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Definitions

• the invention relates to compounds consisting of Mn 2+ , Mg 2+ , Be 2+ , Ni 2+ , Co 2+ , Ru 4+ , Hf 4+ , Th 4+ -co-doped 1-1-2-alkaline earth silicone nitrides, their preparation and their use as phosphors and LED
• This concept is e.g. used to create certain corporate designs, e.g. for illuminated company logos, brands etc.
• Fluorescent-converted LEDs represent a significant lighting technology whose innovation potential leads to the increasing substitution of traditional artificial light sources (incandescent lamps, discharge lamps, etc.). While the semiconductor technology for LEDs is almost exhausted, the phosphors used offer room for improvement. For the LED
• red fluorescent (power) LEDs Manufacturers are constantly stressing the need for red fluorescent (power) LEDs. Required properties of red phosphors for the efficient and effective use in the LED are u. a .:
• fluorescent materials which fluoresce in the red and can be combined in principle with biow (or UV-LEDs) are, in particular: a) ortho-silicates:
• Ortho-silicates are far better suited for LEDs operating at currents below 350 mA (Source: M. Zachau, Presentation Phosphor Global Summit 2006, 15.03.2007).
• Covalent nitrides can be used in principle as a matrix for phosphors, because they have a large band gap, in which the Ground state and typically some to many excited states of the activator ions are located.
• Nitrides, caused by the high covalence, have a large nephelo-excitatory effect, reducing the energy of the lowest crystal field component of the excited 4f5d configuration of rare-earth activators, e.g. As Eu 2+ , Ce 3+ is reduced. This leads to long-wave excitation and emission of nitride phosphors (see Krevel et al., J. Alloys Compd. 1998, 2268, 272)
• Siliconitrides have a higher chemical stability than oxosilicon compounds (see Xie et al, Sei Tech Adv., Mater., 2007, 8, 588)
• silicon nitrides are suitable for doping with activator ions, such as Eu 2+ and Ce 3+ , in which at least an electron in the excited state is not shielded by the action of the crystal field (5s and 5d).
• activators have spectroscopic properties that are highly dependent on the environment (symmetry, covalency, coordination, field strength, bond lengths, lattice size).
• the high formal charge of nitrogen (N 3 " ) in contrast to the lower formal charge of
• Oxygen (O 2 " ) causes the activators in silicon nitrides to show a larger crystal field splitting of the 5d orbitals and the energetic center of gravity of the 5d orbitals is shifted to lower energy than in analogous Si-O materials. and emission bands of the activator have a spectral redshift
• the more stable and rigid grid of silicon nitrides unlike that of the oxo silicon compounds, tends to reduce the Stokes shift, thereby causing thermal quenching at higher temperatures and increasing conversion efficiency.
• the object of the present invention is therefore the o.g. 1-1-2 alkaline earth silicon nitrides to modify so that these compounds achieve an even higher light efficiency.
• the present invention thus provides compounds of the 1-1-2 alkaline earth silicon nitride type with europium doping which additionally contain co-dopants from the series manganese, magnesium, beryllium, nickel, cobalt,
• 1-1-2 alkaline earth silicon nitrides also called “1-1-2 nitrides or” 1-1-2 alkaline earth nitridosilicates
• M is an alkaline earth metal or a mixture of several alkaline earth metals.
• the y value (which stands for the atomic concentration of the co-dopants Me or Ma) is from 0.0005 to 0.2, more preferably from 0.001 to 0.02.
• the particle size of the compounds according to the invention is between 50 nm and 30 .mu.m, preferably between 1 .mu.m and 20 .mu.m, more preferably between 2 and 15 .mu.m.
• monovalent ions such as alkali or alkaline earth metals, e.g. Li, Na, K, Ca, Sr, Ba and halides such as F or Cl may be incorporated. These monovalent ions are preferably used as a flux in phosphor production and serve to increase the crystal quality, coarse particle size distribution and the
• Another object of the present invention is a compound obtainable by mixing silicon nitride, europium and calcium and / or strontium and / or barium-containing educts with at least one manganese, magnesium, beryllium, nickel, cobalt , Ruthenium, hafnium, thorium and / or zirconium-containing co-dopant
• Solid-state diffusion methods and subsequent thermal aftertreatment which may optionally contain a flux from the series of alkali or alkaline earth halides or a borate compound.
