OPTICAL WAVELENGTH CONVERSION MATERIAL, OPTICAL WAVELENGTH CONVERSION DEVICE, AND LIGHT EMITTING DEVICE
20210098657 · 2021-04-01
Inventors
- Tsuneyuki ITO (Nagoya-shi, JP)
- Shohei TAKAKU (Nagoya-shi, JP)
- Yuki SHIMURA (Nagoya-shi, JP)
- Shinji BAN (Nagoya-shi, JP)
- Yusuke KATSU (Nagoya-shi, JP)
Cpc classification
C04B2235/3225
CHEMISTRY; METALLURGY
C04B2235/604
CHEMISTRY; METALLURGY
C04B2235/3286
CHEMISTRY; METALLURGY
H01L33/507
ELECTRICITY
C04B35/80
CHEMISTRY; METALLURGY
C04B2235/9653
CHEMISTRY; METALLURGY
C04B2235/3229
CHEMISTRY; METALLURGY
G03B21/204
PHYSICS
C04B2235/5445
CHEMISTRY; METALLURGY
C04B2235/3224
CHEMISTRY; METALLURGY
C04B2235/5436
CHEMISTRY; METALLURGY
Y02B20/00
GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
International classification
C04B35/80
CHEMISTRY; METALLURGY
Abstract
An optical wavelength conversion member according to one aspect of the present disclosure includes a ceramic sintered body, wherein the ceramic sintered body has a fluorescent phase containing, as a main. component, fluorescent crystal grains that generate fluorescence in response to incident light, and a translucent phase containing translucent crystal grains as a main component. The optical wavelength conversion member includes a metal layer having light reflectivity and provided on a side of the ceramic sintered body opposite the side on which the light is incident, and a dielectric multilayer film including dielectric layers having different optical refractive indices and provided between the ceramic sintered body and the metal layer.
Claims
1. An optical wavelength conversion member comprising a ceramic sintered body, wherein the ceramic sintered body has a fluorescent phase containing, as a main component, fluorescent crystal grains that generate fluorescence in response to incident light, and a translucent phase containing translucent crystal grains as a main component, wherein the optical wavelength conversion member further comprises a metal layer having light reflectivity and provided on a side of the ceramic sintered body opposite the side on which the light is incident, and a dielectric multilayer film including dielectric layers having different optical refractive indices and provided between the ceramic sintered body and the metal layer.
2. An optical wavelength conversion member according to claim 1, wherein the crystal grains of the fluorescent phase have a composition represented by formula A.sub.3B.sub.5O.sub.12:Ce, and each of elements A and B is at least one element selected from the following element groups: A: Sc, Y, and lanthanoids exclusive of Ce, and B: Al and Ga.
3. An optical wavelength conversion member according to claim 1, wherein the crystal grains of the translucent phase have a composition of Al.sub.2O.sub.3.
4. An optical wavelength conversion member according to claim 1, wherein the metal layer contains Ag and/or Al as a component.
5. An optical wavelength conversion member according to claim 4, further comprising an Ni layer and/or an Au layer provided on a side of the metal layer opposite the light incident side.
6. An optical wavelength conversion member according to claim 1, wherein the dielectric multilayer film is formed by alternate stacking of a high-refractive-index film that exhibits a refractive index “a” upon incidence of light having a wavelength of 550 nm and a low-refractive-index film that exhibits a refractive index “b” upon incidence of light having a wavelength of 550 nm, the refractive index b being lower than the refractive index a, wherein the refractive index a and the refractive index b satisfies a relation of 1.3<a/b, and a relation of 1<a/c is satisfied wherein c represents the refractive index of the ceramic sintered body upon incidence of light having a wavelength of 550 nm on the ceramic sintered body.
7. An optical wavelength conversion member according to claim 6, wherein the high-refractive-index film contains at least one element selected from among Ti, Zr, Hf, Ta, and Nb, and the low-refractive-index film is formed of SiO.sub.2 or MgF.sub.2.
8. An optical wavelength conversion member according to claim 1, wherein the dielectric multilayer film has an overall thickness of 300 nm or less.
9. An optical wavelength conversion device comprising an optical wavelength conversion member as recited in claim 1, and a heat dissipation member joined to the metal layer of the optical wavelength conversion member on a side opposite the light incident side.
10. A light-emitting device comprising an optical wavelength conversion device as recited in claim 9 and a light-emitting element which emits the light.
Description
BRIEF DESCRIPTION OF THE DRAWINGS
[0068]
[0069]
[0070]
[0071]
[0072]
[0073]
[0074]
[0075]
[0076]
DESCRIPTION OF REFERENCE NUMERAMS
[0077] 1: optical wavelength conversion member [0078] 3: ceramic sintered body [0079] 7: metal layer [0080] 5: dielectric multilayer film [0081] 5a: high-refractive-index film [0082] 5b: low-refractive-index film [0083] 23: Ni layer [0084] 43: Au layer [0085] 51: optical wavelength conversion device [0086] 61: light-emitting device [0087] 63: light-emitting element.
MODES FOR CARRYING OUT THE INVENTION
[0088] Next will be described embodiments of the optical wavelength conversion member, optical wavelength conversion device, and light-emitting device of the present disclosure.
1. First Embodiment
[1-1. Structure of Optical Wavelength Conversion Member]
[0089] Now will be described the structure of an optical wavelength. conversion member of the first embodiment.
[0090] As shown in
[0091] Details will be described below.
