WO2018189997A1 - 波長変換部材及び波長変換素子、並びにそれらを用いた発光装置 - Google Patents

波長変換部材及び波長変換素子、並びにそれらを用いた発光装置 Download PDF

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Publication number
WO2018189997A1
WO2018189997A1 PCT/JP2018/005780 JP2018005780W WO2018189997A1 WO 2018189997 A1 WO2018189997 A1 WO 2018189997A1 JP 2018005780 W JP2018005780 W JP 2018005780W WO 2018189997 A1 WO2018189997 A1 WO 2018189997A1
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Prior art keywords
wavelength conversion
conversion member
magnesium oxide
light
particles
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PCT/JP2018/005780
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English (en)
French (fr)
Japanese (ja)
Inventor
忠仁 古山
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日本電気硝子株式会社
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    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01LSEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L33/00Semiconductor devices with at least one potential-jump barrier or surface barrier specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
    • H01L33/48Semiconductor devices with at least one potential-jump barrier or surface barrier 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
    • H01L33/50Wavelength conversion elements
    • H01L33/501Wavelength conversion elements characterised by the materials, e.g. binder
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01SDEVICES 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
    • H01S5/00Semiconductor lasers
    • H01S5/02Structural details or components not essential to laser action
    • H01S5/022Mountings; Housings
    • H01S5/0239Combinations of electrical or optical elements
    • CCHEMISTRY; METALLURGY
    • C09DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09KMATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
    • C09K11/00Luminescent, e.g. electroluminescent, chemiluminescent materials
    • C09K11/02Use of particular materials as binders, particle coatings or suspension media therefor
    • CCHEMISTRY; METALLURGY
    • C09DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09KMATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
    • C09K11/00Luminescent, e.g. electroluminescent, chemiluminescent materials
    • C09K11/08Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials
    • CCHEMISTRY; METALLURGY
    • C09DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09KMATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
    • C09K11/00Luminescent, e.g. electroluminescent, chemiluminescent materials
    • C09K11/08Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials
    • C09K11/64Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials containing aluminium
    • GPHYSICS
    • G02OPTICS
    • G02BOPTICAL ELEMENTS, SYSTEMS OR APPARATUS
    • G02B5/00Optical elements other than lenses
    • G02B5/20Filters
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01LSEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L33/00Semiconductor devices with at least one potential-jump barrier or surface barrier specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
    • H01L33/48Semiconductor devices with at least one potential-jump barrier or surface barrier 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
    • H01L33/50Wavelength conversion elements