• a further subject matter of the present invention is a process for producing a compound of the europium-doped 1-1-2-alkaline earth-siliconitride type with the following process steps: a) producing an Eu-doped 1-1-2-alkaline earth-siliconitride compound, containing manganese, magnesium, beryllium, nickel, cobalt, ruthenium, hafnium, thorium and / or zirconium Co-doped materials by mixing at least 4 starting materials selected from silicon nitride, europium, calcium, strontium, barium, manganese, magnesium, beryllium, nickel, cobalt, ruthenium, hafnium, thorium and / or zirconium-containing materials, b) thermal aftertreatment of the Mn, Mg, Be, Ni, Co, Ru, Hf, Th and / or Zr-co-doped compound.
• the starting materials for the preparation of the compound consist of silicon nitride (8! 3 N 4 ), calcium hydride and europium fluoride and at least one Mn, Mg, Be, Ni, Co, Ru, Hf, Th and / or Zr-containing co-dopant.
• silicon nitride (8! 3 N 4 ), calcium hydride and europium fluoride and at least one Mn, Mg, Be, Ni, Co, Ru, Hf, Th and / or Zr-containing co-dopant.
• hydrides and fluorides and other inorganic and / or organic substances such as cyanamides, dicyanamides, cyanides, oxalates, malonates, fumarates, carbonates, citrates, ascorbates and acetylacetonates in
• thermal aftertreatment runs for several hours under reducing conditions, for. B with forming gas (e.g. 90/10), pure hydrogen and / or in ammonia
• the temperatures in the annealing process are between 1000 0 C and 1800 0 C, preferably from 1200 ° C to 1650 ° C.
• any desired external forms of the compounds or phosphors according to the invention such as spherical particles, platelets and structured materials and ceramics. According to the invention, these forms are combined under the term "shaped body.”
• the shaped body is preferably a "phosphor body”.
• Another object of the present invention is thus a molding containing the compounds of the invention, wherein it has a rough surface, the nanoparticles of SiO 2 , TiO 2 , Al 2 O 3 , ZnO, ZrO 2 and / or Y 2 O 3 or mixed oxides thereof and / or particles with the compound according to the invention with or without dopants from the series
• the molded article has a patterned (e.g., pyramidal) surface on the side opposite an LED chip (see WO2008 / 058619, Merck, which is fully incorporated by reference into the context of the present application).
• a patterned (e.g., pyramidal) surface on the side opposite an LED chip (see WO2008 / 058619, Merck, which is fully incorporated by reference into the context of the present application).
• the structured surface on the shaped article is produced by subsequent coating with a suitable material, which is already structured, or in a subsequent step by (photo) lithographic processes, etching processes or by writing processes with energy or matter beams or the action of mechanical forces.
• the shaped bodies according to the invention have a rough surface on the side opposite to an LED chip, the nanoparticles of SiO 2 , TiO 2 , Al 2 O 3, ZnO 2 , ZrO 2 and / or Y 2 O 3 or combinations of this
• a rough surface has a roughness of up to several 100 nm.
• the coated surface has the advantage that total reflection can be reduced or prevented and the
• the shaped bodies according to the invention have a refractive index-adapted layer on the surface facing away from the chip, which facilitates the decoupling of the primary radiation and / or the radiation emitted by the phosphor body.
• the shaped bodies have a closed surface coating consisting of SiO 2 , TiO 2 , Al 2 U 3 ,
• This surface coating has the advantage that an adaptation of the refractive index to the environment can be achieved by a suitable graduation of the refractive indices of the coating materials. In this case, the scattering of the light at the surface of the phosphor is reduced and a larger proportion of the light can penetrate into the phosphor where it is absorbed and converted. In addition, the refractive index matched surface coating allows more light to be coupled out of the phosphor because the total internal reflection is reduced.
• a closed layer is advantageous if the phosphor has to be encapsulated. This may be necessary to reduce the sensitivity of the phosphor or parts thereof to diffusing ones
• the shaped body has a porous surface coating consisting of SiO 2 , TiO 2 , Al 2 O 3 , ZnO, ZrO 2 and / or Y 2 O 3 or mixed oxides thereof and / or of the compounds according to formulas I or II with or without dopants from the series Eu, Mn, Mg, Be, Ni, Co, Ru, Hf, Th and / or Zr.
