# US 2010/0164367 A1 · Fluorescent substance, method for producing the same, and light-emitting device using the same

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- Number: US 2010/0164367 A1
- Document ID: US20100164367A1
- Status: Published application
- Kind: A1
- Application number: 12/600,971
- Filed: 2008-05-01
- Published: 2010-07-01
- Earliest claimed: 2007-05-22
- Assignees: National Institute for Materials Science
- Inventors: Kousuke Shioi; Naoto Hirosaki
- Web page: https://patentgrep.com/patent/US20100164367A1

## CPC

- C09K 11/7728: {containing europium}
- C04B 35/597: based on silicon oxynitride, {e.g. SIALONS}
- C04B 35/6262: {of calcined, sintered clinker or ceramics}
- C04B 35/62675: {characterised by the treatment temperature}
- C04B 35/6268: {characterised by the applied pressure or type of atmosphere, e.g. in vacuum, hydrogen or a specific oxygen pressure}
- C04B 35/62685: {characterised by the order of addition of constituents or additives}
- C09K 11/0883: {Arsenides; Nitrides; Phosphides}
- H05B 33/14: characterised by the chemical or physical composition or the arrangement of the electroluminescent material {, or by the simultaneous addition of the electroluminescent material in or onto the light source}
- C04B 2235/3201: Alkali metal oxides or oxide-forming salts thereof
- C04B 2235/3203: Lithium oxide or oxide-forming salts thereof
- C04B 2235/3205: Alkaline earth oxides or oxide forming salts thereof, e.g. beryllium oxide
- C04B 2235/3206: Magnesium oxides or oxide-forming salts thereof
- C04B 2235/3208: Calcium oxide or oxide-forming salts thereof, e.g. lime
- C04B 2235/3213: Strontium oxides or oxide-forming salts thereof
- C04B 2235/3215: Barium oxides or oxide-forming salts thereof
- C04B 2235/3224: Rare earth oxide or oxide forming salts thereof, e.g. scandium oxide
- C04B 2235/3225: Yttrium oxide or oxide-forming salts thereof
- C04B 2235/3227: Lanthanum oxide or oxide-forming salts thereof
- C04B 2235/3229: Cerium oxides or oxide-forming salts thereof
- C04B 2235/3262: Manganese oxides, manganates, rhenium oxides or oxide-forming salts thereof, e.g. MnO
- C04B 2235/3852: Nitrides, e.g. oxynitrides, carbonitrides, oxycarbonitrides, lithium nitride, magnesium nitride
- C04B 2235/3865: Aluminium nitrides
- C04B 2235/3873: Silicon nitrides, e.g. silicon carbonitride, silicon oxynitride
- C04B 2235/3878: Alpha silicon nitrides
- C04B 2235/3891: Silicides, e.g. molybdenum disilicide, iron silicide
- C04B 2235/3895: Non-oxides with a defined oxygen content, e.g. SiOC, TiON
- C04B 2235/5296: with a defined aspect ratio, e.g. indicating sphericity
- C04B 2235/5436: micrometer sized, i.e. from 1 to 100 micron
- C04B 2235/5445: submicron sized, i.e. from 0,1 to 1 micron
- H10H 20/8512: {Wavelength conversion materials}
- H10W 72/01515: {Forming coatings}
- H10W 72/075: {of bond wires}
- H10W 72/5522: {comprising gold [Au]}
- H10W 74/00: Encapsulations, e.g. protective coatings
- H10W 90/756: {between a chip and a stacked lead frame, conducting package substrate or heat sink}
- Y10T 428/265: 1 mil or less
- C09K: MATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
- C04B: LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE {(roofing granules E04D7/005)}; CERAMICS (devitrified glass-ceramics C03C10/00); REFRACTORIES; TREATMENT OF NATURAL STONE
- H05B: ELECTRIC HEATING; ELECTRIC LIGHT SOURCES NOT OTHERWISE PROVIDED FOR; CIRCUIT ARRANGEMENTS FOR ELECTRIC LIGHT SOURCES, IN GENERAL
- H10H: INORGANIC LIGHT-EMITTING SEMICONDUCTOR DEVICES HAVING POTENTIAL BARRIERS
- H10W: GENERIC PACKAGES, INTERCONNECTIONS, CONNECTORS OR OTHER CONSTRUCTIONAL DETAILS OF DEVICES COVERED BY CLASS H10
- Y10T: TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION

