由聚醯亞胺聚矽氧烷樹脂等有機樹脂，形成有平 坦化層（外敷層）。更且，爲防止由此平坦化層殘留之水 分向有機電激發光層擴散，設有Si〇2、SiN等鈍化層。之 後，令ITO或IZO等透明電極做爲陽極，形成呈條紋狀， 於該上形成呈將逆推拔形狀的陰極分離層與透明電極正交 之條紋狀。之後’形成包含發光層之有機電激發光層，更 且’於該上部，將鋁等反射電極做爲陰極加以形成。 包含發光層之有機電激發光層係對於氧或水極爲薄弱 ί, ，僅由剝落部分或陰極缺陥部分入浸了大氣或水分而到達 有機電激發光層時’會發展成DA (黑區）或DS (黑點） 之發光缺陥點。又’陰極（反射電極）亦會氧化，使得導 電性或反射率有惡化之虞。 於此’將氧或水抑制到極限處理室內，伴隨吸濕劑， 將外蓋玻璃等封閉基板’以紫外線硬化環氧樹脂加以封閉 ，以防止空氣或水分的入浸爲一般者。但是，外蓋玻璃等 封閉基板所成封閉方法中，在對向於有機電激發光裝置之 位置’置入吸濕劑時’會有不適用於經由上部，取出光線 -5- 201002128 之頂發射型有機電激發光的問題。 在此提案有做爲封閉膜’使用氧化矽或氮化矽之方法 (例如，參照專利文獻1及2 )。但是’氧化矽（S i Ο X ) 係因在氧、水分的透過性爲不佳之故，在單獨的膜中，無 法抑制DA、DS的發生。又，氮化矽（SiNx )則應力爲大 ，由於經時變化，而恐有產生龜裂或剝離之虞。 專利文獻3中，記載有將封閉膜做爲氮化矽，記載有 令膜質向深方向調整成三階段之部分、連續成膜之部分。 又，對於層積構造所造成殘留應力的減低或防濕性能，進 行了說明。防濕性能優質的「高密度矽氮化膜5 2」係挾持 於低密度矽氮化膜5 1、5 3之中間膜。 另一方面，專利文獻4中，記載有由氮化氧化砂所成 封閉膜中，在膜的深度方向，氮原子和氧原子的比率會傾 斜性變化部分，在封閉膜中包含高氮原子層之部分。高氮 原子層乃說明可遮斷水蒸氣等。 又，專利文獻5中，記載包含由氮化矽所成障壁層之 層積構造的封閉膜。 [專利文獻1〗日本特開200 1 - 1 76653號公報 [專利文獻2 ]日本特開2 0 0 5 - 1 8 3 1 4 7號公報 [專利文獻3]日本特開20〇4-63304號公報、申請專利 範圍、段落〜0015、0027等 [專利文獻4]日本特開2005 -2093 56號公報、申請專 利範圍4〜6、段落0010〜0011、〇〇28〜0029、實施例3〜5、 段落0069等 -6- 201002128 [專利文獻5]日本特開2006- 1 64543號公報 【發明內容】 [發明欲解決之課題] 本發明係有鑑於上述現狀，提高氧、水的耐透過性， 以獲得具備抑制龜裂、剝離發生封閉膜之有機電激發光顯 示器爲目的。 [爲解決課題之手段] 本發明係爲解決上述課題所成者。即，向於由氧氮化 矽（Si OxNy)所成封閉膜的有機電激發光元件之膜，及其 相反側之膜的氮比率爲高’更且，封閉膜的中間層係經由 提高氧氮化矽（SiOxNy )的氧數，調整膜整體的應力，獲 得抑制龜裂、剝離的產生之封閉膜。 ί [發明之效果] 藉由本發明的封閉構造，可使水分及氧的遮斷性優質 ’抑制經由應力所造成龜裂的產生，防止有機電激發光元 件的劣化。又，由於不需吸濕劑，可進行由上部取出光線 之頂發射型有機電激發光顯示器之膜封閉。 【實施方式】 圖1係將有機電激發光元件的構造一部份以底發射型 1顯示。於玻璃基板U上’形成彩色濾光片層1 2及色變 -7- 201002128 換層（CCM層）13，之後，爲使該表面的凹凸被埋入，經 由聚醯亞胺聚矽氧烷樹脂等有機樹脂，形成平坦化層14。 爲防止由此平坦化層殘留之水分向有機電激發光層擴 散，設有無機氧化物、無機氮化物、無機氧化氮化物（ Si02、SiON、SiN 等）鈍化層 1 5。 於此之上，將做爲第一電極16之IZO、ITO等透明電 極，使用濺鍍法加以形成。第一電極係由在於一定方向’ 具有條紋形狀之複數部分所構成。 之後，例如，形成具有逆推拔狀的斷面形狀之電極分 離壁後，除了發光層之外，經由所期望，將包含正孔輸送 層、正孔植入層、電子輸送層、電子植入層之有機電激發 光層1 7，經由蒸鍍等加以形成。於有機電激發光層1 7上 ，第二電極1 8則使用高反射率的金屬、非晶質合金、微 結晶性合金加以形成。 第二電極1 8係經由該材料，採用蒸鍍、濺鍍、離子 電鑛等手段而形成。第二電極係對於條紋形狀之透明電極 1 6，在於正交方向具有條紋形狀，第一電極及第二電極係 以呈現交叉爲佳。經由採用如此的構成’於構成第一電極 部分電極之一，和構成第二電極部分電極之一，經由施加 電場，使此等部分電極交叉部位的有機電激發光層發光。 本發明中，從形成於上述有機電激發光層17上部之 第二電極18及分離壁上，進行氧氮化矽（SiOxNy )所成 膜封閉。膜封閉中，雖提案使用氧化矽（SiOx )或氮化矽 (SiNx )，氧化矽（SiOx )係與氮化矽（SiNx )比較，在 201002128 於氧' 水分的透過性上較差。又，另一方面，氮化矽（ SiNx )係在氧、水分的耐透過性上優、但應力卻大。 氧氮化砂（SiOxNy)係由於膜中的氧和氮比率，內部 應力會有所變化。經由提升對於氧氮化砍（SiOxNy )的氧 之氮比率，使膜質接近氮化矽（SiNx )，可降低氧、水分 的耐透過性，但應力在壓縮方向變強的傾向。經由降低氧 氮化砂（SiOxNy)的氮比率，提升氧的比率，應力向伸張 方向變化，而使氧、水分的耐透過性的變低傾向。 於此，於氧氮化矽（SiOxNy )的成膜工程，面向有機 電激發光元件之側，即，於成膜初期，提升氮比率之條件 。與應由氧或水分保護之有機電激發光元件直接接觸層， 乃難有置入龜裂或空間，而需是被覆性良好。於氧比率高 之氧氮化矽（SiOxNy )膜，具有伸張方向的應力，構成有 機電激發光元件之第二電極、與有機電激發光層的界面則 高度會有發展呈剝離之疑慮。於此，經由使具有壓縮側應 力之氮比率爲高之膜與有機電激發光元件直接接觸之保護 層，可防止由有機電激發光元件的剝離。 另一方面，關於氧、水分直接容易入侵的表面側之膜 ，避開耐透過性低的膜質，採氮比率高之氧氮化矽（ SiOxNy )膜。即，此封閉膜係經由使接近有機電激發光元 件側層及表面側層，成爲氮比率高之氧氮化矽（SiOxNy ) 膜，可提升與氧、水分有直接接觸之虞外部及面向有機電 激發光元件側的耐透過性。 挾持面向有機電激發光元件側及表面側的封閉膜之中 -9- 201002128 間層中，經由形成氧比率高之氧氮化矽（SiOxNy )膜，可 緩和發動於壓縮側之應力。 如上述，氧氮化矽（SiOxNy)膜的氮比率 '即氮/( 氮+氧）的莫爾比率’係可使用RBS (拉塞福後方散亂分 光法）加以側定。 面向有機電激發光元件側層及與面向有機電激發光元 件側相反側層的氮比率，與中間層的氮比率不同時即可， 彼此互爲相同或相異皆可，但以較中間層的氮比率爲大者 爲佳。 接觸有機電激發光元件側層及表面側層之氮比率爲高 之氧氮化矽（SiOxNy )膜和中間層之氧比率爲高之氧氮化 矽（SiOxNy )之成膜時，於各層界面，氧及氮濃度變化不 具有傾斜者爲佳。 又，CVD製程之電漿放電係於各層間無法連續進行， 各層間的電漿放電以斷續進行爲佳。經由形成做爲使各層 間獨立之膜，分散各層針孔的發生，假設即使浸入了水分 之時，可使該路徑複雜化，可將1層產生之針孔，在於其 他層的氧氮化矽（SiOxNy )膜加以封閉修補。 更且，各層係由同一元素所成僅氧、氮比率不同，相 較做爲面向有機電激發光元件側層及表面側層使用氮化矽 之情形，各層間的緊密性爲高。又，氧比率高之氧氮化矽 (S i Ο X N y )膜乃耐透過性爲低。假使，由與面向有機電激 發光元件側之相反側之氧氮化矽（S i Ο X N y )膜，入浸水分 時，在氧比率高之中間膜，具有保濕水分之功能之故，可 -10- 201002128 防止外氣之水分達到面向有機電激發光元件側 做爲成膜材料雖未特別限定，例如可使用 、NH3、N2氣體等。做爲成膜方法，可使用霄 置。 首先，氧氮化矽（SiOxNy )膜的氮/ (氮 爾比率，以 0.7〜0.99爲佳。在此條件下G 100nm~1 000nm爲佳、此時的 SiOxNy膜的應 —20〜—60MPa程度的壓縮側。 電漿放電結束後，更且，於同一批次，連 ，使氧氮化矽（SiOxNy )膜的氮/(氮+氧） 成爲0.3〜0.6，調整氮及氧的氣體比、氣壓， 漿放電而成膜。此時的氧氮化矽（SiOxNy )膜 升高，成爲接近氧化矽（SiOx)之膜質。此條 係以 500〜lOOOnrn爲佳。