JP2008037899A - Electroluminescent phosphor - Google Patents
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- OAICVXFJPJFONN-UHFFFAOYSA-N Phosphorus Chemical compound [P] OAICVXFJPJFONN-UHFFFAOYSA-N 0.000 title claims abstract description 25
- 239000012190 activator Substances 0.000 claims abstract description 4
- 239000011159 matrix material Substances 0.000 claims abstract description 3
- 238000005401 electroluminescence Methods 0.000 description 38
- 238000000295 emission spectrum Methods 0.000 description 10
- 239000000203 mixture Substances 0.000 description 7
- 238000005259 measurement Methods 0.000 description 5
- 239000006104 solid solution Substances 0.000 description 4
- 239000000126 substance Substances 0.000 description 4
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 2
- 229910005191 Ga 2 O 3 Inorganic materials 0.000 description 2
- 238000002149 energy-dispersive X-ray emission spectroscopy Methods 0.000 description 2
- 239000010408 film Substances 0.000 description 2
- 238000010532 solid phase synthesis reaction Methods 0.000 description 2
- 239000007858 starting material Substances 0.000 description 2
- UCKMPCXJQFINFW-UHFFFAOYSA-N Sulphide Chemical compound [S-2] UCKMPCXJQFINFW-UHFFFAOYSA-N 0.000 description 1
- 230000003213 activating effect Effects 0.000 description 1
- 239000011230 binding agent Substances 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 239000004359 castor oil Substances 0.000 description 1
- 235000019438 castor oil Nutrition 0.000 description 1
- 230000005684 electric field Effects 0.000 description 1
- 238000010304 firing Methods 0.000 description 1
- 238000002189 fluorescence spectrum Methods 0.000 description 1
- ZEMPKEQAKRGZGQ-XOQCFJPHSA-N glycerol triricinoleate Natural products CCCCCC[C@@H](O)CC=CCCCCCCCC(=O)OC[C@@H](COC(=O)CCCCCCCC=CC[C@@H](O)CCCCCC)OC(=O)CCCCCCCC=CC[C@H](O)CCCCCC ZEMPKEQAKRGZGQ-XOQCFJPHSA-N 0.000 description 1
- 150000002484 inorganic compounds Chemical group 0.000 description 1
- 229910010272 inorganic material Inorganic materials 0.000 description 1
- 239000004973 liquid crystal related substance Substances 0.000 description 1
- 239000000463 material Substances 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 150000002894 organic compounds Chemical class 0.000 description 1
- 239000012071 phase Substances 0.000 description 1
- 239000000843 powder Substances 0.000 description 1
- 238000000634 powder X-ray diffraction Methods 0.000 description 1
- 238000003786 synthesis reaction Methods 0.000 description 1
- 239000010409 thin film Substances 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 1
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Abstract
【課題】化学的に安定であって、高輝度で発光する、新規のエレクトロルミネッセンス蛍光体を提供する。
【解決手段】一般式：（ＺｎＯ）1-ｘ（ＧａＮ）ｘ（０＜ｘ＜１）で表される母体に賦活剤としてＭｎを含有させた。ｘの値は、高いＥＬ発光強度を得るために、０．６０≦ｘ≦０．８５であることが好ましい。Ｍｎの濃度は、高いＥＬ発光強度を得るために、１モル％以上であることが好ましい。５２０ｎｍ付近にピークを有する比較的シャープな緑色発光と、６００ｎｍ以上にブロードな赤色から赤外領域にかけての発光がみられた。
【選択図】図１A novel electroluminescent phosphor that is chemically stable and emits light with high luminance is provided.
A matrix represented by the general formula: (ZnO) 1-x (GaN) x (0 <x <1) contains Mn as an activator. The value of x is preferably 0.60 ≦ x ≦ 0.85 in order to obtain a high EL emission intensity. The Mn concentration is preferably 1 mol% or more in order to obtain high EL emission intensity. A relatively sharp green light emission having a peak in the vicinity of 520 nm and a light emission from a broad red to infrared region over 600 nm were observed.
