WO2018079373A1 - Light wavelength conversion member and light emission device - Google Patents

Abstract

A light wavelength conversion member which can achieve both high fluorescence intensity and high color homogeneity, and a light emission device are provided. In this light wavelength conversion member 1, A and B in A₃B₅O₁₂ are at least one element selected from the following element groups: A: Sc, Y, lanthanoids (except Ce) B: Al, Ga From N A₃B₅O₁₂:Ce crystal grains in a 20μm square cross-section of a ceramic sintered body, defining a as the number thereof that are present inside of an Al₂O₃ crystal grain, b as the number thereof present on an Al₂O₃ grain boundary without touching another A₃B₅O₁₂:Ce crystal grain, and c as the number present on an Al₂O₃ grain boundary and touching one or more other A₃B₅O₁₂:Ce crystal grains, and defining X, Y and Z as the ratios of said numbers to the total, i.e., a/N, b/N, c/N, respectively, the ratios satisfy the following ranges. 0% ≤ X ≤ 25% 9% ≤ Y ≤ 45% 48% ≤ Z ≤ 90%

Description

Light wavelength conversion member and light emitting device

The present invention relates to an optical wavelength conversion member capable of converting the wavelength of light and a light emitting device including the optical wavelength conversion member.

Conventionally, white lighting equipment that uses light emitting diodes (LEDs: Light Emitting Diodes) and semiconductor lasers (LDs: Laser Diodes) as light sources combines blue LEDs or blue LDs with yellow phosphors that are complementary to blue to produce white light. The obtained lighting equipment is mainstream. *

Resin-based, glass-based, and ceramic-based materials are known as the material of this phosphor, but in recent years, the phosphor tends to increase in temperature due to higher output of the light source, and the ceramic-based phosphor with high durability. Development is underway. *

For example, a garnet-type ceramic represented by the chemical formula A ₃ B ₅ O ₁₂ is often used as the ceramic phosphor. In particular, yttrium aluminum garnet (YAG: Y ₃ Al ₅ O ₁₂ ) exhibits yellow fluorescence when a cerium (Ce) element is added as an activator.

In the following prior arts (Patent Documents 1 to 3), YAG: Ce or Lu ₃ Al ₅ O ₁₂ : Ce (LuAG: Ce) is dispersed and precipitated in alumina (Al ₂ O ₃ ) having excellent thermal conductivity. Thus, a ceramic composite with improved durability has been proposed.

Specifically, in Patent Documents 1 to 3, the balance between color unevenness and thermal conductivity is controlled by the volume ratio of Al ₂ O ₃ / A ₃ B ₅ O ₁₂ : Ce. For example, in Patent Document 1, the amount of YAG: Ce is set to 22 to 55 vol% of the whole. When the amount is less than 22 vol%, blue light is transmitted more, unevenness of color occurs, and when it exceeds 55 vol%, the thermal conductivity is increased. It is said that the durability will decrease.

In Patent Document 2, the LuAG: Ce amount is 25 to 95 vol%. Furthermore, in Patent Document 3, the amount of A ₃ B ₅ O ₁₂ : Ce is 20 to 25 vol%. Moreover, in Patent Document 3, in order to suppress the volatilization of Ce during firing, CeAl ₁₁ O ₁₈ is contained as 0.5 to 5 vol% as a Ce supply source.

Japanese Patent No. 5088977 Japanese Patent No. 5153014 Japanese Patent No. 5740017

However, in these prior arts, since the garnet-based fluorescent component is deposited in Al ₂ O ₃ without particularly controlling the crystal structure, in other words, high color homogeneity is achieved so as not to cause color unevenness in the volume ratio. Is to be obtained. For this reason, important characteristics as an original phosphor such as fluorescence intensity and translucency are impaired, and it cannot be said that sufficient fluorescence characteristics can be exhibited.

In addition, CeAl ₁₁ O ₁₈ in Patent Document 3 does not have both fluorescence and translucency, and therefore is a factor that further impairs the above-described fluorescence characteristics by being contained in the sintered body. This invention is made | formed in view of the said subject, The objective is to provide the light wavelength conversion member and light-emitting device which can make high fluorescence intensity and high color homogeneity compatible.