<Ceramic Sintered Body>
[0092] The ceramic sintered body 3 is a fluorescent body composed of a fluorescent phase containing, as a main component, crystal grains that generate fluorescence in response to externally incident light (i.e., fluorescent phase grains), and a translucent phase containing, as a main component, translucent crystal grains (i.e., translucent phase grains).
[0093] Thus, the ceramic sintered body 3 is composed of a fluorescent phase (cluster) containing one or more fluorescent phase grains, and a translucent phase (cluster) containing one or more translucent phase grains.
[0094] Thus, the ceramic sintered body 3 is substantially composed or fluorescent phase grains and fluorescent phase grains. The amount of fluorescent phase grains and fluorescent phase grains contained in the ceramic sintered body 3 is, for example, 90 vol. % or more (e.g., about 100 vol. %).
[0095] Specifically, the fluorescent phase grains have a composition represented by formula A.sub.3B.sub.5O.sub.12:Ce, and each of elements A and B is at least one element selected from the following element groups:
[0096] Sc, Y, and lanthanoids exclusive of Ce, and
[0097] B: Al and Ga.
[0098] A and B of formula A.sub.3B.sub.5O.sub.12:Ce are elements (different elements) of a substance represented by formula A.sub.3B.sub.5O.sub.12:Ce. In formula A.sub.3B.sub.5O.sub.12:Ce, O is oxygen and Ce is cerium.
[0099] In the ceramic sintered body 3, the amount of the compound (i.e., fluorescent phase grains) having a composition represented by formula A.sub.3B.sub.5O.sub.12:Ce is, for example, 3 vol. % to 70 vol. % relative to the entire ceramic sintered body 3.
[0100] In the fluorescent phase grains, the Ce concentration is, for example, 0.1 mol % to 1.0 mol % relative to the element A of the compound.
[0101] When the element A contains Gd, the Gd concentration is, for example, 30 mol % or less relative to the entirety of element A. When the element B contains Ga, the Ga concentration is, for example, 30 mol % or less relative to the entirety of element B.
[0102] The translucent phase grains have a composition of, for example, Al.sub.2O.sub.3.
[0103] The ceramic sintered body 3 has dimensions of, for example, 10 mm (width)×10 mm (length), and a thickness of, for example, 100 μm to 400 μm (e.g., 100 μm).
<Dielectric Multilayer Film>
[0104] The dielectric multilayer film 5 includes a plurality of dielectric layers having different optical refractive indices and can transmit light.
[0105] Thus, the dielectric multilayer film 5 is a layered product including dielectric films having different optical refractive indices; i.e., a layered product including a high-refractive-index film and a low-refractive-index film (having a refractive index lower than that of the high-refractive-index film).
[0106] Specifically, as shown in
[0107] In the present embodiment, the total number of layers (films) of the dielectric multilayer film 5 is two. However, the total number of layers may be, for example, two to four. Each of the TiO.sub.2 film 5a and the SiO.sub.2 film 5b may have, for example, 25 nm to 100 nm. The overall thickness of the dielectric multilayer film 5 is preferably up to about 300 nm.
[0108] As described above, when the thicknesses of the high-refractive-index film and the low-refractive-index film are determined so as to correspond, to the wavelength of incident light, the intensity of reflected light can be enhanced. Therefore, the thicknesses of the TiO.sub.2 film 5a and the SiO.sub.2 film 5b are determined so that the intensity of reflected light can be enhanced in accordance with the wavelength λ of incident light.
[0109] When the wavelength of incident light is, for example, 465 nm, the thickness of each of the TiO.sub.2 film 5a and the SiO.sub.2 film 5b is preferably 50 nm.
<Metal Layer>
[0110] The metal layer 7 is formed of a metal having light reflectivity.
[0111] In the present embodiment, the metal layer 7 has a structure including, for example, a single layer of Ag (Ag layer). However, the metal layer 7 may be formed. of a layer of another metal (e.g., Al).
[0112] Alternatively, the metal layer 7 may have a multilayer structure including layers of different metals (e.g., an Ag layer and an Al layer).
[0113] The metal layer 7 may have a thickness of, for example, 100 nm to 500 nm.
[1-2. Production Method for Optical Wavelength Conversion Member]
[0114] A schematic production process for the optical wavelength conversion member 1 will now be briefly described with reference to
[0115] Firstly, powder materials of the ceramic sintered body 3 were weighed so as to satisfy the aforementioned requirement of the first embodiment and subjected to another process (i.e., the powder materials were prepared).
[0116] Subsequently, an organic solvent and a dispersant were added to the prepared powder materials, and these materials were grind-mixed in a ball mill, to thereby prepare a slurry.
[0117] The slurry was then dried and formed into granules.
[0118] The resultant granules were then subjected to press molding.
[0119] The resultant pressed compact was then fired at a predetermined temperature for a predetermined period of time, to thereby produce the ceramic sintered body 3.
[0120] Instead of the aforementioned production method for the ceramic sintered body 3 by press molding, the ceramic sintered. body 3 may be produced by firing of a sheet compact prepared through sheet molding of the slurry.
[0121] Subsequently, the dielectric multilayer film 5 was formed on one surface (on the reflection side) of the ceramic sintered body 3 in a thickness direction.
[0122] Specifically, the TiO.sub.2 film 5a was firstly formed by vacuum vapor deposition. Thereafter, the SiO.sub.2 film 5b was formed on a surface (i.e., an exposed surface on the reflection side) of the TiO.sub.2 film 5a by vacuum vapor deposition.