[Selection] Figure 1
Description
本発明は、新規のエレクトロルミネッセンス蛍光体に関する。 The present invention relates to a novel electroluminescent phosphor.
エレクトロルミネッセンス（Electroluminescence；ＥＬ）とは、発光体に電界を印加することによって得られる発光である。このＥＬは、発光するときに熱をほとんど出さず、消費電力が少なく、デバイスにした際に構造がシンプルであって薄型化が可能であり、自発発光かつ高輝度発光であってバックライトが不要である、といった利点があり、ディスプレイ用デバイスとして利用されている。 Electroluminescence (EL) is light emission obtained by applying an electric field to a light emitter. This EL emits little heat when emitting light, consumes little power, has a simple structure and can be thinned when made into a device, and emits light spontaneously and with high brightness, eliminating the need for a backlight And is used as a display device.
ＥＬには、有機発光体を用いた有機ＥＬと、無機発光体を用いた無機ＥＬとが知られている。現在、薄膜ディスプレイとして有機ＥＬが実用化の段階にあり、例えば、携帯電話の背面ディスプレイなどの小画面製品に使用されているが、有機ＥＬは発光体が有機化合物であり、熱に弱く、酸素や水と反応して劣化しやすいという欠点がある。これに対し、無機ＥＬは発光体が無機化合物であり、耐熱性や化学的安定性に優れている。また、無機ＥＬは、有機ＥＬと比較して輝度が低いものの、ディスプレイの大型化が比較的容易であり、次世代のディスプレイとして注目されている。 As the EL, an organic EL using an organic light emitter and an inorganic EL using an inorganic light emitter are known. At present, organic EL is in the stage of practical use as a thin film display, and is used for small screen products such as a back display of a mobile phone. For example, organic EL is an organic compound and is weak against heat. There is a disadvantage that it reacts with water and easily deteriorates. On the other hand, the inorganic EL has a luminous body that is an inorganic compound and is excellent in heat resistance and chemical stability. In addition, although inorganic EL has lower luminance than organic EL, it is relatively easy to increase the size of the display, and is attracting attention as a next-generation display.
無機ＥＬの代表的な発光体としては、ＺｎＳを母体としたものが知られている。そして、ＺｎＳを母体としたものは、高輝度で発光することから、すでに店舗用のレジスターや医療機器のディスプレイのほか、液晶のバックライトなどで実用化されている。
しかしながら、ＺｎＳなどの硫化物系の発光体は、化学的に不安定であるという問題があった。 However, sulfide-based light emitters such as ZnS have a problem that they are chemically unstable.
そこで、本発明は、化学的に安定であって、高輝度で発光する、新規のエレクトロルミネッセンス蛍光体を提供することを目的とする。 Therefore, an object of the present invention is to provide a novel electroluminescent phosphor that is chemically stable and emits light with high luminance.
上記課題を達成するため種々検討した結果、（ＺｎＯ）−（ＧａＮ）系酸窒化物にＭｎを賦活することによって、高輝度で発光するＥＬ蛍光体が得られることを見出し、本発明を完成させた。 As a result of various studies to achieve the above-mentioned problems, it has been found that an EL phosphor that emits light with high brightness can be obtained by activating Mn to a (ZnO)-(GaN) -based oxynitride, thereby completing the present invention. It was.
すなわち、本発明の請求項１記載のエレクトロルミネッセンス蛍光体は、一般式：（ＺｎＯ）1-ｘ（ＧａＮ）ｘ（０＜ｘ＜１）で表される母体に賦活剤としてＭｎを含有することを特徴とする。 That is, the electroluminescent phosphor according to claim 1 of the present invention contains Mn as an activator in the matrix represented by the general formula: (ZnO) 1-x (GaN) x (0 <x <1). It is characterized by.