(1) A first aspect of the present invention is a ceramic sintered body which is a polycrystalline body mainly composed of Al ₂ O ₃ crystal particles and crystal particles of a component represented by the chemical formula A ₃ B ₅ O ₁₂ : Ce. It is related with the optical wavelength conversion member comprised from these.

In this light wavelength conversion member, A and B in A ₃ B ₅ O ₁₂ are at least one element selected from the following element group. A: Sc, Y, lanthanoid (excluding Ce)















B: Al, Ga















Moreover, among the N A ₃ B ₅ O ₁₂ : Ce crystal particles in the 20 μm square range of the cut surface of the ceramic sintered body, the number of those existing in the Al ₂ O ₃ crystal particles is a, and other A ₃ The number of B ₅ O ₁₂ : B existing in the Al ₂ O ₃ crystal grain boundary without being in contact with the Ce crystal grain is b, and one or more other A ₃ B ₅ O ₁₂ : Ce crystal grains are in contact with the Al ₂ When the number of O ₃ crystal grain boundaries is c, and the total ratios a / N, b / N, and c / N with respect to the respective numbers are X, Y, and Z, the ratios are within the following ranges. Satisfies.

0% ≦ X ≦ 25%















9% ≦ Y ≦ 45%















48% ≦ Z ≦ 90%















As described above, since the light wavelength conversion member of the first aspect has the above-described configuration, high fluorescence intensity and high color homogeneity (that is, less color unevenness, as will be apparent from experimental examples described later). ) Can be realized. Details will be described below.

Since the A ₃ B ₅ O ₁₂ : Ce crystal particles corresponding to X are completely taken into the Al ₂ O ₃ crystal particles, the volatilization of Ce can be suppressed. As a result, stable fluorescence without color unevenness is exhibited without causing a difference in Ce concentration.

Here, when X is more than 25%, the ratio (Y) of A ₃ B ₅ O ₁₂ : Ce crystal particles existing alone in the Al ₂ O ₃ crystal grain boundary decreases, and the grain growth of Al ₂ O ₃ occurs. As a result, the so-called pinning effect does not work, and Al ₂ O ₃ grows and the permeability is lowered, resulting in a decrease in fluorescence intensity. When X is less than 1%, color unevenness tends to increase.

By the Y is in the above range, the pinning effect is exerted against the _Al 2 _{O 3,} grain growth of _Al 2 _{O 3} is suppressed. As a result, it is possible to obtain a sufficient translucency for extracting fluorescence.

Here, if Y is less than 9%, the pinning effect is not sufficiently exhibited, causing Al ₂ O ₃ grain growth, resulting in a decrease in fluorescence intensity due to insufficient permeability, and further due to coarsening of the grains Color unevenness is likely to occur. On the other hand, when Y is more than 45%, light dispersion at the Al ₂ O ₃ / A ₃ B ₅ O ₁₂ : Ce grain boundary increases, and the translucency decreases, resulting in a decrease in fluorescence intensity.

Since light dispersion does not occur at the A ₃ B ₅ O ₁₂ : Ce / A ₃ B ₅ O ₁₂ : Ce grain boundary, the Z is in the above range, so that sufficient transparency can be taken out. Have. Here, when Z is less than 48%, the fluorescence intensity is reduced due to insufficient translucency. On the other hand, if Z is more than 90%, the translucency becomes too high, and the amount of transmitted excitation light increases, resulting in color unevenness. Moreover, it becomes difficult to form a connection path between the Al ₂ O ₃ crystal particles, and the thermal conductivity is lowered.

Therefore, by setting the ranges of X, Y, and Z to the ranges described above, high fluorescence intensity and high color homogeneity can be realized. Moreover, since the light wavelength conversion member of the first aspect has high thermal conductivity due to the above-described configuration, even when the light source has a high output, it is possible to suppress the influence of heat, for example, light Disappearance can be prevented. *

Furthermore, since this light wavelength conversion member is a ceramic sintered body, its strength is high, and even when light is repeatedly irradiated from a light source, its performance is not easily deteriorated, and furthermore, weather resistance is also excellent. There is an advantage. *

(2) In the second aspect of the present invention, the proportion of A ₃ B ₅ O ₁₂ : Ce crystal particles in the ceramic sintered body is 5 to 50 vol%. In the second aspect, since the ratio of A ₃ B ₅ O ₁₂ : Ce crystal particles is 5 to 50 vol%, there is an advantage that sufficient fluorescence intensity can be obtained as will be apparent from the experimental examples described later. .

