CN1908116A - 蓝光无机发光材料及使用该材料的发光器件 - Google Patents
蓝光无机发光材料及使用该材料的发光器件 Download PDFInfo
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- OAICVXFJPJFONN-UHFFFAOYSA-N Phosphorus Chemical compound [P] OAICVXFJPJFONN-UHFFFAOYSA-N 0.000 title claims abstract description 156
- 229910052693 Europium Inorganic materials 0.000 claims abstract description 27
- OGPBJKLSAFTDLK-UHFFFAOYSA-N europium atom Chemical compound [Eu] OGPBJKLSAFTDLK-UHFFFAOYSA-N 0.000 claims abstract description 24
- 150000004645 aluminates Chemical class 0.000 claims abstract description 16
- 229910052788 barium Inorganic materials 0.000 claims abstract description 16
- 229910052791 calcium Inorganic materials 0.000 claims abstract description 15
- 239000004065 semiconductor Substances 0.000 claims abstract description 6
- 239000011572 manganese Substances 0.000 claims description 31
- 230000003287 optical effect Effects 0.000 claims description 21
- 229910052748 manganese Inorganic materials 0.000 claims description 13
- MYLBTCQBKAKUTJ-UHFFFAOYSA-N 7-methyl-6,8-bis(methylsulfanyl)pyrrolo[1,2-a]pyrazine Chemical compound C1=CN=CC2=C(SC)C(C)=C(SC)N21 MYLBTCQBKAKUTJ-UHFFFAOYSA-N 0.000 claims description 12
- 229910052712 strontium Inorganic materials 0.000 claims description 12
- 229910052749 magnesium Inorganic materials 0.000 claims description 10
- PWHULOQIROXLJO-UHFFFAOYSA-N Manganese Chemical compound [Mn] PWHULOQIROXLJO-UHFFFAOYSA-N 0.000 claims description 9
- 239000000463 material Substances 0.000 claims description 9
- 150000004767 nitrides Chemical class 0.000 claims description 6
- -1 europium activated silicate Chemical class 0.000 claims description 5
- FNWBQFMGIFLWII-UHFFFAOYSA-N strontium aluminate Chemical class [O-2].[O-2].[O-2].[O-2].[O-2].[Al+3].[Al+3].[Sr+2].[Sr+2] FNWBQFMGIFLWII-UHFFFAOYSA-N 0.000 claims description 4
- 229910052725 zinc Inorganic materials 0.000 claims description 4
- 229910052688 Gadolinium Inorganic materials 0.000 claims description 3
- 229910052765 Lutetium Inorganic materials 0.000 claims description 3
- 229910052782 aluminium Inorganic materials 0.000 claims description 3
- 229910052733 gallium Inorganic materials 0.000 claims description 3
- 229910052738 indium Inorganic materials 0.000 claims description 3
- 229910052746 lanthanum Inorganic materials 0.000 claims description 3
- 229910052706 scandium Inorganic materials 0.000 claims description 3