また、本発明の請求項２記載のエレクトロルミネッセンス蛍光体は、請求項１において、０．６０≦ｘ≦０．８５であることを特徴とする。
The electroluminescent phosphor according to
さらに、本発明の請求項３記載のエレクトロルミネッセンス蛍光体は、請求項１又は２において、Ｍｎの濃度が１モル％以上であることを特徴とする。
Furthermore, the electroluminescent phosphor according to
本発明のエレクトロルミネッセンス蛍光体によれば、化学的に安定であって、高輝度で発光する、新規のエレクトロルミネッセンス蛍光体を提供することができる。 According to the electroluminescent phosphor of the present invention, a novel electroluminescent phosphor that is chemically stable and emits light with high luminance can be provided.
本発明のエレクトロルミネッセンス（ＥＬ）蛍光体は、一般式：（ＺｎＯ）1-ｘ（ＧａＮ）ｘ（０＜ｘ＜１）で表される母体に賦活剤としてＭｎを含有する。 The electroluminescent (EL) phosphor of the present invention contains Mn as an activator in a base represented by the general formula: (ZnO) 1-x (GaN) x (0 <x <1).
ここで、ｘの値は、高いＥＬ発光強度を得るために、０．６０≦ｘ≦０．８５であることが好ましい。また、ＥＬ蛍光体中のＭｎの濃度は、高いＥＬ発光強度を得るために、１モル％以上であることが好ましい。 Here, the value of x is preferably 0.60 ≦ x ≦ 0.85 in order to obtain high EL emission intensity. Further, the Mn concentration in the EL phosphor is preferably 1 mol% or more in order to obtain high EL emission intensity.
本発明のＥＬ蛍光体は、通常の固相法によって得ることができる。すなわち、ＺｎＯ、Ｇａ２Ｏ３、ＭｎＯを混合し、ＮＨ３雰囲気下で焼成することで得ることができる。 The EL phosphor of the present invention can be obtained by an ordinary solid phase method. That is, it can be obtained by mixing ZnO, Ga 2 O 3 , and MnO and firing in an NH 3 atmosphere.
本発明のＥＬ蛍光体は、正弦波交流電圧をかけることによって面発光を示す。そして、５２０ｎｍ付近にピークを有する比較的シャープな緑色発光と、６００ｎｍ以上にブロードな赤色から赤外領域にかけての発光がみられることから、化学的に安定なＥＬ蛍光体として、ディスプレイのデバイスへの応用が期待される。 The EL phosphor of the present invention exhibits surface emission by applying a sinusoidal AC voltage. Since a relatively sharp green light emission having a peak near 520 nm and a light emission from a broad red color to an infrared region at 600 nm or more are observed, as a chemically stable EL phosphor, it is applied to a display device. Application is expected.
以下に本発明のＥＬ蛍光体について実施例に基づき詳細に説明するが、本発明は以下の実施例に限定されるものではなく、本発明の思想を逸脱しない範囲で種々の変形実施が可能である。 Hereinafter, the EL phosphor of the present invention will be described in detail based on examples. However, the present invention is not limited to the following examples, and various modifications can be made without departing from the spirit of the present invention. is there.