[0123] Subsequently, the metal layer (e.g., Ag layer) 7 was formed on a surface (i.e., an exposed surface on the reflection side) of the SiO.sub.2 film 5b of the dielectric multilayer film 5 by, for example, vacuum vapor deposition.
[0124] The metal layer 7 may be formed by any thin film formation technique other than vacuum vapor deposition (e.g., sputtering or plating).
[0125] Thus, the optical wavelength conversion member 1 was produced.
[1-3. Effects]
[0126] The effects of the first embodiment will next be described.
[0127] (1) The optical wavelength conversion member 1 of the first embodiment includes the metal layer (Ag layer) 7 having light reflectivity and provided on the side of the ceramic sintered body 3 opposite the side on which light is incident, and the dielectric multilayer film 5 including dielectric layers having different optical refractive indices and provided between the ceramic sintered body 3 and the metal layer 7.
[0128] The dielectric multilayer film 5 has a structure including the high-refractive-index film 5a and the low-refractive-index film on that are sequentially stacked from the light incident side. Light reflected at the interface between the films 5a and 5b is reinforced by interference.
[0129] According to this structure, the optical wavelength conversion member exhibits a higher reflectivity (i.e., reflectance) than a conventional optical wavelength converter including only a metal layer. Accordingly, the optical wavelength. conversion member 1 can efficiently reflect incident light or fluorescence as compared with a conventional one. Therefore, the optical wavelength conversion member 1 can achieve efficient light extraction, and thus exhibits high emission intensity (i.e., fluorescence intensity).
[0130] (2) In the first embodiment, the crystal grains of the fluorescent phase have a composition represented by formula A.sub.3B.sub.5O.sub.12:Ce, and each of elements A and B is at least one element selected. from the following element groups.
[0131] A: Sc, Y, and lanthanoids exclusive of Ce, and
[0132] B: Al and Ga.
[0133] This composition enables efficient conversion of blue light into visible light. Use of the ceramic sintered body 3 can cause light scattering at the interface between the fluorescent phase and the translucent phase, thereby reducing the angular dependence of the color of light, leading to an improvement in color uniformity (i.e., reduced color unevenness).
[0134] Also, use of the ceramic sintered body 3, which exhibits high thermal conductivity, can efficiently dissipate heat generated in the optical wavelength conversion. member 1 by light (e.g., laser light) to the outside (e.q., the metal layer 7 or the heat dissipation member), thereby preventing temperature quenching (i.e., no generation of fluorescence by the ceramic sintered body 3). Thus, even when high-output laser light is incident on the optical wavelength conversion member 1, fluorescence can be maintained at an appropriate level.
[0135] (3) In the first embodiment, the metal layer 7 is formed of Ag. Thus, the metal layer 7 effectively reflects light, such as externally incident light or fluorescence generated in the ceramic sintered body 3. The metal layer 7 may be, for example, an Al layer instead of an Ag layer.
2. Second Embodiment
[0136] Next will be described an optical wavelength conversion member of a second embodiment. Description of the same components as those in the first embodiment is omitted or simplified. The same components as those in the first embodiment are denoted by the same reference numerals.
[0137] As shown in
[0138] Particularly in the second embodiment, an Al.sub.2O.sub.3 layer 13 is formed on the reflection side (the lower side of
[0139] The Al.sub.2O.sub.3 layer 13 can be formed by, for example, vacuum vapor deposition.
[0140] The second embodiment achieves the same effects as in the first embodiment. Since the surface of the Ag layer 7 is covered with the Al.sub.2O.sub.3 layer 13 in the second embodiment, oxidation of Ag can be prevented. Thus, deterioration of the reflectivity of the Ag layer 7 can be prevented.
[0141] The Ag layer 7 may be replaced for an Al layer. The Ag layer 7 and an Al layer may be stacked. together (the same shall apply hereinafter).
3. Third Embodiment
[0142] Next will be described an optical wavelength conversion. member of a third embodiment. Description of the same components as those in the first embodiment is omitted or simplified. The same components as those in the first embodiment are denoted by the same reference numerals.
[0143] As shown in
[0144] Particularly in the third. embodiment, an Ni layer 23 is formed on the reflection side (the lower side of
[0145] When the surface of the Ag layer 7 is covered with another metal layer (e.g., the Ni layer 23), the structure including the Ag layer (i.e., metal layer) 7 and another metal layer (e.g., the Ni layer 23) will be referred to as “metal coating 25.”
[0146] Similar to the case of the Ag layer 7, the Ni layer 23 can be formed by any thin film formation technique such as vacuum vapor deposition, sputtering, or plating.
[0147] The third embodiment achieves the same effects as in the first embodiment. Since the surface of the Ag layer 7 is covered with the Ni layer 23 in the third embodiment, oxidation of Ag can be prevented.
4. Fourth Embodiment
[0148] Next will be described an optical wavelength conversion. member of a fourth embodiment. Description of the same components as those in the second embodiment is omitted or simplified. The same components as those in the second embodiment are denoted by the same reference numerals.
[0149] As shown in
[0150] Particularly in the fourth embodiment, an Ni layer 23 (as in the case of the third embodiment) is formed on the reflection side (the lower side of
[0151] The fourth embodiment achieves the same effects as in the first embodiment. Since the surface of the Ag layer 7 is covered with the Al.sub.2O.sub.3 layer 13 and the Ni layer 23 in the fourth embodiment, oxidation of AG, can be effectively prevented.
