WO2007052200A1 - Light emitting device with an improved caalsin light converting material - Google Patents

Light emitting device with an improved caalsin light converting material Download PDF

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Publication number
WO2007052200A1
WO2007052200A1 PCT/IB2006/053969 IB2006053969W WO2007052200A1 WO 2007052200 A1 WO2007052200 A1 WO 2007052200A1 IB 2006053969 W IB2006053969 W IB 2006053969W WO 2007052200 A1 WO2007052200 A1 WO 2007052200A1
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WIPO (PCT)
Prior art keywords
light
caalsin
converting material
emitting device
systems
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Ceased
Application number
PCT/IB2006/053969
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English (en)
French (fr)
Inventor
Peter J. Schmidt
Joerg Meyer
Walter Mayr
Wolfgang Busselt
Hans-Helmut Bechtel
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Philips Intellectual Property and Standards GmbH
Koninklijke Philips NV
Original Assignee
Philips Intellectual Property and Standards GmbH
Koninklijke Philips Electronics NV
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Priority to US12/092,745 priority Critical patent/US8159126B2/en
Application filed by Philips Intellectual Property and Standards GmbH, Koninklijke Philips Electronics NV filed Critical Philips Intellectual Property and Standards GmbH
Priority to EP06821213.3A priority patent/EP1948757B1/en
Priority to JP2008538472A priority patent/JP5356822B2/ja
Priority to CN200680041470.6A priority patent/CN101305072B/zh
Publication of WO2007052200A1 publication Critical patent/WO2007052200A1/en
Anticipated expiration legal-status Critical
Ceased legal-status Critical Current

