WO2017135373A1 - 蛍光体及びその製造方法、蛍光体含有部材、及び発光装置又はプロジェクター - Google Patents

蛍光体及びその製造方法、蛍光体含有部材、及び発光装置又はプロジェクター Download PDF

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Publication number
WO2017135373A1
WO2017135373A1 PCT/JP2017/003793 JP2017003793W WO2017135373A1 WO 2017135373 A1 WO2017135373 A1 WO 2017135373A1 JP 2017003793 W JP2017003793 W JP 2017003793W WO 2017135373 A1 WO2017135373 A1 WO 2017135373A1
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WIPO (PCT)
Prior art keywords
phosphor
single crystal
light emitting
containing member
particulate
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Ceased
Application number
PCT/JP2017/003793
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English (en)
French (fr)
Japanese (ja)
Inventor
猪股　大介
祐輔 新井
島村　清史
ビジョラ エンカルナシオン アントニア ガルシア
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
National Institute for Materials Science
Tamura Corp
Koha Co Ltd
Original Assignee
National Institute for Materials Science
Tamura Corp
Koha Co Ltd
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Filing date
Publication date
Application filed by National Institute for Materials Science, Tamura Corp, Koha Co Ltd filed Critical National Institute for Materials Science
Priority to EP17747524.1A priority Critical patent/EP3412752B1/en
Priority to CN201780009385.XA priority patent/CN108603113B/zh
Priority to US16/074,163 priority patent/US11525082B2/en
Publication of WO2017135373A1 publication Critical patent/WO2017135373A1/ja
Anticipated expiration legal-status Critical
Ceased legal-status Critical Current

