TWI615995B - 發光裝置 - Google Patents
發光裝置 Download PDFInfo
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- TWI615995B TWI615995B TW103122432A TW103122432A TWI615995B TW I615995 B TWI615995 B TW I615995B TW 103122432 A TW103122432 A TW 103122432A TW 103122432 A TW103122432 A TW 103122432A TW I615995 B TWI615995 B TW I615995B
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- OAICVXFJPJFONN-UHFFFAOYSA-N Phosphorus Chemical compound [P] OAICVXFJPJFONN-UHFFFAOYSA-N 0.000 claims description 92
- 239000011572 manganese Substances 0.000 claims description 55
- 229910052751 metal Inorganic materials 0.000 claims description 26
- 239000002184 metal Substances 0.000 claims description 26
- 229910052748 manganese Inorganic materials 0.000 claims description 24
- PWHULOQIROXLJO-UHFFFAOYSA-N Manganese Chemical compound [Mn] PWHULOQIROXLJO-UHFFFAOYSA-N 0.000 claims description 22
- 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 21
- 229910004298 SiO 2 Inorganic materials 0.000 claims description 19
- 238000006243 chemical reaction Methods 0.000 claims description 19
- 150000003839 salts Chemical class 0.000 claims description 18
- 229910052693 Europium Inorganic materials 0.000 claims description 17
- 239000000203 mixture Substances 0.000 claims description 13
- OGPBJKLSAFTDLK-UHFFFAOYSA-N europium atom Chemical compound [Eu] OGPBJKLSAFTDLK-UHFFFAOYSA-N 0.000 claims description 11
- 229910052718 tin Inorganic materials 0.000 claims description 10
- 229910003564 SiAlON Inorganic materials 0.000 claims description 8
- 229910052791 calcium Inorganic materials 0.000 claims description 8
- 229910052732 germanium Inorganic materials 0.000 claims description 8
- 229910052710 silicon Inorganic materials 0.000 claims description 8
- 229910052712 strontium Inorganic materials 0.000 claims description 8
- 229910052719 titanium Inorganic materials 0.000 claims description 8
- 229910052726 zirconium Inorganic materials 0.000 claims description 8
- 229910052784 alkaline earth metal Inorganic materials 0.000 claims description 7
- 150000001342 alkaline earth metals Chemical class 0.000 claims description 7
- -1 europium activated citrate Chemical class 0.000 claims description 7
- 229910052749 magnesium Inorganic materials 0.000 claims description 7
- 239000004065 semiconductor Substances 0.000 claims description 6
- 229910052725 zinc Inorganic materials 0.000 claims description 6
- JMASRVWKEDWRBT-UHFFFAOYSA-N Gallium nitride Chemical group [Ga]#N JMASRVWKEDWRBT-UHFFFAOYSA-N 0.000 claims description 5
- 229910052788 barium Inorganic materials 0.000 claims description 5
- 229910052783 alkali metal Inorganic materials 0.000 claims description 4
- 150000001340 alkali metals Chemical class 0.000 claims description 4
- 229910052792 caesium Inorganic materials 0.000 claims description 4
- 229910052700 potassium Inorganic materials 0.000 claims description 4
- 229910052701 rubidium Inorganic materials 0.000 claims description 4
- 229910052708 sodium Inorganic materials 0.000 claims description 4
- 229910002601 GaN Inorganic materials 0.000 claims description 3
- 229910052744 lithium Inorganic materials 0.000 claims description 3