Definitions

  • the present invention relates to a wavelength conversion member and a wavelength conversion element for converting the wavelength of light emitted from a light emitting diode (LED: Light Emitting Diode) or a laser diode (LD: Laser Diode), etc., and a light emitting device using them.
  • LED Light Emitting Diode
  • LD Laser Diode
  • next-generation light-emitting device that replaces fluorescent lamps and incandescent lamps
  • attention has been focused on light-emitting devices using LEDs and LDs from the viewpoint of low power consumption, small size and light weight, and easy light quantity adjustment.
  • a wavelength conversion member that absorbs part of light from the LED and converts it into yellow light is disposed on the LED that emits blue light.
  • a light emitting device is disclosed. This light emitting device emits white light that is a combined light of blue light emitted from the LED and yellow light emitted from the wavelength conversion member.
  • the wavelength conversion member As the wavelength conversion member, a material in which inorganic phosphor particles are dispersed in a resin matrix is conventionally used. However, when the wavelength conversion member is used, there is a problem that the resin matrix is discolored or deformed by light from the LED. Accordingly, a wavelength conversion member made of a completely inorganic solid in which a phosphor is dispersed and fixed in a glass matrix instead of a resin has been proposed (see, for example, Patent Documents 2 and 3).
  • the wavelength conversion member has a feature that a glass matrix as a base material is not easily deteriorated by heat or irradiation light from an LED, and problems such as discoloration and deformation hardly occur.
  • the output of LEDs and LDs used as light sources has increased for the purpose of increasing the power of light emitting devices. Accordingly, there is a problem that the temperature of the wavelength conversion member rises due to the heat of the light source or the heat emitted from the phosphor irradiated with the excitation light, and as a result, the emission intensity decreases with time (temperature quenching). In some cases, the temperature rise of the wavelength conversion member becomes significant, and the constituent material (glass matrix or the like) may be dissolved.
  • the present invention provides a wavelength conversion member, a wavelength conversion element, and a wavelength conversion member that can suppress a decrease in light emission intensity over time and dissolution of constituent materials when irradiated with high-power LED or LD light, and
  • An object is to provide a light emitting device using them.
  • the wavelength conversion member of the present invention is a wavelength conversion member containing inorganic phosphor particles and magnesium oxide particles, wherein the magnesium oxide particles are interposed between the inorganic phosphor particles, and the inorganic phosphor particles are It is characterized by being bound by magnesium oxide particles.
  • magnesium oxide particles are interposed between the inorganic phosphor particles.
  • the magnesium oxide particles are excellent in thermal conductivity as compared with glass or the like, the heat generated in the inorganic phosphor particles can be efficiently released to the outside. As a result, the temperature rise of the wavelength conversion member is suppressed and temperature quenching is less likely to occur.
  • Magnesium oxide particles also have excellent heat resistance, so they are difficult to dissolve even when irradiated with light from high-power LEDs and LDs, or suppress the occurrence of problems such as thermal cracks due to rapid temperature rise. There is also an advantage of being able to.
  • magnesium oxide particles have an advantage that they can be sintered at a lower temperature than ceramic particles such as aluminum oxide and zirconium oxide. Therefore, the baking temperature at the time of wavelength conversion member preparation can also be made low, and deterioration of the inorganic fluorescent substance powder at the time of baking can be suppressed.
  • the wavelength conversion member of the present invention preferably contains 3 to 80% inorganic phosphor particles and 20 to 97% magnesium oxide particles by mass%.
  • the average particle diameter of the magnesium oxide particles is preferably 0.01 to 10 ⁇ m. In this way, the denseness of the wavelength conversion member is improved and a heat conduction path is easily formed, so that heat generated in the inorganic phosphor particles can be released to the outside more efficiently.
  • the purity of the magnesium oxide particles is preferably 99% or more. In this way, the magnesium oxide particles can be sintered at a relatively low temperature.
  • the average particle diameter of the inorganic phosphor particles is preferably 1 to 50 ⁇ m.
  • the inorganic phosphor particles are preferably made of an oxide phosphor having a garnet structure. Since the oxide phosphor having a garnet structure is excellent in heat resistance, deterioration of the inorganic phosphor particles per se can be suppressed when irradiated with light from a high-power LED or LD.
  • (average particle diameter of magnesium oxide particles) / (average particle diameter of inorganic phosphor particles) is preferably 0.5 or less. In this way, the denseness of the wavelength conversion member is improved and a heat conduction path is easily formed, so that heat generated in the inorganic phosphor particles can be released to the outside more efficiently.
  • the wavelength conversion element of the present invention is characterized by comprising a laminate in which the above-described wavelength conversion member and a heat dissipation layer having a higher thermal conductivity than the wavelength conversion member are laminated. If it does in this way, since the heat generated in the wavelength conversion member can be transmitted to the heat dissipation layer, it becomes easy to suppress the temperature rise of the wavelength conversion member.