5. Fifth Embodiment
[0152] Next will be described an optical wavelength conversion member of a fifth embodiment. Description of the same components as those in the third embodiment is omitted or simplified. The same components as those in the third embodiment are denoted by the same reference numerals.
[0153] As shown in
[0154] Particularly in the fifth embodiment, an Au layer 43 is formed on the reflection side (the lower side of
[0155] Similar to the case of the Ni layer 23, the Au layer 43 can be formed by any thin film formation technique such as vacuum vapor deposition, sputtering, or plating.
[0156] The fifth embodiment achieves the same effects as in the third embodiment. Since the surface of the Ag layer 7 is covered with the Ni layer 23 and the Au layer 43 in the fifth embodiment, oxidation of Ag can be effectively prevented.
[0157] The Ag layer 7 may be replaced for an Al layer, and the Au layer 43 may be replaced for an Ag layer. In addition, an Al.sub.2O.sub.3 layer 13 (as in the case of the fourth embodiment) may be provided between the Ag layer 7 and the Ni layer 23.
6. Sixth Embodiment
[0158] Next will be described an optical wavelength conversion member of a sixth embodiment. Description of the same components as those in the fifth embodiment is omitted or simplified. The same components as those in the fifth embodiment are denoted by the same reference numerals.
[0159] As shown in
[0160] The optical wavelength conversion member 41 has a structure similar to that in the fifth embodiment; specifically, a structure formed by sequential stacking of a ceramic sintered body 3, a dielectric multilayer film 5 including a TiO.sub.2 film 5a and an SiO.sub.2 film 5b, a metal layer (i.e., Ag layer) 7, an Ni layer 23, and an Au layer 43 from the upper side (incident side) of
[0161] The bonding member 53 is formed of a bonding material having high thermal conductivity; for example, a metal bonding material such as solder containing, Pb. The bonding member 53 may be formed of, besides a metal bonding material, a well-known thermally conductive adhesive having high thermal conductivity.
[0162] The heat dissipation member 55 has an outer size larger than that of the optical wavelength conversion member 41 in plan view (as viewed in a vertical direction of
[0163] The heat dissipation member 55 has higher heat dissipation (i.e., thermal conductivity) than the ceramic sintered body 3. The heat dissipation member 55 may be formed of, for example, a metal such as aluminum or copper.
[0164] Although not illustrated, a protective layer may be formed between the optical wavelength conversion member 41 and the bonding member 53 for improving bonding property. The protective layer may be an Ni sheet.
[0165] The sixth embodiment achieves the same effects as in the fifth embodiment. In the sixth embodiment, high heat dissipation is achieved, since the optical wavelength conversion member 41 is joined to the heat dissipation member 55. Thus, since an increase in the temperature of the ceramic sintered body 3 can be reduced, temperature quenching can be prevented, thereby achieving superior emission property (i.e., fluorescence property).
7. Seventh Embodiment
[0166] Next will be described a light-emitting device of a seventh embodiment. Description of the same components as those in the sixth embodiment is omitted or simplified. The same components as those in the sixth embodiment are denoted by the same reference numerals.
[0167] As shown in
[0168] The light-emitting element 63 may be any known element such as an LED or LD.
[0169] In the light-emitting device 61, blue light is emitted from the light-emitting element 63 onto the surface of the ceramic sintered body 3. The light undergoes wavelength conversion in the ceramic sintered body 3 and is reflected by, for example, the Ag layer 7. Consequently, white light (resulting from mixing of different colors of light) emitted through the upper surface of the optical wavelength conversion member 41 (i.e., the upper surface 3a of the ceramic sintered body) toward the upper side of
[0170] The seventh embodiment achieves the same effects as in the sixth embodiment. The light-emitting device 61 of the seventh embodiment can emit light of high intensity to the outside.
8. Examples
[0171] The aforementioned embodiments will next be described in detail by way of specific working examples.
[0172] There were prepared optical wavelength convey members (samples Nos. 1 to 18) shown in Table 1 below.
[0173] Samples Nos. 1 to 6 and. 10 to 18 fall within the scope of the present disclosure, and samples Nos. 7 to 9 fall outside the scope of the present disclosure (Comparative Examples).
[0174] The optical wavelength conversion member having the same structure as in the third embodiment was used as the optical wavelength conversion member of the present disclosure. Specifically, there was used a structure formed by stacking of a ceramic sintered body, a dielectric multilayer film, an Ag layer, and an Ni layer. In the column “Dielectric multilayer film” of Table 1, the structure of a dielectric multilayer film corresponding to each sample nearer to the ceramic sintered body is placed in the left.
[8-1. Evaluation of Samples]
[0175] As described below, the samples were evaluated for the following items.
<Relative Density>
[0176] The open porosity of the ceramic sintered body of the optical wavelength conversion member of each sample was measured by the method according to JIS R1634. The measured value was used to determine the relative density of the ceramic sintered body.
<Laser Output Resistance>
[0177] Blue LD light having a. wavelength of 465 nm was focused to a width of 0.1 mm by means of a lens, and the optical wavelength conversion member of each sample was irradiated with the focused light. Reflected light was focused with a lens, and the chromaticity (X) of the focused light was measured by means of a spectroradiometer (CL-500A, manufactured by KONICA MINOLTA, INC.). The sample was irradiated with the light at a power density of 0 to 100 W/mm.sup.2.