(3) In a third aspect of the present invention, the ratio of Ce is less 10.0 mol% relative to A of _A 3 _B 5 _{O 12} (where not including 0). In the third aspect, since the ratio of Ce is 10.0 mol% or less (excluding 0) with respect to A of A ₃ B ₅ O ₁₂ , sufficient fluorescence is obtained as will be apparent from the experimental examples described later. There is an advantage that strength can be obtained.

(4) In the fourth aspect of the present invention, the average crystal grain size of Al ₂ O ₃ crystal particles is 0.3 to 10 μm, and the average crystal grain size of A ₃ B ₅ O ₁₂ : Ce crystal particles is 0.3 to 5 μm. It is. In the fourth aspect, the average crystal grain size of Al ₂ O ₃ crystal particles is 0.3 to 10 μm, and the average crystal grain size of A ₃ B ₅ O ₁₂ : Ce crystal particles is 0.3 to 5 μm. As is clear from the experimental examples, there is an advantage that sufficient fluorescence intensity and appropriate translucency can be obtained.

This means that in the case of the average crystal grain size described above, it becomes easier to achieve the crystal grain state including the ratios of X, Y, and Z in the first aspect. (5) A fifth aspect of the present invention is a light emitting device including the light wavelength conversion member according to any one of the first to fourth aspects. *

The light whose wavelength is converted by the light emitting device of the fifth aspect (specifically, the light wavelength conversion member) (that is, fluorescence) has high fluorescence intensity and high color homogeneity. In addition, as a light emitting element of the light emitting device, a known element such as an LED or an LD can be used. *

<Each configuration of the present invention will be described below>

The “light wavelength conversion member” is a ceramic sintered body having the above-described configuration, and a grain boundary of each crystal particle includes a part of components constituting each crystal particle and inevitable impurities. Also good.

The “main component” indicates that the crystal particle is present in the largest amount (volume) in the light wavelength conversion member.

-The above "A ₃ B ₅ O ₁₂ : Ce" indicates that Ce is a solid solution substitution in a part of A in A ₃ B ₅ O _12. By having such a structure, The compound exhibits fluorescence characteristics.

The “cut surface of the light wavelength conversion member” is at least one cut surface in a portion where light is transmitted. For example, when a plurality of (for example, five) cut surfaces are observed, the average values satisfy X, Y, and Z can be employed. Moreover, when calculating | requiring X, Y, Z in multiple places (for example, 5 places) in each cut surface, the average value is employable.

In addition, in order to make said X, Y, and Z into the said range, as mentioned later, it is necessary to make the amount of dispersing agents and baking conditions into appropriate conditions. For example, if the firing temperature is too low, X decreases, which is not preferable. Further, if the amount of the dispersant is too large, Y decreases, and if it is too small, Z increases, so it is necessary to set the conditions appropriately.

It is the schematic of the structure | tissue of the light wavelength conversion member of embodiment. It is sectional drawing which shows the cross section which fractured | ruptured the light-emitting device in the thickness direction.

Next, embodiments of the light wavelength conversion member and the light emitting device of the present invention will be described.















[1. Embodiment]















[1-1. Configuration of optical wavelength conversion member]















First, the light wavelength conversion member of the embodiment will be described. As shown in FIG. 1, the light wavelength conversion member 1 (see FIG. 2) of the embodiment is, for example, a plate-like ceramic sintered body, and has Al ₂ O ₃ crystal particles and a chemical formula A ₃ B ₅ O ₁₂ : Ce. It is composed of a polycrystal having a main component of crystal particles (hereinafter also referred to as A ₃ B ₅ O ₁₂ : Ce crystal particles) of the components represented.