  • a heat radiation layer made of translucent ceramics can be used.
  • the translucent ceramic aluminum oxide ceramics, aluminum nitride ceramics, silicon carbide ceramics, boron nitride ceramics, magnesium oxide ceramics, titanium oxide ceramics, niobium oxide ceramics, oxidation At least one selected from zinc-based ceramics and yttrium oxide-based ceramics can be used.
  • a light-emitting device of the present invention is characterized by comprising the above-described wavelength conversion member and a light source that irradiates the wavelength conversion member with excitation light.
  • the light-emitting device of the present invention is characterized by comprising the above-described wavelength conversion element and a light source that irradiates the wavelength conversion element with excitation light.
  • the light source is preferably a laser diode. Since the wavelength conversion member and wavelength conversion element of the present invention are excellent in heat resistance and heat dissipation, it is easy to enjoy the effects of the present invention when a laser diode having a relatively high power is used as the light source.
  • a wavelength conversion member and a wavelength conversion element capable of suppressing a decrease in light emission intensity over time and dissolution of constituent materials when irradiated with light of a high-power LED or LD, and the above
  • the used light-emitting device can be provided.
  • FIG. 1 is a schematic cross-sectional view showing an embodiment of the wavelength conversion member of the present invention.
  • the wavelength conversion member 10 contains inorganic phosphor particles 1 and magnesium oxide particles 2.
  • the magnesium oxide particles 2 are interposed between the inorganic phosphor particles 1, and the inorganic phosphor particles 1 are bound by the magnesium oxide particles 2.
  • the inorganic phosphor particles 1 are not particularly limited as long as they emit fluorescence when incident excitation light is incident.
  • Specific examples of the inorganic phosphor particles 1 include, for example, oxide phosphors, nitride phosphors, oxynitride phosphors, chloride phosphors, acid chloride phosphors, sulfide phosphors, and oxysulfide phosphors. , Halide phosphors, chalcogenide phosphors, aluminate phosphors, halophosphate phosphors, and the like. These can be used individually or in mixture of 2 or more types.
  • the inorganic phosphor particles 1 are oxide phosphors, particularly oxide phosphors having a garnet structure (Y 3 Al 5 O 12 : Ce 3+ , Lu 3 Al 5 O 12 : Ce 3+ etc.). Preferably there is.
  • the average particle diameter (D 50 ) of the inorganic phosphor particles 1 is preferably 1 to 50 ⁇ m, particularly preferably 5 to 25 ⁇ m. If the average particle size of the inorganic phosphor particles 1 is too small, the emission intensity tends to decrease. On the other hand, if the average particle size of the inorganic phosphor particles 1 is too large, the emission color tends to be non-uniform.
  • the average particle diameter (D 50 ) of the magnesium oxide particles 2 is preferably 0.01 to 10 ⁇ m, particularly 0.05 to 5 ⁇ m, and particularly preferably 0.08 to 1 ⁇ m. By setting the average particle diameter in the above range, the magnesium oxide particles 2 can be sintered at a relatively low temperature.
  • the purity of the magnesium oxide particles 2 is preferably 99% or more, 99.9% or more, particularly 99.98% or more. By setting the purity of the magnesium oxide particles 2 in the above range, the magnesium oxide particles 2 can be sintered at a relatively low temperature.
  • the sintering temperature can be lowered by appropriately adjusting the average particle diameter and purity of the magnesium oxide particles 2. Specifically, it can be densely sintered even when fired at a relatively low temperature of 1000 to 1400 ° C., 1020 to 1250 ° C., or even less than 1050 to 1100 ° C.
  • Examples of the method for producing the magnesium oxide particles 2 include a synthesis method using a gas phase oxidation reaction, an underwater spark discharge method, and the like. Among them, the synthesis method by the gas phase oxidation reaction is preferable because high-purity magnesium oxide particles can be easily obtained. In addition, as a commercial item of a magnesium oxide particle, 50A, 2000A, etc. made from Ube Materials can be used.
  • (average particle diameter of the magnesium oxide particles 2) / (average particle diameter of the inorganic phosphor particles 1) is preferably 0.5 or less, 0.2 or less, 0.1 or less, and particularly preferably 0.05 or less. . In this way, the denseness of the wavelength conversion member 10 is improved and a heat conduction path is easily formed, so that the heat generated in the inorganic phosphor particles 1 can be released to the outside more efficiently.
  • the ratio of the inorganic phosphor particles 1 and the magnesium oxide particles 2 in the wavelength conversion member 10 is mass%, and is preferably 3 to 80% inorganic phosphor particles 1 and 20 to 97% magnesium oxide particles 2. More preferably, the particle 1 is 15 to 75%, the magnesium oxide particle 2 is 25 to 95%, and the inorganic phosphor particle 1 is 8 to 70%, and the magnesium oxide particle 2 is 30 to 92%. If the content of the inorganic phosphor particles 1 is too small (the content of the magnesium oxide particles 2 is too large), the light emission intensity of the wavelength conversion member 10 tends to decrease.
  • the content of the inorganic phosphor particles 1 is too large (the content of the magnesium oxide particles 2 is too small), it becomes difficult to form a heat conduction path composed of the magnesium oxide particles 2 in the wavelength conversion member 10. Heat generated in the body particles 1 is not easily released to the outside. Moreover, the binding property of the inorganic phosphor particles 1 is lowered, and the mechanical strength of the wavelength conversion member 10 is easily lowered.
