JPH07242869A - Thin-film electroluminescence element - Google Patents
Thin-film electroluminescence elementInfo
- Publication number
- JPH07242869A JPH07242869A JP6058362A JP5836294A JPH07242869A JP H07242869 A JPH07242869 A JP H07242869A JP 6058362 A JP6058362 A JP 6058362A JP 5836294 A JP5836294 A JP 5836294A JP H07242869 A JPH07242869 A JP H07242869A
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- JP
- Japan
- Prior art keywords
- thin film
- thin
- heating
- electroluminescent material
- electroluminescence element
- Prior art date
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- Electroluminescent Light Sources (AREA)
Abstract
Description
【0001】[0001]
【産業上の利用分野】本発明は電界の印加によって発光
する薄膜エレクトロルミネッセンス(EL)素子および
その材料に関するものであり、特にその薄膜発光層に用
いられる薄膜EL材料および該材料を用いた薄膜EL素
子に関する。BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a thin film electroluminescence (EL) element which emits light when an electric field is applied and its material, and particularly to a thin film EL material used for the thin film light emitting layer and a thin film EL using the material. Regarding the device.
【0002】[0002]
【従来の技術】薄膜ELパネルのフルカラー化のために
赤色、緑色、青色を呈するEL発光層の研究が進められ
ている。しかし現在のところ輝度が高く、色純度に優れ
た青色発光材料に良いものがなかった。青色発光体の中
で最も進んだ材料としてはSrS:Ceがあり,近年の
開発により輝度、色純度ともに著しく向上している。し
かしSrS:Ceの発光ピークは、Ceの置換するサイ
トの大きさ等から480nm程度より短波長側にはなら
ないことが予想され、純粋な青色は呈さない。またSr
S自体に潮解性があることや、完全な焼成には1400
℃以上の加熱が必要である等の問題があり、工業的な製
造工程の中での障害となっている。2. Description of the Related Art Studies have been conducted on EL light emitting layers exhibiting red, green, and blue in order to realize full-color thin film EL panels. However, at present, there is no good blue light emitting material having high brightness and excellent color purity. SrS: Ce is the most advanced material among the blue light-emitting materials, and the brightness and color purity have been remarkably improved by recent development. However, the emission peak of SrS: Ce is expected not to be on the shorter wavelength side than about 480 nm due to the size of the site to be replaced by Ce, etc., and a pure blue color is not exhibited. Also Sr
1400 for S itself to be deliquescent and for complete firing
There are problems such as the need for heating above ℃, which is an obstacle in the industrial manufacturing process.
【0003】最近、MGa4S4:Ce(M:アルカリ土
類元素)を用いた薄膜EL素子が開発され、高輝度でよ
り短波長で発光する点から注目を集めている(特開平5
−65478号公報)。また,DavlosらはEu2+
を添加したストロンチウムチオガレートとバリウムチオ
ガレートが主として青色領域で発光することを報告して
いる(J,Solid.State Chem.83,
316(1989))。SrSに比べこれらのチオガレ
ートは一般に潮解性が低く、焼成温度が1100℃程度
で良い等の利点を持ち工業的に優れている。Recently, MGaFourSFour: Ce (M: alkaline earth
A thin film EL device that uses
It is attracting attention because it emits light at a shorter wavelength (Japanese Patent Laid-Open No. Hei 5
-65478). Also, Davlos et al.2+
Strontium thiogallate and barium thiol
Report that gallate emits mainly in the blue region
(J, Solid. State Chem. 83,
316 (1989)). Compared to SrS, these
Generally has a low deliquescent property and a firing temperature of about 1100 ° C.
It has advantages such as good and is industrially excellent.
【0004】しかしながら、色純度、色座標に優れ、良
好な青色を呈する薄膜EL素子は得られていない。However, a thin film EL element which is excellent in color purity and color coordinates and exhibits a favorable blue color has not been obtained.
