EP3137576A1 - Substances luminescentes - Google Patents

Substances luminescentes

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Publication number
EP3137576A1
EP3137576A1 EP15720907.3A EP15720907A EP3137576A1 EP 3137576 A1 EP3137576 A1 EP 3137576A1 EP 15720907 A EP15720907 A EP 15720907A EP 3137576 A1 EP3137576 A1 EP 3137576A1
Authority
EP
European Patent Office
Prior art keywords
compound according
light source
group
compound
emission
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.)
Withdrawn
Application number
EP15720907.3A
Other languages
German (de)
English (en)
Inventor
Ralf Petry
Holger Winkler
Thomas Juestel
Florian BAUR
Kira Heerdt
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.)
Merck Patent GmbH
Original Assignee
Merck Patent GmbH
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
Application filed by Merck Patent GmbH filed Critical Merck Patent GmbH
Publication of EP3137576A1 publication Critical patent/EP3137576A1/fr
Withdrawn legal-status Critical Current

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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
    • C09K11/59—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials containing silicon
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01G—COMPOUNDS CONTAINING METALS NOT COVERED BY SUBCLASSES C01D OR C01F
    • C01G23/00—Compounds of titanium
    • C01G23/04—Oxides; Hydroxides
    • 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
    • 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
    • C09K11/57—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials containing manganese or rhenium
    • 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
    • C09K11/66—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials containing germanium, tin or lead
    • C09K11/661—Chalcogenides
    • 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
    • C09K11/66—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials containing germanium, tin or lead
    • C09K11/666—Aluminates; Silicates
    • 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
    • C09K11/67—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials containing refractory metals
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F21—LIGHTING
    • F21K—NON-ELECTRIC LIGHT SOURCES USING LUMINESCENCE; LIGHT SOURCES USING ELECTROCHEMILUMINESCENCE; LIGHT SOURCES USING CHARGES OF COMBUSTIBLE MATERIAL; LIGHT SOURCES USING SEMICONDUCTOR DEVICES AS LIGHT-GENERATING ELEMENTS; LIGHT SOURCES NOT OTHERWISE PROVIDED FOR
    • F21K2/00—Non-electric light sources using luminescence; Light sources using electrochemiluminescence
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L33/00—Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
    • H01L33/02—Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by the semiconductor bodies
    • H01L33/26—Materials of the light emitting region
    • H01L33/30—Materials of the light emitting region containing only elements of Group III and Group V of the Periodic Table
    • H01L33/32—Materials of the light emitting region containing only elements of Group III and Group V of the Periodic Table containing nitrogen
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L33/00—Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
    • H01L33/48—Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by the semiconductor body packages
    • H01L33/50—Wavelength conversion elements
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L33/00—Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
    • H01L33/48—Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by the semiconductor body packages
    • H01L33/50—Wavelength conversion elements
    • H01L33/501—Wavelength conversion elements characterised by the materials, e.g. binder
    • H01L33/502—Wavelength conversion materials
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L33/00—Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
    • H01L33/48—Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by the semiconductor body packages
    • H01L33/52—Encapsulations
    • H01L33/56—Materials, e.g. epoxy or silicone resin
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L33/00—Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
    • H01L33/48—Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by the semiconductor body packages