- 239000000126 substance Substances 0.000 claims 2
- 230000000052 comparative effect Effects 0.000 description 9
- 238000001748 luminescence spectrum Methods 0.000 description 6
- 239000000843 powder Substances 0.000 description 6
- 238000010586 diagram Methods 0.000 description 5
- 239000000565 sealant Substances 0.000 description 5
- 229920005989 resin Polymers 0.000 description 4
- 239000011347 resin Substances 0.000 description 4
- 229910052727 yttrium Inorganic materials 0.000 description 4
- KJTLSVCANCCWHF-UHFFFAOYSA-N Ruthenium Chemical group [Ru] KJTLSVCANCCWHF-UHFFFAOYSA-N 0.000 description 3
- 229910004283 SiO 4 Inorganic materials 0.000 description 3
- 230000005284 excitation Effects 0.000 description 3
- 238000004020 luminiscence type Methods 0.000 description 3
- 238000010791 quenching Methods 0.000 description 3
- 230000000171 quenching effect Effects 0.000 description 3
- 229910052707 ruthenium Inorganic materials 0.000 description 3
- VWQVUPCCIRVNHF-UHFFFAOYSA-N yttrium atom Chemical compound [Y] VWQVUPCCIRVNHF-UHFFFAOYSA-N 0.000 description 3
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- PXGOKWXKJXAPGV-UHFFFAOYSA-N Fluorine Chemical compound FF PXGOKWXKJXAPGV-UHFFFAOYSA-N 0.000 description 2
- 229910017857 MgGa Inorganic materials 0.000 description 2
- ATJFFYVFTNAWJD-UHFFFAOYSA-N Tin Chemical compound [Sn] ATJFFYVFTNAWJD-UHFFFAOYSA-N 0.000 description 2
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 2
- 238000000295 emission spectrum Methods 0.000 description 2
- 229910052731 fluorine Inorganic materials 0.000 description 2
- 239000011737 fluorine Substances 0.000 description 2
- 239000004973 liquid crystal related substance Substances 0.000 description 2
- 239000011159 matrix material Substances 0.000 description 2
- 238000000034 method Methods 0.000 description 2
- 239000001301 oxygen Substances 0.000 description 2
- 229910052760 oxygen Inorganic materials 0.000 description 2
- 230000003595 spectral effect Effects 0.000 description 2
- 238000001228 spectrum Methods 0.000 description 2
- WFKWXMTUELFFGS-UHFFFAOYSA-N tungsten Chemical compound [W] WFKWXMTUELFFGS-UHFFFAOYSA-N 0.000 description 2
- 229910052721 tungsten Inorganic materials 0.000 description 2
- 239000010937 tungsten Substances 0.000 description 2
- XBSLKMQADAAKGP-UHFFFAOYSA-N 2-hydroxypropane-1,2,3-tricarboxylic acid;phosphane Chemical class P.OC(=O)CC(O)(C(O)=O)CC(O)=O XBSLKMQADAAKGP-UHFFFAOYSA-N 0.000 description 1
- 229910018072 Al 2 O 3 Inorganic materials 0.000 description 1
- 229910052688 Gadolinium Inorganic materials 0.000 description 1
- GYHNNYVSQQEPJS-UHFFFAOYSA-N Gallium Chemical compound [Ga] GYHNNYVSQQEPJS-UHFFFAOYSA-N 0.000 description 1
- 229910010413 TiO 2 Inorganic materials 0.000 description 1
- 229920001807 Urea-formaldehyde Polymers 0.000 description 1
- GEIAQOFPUVMAGM-UHFFFAOYSA-N ZrO Inorganic materials [Zr]=O GEIAQOFPUVMAGM-UHFFFAOYSA-N 0.000 description 1
- PQNPPVJWBYLFNT-UHFFFAOYSA-N [Bi].C1=CC=CC=2C3=CC=CC=C3CC12 Chemical compound [Bi].C1=CC=CC=2C3=CC=CC=C3CC12 PQNPPVJWBYLFNT-UHFFFAOYSA-N 0.000 description 1
- 239000012190 activator Substances 0.000 description 1