【0005】[0005]
【発明が解決しようとする課題】本発明の目的は、色純
度、色座標に優れ、化学的に安定な青色発光体が得られ
る薄膜EL材料および該材料を発光層とする薄膜EL素
子を提供することにある。SUMMARY OF THE INVENTION An object of the present invention is to provide a thin film EL material which is excellent in color purity and color coordinates and which can obtain a chemically stable blue light emitting body, and a thin film EL element using the material as a light emitting layer. To do.
【0006】[0006]
【課題を解決するための手段】本発明の上記目的は、次
に示す薄膜EL材料によって達成される。The above object of the present invention is achieved by the following thin film EL material.
【0007】すなわち、本発明は、組成式が次式;That is, in the present invention, the composition formula is as follows:
【化1】 [但し、MはSrまたはBa、REはランタノイド系元
素をそれぞれ示し、xとyは整数であるが、xとyは等
しくない]で表されるアルカリ土類チオガレートからな
ることを特徴とする薄膜EL材料にある。[Chemical 1] [Wherein M represents Sr or Ba, RE represents a lanthanoid element, x and y are integers, but x and y are not equal to each other], and a thin film comprising an alkaline earth thiogallate. It is in EL material.
【0008】上記したように、上式中、Mはストロンチ
ウム(Sr)またはバリウム(Ba)を示す。また、R
Eはランタン(La)、セリウム(Ce)、プラセオジ
ム(Pr)、ネオジム(Nd)、ユウロビウム(Eu)
等のランタノイド系元素を示すが、その中でもセリウム
が好ましく用いられる。このセリウムは経済的に安価で
あり、この点からも優れている。また、xとyは何れも
整数であるが、xとyは等しくない。As described above, in the above formula, M represents strontium (Sr) or barium (Ba). Also, R
E is lanthanum (La), cerium (Ce), praseodymium (Pr), neodymium (Nd), eurobium (Eu)
Among these, lanthanoid-based elements are shown, among which cerium is preferably used. This cerium is economically inexpensive and is excellent in this respect as well. Further, both x and y are integers, but x and y are not equal.
【0009】本発明では、このように上記したアルカリ
チオガーレートを母体材料とし、セリウム等のランタノ
イド系元素を付活剤(発光中心)とするものである。こ
のような具体的な薄膜EL材料の組成としては、BaG
a4S7:Ce、Ba3Ca2S6:Ce、Sr2Ga2S5:
Ce等が挙げられる。また、本発明の薄膜EL材料に
は、さらに電荷補償剤としてカリウム等を含有すること
は好ましいことである。In the present invention, the above-mentioned alkali thiogallate is used as the base material, and the lanthanoid element such as cerium is used as the activator (emission center). As a specific composition of such a thin film EL material, BaG
a 4 S 7: Ce, Ba 3 Ca 2 S 6: Ce, Sr 2 Ga 2 S 5:
Ce etc. are mentioned. Further, it is preferable that the thin film EL material of the present invention further contains potassium or the like as a charge compensating agent.
【0010】このような薄膜EL材料を得るには、例え
ば以下の方法で行なわれる。すなわち、SrCO3また
はBaCO3とGa2O3を適当なモル比で混合し、付活
剤としてCeF3、電荷補償剤としてKClを加えた混
合物を、900〜1100℃の温度でH2S中において
焼成することにより得られる。勿論、これらの材料に代
えてSrS、BaS、Ga2S3、CeO2等を使用する
ことも可能であり、電荷補償剤としてはKClのみなら
ず、適当なイオン半径をもつ1価の陽イオンを提供可能
な化合物ならいずれでもよい。あるいは適当なイオン半
径をもつ3価の陰イオンを用いることも可能である。To obtain such a thin film EL material, for example, the following method is used. That is, SrCO 3 or BaCO 3 and Ga 2 O 3 were mixed at an appropriate molar ratio and CeF 3 as an activator and KCl as a charge compensator were added to a mixture in H 2 S at a temperature of 900 to 1100 ° C. It is obtained by firing at. Of course, it is possible to use SrS, BaS, Ga 2 S 3 , CeO 2 or the like instead of these materials, and not only KCl but also a monovalent cation having an appropriate ionic radius as the charge compensator. Any compound capable of providing Alternatively, a trivalent anion having an appropriate ionic radius can be used.