此時的 SiOxNy膜的 於30~90MPa的程度之伸張側。 更且，電漿放電結束後，於同一批次，連 ’與成膜初期相同，使氧氮化矽（SiOxNy ) I +氧）的莫爾比率成爲0.7〜0.99調整氣體比、 係1 00〜1 000nm，再開始電漿放電而持續成膜。 頂發射型之時，例如，於具備薄膜電晶體 將有機電激發光層以第一電極及第二電極挾持 機電激發光元件，經由本發明的製法，可形成 (S i 0 xN y )所成封閉膜。之後，封閉膜的外表 於第三封閉層表面，經由貼合形成C C Μ及彩 層。 SiH4 ' n2〇 漿 CVD裝 +氧）的莫 勺膜厚係以 力係工作於 續供給氣體 的莫爾比率 再開始、電 係氧比率則 件下的膜厚 應力係工作 續供給氣體 莫的氮/ (氮 氣壓，膜厚 等之基板， ，而形成有 由氧氮化矽 面側、即， 色瀘光片之 201002128 基板，可形成頂發射型的有機電激發光顯示器。 [實施例1] 首先，爲發光紅、綠、藍（以下簡略爲RGB )之3色 ，於基板將彩色濾光片或CCM層以照相製程加以形成。 之後，以聚醯亞胺改性聚矽氧烷樹脂，形成平滑層，接者 ，經由濺鍍法，將第二氧化物層之Si〇2膜成膜爲3 00nm 。對於濺鍍標靶，使用硼掺雜型的Si標靶，對於濺鍍氣 體中，使用Ar及02混合氣體。經由DC濺鍍法（標靶： IZO(In2 03-10 %ZnO)、濺鍍氣體：Ar、功率 250W)， 層積厚度220nm的IZO，而形成陽極，接著，經由微縮術 法，令IZO形成成特定的圖案。由此，塗佈Ιμιη的光阻 膜，經由照相製程，於發光的部位開窗，形成掩蔽罩。光 罩開口部約爲8 0x24 Ομηι。其次，排列於ΙΖΟ的資料線上 之掩蔽罩的窗間隙，在與ΙΖΟ正交方向，配置陰極分離壁 ，製作矩陣驅動的構造。其次，於真空中，將有機電激發 光層經由蒸鍍成膜後，不破壞真空下，將膜厚：200nm的 A1電極，形成成與IZO正交的圖案。 圖1乃本發明的封閉構造。如上述，於玻璃基板Η 上，形成於有機電激發光元件2 1後，不使有機電激發光 元件21曝露於大氣，於乾燥氮環境下’置入平行平板型 CVD裝置，做爲封閉膜，成膜氧氮化矽（SiOxNy )膜。 做爲初期成膜條件，使之成爲SiH4氣體爲60sccm、NH3 氣體爲 5 00secm、N20 氣體爲 1 5 0 s c c m、N 2氣體爲 -12- 201002128 2000sccm，氣壓係l〇〇pa、RF施加電力係1000W，基板平 台的溫度爲l〇〇t，膜厚爲300nm，調整成膜時間，形成 氮/(氮+氧）的莫爾比率0.7的第一封閉層22。 更且，將同一批次連續成膜條件，成爲SiH4氣體爲 60sccm、NH3 氣體爲 150sccm、N2O 氣體爲 300sccm、N2 氣體爲2000sccm，氣壓係lOOPa、RF施加電力係1 000W ，基板平台的溫度爲1 00 °C。於此條件下，使中間部約成 爲lOOOnm，調整成膜時間，而形成氮/(氮+氧）的莫爾 比率0.3的第二封閉層23。 更且，將同一批次連續成膜條件，保持在Si H4氣體 爲 60sccm、NH3 氣體爲 500sccm、N2〇 氣體爲 150sccm、 N2氣體爲 2000Sccm，氣壓係l〇〇pa、rf施加電力係 1 000W ’基板平台的溫度爲100°c，於此條件，使膜厚成 爲3 0 0 n m，調整成膜時間，形成氮/(氮+氧）的莫爾比 率0.7的第三封閉層24。之後，使用玻璃基板和UV硬化 黏著劑’於手套操作箱內加以封閉，而獲得有機電激發光 顯不器。 [實施例2] 做爲初期成膜條件，使之成爲SiH4氣體爲60sccm、 NH3氣體爲5 00 sccm' N20氣體爲50sccm、N2氣體爲 2000sccm’氣壓係l〇〇Pa、RF施加電力係1000w,基板平 台的溫度爲100°C ’膜厚爲300nm，調整成膜時間，形成 氮/ (氮+氧）的莫爾比率0.7的第一封閉層22。 -13- 201002128 更且’將同一批次連續成膜條件，成爲SiH4氣體爲 60sccm、NH3 氣體爲 4 5 0sccm、N20 氣體爲 200sccm、N2 氣體爲2000sccm，氣壓係i〇〇pa、r_f施加電力係i〇〇〇w ，基板平台的溫度爲1 〇 0 °C。於此條件下，使中間部約成 爲lOOOnm ’調整成膜時間，而形成氮/ (氮+氧）的莫爾 比率0.65的第二封閉層23。 更且，將同一批次連續成膜條件，保持在Si H4氣體 爲 60sccm、NH3 氣體爲 5 00sccm、N20 氣體爲 150secm、 N2氣體爲 2000scCm，氣壓係l〇〇pa、rf施加電力係 1 000W ’基板平台的溫度爲1〇〇 °c，於此條件，使膜厚成 爲3 00nm，調整成膜時間，形成氮/ (氮+氧）的莫爾比 率0.7的第三封閉層24。 [實施例3] 做爲初期成膜條件，使之成爲SiH4氣體爲60sccm、 NH3氣體爲170sccm、N20氣體爲20〇sccm、n2氣體爲 2000sccm，氣壓係l〇〇Pa、RF施加電力係1000W，基板平 台的溫度爲1 〇〇°C，膜厚爲3 00nm，調整成膜時間，形成 氮/ (氮+氧）的莫爾比率〇·5的第一封閉層22。更且， 將同一批次連續成膜條件，成爲SiH4氣體爲6〇sccm、 NH3氣體爲〗50sccm、N20氣體爲30〇sccni、N2氣體爲 2000sccm，氣壓係l〇〇Pa、RF施加電力係l〇〇〇W，基板平 台的溫度爲l〇〇°C。於此條件下，使中間部約成爲lOOOnrn ，調整成膜時間，而形成氮/(氮+氧）的莫爾比率0.3的 -14- 201002128 第二封閉層23。 更且，將同一批次連續成膜條件，保持在SiH4氣體 爲 60sccm、NH3 氣體爲 170sccm、N2O 氣體爲 200sccm、 N2氣體爲 2000sccm，氣壓係 lOOPa、RF施加電力係 1000W，基板平台的溫度爲100°C，於此條件，使膜厚成 爲3 OOnm，調整成膜時間，形成氮/ (氮+氧）的莫爾比 率0.5的第三封閉層24。 (比較例1 ) 做爲封閉膜，於有機電激發光元件上，將氧氮化矽（ SiOxNy )膜以下述條件成膜，其他的條件係與實施例1相 同。SiH4氣體爲60sccm、NH3氣體爲150sccm、N20氣體 爲 300sccm、N2 氣體爲 2000sccm，氣壓係 lOOPa、RF 施 加電力係 1000W，基板平台的溫度爲l〇〇°C 、而成膜 1 0 0 0 n m 〇 如此，進行實施例1到3、及比較例1獲得的有機電 激發光顯示器的可靠性評估。於60 °C、8 5%環境下’進行 1 000小時之放置，觀察每1 00cm2的暗點之個數’將此個 數收集3 00像素部分，將算出該平均値的結果’示於表1 [表Π 暗點之個數 實施例1 0.006 實施例2 0.1 實施例3 1 比較例1 3 -15- 201002128 由表1，令封閉膜的第一封閉層、第二封閉層及第二 封閉層之氮/(氮+氧）的莫爾比率的値’使之相對不同 時，明顯會影響到暗點之數。 【圖式簡單說明】 圖1乃顯示關於底發射型的有機電激發光顯示器之模 式截面圖。 圖2乃顯示關於有機電激發光顯示器之封閉構造模式 截面圖。 【主要元件符號說明】 1 :底發射型有機電激發光顯示器 10:有機電激發光顯示器 1 1 :玻璃基板 1 2 :彩色濾光片層 13 :色變換層 1 4 :平坦化層 1 5 :鈍化層 1 6 :第一電極 1 7 :有機電激發光層 1 8 :第二電極 21:有機電激發光元件 22 :第一封閉層 -16- 201002128 2 3 :第二封閉層 24 :第三封閉層 -17-201002128 VI. Description of the Invention: TECHNICAL FIELD OF THE INVENTION The present invention relates generally to organic electroluminescent display. [Prior Art] In an organic electroluminescence display, a bottom emission structure is formed by forming a color filter layer and a CCM layer on a glass substrate, so that the step is buried by f' via polyimine. An organic resin such as an alkyl