WO2020246395A1 - Matériau fluorescent, élément de conversion de longueur d'onde et dispositif d'éclairage - Google Patents

Matériau fluorescent, élément de conversion de longueur d'onde et dispositif d'éclairage Download PDF

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Publication number
WO2020246395A1
WO2020246395A1 PCT/JP2020/021435 JP2020021435W WO2020246395A1 WO 2020246395 A1 WO2020246395 A1 WO 2020246395A1 JP 2020021435 W JP2020021435 W JP 2020021435W WO 2020246395 A1 WO2020246395 A1 WO 2020246395A1
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Prior art keywords
light
phosphor
wavelength conversion
conversion member
group
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PCT/JP2020/021435
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English (en)
Japanese (ja)
Inventor
大長 久芳
四ノ宮 裕
岩崎 剛
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株式会社小糸製作所
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Publication of WO2020246395A1 publication Critical patent/WO2020246395A1/fr

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    • 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
    • C09K11/61Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials containing fluorine, chlorine, bromine, iodine or unspecified halogen 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
    • C09K11/08Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials
    • C09K11/63Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials containing boron
    • 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
    • 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
    • C09K11/70Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials containing phosphorus
    • FMECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F21LIGHTING
    • F21VFUNCTIONAL FEATURES OR DETAILS OF LIGHTING DEVICES OR SYSTEMS THEREOF; STRUCTURAL COMBINATIONS OF LIGHTING DEVICES WITH OTHER ARTICLES, NOT OTHERWISE PROVIDED FOR
    • F21V9/00Elements for modifying spectral properties, polarisation or intensity of the light emitted, e.g. filters
    • F21V9/30Elements containing photoluminescent material distinct from or spaced from the light source
    • F21V9/32Elements containing photoluminescent material distinct from or spaced from the light source characterised by the arrangement of the photoluminescent material
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01LSEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L33/00Semiconductor 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
    • H01L33/48Semiconductor 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
    • H01L33/50Wavelength conversion elements