［ＥＬ蛍光体の作成］
（ＺｎＯ）−（ＧａＮ）：Ｍｎ固溶体の合成を、通常の固相法により行った。出発原料としてＺｎＯ（高純度化学製、純度＞９９．９９％）、Ｇａ２Ｏ３（高純度化学製、純度＞９９．９９％）、ＭｎＯ（高純度化学製、純度＞９９．９％）を用い、これらの出発原料を所定の化学量論比になるように秤量し、エタノール湿式混合を行った。得られた混合物を３００ｋｇ／ｃｍ２で一軸加圧成形後、ＮＨ３流通下、８５０℃で５時間焼成することで、（ＺｎＯ）−（ＧａＮ）：Ｍｎ固溶体を得た。得られた固溶体についてエネルギー分散型蛍光Ｘ線分析装置（ＥＤＳ）（日本電子データム製、ＪＥＤ−２１４０）を用いて元素組成を分析した。また、粉末Ｘ線回折装置（マックサイエンス製、ＭＸ−Ｌａｂｏ）を用いて粉末Ｘ線回折測定を行い、単一相の固溶体としてＥＬ蛍光体が得られたことを確認した。なお、分光蛍光光度計（日本分光製、ＦＰ−６５００）を用いて蛍光スペクトル測定を行ったが、組成に関係なく蛍光はほとんど見られなかった。
[Create EL phosphor]
The synthesis of (ZnO)-(GaN): Mn solid solution was performed by a normal solid phase method. As starting materials, ZnO (manufactured by high purity chemical, purity> 99.99%), Ga 2 O 3 (manufactured by high purity chemical, purity> 99.99%), MnO (manufactured by high purity chemical, purity> 99.9%) These starting materials were weighed so as to have a predetermined stoichiometric ratio, and ethanol wet mixing was performed. The obtained mixture was uniaxially pressed at 300 kg / cm 2 and then calcined at 850 ° C. for 5 hours under NH 3 flow to obtain a (ZnO) — (GaN): Mn solid solution. The obtained solid solution was analyzed for elemental composition using an energy dispersive X-ray fluorescence spectrometer (EDS) (JED-2140, manufactured by JEOL Datum). Further, powder X-ray diffraction measurement was performed using a powder X-ray diffractometer (manufactured by Mac Science, MX-Labo), and it was confirmed that an EL phosphor was obtained as a single-phase solid solution. In addition, although the fluorescence spectrum measurement was performed using the spectrofluorometer (the JASCO make, FP-6500), the fluorescence was hardly seen irrespective of the composition.
［ＥＬ発光スペクトル測定］
実施例１で得たＥＬ蛍光体を用いて、ＥＬ素子を作成した。有機バインダー（ひまし油）、ＥＬ蛍光体、誘電体（ＢａＴｉＯ３）を２：１：１０の質量比で混合し、ＩＴＯ電極上に膜厚３５μｍで成膜した。そして、２００Ｖ、２ｋＨｚの交流電圧を印加して、多波長同時分光計測装置（浜松ホトニクス製、Ｃ７４７３−３６Ｎ（ＢＴＣＣＤ））を用いてＥＬ発光スペクトル測定を行った。
[EL emission spectrum measurement]
An EL element was prepared using the EL phosphor obtained in Example 1. An organic binder (castor oil), EL phosphor, and dielectric (BaTiO 3 ) were mixed at a mass ratio of 2: 1: 10, and a film was formed on the ITO electrode with a film thickness of 35 μm. Then, an alternating-current voltage of 200 V and 2 kHz was applied, and EL emission spectrum measurement was performed using a multi-wavelength simultaneous spectroscopic measurement device (C7473-36N (BTCCD), manufactured by Hamamatsu Photonics).
図１にＭｎの濃度が１モル％のときの（ＺｎＯ）1-ｘ（ＧａＮ）ｘ：Ｍｎ（ｘ＝０．６７）のＥＬ発光スペクトルを示す。５２０ｎｍ付近にピークを有する比較的シャープな緑色発光と、６００ｎｍ以上にブロードな赤色から赤外領域にかけての発光がみられた。なお、５２０ｎｍ付近の発光はＭｎ２＋による発光、赤色から赤外領域にかけての発光は母体である（ＺｎＯ）1-ｘ（ＧａＮ）ｘによる発光であると推定される。 FIG. 1 shows an EL emission spectrum of (ZnO) 1-x (GaN) x : Mn (x = 0.67) when the concentration of Mn is 1 mol%. A relatively sharp green light emission having a peak in the vicinity of 520 nm and a light emission from a broad red to infrared region over 600 nm were observed. In addition, it is estimated that light emission in the vicinity of 520 nm is light emission by Mn 2+ , and light emission from red to infrared region is light emission by (ZnO) 1-x (GaN) x which is a base material.