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Definitions

  • the present invention is directed to light emitting devices, especially to the field of LEDs.
  • So-called phosphor converted light emitting devices comprising an electroluminescent light source and a light converting element to absorb light emitted from the light source at least partially and to re-emit secondary light with longer wavelengths are know from prior art.
  • the scope of LEDs comprising a CaAlSiN light converting phosphor material has been investigated and in this regard it has been found that such a material can be used in LEDs.
  • An example is e.g. described in the EP05101834.9 which is incorporated by reference.
  • a light-emitting device with a light source to emit primary light and a light conversion layer to convert at least a part of the primary light into secondary light comprising a CaAlSiN light converting material with a transmissivity of > 10% to ⁇ 80% for a light in the wavelength range from > 580 to ⁇ lOOOnm.
  • a light emitting device especially a LED is provided, comprising a CaAlSiN light converting material with a transmissivity of >10% to ⁇ 80% for light in the wavelength area from > 580 to ⁇ 1000 nm.
  • the light source may be one or more light sources from the group inorganic LEDs, organic LEDs or laser diodes.
  • CaAlSiN light converting material comprises and/or includes especially the following materials:
  • additives which may be added during ceramic processing.
  • additives may be incorporated fully or in part into the final material, which then may also be a composite of several chemically different species (CaAlSiN crystallites embedded into a glassy matrix of slightly different composition) and particularly include such species known to the art as fluxes.
  • Suitable fluxes include alkaline earth - or alkaline - metal oxides and fluorides, SiO 2 and the like.
  • transmissivity in the sense of the present invention means especially that > 10%, according to an embodiment of the present invention >20%, according to an embodiment of the present invention >30%, according to an embodiment of the present invention >40% and ⁇ 80% of the incident light of a wavelength, which cannot be absorbed by the material, is transmitted through the sample for normal incidence in air .
  • This wavelength is according to an embodiment of the present invention, in the range of > 580 nm and ⁇ IOOO nm.
  • the features of the light- emitting device may in most applications be greatly improved (as will for some applications be described later on).
  • the CaAlSiN light converting material emits secondary light in the red visible light wavelength area with a maximum intensity at a wavelength of > 590 nm to ⁇ 700 nm. This allows building up a light emitting device with improved characteristics.
  • the CaAlSiN light converting material has an emission band in the red visible light wavelength area with a maximum of > 600 nm to ⁇ 680 nm, according to an embodiment of the present invention, of > 620 nm to ⁇ 670 nm.
  • the CaAlSiN light converting material emits secondary light with a wavelength distribution with a half- width of >50 nm to ⁇ 150 nm. This results in a sharp emission, which allows to further improve the light emitting device. According to an embodiment of the present invention, the CaAlSiN light converting material emits secondary light with a wavelength distribution with a half- width of > 60 nm to ⁇ 110 nm.
  • the CaAlSiN light converting material has > 97% to ⁇ 100 % of the theoretical single crystal density. By doing so, the CaAlSiN light converting material shows greatly improved mechanical and optical characteristics compared to materials with a lesser density. According to an embodiment of the present invention, the CaAlSiN light converting material has > 98 % to ⁇ 100 % of the theoretical single crystal density, according to an embodiment of the present invention > 99 % to ⁇ 100 % of the theoretical single crystal.
  • the CaAlSiN light converting material is a polycrystalline material.
  • polycrystalline material in the sense of the present invention means especially a material with a volume density larger than 90 percent of the main - A -
  • the constituent consisting of more than 80 percent of single crystal domains, with each domain being larger than 0.5 ⁇ m in diameter and having different crystallographic orientations.
  • the single crystal domains may be connected by amorphous or glassy material or by additional crystalline constituents.
  • the CaAlSiN converting material material is a ceramic material.
  • ceramic material in the sense of the present invention means especially a crystalline or polycrystalline compact material or composite material with a controlled amount of pores or which is free of pores.
  • the thickness of the ceramic material D is 30 ⁇ m ⁇ D ⁇ 5000 ⁇ m, according to an embodiment of the present invention 60 ⁇ m ⁇ D ⁇ 2000 ⁇ m and according to an embodiment of the present invention 80 ⁇ m ⁇ D ⁇ 1000 ⁇ m.
  • the shift of the maximum and/or the half- width of the secondary light emission in the red visible light wavelength area of the CaAlSiN light converting material is ⁇ 20 nm over the whole temperature range from >50°C to ⁇ 150 0 C.
  • the shift of the maximum and/or the half-width in the emission band in the red visible light wavelength area of the CaAlSiN light converting material is >0 nm to ⁇ 20 nm over the whole temperature range from. ⁇ 0°C to ⁇ 200 0 C, and according to an embodiment of the present invention, from >-40 o C to ⁇ 250 °C.
  • the shift of the maximum and/or the half-width in the the secondary light emission in the red visible light wavelength area of the CaAlSiN light converting material is >5 nm to ⁇ 18 nm over the whole temperature range from >50°C to ⁇ 150 0 C, According to an embodiment of the present invention, >0°C to ⁇ 200 0 C, and According to an embodiment of the present invention, from >-40°C to ⁇ 250 0 C.
  • the shift of the maximum and/or the half- width in the secondary light emission in the red visible light wavelength area of the CaAlSiN light converting material is >10 nm to ⁇ 15 nm over the whole temperature range from >50°C to ⁇ 150 0 C, According to an embodiment of the present invention, >0°C to ⁇ 200 0 C, and According to an embodiment of the present invention, from >-40°C to ⁇ 250 0 C.
  • the CaAlSiN light converting material is selected out of a material comprising (Cai_ x _ y _ z Sr x Ba y Mg z )i_ n Ali_ a+ bB a Sii_bN3-bO b :RE n with 0 ⁇ x,y,z ⁇ l, 0 ⁇ a ⁇ l, 0 ⁇ b ⁇ l, 0 ⁇ n ⁇ l and RE selected out of the group comprising Eu, Ce, or mixtures thereof.
  • the CaAlSiN light converting material is selected out of a material comprising (Cai_ x _ y _ z Sr x Ba y Mg z )i_ n Ali_ a+b B a Sii_ b N 3 - b O b :M n with 0 ⁇ x,y,z ⁇ l, 0 ⁇ a ⁇ l, 0 ⁇ b ⁇ l, 0.002 ⁇ n ⁇ 0.2 and M being a metal, according to an embodiment of the present invention selected out of the group comprising Ce, Pr, Nd, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb, Lu or mixtures thereof.
  • the CaAlSiN light converting material is selected out of a material comprising (Cai_ x _ y _ z Sr x Ba y Mg z )i_ n Ali_ a+b B a Sii_ b N 3 - b O b :RE n with 0 ⁇ x,y,z ⁇ l, 0 ⁇ a ⁇ l, 0 ⁇ b ⁇ l, 0.002 ⁇ n ⁇ 0.2 and RE selected out of the group comprising Eu, Ce, or mixtures thereof.
