CN113227320A - Wavelength conversion member and light emitting device - Google Patents
Wavelength conversion member and light emitting device Download PDFInfo
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- CN113227320A CN113227320A CN201980086378.9A CN201980086378A CN113227320A CN 113227320 A CN113227320 A CN 113227320A CN 201980086378 A CN201980086378 A CN 201980086378A CN 113227320 A CN113227320 A CN 113227320A
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- wavelength conversion
- conversion member
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- phosphor particles
- wavelength
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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
- C09K11/02—Use of particular materials as binders, particle coatings or suspension media therefor
-
- C—CHEMISTRY; METALLURGY
- C03—GLASS; MINERAL OR SLAG WOOL
- C03C—CHEMICAL COMPOSITION OF GLASSES, GLAZES OR VITREOUS ENAMELS; SURFACE TREATMENT OF GLASS; SURFACE TREATMENT OF FIBRES OR FILAMENTS MADE FROM GLASS, MINERALS OR SLAGS; JOINING GLASS TO GLASS OR OTHER MATERIALS
- C03C3/00—Glass compositions
- C03C3/04—Glass compositions containing silica
- C03C3/076—Glass compositions containing silica with 40% to 90% silica, by weight
- C03C3/089—Glass compositions containing silica with 40% to 90% silica, by weight containing boron
-
- C—CHEMISTRY; METALLURGY
- C03—GLASS; MINERAL OR SLAG WOOL
- C03C—CHEMICAL COMPOSITION OF GLASSES, GLAZES OR VITREOUS ENAMELS; SURFACE TREATMENT OF GLASS; SURFACE TREATMENT OF FIBRES OR FILAMENTS MADE FROM GLASS, MINERALS OR SLAGS; JOINING GLASS TO GLASS OR OTHER MATERIALS
- C03C3/00—Glass compositions
- C03C3/12—Silica-free oxide glass compositions
- C03C3/16—Silica-free oxide glass compositions containing phosphorus
-
- C—CHEMISTRY; METALLURGY
- C03—GLASS; MINERAL OR SLAG WOOL
- C03C—CHEMICAL COMPOSITION OF GLASSES, GLAZES OR VITREOUS ENAMELS; SURFACE TREATMENT OF GLASS; SURFACE TREATMENT OF FIBRES OR FILAMENTS MADE FROM GLASS, MINERALS OR SLAGS; JOINING GLASS TO GLASS OR OTHER MATERIALS
- C03C4/00—Compositions for glass with special properties
- C03C4/12—Compositions for glass with special properties for luminescent glass; for fluorescent glass
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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
- C09K11/7706—Aluminates
-
- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F21—LIGHTING
- F21V—FUNCTIONAL FEATURES OR DETAILS OF LIGHTING DEVICES OR SYSTEMS THEREOF; STRUCTURAL COMBINATIONS OF LIGHTING DEVICES WITH OTHER ARTICLES, NOT OTHERWISE PROVIDED FOR
- F21V9/00—Elements for modifying spectral properties, polarisation or intensity of the light emitted, e.g. filters
- F21V9/30—Elements containing photoluminescent material distinct from or spaced from the light source
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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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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F21—LIGHTING
- F21Y—INDEXING SCHEME ASSOCIATED WITH SUBCLASSES F21K, F21L, F21S and F21V, RELATING TO THE FORM OR THE KIND OF THE LIGHT SOURCES OR OF THE COLOUR OF THE LIGHT EMITTED
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- F21Y2115/30—Semiconductor lasers
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- G02B5/00—Optical elements other than lenses
- G02B5/02—Diffusing elements; Afocal elements
- G02B5/0205—Diffusing elements; Afocal elements characterised by the diffusing properties
- G02B5/0236—Diffusing elements; Afocal elements characterised by the diffusing properties the diffusion taking place within the volume of the element
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- G—PHYSICS
- G02—OPTICS
- G02B—OPTICAL ELEMENTS, SYSTEMS OR APPARATUS
- G02B5/00—Optical elements other than lenses
- G02B5/02—Diffusing elements; Afocal elements
- G02B5/0273—Diffusing elements; Afocal elements characterized by the use
- G02B5/0294—Diffusing elements; Afocal elements characterized by the use adapted to provide an additional optical effect, e.g. anti-reflection or filter
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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
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- 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
- H01S5/005—Optical components external to the laser cavity, specially adapted therefor, e.g. for homogenisation or merging of the beams or for manipulating laser pulses, e.g. pulse shaping
- H01S5/0087—Optical components external to the laser cavity, specially adapted therefor, e.g. for homogenisation or merging of the beams or for manipulating laser pulses, e.g. pulse shaping for illuminating phosphorescent or fluorescent materials, e.g. using optical arrangements specifically adapted for guiding or shaping laser beams illuminating these materials
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Abstract
The purpose of the present invention is to provide a wavelength conversion member and a light-emitting device having high emission intensity. A wavelength conversion member (10) comprising a matrix (1) and phosphor particles (2), wherein the wavelength conversion member (10) has a haze value of 0.7 to 0.999 in a visible light wavelength region in which the spectral intensity in the excitation spectrum of the phosphor particles (2) is 5% or less of the maximum peak intensity.