- 239000000654 additive Substances 0.000 description 1
- 229910052782 aluminium Inorganic materials 0.000 description 1
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 1
- 229910052787 antimony Inorganic materials 0.000 description 1
- WATWJIUSRGPENY-UHFFFAOYSA-N antimony atom Chemical compound [Sb] WATWJIUSRGPENY-UHFFFAOYSA-N 0.000 description 1
- WUKWITHWXAAZEY-UHFFFAOYSA-L calcium difluoride Chemical compound [F-].[F-].[Ca+2] WUKWITHWXAAZEY-UHFFFAOYSA-L 0.000 description 1
- 150000001860 citric acid derivatives Chemical class 0.000 description 1
- 239000003086 colorant Substances 0.000 description 1
- 210000003298 dental enamel Anatomy 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 239000003822 epoxy resin Substances 0.000 description 1
- 239000010436 fluorite Substances 0.000 description 1
- 229910052733 gallium Inorganic materials 0.000 description 1
- OAKJQQAXSVQMHS-UHFFFAOYSA-N hydrazine Substances NN OAKJQQAXSVQMHS-UHFFFAOYSA-N 0.000 description 1
- 230000001771 impaired effect Effects 0.000 description 1
- 229910052746 lanthanum Inorganic materials 0.000 description 1
- FZLIPJUXYLNCLC-UHFFFAOYSA-N lanthanum atom Chemical compound [La] FZLIPJUXYLNCLC-UHFFFAOYSA-N 0.000 description 1
- 239000000463 material Substances 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- 229920000647 polyepoxide Polymers 0.000 description 1
- 238000009877 rendering Methods 0.000 description 1
- 229910052715 tantalum Inorganic materials 0.000 description 1
- GUVRBAGPIYLISA-UHFFFAOYSA-N tantalum atom Chemical compound [Ta] GUVRBAGPIYLISA-UHFFFAOYSA-N 0.000 description 1
Classifications
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- 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
- H01L33/504—Elements with two or more wavelength conversion materials
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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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- 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
- C09K11/0883—Arsenides; Nitrides; Phosphides
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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
- C09K11/7728—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
- C09K11/7728—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials containing rare earth metals containing europium
- C09K11/77348—Silicon Aluminium Nitrides or Silicon Aluminium Oxynitrides
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- G—PHYSICS
- G02—OPTICS
- G02F—OPTICAL DEVICES OR ARRANGEMENTS FOR THE CONTROL OF LIGHT BY MODIFICATION OF THE OPTICAL PROPERTIES OF THE MEDIA OF THE ELEMENTS INVOLVED THEREIN; NON-LINEAR OPTICS; FREQUENCY-CHANGING OF LIGHT; OPTICAL LOGIC ELEMENTS; OPTICAL ANALOGUE/DIGITAL CONVERTERS
- G02F1/00—Devices or arrangements for the control of the intensity, colour, phase, polarisation or direction of light arriving from an independent light source, e.g. switching, gating or modulating; Non-linear optics