[0178] Occurrence of temperature quenching was determined when the chromaticity was reduced to 60% or less of that at a laser power density of 5 W/mm.sup.2 The laser power density at occurrence of temperature quenching is shown in Table 1 below. The “>100” shown in Table 1 corresponds to no temperature quenching even at 100 W/mm.sup.2. A sample exhibiting no temperature quenching at 100 W/mm.sup.2 or more is preferred in terms of laser output resistance.
<Fluorescence Intensity>
[0179] Blue LD light having a wavelength of 465 nm was focused to a width of 0.1 mm by means of a lens, and the optical wavelength conversion member of each sample was irradiated with the focused light. Reflected light was focused with a lens, and the emission intensity (i.e., fluorescence intensity) was measured by means of a power sensor. The sample was irradiated with the light at a power density of 40 W/mm.sup.2. The fluorescence intensity of each sample was compared with that (taken. as 100%) in the case where a single-crystal body (i.e., a YAG:Ce single-crystal body) was used as the ceramic sintered body (fluorescent body). The fluorescence intensity is preferably 100% or more.
<Color Unevenness>
[0180] Color unevenness (variation in color) was evaluated through determination of a variation in chromaticity by means of an illuminometer.
[0181] Specifically, blue LD light having a wavelength of 465 nm. was focused to a width of 0.5 mm. by means of a lens, and the optical wavelength conversion member or each sample was irradiated with the focused light. The chromaticity of reflected light was measured by means of a spectroradiometer (CL-500A, manufactured by MONICA MINOLTA, INC.).
[0182] The light irradiation was performed on a. 9 mm square region (divided into nine regions at intervals of 3 mm) at the center of the surface of each sample (i.e., sample surface). A variation in chromaticity (in X-direction) (i.e., Δx) was evaluated in each of the nine regions. As used herein, the term “variation in chromaticity (Δx)” refers to the maximum deviation of chromaticity (in X-direction). The variation in chromaticity Δx is preferably less than 0.03.
[0183] The term “chromaticity” as used. herein. refers to a chromaticity indicated by the CIE-XYZ color system. established by the International Commission or Illumination (CIE) in 1931. Specifically, the chromaticity is indicated by the xy chromaticity diagram (so-called CIE chromaticity diagram) wherein three primary colors of light are digitized and represented in an xv coordinate space.
<Sample Temperature>
[0184] Blue LD light having a wavelength of 465 nm was focused to a width. of 0.1 mm by means of a lens, and the optical wavelength. conversion member of each sample was irradiated. with the focused light. The temperature of an irradiated portion (i.e., a portion irradiated with the blue LD light) was measured by means of a radiation thermometer. The sample was irradiated with the blue LD light at a power density of 40 W/mm.sup.2.
<Refractive Index Ratio>
[0185] The refractive index ratios a/b and a/c of each sample were calculated from. the refractive indices a and b of the dielectric films forming the dielectric multilayer film of the sample with respect to light having a wavelength of 550 nm (i.e., the refractive index a of a high-refractive-index film, and the refractive index b of a low-refractive-index film (having a refractive index lower than that of the high-refractive-index film)) and the refractive index c of the ceramic sintered body of the sample with respect to light having a wavelength of 550 nm,
[0186] The refractive index a of TiO.sub.2, Ta.sub.2O.sub.5, HfO.sub.2, ZrO.sub.2, or Nb.sub.2O.sub.5 is greater than the refractive index b of SiO.sub.2, and the refractive index a of TiO.sub.2 is greater than the refractive index b of MgF.sub.2.
<Overall Thickness of Dielectric Multilayer Film>
[0187] The overall thickness of the dielectric multilayer film of each sample corresponds to the sum of the thicknesses of the dielectric films forming the dielectric multilayer film of the sample.
<Film Adhesion>
[0188] Each sample was subjected to a tape test for determining film adhesion. The test was performed according to JIS R3255, to thereby determine occurrence of exfoliation at the interface between the ceramic sintered body and the dielectric multilayer film or at the interface between the dielectric films forming the dielectric multilayer film. The film adhesion was evaluated on the basis of the following criteria: no exfoliation, partial exfoliation, and complete exfoliation.
[8-2. Production Method for Sample and Results of Evaluation]
[0189] Next will be described a production method for each sample and the results of evaluation of the sample.
Experimental Example 1
[0190] Optical wavelength conversion members (samples Nos. 1 to 4) were prepared under the conditions shown in Table 1 below.
[0191] (1) Firstly, a ceramic sintered body (fluorescent body) was prepared through the procedure described below. The dimensions of the ceramic sintered body were 10 mm (width)×10 mm (length)×200 μm (thickness).
[0192] Specifically, as shown in Table 1 below, Al.sub.2O.sub.3 powder (mean particle size: 0.2 ,μm), Y.sub.2O.sub.3 powder (mean particle size: 1.2 μm), and CeO.sub.2 powder (mean particle size: 1.5 μm) were weighed in accordance with the composition of the ceramic sintered body of each of samples Nos. 1 to 4 (specifically, for the production of the ceramic sintered body having the composition of each sample).
[0193] These powder materials were added to a ball mill together with ethanol, and these materials were grind-mixed for 16 hours. The resultant slurry was dried and formed into granules. A predetermined amount (2 wt. % of total) of a completely melted binder was added to the granules, and the mixture was thoroughly stirred and dried, to thereby yield a predetermined powder.
[0194] The powder was subjected to press molding and then. CIP molding, to thereby prepare a compact. The compact was degreased and then fired in an air atmosphere at a temperature of 1,600° C. for 10 hours, to thereby prepare a ceramic sintered body.
[0195] Although not illustrated in Tables 1 and 2, each sample had a relative density of 99% or more (the same shall apply to other samples described below).
