JP4836429B2 - 蛍光体およびこれを用いた発光装置 - Google Patents
蛍光体およびこれを用いた発光装置 Download PDFInfo
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- OAICVXFJPJFONN-UHFFFAOYSA-N Phosphorus Chemical compound [P] OAICVXFJPJFONN-UHFFFAOYSA-N 0.000 title claims description 105
- 238000000295 emission spectrum Methods 0.000 claims description 31
- 239000000463 material Substances 0.000 claims description 14
- 239000010410 layer Substances 0.000 claims description 10
- 239000002344 surface layer Substances 0.000 claims description 9
- 229910052792 caesium Inorganic materials 0.000 claims description 6
- 239000011575 calcium Substances 0.000 claims description 6
- 229910052746 lanthanum Inorganic materials 0.000 claims description 6
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 4
- 239000003822 epoxy resin Substances 0.000 claims description 4
- 229920000647 polyepoxide Polymers 0.000 claims description 4
- BOTDANWDWHJENH-UHFFFAOYSA-N Tetraethyl orthosilicate Chemical compound CCO[Si](OCC)(OCC)OCC BOTDANWDWHJENH-UHFFFAOYSA-N 0.000 claims description 3
- 239000004110 Zinc silicate Substances 0.000 claims description 3
- YKTSYUJCYHOUJP-UHFFFAOYSA-N [O--].[Al+3].[Al+3].[O-][Si]([O-])([O-])[O-] Chemical compound [O--].[Al+3].[Al+3].[O-][Si]([O-])([O-])[O-] YKTSYUJCYHOUJP-UHFFFAOYSA-N 0.000 claims description 3
- 229910052751 metal Inorganic materials 0.000 claims description 3
- 239000002184 metal Substances 0.000 claims description 3
- 229920002050 silicone resin Polymers 0.000 claims description 3
- 235000019352 zinc silicate Nutrition 0.000 claims description 3
- 239000004132 Calcium polyphosphate Substances 0.000 claims description 2
- 235000019827 calcium polyphosphate Nutrition 0.000 claims description 2
- 239000004519 grease Substances 0.000 claims description 2
- 229920001296 polysiloxane Polymers 0.000 claims description 2
- 239000000377 silicon dioxide Substances 0.000 claims description 2
- 229920002545 silicone oil Polymers 0.000 claims description 2
- XSMMCTCMFDWXIX-UHFFFAOYSA-N zinc silicate Chemical compound [Zn+2].[O-][Si]([O-])=O XSMMCTCMFDWXIX-UHFFFAOYSA-N 0.000 claims 1
- 239000000843 powder Substances 0.000 description 47
- 239000013078 crystal Substances 0.000 description 25
- 229910004283 SiO 4 Inorganic materials 0.000 description 20
- 239000002994 raw material Substances 0.000 description 17
- 230000000052 comparative effect Effects 0.000 description 16
- 239000000203 mixture Substances 0.000 description 16
- 239000003795 chemical substances by application Substances 0.000 description 12
- 229920005989 resin Polymers 0.000 description 12
- 239000011347 resin Substances 0.000 description 12
- 238000002441 X-ray diffraction Methods 0.000 description 11
- 229910004298 SiO 2 Inorganic materials 0.000 description 8
- 239000002245 particle Substances 0.000 description 7
- NLXLAEXVIDQMFP-UHFFFAOYSA-N Ammonia chloride Chemical compound [NH4+].[Cl-] NLXLAEXVIDQMFP-UHFFFAOYSA-N 0.000 description 6
- AIYUHDOJVYHVIT-UHFFFAOYSA-M caesium chloride Chemical compound [Cl-].[Cs+] AIYUHDOJVYHVIT-UHFFFAOYSA-M 0.000 description 6
- 150000001875 compounds Chemical class 0.000 description 6
- BPQQTUXANYXVAA-UHFFFAOYSA-N Orthosilicate Chemical compound [O-][Si]([O-])([O-])[O-] BPQQTUXANYXVAA-UHFFFAOYSA-N 0.000 description 5
- 238000004519 manufacturing process Methods 0.000 description 5
- 231100000419 toxicity Toxicity 0.000 description 5
- 230000001988 toxicity Effects 0.000 description 5
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 4
- 229910052688 Gadolinium Inorganic materials 0.000 description 4
- 229910021193 La 2 O 3 Inorganic materials 0.000 description 4
- 229910052788 barium Inorganic materials 0.000 description 4
- 239000004570 mortar (masonry) Substances 0.000 description 4
- 229910052700 potassium Inorganic materials 0.000 description 4
- 229910052712 strontium Inorganic materials 0.000 description 4
- 239000000126 substance Substances 0.000 description 4
- 229910052693 Europium Inorganic materials 0.000 description 3
- 229910052915 alkaline earth metal silicate Inorganic materials 0.000 description 3
- 235000019270 ammonium chloride Nutrition 0.000 description 3