- G02F1/01—Devices or arrangements for the control of the intensity, colour, phase, polarisation or direction of light arriving from an independent light source, e.g. switching, gating or modulating; Non-linear optics for the control of the intensity, phase, polarisation or colour
- G02F1/13—Devices or arrangements for the control of the intensity, colour, phase, polarisation or direction of light arriving from an independent light source, e.g. switching, gating or modulating; Non-linear optics for the control of the intensity, phase, polarisation or colour based on liquid crystals, e.g. single liquid crystal display cells
- G02F1/133—Constructional arrangements; Operation of liquid crystal cells; Circuit arrangements
- G02F1/1333—Constructional arrangements; Manufacturing methods
- G02F1/1335—Structural association of cells with optical devices, e.g. polarisers or reflectors
- G02F1/1336—Illuminating devices
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- 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
- H01L33/02—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 bodies
- H01L33/26—Materials of the light emitting region
- H01L33/30—Materials of the light emitting region containing only elements of Group III and Group V of the Periodic Table
- H01L33/32—Materials of the light emitting region containing only elements of Group III and Group V of the Periodic Table containing nitrogen
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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
- H01L33/505—Wavelength conversion elements characterised by the shape, e.g. plate or foil
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- 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
- H01L33/507—Wavelength conversion elements the elements being in intimate contact with parts other than the semiconductor body or integrated with parts other than the semiconductor body
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- 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
- H01L33/52—Encapsulations
- H01L33/56—Materials, e.g. epoxy or silicone resin
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- G—PHYSICS
- G02—OPTICS
- G02F—OPTICAL DEVICES OR ARRANGEMENTS FOR THE CONTROL OF LIGHT BY MODIFICATION OF THE OPTICAL PROPERTIES OF THE MEDIA OF THE ELEMENTS INVOLVED THEREIN; NON-LINEAR OPTICS; FREQUENCY-CHANGING OF LIGHT; OPTICAL LOGIC ELEMENTS; OPTICAL ANALOGUE/DIGITAL CONVERTERS
- G02F1/00—Devices or arrangements for the control of the intensity, colour, phase, polarisation or direction of light arriving from an independent light source, e.g. switching, gating or modulating; Non-linear optics
- G02F1/01—Devices or arrangements for the control of the intensity, colour, phase, polarisation or direction of light arriving from an independent light source, e.g. switching, gating or modulating; Non-linear optics for the control of the intensity, phase, polarisation or colour
- G02F1/13—Devices or arrangements for the control of the intensity, colour, phase, polarisation or direction of light arriving from an independent light source, e.g. switching, gating or modulating; Non-linear optics for the control of the intensity, phase, polarisation or colour based on liquid crystals, e.g. single liquid crystal display cells