Description
Technical Field
The present invention relates to a wavelength conversion member and a Light Emitting device that convert the wavelength of Light emitted from a Light Emitting Diode (LED), a Laser Diode (LD), or the like into another wavelength.
Background
In recent years, as a next-generation light emitting device that replaces a fluorescent lamp or an incandescent lamp, attention has been increasingly focused on a light emitting device using an LED or an LD from the viewpoints of low power consumption, small size, light weight, and easy light amount adjustment. As an example of such a next-generation light-emitting device, a light-emitting device in which a wavelength conversion member that absorbs a part of blue light and converts the blue light into yellow light is disposed on an LED that emits blue light is disclosed (patent documents 1 and 2). These light emitting devices emit white light as a composite light of blue light (excitation light) emitted from the LED and yellow light (fluorescence) emitted from the wavelength conversion member.
Documents of the prior art
Patent document
Patent document 1: japanese laid-open patent publication No. 2000-208815
Patent document 2: japanese patent laid-open publication No. 2003-258308
Disclosure of Invention
Technical problem to be solved by the invention
In recent years, with the enhancement of the performance of light emitting devices, wavelength conversion members capable of extracting white light of higher intensity have been demanded. However, the conventional wavelength conversion member has a problem that the light flux value of the combined light of the excitation light and the fluorescence taken out to the outside is insufficient, and the emission intensity cannot be sufficiently increased.
In view of the above circumstances, an object of the present invention is to provide a wavelength conversion member and a light emitting device having high emission intensity.
Technical solution for solving technical problem
As a result of intensive studies, the inventors of the present invention have found that the beam value of the combined light of the excitation light and the fluorescence extracted from the wavelength conversion member can be improved by adjusting the haze value of the wavelength conversion member in the specific wavelength region.
That is, the wavelength conversion member of the present invention is a wavelength conversion member containing phosphor particles in a matrix, and is characterized in that the wavelength conversion member has a haze value of 0.7 to 0.999 in a visible light wavelength region where the spectral intensity in the excitation spectrum of the phosphor particles is 5% or less of the maximum peak intensity.
The wavelength converting member of the present invention preferably has a substrate of glass.
The wavelength conversion member of the present invention may be a wavelength conversion member in which phosphor particles absorb a part of fluorescence. When such phosphor particles are used, the effects of the present invention can be easily obtained.
The wavelength conversion member of the present invention is preferably such that the phosphor particles are garnet-based ceramic phosphor particles.
The wavelength converting member of the present invention preferably contains a scattering material.
The wavelength conversion member of the present invention preferably has a thickness of 1000 μm or less.
The light-emitting device of the present invention includes the wavelength conversion member and a light source for irradiating the wavelength conversion member with excitation light.
The light emitting device of the present invention preferably has a light source of a light emitting diode or a laser diode.
ADVANTAGEOUS EFFECTS OF INVENTION
According to the present invention, a wavelength conversion member and a light-emitting device having high emission intensity can be provided.
Drawings
Fig. 1 is a schematic cross-sectional view showing a wavelength conversion member according to an embodiment of the present invention.
Fig. 2 is a diagram illustrating a decrease in the beam value of the combined light of the wavelength conversion member having a high haze value.
Fig. 3 is a diagram illustrating a decrease in the beam value of the combined light of the wavelength conversion member having a low haze value.
Fig. 4 is a schematic diagram showing an excitation spectrum and a fluorescence spectrum of YAG phosphor particles.
Fig. 5 is a schematic cross-sectional view showing a light-emitting device according to an embodiment of the present invention.
FIG. 6 is a graph showing the relationship between relative beam value and haze for the examples of the present invention.
Detailed Description
Hereinafter, embodiments of the present invention will be described in detail with reference to the drawings. However, the present invention is not limited to the following embodiments.
(wavelength conversion member 10)
Fig. 1 is a schematic cross-sectional view showing a wavelength conversion member according to an embodiment of the present invention. As shown in fig. 1, the wavelength conversion member 10 contains phosphor particles 2 in a matrix 1. And has a first main surface 11 and a second main surface 12.
As shown in fig. 1, the excitation light a emitted from the light source 6 enters the wavelength conversion member 10 from the second main surface 12 side of the wavelength conversion member 10. The phosphor particles 2 are irradiated with the excitation light a, and the fluorescence is emitted. Then, the combined light B of the excitation light a and the fluorescence is emitted from the first main surface 11 side of the wavelength conversion member 10.
The wavelength conversion member 10 has a haze value of 0.7 to 0.999 in a visible light wavelength region where the spectral intensity in the excitation spectrum of the phosphor particles 2 is 5% or less of the maximum peak intensity. In the present invention, the visible light region represents a region of 380nm to 780 nm. The haze value is calculated from the values of the total light transmittance and the diffuse transmittance in the visible light wavelength region by the following equation.
Haze value ═ (diffuse transmittance)/(total light transmittance)
As a result of intensive studies, the inventors of the present invention have found that, in the wavelength conversion member 10 containing the phosphor particles 2 in the matrix 1, the beam value of the combined light B extracted from the first main surface 11 can be improved by adjusting the haze value in the visible light wavelength region in which the spectral intensity in the excitation spectrum of the phosphor particles 2 is 5% or less of the maximum peak intensity. The mechanism thereof is explained as follows.