- 230000007423 decrease Effects 0.000 description 3
- 238000010586 diagram Methods 0.000 description 3
- 230000000694 effects Effects 0.000 description 3
- 238000000695 excitation spectrum Methods 0.000 description 3
- 239000007789 gas Substances 0.000 description 3
- 238000000034 method Methods 0.000 description 3
- 239000004065 semiconductor Substances 0.000 description 3
- -1 silicate compound Chemical class 0.000 description 3
- 239000000758 substrate Substances 0.000 description 3
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 2
- 229910052784 alkaline earth metal Inorganic materials 0.000 description 2
- 150000001342 alkaline earth metals Chemical class 0.000 description 2
- 239000006185 dispersion Substances 0.000 description 2
- ZOIVSVWBENBHNT-UHFFFAOYSA-N dizinc;silicate Chemical compound [Zn+2].[Zn+2].[O-][Si]([O-])([O-])[O-] ZOIVSVWBENBHNT-UHFFFAOYSA-N 0.000 description 2
- 239000001257 hydrogen Substances 0.000 description 2
- 229910052739 hydrogen Inorganic materials 0.000 description 2
- 229910052757 nitrogen Inorganic materials 0.000 description 2
- 238000009877 rendering Methods 0.000 description 2
- 229910018072 Al 2 O 3 Inorganic materials 0.000 description 1
- QGZKDVFQNNGYKY-UHFFFAOYSA-O Ammonium Chemical compound [NH4+] QGZKDVFQNNGYKY-UHFFFAOYSA-O 0.000 description 1
- 241000566146 Asio Species 0.000 description 1
- CPELXLSAUQHCOX-UHFFFAOYSA-M Bromide Chemical compound [Br-] CPELXLSAUQHCOX-UHFFFAOYSA-M 0.000 description 1
- VEXZGXHMUGYJMC-UHFFFAOYSA-M Chloride anion Chemical compound [Cl-] VEXZGXHMUGYJMC-UHFFFAOYSA-M 0.000 description 1
- KRHYYFGTRYWZRS-UHFFFAOYSA-M Fluoride anion Chemical compound [F-] KRHYYFGTRYWZRS-UHFFFAOYSA-M 0.000 description 1
- 229910001218 Gallium arsenide Inorganic materials 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
- 230000002411 adverse Effects 0.000 description 1
- 229910052783 alkali metal Inorganic materials 0.000 description 1
- 150000001340 alkali metals Chemical class 0.000 description 1
- 229910045601 alloy Inorganic materials 0.000 description 1
- 239000000956 alloy Substances 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
- 229910014307 bSiO Inorganic materials 0.000 description 1
- 229910052791 calcium Inorganic materials 0.000 description 1
- 239000003086 colorant Substances 0.000 description 1
- 239000000470 constituent Substances 0.000 description 1
- 230000002939 deleterious effect Effects 0.000 description 1
- 238000001035 drying Methods 0.000 description 1
- OGPBJKLSAFTDLK-UHFFFAOYSA-N europium atom Chemical compound [Eu] OGPBJKLSAFTDLK-UHFFFAOYSA-N 0.000 description 1
- 230000005284 excitation Effects 0.000 description 1
- 238000010304 firing Methods 0.000 description 1
- 238000010438 heat treatment Methods 0.000 description 1
- XMBWDFGMSWQBCA-UHFFFAOYSA-N hydrogen iodide Chemical compound I XMBWDFGMSWQBCA-UHFFFAOYSA-N 0.000 description 1
- 238000005286 illumination Methods 0.000 description 1
- WABPQHHGFIMREM-VENIDDJXSA-N lead-201 Chemical compound [201Pb] WABPQHHGFIMREM-VENIDDJXSA-N 0.000 description 1
- WABPQHHGFIMREM-FTXFMUIASA-N lead-202 Chemical compound [202Pb] WABPQHHGFIMREM-FTXFMUIASA-N 0.000 description 1
- 230000031700 light absorption Effects 0.000 description 1
- 238000000465 moulding Methods 0.000 description 1
- 238000005375 photometry Methods 0.000 description 1
- 238000000634 powder X-ray diffraction Methods 0.000 description 1
- 238000010298 pulverizing process Methods 0.000 description 1
- 238000010926 purge Methods 0.000 description 1
- 238000010791 quenching Methods 0.000 description 1
- 230000000171 quenching effect Effects 0.000 description 1
- 230000001105 regulatory effect Effects 0.000 description 1
- 150000004760 silicates Chemical class 0.000 description 1
- 238000005979 thermal decomposition reaction Methods 0.000 description 1
- 231100000167 toxic agent Toxicity 0.000 description 1
- 239000003440 toxic substance Substances 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 1
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- H—ELECTRICITY
- H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
