TWI229569B - Light emitting device and method for producing the same - Google Patents
Light emitting device and method for producing the same Download PDFInfo
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12295691229569
【發明所屬之技術領域】 本發明係有關於一種發光裝置,尤指一種具有三波長 發白光特性之有機電激發光裝置及其製作方法。 【先前技術】 有機電激發光裝置(0rganic Light Emitting Deviee ;〇LED)自從1 987 年由柯達公司的c· w· Tang&s· A. VanSiyk e利用真空蒸鍍方式,將電洞傳輸材料及電子傳輸材料, 如Alq3,分別鍍覆於透明之IT〇玻璃上,其後再蒸鍍一金 屬電極形成具有自發光性、高應答速度、重量輕、厚度薄 、低耗電、廣視角、高亮度及可全彩化的有機電激發光元 件το件(0LED)。此後,有機電激發光元件被視為是顯示器 產業之明星產品,大家莫不希望其可早曰運用於全彩化顯 不器或投射出白色光源,以達到真正可兼具綠色環保及省 電功效之照明理想境界。 請參閱第1圖,係為習用〇LED之構造剖視圖,該有機 電激發光裝置(OLED)IO主要係在一透光基板u上蒸鍍形成 一透光可導電性之陽極(IT0)13,並於該17()陽極13上再依 序形成一電洞傳輸層(HTL)15、發光層(EML)17及一金屬陰 極19,另外於發光層17内摻雜(Doping) 一螢光物質(未顯 示),當陽極1 3及陰極1 9受到外加偏壓作用時:電洞將可 自I TO陽極1 3經由電洞傳輸層i 5傳輸至發光層,而電子 也相對可從陰極1 9傳輸至發光層1 7,發光層1 7内的電子及 電洞將可因為再結合作用(Rec〇mbi nat i〇n )而產生激態分[Technical field to which the invention belongs] The present invention relates to a light-emitting device, and more particularly to an organic electro-optical light-emitting device having three-wavelength white light emission characteristics and a method for manufacturing the same. [Prior technology] Organic light-excitation light-emitting devices (0rganic Light Emitting Deviee; 0LED) have been used by Kodak's c · w · Tang & s · A. VanSiyk e to transfer materials and Electron transmission materials, such as Alq3, are respectively plated on transparent IT0 glass, and then a metal electrode is evaporated to form a self-luminous, high response speed, light weight, thin thickness, low power consumption, wide viewing angle, high Bright and full-colorable organic electro-optic light emitting element το (0LED). Since then, organic electroluminescent devices have been regarded as the star products of the display industry. Everyone hopes that they can be applied to full-color displays or project white light sources to achieve true environmental protection and power saving effects. The ideal state of lighting. Please refer to FIG. 1, which is a cross-sectional view of the structure of a conventional OLED. The organic electroluminescent device (OLED) IO is mainly deposited on a transparent substrate u to form a transparent conductive anode (IT0) 13. A hole transport layer (HTL) 15, a light emitting layer (EML) 17 and a metal cathode 19 are sequentially formed on the 17 () anode 13 and a fluorescent substance is doped in the light emitting layer 17 (Not shown), when the anode 13 and the cathode 19 are subjected to an external bias: holes can be transferred from the ITO anode 13 to the light-emitting layer through the hole transport layer i 5, and the electrons can also be relatively discharged from the cathode 1 9 is transmitted to the light-emitting layer 17 and the electrons and holes in the light-emitting layer 17 can generate excitatory components due to recombination (Rec〇mbi nat i〇n).