Fig. 2 is a diagram illustrating a decrease in the beam value of the combined light of the wavelength conversion member having a high haze value. The wavelength conversion member 20 shown in fig. 2 contains phosphor particles 2 and a scattering material 3 in a matrix 1. Also, the scattering material 3 has a high haze value because of its high content. In the wavelength conversion member 20, the excitation light a and the fluorescence C are excessively scattered by the scattering material 3 and easily become the return light D. Therefore, the combined light B is difficult to be emitted from the first main surface 11, and the beam value of the combined light B is likely to decrease.
In view of the above problems, the present invention limits the upper limit of the haze value. Specifically, the upper limit of the haze value of the wavelength conversion member 10 is 0.999 or less, preferably 0.995 or less, and particularly preferably 0.99 or less. This arrangement can suppress excessive scattering of the excitation light a and the fluorescence C, and can suppress a decrease in the beam value of the combined light B emitted from the first main surface 11.
Fig. 3 is a diagram illustrating a decrease in the beam value of the combined light of the wavelength conversion member having a low haze value. The wavelength conversion member 30 shown in fig. 3 contains phosphor particles 2 in a matrix 1 without containing a scattering material 3, and thus has a low haze value. In general, in the wavelength conversion member 30 not including the scattering material 3, the excitation light a is not easily scattered in the matrix 1, and therefore the amount of the excitation light a irradiated per unit area of the phosphor particles 2 is relatively small, and the intensity of the emitted fluorescence is easily decreased. Therefore, in the wavelength conversion member 30, the content of the phosphor particles 2 is increased in order to obtain a desired chromaticity. However, if the content of the phosphor particles 2 becomes large, so-called fluorescence re-absorption in which the phosphor particles 2 themselves absorb a part of the fluorescence tends to occur. That is, as shown in fig. 3, the fluorescence C emitted from the phosphor particle 2a is absorbed by another phosphor particle 2b existing in the vicinity of the phosphor particle 2a, and is emitted from the phosphor particle 2b again as the fluorescence E. Further, since energy loss accompanying wavelength conversion occurs, the intensity of fluorescence E is lower than that of fluorescence C. Therefore, if the fluorescence re-absorption occurs, the intensity of the fluorescence emitted from the first main surface 11 decreases, and the beam value of the combined light B decreases.
In view of the above, the present invention limits the lower limit of the haze value. Specifically, the lower limit of the haze value of the wavelength conversion member 10 is 0.7, preferably 0.75 or more, and particularly preferably 0.80 or more. This arrangement can suppress the re-absorption of fluorescence and suppress the decrease in the beam value of the combined light B emitted from the first main surface 11.
In the present invention, the haze value is measured in a visible light wavelength region where the spectral intensity in the excitation spectrum of the phosphor particles 2 is 5% or less of the maximum peak intensity. The visible light region is 380nm to 780 nm. The excitation spectrum is a spectrum indicating a mode in which the fluorescence intensity of the phosphor at a specific wavelength (monitor wavelength) changes when the wavelength of the excitation light is changed. The monitoring wavelength can be any wavelength, but a wavelength at which the fluorescence intensity of the phosphor particles 2 is maximized is usually selected.
For example, if the phosphor particles 2 are irradiated with light having a wavelength at which the spectral intensity of the excitation spectrum becomes maximum, the fluorescence intensity at the monitor wavelength emitted from the phosphor particles 2 becomes maximum because the excitation probability of the phosphor particles 2 is high. On the other hand, if the phosphor particles 2 are irradiated with light having a wavelength with a small spectral intensity, the excitation probability of the phosphor particles 2 becomes low, and the fluorescence intensity becomes small. Further, if the phosphor particles 2 are irradiated with light having a wavelength with a smaller spectral intensity, the phosphor particles 2 are not excited and do not emit fluorescence.
Fig. 4 is a schematic diagram showing an excitation spectrum and a fluorescence spectrum of YAG phosphor particles. The broken line indicates the excitation spectrum (monitoring wavelength: 555nm), and the solid line indicates the fluorescence spectrum. The emission intensities of the excitation spectrum and the fluorescence spectrum are represented by relative values when the maximum spectral intensity of each spectrum is 1. As shown in FIG. 4, the YAG phosphor particles have an excitation spectrum at a wavelength of 380nm to 540 nm. Therefore, in this wavelength region, absorption typified by fluorescence reabsorption occurs. In the wavelength region where absorption occurs, there is a problem that the spectral shapes of the total light transmittance and the diffuse transmittance are likely to vary due to the influence of a scattering factor described later, and it is difficult to obtain the correlation between the haze value and the emission intensity.
On the other hand, as described above, even when the phosphor particles 2 are irradiated with light in a wavelength region where the spectral intensity of the excitation spectrum is sufficiently small, the phosphor particles 2 are hardly excited, and the fluorescence is hardly emitted. Accordingly, in the present invention, a visible light wavelength region (540 nm to 780nm in fig. 4) having a maximum peak intensity of 5% or less in the excitation spectrum is defined as the wavelength region. Further, the present inventors have found that the correlation between the haze value and the beam value can be obtained without the influence of absorption or the like in the wavelength region, and have completed the present invention.