- G02F1/133—Constructional arrangements; Operation of liquid crystal cells; Circuit arrangements
- G02F1/1333—Constructional arrangements; Manufacturing methods
- G02F1/1335—Structural association of cells with optical devices, e.g. polarisers or reflectors
- G02F1/1336—Illuminating devices
- G02F1/133614—Illuminating devices using photoluminescence, e.g. phosphors illuminated by UV or blue light
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
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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
- H01L2224/01—Means for bonding being attached to, or being formed on, the surface to be connected, e.g. chip-to-package, die-attach, "first-level" interconnects; Manufacturing methods related thereto
- 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
- H01L2224/4805—Shape
- H01L2224/4809—Loop shape
- H01L2224/48091—Arched
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L2224/00—Indexing scheme for arrangements for connecting or disconnecting semiconductor or solid-state bodies and methods related thereto as covered by H01L24/00
- H01L2224/01—Means for bonding being attached to, or being formed on, the surface to be connected, e.g. chip-to-package, die-attach, "first-level" interconnects; Manufacturing methods related thereto
- 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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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- 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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- Physics & Mathematics (AREA)
- Organic Chemistry (AREA)
- Materials Engineering (AREA)
- Inorganic Chemistry (AREA)
- Nonlinear Science (AREA)
- Mathematical Physics (AREA)
- Crystallography & Structural Chemistry (AREA)
- General Physics & Mathematics (AREA)
- Optics & Photonics (AREA)
- Luminescent Compositions (AREA)
- Led Device Packages (AREA)
Description
本發明係關於一種發光裝置,其包括發射初級光之發光元件,及吸收自發光元件發射之初級光之一部分、並發射具有較初級光之波長更長之波長的次級光之波長轉換部。
半導體發光元件與螢光體組合之發光裝置,作為於低電力消耗、小型化、高亮度、進而廣範圍之色再現性方面備受期待的下一代發光裝置而受到關注,正在活躍地進行研究、開發。自發光元件所發射之初級光,通常係使用自長波長之紫外線至藍色之範圍、即380~480nm者。又,亦提出有使用適於該用途之各種螢光體之波長轉換部。
進而,近年來小型液晶顯示器(以下稱為LCD(Liquid Crystal Display))用背光之開發競爭正在激化。於此領域中雖提出有各種方式,但並未發現同時滿足亮度與色再現性(NTSC比)之方式。
現在,作為白色之發光裝置,主要係使用藍色發光之發光元件(峰值波長:450nm左右)與顯示由該藍色所激發之黃色發光的以3價鈰活化之(Y、Gd)3(Al,Ga)5O12螢光體或以2價銪活化之(Sr,Ba,Ca)2SiO4螢光體之組合。然而,該等發光裝置之色再現性(NTSC比)為65%左右(CIE1931)。另一方面,近年來,小型LCD亦要求色再現性更好者。於此背景下,小型LCD用背光之色再現性(NTSC比)之改善成為當務之急。
作為著眼於LCD之色再現性(NTSC比)者,例如有日本專利特開2003-121838號公報(專利文獻1)。專利文獻1中記載有,作為背光光源,於505~535nm之範圍內具有光譜峰值;以及,作為該光源中所使用之綠螢光體之活化劑,而包含銪、鎢、錫、銻、錳中之任一者;進而,實施例中記載有使用MgGa2O4:Mn、Zn2SiO4:Mn作為綠螢光體。然而,於發光元件之峰值波長為430~480nm之範圍之情形時,包含銪、鎢、錫、銻、錳中之任一者之螢光體並非全部適用。即,專利文獻1之實施例中所記載之MgGa2O4:Mn、Zn2SiO4:Mn,若為430~480nm之範圍內之激發光,則其發光效率明顯降低。
又,例如於日本專利特開2004-287323號公報(專利文獻2)中記載有,作為背光,除紅發光LED晶片、綠發光LED晶片與藍發光LED晶片成為1個封裝體之RGB-LED以外,亦有3波長型螢光管、紫外光LED+RGB螢光體、有機EL光源等。然而於專利文獻2中並無以藍色光作為激發源之RG螢光體之相關具體記載。
另一方面,關於4價錳活化氟化金屬鹽螢光體,例如於US20060169998A1(專利文獻3)中有記載。然而於專利文獻3中,與高效率之綠色螢光體組合,並未言及其色再現性(NTSC比)。
專利文獻1:日本專利特開2003-121838號公報
專利文獻2:日本專利特開2004-287323號公報
專利文獻3:US20060169998A1