resin is formed with a planarization layer (overcoat layer). Further, in order to prevent the water remaining in the planarization layer from diffusing into the organic electroluminescence layer, a passivation layer such as Si〇2 or SiN is provided. Thereafter, a transparent electrode such as ITO or IZO is used as an anode to form a stripe shape, and a cathode separation layer having a reversely drawn shape and a transparent electrode are formed in a stripe shape. Thereafter, an organic electroluminescence layer containing a light-emitting layer is formed, and a reflective electrode such as aluminum is used as a cathode in the upper portion. The organic electroluminescent layer containing the luminescent layer is extremely weak to oxygen or water. When only the exfoliated portion or the cathode defect portion is immersed in the atmosphere or moisture to reach the organic electroluminescent layer, it will develop into DA (black region). ) or DS (black dot) of the missing point. Further, the cathode (reflective electrode) is also oxidized, so that the conductivity or the reflectance is deteriorated. Here, oxygen or water is suppressed in the limit processing chamber, and the sealing substrate such as the cover glass is sealed with an ultraviolet-curable epoxy resin to prevent the intrusion of air or moisture into a general state. However, in the method of closing a closed substrate such as a cover glass, when the moisture absorbent is placed at a position opposite to the organic electroluminescent device, there is a possibility that it is not applied to the top emission of the light through the upper portion - 5 - 201002128 The problem of type organic electroluminescence. Here, there is proposed a method of using ruthenium oxide or tantalum nitride as a sealing film (for example, refer to Patent Documents 1 and 2). However, since osmium oxide (S i Ο X ) is poor in oxygen and moisture permeability, it is not possible to suppress the occurrence of DA and DS in a single film. Further, since tantalum nitride (SiNx) has a large stress, it may cause cracks or peeling due to changes over time. In Patent Document 3, a closed film is described as a tantalum nitride, and a portion in which the film quality is adjusted in three stages in the deep direction and a film is continuously formed is described. Further, the reduction in the residual stress or the moisture-proof performance caused by the laminated structure has been described. The high-density tantalum nitride film 5 2 which is excellent in moisture resistance is held in the interlayer film of the low-density tantalum nitride film 5 1 and 5 3 . On the other hand, Patent Document 4 describes a portion in which a ratio of nitrogen atoms to oxygen atoms changes in the depth direction of the film in a closed film formed of oxidized oxidized sand, and a high nitrogen atom layer is contained in the closed film. Part of it. The high nitrogen atomic layer means that water vapor and the like can be blocked. Further, Patent Document 5 describes a sealing film comprising a laminated structure of a barrier layer formed of tantalum nitride. [Patent Document 1] Japanese Patent Laid-Open Publication No. JP-A No. JP-A No. Hei. No. Hei. Japanese Patent Laid-Open No. 2005-2093, Japanese Patent Application Laid-Open No. Hei No. Hei No. Hei No. Hei No. Hei No. Hei No. Hei No. Hei. In the present invention, the permeability of oxygen and water is improved in view of the above-described state of the art, and the present invention has been made in view of the above-mentioned state of the art. It is intended to obtain an organic electroluminescence