The haze value may be 0.7 to 0.999 in a part of a visible light wavelength region having a maximum peak intensity of 5% or less in the excitation spectrum, but it is particularly preferable that the haze value is satisfied in the entire wavelength region.
The shape of the wavelength conversion member 10 is not particularly limited, and is generally a plate shape (rectangular plate shape, disk shape, or the like). The thickness of the wavelength conversion member 10 can be appropriately selected so as to obtain a target chromaticity, and specifically, is preferably 1000 μm or less, more preferably 800 μm or less, and particularly preferably 500 μm or less. If the thickness is too large, the beam value of the combined light B may decrease. The lower limit of the thickness of the wavelength conversion member 10 is preferably about 50 μm. If the thickness is too small, the mechanical strength is liable to be lowered.
The chromaticity of the wavelength conversion member 10 is not particularly limited, and when YAG phosphor particles that emit yellow light are used as the phosphor particles 2 and blue light (having a central wavelength of about 450nm) is used as the excitation light a, it is preferable that the synthesized light B emitted from the wavelength conversion member 10 has the chromaticity shown below. Specifically, the chromaticity (Cx) measured by a spectroscope by condensing the synthesized light B when the excitation light a is irradiated to the wavelength conversion member 10 provided in the opening of the integrating sphere is preferably 0.22 to 0.44, more preferably 0.23 to 0.37, and particularly preferably 0.24 to 0.33. If the chromaticity of the combined light B is too low, the proportion of blue light becomes too high, and it becomes difficult to obtain a desired color matching. In this case, too, the amount of the phosphor particles 2 added is often small, and it is difficult to obtain a predetermined haze value. On the other hand, if the chromaticity of the combined light B is too high, the proportion of yellow light becomes too high, and it becomes difficult to obtain a desired color matching. In this case, the amount of addition of the phosphor particles 2 is often large, and the light flux value tends to be low due to the influence of fluorescence reabsorption.
The total light transmittance of the wavelength conversion member 10 is preferably 20% or more, more preferably 30% or more, and particularly preferably 40% or more in the visible light wavelength region in which the maximum peak intensity in the excitation spectrum of the phosphor particles 2 is 5% or less. If the total light transmittance is too low, the luminous flux value of the combined light B emitted from the first main surface 11 is excessively reduced, and the emission intensity of the wavelength conversion member 10 is reduced.
In the present invention, the haze value can be adjusted to an arbitrary value by changing the scattering factor constituting the wavelength conversion member 10. Specifically, the refractive index of the matrix 1, the contents of the phosphor particles 2 and the scattering material 3, the particle diameter, the refractive index, and the like can be changed to adjust. Hereinafter, each scattering factor will be described in detail.
(substrate 1)
The matrix 1 of the present invention can contain the phosphor particles 2 therein, and is not particularly limited as long as it is a transparent material that transmits the excitation light a and the synthesized light B. For example, resin or glass can be used. From the viewpoint of obtaining the wavelength conversion member 10 having high heat resistance and weather resistance, glass is preferably used. In addition, from the viewpoint of obtaining a lightweight wavelength conversion member 10, a resin is preferably used.
Examples of the glass include SiO2-B2O3Glass, SiO2-B2O3-RO (RO is an alkali metal oxide) glass, SnO-P2O5Is made of glass, TeO2Glass series and Bi2O3Glass, etc.
SiO2-B2O3The glass preferably contains SiO in mol% as a composition 2 30～80％、B2O3 1～40％、MgO 0～10％、CaO 0～30％、SrO 0～20％、BaO0～40％、MgO+CaO+SrO+BaO 5～45％、Al2O3 0～20％、ZnO 0～20％。
In addition, SiO2-B2O3The RO glass preferably contains SiO in mol% as a composition2 70～90％、B2O39～25％、Li2O 0～5％、Na2O 0～5％、K2O 0～5％、Li2O+Na2O+K2O 0.1～5％、Al2O3 0～5％、MgO 0～5％、CaO+SrO+BaO 0～5％。
As SnO-P2O5The glass composition preferably contains SnO 35-80% and P in mol%2O5 5～40％、B2O3 0～30％。
As the resin, for example, a light-transmitting thermoplastic resin, a thermosetting resin, or an ultraviolet curable resin can be used. Specifically, polyvinyl chloride, polyvinylidene chloride, polyethylene terephthalate, polyvinyl alcohol, polystyrene, polycarbonate, acrylic resin, melamine resin, epoxy resin, or the like can be used. In particular, polycarbonate and acrylic resin are preferably used in view of excellent light transmittance.
The refractive index (nd) of the substrate 1 is preferably 1.3 to 2.2, more preferably 1.4 to 2.1, still more preferably 1.45 to 2.05, still more preferably 1.5 to 2, and particularly preferably 1.55 to 1.95. This makes it easy to suppress excessive scattering at the interface between the phosphor particles 2 and the matrix 1, and to adjust the haze value of the wavelength conversion member 10.