本發明係為解決上述課題而完成者,其目的在於使用藉由來自發光元件之430~480nm之範圍的光而高效率地發光之特定螢光體,藉此提供色再現性(NTSC比)優異之發光裝置。
本發明之發光裝置之特徵在於包括:發光元件,其係發射初級光;及波長轉換部,其係吸收自發光元件發射之初級光之一部分,並發射具有較初級光之波長更長之波長的次級光;且上述波長轉換部包含綠色系發光螢光體及紅色系發光螢光體,上述綠色系發光螢光體包含:選自實質上以通式(A):EuaSibAlcOdNe
(於上述通式(A)中,0.005≦a≦0.4,b+c=12,d+e=16)表示之β型SiAlON即2價銪活化氧氮化物螢光體,以及實質上以通式(B):2(Ba1-f-gMIfEug)O‧SiO2
(於上述通式(B)中,MI表示選自Mg、Ca及Sr中之至少一種之鹼土金屬元素,0<f≦0.55,0.03≦g≦0.10)表示之2價銪活化矽酸鹽螢光體中之至少一種;上述紅色系發光螢光體(5)包含:選自實質上以通式(C):MII2(MIII1-hMnh)F6
(於上述通式(C)中,MII表示選自Li、Na、K、Rb及Cs中之至少一種鹼金屬元素,MIII表示選自Ge、Si、Sn、Ti及Zr中之至少一種之4價金屬元素,0.001≦h≦0.1)表示之4價錳活化氟化4價金屬鹽螢光體;及實質上以通式(D):MIV(MIII1-hMnh)F6
(於上述通式(D)中,MIV表示選自Mg、Ca、Sr、Ba及Zn中之至少一種之鹼土金屬元素,MIII表示選自Ge、Si、Sn、Ti及Zr中之至少一種之4價金屬元素,0.001≦h≦0.1)表示之4價錳活化氟化4價金屬鹽螢光體中之至少一種。
此處,較好的是MII為K,MIII為Ti。
又,於本發明之發光裝置中,較好的是0.005≦h≦0.05。
又,於本發明之發光裝置中,較好的是MI為Sr。
本發明之發光裝置之發光元件,較好的是發射峰值波長430~480nm之初級光之氮化鎵系半導體。
根據本發明,可提供一種發光裝置,其可於波長轉換部高效率地吸收來自發光元件之發光,發出高效率之白色光,並且獲得色再現性(NTSC比)明顯良好之白色光。
1‧‧‧發光裝置
2‧‧‧發光元件
3‧‧‧波長轉換部
4‧‧‧綠色系發光螢光體
5‧‧‧紅色系發光螢光體
6‧‧‧密封劑
圖1係示意性地表示本發明之較好一例的發光裝置1之剖面圖。
圖2係表示可用於本發明之發光裝置中之β型SiAlON即2價銪活化氧氮化物螢光體之具體一例的發光光譜分布之圖表。
圖3係表示可用於本發明之發光裝置中之2價銪活化矽酸鹽螢光體之具體一例的發光光譜分布之圖表。
圖4係表示可用於本發明之發光裝置中之4價錳活化氟化4價金屬鹽螢光體之具體一例的發光光譜分布之圖表。
圖5係表示本發明之較好一例之發光裝置的發光光譜分布之圖表。
圖6係表示組入有本發明之較好一例之發光裝置作為背光光源的LCD之色再現性之色度圖。
圖7係表示使用黃色系發光螢光體之先前之發光裝置的發光光譜分布之圖表。
圖8係表示組入有使用黃色系發光螢光體之先前之發光裝置作為背光光源的LCD之色再現性之色度圖。
圖1係模式性地表示本發明較好一例的發光裝置1之剖面圖。本發明之發光裝置1如圖1所示,基本上包括:發射初級光之發光元件2,及吸收自發光元件2發射之初級光之一部分並發射具有較初級光之
波長更長之波長之次級光的波長轉換部3;波長轉換部3包含綠色系發光螢光體4及紅色系發光螢光體5。圖1中表示以如下方式實現波長轉換部3之例:發光元件2、綠色系發光螢光體4及紅色系發光螢光體5密封於密封劑6中,吸收自發光元件2發射之初級光之一部分,可發射具有初級光波長以上之長度波長之次級光。本發明之發光裝置1中之波長轉換部3,其特徵在於:包含選自以下之(A)β型SiAlON即2價銪活化氧氮化物螢光體及(B)2價銪活化矽酸鹽螢光體中的至少一種作為綠色系發光螢光體4;包含選自以下2種之(C)、(D)4價錳活化氟化4價金屬鹽螢光體中的至少一種作為紅色系發光螢光體。
(A)β型SiAlON即2價銪活化氧氮化物綠色系發光螢光體
該2價銪活化氧氮化物綠色系發光螢光體實質上以通式(A):EuaSibAlcOdNe
表示(以下,將該2價銪活化氧氮化物綠色系發光螢光體稱為「第1綠色系發光螢光體」)。於通式(A)中,Eu表示銪,Si表示矽,Al表示鋁,O表示氧,N表示氮。於通式(A)中,表示Eu之組成比(濃度)之a之值為0.005≦a≦0.4。因為於a之值未滿0.005之情形時,無法獲得充分之亮度;又因為於a之值超過0.4之情形時,由於濃度淬滅而亮度大幅度下降。再者,考慮到粉體特性之穩定性、母體之均質性,上述式中之a之值較好的是0.01≦a≦0.2。又,於通式(A)中,表示Si之組成比(濃度)之b及表示Al之組成比(濃度)之c係滿足b+c=12之數,表示O之組成比(濃度)之d及表示N之組成比(濃度)之e係滿足d+e=16之數。
作為該第1綠色系發光螢光體,具體而言可列舉Eu0.05Si11.50Al0.50O0.05N15.95、Eu0.10Si11.00Al1.00O0.10N15.90、Eu0.30Si9.8OAl2.20O0.30N15.70、Eu0.15Si10.00Al2.00O0.20N15.80、Eu0.01Si11.60Al0.40O0.01N15.99、Eu0.005Si11.70Al0.30O0.03N15.97等,當然並不限定於此。
(B)2價銪活化矽酸鹽螢光體
該2價銪活化矽酸鹽螢光體實質上以通式(B):2(Ba1-f-gMIfEug)O‧SiO2
表示(以下,將該2價銪活化矽酸鹽螢光體稱為「第2綠色系發光螢光體」)。於通式(B)中,Ba表示鋇,Eu表示銪,O表示氧,Si表示矽。於通式(B)中,MI表示選自Mg、Ca及Sr中之至少一種之鹼土金屬元素,為獲得高效率之母體,較好的是Mi為Sr。於通式(B)中,表示MI之組成比(濃度)之f之值為0<f≦0.55,藉由f之值為於此範圍內,可獲得510~540nm之範圍之綠色系發光。於f之值超過0.55之情形時,會成為發黃之綠色系發光,導致色純度變差。進而,就效率、色純度之觀點而言,較好的是f之值為0.15≦f≦0.45之範圍之範圍內。又於通式(B)中,表示Eu之組成比(濃度)之g之值為0.03≦g≦0.10。因為於g之值未滿0.03之情形時,無法獲得充分之亮度;又,因為於g之值超過0.10之情形時,由於濃度淬滅而亮度大幅度下降。再者,考慮到亮度及粉體特性之穩定性,較好的是g之值於0.04≦g≦0.08之範圍內。
作為該第2綠色系發光螢光體,具體而言可列舉2(Ba0.70Sr0.26Eu0.04)‧SiO2、2(Ba0.57Sr0.38Eu0.05)O‧SiO2、2(Ba0.53Sr0.43Eu0.04)O‧SiO2、2(Ba0.82Sr0.15Eu0.03)O‧SiO2、2(Ba0.46Sr0.49Eu0.05)O‧SiO2、2(Ba0.59Sr0.35Eu0.06)O‧SiO2、2(Ba0.52Sr0.40Eu0.08)O‧SiO2、2(Ba0.85Sr0.10Eu0.05)O‧SiO2、2(Ba0.47Sr0.50Eu0.03)O‧SiO2、2(Ba0.54Sr0.36Eu0.10)O‧SiO2、2(Ba0.69Sr0.25Ca0.02Eu0.04)O‧SiO2、2(Ba0.56Sr0.38Mg0.01Eu0.05)O‧SiO2、2(Ba0.81Sr0.13Mg0.01Ca0.01Eu0.04)O.SiO2等,當然並不限定於此。