## Abstract

The present invention provides a fluorescent substance exhibiting higher brightness as compared to conventional fluorescent substances, a method for producing the same, and a light-emitting device using such a fluorescent substance. Specifically, the fluorescent substance comprises an α-sialon crystal structure having the same crystal structure with an α-type silicon nitride crystal, which includes at least an M(0) element (where M(0) represents one or two elements selected from Sr and La), an M(1) element (where M(1) represents one or more elements selected from Mn, Ce, Pr, Nd, Sm, Eu, Tb, Dy, Ho, Er, Tm and Yb), Si, Al, and nitrogen.

## Claims

### Claim 1

A fluorescent substance comprising an α-sialon crystal structure having the same crystal structure with an α-type silicon nitride crystal, which includes at least an M(0) element (where M(0) represents one or two elements selected from Sr and La), an M(1) element (where M(1) represents one or more elements selected from Mn, Ce, Pr, Nd, Sm, Eu, Tb, Dy, Ho, Er, Tm, and Yb), Si, Al, and nitrogen.

### Claim 2 (depends on 1)

The fluorescent substance according to claim 1, further including oxygen.

### Claim 3 (depends on 1)

The fluorescent substance according to claim 1, further including an M(2) element (where M(2) represents one or more elements selected from Li, Na, Be, Mg, Ca, Ba, Sc, Y, Gd, and Lu).

### Claim 4 (depends on 1)

The fluorescent substance according to claim 1, wherein said fluorescent substance comprises a composition represented by the following composition formula:
M(0)xM(1)yM(2)zSi12-(m+n)Al(m+n)OnN16-n
where x, y, and z representing the composition ratio satisfy the inequations of 0.01≦x≦4, 0.001<y≦2, and 0≦z≦2, and
m and n representing the composition ratio satisfy the inequations of 0.8·me≦m≦1.2·me and 0≦n<4 provided that me=x·v(0)+y·v(1)+z·v(2) (where v(0) represents a valence of the M(0) ion, v(1) represents a valence of the M(1) ion, and v(2) represents a valence of the M(2) ion).

### Claim 5

A fluorescent substance comprising an α-sialon crystal structure having the same crystal structure with an α-type silicon nitride crystal, which includes at least an M(0) element (where M(0) represents one or two elements selected from Sr and La), an M(1) element (where M(1) represents one or more elements selected from Mn, Ce, Pr, Nd, Sm, Eu, Tb, Dy, Ho, Er, Tm, and Yb), Si, Al, and nitrogen, wherein
the fluorescent substance comprises an α-sialon powder, and an amount of oxygen included in the α-sialon powder is larger than the value calculated on the basis of the following composition formula, by a difference within the range of 0.4 mass % or less:
M(0)xM(1)yM(2)zSi12-(m+n)Al(m+n)OnN16-n
where x, y, and z representing the composition ratio satisfy the inequations of 0.01≦x≦4, 0.001<y≦2, and 0≦z≦2, and
m and n representing the composition ratio satisfy the inequations of 0.8·me≦m≦1.2·me and 0≦n<4 provided that me=x·v(0)+y·v(1)+z·v(2) (where v(0) represents a valence of the M(0) ion, v(1) represents a valence of the M(1) ion, and v(2) represents a valence of the M(2) ion).

### Claim at position 6

-14. (canceled)

### Claim 15

A method for producing a fluorescent substance comprising an α-sialon crystal having the same crystal structure with an α-type silicon nitride crystal, which includes at least an M(0) element (where M(0) represents one or two elements selected from Sr and La), an M(1) element (where M(1) represents one or more elements selected from Mn, Ce, Pr, Nd, Sm, Eu, Tb, Dy, Ho, Er, Tm, and Yb), Si, Al, and nitrogen, wherein
one or more raw materials selected from MSiN2, M2Si5N8, M3Al2N4, and MSi6N8 are at least used as a starting material, in the form of an M-containing compound (where M represents one or more elements selected from divalent elements in the element group consisting of Sr and M(1)).