- 229910052727 yttrium Inorganic materials 0.000 claims description 3
- FIMLVRCVMNGRMP-UHFFFAOYSA-N [Mn].[Eu] Chemical compound [Mn].[Eu] FIMLVRCVMNGRMP-UHFFFAOYSA-N 0.000 abstract 1
- 230000001747 exhibiting effect Effects 0.000 abstract 1
- 230000000052 comparative effect Effects 0.000 description 37
- 229910020068 MgAl Inorganic materials 0.000 description 17
- 102100032047 Alsin Human genes 0.000 description 13
- 101710187109 Alsin Proteins 0.000 description 13
- 241001062009 Indigofera Species 0.000 description 12
- 239000000203 mixture Substances 0.000 description 12
- 229910004298 SiO 2 Inorganic materials 0.000 description 8
- 238000002360 preparation method Methods 0.000 description 7
- JAWMENYCRQKKJY-UHFFFAOYSA-N [3-(2,4,6,7-tetrahydrotriazolo[4,5-c]pyridin-5-ylmethyl)-1-oxa-2,8-diazaspiro[4.5]dec-2-en-8-yl]-[2-[[3-(trifluoromethoxy)phenyl]methylamino]pyrimidin-5-yl]methanone Chemical compound N1N=NC=2CN(CCC=21)CC1=NOC2(C1)CCN(CC2)C(=O)C=1C=NC(=NC=1)NCC1=CC(=CC=C1)OC(F)(F)F JAWMENYCRQKKJY-UHFFFAOYSA-N 0.000 description 5
- 229910052784 alkaline earth metal Inorganic materials 0.000 description 5
- 238000010791 quenching Methods 0.000 description 4
- 230000000171 quenching effect Effects 0.000 description 4
- 230000002349 favourable effect Effects 0.000 description 3
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 2
- 239000012190 activator Substances 0.000 description 2
- AYJRCSIUFZENHW-UHFFFAOYSA-L barium carbonate Chemical compound [Ba+2].[O-]C([O-])=O AYJRCSIUFZENHW-UHFFFAOYSA-L 0.000 description 2
- 239000002585 base Substances 0.000 description 2
- 238000006243 chemical reaction Methods 0.000 description 2
- 238000011156 evaluation Methods 0.000 description 2
- CMIHHWBVHJVIGI-UHFFFAOYSA-N gadolinium(iii) oxide Chemical compound [O-2].[O-2].[O-2].[Gd+3].[Gd+3] CMIHHWBVHJVIGI-UHFFFAOYSA-N 0.000 description 2
- 229910052814 silicon oxide Inorganic materials 0.000 description 2
- 238000005406 washing Methods 0.000 description 2
- QEZGRWSAUJTDEZ-UHFFFAOYSA-N 2-[4-[2-(2,3-dihydro-1H-inden-2-ylamino)pyrimidin-5-yl]-3-(piperidine-1-carbonyl)pyrazol-1-yl]-1-(2,4,6,7-tetrahydrotriazolo[4,5-c]pyridin-5-yl)ethanone Chemical compound C1C(CC2=CC=CC=C12)NC1=NC=C(C=N1)C=1C(=NN(C=1)CC(=O)N1CC2=C(CC1)NN=N2)C(=O)N1CCCCC1 QEZGRWSAUJTDEZ-UHFFFAOYSA-N 0.000 description 1
- QXQVDANUNXECKG-UHFFFAOYSA-N OP(O)(Cl)=O.OP(O)(Cl)=O.OP(O)(Cl)=O.P.P Chemical compound OP(O)(Cl)=O.OP(O)(Cl)=O.OP(O)(Cl)=O.P.P QXQVDANUNXECKG-UHFFFAOYSA-N 0.000 description 1