(C)4價錳活化氟化4價金屬鹽螢光體
該4價錳活化氟化4價金屬鹽螢光體,實質上以通式(C):MII2(MIII1-hMnh)F6
表示(以下,將該4價錳活化氟化4價金屬鹽螢光體稱為「第1紅色系發光螢光體」)。再者,於通式(C)中,Mn表示錳,F表示氟。於通式(C)中,MII表示選自Na、K、Rb及Cs中的至少一種之鹼金屬元素,考慮到亮度及粉體特性之穩定性,較好的是MII為K。又於通式(C)中,MIII表示選自Ge、Si、Sn、Ti及Zr中的至少一種之4價金屬元素,考慮到亮度及粉體特性之穩定性,較好的是MIII為Ti。又,於通式(C)中,表示Mn之組成比(濃度)之h之值為0.001≦h≦0.1。因為於h之值未滿0.001之情形時,具有無法獲得充分之亮度之不良情況,又,於h之值超過0.1之情形時,具有由於濃度淬滅而亮度大幅度下降之不良情況。考慮到亮度及粉體特性之穩定性,較好的是h之值為0.005≦h≦0.5。
作為該第1紅色系發光螢光體,具體而言可列舉K2(Ti0.99Mn0.01)F6、K2(Ti0.9Mn0.1)F6、K2(Ti0.999Mn0.001)F6、Na2(Zr0.98Mn0.02)F6、Cs2(Si0.95Mn0.05)F6、Cs2(Sn0.98Mn0.02)F6、K2(Ti0.88Zr0.10Mn0.02)F6、Na2(Ti0.75Sn0.20Mn0.05)F6、Cs2(Ge0.999Mn0.001)F6、(K0.80Na0.20)2(Ti0.69Ge0.30Mn0.01)F6等,當然並不限定於此。
(D)4價錳活化氟化4價金屬鹽螢光體
該4價錳活化氟化4價金屬鹽螢光體,實質上以通式(D):MIV(MIII1-hMnh)F6
表示(以下,將該4價錳活化氟化4價金屬鹽螢光體稱為「第2紅色系發光螢光體」)。再者,於通式(D)中,Mn表示錳,F表示氟。於通式(D)中,MIII與上述通式(C)中之MIII相同,表示選自Ge、Si、Sn、Ti及Zr中的至少一種之4價金屬元素,出於同樣之理由,較好的是MIII為Ti。又於通式(D)中,MIV表示選自Mg、Ca、Sr、Ba及Zn中的至少一種之鹼土金屬元素,考慮到亮度及粉體特性之穩定性,較好的
是MIV為Ca。又,於通式(D)中,表示Mn之組成比(濃度)之h之值與上述通式(C)中之h相同,為0.001≦h≦0.1,出於同樣之理由,較好的是0.005≦h≦0.5。
作為該第2紅色系發光螢光體,具體而言可列舉Zn(Ti0.98Mn0.02)F6、Ba(Zr0.995Mn0.005)F6、Ca(Ti0.995Mn0.005)F6、Sr(Zr0.98Mn0.02)F6等,當然並不限定於此。
本發明之發光裝置中之波長轉換部,包含選自上述之(A)β型SiAlON即2價銪活化氧氮化物螢光體(第1綠色系發光螢光體)及(B)2價銪活化矽酸鹽螢光體(第2綠色系發光螢光體)中的至少一種來作為綠色系發光螢光體;包含選自上述2種之(C)4價錳活化氟化4價金屬鹽螢光體(第1紅色系發光螢光體)及(D)4價錳活化氟化4價金屬鹽螢光體(第2紅色系發光螢光體)中的至少一種來作為紅色系發光螢光體。再者,分別於圖2中表示可用於本發明之發光裝置中的β型SiAlON即2價銪活化氧氮化物螢光體之具體一例(具體組成:Eu0.05Si11.50Al0.50O0.05N15.95)之發光光譜分布,於圖3中表示可用於本發明之發光裝置中的2價銪活化矽酸鹽螢光體之具體一例(具體組成:2(Ba0.70Sr0.26Eu0.04)O‧SiO2)之發光光譜分布,於圖4中表示可用於本發明之發光裝置中的4價錳活化氟化4價金屬鹽螢光體之具體一例(具體組成:K2(Ti0.99Mn0.01)F6)之發光光譜分布。圖2至圖4所表示之發光光譜均為利用激發波長450nm、使用螢光分光光度計所測定之結果,縱軸為強度(任意單位),橫軸為波長(nm)。
於本發明之發光裝置中,綠色系發光螢光體與紅色系發光螢光體之混合比率並無特別限制,相對於紅色系發光螢光體,較好的是以重量比為5~70%之範圍內之混合比率混合綠色系發光螢光體,更好的是以15~45%之範圍內之混合比率混合。
此處,圖5係表示本發明之較好一例之發光裝置(後述之實施例1
中製作之發光裝置)的發光光譜分布之圖表,於圖5中,縱軸為強度(任意單位),橫軸為波長(nm)。又圖6係表示組入有本發明之較好一例之發光裝置(後述之實施例1所製作之發光裝置)作為背光光源的LCD之色再現性之色度圖(CIE1931)。相對於此,圖7係表示使用黃色系發光螢光體之先前之發光裝置(後述之比較例1中製作之發光裝置)的發光光譜分布之圖表,圖8係表示組入有使用該發光裝置作為背光光源的LCD之色再現性之色度圖(CIE1931)。再者,圖5及圖7所表示之發光裝置之發光光譜分布,係使用MCPD-2000(大塚電子股份有限公司製造)所測定之結果;又,圖6及圖8所表示之色再現性,係使用Bm5(拓普康股份有限公司製造)所測定之結果。自圖5至圖8可知,根據本發明,提供如下發光裝置,其與先前之發光裝置不同,於波長轉換部高效率地吸收來自發光元件之發光,發出高效率之白色光,並且可獲得色再現性(NTSC比)明顯良好之白色光。再者,所謂NTSC比,係指:NTSC(National Television System Committee)所規定之紅、綠、藍各色之XYZ表色系色度圖中之色度座標(x、y)分別為紅(0.670,0.330)、綠(0.210,0.710)、藍(0.140,0.080),相對於連結該紅、綠、藍各自之色度座標所獲得之三角形之面積之比率。
作為用於上述本發明之發光裝置中之發光元件,並無特別限制,可較好地使用發射峰值波長為430~480nm(更合適的是440~480nm)之藍色區域的初級光之氮化鎵(GaN)系半導體來作為發光元件。因為於使用峰值波長未滿430nm之發光元件之情形時,有藍色光成分之貢獻變小、顯色性變差,而變得不實用之虞;又,因為於使用峰值波長超過480nm之發光元件之情形時,有白色下之亮度降低,而變得不實用之虞。
本發明之發光裝置,若具備上述特徵,則對於其他構成並無特別限制。作為密封劑6,可使用具有透光性之樹脂材料即環氧樹脂、
矽樹脂、尿素樹脂等,但並不限定於此。又,於波長轉換部3中,除上述螢光體及密封劑以外,於不妨礙本發明之效果範圍內,當然亦可含有適宜之SiO2、TiO2、ZrO2、Al2O3、Y2O3等添加劑。
再者,用於本發明之發光裝置中之上述綠色系發光螢光體、紅色系發光螢光體,均為眾所周知者,可藉由先前眾所周知之適宜之方法製造、或作為產品而獲得。
以下,列舉實施例及比較例對本發明進行更詳細之說明,但本發明並不限定於該等。
<實施例1>
按以下方式製作圖1所示之例之發光裝置1。使用於450nm具有峰值波長之氮化鎵(GaN)系半導體作為發光元件2,波長轉換部3中,使用Eu0.05Si11.50Al0.50O0.05N15.95(β型SiAlON)作為綠色系發光螢光體,使用K2(Ti0.99Mn0.01)F6作為紅色系發光螢光體。將該等綠色系發光螢光體與紅色系發光螢光體以30:70之比例(重量比)混合而成者分散於規定之樹脂中(樹脂與螢光體之比率為1.00:0.25),製作波長轉換部。按此方式製作實施例1之發光裝置。
<比較例1>
除於波長轉換部中使用以(Y0.40Gd0.45Ce0.15)3Al5O12所表示之黃色系發光螢光體以外,與實施例1同樣製作發光裝置。