    • H01L33/58—Optical field-shaping elements
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K59/00—Integrated devices, or assemblies of multiple devices, comprising at least one organic light-emitting element covered by group H10K50/00
    • G—PHYSICS
    • G02—OPTICS
    • G02F—OPTICAL DEVICES OR ARRANGEMENTS FOR THE CONTROL OF LIGHT BY MODIFICATION OF THE OPTICAL PROPERTIES OF THE MEDIA OF THE ELEMENTS INVOLVED THEREIN; NON-LINEAR OPTICS; FREQUENCY-CHANGING OF LIGHT; OPTICAL LOGIC ELEMENTS; OPTICAL ANALOGUE/DIGITAL CONVERTERS
    • G02F1/00—Devices or arrangements for the control of the intensity, colour, phase, polarisation or direction of light arriving from an independent light source, e.g. switching, gating or modulating; Non-linear optics
    • G02F1/01—Devices or arrangements for the control of the intensity, colour, phase, polarisation or direction of light arriving from an independent light source, e.g. switching, gating or modulating; Non-linear optics for the control of the intensity, phase, polarisation or colour 
    • G02F1/13—Devices or arrangements for the control of the intensity, colour, phase, polarisation or direction of light arriving from an independent light source, e.g. switching, gating or modulating; Non-linear optics for the control of the intensity, phase, polarisation or colour  based on liquid crystals, e.g. single liquid crystal display cells
    • G02F1/133—Constructional arrangements; Operation of liquid crystal cells; Circuit arrangements
    • G02F1/1333—Constructional arrangements; Manufacturing methods
    • G02F1/1335—Structural association of cells with optical devices, e.g. polarisers or reflectors
    • G02F1/1336—Illuminating devices
    • G02F1/133614—Illuminating devices using photoluminescence, e.g. phosphors illuminated by UV or blue light
    • G—PHYSICS
    • G02—OPTICS
    • G02F—OPTICAL DEVICES OR ARRANGEMENTS FOR THE CONTROL OF LIGHT BY MODIFICATION OF THE OPTICAL PROPERTIES OF THE MEDIA OF THE ELEMENTS INVOLVED THEREIN; NON-LINEAR OPTICS; FREQUENCY-CHANGING OF LIGHT; OPTICAL LOGIC ELEMENTS; OPTICAL ANALOGUE/DIGITAL CONVERTERS
    • G02F1/00—Devices or arrangements for the control of the intensity, colour, phase, polarisation or direction of light arriving from an independent light source, e.g. switching, gating or modulating; Non-linear optics
    • G02F1/01—Devices or arrangements for the control of the intensity, colour, phase, polarisation or direction of light arriving from an independent light source, e.g. switching, gating or modulating; Non-linear optics for the control of the intensity, phase, polarisation or colour 
    • G02F1/13—Devices or arrangements for the control of the intensity, colour, phase, polarisation or direction of light arriving from an independent light source, e.g. switching, gating or modulating; Non-linear optics for the control of the intensity, phase, polarisation or colour  based on liquid crystals, e.g. single liquid crystal display cells
    • G02F1/133—Constructional arrangements; Operation of liquid crystal cells; Circuit arrangements
    • G02F1/1333—Constructional arrangements; Manufacturing methods
    • G02F1/1335—Structural association of cells with optical devices, e.g. polarisers or reflectors
    • G02F1/1336—Illuminating devices
    • G02F1/133621—Illuminating devices providing coloured light
    • G—PHYSICS
    • G02—OPTICS
    • G02F—OPTICAL DEVICES OR ARRANGEMENTS FOR THE CONTROL OF LIGHT BY MODIFICATION OF THE OPTICAL PROPERTIES OF THE MEDIA OF THE ELEMENTS INVOLVED THEREIN; NON-LINEAR OPTICS; FREQUENCY-CHANGING OF LIGHT; OPTICAL LOGIC ELEMENTS; OPTICAL ANALOGUE/DIGITAL CONVERTERS
    • G02F2203/00—Function characteristic
    • G02F2203/05—Function characteristic wavelength dependent

Definitions

  • the present invention relates to compounds of the formula I,
  • a compound of the formula I Another subject of the present invention relates to a light-emitting device which comprises at least one compound of the formula I according to the invention.
  • Inorganic fluorescent powders excitable in the blue and / or UV spectral range are of great importance as conversion phosphors for phosphor converted LEDs, in short pc LEDs.
  • conversion phosphor systems are known, such as alkaline earth orthosilicates, thiogallates, garnets, nitrides and oxynitrides each doped with Ce 3+ or Eu 2+ .