第5頁 1229569Page 5 1229569
子(exciton),激態分子在釋放出能量而再回至基態時 可自行在發光層17内發光,或再激發摻雜之螢光物 發狀態並投射出所設定之特定範圍波長光源。 、' 雖然上述第一種習用之0LED構造及技術雖然可達到 射光源之效果,惟其僅可投射單色光源而無法達到投射白 色光源或全彩化之終極目標。 請參閱第2圖,係為另一種習用0LED之各元件能階示 意圖,該項技術主要是除了 IT0陽極22、電子傳輸層(ETL) 24及陰極25外,還包括有一介於陽極22及電子傳輸層間 之電洞傳輸層(HTL)23,由於搭配電子傳輸層24及^洞 輸層23材質之選用,致使電子傳輸層24及電洞傳輸層23 帶間之能階差(EC1-EC2 )將小於兩者間之傳導帶間^能二 差(EV1-EV2),如此一來,電子傳輸層24内傳輪至電洞傳 輸層23之電子數量將遠超過反方向傳輸至電子傳輸層“之 電洞數量,因此電子與電洞之再結合及投射光源之^置將 發生於電洞傳輸層23。另外,為了方便電洞之自陽極以傳 輸並注入電洞傳輸層2 3中,於此專利中還揭露有一設於 極2 2與電洞傳輸層2 3間之電洞注入層。 雖然上述之摩托羅拉專利技術中,可將速度移動較快 的電洞留置於電洞傳輸層23中與電子進行再結合程序而提 高發光效率,惟其亦僅可投射出單色光源,且同樣無法達 到投射白色光源或全彩化之終極目標。 為了達到0LED可用於白色光源及全彩化之終極目標, 業界莫不尋求各種解決之技術方案,目前主要可達到Ζ乘Exciton, when the excimer molecule releases energy and returns to the ground state, it can emit light in the light-emitting layer 17 by itself, or re-excite the doped fluorescent light emitting state and project a set range of wavelength light source. Although the above-mentioned first conventional 0LED structure and technology can achieve the effect of a light source, it can only project a monochromatic light source and cannot reach the ultimate goal of projecting a white light source or full color. Please refer to Figure 2, which is a schematic diagram of the energy levels of another conventional 0LED. The technology mainly includes an anode 22 and an electron in addition to the IT0 anode 22, the electron transport layer (ETL) 24 and the cathode 25. The hole transport layer (HTL) 23 between the transmission layers, due to the choice of materials for the electron transport layer 24 and the hole transport layer 23, results in the energy step difference between the electron transport layer 24 and the hole transport layer 23 (EC1-EC2) It will be less than the energy difference between the two conduction bands (EV1-EV2). In this way, the number of electrons transferred to the hole transport layer 23 in the electron transport layer 24 will far exceed the number of electrons transferred to the electron transport layer in the opposite direction. The number of holes, so the recombination of electrons and holes and the placement of the projection light source will occur in the hole transmission layer 23. In addition, in order to facilitate the hole from the anode to transmit and inject into the hole transmission layer 23, in This patent also discloses a hole injection layer provided between the electrode 22 and the hole transmission layer 23. Although the aforementioned Motorola patented technology, a hole that moves faster can be left in the hole transmission layer 23. Improve the luminous efficiency by recombination procedure with electrons However, it can only project a monochromatic light source, and it cannot reach the ultimate goal of projecting a white light source or full color. In order to achieve the ultimate goal of 0LED being used as a white light source and full color, the industry must seek various technical solutions. At present, Mainly can reach ZO multiplication
第6頁 1229569 五、發明說明(3) 效果之解決方案計有下列三種: 1.光色轉換法(Color Conversion): 其主要是利用藍光為發射源,再將此藍光激發一光色 轉換薄膜以取得紅綠藍(R G B )三原色可見光,並希望 藉此以達到全彩化或投射白色光源之目的; 王 惟,在此種技術中,不僅光色轉換薄膜之光色純度及 發光效率不甚滿意,且因為色轉換材料會吸收環境之 藍光(或紫外光),將造成潛在之對比及畫素問題f 2·彩色濾光膜法(ColorFilter): 、 利用白色有機電激材料為背光源,搭配使用已用.於lc D之彩色濾光片,以期望達到全彩的效果; 然,此種技術之關鍵點在於白色光源如何取得,且白 色光源是否為全波段連續光源及如何提升發光效率, 皆是產品欲量產化之前必須突破之技 3·紅藍綠三色獨立發光法: ‘‘” 主要是將RGB三原色獨自發光,#月望 取得全彩效果,或再搭配以成為白色光源。万式以 但色要獨立各自發光,其色彩平衡性較差 ,二:精細J之要求亦增加製程之 不同色彩之有機物質獨立發光, ^個 命及控制難易度亦各有不n ^尤政旱、使用辱 釗蚰虹的产只& & ^有不冋,例如紅色光源就難以達 到、,,屯、…兄界而偏向橘紅色’其使用壽命相對亦短。 