- 239000005084 Strontium aluminate Substances 0.000 description 1
- 238000010521 absorption reaction Methods 0.000 description 1
- 229910052915 alkaline earth metal silicate Inorganic materials 0.000 description 1
- 150000001342 alkaline earth metals Chemical class 0.000 description 1
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 1
- 238000006073 displacement reaction Methods 0.000 description 1
- 238000001035 drying Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- AEBZCFFCDTZXHP-UHFFFAOYSA-N europium(3+);oxygen(2-) Chemical compound [O-2].[O-2].[O-2].[Eu+3].[Eu+3] AEBZCFFCDTZXHP-UHFFFAOYSA-N 0.000 description 1
- 230000005284 excitation Effects 0.000 description 1
- BDAGIHXWWSANSR-NJFSPNSNSA-N hydroxyformaldehyde Chemical compound O[14CH]=O BDAGIHXWWSANSR-NJFSPNSNSA-N 0.000 description 1
- 230000001939 inductive effect Effects 0.000 description 1
- 229910010272 inorganic material Inorganic materials 0.000 description 1
- 239000011147 inorganic material Substances 0.000 description 1
- 230000003993 interaction Effects 0.000 description 1
- 238000004255 ion exchange chromatography Methods 0.000 description 1
- 150000002500 ions Chemical class 0.000 description 1
- 229910000021 magnesium carbonate Inorganic materials 0.000 description 1
- ZLNQQNXFFQJAID-UHFFFAOYSA-L magnesium carbonate Chemical compound [Mg+2].[O-]C([O-])=O ZLNQQNXFFQJAID-UHFFFAOYSA-L 0.000 description 1
- 239000001095 magnesium carbonate Substances 0.000 description 1
- 229960001708 magnesium carbonate Drugs 0.000 description 1
- 235000014380 magnesium carbonate Nutrition 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- QSHDDOUJBYECFT-UHFFFAOYSA-N mercury Chemical compound [Hg] QSHDDOUJBYECFT-UHFFFAOYSA-N 0.000 description 1
- 229910052753 mercury Inorganic materials 0.000 description 1
- 238000000034 method Methods 0.000 description 1
- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical compound O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 description 1
- SIWVEOZUMHYXCS-UHFFFAOYSA-N oxo(oxoyttriooxy)yttrium Chemical group O=[Y]O[Y]=O SIWVEOZUMHYXCS-UHFFFAOYSA-N 0.000 description 1
- 239000002245 particle Substances 0.000 description 1
- 239000000843 powder Substances 0.000 description 1
- 239000008213 purified water Substances 0.000 description 1
- 229910001404 rare earth metal oxide Inorganic materials 0.000 description 1
