WO2009072043A1 - Light emitting device comprising a green emitting sialon-based material - Google Patents
Light emitting device comprising a green emitting sialon-based material Download PDFInfo
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- WO2009072043A1 WO2009072043A1 PCT/IB2008/054994 IB2008054994W WO2009072043A1 WO 2009072043 A1 WO2009072043 A1 WO 2009072043A1 IB 2008054994 W IB2008054994 W IB 2008054994W WO 2009072043 A1 WO2009072043 A1 WO 2009072043A1
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- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09K—MATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
- C09K11/00—Luminescent, e.g. electroluminescent, chemiluminescent materials
- C09K11/08—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials
- C09K11/0883—Arsenides; Nitrides; Phosphides
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- C04B35/00—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
- C04B35/515—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on non-oxide ceramics
- C04B35/58—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on non-oxide ceramics based on borides, nitrides, i.e. nitrides, oxynitrides, carbonitrides or oxycarbonitrides or silicides
- C04B35/597—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on non-oxide ceramics based on borides, nitrides, i.e. nitrides, oxynitrides, carbonitrides or oxycarbonitrides or silicides based on silicon oxynitride, e.g. SIALONS
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- C04B35/00—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
- C04B35/622—Forming processes; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
- C04B35/626—Preparing or treating the powders individually or as batches ; preparing or treating macroscopic reinforcing agents for ceramic products, e.g. fibres; mechanical aspects section B
- C04B35/62605—Treating the starting powders individually or as mixtures
- C04B35/6261—Milling
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- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09K—MATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
- C09K11/00—Luminescent, e.g. electroluminescent, chemiluminescent materials
- C09K11/08—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials
- C09K11/77—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials containing rare earth metals
- C09K11/7728—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials containing rare earth metals containing europium
- C09K11/77348—Silicon Aluminium Nitrides or Silicon Aluminium Oxynitrides
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- C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
- C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
- C04B2235/30—Constituents and secondary phases not being of a fibrous nature
- C04B2235/32—Metal oxides, mixed metal oxides, or oxide-forming salts thereof, e.g. carbonates, nitrates, (oxy)hydroxides, chlorides
- C04B2235/3205—Alkaline earth oxides or oxide forming salts thereof, e.g. beryllium oxide
- C04B2235/3213—Strontium oxides or oxide-forming salts thereof
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- C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
- C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
- C04B2235/30—Constituents and secondary phases not being of a fibrous nature
- C04B2235/32—Metal oxides, mixed metal oxides, or oxide-forming salts thereof, e.g. carbonates, nitrates, (oxy)hydroxides, chlorides
- C04B2235/3224—Rare earth oxide or oxide forming salts thereof, e.g. scandium oxide
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- C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
- C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
- C04B2235/30—Constituents and secondary phases not being of a fibrous nature
- C04B2235/38—Non-oxide ceramic constituents or additives
- C04B2235/3852—Nitrides, e.g. oxynitrides, carbonitrides, oxycarbonitrides, lithium nitride, magnesium nitride
- C04B2235/3865—Aluminium nitrides
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- C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
- C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
- C04B2235/30—Constituents and secondary phases not being of a fibrous nature
- C04B2235/38—Non-oxide ceramic constituents or additives
- C04B2235/3852—Nitrides, e.g. oxynitrides, carbonitrides, oxycarbonitrides, lithium nitride, magnesium nitride
- C04B2235/3873—Silicon nitrides, e.g. silicon carbonitride, silicon oxynitride
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- C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
- C04B2235/70—Aspects relating to sintered or melt-casted ceramic products
- C04B2235/74—Physical characteristics
- C04B2235/76—Crystal structural characteristics, e.g. symmetry
- C04B2235/761—Unit-cell parameters, e.g. lattice constants
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- C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
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- C04B2235/77—Density
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- C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
- C04B2235/70—Aspects relating to sintered or melt-casted ceramic products
- C04B2235/96—Properties of ceramic products, e.g. mechanical properties such as strength, toughness, wear resistance
- C04B2235/9607—Thermal properties, e.g. thermal expansion coefficient
Definitions
- Light emitting device comprising a green emitting SiAlON-based material
- the present invention is directed to light emitting devices, especially to the field of LEDs.
- Phosphors comprising silicates, phosphates (for example, apatite) and aluminates as host materials, with transition metals or rare earth metals added as activating materials to the host materials, are widely known.