1229569Page 6 1229569 V. Explanation of the invention (3) There are three solutions for the effect: 1. Color conversion method: It mainly uses blue light as the emission source, and then excites this blue light into a light color conversion film. In order to obtain the three primary colors of red, green and blue (RGB) visible light, and hope to use it to achieve the purpose of full color or project a white light source; Wang Wei, in this technology, not only the light color purity and luminous efficiency of the light color conversion film is not very good Satisfactory, and because the color conversion material will absorb the blue light (or ultraviolet light) of the environment, it will cause potential contrast and pixel problems. F 2 · Color Filter Method: Use white organic electro-active material as the backlight. Use color filters that have been used in lc D to achieve full-color effects; however, the key point of this technology is how to obtain a white light source, and whether the white light source is a full-band continuous light source and how to improve luminous efficiency. , Are the technologies that must be broken before the product is mass-produced 3. Red, blue and green three-color independent light-emitting method: "" The main three colors of RGB are emitted alone, # 月 望 achieved full color effect Or, it can be matched to become a white light source. The color must be independently emitted, and its color balance is poor. Second: The requirement of fine J also increases the independent emission of organic substances of different colors in the manufacturing process. There are also differences ^ You Zhenghan, the use of insulting Zhao Honghong's production is only okay, for example, the red light source is difficult to reach ,,,,,,,,,,,, ... Also short. 1229569
1229569 五、發明說明(5) 【實施方式】 茲為使貴審查委員對本發明之結構特徵及所達成之 功效有更進一步之暸解與認識,謹佐以較佳之實施例圖及 配合詳細之說明,說明如后: ^首先,請參閱第3圖,係為本發明一較佳實施例之構 造截面圖;如圖所示,本發明有機電激發光裝置3〇主要係 f 一透光基板31之上側以蒸鍍或濺鍍等方式以形成一第二 ‘ 層3 3 (如魴極)’而在陽極3 3之上侧再依序形成一電 洞傳輸層35 (HTL ;第一載子傳輸層)及一具有阻隔第二載 子(電子)前進之電子阻隔層47 (electron blocking layer),電子阻隔層47之上侧再依序形成有一第一主體材 料層41 (Host 1)、弟一主體材料層42 (Host 2)及第三主 ,材料層43 (Host 3),且於第三主體材料層43之上;;依 序形成有一可阻隔電洞前進之電洞阻隔層45 (h〇le mnLuyer)、電子傳輸層37 (etl ;第二載子傳輸層 ^及陰極3 9。 藉由電子阻隔層47,可將來自於陰極39 電洞傳輸層35之上側,換言之,即是將電子限 3 (43)、Host 2 “㈧及化以丨(41)内;另 將來自於陽極33之電洞阻隔於電4二 之底側,換s之,即是將電洞同樣限制於η〇^ ^1229569 V. Description of the invention (5) [Embodiment] In order to make your reviewing members have a better understanding and understanding of the structural features and effects achieved by the present invention, I would like to provide a better description of the embodiment and the detailed description, The explanation is as follows: ^ First, please refer to FIG. 3, which is a structural cross-sectional view of a preferred embodiment of the present invention; as shown in the figure, the organic electro-optical excitation device 30 of the present invention is mainly a light-transmitting substrate 31. The upper side is formed by a method such as evaporation or sputtering to form a second 'layer 3 3 (e.g., ytterbium electrode)', and a hole transport layer 35 (HTL; first carrier transport) is sequentially formed on the upper side of the anode 3 3. Layer) and an electron blocking layer 47 (electron blocking layer) that blocks the second carrier (electrons) from advancing. A first host material layer 41 (Host 1), a first The host material layer 42 (Host 2) and the third host material layer 43 (Host 3) are on top of the third host material layer 43; a hole blocking layer 45 (h 〇le mnLuyer), electron transport layer 37 (etl; second carrier transport layer ^, and cathode 3 9 With the electron blocking layer 47, it can come from the upper side of the cathode 39 hole transport layer 35, in other words, the electron limit 3 (43) and Host 2 are reduced to within (41); The hole on the anode 33 is blocked on the bottom side of the battery 42. In other words, the hole is also limited to η〇 ^ ^
Host 2 (42)及Host 3 (43)内。由於大部分的電及洞 將被引導且被限制在Host丨、H〇 兩、 nost3乾圍内,因 此電子電洞對在此相對亦有較大的機率於各主體材料層Host 2 (42) and Host 3 (43). Since most of the holes and holes will be guided and confined to the host, H0, and nost3, the electron hole pair will have a greater chance of being in each main material layer.