  • red-emitting phosphors with emission wavelengths above 600 nm are required in addition to the yellow- or green-emitting garnets or ortho-silicates which emit sufficiently strong at the corresponding wavelength of the primary radiation (370-480 nm).
  • Most of the currently commercially available cold white LEDs contain a colorimetrically optimized Ce 3+ -doped garnet phosphor according to the general formula (Y, Gd, Lu, Tb) 3 (Al, Ga, Sc) 50i 2: Ce.
  • Warm white LEDs also contain a second red-emitting phosphor which is either an Eu 2+ -doped ortho-silicate phosphor or an Eu 2+ -doped (oxy) nitride phosphor.
  • a second red-emitting phosphor which is either an Eu 2+ -doped ortho-silicate phosphor or an Eu 2+ -doped (oxy) nitride phosphor.
  • the main disadvantage of using an LED light source with a broadband emitting Ce 3+ -doped garnet phosphor and a broadband emitting Eu 2+ -doped ortho-silicate phosphor or (oxy) nitride in the red spectral range are in addition to any chemical instability, especially against moisture, the pronounced reabsorption and the emission of radiation in the NIR range, so that the lumen output of warm white LEDs is significantly lower (about a factor of 2 or more) than that of a corresponding cold white LED.
  • Reabsorbtion in this context means that fluorescent light generated in the phosphor to a certain extent can not leave the phosphor, because this is totally reflected at the interface to the optically thinner environment and migrated in the phosphor via waveguiding processes and eventually lost.
  • NIR near infrared
  • Emission band is distinguished.
  • the major drawback of these Eu 2+ activated materials is their relatively high sensitivity to photodegradation since divalent Eu 2+ tends to photoionize, especially in relatively low band gap host materials.
  • An advantage of Mn 4+ -activated phosphors lies in the underlying optical transition [Ar] 3d 3 - [Ar] 3d 3 , that is a
  • Tanabe-Sugano diagram for Mn + shows that this transition lies on the one hand in the red spectral range and on the other hand is optically narrow and thus allows red phosphors with high color saturation and at the same time acceptable lumen equivalent.
  • the Tanabe-Sugano diagram is a diagram in which, for all electronic states of a system, the energy difference E is typically the lowest state against
  • the Tanabe-Sugano diagram is thus a correlation diagram, which allows the interpretation of absorption spectra of chemical compounds.
  • Radiation converter should be suitable.
  • D at least one element selected from the group of Ca or Ba,
  • M at least one element selected from the group of Ti
  • n 0 or 1
  • the compounds according to the invention are usually excitable in the near UV or blue spectral range, preferably at about 280 to 470 nm, particularly preferably at about 300 to 400 nm, and usually have line emission in the red spectral range of about 600 to 700 nm, preferably about 620 to 680 nm, with a half-width (FWHM) of the main emission peak of a maximum of 50 nm, preferably a maximum of 40 nm.
  • the full width at half maximum (half width or FWHM) is a parameter that is commonly used to describe the width of a peak or function. It is defined in a two-dimensional coordinate system (x, y) by the distance ( ⁇ ) between two points on the curve with the same y-value, at which the function reaches half its maximum value (y ma x / 2).
  • blue light is defined as light whose emission maximum lies between 400 and 459 nm, cyan light whose emission maximum is between 460 and 505 nm, green light whose emission maximum lies between 506 and 545 nm as yellow light such, whose
  • Emission maximum between 546 and 565 nm such as orange light whose emission maximum is between 566 and 600 nm and as red light, whose emission maximum is between 601 and 700 nm.
  • the compound of the invention is preferably a red-emitting conversion phosphor.
  • the compounds according to the invention are distinguished by a high photoluminescence quantum yield of more than> 80%, preferably more than 90%, particularly preferably more than 95%.
  • the photoluminescence quantum yield (also called quantum efficiency or quantum efficiency) describes the ratio between the number of emitted and absorbed photons of a compound.