Definitions

  • the present invention relates to a phosphor, a wavelength conversion member, and a lighting device.
  • a remote phosphor type lighting fixture in which a wavelength conversion member is arranged at a position separated from an LED that emits primary light by a predetermined distance has also been proposed (see, for example, Patent Document 1 and the like).
  • the area of the wavelength conversion member can be increased and the distance from a plurality of LEDs to the wavelength conversion member can be secured, so that the region excited by the light from one LED becomes wide. , Brightness unevenness and glare can be reduced.
  • the wavelength conversion member absorbs a part of natural light even when the luminaire is not lit. It will be colored with. This is particularly remarkable in a phosphor material that uses blue light or short-wavelength visible light as the primary light and emits yellow light as the secondary light.
  • a wavelength conversion member containing a YAG-based phosphor is entirely under natural light. It is recognized as being colored yellow.
  • the white LED which is a combination of the purple LED and the phosphor of each color of RGB, the appearance when not lit is orange.
  • a luminaire it is not preferable for a luminaire to have a non-white appearance when it is not lit, because it causes a difference in the color of the ceiling or wall surface to which the luminaire is attached and reduces the degree of freedom in design.
  • a sense of discomfort occurs because the distance from the user's head is short.
  • the phosphor of the present invention has a general formula of (M 2 x , M 3 y , M 4 z ) a (M 1 O 3 ) b X c (where M 1 is Si, One or more elements containing at least Si selected from the group consisting of Al, P and B, M 2 is one or more elements containing at least Ca selected from the group consisting of Ca, Mg, Ba and Zn, and M 3 is One or more elements containing at least Sr selected from the group consisting of Sr, Mg, Ba and Zn, M 4 is one or more elements containing at least Eu 2+ selected from the group consisting of rare earth elements and Mn 2+ , and X is It represents at least one halogen element mainly composed of Cl.
  • the phosphor of the present invention does not contain short-wavelength visible light such as blue or purple in the excitation band of the phosphor, it suppresses coloring due to absorption of visible light under natural light and has a good appearance even when not lit. Can be realized.
  • the wavelength conversion member of the present invention includes the above-mentioned phosphor and a medium that transmits visible light, and the said phosphor is contained in the said medium.
  • the medium contains a blue phosphor that is excited by ultraviolet light or short-wavelength visible light to emit blue light.
  • the lighting apparatus of the present invention includes the wavelength conversion member according to any one of the above, and a light source having an emission peak wavelength in the range of 365 to 400 nm.
  • the light source and the wavelength conversion member are arranged apart from each other.
  • the present invention can provide a phosphor, a wavelength conversion member, and a lighting device that can realize a good appearance even when not lit.
  • FIG. 5A shows the emission spectrum of Example 1
  • FIG. 5B shows the emission spectrum of Example 2
  • FIG. 5C shows the emission spectrum of Example 2.
  • the emission spectrum of Example 3 is shown.
  • FIG. 1 is a schematic cross-sectional view showing the lighting device 10 in the present embodiment.
  • the lighting device 10 includes a mounting substrate 11, a light emitting element 12, a phosphor layer 13, a yellow phosphor 14a, a blue phosphor 14b, and a side wall portion 15.
  • the mounting board 11 is a circuit board on which a conductive pattern is formed on the surface and a plurality of light emitting elements 12 are mounted to form a circuit.
  • the material constituting the mounting substrate 11 may be any material used as a normal printed wiring board, such as an insulating material such as glass epoxy resin, a metal plate having an insulating film formed on the front and back surfaces, and a flexible substrate. There may be.
  • the light emitting element 12 is an element mounted on a mounting substrate 11 and electrically connected to a wiring pattern to emit primary light by applying a voltage.
  • an LED chip or an LED package can be used.
  • the primary light emitted by the light emitting element 12 the wavelength from ultraviolet light of 365 to 400 nm to near ultraviolet light (short wavelength visible light) is preferable, and a known compound semiconductor material such as an InGaN system can be used.
  • the emission wavelength of the light emitting element 12 is 365 nm or less, the light emitting layer needs to be doped with Al in order to increase the band gap, which is not preferable because the luminous efficiency of the chip is extremely lowered.
  • the emission wavelength is 400 nm or more
  • the primary light absorption rate of the yellow phosphor 14a having a reduced Eu 2+ concentration which will be described later, decreases, and sufficient excitation intensity cannot be obtained, so that the emission color of the white LED shifts to blue. Therefore, it is not preferable.
  • the phosphor layer 13 is a plate-shaped member in which phosphor particles are dispersed in a medium, and corresponds to the wavelength conversion member in the present invention.
  • the resin material constituting the medium of the phosphor layer 13 is not particularly limited as long as it is a material that transmits primary light and secondary light, and silicone resin, glass, or the like can be used.
  • the phosphor layer 13 is arranged so as to face the mounting substrate 11 at a predetermined distance from the plurality of light emitting elements 12, and constitutes a remote phosphor type lighting device 10. doing.