- phosphates for example, apatite
- aluminates as host materials, with transition metals or rare earth metals added as activating materials to the host materials.
- transition metals or rare earth metals added as activating materials to the host materials
- a light emitting device especially a LED comprising a green emitting material essentially of the composition
- green emitting especially means and/or includes that the material shows an emission in the visible range (upon suitable excitation) with a maximum between 500 and 600 nm.
- essentially means especially that > 95 %, preferably > 97 % and most preferred > 99 % of the material has the desired composition.
- the stability of the material is usually improved comprising to materials of the prior art.
- the material has usually a very high thermal, especially photothermal stability.
- y is > 0.5 to ⁇ 3. It has been shown that by doing so, a "tuning" of the spectrum is possible for many applications. E.g. substitution of a part of Sr by Ca leads to a red shift of the emission while substitution of a part of Sr by Ba leads to a blue shift of the emission.
- a is set to be 0 ⁇ a
- x is set to be 1 ⁇ x ⁇ 4, more preferred X is set to be 1.5 ⁇ x ⁇ 3
- the green emitting material has a orthorhombic crystal structure. It has been found for many applications within the present invention that by doing so, the properties (especially the emission profile) of the material may be further enhanced.
- the crystal structure of the green emitting material Eu (II) and/or Ce (III) are positioned in a 6- or 7-fold coordination sphere.
- the inventors believe that by setting the material this way, the emission band of the material can be narrowed for many applications.
- the half- width of the emission band in the visible range is ⁇ 90 nm.
- the material is provided as a ceramic material.
- ceramic material in the sense of the present invention means and/or includes especially a crystalline or polycrystalline compact material or composite material with a controlled amount of pores or which is pore free.
- polycrystalline material in the sense of the present invention means and/or includes especially a material with a volume density larger than 90 percent of the main constituent, consisting of more than 80 percent of single crystal domains, with each domain being larger than 0.5 ⁇ m in diameter and may have different crystallo graphic orientations.
- the single crystal domains may be connected by amorphous or glassy material or by additional crystalline constituents.
- the photothermal stability of the ceramic material is >80% to ⁇ 100% after exposure of the ceramic material for 1000 hrs at 200 0 C with a light power density of 10W/cm 2 and an average photon energy of 2.75 eV.
- photothermal stability in the sense of the present invention especially means and/or includes the conservation of the luminescence intensity under simultaneous application of heat and high intensity excitation, i.e. a photothermal stability of 100% indicates that the material is virtually unaffected by the simultaneous irradiation and heat up.
- the photothermal stability of the ceramic material is >82.5% to ⁇ 95%, preferably >85% to ⁇ 97%, after exposure of the ceramic material for 1000 hrs at 200 0 C with a light power density of 10W/cm 2 and an average photon energy of 2.75 eV.
- the thermal conductivity of the ceramic material is > 0.04 W cm “ 1 K “1 to ⁇ 0.15 W cm “ 1 K “1
- the ceramic material shows a transparency for normal incidence in air of >10 % to ⁇ 85 % for light in the wavelength range from > 550 nm to ⁇ 1000 nm.
- the transparency for normal incidence is in air of >20 % to ⁇ 80 % for light in the wavelength range from > 550 nm to ⁇ 1000 nm, more preferred >30 % to ⁇ 75 % and most preferred > 40% to ⁇ 70% for a light in the wavelength range from > 550 nm to ⁇ 1000 nm.
- transparency in the sense of the present invention means especially that > 10% preferably >20%, more preferred >30%, most preferred >40% and ⁇ 85% of the incident light of a wavelength, which cannot be absorbed by the material, is transmitted through the sample for normal incidence in air (at an arbitrary angle). This wavelength is preferably in the range of > 550 nm and ⁇ 1000 nm.
- the ceramic material has a density of >95% and ⁇ 101% of the theoretical density.
- the ceramic material has a density of >97% and ⁇ 100% of the theoretical density.
- the densities lower than 100% according to the described preferred embodiment of the present invention are preferably obtained by sintering of the ceramic to a stage where still pores are present in the ceramic matrix. Most preferred are densities in the range >98.0% and ⁇ 99.8% with total pore volumes in the ceramic matrix within the >0.2 - ⁇ 2% range. A preferred mean pore diameter is in the >400 - ⁇ 1500 nm range.