【0011】本発明の薄膜EL素子は、上記した薄膜E
L材料を発光層として用いるものである。このような薄
膜EL素子の構成を示す一例を図1に示す。同図におい
て、1はAl等の上部電極(背面電極)、2は上部絶縁
層、3はバッフア層、4は発光層、5は下部絶縁層、6
はITO等の下部電極(透明電極)、7はガラス基板で
ある。上部絶縁層2はSiO2層21、Si3N4層22
からなり、下部絶縁層5はSi3N4層51、Si O2層
52からなる。The thin film EL device of the present invention is a thin film E described above.
The L material is used for the light emitting layer. Such thin
An example showing the structure of the film EL element is shown in FIG. In the figure
, 1 is the upper electrode (back electrode) such as Al, 2 is the upper insulation
Layer, 3 is a buffer layer, 4 is a light emitting layer, 5 is a lower insulating layer, 6
Is a lower electrode (transparent electrode) such as ITO, and 7 is a glass substrate
is there. The upper insulating layer 2 is SiO2Layer 21, Si3NFourLayer 22
And the lower insulating layer 5 is made of Si.3NFourLayer 51, Si O2layer
It consists of 52.
【0012】これら各層の厚みは、例えばSiO2層2
1:0.005μm、Si3N4層22:0.12μm、
バッファ層3:0.1μm、発光層4:0.6μm、S
i3N4層51:0.2μm、SiO2層52:0.05
μmである。The thickness of each of these layers is, for example, the SiO 2 layer 2
1: 0.005 μm, Si 3 N 4 layer 22: 0.12 μm,
Buffer layer 3: 0.1 μm, light emitting layer 4: 0.6 μm, S
i 3 N 4 layer 51: 0.2 μm, SiO 2 layer 52: 0.05
μm.
【0013】[0013]
【実施例】以下、実施例に基づいて本発明を具体的に説
明する。EXAMPLES The present invention will be specifically described below based on examples.
【0014】実施例1 BaCO3とGa2O3をモル比で1:2の割合で混合し
たものを出発原料とし、H2S中、900℃で5時間加
熱した。これをふるいにかけて粒度を揃えた後、H2S
中、1000℃で5時間加熱した。再びふるいにかけて
粒度を揃えた後、CeF3とKClを10mol%ずつ
添加し、さらにH2S中、1100℃で5時間加熱し
た。得られた化合物(BaGa4S7:Ce,K)の37
4nmで励起したフォトルミネッセンスを図2に示す。
この図2から460nm付近にピークがあることが判
る。 Example 1 A mixture of BaCO 3 and Ga 2 O 3 in a molar ratio of 1: 2 was used as a starting material, and heated in H 2 S at 900 ° C. for 5 hours. After sifting this to make the particle size uniform, H 2 S
In the middle, it heated at 1000 degreeC for 5 hours. After sieving again to make the particle size uniform, 10 mol% each of CeF 3 and KCl were added, and the mixture was further heated in H 2 S at 1100 ° C. for 5 hours. 37% of the obtained compound (BaGa 4 S 7 : Ce, K)
The photoluminescence excited at 4 nm is shown in FIG.
From this FIG. 2, it can be seen that there is a peak near 460 nm.
【0015】また、この原料を用いて表1に示す条件
下、薄膜からなる発光層および絶縁層を形成し、さらに
図1に示されるような薄膜EL素子を作製した。この薄
膜EL素子は青色のエレクトロルミネッセンスを呈し
た。この薄膜EL素子のエレクトロルミネッセンスを図
3に示す。この時の色座標はX=0.153、Y=0.