  • the compounds according to the invention have high values for the lumen equivalent (> 250 Im / W) and are furthermore distinguished by very good thermal and chemical stability. Furthermore, the compounds according to the invention are excellently suited for use in white LEDs, color-on-demand (COD) applications, TV backlighting LEDs and electric lamps such as, for example
  • the compounds of the formula I are selected from the compounds of the following sub-formulas:
  • Eutectic comes, and thus to a melting point depression which simplifies the synthesis and ensures a better crystallinity.
  • Invention is equal to zero.
  • the compounds of the formula I are selected from the group of the compounds of the formulas Ia-1 to Ia-4,
  • Spectral range in the range of 600 nm to 700 nm can be selectively varied.
  • germanium is in the
  • compounds of the formula I are selected from the compounds in which m is 0, wherein at the same time y is 4, x is 1 and 0.001 ⁇ z is 0.004.
  • A represents exactly one element selected from the group of Li, Na, K and Rb. But they are equal as well
  • A corresponds to a mixture of these elements, ie at least two elements selected from the group of Li, Na, K and Rb.
  • the compounds according to the invention are particularly preferably selected from the following sub-formulas:
  • A represents at least two elements selected from the group of Li, Na, K and Rb, such as Nai.8Üo.2Geo.999Mno.oo-tSi309.
  • the compounds according to the invention can be present as phase mixtures but also in phase.
  • the compounds according to the invention are pure in phase.
  • An X-ray diffractogram can be used to examine the phase purity of a crystalline powder, i. H. whether the sample consists only of one crystalline (pure phase) or more (multi-phase) compounds. In phase-pure powders all reflections can be observed and assigned to the compound.
  • the particle size of the compounds according to the invention is usually between 50 ⁇ m and 1 ⁇ m, preferably between 30 ⁇ m and 3 ⁇ m, particularly preferably between 20 ⁇ m and 5 ⁇ m.
  • Another object of the present invention is a process for preparing a compound of the invention, characterized
  • step a) suitable starting materials selected from the group of corresponding oxides, carbonates, oxalates or corresponding reactive forms are mixed and the mixture is thermally treated in a step b).
  • suitable starting materials selected from the group of corresponding oxides, carbonates, oxalates or corresponding reactive forms are mixed and the mixture is thermally treated in a step b).
  • Manganese source at least one lithium, sodium, potassium, rubidium, calcium, barium and / or strontium source;
  • At least one source of manganese at least one
  • Germanium source and optionally a titanium, zirconium, hafnium, silicon and / or tin source
  • the manganese source used in step (a) may be any conceivable manganese compound with which a compound according to the invention can be prepared.
  • the manganese source used is preferably carbonates, oxalates and / or oxides, in particular manganese oxalate dihydrate
  • step (a) As germanium source in step (a), any conceivable
  • Germanium compound are used with which a compound of the invention can be prepared.
  • a compound of the invention can be prepared.
  • germanium source oxides especially germanium oxide
  • any conceivable lithium, sodium, potassium, rubidium, calcium, barium and / or strontium compound can be used with which a compound of the invention can be prepared.
  • Corresponding carbonates or oxides in particular lithium carbonate (U 2 CO 3), sodium carbonate (Na 2 CO 3), potassium carbonate (K 2 CO 3), rubidium carbonate (in the process according to the invention as lithium, sodium, potassium, rubidium, calcium, barium and / or strontium compound) are preferably used.
  • titanium, zirconium, hafnium, silicon and / or tin source in step (a) any conceivable titanium, zirconium, hafnium, silicon and / or tin compound can be used with which an inventive
  • inventive method as titanium, zirconium, hafnium, silicon and / or tin source corresponding nitrides and / or oxides used.
  • the compounds are preferably used in a ratio to one another such that the atomic number corresponds to the desired ratio in the product of the abovementioned formulas.
  • the starting compounds in step (a) are preferably used in powder form and processed together, for example by a mortar, to form a homogeneous mixture.