As described later, the form of the matrix 1 is not particularly limited as long as the phosphor particles 2 are contained therein. For example, when the wavelength conversion member 10 includes a sintered body of glass powder and phosphor particles 2, the matrix 1 includes a sintered body of glass powder. Average particle diameter (D) of glass powder50) Preferably 0.1 to 50 μm, 0.5 to 40 μm, and particularly preferably 1 to 30 μm. If the average particle diameter (D)50) If the particle size is too small, the influence of the particle boundary, which is one of the scattering factors, tends to be large, and the haze value may become too high. On the other hand, if the average particle diameter (D)50) If the size is too large, the phosphor particles 2 are difficult to be uniformly dispersed in the matrix 1, and the chromaticity of the combined light B tends to be nonuniform.
(phosphor particle 2)
The phosphor particles 2 may be particles that absorb a part of the fluorescence, and in this case, the effect of the present invention can be easily obtained. Here, "absorb a part of fluorescence" means that the excitation wavelength region overlaps with the emission wavelength region, and specifically, as shown in fig. 4, means that the excitation spectrum overlaps with the fluorescence spectrum in a wavelength region where the maximum peak intensity of the excitation spectrum is 5% or more.
The phosphor particles 2 have a peak of an excitation spectrum wavelength at a wavelength of 300 to 500nm, preferably have a light emission peak at a wavelength of 380 to 780nm, and particularly preferably are garnet-based ceramic phosphor particles such as YAG (yttrium-aluminum garnet) phosphor particles. The phosphor particles 2 are not limited to the above, and examples of the phosphor particles include oxides, nitrides, oxynitrides, sulfides, oxysulfides, rare earth sulfides, aluminate chlorides, and halophosphoric acid chlorides.
The content of the phosphor particles 2 in the wavelength conversion member 10 is preferably 0.01 to 30% by volume, more preferably 0.1 to 20% by volume, and particularly preferably 1 to 15% by volume. If the content is too large, the fluorescence reabsorption is likely to occur, and the emission intensity of the wavelength conversion member 10 is likely to decrease. If the content is too small, the color of the combined light B tends to be inhomogeneous, and it is difficult to obtain a desired chromaticity.
Average particle diameter (D) of phosphor particles 250) Preferably 0.001 to 50 μm, more preferably 0.1 to 30 μm, and particularly preferably 1 to 30 μm. If the average particle diameter of the phosphor particles 2 is too small, the phosphor particles 2 are likely to aggregate with each other, and chromaticity of the combined light B may become uneven. Further, scattering tends to become excessive, and the haze value may become too high. If the average particle size is too large, it is difficult to uniformly disperse the phosphor particles 2 in the matrix 1, and the chromaticity of the combined light B may be uneven.
In the present invention, the average particle diameter (D) of the particles in the form of powder50) Means a value measured by a laser diffraction method, and indicates that the cumulative particle size distribution curve of the volume basis measured by the laser diffraction method has a cumulative amount from the smaller side of the particlesStarting to accumulate to a particle size of 50%. On the other hand, the particle diameter of the particles in the wavelength conversion member 10 (for example, the average particle diameter of the phosphor particles 2 dispersed in the matrix 1) can be measured using, for example, an X-ray CT scanner or the like. In this case, the cumulative particle size distribution curve based on the volume measured by CT scanning means a particle size in which the cumulative amount is 50% cumulative from the smaller side of the particles.
The refractive index (nd) of the phosphor particles 2 is not particularly limited, and in general, the refractive index of the phosphor particle 2 powder is often higher than the refractive index of the resin or glass that becomes the matrix 1. For example, borosilicate glass has a refractive index of about 1.5 to 1.6, while YAG phosphor particles have a refractive index of about 1.83. If the refractive index difference between the phosphor particles 2 and the matrix 1 is too large, the ratio of the excitation light a reflected at the interface between the phosphor particles 2 and the matrix 1 becomes large, and the haze value tends to become too high. Therefore, the difference in refractive index between the matrix 1 and the phosphor particles 2 is preferably 0.5 or less, more preferably 0.4 or less, more preferably 0.3 or less, and particularly preferably 0.25 or less. This makes it easy to suppress excessive scattering at the interface between the phosphor particles 2 and the matrix 1, and to adjust the haze value of the wavelength conversion member 10. Of course, the refractive index difference is not limited to the above.
In addition, the range of the preferable haze value for maximizing the light flux value is related to the refractive index difference between the matrix 1 and the phosphor particles 2. Specifically, the refractive index difference and haze value between the matrix 1 and the phosphor particles 2 are preferably controlled as follows.
(1) When the difference between the refractive index of the matrix 1 and the refractive index of the phosphor particles 2 is 0.5 to 0.35, the haze value is preferably 0.7 to 0.99, more preferably 0.72 to 0.9, and particularly preferably 0.7 to 0.85.
(2) When the difference between the refractive index of the matrix 1 and the refractive index of the phosphor particles 2 is less than 0.35 to 0.25, the haze value is preferably 0.7 to 0.99, more preferably 0.75 to 0.95, and particularly preferably 0.8 to 0.9.
(3) When the difference in refractive index between the matrix 1 and the phosphor particles 2 is less than 0.25, the haze value is preferably 0.7 to 0.999, more preferably 0.8 to 0.995, and particularly preferably 0.9 to 0.99.