• porous surface coatings offer the possibility of further reducing the refractive index of a single layer. The production of such porous
• Coatings may be made by three conventional methods as described in WO 03/027015, which is fully incorporated by reference into the context of the present application: etching of glass (eg soda-lime glasses (see US 4019884)), the application of a porous layer and the combination of porous layer and an etching process.
• etching of glass eg soda-lime glasses (see US 4019884)
• the shaped body has a surface which carries functional groups which allow a chemical or physical connection to the environment, preferably consisting of epoxy or silicone resin.
• functional groups can be, for example, esters attached via oxo groups or other derivatives which can form linkages with constituents of the binders based on epoxides and / or silicones.
• Such surfaces have the advantage that a homogeneous mixing of the phosphors is made possible in the binder.
• the rheological properties of the system phosphor / binder and also the pot life can be adjusted to a certain extent. This simplifies the processing of the mixtures.
• a physical connection to the environment is referred to when between the systems electrostatic interactions via charge fluctuations or partial charges act.
• the phosphor layer of the invention applied to the LED chip preferably consists of a mixture of silicone and homogeneous phosphor particles, and the silicone has a surface tension, this phosphor layer is not uniform at the microscopic level or the thickness of the layer is not consistently constant.
• platelet-shaped phosphors as a further preferred embodiment is done by conventional methods from the corresponding metal and / or rare earth salts.
• the preparation process is described in detail in EP 763573 and WO2008 / 058620, which are incorporated by reference in the context of the present application.
• These platelet-shaped phosphors can be prepared by a natural or synthetically produced highly stable support or a substrate of, for example mica, SiO 2 , Al 2 O 3 , ZrO 2 , glass or TiO 2 platelets, which is a very has high aspect ratio, has an atomically smooth surface and an adjustable thickness, can be coated by precipitation reaction in aqueous dispersion or suspension with a phosphor layer.
• the platelets may also consist of the phosphor material itself, or be composed of a material. If the wafer itself merely serves as a carrier for the phosphor coating, it must be made of a material which is transparent to the primary radiation of the LED, or absorbs the primary radiation and transfers this energy to the phosphor layer.
• the platelet-shaped phosphors are dispersed in a resin (eg, silicone or epoxy resin), and this dispersion is applied to the LED chip.
• the platelet-shaped phosphors can be produced on a large scale in thicknesses of 50 nm up to about 20 ⁇ m, preferably between 150 nm and 5 ⁇ m.
• the diameter is from 50 nm to 20 microns. It usually has an aspect ratio (ratio of diameter to particle thickness) of 1: 1 to 400: 1, and in particular 3: 1 to 100: 1.
• the platelet extent depends on the arrangement. Platelets are also suitable as scattering centers within the conversion layer, especially if they have particularly small dimensions.
• the surface of the platelet-shaped phosphor according to the invention facing the LED chip can be provided with a coating which acts in an anti-reflection manner with respect to the primary radiation emitted by the LED chip. This leads to a reduction in the backscattering of the primary radiation, as a result of which it can be better coupled into the phosphor body according to the invention.
• This coating can also consist of photonic crystals. This also includes a structuring of the surface of the platelet-shaped phosphor in order to achieve certain functionalities.
• the phosphor is prepared by mixing the corresponding reactants and dopants, then isostatically pressed and applied in the form of a homogeneous thin and non-porous platelets directly on the surface of the chip or at a distance from the chip (remote phosphor concept).
• the particular arrangement depends, among other things, on the architecture of the LED devices, wherein the skilled person is able to select the advantageous arrangement.
• no location-dependent variation of the excitation and emission of the phosphor takes place, as a result of which the LED equipped with it emits a homogeneous and color-constant light cone and has a high light output.
• Phosphor bodies can be produced industrially, for example, as platelets in thicknesses of a few 100 nm up to about 500 ⁇ m.
• the platelet extent (length x width) depends on the arrangement.
• the size of the wafer according to the chip size from about 100 .mu.m * 100 microns to several mm 2 ) with a certain excess of about 10% - 30% of the chip surface with a suitable chip arrangement (eg Flip Chip arrangement) or to choose accordingly. If the phosphor plate is placed over a finished LED, the emerging cone of light is completely covered by the plate.