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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
    • C09K11/7766—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials containing rare earth metals containing two or more rare earth metals
    • C09K11/7774—Aluminates
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01F—COMPOUNDS OF THE METALS BERYLLIUM, MAGNESIUM, ALUMINIUM, CALCIUM, STRONTIUM, BARIUM, RADIUM, THORIUM, OR OF THE RARE-EARTH METALS
    • C01F17/00—Compounds of rare earth metals
    • C01F17/30—Compounds containing rare earth metals and at least one element other than a rare earth metal, oxygen or hydrogen, e.g. La4S3Br6
    • C01F17/32—Compounds containing rare earth metals and at least one element other than a rare earth metal, oxygen or hydrogen, e.g. La4S3Br6 oxide or hydroxide being the only anion, e.g. NaCeO2 or MgxCayEuO
    • C01F17/34—Aluminates, e.g. YAlO3 or Y3-xGdxAl5O12
    • 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
    • C09K11/02—Use of particular materials as binders, particle coatings or suspension media therefor
    • C—CHEMISTRY; METALLURGY
    • C30—CRYSTAL GROWTH
    • C30B—SINGLE-CRYSTAL GROWTH; UNIDIRECTIONAL SOLIDIFICATION OF EUTECTIC MATERIAL OR UNIDIRECTIONAL DEMIXING OF EUTECTOID MATERIAL; REFINING BY ZONE-MELTING OF MATERIAL; PRODUCTION OF A HOMOGENEOUS POLYCRYSTALLINE MATERIAL WITH DEFINED STRUCTURE; SINGLE CRYSTALS OR HOMOGENEOUS POLYCRYSTALLINE MATERIAL WITH DEFINED STRUCTURE; AFTER-TREATMENT OF SINGLE CRYSTALS OR A HOMOGENEOUS POLYCRYSTALLINE MATERIAL WITH DEFINED STRUCTURE; APPARATUS THEREFOR
    • C30B29/00—Single crystals or homogeneous polycrystalline material with defined structure characterised by the material or by their shape
    • C30B29/10—Inorganic compounds or compositions
    • C30B29/16—Oxides
    • C30B29/22—Complex oxides
    • C30B29/28—Complex oxides with formula A3Me5O12 wherein A is a rare earth metal and Me is Fe, Ga, Sc, Cr, Co or Al, e.g. garnets
    • C—CHEMISTRY; METALLURGY
    • C30—CRYSTAL GROWTH
    • C30B—SINGLE-CRYSTAL GROWTH; UNIDIRECTIONAL SOLIDIFICATION OF EUTECTIC MATERIAL OR UNIDIRECTIONAL DEMIXING OF EUTECTOID MATERIAL; REFINING BY ZONE-MELTING OF MATERIAL; PRODUCTION OF A HOMOGENEOUS POLYCRYSTALLINE MATERIAL WITH DEFINED STRUCTURE; SINGLE CRYSTALS OR HOMOGENEOUS POLYCRYSTALLINE MATERIAL WITH DEFINED STRUCTURE; AFTER-TREATMENT OF SINGLE CRYSTALS OR A HOMOGENEOUS POLYCRYSTALLINE MATERIAL WITH DEFINED STRUCTURE; APPARATUS THEREFOR
    • C30B29/00—Single crystals or homogeneous polycrystalline material with defined structure characterised by the material or by their shape
    • C30B29/60—Single crystals or homogeneous polycrystalline material with defined structure characterised by the material or by their shape characterised by shape
    • C—CHEMISTRY; METALLURGY
    • C30—CRYSTAL GROWTH
    • C30B—SINGLE-CRYSTAL GROWTH; UNIDIRECTIONAL SOLIDIFICATION OF EUTECTIC MATERIAL OR UNIDIRECTIONAL DEMIXING OF EUTECTOID MATERIAL; REFINING BY ZONE-MELTING OF MATERIAL; PRODUCTION OF A HOMOGENEOUS POLYCRYSTALLINE MATERIAL WITH DEFINED STRUCTURE; SINGLE CRYSTALS OR HOMOGENEOUS POLYCRYSTALLINE MATERIAL WITH DEFINED STRUCTURE; AFTER-TREATMENT OF SINGLE CRYSTALS OR A HOMOGENEOUS POLYCRYSTALLINE MATERIAL WITH DEFINED STRUCTURE; APPARATUS THEREFOR
    • C30B33/00—After-treatment of single crystals or homogeneous polycrystalline material with defined structure
    • G—PHYSICS