第9頁 1229569 五、發明說明(6) 内進形再結合動作,藉此,以有效提高各主體材料層之發 光效率者。 在第一主體材料層4 1内混雜(m丨x i ng )有一第一客發光 體物質,第二主體材料層42内同樣混雜設有一 相對應之第一各發光體物質(Guest 2),而第三主體材料 層43内一樣混雜設有一相對應之第三客發光體物質(Guest 3 ),這些客發光體物質係可選擇為一可相對應搭配之螢光 物質、磷光物質或兩者之混合物,其可在電子電洞對再結 合時,受到激態分子之能量釋放而投射出相對應之不同色 光源,例如在此實施例中,Guest 1可投射紅光(R),, Guest 2投射藍光(B),而Guest 3投射綠光(G),如此即可 因此產出RGB二波段三原色,而組合出一全波段連續光譜 之白色光源或全彩化產品,不僅製程相對簡單,且可有效 增加發光效率。 當然’對白光或全彩之理想c丨E色度圖體系規袼而言 ’綠光之濃度相對於紅光及藍光要稍微增加,因此,在此 實施例中’可投射出綠光之Guest 3濃度相對於Guest 1及 Guest 2的濃度.也要相對為高,且,在H〇st 3之電子電洞 對數量也可設計為相對於H〇st 1&H〇st 2為大,而H〇st 1 、Host 2及Host 3之位置安排全有賴於其能階之相對搭配 再者’請參閱第4圖,係為本發明又一實施例之構造 截面圖;如圖所示,在此實施例中,其主要係在一可由玻 璃、石英或塑膠製成之透光基板3丨上以蒸鍍或濺鍍等方式Page 9 1229569 V. Description of the invention (6) Inner shape recombination action, in order to effectively improve the luminous efficiency of each main material layer. A first guest luminous substance is mixed (m 丨 xi ng) in the first host material layer 41, and a corresponding first luminous substance (Guest 2) is also mixed in the second host material layer 42, and A corresponding third guest luminous substance (Guest 3) is also mixed in the third host material layer 43. These guest luminous substances can be selected as a corresponding fluorescent substance, phosphorescent substance, or both. A mixture that can project a different color light source when the electron hole pair is recombined and is released by the energy of the excimer molecule. For example, in this embodiment, Guest 1 can project red light (R), and Guest 2 Projects blue light (B), and Guest 3 projects green light (G), so you can produce RGB two-band three primary colors, and combine a white light source or full-color product with a full-band continuous spectrum. Not only is the process relatively simple, but Can effectively increase luminous efficiency. Of course, for the ideal c 丨 E chromaticity diagram system specification of white light or full color, the concentration of green light is slightly increased relative to red light and blue light. Therefore, in this embodiment, a guest who can project green light The concentration of 3 is relative to that of Guest 1 and Guest 2. It should also be relatively high, and the number of electron hole pairs in H0st 3 can also be designed to be larger than H0st 1 & H0st 2 and The positional arrangement of H0st 1, Host 2 and Host 3 all depends on the relative matching of their energy levels. Also, please refer to FIG. 4, which is a structural cross-sectional view of another embodiment of the present invention; In this embodiment, it is mainly formed on a light-transmitting substrate 3 made of glass, quartz, or plastic by evaporation or sputtering.