  • a mortar for example, a mortar
  • the mixture is dried before calcination.
  • oxidizing conditions is meant any conceivable oxidizing atmosphere, e.g. Air or other
  • At least one substance from the group of ammonium halides preferably ammonium chloride, Aikalifluoride, such as sodium, potassium or lithium fluoride, alkaline earth fluorides such as calcium, strontium or barium fluoride, carbonates, preferably
  • Ammonium hydrogen carbonate or various alcoholates and / or oxalates are used.
  • the calcination is preferably carried out at a temperature in the range of 700 ° C to 1200 ° C, more preferably 800 ° C to 1000 ° C and
  • the period is the calcination preferably 2 to 14 hours, more preferably 4 to 12 hours and especially 6 to 10 hours.
  • the calcination is preferably carried out so that the resulting mixtures are introduced, for example, in a vessel made of boron nitride in a high-temperature furnace.
  • the high-temperature furnace for example, a tube furnace containing a support plate made of molybdenum foil.
  • the compounds obtained are optionally homogenized, wherein a corresponding grinding process can be carried out wet in a suitable solvent, for example in isopropanol, or dry.
  • the calcined product may optionally be re-selected under the above conditions and with the optional addition of a suitable flux selected from the group of ammonium halides, preferably ammonium chloride, alkali metal fluorides such as sodium, potassium or lithium fluoride, alkaline earth fluorides such as calcium, strontium or
  • Barium fluoride, carbonates, preferably ammonium bicarbonate, or various alkoxides and / or oxalates, are calcined.
  • Suitable for this purpose are all the coating methods known to the person skilled in the art according to the prior art and used for phosphors.
  • Suitable materials for the coating are, in particular, metal oxides and metal nitrides, in particular earth metal oxides, such as Al 2 O 3, and
  • Nitrides such as AIN and S1O2.
  • the coating can be carried out, for example, by fluidized bed processes.
  • Another object of the present invention is the use of the compound of the invention as a phosphor, in particular as a conversion phosphor.
  • the term “conversion luminescent material” is understood to mean a material which absorbs radiation in a specific wavelength range of the electromagnetic spectrum, preferably in the blue or UV spectral range, and in another wavelength range of the electromagnetic spectrum, preferably in red or orange
  • the term “radiation-induced emission efficiency” is to be understood, ie the conversion phosphor absorbs radiation in a certain wavelength range and emits radiation in another wavelength range with a certain efficiency. Shifting the emission wavelength "means that a
  • Conversion luminescent material emits light at a different wavelength, that is shifted to a smaller or larger wavelength compared to another or similar conversion luminescent material. So the emission maximum is shifted.
  • Another object of the present invention is an emission-converting material comprising one or more
  • the emission-converting material may consist of one of the compounds according to the invention and in this case would be equivalent to the term "conversion luminescent substance" as defined above.
  • the emission-converting material according to the invention contains, in addition to the compound according to the invention, further conversion phosphors.