針對於實施例1、比較例1中分別獲得之發光裝置,評價亮度、Tc-duv及色再現性(NTSC比)。亮度係藉由於順向電流(IF)20mA之條件下點燈,將來自發光裝置之白色光轉換為光電流而求得。又關於Tc-duv,於順向電流(IF)20mA之條件下點燈,使用大塚電子股份有限公司製造之MCPD-2000測定來自發光裝置之白色光,求得其值。又,關於色再現性(NTSC比),組入所製作之發光裝置作為於市場上出售之LCD電視顯示器之背光光源,使用拓普康股份有限公司製造之
Bm5進行測定,求得其值。結果示於表1中。
自表1可知,本發明之發光裝置與先前產品相比,色再現性(NTSC比)飛躍性地提高,作為中、小型LCD用背光具有較好之特性。
<實施例2>
使用於440nm具有峰值波長之氮化鎵(GaN)系半導體作為發光元件2,使用2(Ba0.70Sr0.26Eu0.04)O‧SiO2作為綠色系發光螢光體,使用K2(Ti0.995Mn0.005)F6作為紅色系發光螢光體,除此以外,與實施例1同樣製作發光裝置。
<比較例2>
除於波長轉換部中使用以(Y0.40Gd0.50Ce0.10)3Al5O12所表示之黃色系發光螢光體以外,與實施例2同樣製作發光裝置。
針對於實施例2、比較例2中分別獲得之發光裝置,與上述實施例1、比較例1之發光裝置之情形同樣評價亮度、Tc-duv及色再現性(NTSC比)。結果示於表2中。
自表2可知,本發明之發光裝置與先前產品相比,色再現性(NTSC比)飛躍性地提高,作為中、小型LCD用背光具有較好之特性。
<實施例3~8、比較例3~8>
除分別使用如下述表3所示之發光元件之峰值波長及螢光體之組合以外,與實施例1同樣製作實施例3~8及比較例3~8之發光裝置,與上述同樣評價亮度、Tc-duv及色再現性(NTSC比)。結果亦合併示於表3中。
自表3亦可知,本發明之發光裝置與先前產品相比,色再現性(NTSC比)飛躍性地提高,作為中、小型LCD用之背光光源具有較好之特性。
1‧‧‧發光裝置
2‧‧‧發光元件
3‧‧‧波長轉換部
4‧‧‧綠色系發光螢光體
5‧‧‧紅色系發光螢光體
6‧‧‧密封劑
Claims (8)
- 一種發光裝置,其包括:發光元件,其發射初級光;及波長轉換部,其吸收自發光元件發射之初級光之一部分,並發射具有較初級光之波長為長之波長的次級光;且上述波長轉換部包含綠色系發光螢光體及紅色系發光螢光體;上述紅色系發光螢光體包含自實質上以通式(C)表示之4價錳活化氟化4價金屬鹽螢光體、與實質上以通式(D)表示之4價錳活化氟化4價金屬鹽螢光體中所選之至少一種:通式(C):MII2(MIII1-hMnh)F6(上述通式(C)中,MII表示選自Li、Na、K、Rb及Cs中之至少一種鹼金屬元素,MIII表示選自Ge、Si、Sn、Ti及Zr中之至少一種4價金屬元素,0.001≦h≦0.1);通式(D):MIV(MIII1-hMnh)F6(上述通式(D)中,MIV表示選自Mg、Ca、Sr、Ba及Zn中之至少一種鹼土金屬元素,MIII表示選自Ge、Si、Sn、Ti及Zr中之至少一種4價金屬元素,0.001≦h≦0.1);以重量比為紅色發光螢光體及綠色系發光螢光體之5~70%之範圍內混合綠色系發光螢光體。
- 如請求項1之發光裝置,其中以重量比為紅色發光螢光體及綠色系發光螢光體之15~45%之範圍內混合上述綠色系發光螢光體。
- 如請求項1之發光裝置,其中綠色系發光螢光體包含自實質上以通式(A)表示之β型SiAlON即2價銪活化氧氮化物螢光體、與實質上以通式(B)表示之2價銪活化矽酸鹽螢光體中所選之至少一種:通式(A):EuaSibAlcOdNe(上述通式(A)中,0.005≦a≦0.4,b+c=12,d+e=16); 通式(B):2(Ba1-f-gMIfEug)O‧SiO2(上述通式(B)中,MI表示選自Mg、Ca及Sr中之至少一種鹼土金屬元素,0<f≦0.55,0.03≦g≦0.10);
- 如請求項1之發光裝置,其中MII為K,MIII為Ti。
- 如請求項1之發光裝置,其中0.005≦h≦0.05。
- 如請求項1之發光裝置,其中MI為Sr。
- 如請求項1之發光裝置,其中發光元件係發射峰值波長430~480nm之初級光之氮化鎵系半導體。
- 一種發光裝置,其包括:發光元件,其發射初級光;及波長轉換部,其吸收自發光元件發射之初級光之一部分,並發射具有較初級光之波長為長之波長的次級光;且上述波長轉換部包含綠色系發光螢光體及紅色系發光螢光體;上述紅色系發光螢光體包含自實質上以通式(C)表示之4價錳活化氟化4價金屬鹽螢光體、與實質上以通式(D)表示之4價錳活化氟化4價金屬鹽螢光體中所選之至少一種:通式(C):MII2(MIII1-hMnh)F6(上述通式(C)中,MII表示選自Li、Na、K、Rb及Cs中之至少一種鹼金屬元素,MIII表示選自Ge、Si、Sn、Ti及Zr中之至少一種4價金屬元素,0.001≦h≦0.1);通式(D):MIV(MIII1-hMnh)F6(上述通式(D)中,MIV表示選自Mg、Ca、Sr、Ba及Zn中之至少一種鹼土金屬元素,MIII表示選自Ge、Si、Sn、Ti及Zr中之至少一種4價金屬元素,0.001≦h≦0.1);上述紅色系發光螢光體之混合比率高於上述綠色系發光螢光體之混合比率。
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US20160064627A1 (en) | 2016-03-03 |
CN101960624B (zh) | 2012-09-26 |
CN102790164A (zh) | 2012-11-21 |
TW201000617A (en) | 2010-01-01 |
US9455381B2 (en) | 2016-09-27 |
CN102790164B (zh) | 2016-08-10 |
TWI655789B (zh) | 2019-04-01 |
CN101960624A (zh) | 2011-01-26 |
US20110043101A1 (en) | 2011-02-24 |
US8362685B2 (en) | 2013-01-29 |
US8829781B2 (en) | 2014-09-09 |
US8237348B2 (en) | 2012-08-07 |
TW201828490A (zh) | 2018-08-01 |
WO2009110285A1 (ja) | 2009-09-11 |
US9184353B2 (en) | 2015-11-10 |
TW201503406A (zh) | 2015-01-16 |
JP2014039052A (ja) | 2014-02-27 |
JPWO2009110285A1 (ja) | 2011-07-14 |
US20130214311A1 (en) | 2013-08-22 |
US20140361332A1 (en) | 2014-12-11 |
US8981639B2 (en) | 2015-03-17 |
US20120267669A1 (en) | 2012-10-25 |
US20150144959A1 (en) | 2015-05-28 |
TWI456789B (zh) | 2014-10-11 |
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