136であり、輝度は1KHz駆動時に0.7cd/m
2であった。Further, using this raw material, a light emitting layer and an insulating layer made of a thin film were formed under the conditions shown in Table 1, and a thin film EL element as shown in FIG. 1 was prepared. This thin film EL device exhibited blue electroluminescence. The electroluminescence of this thin film EL element is shown in FIG. At this time, the color coordinates are X = 0.153, Y = 0.
136, and the brightness is 0.7 cd / m when driven at 1 KHz.
Was 2 .
【0016】[0016]
【表1】 [Table 1]
【0017】実施例2 BaCO3とGa2O3をモル比で3:1の割合で混合し
たものを出発原料とし、H2S、900℃で5時間加熱
した。これをふるいにかけて粒度を揃えた後、H2S
中、1000℃で5時間加熱した。再びふるいにかけて
粒度を揃えた後、CeF3とKClをそれぞれ1mol
%、0.1mol%添加し、さらにH2S中、1100
℃で5時間加熱した。得られた化合物(Ba3Ga
2S6:Ce,K)のフォトルミネッセンスを図4に示
す。この図4から470nm付近にピークがあることが
判る。 Example 2 A mixture of BaCO 3 and Ga 2 O 3 in a molar ratio of 3: 1 was used as a starting material, and heated at H 2 S at 900 ° C. for 5 hours. After sifting this to make the particle size uniform, H 2 S
In the middle, it heated at 1000 degreeC for 5 hours. After sieving again to make the particle size uniform, 1 mol each of CeF 3 and KCl
%, 0.1 mol% was added, and further in H 2 S, 1100
Heated at ° C for 5 hours. Obtained compound (Ba 3 Ga
The photoluminescence of 2 S 6 : Ce, K) is shown in FIG. It can be seen from FIG. 4 that there is a peak near 470 nm.
【0018】実施例3 SrCO3とGa2O3をモル比で2:1の割合で混合し
たものを出発原料とし、H2S中、880℃で5時間加
熱した。これをふるいにかけて粒度を揃えた後、H2S
中、880℃で5時間加熱した。再びふるいにかけて粒
度を揃えた後、CeF3とKClを10mol%ずつ添
加し、さらにH2S中、880℃で5時間加熱した。得
られた化合物(Sr2Ga2S5:Ce,K)のフォトル
ミネッセンスを図5に示す。この図5から460nm付
近にピークがあることが判る。 Example 3 A mixture of SrCO 3 and Ga 2 O 3 in a molar ratio of 2: 1 was used as a starting material, and heated in H 2 S at 880 ° C. for 5 hours. After sifting this to make the particle size uniform, H 2 S
Heated at 880 ° C. for 5 hours. After sieving again to make the particle size uniform, CeF 3 and KCl were added in an amount of 10 mol% each, and the mixture was further heated in H 2 S at 880 ° C. for 5 hours. The photoluminescence of the obtained compound (Sr 2 Ga 2 S 5 : Ce, K) is shown in FIG. It can be seen from FIG. 5 that there is a peak near 460 nm.
【0019】また、この原料を用いて表1に示す条件
下、薄膜からなる発光層および絶縁層を形成し、さらに
図1に示されるような薄膜EL素子を作製した。この薄
膜EL素子は青色のエレクトロルミネッセンスを呈し
た。この薄膜EL素子のエレクトロルミネッセンスを図
6に示す。この時の色座標はX=0.22、Y=0.3
46であり、輝度は1KHz駆動時に2.4cd/m2
であった。Further, using this raw material, a light emitting layer and an insulating layer made of a thin film were formed under the conditions shown in Table 1, and a thin film EL element as shown in FIG. 1 was prepared. This thin film EL device exhibited blue electroluminescence. The electroluminescence of this thin film EL element is shown in FIG. The color coordinates at this time are X = 0.22, Y = 0.3
And the luminance is 2.4 cd / m 2 when driven at 1 KHz.