display having a sealing film that suppresses cracking and peeling. [Means for Solving the Problems] The present invention has been made to solve the above problems. That is, the film of the organic electroluminescent device formed by the yttrium oxynitride (Si OxNy) and the film on the opposite side thereof have a high nitrogen ratio, and the intermediate layer of the sealing film is enhanced by oxygen. The oxygen number of lanthanum nitride (SiOxNy) adjusts the stress of the entire film to obtain a closed film which suppresses generation of cracks and peeling. [Effect of the Invention] According to the closed structure of the present invention, it is possible to suppress the occurrence of cracks caused by stress by suppressing the high-quality barrier property of moisture and oxygen, and to prevent deterioration of the organic electroluminescence element. Further, since the moisture absorbent is not required, the film of the top emission type organic electroluminescence display which takes out the light from the upper portion can be closed. [Embodiment] Fig. 1 shows a part of the structure of an organic electroluminescence element as a bottom emission type 1. Forming a color filter layer 1 2 and a color change -7-201002128 layer (CCM layer) 13 on the glass substrate U, and then, by embedding the unevenness of the surface, via polyimine polyoxyalkylene An organic resin such as a resin forms the planarization layer 14. In order to prevent the moisture remaining in the flattening layer from diffusing into the organic electroluminescent layer, a passivation layer 15 of an inorganic oxide, an inorganic nitride, or an inorganic oxynitride (SiO 2 , SiON, SiN or the like) is provided. On the other hand, a transparent electrode such as IZO or ITO which is the first electrode 16 is formed by sputtering. The first electrode is composed of a plurality of portions having a stripe shape in a certain direction. Thereafter, for example, after forming an electrode separation wall having a reversely-drawn cross-sectional shape, in addition to the light-emitting layer, a positive hole transport layer, a positive hole implant layer, an electron transport layer, and an electron implant may be included as desired. The organic electroluminescence layer 17 of the layer is formed by vapor deposition or the like. On the organic electroluminescence layer 17 , the second electrode 18 is formed using a metal having a high reflectance, an amorphous alloy, or a microcrystalline alloy. The second electrode 18 is formed by means of vapor deposition, sputtering, ionization or the like through the material. The second electrode is a stripe-shaped transparent electrode 16 having a stripe shape in the orthogonal direction, and the first electrode and the second electrode are preferably crossed. By using such a configuration as one of the electrodes constituting the first electrode portion and one of the electrodes constituting the second electrode portion, the organic electroluminescence layer at the intersection of the partial electrodes is caused to emit light by applying an electric field. In the present invention, film formation by yttrium oxynitride (SiOxNy) is performed from the second electrode 18 and the separation wall formed on the upper portion of the organic electroluminescence layer 17. In the film sealing, although cerium oxide (SiOx) or tantalum nitride (SiNx) is proposed, the cerium oxide (SiOx) system is inferior to the permeability of oxygen in 201002128 compared with cerium nitride (SiNx). On the other hand, tantalum nitride (SiNx) is excellent in oxygen and moisture