  • the shape of the wavelength conversion member 10 is not particularly limited, but is usually a plate shape (rectangular plate shape, disk shape, etc.).
  • the thickness of the wavelength conversion member 10 is preferably selected as appropriate so that light having a target color can be obtained. Specifically, the thickness of the wavelength conversion member 10 is preferably 2 mm or less, 1 mm or less, and particularly preferably 0.8 mm or less. However, when the thickness of the wavelength conversion member 10 is too small, the mechanical strength tends to be lowered, and therefore, the thickness is preferably 0.03 mm or more.
  • the wavelength conversion member 10 can be manufactured by pre-molding a raw material powder in which the inorganic phosphor particles 1 and the magnesium oxide particles 2 are mixed at a predetermined ratio, and then firing.
  • organic components such as a binder and a solvent
  • an organic component is removed in a degreasing step (about 600 ° C.), followed by firing at the sintering temperature of the magnesium oxide particles 2, whereby a dense sintered body is easily obtained.
  • hole in the wavelength conversion member 10 can be made to shrink
  • polypropylene carbonate, polybutyl methacrylate, polyvinyl butyral, polymethyl methacrylate, polyethyl methacrylate, ethyl cellulose, nitrocellulose, polyester carbonate and the like can be used, and these can be used alone or in combination.
  • terpineol isoamyl acetate, toluene, methyl ethyl ketone, diethylene glycol monobutyl ether acetate, 2,2,4-trimethyl-1,3-pentadiol monoisobutyrate or the like can be used alone or in combination.
  • the paste may contain a sintering aid.
  • sintering aids include crystalline powders such as magnesium phosphate, zirconium phosphate, manganese oxide, barium oxide, yttrium oxide, and silicon oxide, and amorphous oxide powders such as silicic acid and phosphoric acid. Can be used.
  • FIG. 2 is a schematic cross-sectional view showing an embodiment of the wavelength conversion element of the present invention.
  • the wavelength conversion element 20 is composed of a laminate in which a wavelength conversion member 10 and a heat dissipation layer 3 having a higher thermal conductivity than the wavelength conversion member 10 are laminated.
  • heat generated by irradiating the wavelength conversion member 10 with excitation light is efficiently released to the outside through the heat dissipation layer 3. Therefore, it can suppress that the temperature of the wavelength conversion member 10 rises excessively.
  • the heat dissipation layer 3 has a higher thermal conductivity than the wavelength conversion member 10.
  • the heat conductivity of the heat radiation layer 3 is preferably 5 W / m ⁇ K or more, 10 W / m ⁇ K or more, and particularly preferably 20 W / m ⁇ K or more.
  • the thickness of the heat dissipation layer 3 is preferably 0.05 to 1 mm, 0.07 to 0.8 mm, particularly preferably 0.1 to 0.5 mm. If the thickness of the heat dissipation layer 3 is too small, the mechanical strength tends to decrease. On the other hand, if the thickness of the heat dissipation layer 3 is too large, the wavelength conversion element tends to increase in size.
  • the heat dissipation layer 3 a material made of translucent ceramics can be used. In this way, since excitation light or fluorescence can be transmitted, it can be used as a transmission type wavelength conversion element.
  • the total light transmittance at a wavelength of 400 to 800 nm of the heat-radiating layer made of a translucent ceramic is preferably 10% or more, 20% or more, 30% or more, 40%, particularly 50% or more.
  • the translucent ceramics include aluminum oxide ceramics, aluminum nitride ceramics, silicon carbide ceramics, boron nitride ceramics, magnesium oxide ceramics, titanium oxide ceramics, niobium oxide ceramics, zinc oxide ceramics and yttrium oxide ceramics. At least one selected from ceramics can be used.
  • the heat dissipation layer 3 is formed only on one main surface of the wavelength conversion member 10, but the heat dissipation layer 3 may be formed on both main surfaces of the wavelength conversion member 10. In this way, the heat generated in the wavelength conversion member 10 can be released to the outside more efficiently. Furthermore, the laminated body of four or more layers which laminated
  • the heat dissipation layer 3 may be a layer made of a metal such as Cu, Al, Ag, etc. in addition to the light-transmitting ceramic. If it does in this way, it can be used as a reflection type wavelength conversion element.
  • FIG. 3 is a schematic side view showing an embodiment of the light emitting device of the present invention.
  • the light emitting device according to the present embodiment is a light emitting device using a transmission type wavelength conversion member.
  • the light emitting device 30 includes a wavelength conversion member 10 and a light source 4.
  • the excitation light L0 emitted from the light source 4 is wavelength-converted by the wavelength conversion member 10 into fluorescence L1 having a longer wavelength than the excitation light L0. Further, part of the excitation light L0 passes through the wavelength conversion member 10. For this reason, the combined light L2 of the excitation light L0 and the fluorescence L1 is emitted from the wavelength conversion member 10.
  • the excitation light L0 is blue light and the fluorescence L1 is yellow light
  • white synthetic light L2 can be obtained.
  • the wavelength conversion element 20 described above may be used instead of the wavelength conversion member 10.
  • Examples of the light source 4 include LEDs and LDs. From the viewpoint of increasing the light emission intensity of the light emitting device 30, the light source 4 is preferably an LD capable of emitting high intensity light.
PCT/JP2018/005780 2017-04-13 2018-02-19 波長変換部材及び波長変換素子、並びにそれらを用いた発光装置 WO2018189997A1 (ja)