  • inventive emission-converting material is a mixture of at least two conversion phosphors, one of which is a compound according to the invention. It is particularly preferred that which are at least two conversion phosphors, phosphors that emit light of different wavelengths, which are complementary to each other. Since the compound according to the invention is a red emitting phosphor, it is preferably used in combination with a green or yellow emitting phosphor or else with a cyan or blue emitting phosphor. Alternatively, the inventive red-emitting conversion phosphor in combination with (a) blue and green-emitting
  • Conversion luminescent material s
  • inventive red-emitting conversion phosphor in
  • BaSrMgSi 2 0 7 Eu 2+ , BaTiP 2 0 7 , (Ba, Ti) 2 P 2 O 7 : Ti, Ba 3 WO 6 : U,
  • BaY 2 F 8 Er 3+ , Yb + , Be 2 Si0 4 : Mn + , Bi 4 Ge 3 Oi 2 , CaAl 2 0 4 : Ce 3+ , CaLa 4 O 7 : Ce 3+ , CaAl 2 O 4 : Eu 2+ , CaAl 2 O: Mn 2+ , CaAl 4 O 7 : Pb 2+ , Mn 2+ , CaAl 2 04: Tb 3+ ,
  • CaB 2 O Pb 2+
  • CaB 2 P 2 O 9 Eu 2+
  • Ca 5 B 2 SiOio Eu 3+
  • CaGa4O 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+ , Cal 2 : Eu 2+ in SiO 2 , Cal 2 : Eu 2+ , Mn 2+ in
  • Ca 2 P 2 0 7 Ce 3+, a-Ca 3 (P0 4) 2: Ce 3+, beta-Ca 3 (PO4) 2: Ce 3+, Ca 5 (P04) 3 Cl: Eu 2+, Ca 5 (P0 4) 3 Cl: Mn 2+, Ca 5 (P04) 3 CI: Sb 3+, Ca 5 (P0 4) 3 Cl: Sn 2+,
  • beta-Ca 3 (P04) 2 Eu 2+, Mn 2+, Ca 5 (P04) 3 F: Mn 2+, Cas (P0 4) 3 F: Sb 3+,
  • Ca s (P0 4) 3 F Sn 2+, a-Ca3 (P04) 2: Eu 2+, beta-Ca 3 (P0 4) 2: Eu 2+, Ca 2 P 2 O 7: Eu +, Ca 2 P 2 O 7 : Eu 2+ , Mn 2+ , CaP 2 O 6 : Mn 2+ , a-Ca 3 (PO 4 ) 2 : Pb 2+ , a-Ca 3 (PO 4 ) 2: Sn 2+ , ⁇ -Ca 3 (PO 4 ) 2: Sn 2+ , ⁇ -Ca 2 P 2 O 7: Sn, Mn, ⁇ -Ca 3 (PO 4 ) 2: Tr, CaS: Bi 3+ ,
  • CaSiO 3 Pb 2+ , CaSiO 3 : Pb 2+ , Mn 2+ , CaSiO 3 : Ti 4+ , CaSr 2 (PO 4 ) 2: Bi 3+ ,
  • CdS In, Te, CdS: Te, CdW0 4 , CsF, CsI, CsI: Na + , CsII, (ErCl 3 ) o.25 (BaCl 2) o.75, GaN.Zn, Gd 3 Ga 5 0i 2 : Cr 3+, Gd 3 Ga 5 O 2: Cr, Ce, GdNbO 4: Bi 3+, Gd 2 0 2 S: Eu 3+, Gd 2 O 2 Pr 3+, Gd 2 O 2 S: Pr, Ce, F, Gd 2 O 2 S: Tb 3+ , Gd 2 SiO 5 : Ce 3+ , KAInOi 7 : TI + , KGaiOi 7 : Mn 2+ , K 2 La 2 Ti 3 Oio: Eu, K gF 3 : Eu 2+ , KMgF 3 : n 2+ , K 2 SiF 6: Mn 4+ , LaAl 3 B 4 Oi 2