    • G03—PHOTOGRAPHY; CINEMATOGRAPHY; ANALOGOUS TECHNIQUES USING WAVES OTHER THAN OPTICAL WAVES; ELECTROGRAPHY; HOLOGRAPHY
    • G03B—APPARATUS OR ARRANGEMENTS FOR TAKING PHOTOGRAPHS OR FOR PROJECTING OR VIEWING THEM; APPARATUS OR ARRANGEMENTS EMPLOYING ANALOGOUS TECHNIQUES USING WAVES OTHER THAN OPTICAL WAVES; ACCESSORIES THEREFOR
    • G03B21/00—Projectors or projection-type viewers; Accessories therefor
    • G—PHYSICS
    • G03—PHOTOGRAPHY; CINEMATOGRAPHY; ANALOGOUS TECHNIQUES USING WAVES OTHER THAN OPTICAL WAVES; ELECTROGRAPHY; HOLOGRAPHY
    • G03B—APPARATUS OR ARRANGEMENTS FOR TAKING PHOTOGRAPHS OR FOR PROJECTING OR VIEWING THEM; APPARATUS OR ARRANGEMENTS EMPLOYING ANALOGOUS TECHNIQUES USING WAVES OTHER THAN OPTICAL WAVES; ACCESSORIES THEREFOR
    • G03B21/00—Projectors or projection-type viewers; Accessories therefor
    • G03B21/14—Details
    • G—PHYSICS
    • G03—PHOTOGRAPHY; CINEMATOGRAPHY; ANALOGOUS TECHNIQUES USING WAVES OTHER THAN OPTICAL WAVES; ELECTROGRAPHY; HOLOGRAPHY
    • G03B—APPARATUS OR ARRANGEMENTS FOR TAKING PHOTOGRAPHS OR FOR PROJECTING OR VIEWING THEM; APPARATUS OR ARRANGEMENTS EMPLOYING ANALOGOUS TECHNIQUES USING WAVES OTHER THAN OPTICAL WAVES; ACCESSORIES THEREFOR
    • G03B21/00—Projectors or projection-type viewers; Accessories therefor
    • G03B21/14—Details
    • G03B21/20—Lamp housings
    • G03B21/2006—Lamp housings characterised by the light source
    • G03B21/2033—LED or laser light sources
    • G03B21/204—LED or laser light sources using secondary light emission, e.g. luminescence or fluorescence
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01S—DEVICES USING THE PROCESS OF LIGHT AMPLIFICATION BY STIMULATED EMISSION OF RADIATION [LASER] TO AMPLIFY OR GENERATE LIGHT; DEVICES USING STIMULATED EMISSION OF ELECTROMAGNETIC RADIATION IN WAVE RANGES OTHER THAN OPTICAL
    • H01S5/00—Semiconductor lasers
    • H01S5/02—Structural details or components not essential to laser action
    • H01S5/022—Mountings; Housings
    • H01S5/0239—Combinations of electrical or optical elements
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10H—INORGANIC LIGHT-EMITTING SEMICONDUCTOR DEVICES HAVING POTENTIAL BARRIERS
    • H10H20/00—Individual inorganic light-emitting semiconductor devices having potential barriers, e.g. light-emitting diodes [LED]
    • H10H20/80—Constructional details
    • H10H20/85—Packages
    • H10H20/851—Wavelength conversion means
    • H10H20/8511—Wavelength conversion means characterised by their material, e.g. binder
    • H10H20/8512—Wavelength conversion materials
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
    • C01P2002/00—Crystal-structural characteristics
    • C01P2002/50—Solid solutions
    • C01P2002/52—Solid solutions containing elements as dopants
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
    • C01P2004/00—Particle morphology
    • C01P2004/01—Particle morphology depicted by an image
    • C01P2004/03—Particle morphology depicted by an image obtained by SEM
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
    • C01P2004/00—Particle morphology
    • C01P2004/60—Particles characterised by their size
    • C01P2004/61—Micrometer sized, i.e. from 1-100 micrometer
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
    • C01P2006/00—Physical properties of inorganic compounds
    • C01P2006/32—Thermal properties
    • C01P2006/37—Stability against thermal decomposition