- 238000012827 research and development Methods 0.000 description 1
- 238000001228 spectrum Methods 0.000 description 1
- 229910000018 strontium carbonate Inorganic materials 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 1
- 238000005303 weighing Methods 0.000 description 1
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Abstract
提供一种在半导体发光元件发射的长波长紫外光以及短波长蓝(至紫)光,特别是波长范围为380nm-430nm的光的激发下高效率发光的蓝光无机发光材料(15)。还提供一种采用这种蓝光无机发光材料的具有高发光度和稳定色度的发光器件。这种蓝光无机发光材料(15)包括一种二价铕激活的或二价铕和锰激活的铝酸盐无机发光材料,该发光材料可基本上由通式:a[(MI1-c-dSrcEud)(Mg1-eMne)]O·bAl2O3表示,其中,MI表示选自Ca和Ba的至少一种元素,a、b、c、d和e是满足0.1≤a/b≤1.0,0.2≤c≤0.8,0.01≤d≤0.5和0≤e≤0.05。
Description
本非临时申请基于2005年8月2号提交日本专利局的日本专利申请No.2005-223783,因而其全部内容在此引入作为参考。
技术领域
本发明涉及一种在发光元件发射的初级光的激发下高效率发光的蓝光无机发光材料,以及在波长变换单元中使用该材料的发光器件。
背景技术
作为被期望能实现低功耗、小型化,高发光度和宽范围的色彩重现性的下一代发光器件,将半导体发光元件和无机发光材料结合起来用于发光器件已经引起了关注,为此已经进行了大量的研究和开发。通常,作为发光元件发射的初级光,使用的是从长波长紫外光到蓝光,即波长为380nm至480nm的光。已经提出了采用可作此类用途的各种无机发光材料的波长变换单元。
尽管发光元件发射的初级光的峰波长根据制造条件有微小变化,但无机发光材料的峰波长几乎不会偏离某一设定值。因而,采用由发光元件发射的初级光激发而发光的蓝光无机发光材料、绿光无机发光材料和/或红光无机发光材料,比采用初级光的更有利之处在于,作为发光器件,可以稳定地获得设计的色度。然而,并不是所有的无机发光材料在发光元件发射的初级光的激发下都能够有效发光,特别是需要有在长波长紫外光以及短波长蓝(到紫)光的激发下能够高效率发光的蓝光无机材料。
在长波长紫外光以及短波长蓝(至紫)光的激发下发光的蓝光无机发光材料可以包括二价铕激活的BaMgAl10O17:Eu和(Sr,Ba,Ca)10(PO4)6·Cl2:Eu。然而,它们的发光效率很低,因此需要提高其发光效率。此外,尽管针对上述问题已经研究了各种氮氧化物基体,但是还没有得到能够高效发光的蓝光无机发光材料。
日本专利公开号No.49-077893公开了一种二价铕激活的BaMgAl10O17:Eu无机发光材料。这种材料已经用于低压或高压汞蒸气放电灯,然而对它在长波长紫外光或短波长蓝(至紫)光的激发下的发光效率没有描述。日本专利公开号No.03-106988公开了一种铕和锰激活的用Sr和/或Ca取代部分Ba的碱土金属铝酸盐无机发光材料。然而,这种方法意在提供一种无机发光材料,该无机发光材料在灯打开时其发射光的颜色会有一点小的变化。对其在长波长紫外光或短波长蓝(至紫)光的激发下的发光效率没有描述。
日本专利公开号No.2001-172623公开了一种无机发光材料,该无机发光材料由二价铕激活的碱土金属氯代磷酸盐无机发光材料和二价锰激活的碱土金属铝酸盐无机发光材料的混合物形成。但是,这种无机发光材料意在在185nm和254nm的紫外光的激发下得到高的发光输出,而对其在长波长紫外光或短波长蓝(至紫)光的激发下的发光效率没有描述。
日本专利公开号No.2002-003836公开了一种将氧化硅溶解在碱土金属铝酸盐化合物中的蓝光无机发光材料。日本专利公开号No.2002-003837公开了将氧化硅和选自氧化钇和氧化钆的至少一种稀土金属氧化物溶解于一种碱土金属铝酸盐化合物中而获得的蓝光无机发光材料。但是,例如,这些材料意在提高在254nm紫外光的激发下的发光输出,而对其在长波长紫外光或短波长蓝(至紫)光的激发下的发光效率没有描述。
如所指的,在传统技术中,还没有获得在长波长紫外光或短波长蓝(至紫)光的激发下展示出高发光输出和稳定色度的蓝光无机发光材料。
发明内容
本发明的一个目的是提供一种无机发光材料,该无机发光材料在半导体发光元件发射的长波长紫外光以及短波长蓝(至紫)光,特别是在380nm至430nm波长范围内的光的激发下而高效发光,并且提供通过使用该材料而展示出高发光度和稳定色度的发光器件。
本发明涉及一种蓝光无机发光材料,该蓝光无机发光材料包含二价铕激活的或二价铕和锰激活的铝酸盐无机发光材料,所述的铝酸盐无机发光材料基本上由如下通式(1)表示:
a[(MI1-c-dSrcEud)(Mg1-eMne)]O·bAl2O3...(1)
(在通式(1)中,MI表示选自Ca和Ba的至少一种元素;a、b、c、d和e是满足0.1≤a/b≤1.0,0.2≤c≤0.8,0.01≤d≤0.5和0≤e≤0.05的数)。
根据本发明所述的蓝光无机发光材料中,优选上述通式(1)中的MI为Ba。
根据本发明所述的蓝光无机发光材料优选包含二价铕激活的铝酸盐无机发光材料,其上述通式(1)中的e值为0。