- H05B—ELECTRIC HEATING; ELECTRIC LIGHT SOURCES NOT OTHERWISE PROVIDED FOR; CIRCUIT ARRANGEMENTS FOR ELECTRIC LIGHT SOURCES, IN GENERAL
- H05B33/00—Electroluminescent light sources
- H05B33/12—Light sources with substantially two-dimensional radiating surfaces
- H05B33/14—Light sources with substantially two-dimensional radiating surfaces characterised by the chemical or physical composition or the arrangement of the electroluminescent material, or by the simultaneous addition of the electroluminescent material in or onto the light source
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- C09K—MATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
- C09K11/00—Luminescent, e.g. electroluminescent, chemiluminescent materials
- C09K11/08—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials
- C09K11/77—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials containing rare earth metals
- C09K11/7728—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials containing rare earth metals containing europium
- C09K11/77342—Silicates
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- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09K—MATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
- C09K11/00—Luminescent, e.g. electroluminescent, chemiluminescent materials
- C09K11/08—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials
- C09K11/77—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials containing rare earth metals
- C09K11/7783—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials containing rare earth metals containing two or more rare earth metals one of which being europium
- C09K11/77922—Silicates
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- H01L2224/00—Indexing scheme for arrangements for connecting or disconnecting semiconductor or solid-state bodies and methods related thereto as covered by H01L24/00
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- H01L2224/42—Wire connectors; Manufacturing methods related thereto
- H01L2224/47—Structure, shape, material or disposition of the wire connectors after the connecting process
- H01L2224/48—Structure, shape, material or disposition of the wire connectors after the connecting process of an individual wire connector
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- H01L2224/42—Wire connectors; Manufacturing methods related thereto
- H01L2224/47—Structure, shape, material or disposition of the wire connectors after the connecting process
- H01L2224/48—Structure, shape, material or disposition of the wire connectors after the connecting process of an individual wire connector
- H01L2224/481—Disposition
- H01L2224/48151—Connecting between a semiconductor or solid-state body and an item not being a semiconductor or solid-state body, e.g. chip-to-substrate, chip-to-passive
- H01L2224/48221—Connecting between a semiconductor or solid-state body and an item not being a semiconductor or solid-state body, e.g. chip-to-substrate, chip-to-passive the body and the item being stacked
- H01L2224/48245—Connecting between a semiconductor or solid-state body and an item not being a semiconductor or solid-state body, e.g. chip-to-substrate, chip-to-passive the body and the item being stacked the item being metallic
- H01L2224/48247—Connecting between a semiconductor or solid-state body and an item not being a semiconductor or solid-state body, e.g. chip-to-substrate, chip-to-passive the body and the item being stacked the item being metallic connecting the wire to a bond pad of the item
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- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L33/00—Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
- H01L33/48—Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by the semiconductor body packages
- H01L33/50—Wavelength conversion elements
- H01L33/501—Wavelength conversion elements characterised by the materials, e.g. binder
- H01L33/502—Wavelength conversion materials
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- Y10T428/2991—Coated
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- Y10T428/2993—Silicic or refractory material containing [e.g., tungsten oxide, glass, cement, etc.]