resistance, but has a large stress. The oxynitride sand (SiOxNy) has a change in internal stress due to the ratio of oxygen to nitrogen in the film. By increasing the ratio of oxygen to oxygen in the oxynitriding (SiOxNy), the film quality is close to that of tantalum nitride (SiNx), and the permeability of oxygen and moisture can be lowered, but the stress tends to be stronger in the compression direction. By lowering the nitrogen ratio of oxynitride sand (SiOxNy), the ratio of oxygen is increased, and the stress is changed in the direction of stretching, and the permeability of oxygen and moisture tends to be low. Here, in the film formation process of yttrium oxynitride (SiOxNy), the side facing the organic electroluminescence element, that is, the condition for increasing the nitrogen ratio at the initial stage of film formation. It is difficult to place cracks or spaces with the organic electroluminescent element that should be protected by oxygen or moisture, and it is difficult to have cracking or space. The yttrium oxynitride (SiOxNy) film having a high oxygen ratio has a stress in the stretching direction, and the second electrode of the electromechanical excitation light element and the interface with the organic electroluminescence layer have a high degree of development and peeling. Here, the peeling of the organic electroluminescent device can be prevented by the protective layer in which the film having the nitrogen ratio of the compressive side stress is directly in contact with the organic electroluminescent device. On the other hand, the film on the surface side where oxygen and water are directly invaded easily avoids a film having a low permeation resistance and a zirconia (SiOxNy) film having a high nitrogen extraction ratio. In other words, the closed film is made of a yttrium oxynitride (SiOxNy) film having a high nitrogen ratio by being close to the side layer and the surface side layer of the organic electroluminescent device, thereby improving the direct contact with oxygen and moisture, and facing the outside. The permeability of the electromechanical excitation element side. In the interlayer film of the side of the organic electroluminescence element and the surface side of the -9-201002128, the stress on the compression side can be alleviated by forming a yttrium oxynitride (SiOxNy) film having a high oxygen ratio. As described above, the nitrogen ratio '', i.e., the molar ratio of nitrogen/(nitrogen + oxygen)' of the oxynitride (SiOxNy) film can be set side by side using RBS (Roseford rear scattered spectroscopy). When the nitrogen ratio of the side layer facing the organic electroluminescence element and the side opposite to the side facing the organic electroluminescence element is different from the nitrogen ratio of the intermediate layer, they may be the same or different from each other, but in the middle layer The nitrogen ratio is preferably greater. When the oxynitride (SiOxNy) film having a high nitrogen ratio of the side layer and the surface side layer of the organic electroluminescent device is formed, and the oxynitride (SiOxNy) having a high oxygen ratio of the intermediate layer is formed, the interface is formed at each layer. It is better to change the oxygen and nitrogen concentration without tilting. Further, the plasma discharge of the CVD process cannot be continuously performed between the layers, and the plasma discharge between the layers is preferably performed intermittently. By forming a film which is independent of each layer, the occurrence of pinholes in each layer is dispersed, and it is assumed that the path