• the side surfaces of the ceramic phosphor body can be mirrored with a light or noble metal, preferably aluminum or silver.
• the mirroring causes no light to emerge laterally from the phosphor body. Lateral exiting light can reduce the luminous flux to be coupled out of the LED.
• the mirroring of the ceramic phosphor body is carried out in a process step after the isostatic pressing to bars or plates, which may be done before the mirroring a tailor of the rods or plates in the required size.
• the side surfaces are for this purpose e.g. wetted with a solution of silver nitrate and glucose and then exposed at elevated temperature to an ammonia atmosphere.
• a silver coating on the side surfaces e.g. a silver coating on the side surfaces.
• electroless metallization processes are also suitable, see, for example, Hollemann-Wiberg, Lehrbuch der Inorganischen Chemie,
• the ceramic phosphor body can, if necessary, be fixed with a water glass solution on the substrate of an LED chip.
• the ceramic phosphor body has a patterned (e.g., pyramidal) surface on the side opposite an LED chip.
• a patterned (e.g., pyramidal) surface on the side opposite an LED chip.
• a further subject of the present invention is a process for producing a shaped body, preferably a phosphor body, comprising the following process steps: a) producing a europium-doped 1-1-2-alkaline earth-silicon nitride compound containing manganese, magnesium, beryllium , Nickel, cobalt, ruthenium, hafnium, thorium and / or zirconium-containing materials, by mixing at least 4 starting materials selected from silicon nitride, europium, calcium, strontium, barium, manganese .
• the excitability of the phosphors according to the invention also extend over a wide range, ranging from about 410 nm to 530 nm, preferably 430 nm to about 500 nm.
• these phosphors are not only suitable for excitation by UV or blue emitting primary light sources such as LEDs or conventional discharge lamps (eg based on Hg), but also for light sources such as those, the biaue in 3+ -
• Another object of the present invention is a lighting unit with at least one primary light source whose emission maximum or maximum ranges in the range 410 nm to 530 nm, preferably 430 nm to about 500 nm. Particularly preferred is a range between 440 and 480 nm, wherein the primary radiation is partially or completely converted by the compounds or phosphors according to the invention into longer-wave radiation.
• this lighting unit emits white or emits light with a certain color point (color-on-demand principle). Preferred embodiments of the lighting units according to the invention are shown in FIGS. 7 to 18.
• the light source is a luminescent arrangement based on ZnO, TCO (transparent conducting oxide), ZnSe or SiC or else an arrangement based on an organic light-emitting layer (OLED).
• the light source is a source which exhibits electroluminescence and / or photouminance.
• the light source may also be a plasma or discharge source.
• the phosphors of the present invention may be dispersed either in a resin (e.g., epoxy or silicone resin) or in suitable ones
• the optical coupling of the illumination unit between the phosphor and the primary light source is realized by a light-conducting arrangement.
• the primary light source is installed at a central location and this is optically coupled to the phosphor by means of light-conducting devices, such as light-conducting fibers.
• light-conducting devices such as light-conducting fibers.
• the lighting requirements adapted lights only consisting of one or different phosphors, which may be arranged to a fluorescent screen, and a light guide, which is connected to the primary light source is connected, realize.
• Another object of the present invention is the use of the compounds of the invention as a conversion phosphor for the partial or complete conversion of blue or in the near UV-hegenden emission of a light-emitting diode.
• the compounds according to the invention for converting the blue or near-UV emission into visible white radiation. Furthermore, the use of the compounds according to the invention for the conversion of the primary radiation into a specific color point according to the "color on demand" concept is preferred.
• Phosphors are used:
• CaF 2 Ce 3+ , Mn 2+ , CaF 2 ) Ce 3+ Tb 3+ , CaF 2 ) Eu 2+ , CaF 2 ) Mn 2+ , CaF 2 ) U, CaGa 2 O 4 ) Mn 2+ , CaGa 4 O 7 ) Mn 2+ , CaGa 2 S 4 ) Ce 3+ , CaGa 2 S 4 ) Eu 2+ , CaGa 2 S 4 ) Mn 2+ , CaGa 2 S 4 ) Pb 2+ , CaGeO 3 ) Mn 2+ , CaI 2 ) Eu 2+ in SiO 2 , Cal 2 : Eu 2+ , Mn 2+ in SiO 2 , CaLaBO 4 : Eu 3+ , CaLaB 3 O 7 : Ce 3+ , Mn 2+ , Ca 2 La 2 BO 6 .