[0196] (2) A dielectric multilayer film and a metal layer were formed on the ceramic sintered body through the procedure described below.
[0197] Firstly, a dielectric multilayer film was formed on one surface of the ceramic sintered body. Specifically, a TiO.sub.2 film was formed on the surface of the ceramic sintered body, and an SiO.sub.2 film was formed on the surface of the TiO.sub.2 film.
[0198] As shown in detail in Table 1, the dielectric multilayer film was formed of one TiO.sub.2 film and one SiO.sub.2 film, or two TIO.sub.2 films and two SiO.sub.2 films. The thickness of each film was adjusted to 25 nm or 50 nm. In sample No. 3, two TiO.sub.2 films and two SiO.sub.2 films were formed so that a TiO.sub.2 film, a SiO.sub.2 film, a TiO.sub.2 film, and a SiO.sub.2 film were stacked in this order.
[0199] Subsequently, as shown in Table 1 below, the surface of the dielectric multilayer film (i.e., the surface of the SiO.sub.2 film) was coated with a reflective metal (i.e., Ag or Al), to thereby form a metal layer (i.e., an Ag layer or an Al layer). The thickness of the Ag layer or the Al layer was adjusted to 300 nm.
[0200] Thereafter, as shown in Table 1 below, an Ni layer was formed on the surface of the Ag layer or the Al layer. The thickness of the Ni layer was adjusted to 100 nm.
[0201] The Ag, Al, or Ni coating was performed by means of vacuum vapor deposition.
[0202] Thus, the optical wavelength conversion member of each sample was produced.
[0203] (3) The optical wavelength conversion member of each sample was evaluated by the aforementioned evaluation methods. The results of evaluation are shown in Table 2 below.
[0204] As shown in Table 2, samples Nos. 1 to 4 are preferred, since the samples exhibit a laser output resistance of more than 100 W/mm.sup.2 and are less likely to cause temperature quenching. These samples are preferred in view that they include a dielectric multilayer film and a metal layer shown in Table 1, exhibit a refractive index ratio a/b of 2.02, a refractive index ratio a/c of 1.65, a high fluorescence intensity of 108% or more, a small color unevenness of 0.029 or less, and a low irradiated portion temperature of 128° C. or less (i.e., superior heat dissipation). In addition, these samples exhibit superior film adhesion, since the overall thickness of the dielectric multilayer film is as small as 100 nm or less.
Experimental Example 2
[0205] Optical wavelength conversion members (samples Nos. 5 and 6) were prepared under the conditions shown in Table 1 below.
[0206] Basically, the ceramic sintered body sample of Experimental Example 2 was prepared in the same manner as employed in Experimental Example 1.
[0207] However, in sample No. 5, Gd.sub.2O.sub.3 powder (mean particle size: 1.1 μm) was added, and the amount of Gd was adjusted to be 30% by mole relative to the amount of Y. In sample No. 7, Lu.sub.2O.sub.3 powder (mean particle size: 4.1 μm) and Ga.sub.2O.sub.3 powder (mean particle size: 0.9 μm) were added, the amount of Lu was adjusted to be 50% by mole relative to the amount of Y, and the amount of Ga was adjusted to be 50% by mole relative to the amount of Al.
[0208] In the same manner as employed in Experimental Example 1, a dielectric multilayer film and a metal coating were formed on the ceramic sintered body of Experimental Example 2 as shown in Table 1 below, to thereby produce an optical wavelength conversion member. A metal layer is formed of a metal (i.e., Al or Ag) shown at the left end in the column “Metal coating” of Table 1.
[0209] The resultant optical wavelength conversion member of each sample was evaluated by the aforementioned evaluation methods. The results of evaluation are shown in Table 2 below.
[0210] As shown in Table 2, samples Nos. and 7 are preferred, since the samples exhibit a laser output resistance of more than 100 W/mm.sup.2 and are less likely to cause temperature quenching. These samples are preferred in view that they include a dielectric multilayer film and a metal layer shown in Table 1, exhibit a refractive index ratio a/b of 2.02, a refractive index ratio a/c of 1.65, a high fluorescence intensity of 106% or more, a small color unevenness of 0.029, and a low irradiated portion temperature of 132° C. or less. In addition, these samples exhibit superior film adhesion, since the overall thickness of the dielectric multilayer film is as small as 100 nm.
Experimental Example 3
[0211] An optical wavelength conversion member (sample No. 7) was prepared under the conditions shown in Table 1 below. Sample No. 7, which includes no dielectric multilayer film, corresponds to Comparative Example.
[0212] The ceramic sintered body sample of Experimental Example 3 was prepared in the same manner as employed in Experimental Example 1.
[0213] As shown in Table 1 below, a metal coating was formed directly on the ceramic sintered body of Experimental Example 3 without formation of a dielectric multilayer film, to thereby produce an optical wavelength conversion member.
[0214] The resultant optical wavelength conversion member of each sample was evaluated by the aforementioned evaluation methods. The results of evaluation are shown in Table 2 below.
[0215] As shown in Table 2, sample No. 7 is not preferred, since the sample exhibits a low fluorescence intensity of 94% and poor film adhesion.
Experimental Example 4
[0216] Optical wavelength conversion members (samples Nos. 8 and 9) were prepared under the conditions shown in Table 1 below. Samples Nos. 8 and 9 have ceramic sintered bodies different from those of samples Nos. 1 to 7.