In this light wavelength conversion member 1, A and B in A ₃ B ₅ O ₁₂ are at least one element selected from the following element group.

A: Sc, Y, lanthanoid (excluding Ce)















B: Al, Ga















Moreover, among the N A ₃ B ₅ O ₁₂ : Ce crystal particles in the 20 μm square range of the cut surface of the ceramic sintered body, the number of those existing in the Al ₂ O ₃ crystal particles is a, and other A ₃ The number of B ₅ O ₁₂ : B existing in the Al ₂ O ₃ crystal grain boundary without being in contact with the Ce crystal grain is b, and one or more other A ₃ B ₅ O ₁₂ : Ce crystal grains are in contact with the Al ₂ When the number of O ₃ crystal grain boundaries is c, and the total ratios a / N, b / N, and c / N with respect to the respective numbers are X, Y, and Z, the ratios are within the following ranges. Satisfies.

0% ≦ X ≦ 25%















9% ≦ Y ≦ 45%















48% ≦ Z ≦ 90%















In FIG. 1, the one corresponding to a (and hence X), that is, the A ₃ B ₅ O ₁₂ : Ce crystal particle in the Al ₂ O ₃ crystal particle is indicated by Ka. Further, the crystal grains corresponding to b (and therefore Y), that is, A ₃ B ₅ O ₁₂ : Ce particles present alone at the Al ₂ O ₃ grain boundary are indicated by Kb. Further, those corresponding to c (hence Z), i.e. _Al 2 _O 3 more than one _A in ₃ grain boundary _B 5 _O 12: contact with Ce crystal grains _A 3 _B 5 _O 12: Ce, crystal grains, Kc Is shown.

In the present embodiment, 5 to 50 vol% can be adopted as the ratio of A ₃ B ₅ O ₁₂ : Ce crystal particles in the ceramic sintered body. Furthermore, in this embodiment, the ratio of Ce can be 10.0 mol% or less (excluding 0) with respect to A of A ₃ B ₅ O ₁₂ .

Moreover, in this embodiment, the average crystal grain size of Al ₂ O ₃ crystal particles is 0.3 to 10 μm, and the average crystal grain size of A ₃ B ₅ O ₁₂ : Ce crystal particles is 0.3 to 5 μm. it can. [1-2. Configuration of Light Emitting Device] As illustrated in FIG. 2, the light emitting device 3 includes a box-shaped ceramic package (container) 5 such as alumina, and a light emitting element 7 such as an LD disposed inside the container 5. And a plate-shaped optical wavelength conversion member 1 disposed so as to cover the opening 9 of the container 5.

In the light emitting device 3, the light emitted from the light emitting element 7 is transmitted through the light wavelength conversion member 1, and a part of the light is wavelength-converted inside the light wavelength conversion member 1 to emit light. That is, the light wavelength conversion member 1 emits fluorescence having a wavelength different from the wavelength of the light emitted from the light emitting element 7.

[1-3. effect]















Next, effects of the embodiment will be described.

As described above, the light wavelength conversion member 1 of the present embodiment defines the ratios of X, Y, and Z, so that high fluorescence intensity and high color homogeneity can be realized.

Moreover, since the light wavelength conversion member 1 of the present embodiment has high thermal conductivity, even when the output of the light source is increased, the influence of heat can be suppressed, for example, loss of light can be prevented. it can.

Furthermore, since the light wavelength conversion member 1 of the present embodiment is a ceramic sintered body, the strength is high, and even when light is repeatedly irradiated from the light source, the performance is not easily deteriorated, and in addition, the weather resistance is improved. Also has the advantage of being superior. *

Further, when the ratio of A ₃ B ₅ O ₁₂ : Ce crystal particles is 5 to 50 vol%, there is an advantage that sufficient fluorescence intensity can be obtained.

Furthermore, when the ratio of Ce is 10.0 mol% or less (excluding 0) with respect to A of A ₃ B ₅ O ₁₂ , there is an advantage that sufficient fluorescence intensity can be obtained.

In addition, when the average crystal grain size of Al ₂ O ₃ crystal particles is 0.3 to 10 μm and the average crystal grain size of A ₃ B ₅ O ₁₂ : Ce crystal particles is 0.3 to 5 μm, sufficient fluorescence intensity is obtained. There is an advantage that moderate translucency can be obtained.