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JP2017079488A JP6802983B2 (ja) 2017-04-13 2017-04-13 波長変換部材及び波長変換素子、並びにそれらを用いた発光装置
JP2017-079488 2017-04-13

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Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2021015261A1 (ja) * 2019-07-22 2021-01-28 地方独立行政法人神奈川県立産業技術総合研究所 蛍光部材およびその製造方法、並びに発光装置
CN113474439A (zh) * 2019-04-18 2021-10-01 日本电气硝子株式会社 波长转换部件及其制造方法、以及发光装置
CN113544236A (zh) * 2019-04-18 2021-10-22 日本电气硝子株式会社 波长转换部件及其制造方法、以及发光装置

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* Cited by examiner, † Cited by third party
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JPWO2021132212A1 (zh) * 2019-12-23 2021-07-01
CN112174646A (zh) * 2020-09-28 2021-01-05 东北大学 一种激光照明用高导热荧光陶瓷及其制备方法

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JPH10195428A (ja) * 1997-01-16 1998-07-28 Toshiba Corp 蛍光体粒子、その製造方法およびプラズマディスプレイパネル
JP2006059629A (ja) * 2004-08-19 2006-03-02 Matsushita Electric Ind Co Ltd プラズマディスプレイ装置
JP2009013412A (ja) * 2007-07-06 2009-01-22 Samsung Sdi Co Ltd 金属化合物で安定化された混成化されたナノ蛍光体膜、その用途およびその製造方法
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CN113544236A (zh) * 2019-04-18 2021-10-22 日本电气硝子株式会社 波长转换部件及其制造方法、以及发光装置
WO2021015261A1 (ja) * 2019-07-22 2021-01-28 地方独立行政法人神奈川県立産業技術総合研究所 蛍光部材およびその製造方法、並びに発光装置
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JP6802983B2 (ja) 2020-12-23
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JP2018180271A (ja) 2018-11-15
CN208507721U (zh) 2019-02-15

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