  • LaSiO 3 Cl Ce 3+ , Tb 3+ , LaVO 4 : Eu 3+ , La 2 W 3 Oi 2 : Eu 3+ , LiAIF 4 : Mn 2+ , LiAl 5 O 8 : Fe 3+ , LiAlO 2 : Fe 3+ , LiAIO 2 : Mn 2+ , LiAl 5 O 8 : Mn 2+ , Li 2 CaP 2 O 7 : Ce 3+ , Mn 2+ ,
  • LiCeBa4Si4Oi 4 Mn 2+ , LiCeSrBa 3 Si40i4: Mn 2+ , LilnO 2 : Eu 3+ , LilnO 2 : Sm 3+ , LiLaO 2 : Eu 3+ , LuAlO 3 : Ce 3+ , (Lu, Gd) 2 SiO 5 : Ce 3+ , Lu 2 SiO 5 : Ce 3+ , Lu 2 Si 2 O 7 : Ce 3+ , LuTaO 4: Nb 5+ , Lu-x Y x Al 3 : Ce 3+ , MgAl 2 O 4 : Mn 2+ , MgSrAhoOi 7 : Ce,
  • MgB2 O4 Mn +, MgBa 2 (PO 4) 2: Sn 2+, MgBa 2 (PO4) 2: U, MgBaP 2 0 7: Eu 2+,
  • MgBaP 2 O 7 Eu 2+ , Mn 2+ , MgBa 3 Si 2 O 8 : Eu 2+ , MgBa (SO 4 ) 2 : Eu 2+ ,
  • Mg 3 Ca 3 (PO 4 ) 4 Eu 2+
  • MgCaP 20 7 Mn 2+
  • Mg 2 Ca (SO 4 ) 3 Eu 2+
  • Mg 2 Ca (SO 4) 3 Eu 2+ , Mn 2 ( MgCeAl n Oi 9 : Tb 3+ , Mg 4 (F) GeO 6 : Mn 2+ , Mg 4 (F) (Ge, Sn) 06.Mn 2+ 2+ MgF2.Mn, MgGa20 4: Mn 2+, Mg8Ge20nF2.Mn +, MgS: Eu 2+, MgSi03: Mn 2+, Mg2SiO 4: Mn 2+ Mg3SiO3F 4: Ti 4+, MgSO4: Eu 2+, MgS04: Pb 2+, MgSrBa 2 Si 2 07: Eu 2+, MgSrP 2 07: Eu +, MGSR 5 (P0 4) 4: Sn 2+ , MgSr 3 Si 2 O 8 : Eu 2+ , Mn 2+ , Mg 2 Sr (SO 4 ) 3 : Eu + ,
  • gYB04 Eu 3+, Na3Ce (P04) 2: Tb 3+, NaI: TI, Nai.23Ko.4 Euo.i2TiSi40n 2: Eu 3+, Nai.23Ko.42Euo.i2TiSi5Oi3 xH20: Eu 3+, Nai.29Ko .46Ero.o8TiSi4Oii: Eu 3+ ,
  • Na 2 Mg 3 Al 2 Si 2 Oio Tb
  • Na (Mg 2 -x Mn x ) LiSi 4 OioF 2 Mn
  • NaYF 4 Er 3+ , Yb 3+ ,
  • SrB 4 O 7 Eu 2+ (F, CI, Br), SrB40 7 : Pb 2+ , SrB 4 07: Pb 2+ , Mn 2+ , SrB 8 Oi 3: Sm 2+ , SrxBa y ClzAl 2 O 4-z / 2 : Mn 2+, Ce 3+, SrBaSi04: Eu 2+, Sr (CI, Br, l) 2: Eu 2+ in S1O2, SrCl 2: Eu 2+ in SiO 2) Sr 5 Cl (PO 4) 3: Eu, SrwFxB 4 O6.5: Eu 2+ , SrwF x ByOz: Eu 2+ , Sm 2+ , SrF 2 : Eu 2+ , SrGai 20i 9 : Mn 2+ , SrGa 2S 4 : Ce 3+ , SrGa 2 S4: Eu 2+ , SrGa 2 S4: Pb 2+ , Sr
  • Sr 5 (PO 4) 3 F Sb 3+, Sr 5 (P0 4) 3F: Sb 3+, Mn 2+, Sr 5 (PO 4) 3F: Sn 2+, Sr 2 P20 7: Sn 2+, .beta.