Therefore, the light emitting device 3 including the light wavelength conversion member 1 has an effect of generating fluorescence having high fluorescence intensity and high color uniformity.

[2. Example]















Next, specific examples will be described.

<Example 1>















Under the conditions shown in Table 1 and Table 2 below, No. 1 to 9 ceramic sintered body samples were prepared. Of the samples, Nos. 1 to 9 are samples within the scope of the present invention.

Specifically, for each sample, the ratio of YAG (Y ₃ Al ₅ O ₁₂ ) in the ceramic sintered body (that is, the ceramic sintered body constituting the light wavelength conversion member) is 21 vol%. In addition, Al ₂ O ₃ (average particle size 0.3 μm), Y ₂ O ₃ (average particle size 1.2 μm), CeO ₂ (average particle size) so that the Ce concentration is 1 mol% with respect to Y in YAG. Diameter 1.5 μm).

This was put into a ball mill together with pure water and a predetermined amount of a dispersant (2 wt% in terms of solid matter with respect to the raw material powder), and pulverized and mixed for 12 hours. The obtained slurry was dried and granulated, and a molded product was produced using the granulated product. The molded body was fired in the air under normal pressure at a firing temperature of 1450 ° C. to 1750 ° C. and a holding time of 3 to 20 hours. As a result, No. 1 to 9 ceramic sintered body samples (for example, plate-like samples) were obtained. *

As the dispersant, for example, a polycarboxylic acid-based dispersant, SN Dispersant 5468 manufactured by San Nopco, or Marialim AKM-0531 manufactured by Nippon Oil & Fats Co., Ltd. can be used. *

Next, the following characteristics (a) to (f) of the obtained ceramic sintered body were investigated in the same manner as in other examples described later. The results are shown in Table 2 below.

(A) Relative density















The relative density of the obtained ceramic sintered body was calculated by a method of measuring the density by the Archimedes method and converting the measured density into a relative density.

(B) Average crystal grain size















The sample (sample) was mirror-polished and then thermally etched at 1300 ° C. The etched surface was observed with a scanning electron microscope (that is, SEM observation), and an image of 5000 times an arbitrary portion in the ceramic sintered body was obtained. In addition, as an arbitrary location, when a sample is a rectangular plate shape, for example, the center position seen from the thickness direction which is a part which light permeate | transmits (in planar view) is mentioned.

Then, an arbitrary line is drawn in a 20 μm square in the image at the above position (for example, see FIG. 1), and the average crystal grain size of the Al ₂ O ₃ crystal particles and the A ₃ B ₅ O ₁₂ : Ce crystal particles by the intercept method. Asked.

(C) Particle number ratio X, Y, Z















Similar to (b) above, the sample was mirror-polished and then thermally etched at 1300 ° C. The etched surface was observed with an SEM to obtain a 5000 times larger image of an arbitrary portion in the ceramic sintered body. The number of particles a, b, and c in a 20 μm square in the image was counted, and the ratios X, Y, and Z were calculated. The same process was performed for any five visual fields, and the average values of X, Y, and Z were obtained. In addition, the surface regarding this after grinding | polishing corresponds to the cut surface of this invention.

(D) Fluorescence intensity















A sample processed to 13 mm square x 0.5 mm thickness is irradiated with blue LD light having a wavelength of 465 nm to a width of 0.5 mm with a lens, and the transmitted light is condensed with a lens. The emission intensity was measured. At this time, the output power density was set to 40 W / mm ² . The strength was evaluated by a relative value when the strength of the YAG: Ce single crystal was 100.

(E) Color unevenness















Color unevenness (that is, color variation) was evaluated by measuring chromaticity variation with an illuminometer. For a sample processed to 20 mm square x 0.5 mm thickness, blue LD light having a wavelength of 465 nm is condensed by a lens to a width of 0.5 mm, and the color of light transmitted from the opposite surface is irradiated with this light. The chromaticity was measured with a luminometer.