• CaO Sm 3+ , CaOTb 3+ , CaO: TI, CaO: Zn 2+ , Ca 2 P 2 O 7 : Ce 3+ , ⁇ -Ca 3 (PO 4 ) 2 : Ce 3+ , ⁇ -Ca 3 ( PO 4 ) 2 : Ce 3+ , Ca 5 (PO 4 ) 3 CLEu 2+ , Ca 5 (PO 4 ) 3 Cl: Mn 2+ , Ca 5 (PO 4 ) 3 Cl: Sb 3+ , Ca 5 (PO 4 ) 3 CI: Sn 2+ , ⁇ -Ca 3 (PO 4 ) 2 : Eu 2+ , Mn 2+ , Ca 5 (PO 4 ) 3 F: Mn 2+ , Ca s (PO 4 ) 3 F: Sb 3+ , Ca s (PO 4 ) 3 F: Sn 2+ , ⁇ -Ca 3 (PO 4 ) 2 : Eu 2+ , ⁇ -Ca 3 (PO 4 ) 2 : Eu
• CaS Sn 2+ , F, CaSTb 3+ , CaSTb 3+ , CI, CaS: Y 3+ , CaS: Yb 2+ , CaS: Yb 2+ , CI, CaSiO 3 : Ce 3+ , Ca 3 SiO 4 Cl 2 : Eu 2+ , Ca 3 SiO 4 Cl 2 Pb 2+ , CaSiO 3 : Eu 2+ , CaSiO 3 : Mn 2+ , Pb, CaSiO 3 Pb 2+ , CaSiO 3 Pb 2+ , Mn 2+ , CaSiO 3 Ti 4+ , CaSr 2 (PO 4 ) 2 : Bi 3+ , ⁇ - (Ca, Sr) 3 (PO 4 ) 2 : Sn 2+ Mn 2+ , CaTi 0 .
• Ca 3 WO 6 U, CaYAIO 4 : Eu 3+ , CaYBO 4 : Bi 3+ , CaYBO 4 -Eu 3+ , CaYB 0 . 8 O 3 . 7 : Eu 3+ , CaY 2 ZrO 6 : Eu 3+ , (Ca, Zn, Mg) 3 (PO 4 ) 2 : Sn, CeF 3 , (Ce 1 Mg) BaAl 11 O 1 Ce, (Ce, Mg ) SrAlnOi 8 : Ce, CeMgAl 11 O 1 CeTb, Cd 2 B 6 O 11 Mn 2+ , CdS: Ag + , Cr, CdS: In, CdS: In, CdS: In, Te, CdSTe, CdWO 4 , CsF , CsI, CsLNa + , CsITI, (ErCb) 0 25 (BaCl 2 ) 0 .75, GaN: Zn,
• GdNbO 4 Bi 3+ , Gd 2 O 2 S: Eu 3+ , Gd 2 O 2 Pr 3+ , Gd 2 O 2 SPr 1 Ce 1 F, Gd 2 O 2 STb 3+ , Gd 2 SiO 5 : Ce 3 + , KAl 11 O 17 TI + , KGa 11 O 17 Mn 2+ , K 2 La 2 Ti 3 O 10 : Eu, KMgF 3 : Eu 2+ , KMgF 3 : Mn 2+ , K 2 SiF 6 : Mn 4+ , LaAl 3 B 4 O 12 : Eu 3+ , LaAIB 2 O 6 : Eu 3+ , LaAIO 3 : Eu 3+ , LaAIO 3 : Sm 3+ , LaAsO 4 : Eu 3+ , LaBr 3 : Ce 3+ , LaBO 3 : Eu 3+ , (La, Ce, Tb) PO 4 : Ce: Tb, LaCl 3 : Ce 3+ ,
• LuAIO 3 Ce 3+ , (Lu 1 Gd) 2 SiO 5 Oe 3+ , Lu 2 SiO 5 Oe 3+ , Lu 2 Si 2 O 7 : Ce 3+ , LuTaO 4 : Nb 5+ , Lui -x Y ⁇ AIO 3 : Ce 3+ , MgAl 2 O 4 ) Mn 2+ , MgSrAl 10 O 17 : Ce, MgB 2 O 4 : Mn 2+ , MgBa 2 (PO 4 ) 2 : Sn 2+ , MgBa 2 (PO 4 ) 2 : U, MgBaP 2 O 7 : Eu 2+ , MgBaP 2 O 7 : Eu 2+ , Mn 2+ , MgBa 3 Si 2 O 8 IEu 2+ , MgBa (SO 4 ) 2 : Eu 2+ , Mg 3 Ca 3 (PO 4 ) 4 : Eu 2+ , MgCaP 2 O 7 ,
• Mg 4 (F) (Ge, Sn) O 6 Mn 2+ , MgF 2 : Mn 2+ , MgGa 2 O 4 : Mn 2+ , Mg 8 Ge 2 O 11 F 2 ) Mn 4+ , MgS: Eu 2 + , MgSiO 3 ) Mn 2+ , Mg 2 SiO 4 ) Mn 2+ , Mg 3 SiO 3 F 4 ) Ti 4+ , MgSO 4 ) Eu 2+ , MgSO 4 ) Pb 2+ , MgSrBa 2 Si 2 O 7 ) Eu 2+ , MgSrP 2 O 7 ) Eu 2+ , MgSr 5 (PO 4 J 4 ) Sn 2+ , MgSr 3 Si 2 O 8 : Eu 2+ , Mn 2+ , Mg 2 Sr (SO 4 ) 3 : Eu 2+, MgWO 4, MgYBO 4) Eu