[0217] Basically, the ceramic sintered body sample of Experimental Example 4 was prepared in the same manner as employed in Experimental Example 1.
[0218] However, in sample No. 8, the ceramic sintered body was formed of a fluorescent body prepared from a dispersion of YAG particles in glass. In sample No. 9, the ceramic sintered body was formed of a YAG single-crystal fluorescent body.
[0219] In the same manner as employed in Experimental Example 1, a dielectric multilayer film and a metal coating were formed on the ceramic sintered body of Experimental Example 4 as shown in Table 1 below, to thereby produce an optical wavelength conversion member.
[0220] The resultant optical wavelength conversion member of each sample was evaluated by the aforementioned evaluation methods. The results of evaluation are shown in Table 2 below.
[0221] As shown in Table 2, sample No. 8 is not preferred, since the sample exhibits a low laser output resistance of 40 W/mm.sup.2, and a low fluorescence Intensity of 90%. Sample No. 8 is not preferred in view that it exhibits a larger color unevenness and a higher irradiated portion temperature than samples Nos. 1 to 6.
[0222] Sample No. 9 is not preferred, since the sample exhibits a low laser output resistance of 75 W/mm.sup.2. Sample No. 9 is not preferred in view that it exhibits a larger color unevenness and a higher irradiated portion temperature than samples Nos. 1 to 6. Sample No. 9 exhibits a fluorescence intensity of 100%, which is lower than that of samples Nos. 1 to 6.
Experimental Example 5
[0223] Optical wavelength conversion members (samples Nos. 10 and 11) were prepared under the conditions shown in Table 1 below.
[0224] Basically, the ceramic sintered body sample of Experimental Example 5 was prepared in the same manner as employed in Experimental Example 1. However, the structure of a metal coating was changed.
[0225] Specifically, the ceramic sintered body of sample No. 10 or 11 was provided with an Ag or Al layer (200 nm) and an Ni layer (100 nm), and an Au or Ag layer (200 nm) was formed on the Ni layer.
[0226] In the same manner as employed in Experimental Example 1, a dielectric multilayer film and a metal coating were formed on the ceramic sintered body of Experimental Example 5 as shown in Table 1 below, to thereby produce an optical wavelength conversion member.
[0227] The resultant optical wavelength conversion member of each sample was evaluated by the aforementioned evaluation methods. The results of evaluation are shown in Table 2 below. As shown in Table 2, samples Nos. 10 and 11 are preferred, since the samples exhibit a laser output resistance of more than 100 W/mm.sup.2 and are less likely to cause temperature quenching. These samples are preferred in view that they include a dielectric multilayer film and a metal layer shown in Table 1, exhibit a refractive index ratio a/b of 2.02, a refractive index ratio a/c of 1.65, a high fluorescence intensity of 105% or more, a small color unevenness of 0.029 or less, and a low irradiated portion temperature of 126° C. or less. In addition, these samples exhibit superior film adhesion, since the overall thickness of the dielectric multilayer film is as small as 100 nm.
Experimental Example 6
[0228] Optical wavelength conversion members (samples Nos 12 to 18) were prepared under the conditions shown in Table 1 below.
[0229] The ceramic sintered body sample of Experimental Example 6 was prepared. in the same manner as employed in Experimental Example 1.
[0230] In the same manner as employed in Experimental Example 1, a dielectric multilayer film and a metal coating were formed on the ceramic sintered body of Experimental Example 6 as shown in Table 1 below, to thereby produce an optical wavelength conversion member.
[0231] The resultant optical wavelength conversion member of each sample was evaluated by the aforementioned evaluation methods. The results of evaluation are shown in Table 2 below.
[0232] As shown in Table 2, samples Nos. 12 to 17 are preferred, since the samples exhibit a laser output resistance of more than 100 W/mm.sup.2 and are less likely to cause temperature quenching. These samples are preferred in view that they include a dielectric multilayer film and a metal coating shown in Table 1, exhibit a refractive index ratio a/b of 1.32 or more, a refractive index ratio a/c of 1.08 or more, a high fluorescence intensity of 107% or more, a small color unevenness of 0.034 or less, and a low irradiated portion temperature of 135° C. or less. In addition, these samples exhibit superior film adhesion, since the overall thickness of the dielectric multilayer film is as small as 300 nm.
[0233] Sample No. 18 is preferred, since the sample exhibits a laser output resistance of more than 100 W/mm.sup.2 and is less likely to cause temperature quenching. The sample is preferred in view that it includes a dielectric multilayer film and a metal coating shown in Table 1, exhibits a refractive index ratio a/b of 2.02, a refractive index ratio a/c of 1.65, and a high fluorescence intensity of 118%. Since the overall thickness of the dielectric multilayer film is 400 nm, the sample exhibits lower film adhesion than a sample including a dielectric multilayer film having an overall thickness of 300 nm.