Irradiation was carried out by setting an 18 mm square region at the center of the irradiation surface (sample surface) of the sample, and performing 3 mm intervals in the region, and evaluating the variation (ΔX) in the chromaticity (X direction). Here, the variation (ΔX) is the maximum value of deviation of chromaticity (X direction). *

The chromaticity is an international display method established in 1931 by the International Commission on Illumination (CIE) and is a chromaticity represented by the CIE-XYZ color system. That is, the chromaticity is represented by an xy chromaticity diagram (so-called CIE chromaticity diagram) in which the three primary colors on the color are digitized and the colors are expressed in the xy coordinate space. *

(F) Thermal conductivity















The thermal conductivity of the sample processed to 10 mm square x 2 mm thickness was measured. The specific method conformed to JIS R1611.

Of the results obtained for each sample as described above, the fluorescence intensity, color unevenness, and thermal conductivity can be evaluated according to the following evaluation criteria. Other examples can be similarly evaluated. *

About fluorescence intensity, 110 or more are preferable, 100 or more and less than 110 are a little preferable, and less than 100 is considered unpreferable. Regarding color unevenness, ΔX <0.02 is preferable, 0.02 ≦ ΔX <0.06 is slightly preferable, and 0.06 ≦ ΔX is not preferable. *

About thermal conductivity, 20 W / m * K or more is preferable and less than 20 W / m * K is considered unpreferable. In the following, with respect to the first embodiment, evaluation based on the evaluation criteria will be described. *

In any sample of Example 1, the relative density was 99% or more, and the sample was sufficiently densified. The average crystal grain size of Al ₂ O ₃ (referred to as Al ₂ O ₃ grain size in Table 2) is in the range of 0.3 to 10 μm, and the average crystal of A ₃ B ₅ O ₁₂ : Ce (YAG: Ce) It was found that the particle size (referred to as A ₃ B ₅ O ₁₂ particle size in Table 2) was in the range of 0.3-5 μm.

Nos. 3 to 9 in which X, Y, and Z are within the scope of the present invention had good results in all of fluorescence intensity, color unevenness, and thermal conductivity. In addition, No. 1 and 2 (with a lower firing temperature than the other samples) within the scope of the present invention showed more uneven color than the other Nos. 3 to 9. *

<Example 2>















As shown in Tables 1 and 2 below, ceramic sintered body samples (Nos. 10 to 15) were prepared by the same manufacturing method as in Example 1, and evaluated in the same manner.

However, the amount of the dispersant was changed in the range of 1.8 to 5 wt% and the firing time was changed in the range of 5 to 20 hours during the preparation. Of the samples, Nos. 11 to 14 are samples within the scope of the present invention, and Nos. 10 and 15 are samples outside the scope of the present invention (comparative example). *

As a result, all samples were sufficiently densified with a relative density of 99% or more. Further, except for No. 10, the average crystal grain size of Al ₂ O ₃ is in the range of 0.3 to 10 μm, and the average crystal grain size of A ₃ B ₅ O ₁₂ : Ce (YAG: Ce) is 0.3 As can be seen from Table 2 below, Nos. 11 to 14 in which X, Y, and Z are within the range of the present invention have a fluorescence intensity, color unevenness, and heat conduction. Both rates gave good results. On the other hand, No. 10 with less Y had a slightly coarse Al ₂ O ₃ average crystal grain size of 11 μm, slightly reduced fluorescence intensity, and increased color unevenness. Further, in No. 15 with a large amount of Y and a small amount of Z, the fluorescence intensity was lower than 100.

<Example 3>















As shown in Tables 1 and 2 below, samples of ceramic sintered bodies (samples Nos. 16 to 20) were prepared by the same manufacturing method as in Example 1 and evaluated in the same manner.

However, the amount of the dispersant was changed in the range of 0 to 1.5 wt% during the preparation. Of the samples, Nos. 16 to 19 are samples within the scope of the present invention, and No. 20 is a sample outside the scope of the present invention (comparative example). *

As a result, all samples were sufficiently densified with a relative density of 99% or more. It was also found that the average crystal grain size of Al ₂ O ₃ was 0.3 to 10 μm, and the average crystal grain size of A ₃ B ₅ O ₁₂ : Ce (YAG: Ce) was 0.3 to 5 μm.