- Y10T428/2995—Silane, siloxane or silicone coating
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- Y10T428/29—Coated or structually defined flake, particle, cell, strand, strand portion, rod, filament, macroscopic fiber or mass thereof
- Y10T428/2982—Particulate matter [e.g., sphere, flake, etc.]
- Y10T428/2991—Coated
- Y10T428/2993—Silicic or refractory material containing [e.g., tungsten oxide, glass, cement, etc.]
- Y10T428/2996—Glass particles or spheres
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
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- Y10T428/29—Coated or structually defined flake, particle, cell, strand, strand portion, rod, filament, macroscopic fiber or mass thereof
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- Chemical & Material Sciences (AREA)
- Inorganic Chemistry (AREA)
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Description
G.Blasse,W.L.Wanmaher,J.W.terVrugt,and A.Bril,Philips Res.Repts,23,189−200,(1968) S.H.M.Poort,W.Janssen,G.Blasse,J.Alloys and Compounds,260,93−97,(1997)
(Sr 1-x-y-z-w Ca x Ba y A z Eu w ) 2 Si v O 2+2v (2)
(上記一般式(2)中、AはLaおよびCsから選択される少なくとも1種の金属であり、x、y、z、w、およびvは、次の関係を満たす数値である。
0≦x≦0.8, 0≦y≦0.03, 0<z≦0.1, 0.001≦w≦0.2
0<(1−x−y−z−w)<1, 0.9≦v≦1.1)
前記蛍光体の少なくとも一部は、前述の蛍光体であることを特徴とする。
本発明の実施形態にかかる蛍光体は、例えば下記一般式(2)で表わされる。
(上記一般式(2)中、AはLa,Gd,CsおよびKから選択される少なくとも1種の金属であり、x、y、z、w、およびvは、次の関係を満たす数値である。
0<(1−x−y−z−w)<1, 0.9≦v≦1.1)
Caの含有量が多すぎる場合には、発光効率が低下するが、xが0.8以下であれば、これを避けることができる。また、人体への影響を考慮すると、Baの含有量は可能な限り少ないことが望まれ、y=0が最も好ましいが、発光波長を調整するためにBaが含有されてもよい。この場合には、yが0.6以下であれば、毒性の影響を低減することができる。
以下、実施例および比較例を示して本発明をさらに詳細に説明するが、本発明は実施例のみに限定されるものではない。
まず、(Sr0.915La0.06Eu0.025)2SiO4で表わされる組成の蛍光体を調製した。原料粉末としては、SrCO3粉末、La2O3粉末、Eu2O3粉末およびSiO2粉末を用意し、所定量秤量した。原料粉末の全量に対して1.5重量%の割合で結晶成長剤としてのNH4Clを添加して、ボールミルで均一に混合した。
まず、(Sr0.915Gd0.060Eu0.025)2SiO4で表わされる組成の蛍光体を調製した。原料粉末としては、SrCO3粉末、Gd2O3粉末、Eu2O3粉末およびSiO2粉末を用意し、所定量秤量した。原料粉末の全量に対して1.5重量%の割合で結晶成長剤としてのNH4Clを添加して、ボールミルで均一に混合した。