can be complicated even when water is immersed, and the pinholes generated in one layer can be in other layers of yttrium oxynitride. The (SiOxNy) film was closed for repair. Further, each layer is made of the same element only having a different oxygen-to-nitrogen ratio, and the tantalum is used as the side layer and the surface side layer of the organic electroluminescence element, and the adhesion between the layers is high. Further, the yttrium oxynitride (S i Ο X N y ) film having a high oxygen ratio has low permeability. In the case where the yttrium oxynitride (S i Ο XN y ) film on the side opposite to the side facing the organic electroluminescence element is impregnated with water, the intermediate film having a high oxygen ratio has a function of moisturizing moisture. -10-201002128 The surface of the organic electroluminescence element is prevented from being formed as a film-forming material. The film-forming material is not particularly limited. For example, NH3 or N2 gas can be used. As a film forming method, a device can be used. First, the nitrogen/nitride ratio of yttrium oxynitride (SiOxNy) film is preferably 0.7 to 0.99. Under this condition, G 100 nm to 1 000 nm is preferable, and the SiOxNy film at this time should be -20 to 60 MPa. After the discharge of the plasma, in the same batch, the nitrogen/(nitrogen + oxygen) of the yttrium oxynitride (SiOxNy) film is adjusted to 0.3 to 0.6, and the gas ratio of nitrogen to oxygen is adjusted. Atmospheric pressure, slurry discharge film. At this time, the SiOxNy film is raised to become close to yttrium oxide (SiOx). This strip is preferably 500~100Onrn. At this time, the SiOxNy film is 30. Further, after the discharge of the plasma is completed, in the same batch, the Mohr ratio of the yttrium oxynitride (SiOxNy) I + oxygen is set to 0.7 to 0.99 in the same manner as in the initial stage of film formation. The gas ratio was adjusted to be 1 00 to 1 000 nm, and plasma discharge was started to continue film formation. In the case of the top emission type, for example, a thin film transistor is provided, and the organic electroluminescence layer is sandwiched between the first electrode and the second electrode to hold the electromechanical excitation light element, and the method of the present invention can form (S i 0 xN y ). Seal the membrane. Thereafter, the outer surface of the sealing film is formed on the surface of the third sealing layer to form a C C Μ and a color layer via lamination. The film thickness of SiH4 'n2 slurry CVD + oxygen) is based on the Moire ratio of the continuous supply of gas, and the film thickness stress under the electric oxygen ratio is continued to supply the nitrogen of the gas. / (Substrate of nitrogen pressure, film thickness, etc., and a 201002128 substrate having a yttrium oxynitride side surface, that is, a color light-emitting sheet, can be formed, and a top emission type organic electroluminescent display can be formed. [Example 1] First, in order to emit three colors of red, green, and blue (hereinafter abbreviated as RGB), a color filter or a CCM layer is formed on a substrate by a photo process. Thereafter, the polyoxymethylene resin is modified by polyimine. A smoothing layer is formed, and the Si〇2 film of the second oxide layer is formed into a film of 300 nm by sputtering. For the sputtering target, a boron-doped Si target is used for the sputtering gas. Using a mixed gas of Ar and 02. By DC sputtering (target: IZO (In2 03-10% ZnO), sputtering gas: Ar, power 250 W), IZO is laminated to a thickness of 220 nm to form an anode, and then, By the micro-shrinking