Definitions

  • the present invention relates to a phosphor and a manufacturing method thereof, a phosphor-containing member, and a light emitting device or a projector.
  • a phosphor made of a YAG single crystal is known (see, for example, Patent Document 1).
  • a phosphor made of a single crystal has excellent temperature characteristics as compared with a ceramic powder phosphor with less decrease in fluorescence intensity due to an increase in temperature.
  • a light emitting device using a particulate single crystal phosphor obtained by pulverizing a YAG single crystal ingot is known (for example, see Patent Documents 1 and 2).
  • One embodiment of the present invention provides the following phosphors [1] and [2] in order to achieve the above object.
  • the other aspect of this invention provides the fluorescent substance containing member of following [3].
  • the other aspect of this invention provides the light-emitting device of following [4] and [5].
  • Another aspect of the present invention provides the following projectors [6] and [7].
  • the other aspect of this invention provides the manufacturing method of the fluorescent substance of following [8] and [9].
  • a particulate phosphor composed of a YAG-based or LuAG-based single crystal having excellent external quantum efficiency and excellent emission characteristics under high temperature conditions, a method for producing the same, and a phosphor including the phosphor A light-emitting device or a projector having the containing member and the phosphor-containing member can be provided.
  • FIG. 6 is a schematic diagram of a light source unit of a laser headlight which is a light emitting device according to the second embodiment.
  • FIG. 7A is a cross-sectional view of the phosphor-containing member according to the second embodiment.
  • FIG. 7B is a plan view of the phosphor-containing member according to the second embodiment.
  • FIG. 7C is a plan view of the phosphor-containing member according to the second embodiment.
  • FIG. 8 is a schematic diagram illustrating a configuration of a projector according to the third embodiment.
  • FIG. 9A is a plan view of the phosphor-containing member according to the third embodiment.
  • FIG. 9B is a cross-sectional view of the phosphor-containing member according to the third embodiment.
  • FIG. 9A is a plan view of the phosphor-containing member according to the third embodiment.
  • FIG. 9B is a cross-sectional view of the phosphor-containing member according to the third embodiment.
  • FIG. 10 is a schematic diagram illustrating a configuration of an evaluation optical system according to the second embodiment.
  • FIG. 11A shows an output of a laser diode array and three types of phosphor-containing members having different sealing material thicknesses when a conventional YAG-based polycrystalline phosphor is used as the phosphor in the phosphor-containing member. It is a graph which shows the relationship with the surface temperature of the fluorescent substance sealed.
  • FIG. 11B shows the output of the laser diode array and the three types of phosphor-containing members having different sealing material thicknesses when a conventional YAG-based polycrystalline phosphor is used as the phosphor in the phosphor-containing member. It is a graph which shows the relationship with fluorescence intensity.
  • FIG. 11A shows an output of a laser diode array and three types of phosphor-containing members having different sealing material thicknesses when a conventional YAG-based polycrystalline phosphor is used as the phosphor in the phosphor-containing member. It is a
  • the single crystal phosphor according to the first embodiment includes a Y 3 Al 5 O 12 (YAG) crystal or a Lu 3 Al 5 O 12 (LuAG) crystal as a mother crystal. a body, the composition formula (Y 1-x-y- z Lu x Gd y Ce z) 3 + a Al 5-a O 12 (0 ⁇ x ⁇ 0.9994,0 ⁇ y ⁇ 0.0669,0.001 ⁇ z ⁇ 0.004, ⁇ 0.016 ⁇ a ⁇ 0.315).
  • Lu and Gd are components that do not serve as the emission center for substituting Y.
  • Ce is a component (activator) that can serve as a luminescent center for substituting Y.
  • the volume ratio of the phosphor to the material of the sealing member increases as the particle size of the phosphor increases.
  • the sealing material has a lower thermal conductivity than the phosphor, and as a result, the thermal resistance increases. Therefore, by increasing the volume ratio of the phosphor to the material of the sealing member, The thermal resistance of the member can be reduced.
  • a known crushing device such as a roll mill, a ball mill, or a jet mill can be used.
  • a mortar or pestle may be used.
  • the material of the member in contact with the YAG such as a mill or a ball in the pulverizer is preferably high in hardness, and is most preferably single crystal YAG from the viewpoint of contamination, but from the viewpoint of productivity. High purity alumina may also be used.
  • the YAG-based single crystal phosphor has less decrease in fluorescence intensity due to the temperature rise than the YAG-based polycrystalline phosphor manufactured by a sintering method or the like.
  • the decrease in fluorescence intensity is small because the decrease in internal quantum efficiency is small. The same applies to the LuAG single crystal phosphor.
  • the phosphor of the present embodiment has the thermal resistance of the phosphor-containing member by controlling the particle size. Since it has the effect of reducing, it is more suitable for use under high temperature conditions. For example, an excellent function can be exhibited as a phosphor used in a light emitting device having extremely high luminance per unit area, such as a laser projector or laser headlight in which excitation light is laser light. In addition, since the phosphor of the present embodiment is in the form of particles, it has an effect of increasing light scattering, and more uniform emission intensity and emission color can be realized.
  • the obtained mixed powder is put into the crucible 11 and high frequency energy of 30 kW is supplied to the crucible 11 by the high frequency coil 13 in a nitrogen atmosphere to generate an induced current, and the crucible 11 is heated. As a result, the mixed powder is melted to obtain a melt 14.
  • a single crystal phosphor ingot 16 made of a single crystal having a composition represented by 0.0067, ⁇ 0.016 ⁇ a ⁇ 0.315) is obtained.
  • the size of the single crystal phosphor ingot 16 is, for example, about 2.5 cm in diameter and about 5 cm in length.
  • the particulate single crystal phosphor obtained from the pulverized region 18 in which z is distributed in the range of 0.002 to 0.003 is pulverized in which z is distributed in the range of 0.003 to 0.004.
  • the absorptance can be greatly improved by applying hydrofluoric acid treatment to the particulate single crystal phosphor obtained by pulverizing the single crystal phosphor ingot.
  • FIG. 8 is a schematic diagram showing the configuration of the projector 30 according to the third embodiment.
  • the projector 30 includes a blue laser diode 31 that is a light source, and a phosphor-containing member 33 that emits yellow fluorescence by absorbing and exciting part of the blue light emitted from the laser diode 31 and passing through the condenser lens 32.