Further, as apparent from Table 2 below, Nos. 16 to 19 in which X, Y, and Z are within the scope of the present invention showed good results in all of fluorescence intensity, color unevenness, and thermal conductivity. On the other hand, No. 20 having a small amount of Y and a large amount of Z had a slightly low fluorescence intensity, a large color unevenness, and a low thermal conductivity. *

<Example 4>















As shown in Table 1 and Table 2 below, a ceramic sintered body sample (No. 21 to 28 within the scope of the present invention) was prepared and evaluated in the same manner as in Example 1. went.

However, the raw material compounding ratio was changed so that the amount of A ₃ B ₅ O ₁₂ : Ce (YAG: Ce amount) in the ceramic sintered body was 1 to 60 vol%. As a result, all samples were sufficiently densified with a relative density of 99% or more. The average crystal grain size of Al ₂ O ₃ is in the range of 0.3 to 10 μm, and the average crystal grain size of A ₃ B ₅ O ₁₂ : Ce (YAG: Ce) is in the range of 0.3 to 5 μm. I understood that.

Further, as is apparent from Table 2 below, Nos. 23 to 27 in which the YAG: Ce amount is in a predetermined range (ie, 5 to 50 vol%) have good results in all of the fluorescence intensity, color unevenness, and thermal conductivity. It became. On the other hand, Nos. 21 and 22 with a small amount of YAG: Ce had slightly lower fluorescence intensity and slightly increased color unevenness. Further, No. 28 having a large amount of YAG: Ce had a slightly low fluorescence intensity and a low thermal conductivity. *

<Example 5>















As shown in Table 1 and Table 2 below, a ceramic sintered body sample (No. 29 to 38 within the scope of the present invention) was prepared and evaluated in the same manner as in Example 1. went.

However, the raw material mixture ratio was changed so that the Ce concentration with respect to Y in A ₃ B ₅ O ₁₂ (YAG) of the sintered body was 0 to 15 mol%.

As a result, all samples were sufficiently densified with a relative density of 99% or more. The average crystal grain size of Al ₂ O ₃ is in the range of 0.3 to 10 μm, and the average crystal grain size of A ₃ B ₅ O ₁₂ : Ce (YAG: Ce) is in the range of 0.3 to 5 μm. I understood that.

Further, as is apparent from Table 2 below, Nos. 30 to 37 in which the Ce concentration is within a predetermined range (that is, 10.0 mol% or less (excluding 0)) are fluorescent intensity, color unevenness, and thermal conductivity. Both of these showed good results. On the other hand, No. 29 containing no Ce could not measure both fluorescence intensity and color unevenness. Further, No. 38 having a high Ce concentration had a slightly low fluorescence intensity. *

<Example 6>















As shown in Table 1 and Table 2 below, a sintered ceramic sample (No. 39 to 59 within the scope of the present invention) was prepared and evaluated in the same manner as in Example 1. went.

However, not only Y ₂ O ₃ powder at the time of preparation, but also Lu ₂ O ₃ (average particle size 1.3 μm) or Yb ₂ O ₃ (average particle size 1.5 μm), Gd ₂ O ₃ (average particle size 1.5 μm) ), Tb ₂ O ₃ (average particle size: 1.6 μm), and Ga ₂ O ₃ (average particle size: 1.3 μm), one or more powders may be used to synthesize predetermined A ₃ B ₅ O ₁₂ : Ce The blending ratio was changed.

As a result, all samples were sufficiently densified with a relative density of 99% or more. The average crystal grain size of Al ₂ O ₃ is in the range of 0.3 to 10 μm, and the average crystal grain size of A ₃ B ₅ O ₁₂ : Ce (YAG: Ce) is in the range of 0.3 to 5 μm. I understood that.

In all ceramic sintered bodies, good results were obtained in all of the fluorescence intensity, color unevenness, and thermal conductivity. *

[3. Other Embodiments]















It goes without saying that the present invention is not limited to the above-described embodiment, and can be implemented in various modes without departing from the present invention.