此外,本发明涉及一种发光器件,所述发光器件包括:一种发射初级光的发光元件;和一种吸收至少部分初级光并发射波长等于或长于初级光波长的二级光的波长变换单元;其中该波长变换单元由至少一种无机发光材料组成,该无机发光材料包括上述的蓝光无机发光材料。
在本发明的发光器件中,优选波长变换单元由蓝光无机发光材料、绿光无机发光材料和红光无机发光材料组成,并且在波长变换单元的光路中,无机发光材料以自发射较长波长的二级光的无机发光材料起的顺序堆叠在一起。
绿光无机发光材料优选包含如下无机发光材料中至少之一:
一种二价铕和锰激活的铝酸盐无机发光材料,其基本上由如下通式(2)表示:
a(MII,Euf,Mng)O·bAl2O3...(2)
(在通式(2)中,MII表示选自Mg、Ca、Sr、Ba和Zn的至少一种元素;a、b、f和g是满足a>0,b>0,0.1≤a/b≤1.0和0.3≤g/f≤5.0的数);
一种二价铕激活的硅酸盐无机发光材料,其基本上由如下通式(3)表示:
2(MIII1-hEuh)O·SiO2...(3)
(在通式(3)中,MIII表示选自Mg、Ca、Sr和Ba的至少一种元素;h是满足0.005≤h≤0.10的数);和
一种二价铕激活的铝酸锶无机发光材料,其基本上由如下通式(4)表示:
(Sr1-mEum)O·Al2O3...(4)
(在通式(4)中,m是满足0.0001≤m≤0.3的数)。
此外,红光无机发光材料优选包含一种二价铕激活的氮化物无机发光材料,该氮化物无机发光材料基本上由如下通式(5)表示:
(MIII1-kEuk)MIVSiN3...(5)
(在通式(5)中,MIII表示选自Mg、Ca、Sr和Ba的至少一种元素,MIV表示选自Al、Ga、In、Sc、Y、La、Gd和Lu的至少一种元素;k是满足0.001≤k≤0.05的数)。
在本发明的发光器件中,优选发光元件为一种氮化镓(GaN)基半导体,并且该发光元件发出的初级光的峰波长范围为380nm-430nm。
根据本发明,可以得到一种能够有效吸收发光元件的发射光并能够高效率地发射蓝光的蓝光无机发光材料,特别是在长波长紫外光以及短波长蓝(至紫)光的激发下高效发光的蓝光无机发光材料。此外,通过在其波长变换单元中采用相应的蓝光无机发光材料,还可以得到能够有效地吸收发光元件的发射光并且可以发射高发光度和稳定色度的白光的发光器件。
因为根据本发明的蓝光无机发光材料及使用该材料的发光器件确保明显提高的发光效率,所以它们很合适应用于低功耗或小尺寸的发光器件,或应用于要求高发光度和宽范围色彩重现性的发光器件中。
从如下的本发明详细描述并结合附图时,本发明的前述的和别的目的、特征、方面和优点将变得更明显。
附图说明
图1是举例说明作为本发明一个实施方案的发光器件的横截面示意图。
图2显示了作为本发明一个实施方案的蓝光无机发光材料的发射峰分布。
具体实施方式
在本发明中,通过用Sr取代少部分或大部分Ca和/或Ba,可以得到在长波长紫外光以及短波长蓝(至紫)光激发下高效发光的蓝光无机发光材料。
更具体而言,本发明的蓝光无机发光材料是由二价铕激活的或二价铕和锰激活的铝酸盐无机发光材料组成的,该铝酸盐无机发光材料基本上由如下通式(1)表示:
a[(MI1-c-dSrcEud)(Mg1-eMne))]O·bAl2O3 (1)
(在通式(1)中,MI表示选自Ca和Ba的至少一种元素;a、b、c、d和e是满足0.1≤a/b≤1.0,0.2≤c≤0.8,0.01≤d≤0.5和0≤e≤0.05的数)。
特别是在峰波长在380nm-430nm范围内的长波长紫外光以及短波长蓝(至紫)光的激发下,本发明满足上述通式(1)的蓝光无机发光材料能够有效地吸收激发光,并且可以高效率地发射蓝光。
在本发明中,通式(1)中MI优选为Ba。在这种情况下,具有Ba和Sr的配置使二价铕更稳定,从而确保更亮光的发射。
在本发明中,配制Sr使通式(1)中c值落入0.2-0.8的范围内。这样在采用长波长紫外光或短波长蓝(至紫)光照射时,可以得到非常高效率的蓝光发射。如果c值低于0.2,发光效率将会明显降低,这是不实用的。如果c值高于0.8,尽管随着峰波长向长波长方向位移,可见光发光度可能会增加,但转换效率会明显降低,这是不实用的。在本发明中c值的更合适范围为0.4-0.6。
在本发明中,配制Eu使通式(1)中的d值落入0.01-0.5范围内。如果d值低于0.01,构成发光中心的活化剂离子Eu2+的含量将会不足,在这种情况下不能得到想要的发射光。如果d值超过0.5,由于浓度淬灭(例如,认为是由于活化剂的相互作用而导致的),光的发射将会降低。
在本发明中,配制Mn使通式(1)中e值落入0-0.05范围内。如果e值超过0.05,绿光发射成分将变得太强,从而将明显降低由蓝光无机发光材料、红光无机发光材料和绿光无机发光材料组合得到的白光的发光度,这并不是实用的。特别优选将e值设置为0。
本发明也涉及一种发光器件,该器件包含发射初级光的发光元件和吸收至少部分初级光并发射波长等于或长于初级光波长的二级光的波长变换单元,其中该波长变换单元由至少一种无机发光材料组成,该无机发光材料包括本发明的蓝光无机发光材料。特别是,本发明典型地涉及一种包含由蓝光无机发光材料、绿光无机发光材料和红光无机发光材料组成的波长变换单元的发光器件。
在图1中,发光器件10包括发射初级光的发光元件11和吸收至少部分初级光并发射波长长于初级光波长的二级光的波长变换单元12。波长变换单元12由红光无机发光材料13、绿光无机发光材料14和本发明的蓝光无机发光材料15组成,其中三种无机发光材料按照一定厚度比如1∶1∶1堆叠在一起。