method, IZO is formed into a specific pattern. Thus, the photoresist of the coating is applied. Through the photographic process, a window is opened at the light-emitting portion to form a mask. The opening of the mask is about 80×24 Ομηι. Secondly, the window gap of the mask arranged on the data line of the , is arranged in the direction orthogonal to the ΙΖΟ, and the cathode is arranged. The wall was separated to form a matrix-driven structure. Secondly, after the organic electroluminescence layer was formed into a film by vapor deposition in a vacuum, the A1 electrode having a film thickness of 200 nm was formed into a pattern orthogonal to IZO without breaking the vacuum. Fig. 1 is a closed structure of the present invention. As described above, after the organic electroluminescent device 21 is formed on the glass substrate ,, the organic electroluminescent device 21 is not exposed to the atmosphere, and is placed in a dry nitrogen atmosphere. A parallel plate type CVD apparatus is used as a sealing film to form a yttrium oxynitride (SiOxNy) film. As an initial film forming condition, it is 60 sccm for SiH4 gas, 500 sec for NH3 gas, and 150 scm for N20 gas. The N 2 gas is -12-201002128 2000 sccm, the air pressure system l〇〇pa, the RF application power system is 1000 W, the substrate platform temperature is l〇〇t, the film thickness is 300 nm, and the film formation time is adjusted to form nitrogen/(nitrogen+ Oxygen The first sealing layer 22 having a ratio of 0.7. Further, the film forming conditions of the same batch are 60 sccm for SiH4 gas, 150 sccm for NH3 gas, 300 sccm for N2O gas, 2000 sccm for N2 gas, and 100 Pa of air pressure system. 1 000 W, the temperature of the substrate platform is 100 ° C. Under this condition, the intermediate portion is made to be about 100 nm, and the film formation time is adjusted to form a second sealing layer 23 having a Mohr ratio of nitrogen / (nitrogen + oxygen) of 0.3. . Furthermore, the continuous film formation conditions of the same batch were maintained at 60 sccm for Si H4 gas, 500 sccm for NH3 gas, 150 sccm for N2 krypton gas, 2000 Sccm for N2 gas, and 1 000 W for pneumatic system l〇〇pa, rf. The temperature of the substrate stage was 100 ° C. Under this condition, the film thickness was changed to 300 nm, and the film formation time was adjusted to form a third sealing layer 24 having a Mohr ratio of nitrogen/(nitrogen + oxygen) of 0.7. Thereafter, the glass substrate and the UV hardening adhesive were used to be sealed in a glove box to obtain an organic electroluminescence. [Example 2] As an initial film formation condition, it was 60 sccm for SiH4 gas, 50 sccm for NH3 gas, 50 sccm for N20 gas, 2000 sccm for N2 gas, and 100 W for RF electric power. The temperature of the substrate platform was 100 ° C. The film thickness was 300 nm, and the film formation time was adjusted to form a first sealing layer 22 having a molar ratio of nitrogen / (nitrogen + oxygen) of 0.7. -13- 201002128 Further, 'the continuous film formation conditions of the same batch are 60 sccm for SiH4 gas, 460 sccm for NH3 gas, 200 sccm for N20 gas, 2000 sccm for N2 gas, and power system for air pressure system i〇〇pa, r_f I〇〇〇w, the substrate platform temperature is 1 〇 0 °C. Under this condition, the intermediate portion was adjusted to a film formation time of about 100 nm, and a second sealing layer 23 having a nitrogen ratio of nitrogen/(nitrogen + oxygen) of 0.65 was formed. Furthermore, the continuous film formation conditions of the same batch were maintained at 60 sccm for Si H4 gas, 500 sec for NH3 gas, 150 secm for N20 gas, 2000 