第10頁 五、發明說明(7) 形成一可,銦錫氧化物(IT〇)、聚苯胺(pANI)、氧化鋅( ZnOx)、氧化鉬(Μ〇〇χ)、氧化釩(ν〇χ)、氧化釕(Ru〇x)、 Au、CuI、Sn02或ZnO等具透光導電性功效之金屬、合金、 化合物或混合物所構成之陽極33。接續,IT〇 33之上表面 再依續形成一可由M-MTDATA所構成之電洞注入層(hil)53 、由NPB所構成之電洞傳輸層(htl)35、由UF所構成之電 子阻隔層47、由NPB所構成之第一主體材料層41、由DpvBi 所構成之第二主體材料層42、由Alq3所構成之第三主體材 料層43、由BCP所構成之電洞阻隔層45、由Alq所構成之電 子傳輸層(ETL)37、由LiF所構成之電子注入層(EIL)57、 及一可由Au、Al、Mg、Pt、Ag、MgAg、AlLi、AlLiO、AIL ΐ F或Ca等具導電性材質所構成之陰極3 9。 其中,第一主體材料層41之NPB中混雜設有至少一可 才又射出紅光之DCM2物質,第二主體材料層42之DPVBi中混 雜設有至少一可投射出藍光之DSA物質,而第三主體材料 層4 3之A1 q 3中混雜設有至少一可投射出綠光之c 6物質,藉 由上述各主體材料層(Hosts )之能階位置安排,致使因為 電洞阻隔層4 5及電子阻隔層4 7之阻隔作用而被受限於NpB 41、DPVBi 42、Alq3 43範圍内之電子電洞對將可普遍分 ,於各個主體材料層41〜43中。當一外加偏壓作用下,可 藉由各個客發光體物質(Guest),而可投射出紅、藍、綠 三原色光源,形成一個完整之三波長投射光源體系,而可 #易達成全波段之白色光源或全彩化產品。Page 10 V. Description of the invention (7) Formation of indium tin oxide (IT〇), polyaniline (pANI), zinc oxide (ZnOx), molybdenum oxide (MOZO), vanadium oxide (ν〇χ) ), Ruthenium oxide (Ru0x), Au, CuI, Sn02, or ZnO and other anodes 33 composed of metals, alloys, compounds or mixtures with light transmission conductivity. Subsequently, a hole injection layer (hil) 53 made of M-MTDATA, a hole transport layer (htl) 35 made of NPB, and an electron barrier made of UF were sequentially formed on the upper surface of IT03. Layer 47, a first host material layer 41 made of NPB, a second host material layer 42 made of DpvBi, a third host material layer 43 made of Alq3, a hole barrier layer 45 made of BCP, Electron Transport Layer (ETL) 37 made of Alq, Electron Injection Layer (EIL) 57 made of LiF, and one made of Au, Al, Mg, Pt, Ag, MgAg, AlLi, AlLiO, AIL ΐ F or Ca And other cathodes made of conductive material 39. Among them, the NPB of the first host material layer 41 is mixed with at least one DCM2 substance that can emit red light, and the DPVBi of the second host material layer 42 is mixed with at least one DSA substance that can project blue light. The three main material layers 4 3 A1 q 3 are mixed with at least one c 6 substance capable of projecting green light. By the arrangement of the energy level positions of the host material layers (Hosts), the hole blocking layer 4 5 Electron hole pairs in the range of NpB 41, DPVBi 42, Alq3 43 and the blocking effect of the electron blocking layer 47 can be generally divided into each of the main material layers 41 to 43. When an external bias is applied, the three primary color light sources of red, blue, and green can be projected through each guest luminous substance (Guest) to form a complete three-wavelength projection light source system. White light source or full color product.
為了整合後之光源,如白光,具有更符合理想之C i E 1229569 五、發明說明(8) 色度圖體系規格,C6之濃度可比DSA、DCM2之濃度為言 或Alq3 43之厚度可比DPVBi 42、NPB 41之厚度^對 當然,本發明上述實施例中,各層部分所選用之材 可有多種變化’下列所述專利所揭露之材料物質亦可適用 參考:例如,ETL層或HTL層材料可參考美國專利案第5 29 4, 8 70號’ HTL層材料可參考美國專利案第5,〇61,569號、 第5,256,945號1几層材料可參考美國專利案第4 5391>5〇 7號、第5, 886, 464號,HIL層材料可參考美國專利案第3,9 35, 031號、第4, 356, 429號,陽極可參考美國專利案第& 7 73, 929號,EIL層材料可參考美國專利案第4, 539 5〇7號。 綜上所述,本發明係有關於一種發光裝置,’尤指二種 具有三波長發白光特性之有機電激發光裝 :藉此可得以直接獲得一具有三波長特性之連續 形光源者。故本發明實為一具有新穎性、進步性及可供 業上利用者,應符合我國專利法專利申 ,差' 法提出發明專利申請,祈釣戶ϊ萆口姐各㊣、、 。 τ月研釣局早曰賜准專利,至感為禱 惟以上所述者,僅為太恭ΒΗ + _ L 1皇馬本备明之一較佳實施例而已,並 非用來限疋本發明實雜夕誌图 R斛、十-夕j 之靶圍,舉凡依本發明申請專利範 圍所述之形狀、構造、牲舛 ^ ,始;S々紅执士⑺ 4寸被及精神所為之均等變化與修飾 均應包括於本發明之申請專利範圍内。 