  • the distance between the phosphor layer 13 and the light emitting element 12 is too close, uneven brightness will occur, and if it is too far, an overlapping region will appear due to the light emitted from the adjacent light emitting element 12, so it is appropriate depending on the purpose. It is preferable that the distance is large.
  • the yellow phosphor 14a is a phosphor according to the present invention, and is excited by the primary light of short wavelength visible light from the ultraviolet light emitted from the light emitting element 12, and emits yellow light as the secondary light.
  • the specific yellow phosphor 14a has a general formula of (M 2 x , M 3 y , M 4 z ) a (M 1 O 3 ) b X c (where M 1 is derived from Si, Al, P and B).
  • M 2 is one or more elements containing at least Ca selected from the group consisting of Ca, Mg, Ba and Zn
  • M 3 is Sr, Mg, Ba and At least one element containing at least Sr selected from the group consisting of Zn
  • M 4 is one or more elements containing at least Eu 2+ selected from the group consisting of rare earth elements and Mn 2+
  • X is at least Cl-based. It represents one kind of halogen element.
  • the absorption edge of the yellow phosphor 14a contains a wavelength in the blue region, which is not preferable because the appearance is colored light yellow.
  • the blue phosphor 14b is excited by the primary light of short wavelength visible light from the ultraviolet light emitted from the light emitting element 12, and emits blue light as the secondary light.
  • Specific examples of the blue phosphor 14b include BaMgAl 10 O 17 : Eu 2+ , Ca 10 (PO 4 ) 6 Cl 2 : Eu 2+ , Sr 10 (PO 4 ) 6 Cl 2 : Eu 2+ , (Sr, Ca) 10.
  • the side wall portion 15 is a frame-shaped member provided around the mounting substrate 11 and holding the phosphor layer 13. Although an example in which the side wall portion 15 is composed of a separate member is shown here, the mounting substrate 11 and the side wall portion 15 may be integrally formed.
  • the primary light emitted from the light emitting element 12 is incident on the phosphor layer 13, and at least a part of the primary light is dispersed in the phosphor layer 13 with the yellow phosphor 14a and the blue fluorescence.
  • the body 14b and the body 14b are wavelength-converted into secondary light, yellow light and blue light, respectively. Further, the yellow light and the blue light whose wavelengths are converted by the phosphor layer 13 are mixed and irradiated to the outside of the illuminating device 10 as white light.
  • FIG. 2 is a graph showing an emission spectrum of the lighting device 10 of the present embodiment.
  • (Ca 0.510 , Sr 0.484 , Eu 2 + 0.007 ) 7 (SiO 2 ) 6 Cl 2 is used as the yellow phosphor 14a
  • Ba 0.90 is used as the blue phosphor 14b.
  • MgAl 10 O 17 : Eu 2+ 0.10 is used.
  • the weight ratio of the yellow phosphor 14a to the blue phosphor 14b is 62:38, and the fluorescence is dispersed / defoamed in a transparent resin such as a silicone resin, an acrylic resin, a fluororesin, or an epoxy resin so as to be 10% by weight.
  • the body slurry was adjusted to mold the phosphor layer 13 having a thickness of 1 mm and cut into a size of 40 ⁇ 20 mm.
  • the phosphor layer 13 was fixed at a position where the distance from the mounting substrate 11 was 10 mm.
  • the light emitting element 12 10 surface mount type near-ultraviolet LED packages that emit light at 390 nm were used, and solder-mounted in 5 ⁇ 2 rows at 8 mm intervals on the aluminum substrate which is the mounting substrate 11.
  • a light emission spectrum as shown in FIG. 2 was obtained from the lighting device 10, and white light having a chromaticity (0.33, 0.34) and a luminous flux of 630 lm was obtained. Issued. Further, the appearance of the phosphor layer 13 was white when no light was emitted.
  • a plurality of yellow phosphors 14a of the present invention were prepared and their characteristics were evaluated.
  • H 2 / N 2 5/95 atmosphere
  • FIG. 3 is a graph showing the spectral diffuse reflectance of Examples 1 to 3 and Comparative Example. In the figure, the horizontal axis shows the wavelength and the vertical axis shows the diffuse reflectance.
  • the absorption edge at which the reflectance decreases is about 460 nm, and the diffuse reflection curve gradually decreases toward the short wavelength side from there. That is, the high reflectance is maintained in the blue region, and the reflectance is lowered and the absorptance is high in the near-ultraviolet light region where the luminosity factor is low. Therefore, it was confirmed that in Examples 1 to 3, most of the wavelengths in the visible light region with high luminosity factor were reflected, and the appearance was white even under natural light.
  • the absorption edge at which the reflectance decreases is about 490 nm, and the diffuse reflection curve gradually decreases toward the short wavelength side from there. That is, the reflectance is lowered even in the blue region of 445 to 500 nm, and the reflectance of visible light having higher luminosity factor than near-ultraviolet light is lowered and the absorption rate is high. Therefore, in the comparative example, since the wavelength of visible light in the blue region with high luminosity factor is absorbed, it was confirmed that the appearance is colored pale yellow under natural light.
  • FIG. 4 is a graph showing the excitation spectra of Examples 1 to 3 and Comparative Example.
  • Examples 1 to 3 the excitation band is shifted to the shorter wavelength side than in Comparative Examples, and visible light is reflected to show a white appearance. Further, also in Examples 1 to 3, it is suitable that the combination with the light emitting element 12 having an excitation band in the wavelength range of 365 to 400 nm, having an InGaN-based light emitting layer, and emitting primary light of 365 to 400 nm is suitable. Understand.
  • Examples 1 to 3 were measured using a spectrofluorometer. FP-8500DS manufactured by JASCO Corporation was used for the measurement.
  • 5A and 5B are graphs showing the emission spectra of Examples 1 to 3, FIG. 5A shows the emission spectrum of Example 1, and FIG. 5B shows the emission spectrum of Example 2.
  • FIG. (C) shows the emission spectrum of Example 3.