- a light emitting device according to the present invention as well as a ceramic material as produced with the present method may be of use in a broad variety of systems and/or applications, amongst them one or more of the following: - Office lighting systems household application systems shop lighting systems, home lighting systems, accent lighting systems, - spot lighting systems, theater lighting systems, fiber-optics application systems, projection systems, self-lit display systems, - pixelated display systems, segmented display systems, warning sign systems, medical lighting application systems, indicator sign systems, and - decorative lighting systems portable systems automotive applications green house lighting systems
- Fig. 1 shows an XRD- pattern for a material according to Example I of the present invention
- Fig. 2 shows an emission and excitation spectrum of the material according to Example I
- Fig. 3 shows a picture describing a first aspect of the crystal structure of the material of Example I of the present invention.
- Fig. 4 shows a picture describing a second aspect of the crystal structure of the material of Example I of the present invention.
- Fig. 5 shows a picture showing the coordination sites of the luminescent ions in the material of Example I
- Fig.6 shows a photograph of the macroscopic structure of the material of example I.
- Example I which - in a mere illustrative fashion - is one Example of a inventive green emitting material.
- Fig. 1 shows the XRD pattern of the SiAlON phosphor that comprises sharp and diffuse reflections due to stacking disorder within the crystals.
- the degree of disorder can be influenced by dwell time and cooling rate of the firing profile. Surprisingly it was found out that a high degree of disorder of the layer stacking has no influence on the efficiency of the luminescent material.
- Fig. 2 shows the Emission (EM, 450 nm excitation) and excitation (EXC, monitored at 525 nm) spectra of the material of Example I.
- this material is very useful for green emitting applications alone; however, with further red emitting phosphors, such as e.g.
- the material crystallizes in a complex structure which is built up of stacks of undulated layers of corner connected (Si 5 Al)(O ,N) 4 tetrahedra with Si as the main center cation and more planar layers of corner and edge connected (Si 5 Al)(O 5 N) 4 tetrahedra with Al as the main center cation.
- Fig. 2 shows a part of the planar layer of corner and edge connected (Si 5 Al)(O 5 N) 4 tetrahedra.
- the edge sharing tetrahedra are preferably occupied by Al atoms, however, also Si atoms can be built in if the charge compensation is properly done by adjusting the N/O ratio.
- the unit cell of the structure is marked by index IV.
- index IV In one formula unit there exist 30 3-fold connecting anion sites that can only be occupied by N atoms and 7 2-fold connecting anion sites that can be occupied by both N and O.
- the structure comprises a layer of edge and vortex connected tetrahedra. It has been found that usually the edge sharing tetrahedra sites are occupied by Al 5 although this is no "must".
- Fig. 5 shows the coordination of the three crystallo graphically independent cation sites present in the structure of the material of the present invention (which are marked as SrI 5 Sr 2 Sr3 although of course Eu will also occupy this sites). All sites show a similar coordination sphere with 6- or 7-fold coordination (contacts shorter than 3 A) which (although not being bound to this interpretation) could help to explain the rather narrow emission band of the Eu(II) doped phosphor material.
- Fig. 6 shows a photograph of the macroscopic structure of the material of example I. Surprisingly, the material grows voluntarily in rather large plate- shaped crystallites.