第12頁 1229569In order to integrate the light source, such as white light, it is more in line with the ideal C i E 1229569 V. Description of the invention (8) Chromaticity chart system specifications, the concentration of C6 is comparable to that of DSA, DCM2, or the thickness of Alq3 43 is comparable to DPVBi 42 The thickness of NPB 41. Of course, in the above embodiments of the present invention, the materials used for each layer can have various changes. The materials and materials disclosed in the following patents can also be applied for reference: For example, the materials of the ETL layer or HTL layer can be Reference to U.S. Patent No. 5 29 4, 8 70 'HTL layer material can refer to U.S. Patent No. 5, 〇61,569, No. 5,256,945 1 several layers of material can refer to U.S. Patent No. 4 5391 > 507 No. 5, 886, 464. For the material of the HIL layer, please refer to US Patent Nos. 3,9 35, 031 and 4, 356, 429. For the anode, please refer to US Patent No. & 7 73, 929, EIL. For layer material, refer to US Patent No. 4,539,507. In summary, the present invention relates to a light-emitting device, especially two organic electro-excitation light devices having three-wavelength white light emitting characteristics: by this means, a continuous light source having three-wavelength characteristics can be directly obtained. Therefore, the present invention is really a novel, progressive and available for industrial users, should comply with the patent application of China's patent law, the application of the invention patent application method, pray to fishermen and sisters. The τ month research fishing bureau has granted a quasi-patent earlier, but the above is just a prayer. It is only a respectful BΗ + _ L 1 Real Madrid. This is a preferred embodiment, and is not intended to limit the practicality of the present invention. The range of Xi Zhitu R D, Shi-Xi j, for example, the shape, structure, and sacrifice according to the scope of the patent application of the present invention ^, S々 红 士士 ⑺ 4 inch quilt and spiritual behavior equal changes and Modifications should be included in the scope of patent application of the present invention. Page 12 1229569
第13頁 五、發明說明(9) [ 圖號對 昭 說 明 ] • 10 OLED 11 透 光 基 板 13 陽極 15 電 洞 傳 層 17 發光 層 19 陰 極 22 陽極 23 電 洞 傳 層 24 電子 傳 層 25 陰 極 30 OLED 31 基板 33 第一 導 電 層 35 第 _ — 載 子 阻 隔 層 37 第二 載 子 傳 輸 層 39 第 二 導 電 層 41 第一 主 體 材 料 層 42 第 主 體 材 料 層 43 第三 主 體 材 料 層 45 第 —* 載 子 阻 隔 層 47 第二 載 子 阻 隔 層 53 第 一 載 子 注 入 層 57 第二 載 子 注 入 層 1229569 圖式簡單說明 第1圖:係習用發光裝置之構造剖視圖; 第2圖··係另一種習用發光裝置之各元件能階示意圖; 第3圖··係本發明發光裝置之一較佳實施例之構造截面圖 ;及 第4圖:係本發明又一實施例之構造截面圖。Page 13 V. Description of the invention (9) [Illustration of drawing number] • 10 OLED 11 Transparent substrate 13 Anode 15 Hole transfer layer 17 Light emitting layer 19 Cathode 22 Anode 23 Hole transfer layer 24 Electron transfer layer 25 Cathode 30 OLED 31 substrate 33 first conductive layer 35 first carrier barrier layer 37 second carrier transport layer 39 second conductive layer 41 first host material layer 42 first host material layer 43 third host material layer 45 first Sub-blocking layer 47 Second carrier-blocking layer 53 First carrier-injecting layer 57 Second carrier-injecting layer 1229569 Brief description of the diagram Figure 1: A cross-sectional view of the structure of a conventional light-emitting device; Figure 2 ... is another conventional Schematic diagram of the energy levels of each element of the light-emitting device; FIG. 3 is a structural cross-sectional view of a preferred embodiment of the light-emitting device of the present invention; and FIG. 4 is a structural cross-sectional view of yet another embodiment of the present invention.
第14頁Page 14
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