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Physics & Mathematics (AREA)
  • Engineering & Computer Science (AREA)
  • Materials Engineering (AREA)
  • General Physics & Mathematics (AREA)
  • Inorganic Chemistry (AREA)
  • Crystallography & Structural Chemistry (AREA)
  • Metallurgy (AREA)
  • Optics & Photonics (AREA)
  • Condensed Matter Physics & Semiconductors (AREA)
  • Electromagnetism (AREA)
  • Multimedia (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Geology (AREA)
  • Luminescent Compositions (AREA)
  • Projection Apparatus (AREA)
  • Led Device Packages (AREA)
  • Semiconductor Lasers (AREA)
PCT/JP2017/003793 2016-02-02 2017-02-02 蛍光体及びその製造方法、蛍光体含有部材、及び発光装置又はプロジェクター Ceased WO2017135373A1 (ja)

Priority Applications (3)

Application Number Priority Date Filing Date Title
EP17747524.1A EP3412752B1 (en) 2016-02-02 2017-02-02 Phosphor-including member, and light emitting device or projector
CN201780009385.XA CN108603113B (zh) 2016-02-02 2017-02-02 荧光体及其制造方法、含荧光体构件以及发光装置或投影仪
US16/074,163 US11525082B2 (en) 2016-02-02 2017-02-02 Phosphor and production method thereof phosphor-including member, and light emitting device or projector

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
JP2016018448A JP6871665B2 (ja) 2016-02-02 2016-02-02 蛍光体含有部材及びその製造方法、及び発光装置又はプロジェクター
JP2016-018448 2016-02-02

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WO2017135373A1 true WO2017135373A1 (ja) 2017-08-10

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PCT/JP2017/003793 Ceased WO2017135373A1 (ja) 2016-02-02 2017-02-02 蛍光体及びその製造方法、蛍光体含有部材、及び発光装置又はプロジェクター

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US (1) US11525082B2 (enExample)
EP (1) EP3412752B1 (enExample)
JP (1) JP6871665B2 (enExample)
CN (1) CN108603113B (enExample)
WO (1) WO2017135373A1 (enExample)

Cited By (1)

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WO2019156159A1 (ja) * 2018-02-09 2019-08-15 株式会社タムラ製作所 波長変換部材

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JP6917244B2 (ja) * 2017-08-23 2021-08-11 日本特殊陶業株式会社 蛍光体ホイール、ホイールデバイスおよびプロジェクター
JP7037082B2 (ja) * 2019-09-27 2022-03-16 日亜化学工業株式会社 希土類アルミン酸塩蛍光体の製造方法、希土類アルミン酸塩蛍光体及び発光装置
JP7429346B2 (ja) * 2019-10-03 2024-02-08 国立研究開発法人物質・材料研究機構 波長変換部材
EP4443120A3 (en) 2020-02-13 2024-12-25 Hamamatsu Photonics K.K. Imaging unit and measurement device
JP2022039095A (ja) 2020-08-27 2022-03-10 セイコーエプソン株式会社 蛍光体粒子、波長変換素子、光源装置、蛍光体粒子の製造方法、波長変換素子の製造方法、及びプロジェクター

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Publication number Priority date Publication date Assignee Title
WO2019156159A1 (ja) * 2018-02-09 2019-08-15 株式会社タムラ製作所 波長変換部材
JP2019139071A (ja) * 2018-02-09 2019-08-22 株式会社タムラ製作所 波長変換部材
JP7224579B2 (ja) 2018-02-09 2023-02-20 株式会社タムラ製作所 波長変換部材

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CN108603113B (zh) 2022-07-05
EP3412752B1 (en) 2024-11-13
JP6871665B2 (ja) 2021-05-12
US20210122975A1 (en) 2021-04-29
EP3412752A1 (en) 2018-12-12
US11525082B2 (en) 2022-12-13
JP2017137394A (ja) 2017-08-10
CN108603113A (zh) 2018-09-28
EP3412752A4 (en) 2019-09-25

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