• ZnGa 2 O 4 Mn 2+ , ZnGa 2 S 4 : Mn 2+ , Zn 2 GeO 4 : Mn 2+ , (Zn, Mg) F 2 : Mn 2+ , ZnMg 2 (PO 4 ) 2 : Mn 2+ , (Zn, Mg) 3 (PO 4 ) 2 : Mn 2+ , ZnO: Al 3+ , Ga 3+ , ZnO: Bi 3+ , ZnOiGa 3+ , ZnOiGa, ZnO-CdOiGa, ZnOiS, ZnOiSe, ZnOiZn, ZnS : Ag + , Cr, ZnSiAg 1 Cu 1 Cl, ZnSiAg 1 Ni 1 ZnSiAu 1 In 1 ZnS-CdS (25-75), ZnS-CdS (50-50), ZnS-CdS (75-25), ZnS-CdSiA
• ZnTe Mn 2+
• ZnSe Cu +
• CI ZnWO 4
• the preparation of the reference phosphor is carried out in a glove box under a dry N 2 atmosphere (relative air humidity ⁇ 1%).
• the crucible is transferred under a continuous stream of argon in a tube furnace and heated for 8 hours under forming gas 90/10 and NH 3 at 1500 0 C.
• the crucible is transferred under a continuous stream of argon in a tube furnace and heated for 8 hours under forming gas 90/10 and NH 3 at 1500 0 C.
• Example 1b Preparation of 0.005 at% Be codoped CaSiN 2 : Eu
• the crucible is transferred under a continuous stream of argon in a tube furnace and heated for 8 hours under forming gas 90/10 and NH 3 at 1500 0 C.
• Example 1c Preparation of 0.005 at.% Mn codoped CaSiN 2 : Eu
• the crucible is transferred under a continuous stream of argon in a tube furnace and heated for 8 hours under forming gas 90/10 and NH 3 at 1500 0 C.
• Example 1d Preparation of CaSiN 2 : Eu (2 at.%) Cotopated with 0.005 at.% Ni
• the crucible is transferred under a continuous stream of argon in a tube furnace and heated for 8 hours under forming gas 90/10 and NH 3 at 1500 0 C.
• Example 1e Preparation of CaSiN 2 : Eu (2 at.%) Co-doped with 0.005 at.% Co
• the crucible is transferred under a continuous stream of argon in a tube furnace and heated for 8 hours under forming gas 90/10 and NH 3 at 1500 0 C.
• Example 1f Preparation of CaSiN 2 : Eu (2 at.%) Co-coded with 0.005 at.% Ru
• the crucible is transferred under a continuous stream of argon in a tube furnace and heated for 8 hours under forming gas 90/10 and NH 3 at 1500 0 C.