(Scattering Material 3)
The wavelength converting member 10 of the present invention preferably contains a scattering material 3. The scattering material 3 is not particularly limited, and inorganic particles such as ceramic powder or glass powder can be used. Ceramic powders are particularly preferably used. Since the thermal diffusivity of the ceramic powder is generally greater than that of a transparent material such as resin or glass constituting the matrix 1, heat generated when the fluorescent particles 2 fluoresce can be efficiently dissipated to the outside of the wavelength conversion member 10, and thermal degradation of the fluorescent particles 2 can be suppressed. The glass powder is preferable in that the fine adjustment of the refractive index is easy, and thus the haze value of the wavelength conversion member 10 can be easily and precisely adjusted.
Examples of the ceramic powder include silicon dioxide, boron nitride, aluminum oxide, magnesium oxide, titanium oxide, niobium oxide, and zinc oxide.
As the glass powder, for example, a multicomponent glass, a single component glass such as silica glass, or the like can be used. In addition, when the mixture of the matrix 1 and the scattering material 3 is heated in the manufacturing process of the wavelength conversion member 10 described later, if the glass powder as the scattering material 3 softens and flows, the particle diameter may change, and it may be difficult to obtain a desired haze value. Therefore, the softening point of the glass powder is preferably higher than the softening point of the substrate 1 by 30 ℃ or more, more preferably higher by 50 ℃ or more, and particularly preferably higher by 100 ℃ or more.
The content of the scattering material 3 in the wavelength conversion member 10 is preferably 0 to 50% by volume, more preferably 0.01 to 40% by volume, still more preferably 0.1 to 10% by volume, and particularly preferably 1 to 5% by volume. If the content is too large, the haze value of the wavelength conversion member 10 becomes too high, and the emission intensity tends to decrease. In addition, the total light transmittance of the wavelength conversion member 10 may be excessively reduced.
Average particle diameter (D) of the scattering material 350) Preferably 0.1 to 100. mu.m, more preferably 0.3 to 50 μm, and particularly preferably 1 to 30 μm. If the average particle diameter (D) of the scattering material 350) If it is too small, the haze value tends to be too high. In addition, since scattering tends to become excessive, the haze value may become excessively high. On the other hand, if averagedParticle size (D)50) If the amount is too large, the scattering material 3 is not easily dispersed uniformly in the matrix 1, and the chromaticity of the combined light B may be non-uniform.
The shape of the light diffusing material 3 is not particularly limited, and examples thereof include a spherical shape, a crushed shape, a hollow shape, a rod shape, and a fiber shape.
The difference in refractive index between the scattering material 3 and the matrix 1 is preferably 0.5 or less, more preferably 0.4 or less, and particularly preferably 0.3 or less. With this arrangement, excessive scattering at the interface between the scattering material 3 and the matrix 1 can be easily suppressed, and the haze value of the wavelength conversion member 10 can be easily adjusted. Of course, the refractive index difference is not limited to the above range.
The density difference between the phosphor particles 2 and the matrix 1 is preferably 4 or less, 3.5 or less, and particularly preferably 3 or less. If the density difference is too large, the phosphor particles 2 are difficult to be uniformly dispersed in the matrix 1, and the chromaticity of the combined light B tends to be nonuniform. The density difference between the scattering material 3 and the matrix 1 is preferably 4 or less, 3.5 or less, and particularly preferably 3 or less. If the density difference is too large, the scattering material 3 is difficult to be uniformly dispersed in the matrix 1, and the chromaticity of the combined light B tends to be non-uniform.
In addition to the scattering factors described above, voids, grain boundaries, texture, and the like in the wavelength conversion member 10 also affect the haze value as scattering factors. When glass is used as the matrix 1, crystals may be precipitated in a manufacturing process of the wavelength conversion member 10 described later, and the crystals may also serve as a scattering factor. It can also be adjusted to any haze value by taking these scattering factors into account.
The void ratio of the wavelength conversion member 10 is preferably 5% or less, more preferably 3% or less, and particularly preferably 1% or less by volume%. If the void ratio is too large, light is scattered at the boundary between the void and the matrix 1, and thus scattering tends to become excessive.
When the substrate 1 is glass, the crystal precipitated inside is preferably 30% or less, more preferably 25% or less, and particularly preferably 20% or less by volume% with respect to the substrate 1. If the amount of the crystal is too large, light scattering becomes excessive, and the emission intensity of the wavelength conversion member 10 tends to decrease. In addition, the total light transmittance of the wavelength conversion member 10 may be excessively reduced.
The porosity and the volume% of crystals can be measured by using a CT scanner.
The wavelength conversion member 10 is not particularly limited as long as it has a structure in which the phosphor particles 2 are contained in the matrix 1. For example, the wavelength conversion member 10 can be obtained by mixing and firing glass powder and the phosphor particles 2 (and the scattering material 3 if necessary). In particular, it is preferable that the wavelength conversion member 10 is obtained by pressing a mixture of the glass powder and the phosphor particles 2 to produce a preform and then firing the preform. On the other hand, in the sintered body of the glass powder and the phosphor particles 2, the influence of the grain boundary, which is one of the scattering factors, tends to be large. Therefore, from the viewpoint of producing the wavelength conversion member 10 with a small influence of grain boundaries, it is preferable to produce the wavelength conversion member 10 by incorporating the phosphor particles 2 in a liquid or semisolid resin and then curing the resin.
