# US 10,479,935 B2 · Fluorescent material, method of producing the same, and light emitting device using the same

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- Number: US 10,479,935 B2
- Document ID: US10479935B2
- Status: Granted
- Kind: B2
- Application number: 15/843,727
- Filed: 2017-12-15
- Published: 2018-06-21
- Granted: 2019-11-19
- Earliest claimed: 2016-12-15
- Assignees: National Institute for Materials Science; Nichia Corporation
- Applicants: National Institute for Materials Science; Nichia Corporation
- Inventors: Naoto Hirosaki; Takayuki Shinohara; Shoji Hosokawa
- Web page: https://patentgrep.com/patent/US10479935B2

## CPC

- C09K 11/77348: {Silicon Aluminium Nitrides or Silicon Aluminium Oxynitrides}
- C01B 21/0826: {Silicon aluminium oxynitrides, i.e. sialons}
- C01F 17/30: Compounds containing rare earth metals and at least one element other than a rare earth metal, oxygen or hydrogen, e.g. La4S3Br6 (C01F17/247 - C01F17/294 take precedence)
- C01P 2002/72: by d-values or two theta-values, e.g. as X-ray diagram
- C01P 2002/84: by UV- or VIS- data
- H10H 20/8512: {Wavelength conversion materials}
- C09K: MATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
- C01B: NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; {METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C}
- C01F: COMPOUNDS OF THE METALS BERYLLIUM, MAGNESIUM, ALUMINIUM, CALCIUM, STRONTIUM, BARIUM, RADIUM, THORIUM, OR OF THE RARE-EARTH METALS (metal hydrides {monoborane, diborane or addition complexes thereof} C01B6/00; salts of oxyacids of halogens C01B11/00; peroxides, salts of peroxyacids C01B15/00; sulfides or polysulfides of magnesium, calcium, strontium, or barium C01B17/42; thiosulfates, dithionites, polythionates C01B17/64; compounds containing selenium or tellurium C01B19/00; binary compounds of nitrogen with metals C01B21/06; azides C01B21/08; {compounds other than ammonia or cyanogen containing nitrogen and non-metals and optionally metals C01B21/082; amides or imides of silicon C01B21/087}; metal {imides or} amides C01B21/092, {C01B21/0923}; nitrites C01B21/50; {compounds of noble gases C01B23/0005}; phosphides C01B25/08; salts of oxyacids of phosphorus C01B25/16; carbides C01B32/90; compounds containing silicon C01B33/00; compounds containing boron C01B35/00; compounds having molecular sieve properties but not having base-exchange properties C01B37/00; compounds having molecular sieve and base-exchange properties, e.g. crystalline zeolites, C01B39/00; cyanides C01C3/08; salts of cyanic acid C01C3/14; salts of cyanamide C01C3/16; thiocyanates C01C3/20; {double sulfates of magnesium with sodium or potassium C01D5/12; with other alkali metals C01D15/00, C01D17/00})
- C01P: INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
- H10H: INORGANIC LIGHT-EMITTING SEMICONDUCTOR DEVICES HAVING POTENTIAL BARRIERS

## Abstract

Provided are a fluorescent material having a high light emission intensity, a method for producing the same, and a light emitting device using the same. The present fluorescent material includes a composition represented by formula (I): SiuEuvAlwOxNy, wherein when the sum of a parameter u and a parameter w is taken as 13, parameters u, v, w, x, and y in the formula (I) satisfy the following formulae (1) to (5). 2.77≤u≤2.88 (1) 0.04≤v≤0.08 (2) 10.12≤w≤10.23 (3) 0.42≤x≤0.95 (4) 12.89≤y≤13.65 (5)

## Claims

### Claim 1

A fluorescent material comprising a composition represented by formula (I): SiuEuvAlwOxNy, wherein when the sum of a parameter u and a parameter w is taken as 13, parameters u, v, w, x, and y in the formula (I) satisfy the following formulae (1) to (5):
2.77≤u≤2.88 (1),
0.04≤v≤0.08 (2),
10.12≤w≤10.23 (3),
0.42≤x≤0.95 (4), and
12.89≤y≤13.65 (5).

### Claim 2 (depends on 1)

The fluorescent material according to claim 1, which has, as a host crystal, a crystal structure identical with a crystal structure of an inorganic compound represented by a formula: Si2.24Al10.76O0.76N13.24.

### Claim 3 (depends on 1)

The fluorescent material according to claim 1, wherein in the composition represented by the formula (I), a molar ratio of silicon to aluminum (Si/Al ratio) is in a range of 0.20 or more and 0.30 or less, and a molar ratio of oxygen to nitrogen (O/N ratio) is in a range of 0.01 or more and 0.08 or less.

### Claim 4 (depends on 1)

The fluorescent material according to claim 1, which includes a crystal phase in which when in an X-ray diffraction pattern by CuKα rays, an intensity of a diffraction peak at a Bragg angle (2θ) in a range of 35.4° or more and 36.0° or less is taken as 100%,
a relative intensity of a diffraction peak at a Bragg angle (2θ) in a range of 33.0° or more and 33.6° or less is 10% or more and 45% or less,
a relative intensity of a diffraction peak at a Bragg angle (2θ) in a range of 37.6° or more and 38.2° or less is 8% or more and 24% or less,
a relative intensity of a diffraction peak at a Bragg angle (2θ) in a range of 59.8° or more and 60.4° or less is 3% or more and 30% or less, and
a relative intensity of a diffraction peak at a Bragg angle (2θ) in a range of 60.5° or more and 61.1° or less is 6% or more and 32% or less.

### Claim 5 (depends on 1)

A light emitting device comprising the fluorescent material according to claim 1 and an excitation light source.

### Claim 6 (depends on 5)

The light emitting device according to claim 5, wherein the excitation light source has a light emission peak wavelength in a wavelength region of from a near ultraviolet light to a visible light.

### Claim 7

A method of producing a fluorescent material, comprising subjecting a raw material mixture including EuF3 to a heat treatment to obtain a fluorescent material comprising a composition represented by formula (I): SiuEuvAlwOxNy, wherein when the sum of a parameter u and a parameter w is taken as 13, parameters u, v, w, x, and y in the formula (I) satisfy the following formulae (1) to (5):
2.77≤u≤2.88 (1),
0.04≤b≤0.08 (2),
10.12≤w≤10.23 (3),
0.42≤x≤0.95 (4), and
12.89≤y≤13.65 (5).

### Claim 8 (depends on 7)

The method of producing a fluorescent material according to claim 7, wherein in the composition, a molar ratio of silicon to aluminum (Si/Al ratio) is in a range of 0.20 or more and 0.30 or less, and a molar ratio of oxygen to nitrogen (O/N ratio) is in a range of 0.01 or more and 0.08 or less.