Met.
【0020】この実施例1で得られたBaGa4S7:C
e,K薄膜EL素子の色座標X=0.153、Y=0.
136、実施例3で得られたSr2Ga2S5:Ce,K
薄膜EL素子の色座標X=0.22、Y=0.346、
並びに参考としてSrS:Ce薄膜EL素子の色座標X
=0.18、Y=0.38を図7に示す。BaGa 4 S 7 : C obtained in this Example 1
e, K color coordinates of the thin film EL element X = 0.153, Y = 0.
136, Sr 2 Ga 2 S 5 : Ce, K obtained in Example 3
Color coordinates X = 0.22, Y = 0.346 of thin film EL device,
Also, as a reference, the color coordinate X of the SrS: Ce thin film EL element
= 0.18 and Y = 0.38 are shown in FIG.
【0021】[0021]
【発明の効果】以上のような本発明により、色純度、色
座標のよい薄膜EL材料および該材料を発光層とする薄
膜EL素子が得られた。As described above, according to the present invention, a thin film EL material having good color purity and color coordinates and a thin film EL element using the material as a light emitting layer were obtained.
【図1】 薄膜EL素子の構造を示す概略図。FIG. 1 is a schematic diagram showing the structure of a thin film EL element.
【図2】 BaGa4S7:Ce,K材料のフォトルミネ
ッセンスを示すグラフ。FIG. 2 is a graph showing photoluminescence of a BaGa 4 S 7 : Ce, K material.
【図3】 BaGa4S7:Ce,K薄膜EL素子のエレ
クトロルミネッセンスを示すグラフ。FIG. 3 is a graph showing electroluminescence of a BaGa 4 S 7 : Ce, K thin film EL device.
【図4】 Ba3Ga2S6:Ce,K材料のフォトルミ
ネッセンスを示すグラフ。FIG. 4 is a graph showing photoluminescence of a Ba 3 Ga 2 S 6 : Ce, K material.
【図5】 Sr2Ga2S5:Ce,K材料のフォトルミ
ネッセンスを示すグラフ。FIG. 5 is a graph showing the photoluminescence of a Sr 2 Ga 2 S 5 : Ce, K material.
【図6】 Sr2Ga2S5:Ce,K薄膜EL素子のエ
レクトロルミネッセンスを示すグラフ。FIG. 6 is a graph showing the electroluminescence of a Sr 2 Ga 2 S 5 : Ce, K thin film EL device.
【図7】 Sr2Ga2S5:Ce,K薄膜EL素子、B
aGa4S7:Ce,K薄膜EL素子、SrS:Ce薄膜
EL素子の色座標を示すケリー図。FIG. 7 Sr 2 Ga 2 S 5 : Ce, K thin film EL device, B
FIG. 6 is a Kelly diagram showing color coordinates of an aGa 4 S 7 : Ce, K thin film EL element and an SrS: Ce thin film EL element.
1:上部電極(背面電極)、2(21,22):上部絶
縁層、3:バッフア層、4:発光層、5(51,5
2):下部絶縁層、6:ITO等の下部電極(透明電
極)、7:ガラス基板。1: upper electrode (back electrode), 2 (21, 22): upper insulating layer, 3: buffer layer, 4: light emitting layer, 5 (51, 5)
2): lower insulating layer, 6: lower electrode (transparent electrode) such as ITO, 7: glass substrate.