scCm for N2 gas, and 1 000 W for pneumatic system l〇〇pa and rf. The temperature of the substrate stage was 1 ° C. Under the conditions, the film thickness was 300 nm, and the film formation time was adjusted to form a third sealing layer 24 having a Mohr ratio of nitrogen / (nitrogen + oxygen) of 0.7. [Example 3] As an initial film formation condition, the SiH4 gas was 60 sccm, the NH3 gas was 170 sccm, the N20 gas was 20 〇sccm, the n2 gas was 2000 sccm, the gas pressure was 100 Å, and the RF applied power was 1000 W. The substrate platform has a temperature of 1 〇〇 ° C and a film thickness of 300 nm, and the film formation time is adjusted to form a first sealing layer 22 of a nitrogen/nitrogen (nitrogen + oxygen) molar ratio 〇·5. Furthermore, the continuous film formation conditions of the same batch were 6 〇sccm for SiH4 gas, 50 sccm for NH3 gas, 30 〇 sccni for N20 gas, 2000 sccm for N2 gas, l〇〇Pa for air pressure, and power supply for RF. 〇〇〇W, the temperature of the substrate platform is l〇〇°C. Under this condition, the intermediate portion was made approximately 100 nm, and the film formation time was adjusted to form a second sealing layer 23 of -14 - 201002128 having a Mohr ratio of nitrogen / (nitrogen + oxygen) of 0.3. Furthermore, the continuous film formation conditions of the same batch were maintained at 60 sccm for SiH4 gas, 170 sccm for NH3 gas, 200 sccm for N2O gas, 2000 sccm for N2 gas, 1000 Pa for gas pressure, 1000 W for RF, and 100 for substrate platform. °C, under this condition, the film thickness was changed to 300 nm, and the film formation time was adjusted to form a third sealing layer 24 having a Mohr ratio of nitrogen/(nitrogen + oxygen) of 0.5. (Comparative Example 1) As a sealing film, a yttrium oxynitride (SiOxNy) film was formed on the organic electroluminescence device under the following conditions, and other conditions were the same as in Example 1. The SiH4 gas is 60 sccm, the NH3 gas is 150 sccm, the N20 gas is 300 sccm, the N2 gas is 2000 sccm, the gas pressure is 100 Pa, and the RF application power is 1000 W. The substrate platform temperature is 10 °C, and the film is formed at 100 nm. Thus, the reliability evaluation of the organic electroluminescent display obtained in Examples 1 to 3 and Comparative Example 1 was performed. At 60 ° C, 8 5% environment, 'place for 1 000 hours, observe the number of dark spots per 100 cm 2 ' collect the number of 300 pixels, and calculate the result of the average ' 'shown in the table 1 [Table Π Number of dark spots Example 1 0.006 Example 2 0.1 Example 3 1 Comparative Example 1 3 -15- 201002128 From Table 1, the first closed layer, the second closed layer and the second closed of the sealing film When the layer of nitrogen/(nitrogen + oxygen) has a molar ratio of 値' which makes it relatively different, it will obviously affect the number of dark spots. BRIEF DESCRIPTION OF THE DRAWINGS Fig. 1 is a schematic cross-sectional view showing an organic electroluminescent display of a bottom emission type. Figure 2 is a cross-sectional view showing a closed configuration mode of an organic electroluminescent display. [Description of main component symbols] 1 : Bottom emission type organic electroluminescent display 10: Organic electroluminescence display 1 1 : Glass substrate 1 2 : Color filter layer 13 : Color conversion layer 1 4 : Flattening layer 1 5 : Passivation layer 1 6 : first electrode 1 7 : organic electroluminescent layer 18 8 : second electrode 21 : organic electroluminescent element 22 : first sealing layer - 16 - 201002128 2 3 : second sealing layer 24 : third Sealing layer-17-