(light-emitting device)
Fig. 5 is a schematic cross-sectional view showing a light-emitting device according to an embodiment of the present invention. As shown in fig. 5, the light emitting device 50 has a wavelength conversion member 10 and a light source 6. In the present embodiment, the light source 6 is disposed so that the excitation light a enters the second main surface 12. The excitation light a emitted from the light source 6 is converted into fluorescence having a wavelength longer than that of the excitation light a by the wavelength conversion member 10. In addition, a part of the excitation light a passes through the wavelength conversion member 10. Therefore, the wavelength conversion member 10 emits the combined light B of the excitation light a and the fluorescence. For example, when the excitation light a is blue light and the fluorescence is yellow light, the white synthesized light B can be obtained.
The light source 6 may be an LED or an LD, and an LD capable of emitting light of high intensity is preferably used from the viewpoint of increasing the light emission intensity of the light emitting device 50. In the present embodiment, the light source 6 is disposed in a state of being separated from the wavelength conversion member 10, but is not limited to this configuration. For example, the light source 6 may be in direct contact with the wavelength conversion member 10 or may be bonded to the wavelength conversion member via an adhesive layer.
Examples
Hereinafter, the wavelength conversion member of the present invention will be described in detail using examples, but the present invention is not limited to the following examples.
Tables 1 to 3 show examples (Nos. 1 to 6 and 9 to 23) and comparative examples (Nos. 7 and 8) of the present invention.
[ Table 1]
[ Table 2]
[ Table 3]
Examples (Nos. 1 to 6, 9 to 23) and comparative examples (Nos. 7 and 8) were produced as follows. First, a mixture was obtained by mixing a matrix, phosphor particles, and a scattering material as needed so as to have the contents shown in tables 1 to 3. The following materials were used. In table 1, the volume concentration (%) indicates the volume concentration occupied in the total volume of the matrix, the phosphor particles and the scattering material.
(a) Substrate
Glass A powder-borosilicate glass (SiO)2-B2O3Glass), refractive index (nd): 1.58, density: 3.1g/cm3Average particle diameter D50: 2.5 μm, softening point: 850 deg.C
Glass B powder-alkali borosilicate glass (SiO)2-B2O3RO glass), refractive index (nd): 1.46, density: 2.1g/cm3Average particle diameter D50: 2.5 μm, softening point: 825 deg.C
Resin C — photocurable resin, refractive index (nd): 1.58, density: 2.4g/cm3
Resin D-silicone resin, refractive index (nd): 1.46, density: 2.0g/cm3
Resin E — photocurable resin, refractive index (nd): 1.51, density: 2.4g/cm3
(b) Phosphor particle YAG-Y3Al5O12Refractive index (nd): 1.82, average particle diameter D50: 25 μm, density: 4.8g/cm3
(c) Scattering material alumina-Al2O3Average particle diameter D50: 1 μm, density: 4.0g/cm3
In Nos. 1 to 7 and 9 to 18, the mixture was placed in a mold, pressed at a pressure of 0.20MPa to obtain a preform, and then fired in the vicinity of the softening point of the glass to produce a glass sintered body.
In Nos. 8 and 20 to 23, the mixture was placed in a mold, and then irradiated with ultraviolet light (central wavelength of 405nm) to be cured, thereby producing a cured resin body.
In No.19, the mixture was placed in a mold, and then heated to 40 ℃ to be cured, thereby producing a cured resin body.
By grinding and polishing the glass sintered body and the cured resin body, a wavelength conversion member having a rectangular plate shape with a thickness of 200 μm was obtained in Nos. 1 to 13 and 20 to 23, and a wavelength conversion member having a rectangular plate shape with a thickness of 180 μm was obtained in Nos. 14 to 19.
The obtained wavelength conversion member was evaluated for haze value, luminous flux value, and chromaticity by the following methods.
Haze value Using a Nihon spectrophotometer V-670, the total light transmittance and the diffusion transmittance were measured, and the haze value at a wavelength of 600nm was calculated by the following equation. The phosphor used in the present example had an excitation spectrum with a spectral intensity of 5% or less of the maximum peak intensity at a wavelength of 600 nm.
Haze value ═ (diffuse transmittance)/(total light transmittance)
The luminous flux value and chromaticity are measured by irradiating excitation light from a light source and condensing the light emitted from the wavelength conversion member by an integrating sphere. A blue LED (maximum peak of excitation spectrum: 450nm) was used as a light source, and the output was fixed. The measurement apparatus used a Hamamatsu photonics spectrometer PMA-12. The light flux values were represented by relative values, with the value of example No.6 showing the highest value among examples (Nos. 1 to 6 and 9 to 23) and comparative examples (Nos. 7 and 8) being 1, and the remaining values being represented by examples 6.
Fig. 6 is a graph obtained by plotting the haze value and the relative beam value for each sample.
As shown in tables 1 to 3 and FIG. 6, in examples (Nos. 1 to 6, 9 to 23), wavelength conversion members having high luminous flux values and high emission intensities were obtained. Specifically, the relative beam value is 0.95 or more.