───────────────────────────────────────────────────── フロントページの続き (72)発明者 三上 明義 大阪府大阪市阿倍野区長池町22番22号シャ ープ株式会社内 (72)発明者 寺田 幸祐 大阪府大阪市阿倍野区長池町22番22号シャ ープ株式会社内 ─────────────────────────────────────────────────── ─── Continuation of the front page (72) Inventor Akiyoshi Mikami 22-22 Nagaike-cho, Abeno-ku, Osaka-shi, Osaka Within Sharp Corporation (72) Inventor Kosuke Terada 22-22 Nagaike-cho, Abeno-ku, Osaka-shi, Osaka Sharp Corporation
Claims (5)
素をそれぞれ示し、xとyは整数であるが、xとyは等
しくない]で表されるアルカリ土類チオガレートからな
ることを特徴とする薄膜エレクトロルミネッセンス材
料。1. The composition formula is as follows; [Wherein M represents Sr or Ba, RE represents a lanthanoid element, x and y are integers, but x and y are not equal to each other], and a thin film comprising an alkaline earth thiogallate. Electroluminescent material.
請求項1に記載の薄膜エレクトロルミネッセンス材料。2. The thin film electroluminescent material according to claim 1, wherein the composition formula is BaGa 4 S 7 : Ce.
る請求項1に記載の薄膜エレクトロルミネッセンス材
料。3. The thin film electroluminescent material according to claim 1, wherein the composition formula is Ba 3 Ga 2 S 6 : Ce.
る請求項1に記載の薄膜エレクトロルミネッセンス材
料。4. The thin film electroluminescent material according to claim 1, wherein the composition formula is Sr 2 Ga 2 S 5 : Ce.
ミネッセンス材料を発光層に用いた薄膜エレクトロルミ
ネッセンス素子。5. A thin film electroluminescent device using the thin film electroluminescent material according to claim 1 for a light emitting layer.
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WO2022209033A1 (en) * | 2021-03-30 | 2022-10-06 | 三井金属鉱業株式会社 | Phosphor, method for producing same, light emitting element containing phosphor, and light emitting device |
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1994
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Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
WO1996015648A1 (en) * | 1994-11-14 | 1996-05-23 | Mitsui Mining & Smelting Co., Ltd. | Thin-film electroluminescent element |
US9196800B2 (en) | 1996-06-26 | 2015-11-24 | Osram Gmbh | Light-radiating semiconductor component with a luminescence conversion element |
FR2755122A1 (en) * | 1996-10-31 | 1998-04-30 | Rhodia Chimie Sa | COMPOUND BASED ON AN ALKALINE EARTH, SULFUR AND ALUMINUM, GALLIUM OR INDIUM, METHOD FOR PREPARING SAME AND USE THEREOF AS LUMINOPHORE |
WO1998018721A1 (en) * | 1996-10-31 | 1998-05-07 | Rhodia Chimie | Compound with base of an alkaline-earth, sulphur and aluminium, gallium or indium, method of preparing same and use as luminophore |
US6180073B1 (en) * | 1996-10-31 | 2001-01-30 | Rhodia Chimie | Compound with base of an alkaline-earth, sulphur and aluminium, gallium or indium, method of preparing same and use as luminophore |
KR100355729B1 (en) * | 1996-10-31 | 2002-10-19 | 로디아 쉬미 | Compound with Base of an Alkaline-Earth, Sulphur and Aluminium, Gallium or Indium, Method of Preparing Same and Use as Luminophore |
KR100430565B1 (en) * | 2001-05-31 | 2004-05-10 | 한국전자통신연구원 | Phosphor including aluminium sulfide and the preparation thereof |
WO2003081957A1 (en) * | 2002-03-27 | 2003-10-02 | Ifire Technology Inc. | Yttrium substituted barium thioaluminate phosphor materials |
JP2017088719A (en) * | 2015-11-09 | 2017-05-25 | 堺化学工業株式会社 | Red phosphor |
WO2022209033A1 (en) * | 2021-03-30 | 2022-10-06 | 三井金属鉱業株式会社 | Phosphor, method for producing same, light emitting element containing phosphor, and light emitting device |
JPWO2022209033A1 (en) * | 2021-03-30 | 2022-10-06 |
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