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- Luminescent Compositions (AREA)
Abstract
Description
Claims
Priority Applications (6)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
US12/745,701 US8546845B2 (en) | 2007-12-03 | 2008-11-27 | Light emitting device comprising a green emitting sialon-based material |
KR1020107014782A KR101535162B1 (en) | 2007-12-03 | 2008-11-27 | Light emitting device comprising a green emitting sialon-based material |
EP08856568A EP2229426B1 (en) | 2007-12-03 | 2008-11-27 | Light emitting device comprising a green emitting sialon-based material |
AT08856568T ATE510901T1 (en) | 2007-12-03 | 2008-11-27 | LIGHT EMITTING DEVICE HAVING A SIALON-BASED GREEN LIGHT EMITTING MATERIAL |
CN200880118916XA CN101883835B (en) | 2007-12-03 | 2008-11-27 | Light emitting device comprising a green emitting SiAlON-based material |
JP2010535497A JP5723597B2 (en) | 2007-12-03 | 2008-11-27 | Light emitting device containing a material based on green light emitting SiAlON |
Applications Claiming Priority (2)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
EP07122138.6 | 2007-12-03 | ||
EP07122138 | 2007-12-03 |
Publications (1)
Publication Number | Publication Date |
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WO2009072043A1 true WO2009072043A1 (en) | 2009-06-11 |
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Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
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PCT/IB2008/054994 WO2009072043A1 (en) | 2007-12-03 | 2008-11-27 | Light emitting device comprising a green emitting sialon-based material |
Country Status (9)
Country | Link |
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US (1) | US8546845B2 (en) |
EP (1) | EP2229426B1 (en) |
JP (1) | JP5723597B2 (en) |
KR (1) | KR101535162B1 (en) |
CN (1) | CN101883835B (en) |
AT (1) | ATE510901T1 (en) |
RU (1) | RU2010127293A (en) |
TW (1) | TW200938612A (en) |
WO (1) | WO2009072043A1 (en) |
Cited By (15)
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WO2011016486A1 (en) * | 2009-08-06 | 2011-02-10 | 昭和電工株式会社 | Fluorescent substance, process for producing same, and luminescent device including same |
WO2011024818A1 (en) | 2009-08-26 | 2011-03-03 | 三菱化学株式会社 | Semiconductor white light-emitting device |
JP2011508001A (en) * | 2007-12-19 | 2011-03-10 | コーニンクレッカ フィリップス エレクトロニクス エヌ ヴィ | Red light emitting SiAlON base material |
JP2011052099A (en) * | 2009-09-01 | 2011-03-17 | Mitsubishi Chemicals Corp | Method for producing nitride phosphor |
WO2011105571A1 (en) | 2010-02-26 | 2011-09-01 | 三菱化学株式会社 | Halophosphate phosphor and white light emitting device |
WO2011122655A1 (en) | 2010-03-30 | 2011-10-06 | 三菱化学株式会社 | Light-emitting device |
WO2011122576A1 (en) | 2010-03-30 | 2011-10-06 | 三菱化学株式会社 | Light-emitting device |
WO2012114640A1 (en) | 2011-02-25 | 2012-08-30 | 三菱化学株式会社 | Halophosphate fluorescent body and white light emitting device |
JP2013127055A (en) * | 2011-11-15 | 2013-06-27 | National Institute For Materials Science | Phosphor, production method thereof, illumination device and image display device |
US8501039B2 (en) | 2010-02-19 | 2013-08-06 | Kabushiki Kaisha Toshiba | Fluorescent material and light-emitting device employing the same |
WO2013147195A1 (en) | 2012-03-30 | 2013-10-03 | 三菱化学株式会社 | Semiconductor light-emitting device, and illumination device |
CN104024377A (en) * | 2011-11-07 | 2014-09-03 | 独立行政法人物质·材料研究机构 | Phosphor and production method therefor, and light emission device and image display device using phosphor |
US8829780B2 (en) | 2010-06-25 | 2014-09-09 | Mitsubishi Chemical Corporation | White semiconductor light emitting device |
US20140307415A1 (en) * | 2011-02-06 | 2014-10-16 | National Institute For Materials Science | Phosphor, production method for the same, and light-emitting device |
WO2015018474A1 (en) * | 2013-08-08 | 2015-02-12 | Merck Patent Gmbh | Luminescent substances |
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KR101077990B1 (en) | 2010-02-12 | 2011-10-31 | 삼성엘이디 주식회사 | Phosphor, light emitting device, surface light source apparatus, display apparatus and illumination apparatus |
US8679367B2 (en) * | 2012-08-09 | 2014-03-25 | Intematix Corporation | Green-emitting (oxy)nitride-based phosphors and light-emitting device using the same |
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Also Published As
Publication number | Publication date |
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ATE510901T1 (en) | 2011-06-15 |
RU2010127293A (en) | 2012-01-10 |
US20100244076A1 (en) | 2010-09-30 |
TW200938612A (en) | 2009-09-16 |
US8546845B2 (en) | 2013-10-01 |
EP2229426B1 (en) | 2011-05-25 |
JP5723597B2 (en) | 2015-05-27 |
JP2011505451A (en) | 2011-02-24 |
KR101535162B1 (en) | 2015-07-09 |
KR20100107000A (en) | 2010-10-04 |
CN101883835B (en) | 2013-05-29 |
CN101883835A (en) | 2010-11-10 |
EP2229426A1 (en) | 2010-09-22 |
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