まず、(Sr0.920K0.055Eu0.025)2SiO4で表わされる組成の蛍光体を調製した。原料粉末としては、SrCO3粉末、KCl粉末、Eu2O3粉末およびSiO2粉末を用意し、所定量秤量し、ボールミルで均一に混合した。ここでは、K原料であるKClが結晶成長剤としての役割を果たすため、NH4Clは添加しなかった。
まず、(Sr0.915Cs0.03La0.03Eu0.025)2SiO4で表わされる組成の蛍光体を調製した。原料粉末としては、SrCO3粉末、CsCl粉末、La2O3粉末、Eu2O3粉末およびSiO2粉末を用意し、所定量秤量し、ボールミルで均一に混合した。ここでは、Cs原料であるCsClが結晶成長剤としての役割を果たすが、Cl比率調整のため、NH4Clも同時に添加した。
まず、(Sr0.915Ba0.03La0.03Eu0.025)2SiO4で表わされる組成の蛍光体を調製した。原料粉末としては、SrCO3粉末、BaCO3粉末、La2O3粉末、Eu2O3粉末およびSiO2粉末を用意し、所定量秤量し、ボールミルで均一に混合した。原料粉末の全量に対して1.5重量%の割合で結晶成長剤としてのNH4Clを添加して、ボールミルで均一に混合した。
実施例1の蛍光体、青色蛍光体、および赤色蛍光体をエポキシ樹脂に分散させて、この樹脂混合物を調製した。なお、青色蛍光体としては、ユーロピウム付活アルカリ土類クロロリン酸塩蛍光体を用い、赤色蛍光体としては、ユーロピウム付活酸硫化ランタン蛍光体を用いた。この樹脂混合物を、発光ピーク波長395nmなるLEDチップをマウントしたLEDパッケージに塗布して、図1に示したような発光装置を作製した。
実施例1の蛍光体をエポキシ樹脂に分散させて、樹脂混合物を調製した。この樹脂混合物を、発光ピーク波長470nmなるLEDチップをマウントしたLEDパッケージに塗布して、白色LEDを作製した。
まず、(Sr0.285Ba0.665Eu0.05)2SiO4で表わされる組成の蛍光体を調製した。原料粉末としては、SrCO3粉末、BaCO3粉末、Eu2O3粉末およびSiO2粉末を用意し、所定量秤量した。原料粉末の全量に対して1.5重量%の割合で結晶成長剤としてのNH4Clを添加して、ボールミルで均一に混合した。
(Sr0.915Ba0.06Eu0.025)2SiO4で表わされる組成の蛍光体を調製した。原料粉末としては、SrCO3粉末、BaCO3粉末、Eu2O3粉末およびSiO2粉末を用意し、所定量秤量した。原料粉末の全量に対して1.5重量%の割合で結晶成長剤としてのNH4Clを添加して、ボールミルで均一に混合した。その後、実施例1と同様の製造方法にて比較例2の蛍光体を得た。
204…反射面; 205…凹部; 206…発光チップ
207…ボンディングワイヤー; 208…ボンディングワイヤー; 209…蛍光層
210…蛍光体; 211…樹脂層。
Claims (6)
- 下記一般式(2)で表わされることを特徴とする蛍光体。
(Sr 1-x-y-z-w Ca x Ba y A z Eu w ) 2 Si v O 2+2v (2)
(上記一般式(2)中、AはLaおよびCsから選択される少なくとも1種の金属であり、x、y、z、w、およびvは、次の関係を満たす数値である。
0≦x≦0.8, 0≦y≦0.03, 0<z≦0.1, 0.001≦w≦0.2
0<(1−x−y−z−w)<1, 0.9≦v≦1.1) - 波長360nm乃至500nmの光で励起した際の発光スペクトルが、波長520nm乃至600nmの間に単一の発光バンドを有することを特徴とする請求項1に記載の蛍光体。
- 表層材をさらに具備することを特徴とする請求項1または2に記載の蛍光体。
- 前記表層材は、シリコーン樹脂、エポキシ樹脂、フッ素樹脂、テトラエトキシシラン、シリカ、ケイ酸亜鉛、ケイ酸アルミニウム、カルシウムポリフォスフェート、シリコーンオイル、およびシリコーングリースからなる群から選択される少なくとも一種からなることを特徴とする請求項3に記載の蛍光体。
- 360nm乃至500nmの波長の光を発光する発光素子と、
前記発光素子上に配置され、蛍光体を含有する蛍光体層とを具備し、
前記蛍光体の少なくとも一部は、請求項1乃至4のいずれか1項に記載の蛍光体であることを特徴とする発光装置。 - 前記蛍光体層は、青色発光蛍光体および赤色発光蛍光体をさらに含むことを特徴とする請求項5に記載の発光装置。
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