  • the excitation light short wavelength visible light having a wavelength of 395 nm was used.
  • the general formula is (M 2 x , M 3 y , M 4 z ) a (M 1 O 3 ) b X c (here, M) as the yellow phosphor 14a.
  • 1 is at least one element containing Si selected from the group consisting of Si, Al, P and B
  • M 2 is one or more elements containing at least Ca selected from the group consisting of Ca, Mg, Ba and Zn.
  • M 3 is at least one element containing at least Sr selected from the group consisting of Sr, Mg, Ba and Zn
  • M 4 is one or more elements containing at least Eu 2+ selected from the group consisting of rare earth elements and Mn 2+ .
  • the element, X represents at least one halogen element mainly composed of Cl.
  • a, b, and c are in the range satisfying 5 ⁇ a ⁇ 9, 5 ⁇ b ⁇ 9, 1 ⁇ c ⁇ 3.
  • FIG. 6 is a schematic cross-sectional view showing the LED package 20 in this embodiment. Since the LED package 20 of the present embodiment emits light when electric power is supplied, it corresponds to the lighting device of the present invention.
  • the LED package 20 of the present embodiment includes a housing portion 21, an LED chip 22, a phosphor layer 23, a yellow phosphor 24a, a blue phosphor 24b, a reflecting portion 25, and a through portion. It is a surface mount type having a hole 26 and an electrode 27.
  • the LED package 20 may be of a surface mount type in which the electrodes 27 are exposed on the back surface side of the housing portion 21, and other specific structures are not limited to those shown in FIG.
  • the housing portion 21 is a thin plate-shaped member on which the LED chip 22 is mounted, and is made of, for example, metal, ceramic, resin, or the like.
  • the LED chip 22 is mounted in the recess formed in the housing portion 21, and the phosphor layer 23 is filled in the recess to seal the LED chip 22.
  • the LED chip 22 emits primary light according to the electric power supplied from the outside through the electrode 27 and the through hole 26.
  • the phosphor layer 23 is a member that seals the LED chip 22 in a recess surrounded by the reflecting portion 25.
  • the yellow phosphor 24a and the blue phosphor 24b are dispersed in a medium such as a silicone resin or an epoxy resin. ing.
  • the phosphor layer 23 corresponds to the wavelength conversion member in the present invention.
  • the yellow phosphor 24a is a phosphor according to the present invention, and is excited by the primary light of short wavelength visible light from the ultraviolet light emitted from the LED chip 22, and emits yellow light as the secondary light. Specific examples of the yellow phosphor 24a are the same as those in the first embodiment.
  • the blue phosphor 24b is excited by the primary light of short wavelength visible light from the ultraviolet light emitted from the LED chip 22, and emits blue light as the secondary light. Specific examples of the blue phosphor 24b are the same as those in the first embodiment.
  • the reflecting portion 25 is provided on the housing portion 21 so as to surround the LED chip 22, and is a member that reflects the light from the LED chip 22.
  • FIG. 6 shows an example in which the reflecting portion 25 is integrally formed with the housing portion 21, each may be formed as a separate body and combined. Further, the LED package 20 may not be provided with the reflecting portion 25.
  • the through hole 26 is a through hole formed from the front surface to the back surface side of the housing portion 21, and the inside is filled with a conductive material.
  • the electrode 27 is an electrode provided on the back surface side of the housing portion 21, and constitutes an anode and a cathode of the LED package 20, respectively.
  • FIG. 6 shows an example in which the upper surface of the LED chip 22 and the through hole 26 are electrically connected by a wire. However, assuming that a wiring layer is formed on the surface side of the housing portion 21 and the LED chip 22 is flip-chip connected. May be good.
  • FIG. 7 is a graph showing the emission spectrum of the LED package 20 of the present embodiment.
  • (Ca 0.510 , Sr 0.481 , Eu 2 + 0.009 ) 7 (SiO 2 ) 6 Cl 2 is used as the yellow phosphor 24a, and Ca 9.92 is used as the blue phosphor 24b.
  • (PO 4 ) 6 Cl 2 : Eu 2+ 0.08 is used.
  • the weight ratio of the yellow phosphor 24a to the blue phosphor 24b is 55:45, and the fluorescence is dispersed / defoamed in a transparent resin such as a silicone resin, an acrylic resin, a fluororesin, or an epoxy resin so as to be 30% by weight.
  • the body slurry was adjusted.
  • an alumina substrate having outer dimensions of 3 mm in length and width and 0.8 mm in thickness was prepared as the housing portion 21, a recess having a diameter of 2 mm and a depth of 0.5 mm was formed, and a through hole 26 and a gold pad electrode were formed in the recess. And an electrode 27 was formed on the back surface side.
  • the LED chip 22 was mounted in the recess of the housing portion 21, and after wire bonding, the recess was filled with the phosphor slurry and cured to obtain the LED package 20.
  • an InGaN-based LED that emits light at 395 nm was used.
  • the general formula is (M 2 x , M 3 y , M 4 z ) a (M 1 O 3 ) b X c (where M 1 is Si, Al) as the yellow phosphor 14a.
  • P and at least one element containing Si selected from the group consisting of P and B M 2 is one or more elements containing at least Ca selected from the group consisting of Ca, Mg, Ba and Zn, and M 3 is Sr.
  • M 4 is one or more elements containing at least Eu 2+ selected from the group consisting of rare earth elements and Mn 2+
  • X is Cl.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Inorganic Chemistry (AREA)
  • Materials Engineering (AREA)
  • Organic Chemistry (AREA)
  • Microelectronics & Electronic Packaging (AREA)
  • Spectroscopy & Molecular Physics (AREA)
  • Physics & Mathematics (AREA)
  • General Engineering & Computer Science (AREA)
  • Manufacturing & Machinery (AREA)
  • Computer Hardware Design (AREA)
  • Power Engineering (AREA)
  • Luminescent Compositions (AREA)
  • Led Device Packages (AREA)