TABLE-US-00001 TABLE 1 Type of fluorescent body Al.sub.2O.sub.3 A.sub.3B.sub.5O.sub.12:Ce amount Amount No. [vol %] A B [vol %] Dielectric multilayer film Metal coating Examples of Experimental 1 75 Y Al 25 TiO.sub.2/50 nm, SiO.sub.2/50 nm Ag/300 nm, Ni/100 nm the present Example 1 2 75 Y Al 25 TiO.sub.2/25 nm, SiO.sub.2/25 nm Ag/300 nm, Ni/100 nm disclosure 75 Y Al 25 TiO.sub.2/25 nm, SiO.sub.2/25 nm, Ag/300 nm, Ni/100 nm Two layers for each 4 75 Y Al 25 TiO.sub.2/50 nm, SiO.sub.2/50 nm Al/300 nm, Ni/100 nm Experimental 5 75 Y, Gd Al 25 TiO.sub.2/50 nm, SiO.sub.2/50 nm Al/300 nm, Ni/100 nm Example 2 6 75 Y, Lu Al, Ga 25 TiO.sub.2/50 nm, SiO.sub.2/50 nm Al/300 nm, Ni/100 nm Comparative Experimental 7 75 Y Al 25 None Ag/300 nm, Ni/100 nm Examples Example 3 Experimental 8 YAG powder + glass mixture TiO.sub.2/50 nm, SiO.sub.2/50 nm Ag/300 nm, Ni/100 nm Example 4 9 YAG single-crystal TiO.sub.2/50 nm, SiO.sub.2/50 nm Ag/300 nm, Ni/100 nm Examples of Experimental 10 75 Y Al 25 TiO.sub.2/50 nm, SiO.sub.2/50 nm Ag/200 nm, Ni/100 nm, Au/200 nm the present Example 5 11 75 Y Al 25 TiO.sub.2/50 nm, SiO.sub.2/50 nm Al/200 nm, Ni/100 nm, Ag/200 nm disclosure Experimental 12 75 Y Al 25 Ta.sub.2O.sub.5/50 nm, SiO.sub.2/50 nm Al/200 nm, Ni/100 nm, Ag/200 nm Example 6 13 75 Y Al 25 HfO.sub.2/50 nm, SiO.sub.2/50 nm Al/200 nm, Ni/100 nm, Ag/200 nm 14 75 Y Al 25 ZrO.sub.2/50 nm, SiO.sub.2/50 nm Al/200 nm, Ni/100 nm, Ag/200 nm 15 75 Y Al 25 Nb.sub.2O.sub.5/50 nm, SiO.sub.2/50 nm Al/200 nm, Ni/100 nm, Ag/200 nm 16 75 Y Al 25 TiO.sub.2/50 nm, MgF.sub.2/50 nm Al/200 nm, Ni/100 nm, Ag/200 nm 17 75 Y Al 25 TiO.sub.2/50 nm, SiO.sub.2/50 nm, Al/200 nm, Ni/100 nm, Ag/200 nm Three layers for each 18 75 Y Al 25 TiO.sub.2/50 nm, SiO.sub.2/50 nm, Al/200 nm, Ni/100 nm, Ag/200 nm Four layers for each
TABLE-US-00002 TABLE 2 Overall Irradiation thickness of Laser output Fluorescence portion Refractive Refractive dielectric resistance intensity Color temperature index ratio index ratio multilayer film No. [w/mm.sup.2] [%] unevenness [° C.] (a/b) (a/c) [nm] Film adhesion Examples of Experimental 1 >100 120 0.024 108 2.02 1.65 100 No exfoliation the present Example 1 2 >100 123 0.026 108 2.02 1.65 50 No exfoliation disclosure 3 >100 115 0.025 108 2.02 1.65 100 No exfoliation 4 >100 108 0.029 128 2.02 1.65 100 No exfoliation Experimental 5 >100 106 0.029 132 2.02 1.65 100 No exfoliation Example 2 6 >100 109 0.029 119 2.02 1.65 100 No exfoliation Comparative Experimental 7 >100 94 0.028 102 — — 0 Complete Examples Example 3 exfoliation Experimental 8 40 90 0.034 320 2.02 1.90 100 No exfoliation Example 4 9 75 100 0.12 215 2.02 1.61 100 No exfoliation Examples of Experimental 10 >100 118 0.024 115 2.02 1.65 100 No exfoliation the present Example 5 11 >100 105 0.029 126 2.02 1.65 100 No exfoliation disclosure Experimental 12 >100 107 0.034 125 1.48 1.21 100 No exfoliation Example 6 13 >100 108 0.023 128 1.32 1.24 100 No exfoliation 14 >100 112 0.024 129 1.52 1.08 100 No exfoliation 15 >100 116 0.032 130 1.59 1.30 100 No exfoliation 16 >100 122 0.024 126 2.13 1.65 100 No exfoliation 17 >100 118 0.030 135 2.02 1.65 300 No exfoliation 18 >100 118 0.039 144 2.02 1.65 400 Partial exfoliation
9. Other Embodiments
[0234] Needless to say, the present disclosure is not limited to the aforementioned embodiment, but may be implemented in various other forms without departing from the scope of the disclosure.
[0235] For example, a sample was prepared through firing in air in the Examples described above. However, a sample having the same performance as that of the Examples can be prepared through another firing technique, such as hot press firing, vacuum firing, firing in a reducing atmosphere, HIP, or any combination of these.
[0236] (2) The aforementioned optical wavelength conversion member or light-emitting device can be used for various applications, including fluorescent bodies, optical wavelength conversion apparatuses, head lamps, lighting apparatuses, and optical apparatuses (e.g., projectors).
[0237] (3) No particular limitation is imposed on the light-emitting element used in the light-emitting device. The light-emitting element may be any known element, such as an LED or LD.
[0238] (4) in the aforementioned embodiments, the function of a single component may be shared by a plurality of components, or a single component may exert the functions of a plurality of components. Some of the components in the aforementioned embodiments may be omitted. At least some of the components in the aforementioned embodiments may be, for example, added to or replaced with components in another embodiment. Embodiments of the present disclosure encompass any fore included in technical ideas specified by the appended claims.