本发明发光器件中的发光元件优选使用氮化镓(GaN)基半导体。此外,发光元件发射的初级光峰波长优选落入380nm-430nm范围内。初级光峰波长为380nm或更长对发光元件的发光效率是有利的,这是很实用的。峰波长为430nm或更短对发蓝光和发绿光的铝酸盐无机发光材料的发光效率是有利的,这是很实用的。特别是,初级光落入395nm-415nm之间的峰波长范围适合用于本发明中。
图2显示了本发明组成为(Ba0.5Sr0.4Eu0.1)MgAl10O17、二级光峰波长为456nm左右的蓝光无机发光材料的发射光谱。
从得到更高亮度的发射光这个角度出发,在本发明的发光器件中,优选多个无机发光材料,包括本发明的蓝光无机发光材料,以自发射较长波长二级光的无机发光材料起的顺序堆叠在一起,以形成一条光路。无机发光材料也优选包含蓝光无机发光材料、绿光无机发光材料和红光无机发光材料。
用于本发明发光器件的波长变换单元中的绿光无机发光材料优选由以下无机发光材料中的至少一种构成:
二价铕和锰激活的铝酸盐无机发光材料,其基本上由如下通式(2)表示:
a(MII,Euf,Mng)O·bAl2O3...(2)
(在通式(2)中,MII表示选自Mg、Ca、Sr、Ba和Zn的至少一种元素;a、b、f和g是满足a>0,b>0,0.1≤a/b≤1.0和0.3≤g/f≤5.0的数);
二价铕激活的硅酸盐无机发光材料,其基本上由如下通式(3)表示:
2(MIII1-hEuh)O·SiO2...(3)
(在通式(3)中,MIII表示选自Mg、Ca、Sr和Ba的至少一种元素;h是满足0.005≤h≤0.10的数);和
二价铕激活的铝酸锶无机发光材料,其基本上由如下通式(4)表示:
(Sr1-mEum)O·Al2O3...(4)
(在通式(4)中,m是满足0.0001≤m≤0.3的数)。当上述的绿光无机发光材料和本发明满足通式(1)的蓝光无机发光材料结合使用时,可以得到一种发射特别亮的光的发光器件。
在基本上由通式(2)表示的BAM:Eu,Mn无机发光材料中,通式中a和b的值设定为a>0,b>0和0.1≤a/b≤1.0。当g/f的值为0.3或更大时,Mn2+的量不会变得太小,因此得到足够强的发射绿光。当g/f的值为5.0或更小时,由于足够多的能量被转移给Mn2+,因此也得到足够强的发射绿光。
在基本上由通式(3)表示的碱土金属硅酸盐无机发光材料中,当通式中的h值为0.005或更高时,有足够量的Eu2+,因此可以确保足够强的光发射。当h值为0.10或更小时,能够避免由于浓度淬灭所引起的发射光的减少。
在基本上由通式(4)表示的铝酸锶无机发光材料中,当通式中的m值为0.0001或更大时,有足够量的Eu2+,因此可以确保足够强的光发射。当m值为0.3或更小时,能够避免由于浓度淬灭所引起的发射光的减少。
在本发明的发光器件中,尽管多个无机发光材料可以如上所述地自发射较长波长的二级光的无机发光材料起的顺序堆叠在一起,但在使用基本上由通式(2):a(MII,Euf,Mng)O·bAl2O3(这里MII表示选自Mg、Ca、Sr、Ba和Zn的至少一种元素;a、b、f和g是满足a>0,b>0,0.1≤a/b≤1.0和0.3≤g/f≤5.0的数)表示的二价铕和锰激活的铝酸盐无机发光材料作为绿光无机发光材料的情况下,还可以将本发明的蓝光无机发光材料和相关的绿光无机发光材料混合在一起使用。还是在此情况下,得到的功能和效果类似于单个蓝光无机发光材料和绿光无机发光材料的堆叠。
此外,在本发明发光器件的波长转换单元中使用的红光无机发光材料优选为二价铕激活的氮化物无机发光材料,其基本上由如下通式(5)表示:
(MIII1-kEuk)MIVSiN3...(5)
(在通式(5)中,MIII表示选自Mg、Ca、Sr和Ba的至少一种元素,MIV表示选自Al、Ga、In、Sc、Y、La、Gd和Lu的至少一种元素;k是满足0.001≤k≤0.05的数)。当这样一种红光无机发光材料与本发明满足通式(1)的蓝光无机发光材料结合使用时,可以得到一种发射特别亮的光的发光器件。
在基本上由通式(5)表示的氮化物无机发光材料中,当通式中的k值为0.001或更大时,有足够量的Eu2+,从而可以确保足够强的光发射。当k值为0.05或更小时,能够避免由于浓度淬灭所引起的发射光的减少。
值得指出的是,各个无机发光材料的组成可以采用ICP(感应耦合等离子)光谱法、离子交换色谱法等进行分析和评价。
实施例
在下文中,将通过具体实施例更详细地描述本发明,尽管本发明不限于这些实施例。
(实施例1)
准确称量24.98g BaCO3(碳酸钡)、14.95g SrCO3(碳酸锶)、21.35gMgCO3(碳酸镁)、134.26g Al2O3(氧化铝)和4.46g Eu2O3(氧化铕),采用球磨机充分混合。将该混合物料引入到一个带盖子的氧化铝坩埚中,在1550℃于还原气氛(H:体积5%;N2:体积95%)中烘烤4小时。烘烤后的混合物用球磨机磨成细粒,然后用暖和的纯化水充分洗涤。将洗涤后的无机发光材料颗粒过滤和干燥,从而制备组成为(Ba0.5Sr0.4Eu0.1)MgAl10O17的蓝光无机发光材料。
(实施例2-8)
以与上述实施例1类似的方式制备组成如表1所示的蓝光无机发光材料。
(比较例1-8)
制备组成如表1所示的蓝光无机发光材料。
实施例1-8和比较例1-8中制备的蓝光无机发光材料的组成是用ICP光谱法证实的。
<发光度的评价>
对于如上所述得到的实施例1-8和比较例1-8的蓝光无机发光材料,测量在波长如表1所示的激发光的激发下的发光度。比较例1-8的结果均设定为100%,而实施例1-8的结果表示为与比较例结果相对应的相对值,结果如表1所示。
(实施例9)