  • the CaAlSiN light converting material is selected out of a material comprising ((Cai_ x _ y _ z Sr x Ba y Mg z )i_ 0 ,.5 -.k+ 5*k*nRE n)i.a(Ali.
  • the CaAlSiN light converting material is selected out of a material comprising ((Cai_ x _ y _ z Sr x Ba y Mg z )i_ 0, 5 *k*nRE k+ n)i.a(Ali.
  • the CaAlSiN light converting material is selected out of a material comprising ((Cai_ x _ y _ z Sr x Ba y Mg z )i_ o, 5*k*n RE k+ n ) 1 _ a (Al 1 _ m B m ) b Si 2 . b N 3 .
  • the glass phase ratio of the CaAlSiN light converting material is >2 vol% to ⁇ 5 vol%, according to an embodiment of the present invention, >3 vol% to ⁇ 4 vol%. It has been shown in practice that materials with such a glass phase ratio show the improved characteristics, which are advantageous and desired for the present invention.
  • the term "vol%" denotes the volume fraction given in percentage.
  • glass phase in the sense of the present invention means especially non-crystalline grain boundary phases, which may be detected by scanning electron microscopy or transmission electron microscopy.
  • the surface roughness RMS (disruption of the planarity of a surface; measured as the geometric mean of the difference between highest and deepest surface features) of the surface(s) of the CaAlSiN light converting material is ⁇ O.OOl ⁇ m and ⁇ IOO ⁇ m.
  • the surface roughness of the surface(s) of the CaAlSiN light converting material is ⁇ O.Ol ⁇ m and ⁇ IO ⁇ m, according to an embodiment of the present invention ⁇ O.l ⁇ m and ⁇ 5 ⁇ m, according to an embodiment of the present invention ⁇ O.l 5 ⁇ m and ⁇ 3 ⁇ m. and according to an embodiment of the present invention >0.2 ⁇ m and ⁇ 2 ⁇ m.
  • the specific surface area of the CaAlSiN light converting material structure is >10 "7 m 2 /g and ⁇ l m 2 /g.
  • the present invention furthermore relates to a method of producing a CaAlSiN light converting material for a light-emitting device according to the present invention comprising a sintering step.
  • the term "sintering step" in the sense of the present invention means especially densification of a precursor powder under the influence of heat, which may be combined with the application of uniaxial or isostatic pressure, without reaching the liquid state of the main constituents of the sintered material.
  • the sintering step is performed at ambient pressure, preferably in reducing or inert atmosphere.
  • method furthermore comprises the step of pressing the CaAlSiN precursor material to >50% to ⁇ 70 %, according to an embodiment of the present invention, >55% to ⁇ 60 % of its theoretical single crystal density before sintering. It has been shown in practice that this improves the sintering steps for most CaAlSiN light converting materials as described with the present invention.
  • the method of producing CaAlSiN light converting material for a light-emitting device according to the present invention comprises the following steps:
  • a first pressing step preferably a uniaxial pressing step at >10 kN using a suitable powder compacting tool with a mould in the desired shape (e.g. rod- or pellet- shape) and/ or a cold isostatic pressing step preferably at >3000 bar to ⁇
  • a hot pressing step preferably a hot isostatic pressing step preferably at > 100 bar to ⁇ 2500 bar and preferably at a temperature of ⁇ 1500 0 C to ⁇ 2000 0 C and/or a hot uniaxial pressing step preferably at > 100 bar to ⁇ 2500 bar and preferably at a temperature of ⁇ 1500 0 C to ⁇ 2000 0 C
  • a post annealing step at >1000°C to ⁇ 1700 0 C in inert atmosphere or air
  • the light-emitting device comprises a light emitting diode (LED), according to an embodiment of the present invention a LED based on AlInGaN material as the electroluminescent material.
  • LED light emitting diode
  • the light-emitting device comprises a first light converting material, according to an embodiment of the present invention a ceramic first light converting material, and a second light converting material.
  • this second light converting comprises a YAG :Ce material.
  • the light emitting device has a color temperature of >3000K to ⁇ 5000K, according to an embodiment of the present invention 3500K to ⁇ 4000K.
  • the present invention also includes a method of preparing a light-emitting device according to the present invention comprising the steps of:
  • steps (b) and (c) may be repeated ad libitum.
  • This method allows for most applications to define the color temperature of the light emitting device as desired and for most applications also to adjust the color temperature of the light-emitting device even after production.
  • step c) is performed by abrasion of either the CaIAlSiN material and/or the second luminescence color converter material.
  • step c) is performed by changing the ratio of the amount of CaAlSiN light converting material and the second light converting material.
  • this is performed by using plates or stripes of the CaAlSiN light converting material and the second luminescent color converter material, which are arranged laterally on the light emitting area of the LED chip.
  • the color adjustment is performed by changing the ratio of plates or stripes of the CaAlSiN light converting material towards the plates or stripes of the second light converting material.
  • color adjustment is performed by using several prefabricated LED chips which comprise certain different ratios of the CaAlSiN light converting material and second luminescent color converter material or comprise only one of the two materials, so that the adjustment may be performed by changing the brightness of the different LED chips in the light emitting device, or the amount of LED chips of a certain type.
  • the first option will result in a color tunable device.
  • the color temperature may be set by changing the doping level in either the CaAlSiN light converting material and the second luminescent color converter material or changing the host lattice of either the CaAlSiN light converting material and the second light converting material (e.g. by adding Ga, Gd or Lu in case of a YAG material and/or adding Sr, Ba, Mg or O in case of the CaAlSiN light converting material). These measures may be used alone or in combination with the methods stated above.
  • a light emitting device as well as a CaAlSiN light converting 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:
  • Fig. 1 shows an emission spectra of an LED comprising a CaAlSiN light converting material according to Example I of the present invention
  • Fig. 1 refers to (Cao.95Sro.o5)o.98AlSiN 3 :Euo.o2 (Example I) which was produced as follows:
  • the obtained powder was compressed into pellets, cold isostatically pressed at 3200 bar and sintered at 1700 0 C in forming gas atmosphere for 4h.
  • the resulting pellets displayed a closed porosity and were subsequently hot isostatically pressed at 2000 bar and 1700 0 C to obtain dense ceramics with >98% of the theoretical density.
  • Fig. 1 shows an emission spectra of this LED.

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JP2008538472A JP5356822B2 (ja) 2005-11-07 2006-10-27 向上したＣａＡｌＳｉＮ光変換材料を有する発光デバイス
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