(1) For example, in the above embodiment, the atmospheric pressure firing method in the air was used as the firing method, but in addition, a vacuum atmosphere firing method, a reducing atmosphere firing method, a hot press (HP) method, hot isotropy, etc. A sample having equivalent performance can also be produced by a pressure and pressure (HIP) method or a firing method combining these methods. *

(2) Examples of uses of the light wavelength conversion member and the light emitting device include various uses such as phosphors, light wavelength conversion devices, headlamps, illumination, and optical devices such as projectors.

(3) In addition, the function which one component in the said embodiment has may be shared by a some component, or the function which a some component has may be exhibited by one component. Moreover, you may abbreviate | omit a part of structure of the said embodiment. In addition, at least a part of the configuration of the above embodiment may be added to or replaced with the configuration of another embodiment. In addition, all the aspects included in the technical idea specified from the wording described in the claims are embodiments of the present invention.

1 ... Light wavelength conversion member















3. Light emitting device















7 Light emitting element

Claims (5)

1. 
   
   
   
   
   
   
   
   
   
   
   
   
   
   
   A light wavelength conversion member composed of a ceramic sintered body that is a polycrystalline body mainly composed of Al ₂ O ₃ crystal particles and crystal particles of a component represented by the chemical formula A ₃ B ₅ O ₁₂ : Ce. A and B in the A ₃ B ₅ O ₁₂ are at least one element selected from the following element group:
   
   
   
   
   
   
   
   
   
   
   
   
   
   
   
   A: Sc, Y, lanthanoid (excluding Ce)
   
   
   
   
   
   
   
   
   
   
   
   
   
   
   
   B: Al, Ga
   
   
   
   
   
   
   
   
   
   
   
   
   
   
   
   In addition, among the A ₃ B ₅ O ₁₂ : Ce crystal particles N in the 20 μm square range of the cut surface of the ceramic sintered body, the number of those existing in the Al ₂ O ₃ crystal particles is a, and others The number of those existing in the Al ₂ O ₃ crystal grain boundary without being in contact with the A ₃ B ₅ O ₁₂ : Ce crystal particle is one, and one or more other A ₃ B ₅ O ₁₂ : Ce crystal particles When the number of those in contact with the Al ₂ O ₃ crystal grain boundary is c and the total ratios a / N, b / N, and c / N with respect to each number are X, Y, and Z, respectively, An optical wavelength conversion member characterized in that the ratio satisfies the following range.
   
   
   
   
   
   
   
   
   
   
   
   
   
   
   
   0% ≦ X ≦ 25%
   
   
   
   
   
   
   
   
   
   
   
   
   
   
   
   9% ≦ Y ≦ 45%
   
   
   
   
   
   
   
   
   
   
   
   
   
   
   
   48% ≦ Z ≦ 90%
   
   
   
   
   
   
   
   
   
   
   
   
   
   
   
2. 
   
   
   
   
   
   
   
   
   
   
   
   
   
   
   The light wavelength conversion member according to claim 1, wherein a ratio of the A ₃ B ₅ O ₁₂ : Ce crystal particles in the ceramic sintered body is 5 to 50 vol%.
   
   
   
   
   
   
   
   
   
   
   
   
   
   
   
3. 
   
   
   
   
   
   
   
   
   
   
   
   
   
   
   _3. The light wavelength conversion member according to claim 1, wherein a ratio of the Ce is 10.0 mol% or less (excluding 0) with respect to A of the A ₃ B ₅ O ₁₂ .
   
   
   
   
   
   
   
   
   
   
   
   
   
   
   
4. 
   
   
   
   
   
   
   
   
   
   
   
   
   
   
   The average crystal grain size of the Al ₂ O ₃ crystal particles is 0.3 to 10 µm, and the average crystal grain size of the A ₃ B ₅ O ₁₂ : Ce crystal particles is 0.3 to 5 µm. 4. The light wavelength conversion member according to any one of 1 to 3.
   
   
   
   
   
   
   
   
   
   
   
   
   
   
   
5. 
   
   
   
   
   
   
   
   
   
   
   
   
   
   
   A light emitting device comprising the light wavelength conversion member according to any one of claims 1 to 4.

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