Abstract

L'invention concerne un matériau fluorescent représenté par la formule générale (M2 x,M3 y,M4 z)a(M1O3)bXc (où : M1 est au moins un type d'élément choisi dans le groupe constitué par Si, Al, P et B et comprend au moins du Si ; M2 représente au moins un type d'élément choisi dans le groupe constitué par Ca, Mg, Ba et Zn et comprend au moins du Ca ; M3 est au moins un type d'élément choisi dans le groupe constitué par Sr, Mg, Ba et Zn et comprend au moins du Sr ; M4 représente au moins un type d'élément choisi dans le groupe constitué par les éléments des terres rares et Mn2+ et comprend au moins de l'Eu2+ ; et X est au moins un type d'élément halogène et comprend principalement du Cl. De plus, les valeurs de a, b et c satisfont aux relations 5 < a < 9, 5 < b < 9 et 1 < c < 3 et les valeurs de x, y et z satisfont aux relations x+y+z = 1, 0 < x < 1, 0 < y < 1 et 0,003 < z < 0,01.)
PCT/JP2020/021435 2019-06-04 2020-05-29 Matériau fluorescent, élément de conversion de longueur d'onde et dispositif d'éclairage WO2020246395A1 (fr)

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JP2019-104160 2019-06-04
JP2019104160A JP2020196824A (ja) 2019-06-04 2019-06-04 蛍光体、波長変換部材および照明装置

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Citations (6)

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Publication number Priority date Publication date Assignee Title
JP2011057764A (ja) * 2009-09-07 2011-03-24 Nichia Corp 蛍光体及びそれを用いた発光装置並びに蛍光体の製造方法
JP2011057763A (ja) * 2009-09-07 2011-03-24 Nichia Corp 蛍光体及びそれを用いた発光装置並びに蛍光体の製造方法
WO2011077637A1 (fr) * 2009-12-21 2011-06-30 株式会社小糸製作所 Phosphore et dispositif électroluminescent
WO2011145238A1 (fr) * 2010-05-17 2011-11-24 株式会社小糸製作所 Dispositif d'éclairage
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JP2011057764A (ja) * 2009-09-07 2011-03-24 Nichia Corp 蛍光体及びそれを用いた発光装置並びに蛍光体の製造方法
JP2011057763A (ja) * 2009-09-07 2011-03-24 Nichia Corp 蛍光体及びそれを用いた発光装置並びに蛍光体の製造方法
WO2011077637A1 (fr) * 2009-12-21 2011-06-30 株式会社小糸製作所 Phosphore et dispositif électroluminescent
WO2011145238A1 (fr) * 2010-05-17 2011-11-24 株式会社小糸製作所 Dispositif d'éclairage
CN104194781A (zh) * 2014-07-25 2014-12-10 兰州大学 一种单一基质余辉颜色可调的长余辉发光材料及制备方法
JP2016157795A (ja) * 2015-02-24 2016-09-01 株式会社小糸製作所 発光モジュール

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WANYING GENG; ZHOU XUFENG; WANG YUHUA: "Potential single-phasedwhite-emitting phosphor(CaO.33SrO.67)7(Si03)6C12:Ce3+,Eu2+ forultraviolet light-emitting diode", RSC ADVANCES, vol. 6, 23 October 2016 (2016-10-23), pages 108964 - 108968, XP055770241 *

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