### Claim 16

A method for producing a fluorescent substance comprising an α-sialon crystal structure having the same crystal structure with an α-type silicon nitride crystal, which includes at least Sr, an M(1) element (where M(1) represents one or more elements selected from Mn, Ce, Pr, Nd, Sm, Eu, Tb, Dy, Ho, Er, Tm, and Yb), Si, Al, and nitrogen, wherein the method comprises:
a process of preparing one or more raw materials selected from MSiN2, M2Si5N8, M3Al2N4, and MSi6N8 as a starting material, in the form of an M-containing compound (where M represents one or more elements selected from divalent elements in the element group consisting of Sr and M(1));
a process of kneading the raw materials to yield a raw material mixture;
a process of forming a compact of the raw material mixture;
a process of calcinating the compact; and
a process of heat-treating the calcinated compact.

### Claim 17

(canceled)

### Claim 18 (depends on 15)

The method for producing a fluorescent substance according to claim 15, wherein LiSi2N3 is used as a starting material in the form of an Li-containing compound, for further including an M(2) element (where M(2) represents one or more elements selected from Li, Na, Be, Mg, Ca, Ba, Sc, Y, Gd, and Lu).

### Claim 19 (depends on 16)

The method for producing a fluorescent substance according to claim 16, wherein a fluorescent substance powder having a target composition previously synthesized as a seed, is added to said raw material mixture.

### Claim at position 12

-28. (canceled)

### Claim 29 (depends on 1)

A fluorescent substance comprising a transparent layer in a thickness of (10 to 180)/n (unit: nanometer) on at least a part of the surfaces of α-sialon particles constituting the fluorescent substance according to claim 1, provided that n represents a refractive index of the transparent layer within the range of 1.2 to 2.5.

### Claim 30

(canceled)

### Claim 31

A method for producing a fluorescent substance, wherein the method comprises: suspending a fluorescent substance comprising an α-sialon crystal structure having the same crystal structure with an α-type silicon nitride crystal, which includes at least an M(0) element (where M(0) represents one or two elements selected from Sr and La), an M(1) element (where M(1) represents one or more elements selected from Mn, Ce, Pr, Nd, Sm, Eu, Tb, Dy, Ho, Er, Tm, and Yb), Si, Al, and nitrogen, in an organic solvent; and adding an organometallic complex or metalalkoxide dropwise thereto, to thereby form a transparent layer in a thickness of (10 to 180)/n (unit: nanometer) on at least a part of the surfaces of a-sialon particles, provided that n represents a refractive index of the transparent layer within the range of 1.2 to 2.5.

### Claim 32

A method for producing a fluorescent substance, wherein the method comprises; suspending a fluorescent substance comprising an α-sialon crystal structure having the same crystal structure with an α-type silicon nitride crystal, which includes at least an M(0) element (where M(0) represents one or two elements selected from Sr and La), an M(1) element (where M(1) represents one or more elements selected from Mn, Ce, Pr, Nd, Sm, Eu, Tb, Dy, Ho, Er, Tm, and Yb), Si, Al, and nitrogen, in water; and adding a metal salt aqueous solution dropwise thereto while keeping a constant pH, to thereby form a transparent layer in a thickness of (10 to 180)/n (unit: nanometer) on at least a part of the surfaces of a-sialon particles, provided that n represents a refractive index of the transparent layer within the range of 1.2 to 2.5.

### Claim 33 (depends on 1)

A light-emitting device comprising a light emitting light source and a fluorescent substance, wherein the fluorescent substance according to claim 1 is used.

### Claim 34 (depends on 1)

A light-emitting device comprising a light emitting light source and a fluorescent substance, wherein the fluorescent substance according to claim 1 and CaAlSiN3:Eu are used.

### Claim at position 19

-37. (canceled)

### Claim 38 (depends on 29)

A light-emitting device comprising a light emitting light source and a fluorescent substance, wherein the fluorescent substance according to claim 29 is used.

### Claim 39 (depends on 29)

A light-emitting device comprising a light emitting light source and a fluorescent substance, wherein the fluorescent substance according to claim 29 and CaAlSiN3:Eu are used.