• Example 1h Preparation of CaSiN 2 : Eu (2 at.%) Coded with 0.005 at.% Th
• the crucible is transferred under a continuous stream of argon in a tube furnace and heated for 8 hours under forming gas 90/10 and NH 3 at 1500 0 C.
• Fig. 1 shows the emission spectrum of Ca o , 98SiN 2 : Eu o , o2 and co-doped phosphor at 450 nm excitation
• b Mg
• FIG. 2 shows a detail enlargement of FIG. 1 for a better differentiation of the emission spectra a to j.
• Fig. 3 shows the emission spectrum of Sro.g ⁇ SiN ⁇ uo.o ⁇ and co-doped
• Phosphor at an excitation wavelength of 450 nm. 4 shows an enlarged detail of FIG. 3 for better differentiation of the emission spectra. It means a) pure Sro, 98SiN 2 : Eu o , o2, b) Sr o , 98SiN 2 : Euo, o2 co-doped with 0.005 at% Mg or Be; c) Sr o , 98 SiN 2 : Euo, o2 co-doped with 0.005 at% Ni or Co; d) Sr O
• Fig. 5 shows the emission spectrum of Ba o , 98SiN 2 : Eu 0 , o2 and co-doped phosphor at an excitation wavelength of 450 nm.
• FIG. 6 shows an enlarged detail of FIG. 5 for better differentiation of the emission spectra. It means: a) pure Ba o , 98SiN 2 : Euo, o2; b) Bao, 98SiN 2 : Eu o , o2 co-doped with 0.005 at% Mg; c) Ba o , 9 8 SiN 2 : Euo, o2 co-doped with 0.005 at% Be; d) Ba o , 98SiN 2 : Eu o , o2 co-doped with 0.005 at% Mn; e) Ba o , 98SiN 2 : Eu 0 , o2 co-doped with 0.005 at% Ni or Co; f) Ba o , 98SiN 2 : Eu o , o2 co-doped with 0.005 at% Zr; g) Ba 0 ⁇ sSiN 2 : Eu o
• Fig. 7 shows the schematic illustration of a light emitting diode with a
• the component comprises a chip-type LED 1 as a radiation source.
• the LED is attached to a cup-shaped reflector, which is held by a Justageahmen 2.
• the chip 1 is connected via a flat cable 7 to a first contact 6 and directly to a second electrical contact 6 "
• a coating comprising a conversion phosphor according to the invention has been applied to the inner curvature of the reflector cup
• the phosphors are either separated from one another or as a mixture (List of part numbers: 1 light-emitting diode, 2 reflectors, 3 resin, 4 conversion phosphors, 5 diffusers, 6 electrodes, 7 flat cables)
• the conversion phosphor is dispersed in a binder, the mixture filling the cavity.
• This form of phosphor / binder layer may act as a secondary optical element and may be e.g. B. influence the light propagation.
• Bonding wire wherein the phosphor is applied as a thin layer dispersed in a binder.
• a further component acting as a secondary optical element, such as a lens, can easily be applied to this layer.
• Fig. 11 shows an example of another application, as already known in principle from US Pat. No. 6,700,322.
• the light source is an organic light-emitting diode 31, consisting of the actual organic film 30 and a transparent substrate 32.
• the film 30 emits in particular blue primary light, produced for example by means of PVK: PBD: coumarin (PVK, abbreviation for poly (n-vinylcarbazole) PBD, abbreviation for 2- (4-biphenyl) -5- (4-tert-butylphenyl) -1, 3,4-oxadiazole)).
• the emission is partially converted into a yellow, secondarily emitted light by a cover layer, formed from a layer 33 of the phosphor according to the invention, so that overall by color mixing of the primary and secondary emitted light, a white emission is realized.
• the OLED consists essentially of at least one layer of a light-emitting polymer or of so-called small molecules between two electrodes, which consist of materials known per se, such as ITO (abbreviation for "indium tin oxide”) as the anode and a highly reactive metal, For example, Ba or Ca, as a cathode, often multiple layers are used between the electrodes, which either serve as a hole transport layer or serve as electron transport layers in the area of the "small molecules".
• As emitting polymers for example, polyfluorenes or polyspiro materials are used.

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• 2008
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