Description of the symbols
1: a substrate; 2: phosphor particles; 2 a: phosphor particles; 2 b: phosphor particles; 3: a scattering material; 6: a light source; 10: a wavelength conversion member; 11: a first major face; 12: a second major face; 20: a wavelength conversion member; 30: a wavelength conversion member; 50: a light emitting device; a: exciting light; b: synthesizing light; c: fluorescence; d: returning light; e: fluorescence.
Claims (8)
1. A wavelength conversion member comprising a matrix and phosphor particles contained therein, characterized in that:
the wavelength conversion member has a haze value of 0.7 to 0.999 in a visible light wavelength region where a spectral intensity in an excitation spectrum of the phosphor particles is 5% or less of a maximum peak intensity.
2. The wavelength converting member according to claim 1, wherein:
the substrate is glass.
3. The wavelength converting member according to claim 1 or 2, wherein:
the phosphor particles absorb a portion of the fluorescence.
4. The wavelength conversion member according to any one of claims 1 to 3, wherein:
the phosphor particles are garnet-based ceramic phosphor particles.
5. The wavelength conversion member according to any one of claims 1 to 4, wherein:
containing a scattering material.
6. The wavelength conversion member according to any one of claims 1 to 5, wherein:
the wavelength conversion member has a thickness of 1000 [ mu ] m or less.
7. A light-emitting device, comprising:
the wavelength conversion member according to any one of claims 1 to 6, and a light source for irradiating the wavelength conversion member with excitation light.
8. The light-emitting apparatus according to claim 7, wherein:
the light source is a light emitting diode or a laser diode.
Applications Claiming Priority (5)
| Application Number | Priority Date | Filing Date | Title |
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| JP2018-244763 | 2018-12-27 | ||
| JP2018244763 | 2018-12-27 | ||
| JP2019225084A JP2020106831A (en) | 2018-12-27 | 2019-12-13 | Wavelength conversion member and light-emitting device |
| JP2019-225084 | 2019-12-13 | ||
| PCT/JP2019/049764 WO2020137780A1 (en) | 2018-12-27 | 2019-12-19 | Wavelength conversion member and light emitting device |
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| CN113227320A true CN113227320A (en) | 2021-08-06 |
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| CN (1) | CN113227320A (en) |
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| JP2011222751A (en) * | 2010-04-09 | 2011-11-04 | Nippon Electric Glass Co Ltd | Wavelength conversion member and semiconductor light-emitting element device having and using the wavelength conversion member |
| CN102299237A (en) * | 2010-06-22 | 2011-12-28 | 日东电工株式会社 | Semiconductor light emitting device |
| CN102347423A (en) * | 2010-07-27 | 2012-02-08 | 日东电工株式会社 | Component for light-emitting device, light-emitting device and producing method thereof |
| JP2013197325A (en) * | 2012-03-21 | 2013-09-30 | Nippon Electric Glass Co Ltd | Wavelength conversion member and light-emitting device |
| CN107430303A (en) * | 2015-04-02 | 2017-12-01 | 凸版印刷株式会社 | Quantum dot diaphragm and use wavelength conversion sheet and back light unit obtained from it |
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| TW383508B (en) | 1996-07-29 | 2000-03-01 | Nichia Kagaku Kogyo Kk | Light emitting device and display |
| JP4158012B2 (en) | 2002-03-06 | 2008-10-01 | 日本電気硝子株式会社 | Luminescent color conversion member |
| JP5519440B2 (en) * | 2010-08-03 | 2014-06-11 | 日東電工株式会社 | Light emitting device |
| JP6134176B2 (en) * | 2013-03-22 | 2017-05-24 | スタンレー電気株式会社 | Light emitting device and manufacturing method thereof |
| KR101966672B1 (en) * | 2017-03-22 | 2019-04-09 | 신화인터텍 주식회사 | Wavelength converting member and display device including the same |
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2019
- 2019-12-13 JP JP2019225084A patent/JP2020106831A/en active Pending
- 2019-12-19 CN CN201980086378.9A patent/CN113227320A/en active Pending
- 2019-12-19 DE DE112019006473.8T patent/DE112019006473T5/en active Pending
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Patent Citations (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2011222751A (en) * | 2010-04-09 | 2011-11-04 | Nippon Electric Glass Co Ltd | Wavelength conversion member and semiconductor light-emitting element device having and using the wavelength conversion member |
| CN102299237A (en) * | 2010-06-22 | 2011-12-28 | 日东电工株式会社 | Semiconductor light emitting device |
| CN102347423A (en) * | 2010-07-27 | 2012-02-08 | 日东电工株式会社 | Component for light-emitting device, light-emitting device and producing method thereof |
| JP2013197325A (en) * | 2012-03-21 | 2013-09-30 | Nippon Electric Glass Co Ltd | Wavelength conversion member and light-emitting device |
| CN107430303A (en) * | 2015-04-02 | 2017-12-01 | 凸版印刷株式会社 | Quantum dot diaphragm and use wavelength conversion sheet and back light unit obtained from it |
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| TW202033745A (en) | 2020-09-16 |
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