采用实施例1制备的蓝光无机发光材料制造具有图1构造的发光器件。图1中的发光元件11采用峰波长为410nm的氮化镓(GaN)基发光二极管。为了形成波长变换单元12,将组成为(Ca0.99Eu0.01)AlSiN3的红光无机发光材料13、组成为(Ba0.85Eu0.15)(Mg0.70Mn0.30)Al10O17的绿光无机发光材料14和实施例1制备的组成为(Ba0.5Sr0.4Eu0.1)MgAl10O17的蓝光无机发光材料15堆叠,使得三个无机发光材料的厚度比为蓝光无机发光材料∶绿光无机发光材料∶红光无机发光材料=1∶1∶1。
(比较例9)
以与实施例9类似的方式制造发光器件,不同之处在于,将组成与实施例9中相同的红光无机发光材料和绿光无机发光材料以及比较例1制备的蓝光无机发光材料,按照蓝光无机发光材料∶绿光无机发光材料∶红光无机发光材料=2.5∶1.6∶1.0的质量比进行混合,并且用于波长变换单元。
(实施例10-16)
以与实施例9类似的方式制造发光器件,不同之处在于,将峰波长如表2和3所示的氮化镓(GaN)基发光二极管用作发光元件11,并且将组成如表2和3所示的无机发光材料用作波长变换单元12中使用的发红光、绿光和蓝光的无机发光材料。
(比较例10-16)
以与比较例9类似的方式制造发光器件,不同之处在于,将峰波长如表2和3所示的氮化镓(GaN)基发光二极管用作发光元件11,并且将组成如表2和3所示的无机发光材料用作将要混合在一起用于波长变换单元的发红光、绿光和蓝光的无机发光材料。
<亮度和色温的评价>
对实施例9-16和比较例9-16中得到的发光器件的亮度和色温进行评价。实施例9-16的每个结果均设定为100%,而比较例9-16的结果表示为与实施例结果相对应的相对值,结果如表2和3所示。
[表1]
激发光(nm) | 蓝光无机发光材料的组成 | 发光度(相对值) | |
实施例1 | 410 | (Ba0.5Sr0.4Eu0.1)MgAl10O17 | 115.3% |
比较例1 | 410 | (Ba0.9Eu0.1)MgAl10O17 | 100.0% |
实施例2 | 400 | (Ba0.25Sr0.60Eu0.15)MgAl10O17 | 121.2% |
比较例2 | 400 | (Ba0.85Eu0.15)MgAl10O17 | 100.0% |
实施例3 | 420 | (Ba0.50Sr0.30Eu0.20)MgAl10O17 | 114.7% |
比较例3 | 420 | (Ba0.80Eu0.20)MgAl10O17 | 100.0% |
实施例4 | 380 | (Ba0.20Sr0.50Ca0.10Eu0.20)MgAl10O17 | 120.0% |
比较例4 | 380 | (Ba0.70Ca0.10Eu0.20)MgAl10O17 | 100.0% |
实施例5 | 430 | (Ba0.05Sr0.80Eu0.15)MgAl10O17 | 123.5% |
比较例5 | 430 | (Ba0.85Eu0.15)MgAl10O17 | 100.0% |
实施例6 | 395 | (Ba0.60Sr0.20Eu0.20)MgAl10O17 | 111.9% |
比较例6 | 395 | (Ba0.80Eu0.20)MgAl10O17 | 100.0% |
实施例7 | 400 | (Ba0.30Sr0.50Eu0.20)(Mg0.99Mn0.01)Al10O17 | 122.8% |
比较例7 | 400 | (Ba0.80Eu0.20)(Mg0.99Mn0.01)Al10O17 | 100.0% |
实施例8 | 410 | (Ba0.30Sr0.60Eu0.10)MgAl10O17 | 121.6% |
比较例8 | 410 | (Ba0.90Eu0.10)MgAl10O17 | 100.0% |
[表2]
初级光(nm) | 蓝光无机发光材料的组成 | 红光无机发光材料和绿光无机发光材料的组成 | 亮度(相对值) | 色温 | |
实施例9 | 410 | 实施例1 | 红:(Ca0.99Eu0.01)AlSiN3绿:(Ba0.85Eu0.15)(Mg0.70Mn0.30)Al10O17 | 100% | 6850K-0.001 |
比较例9 | 410 | 比较例1 | 红:(Ca0.99Eu0.01)AlSiN3绿:(Ba0.85Eu0.15)(Mg0.70Mn0.30)Al10O17 | 62% | 6850K-0.001 |
实施例10 | 400 | 实施例2 | 红:(Ca0.985Eu0.015)AlSiN3绿:2(Ba0.60Sr0.38Eu0.02)O·SiO2 | 100% | 7100k+0.002 |
比较例10 | 400 | 比较例2 | 红:(Ca0.985Eu0.015)AlSiN3绿:2(Ba0.60Sr0.38Eu0.02)O·SiO2 | 59% | 7100k+0.002 |
实施例11 | 420 | 实施例3 | 红:(Ca0.94Sr0.05Eu0.01)AlSiN3绿:(Ba0.90Eu0.10)(Mg0.65Mn0.35)Al10O17 | 100% | 5900K+0.002 |
比较例11 | 420 | 比较例3 | 红:(Ca0.94Sr0.05Eu0.01)AlSiN3绿:(Ba0.90Eu0.10)(Mg0.65Mn0.35)Al10O17 | 65% | 5900K+0.002 |
实施例12 | 380 | 实施例4 | 红:(Ca0.99Eu0.01)(Al0.90Ga0.10)SiN3绿:2(Ba0.65Sr0.33Ca0.01Eu0.01)O·SiO2 | 100% | 9000K-0.001 |
比较例12 | 380 | 比较例4 | 红:(Ca0.99Eu0.01)(Al0.90Ga0.10)SiN3绿:2(Ba0.65Sr0.33Ca0.01Eu0.01)O·SiO2 | 60% | 9000K-0.001 |