また、Ｍｎの濃度が１モル％のときの（ＺｎＯ）1-ｘ（ＧａＮ）ｘ：Ｍｎのｘの値を変化させたときの各組成について、ＥＬ発光スペクトルの５２０ｎｍ付近のピーク強度を図２に示す。図２からわかるように、ｘ＝０．６７の組成のときに最も発光強度が強くなることが確認された。また、ｘが０．６０未満、又は０．８５超では十分な発光強度が得られないことから、ＥＬ蛍光体の組成としては０．６０≦ｘ≦０．８５が好適であることが確認された。 Further, the peak intensity around 520 nm of the EL emission spectrum is shown in FIG. 2 for each composition when the value of x of (ZnO) 1-x (GaN) x : Mn when the concentration of Mn is 1 mol% is changed. Shown in As can be seen from FIG. 2, it was confirmed that the emission intensity was strongest when the composition was x = 0.67. In addition, when x is less than 0.60 or more than 0.85, sufficient light emission intensity cannot be obtained, so that it is confirmed that 0.60 ≦ x ≦ 0.85 is preferable as the composition of the EL phosphor. It was.
また、ｘ＝０．６７の組成のときにＭｎの濃度を変化させてＥＬ発光スペクトルの５２０ｎｍ付近のピーク強度を測定した結果を図３に示す。Ｍｎの濃度が１モル％以上のときに強い発光が見られ、１モル％以上では、ほぼ一定の発光強度となった。したがって、ＥＬ蛍光体中のＭｎの濃度は、１モル％以上が好適であることが確認された。 FIG. 3 shows the result of measuring the peak intensity around 520 nm of the EL emission spectrum by changing the Mn concentration when the composition is x = 0.67. Strong light emission was observed when the Mn concentration was 1 mol% or more, and almost constant light emission intensity was obtained at 1 mol% or more. Therefore, it was confirmed that the Mn concentration in the EL phosphor is preferably 1 mol% or more.
また、ｘ＝０．６７、Ｍｎの濃度が１モル％と４モル％のときに印加電圧を変化させてＥＬ発光スペクトルの５２０ｎｍ付近のピーク強度を測定した結果を図４に示す。印加電圧が２００Ｖ以下ではＭｎの濃度に関わらず同等の発光強度であり、印加電圧の増加に伴い発光強度も増加した。しかし、Ｍｎの濃度が１モル％のときは２００Ｖを超えたあたりから発光強度の増加が見られなくなった。一方、Ｍｎの濃度が４モル％のときは電圧に比例して発光強度が増加した。このことから、Ｍｎの濃度と印加電圧の両方を増加させることにより、高い発光強度が得られることが確認された。 FIG. 4 shows the results of measuring the peak intensity around 520 nm of the EL emission spectrum by changing the applied voltage when x = 0.67 and the Mn concentration is 1 mol% and 4 mol%. When the applied voltage was 200 V or less, the emission intensity was the same regardless of the Mn concentration, and the emission intensity increased as the applied voltage increased. However, when the concentration of Mn was 1 mol%, the increase in emission intensity was not observed from around 200 V. On the other hand, when the Mn concentration was 4 mol%, the emission intensity increased in proportion to the voltage. From this, it was confirmed that high emission intensity can be obtained by increasing both the Mn concentration and the applied voltage.
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2016050211A (en) * | 2014-08-28 | 2016-04-11 | 堺化学工業株式会社 | Method for producing sulfide phosphor |
Citations (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPH0240891A (en) * | 1988-07-29 | 1990-02-09 | Toshiba Corp | Thin film electroluminescent display element |
| JPH10270168A (en) * | 1997-03-27 | 1998-10-09 | Uchitsugu Minami | Phosphor thin film for electroluminescent element |
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Patent Citations (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPH0240891A (en) * | 1988-07-29 | 1990-02-09 | Toshiba Corp | Thin film electroluminescent display element |
| JPH10270168A (en) * | 1997-03-27 | 1998-10-09 | Uchitsugu Minami | Phosphor thin film for electroluminescent element |
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2016050211A (en) * | 2014-08-28 | 2016-04-11 | 堺化学工業株式会社 | Method for producing sulfide phosphor |
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