[表3]
初级光(nm) | 蓝光无机发光材料的组成 | 红光无机发光材料和绿光无机发光材料的组成 | 亮度(相对值) | 色温 | |
实施例13 | 430 | 实施例5 | 红:(Ca0.97Ba0.01Eu0.02)(Al0.99In0.01)SiN3绿:(Ba0.50Sr0.35Eu0.15)(Mg0.80Mn0.20)Al10O17 | 100% | 6100K+0.002 |
比较例13 | 430 | 比较例5 | 红:(Ca0.97Ba0.01Eu0.02)(Al0.99In0.01)SiN3绿:(Ba0.50Sr0.35Eu0.15)(Mg0.80Mn0.20)Al10O17 | 57% | 6100K+0.002 |
实施例14 | 395 | 实施例6 | 红:(Ca0.94Sr0.05Eu0.01)AlSiN3绿:2(Ba0.55Sr0.44Eu0.01)O·SiO2 | 100% | 4200k-0.002 |
比较例14 | 395 | 比较例6 | 红:(Ca0.94Sr0.05Eu0.01)AlSiN3绿:2(Ba0.55Sr0.44Eu0.01)O·SiO2 | 67% | 4200k-0.002 |
实施例15 | 400 | 实施例7 | 红:(Ca0.99Eu0.01)AlSiN3绿:(Ba0.40Sr0.40Eu0.20)(Mg0.70Mn0.30)Al10O17 | 100% | 5000K+0.001 |
比较例15 | 400 | 比较例7 | 红:(Ca0.99Eu0.01)AlSiN3绿:(Ba0.40Sr0.40Eu0.20)(Mng0.70Mn0.30)Al10O17 | 58% | 5000K+0.001 |
实施例16 | 410 | 实施例8 | 红:(Ca0.985Eu0.015)AlSiN3绿:(Sr0.99Eu0.01)O·Al2O3 | 100% | 6700K+0.001 |
比较例16 | 410 | 比较例8 | 红:(Ca0.985Eu0.015)AlSiN3绿:(Sr0.99Eu0.01)O·Al2O3 | 64% | 6700K+0.001 |
如表1所示,实施例1-8的蓝光无机发光材料的发光度相对于比较例1-8的蓝光无机发光材料有明显改善。此外,如表2和3所示,实施例9-16的发光器件的亮度在类似色温的情况下相对于比较例9-16的发光器件有相当大的改善。可以理解本发明的发光器件具有稳定的色度和高发光度。
尽管已经详细描述和通过插图解释了本发明,但是应该清楚地理解,插图和实施例仅是为了用插图和实施例进行说明,而不应理解为限制性的,本发明的精神和范围仅由后附权利要求书的各项所限制。
Claims (8)
1.一种蓝光无机发光材料,其包含二价铕激活的或二价铕和锰激活的铝酸盐无机发光材料,所述铝酸盐无机发光材料基本上由如下通式(1)表示:
a[(MI1-c-dSrcEud)(Mg1-eMne)]O·bAl2O3… (1)
在通式(1)中,MI表示选自Ca和Ba的至少一种元素,a、b、c、d和e是满足0.1≤a/b≤1.0,0.2≤c≤0.8,0.01≤d≤0.5和0≤e≤0.05的数。
2.根据权利要求1所述的蓝光无机发光材料,其中MI为Ba。
3.根据权利要求1所述的蓝光无机发光材料,其包含e值为0的二价铕激活的铝酸盐无机发光材料。
4.一种发光器件,其包含:
发射初级光的发光元件;和
吸收至少部分所述初级光并发射波长等于或长于所述初级光波长的二级光的波长变换单元;
所述波长变换单元由至少一种无机发光材料组成,并且所述无机发光材料包括权利要求1所述的蓝光无机发光材料。
5.根据权利要求4所述的发光器件,其中所述发光元件为氮化镓(GaN)基半导体,并且从所述发光元件发射的所述初级光的峰波长范围为380nm至430nm。
6.根据权利要求4所述的发光器件,其中所述波长变换单元由蓝光无机发光材料、绿光无机发光材料和红光无机发光材料形成,并且在所述波长变换单元的一条光路里,所述无机发光材料以自发射较长波长二级光的无机发光材料起的顺序堆叠在一起。
7.根据权利要求6所述的发光器件,其中所述绿光无机发光材料包括如下无机发光材料中的至少一种:
一种基本上由如下通式(2)表示的二价铕和锰激活的铝酸盐无机发光材料:
a(MII,Euf,Mng)O·bAl2O3… (2)
在通式(2)中,MII表示选自Mg、Ca、Sr、Ba和Zn的至少一种元素,a、b、f和g是满足a>0,b>0,0.1≤a/b≤1.0和0.3≤g/f≤5.0的数;
一种基本上由如下通式(3)表示的二价铕激活的硅酸盐无机发光材料:2(MIII1-hEuh)O·SiO2…(3)
在通式(3)中,MIII表示选自Mg、Ca、Sr和Ba的至少一种元素,h是满足0.005≤h≤0.10的数;和
一种基本上由如下通式(4)表示的二价铕激活的铝酸锶无机发光材料:(Sr1-mEum)O·Al2O3…(4)
在通式(4)中,m是满足0.0001≤m≤0.3的数。
8.根据权利要求6所述的发光器件,其中所述红光无机发光材料包括一种二价铕激活的氮化物无机发光材料,所述氮化物无机发光材料基本上由如下通式(5)表示:
(MIII1-kEuk)MIVSiN3… (5)
在通式(5)中,MIII表示选自Mg、Ca、Sr和Ba的至少一种元素,MIV表示选自Al、Ga、In、Sc、Y、La、Gd和Lu的至少一种元素,k是满足0.001≤k≤0.05的数。
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