  • YAbB4Oi2 Ce 3+ , YAl3B 4 0i 2: Ce 3+ , Mn, YAl 3 B40i 2: Ce 3+ , Tb 3+ , YAl 3B 4 Oi 2: Eu 3+ , YAl 3 B 4 0i 2: Eu 3+ , Cr 3+ , YAI 3 B40i2: Th 4+, Ce 3+, Mn 2+, YAI0 3: Ce 3+, Oi2 Y3AI 5: Ce 3+, Y 3 Al 5 O 2: Cr 3+, YAI0 3: Eu 3+, Y3AI 5 Oi 2 : Eu 3r , Y 4 Al 2 O 9: Eu 3+ , Y 3 Al 5 O 2 : Mn 4+ , YAl 3 : Sm 3+ , YAl 3 : Tb 3+ , Y 3 AI 5 O 2 : Tb 3+ , YAsO 4: Eu 3+ , YBO 3 :
  • Y 2 0 3 Bi 3+ , YOBr: Eu 3+ , ⁇ 2 ⁇ 3 : ⁇ , Y 2 0 3 : Er 3+ , Y 2 O 3 : Eu 3+ (YOE), Y 2 0 3 : Ce 3 +, Tb3 +, YOCI: Ce 3+, YOCI: Eu 3+, YOF: Eu 3+, YOF: Tb 3+, Y 2 03: Ho 3+, Y 2 02S: Eu 3+, Y 2 0 2 S: Pr 3+ , Y 2 O 2 S: Tb 3+ , Y 2 O 3 : Tb 3+ , YPO 4 : Ce 3+ , YPO 4 : Ce 3+ , Tb 3+ ,
  • YPO 4 Eu 3+
  • YPO 4 Mn 2+ , Th +
  • Y PO 4 V 5+
  • Y (P, V) O 4 Eu
  • Y 2 SiO 4 Ce 3+
  • YTaO 4 YTaO 4
  • YVO 4 Dy 3+
  • YVO 4 Eu 3+
  • ⁇ 2 ⁇ 4 ⁇ 2+
  • ZnB 2 O 4 Mn 2+
  • ZnBa 2 S3 Mn 2+ , (Zn, Be) 2SiO 4: Mn 2+ , ZncuCdo.eSiAg, Zno.6Cdo.4S: Ag,
  • (Zn, Cd) S Ag, Cl, (Zn, Cd) S: Cu, ZnF 2 .Mn 2+ , ZnGa 2 0 4 , ZnGa 2 04.Mn 2+ , ZnGa 2 S4: Mn 2+, Zn2Ge04: n 2+, (Zn, Mg) F 2: Mn 2+, ZnMg 2 (P04) 2: Mn 2+, (Zn, Mg) 3 (P04) 2: Mn 2 + , ZnO: Al 3+ , Ga 3+ , ZnO: Bi 3+ , ZnO: Ga 3+ , ZnO: Ga, ZnO-CdO: Ga, ZnO: S, ZnO: Se, ZnO: Zn, ZnS: Ag + , CI, ZnS: Ag, Cu, Cl, ZnS: Ag, Ni, ZnS: Au, In, ZnS-CdS (25-75), ZnS-C
  • ZnS Cu, Sn, ZnS: Eu 2+ , ZnS: Mn 2+ , ZnS: Mn, Cu, ZnS: Mn 2+ , Te 2+ , ZnS: P, ZnS: P 3 -, C
  • Zn 2 SiO 4 Mn 2+, Zri2SiO4: n 2+, As 5+, Zn 2 Si04: Mn, Sb 2 O 2, Zn 2 SiO 4: Mn 2+, P, Zn 2 SiO 4: Ti 4+, ZnS: Sn 2+ , ZnS: Sn, Ag, ZnS: Sn 2+ , Li + , ZnS: Te, Mn, ZnS-ZnTe: Mn 2+ , ZnSe: Cu + , Cl or ZnWO 4.
  • LED quality is described by common parameters such as the Color Rendering Index, Correlated Color Temperature, Lumen Equivalents or Absolute Lumens, or the color point in CIE x and CIE y coordinates.
  • Color rendering index is a unitary photometric quantity known to those skilled in the art, which is the color fidelity of an artificial light source to that of sunlight
  • Filament light sources compare (the latter two have a CRI of 100).
  • the CCT or Correlated Color Temperature is a photometric quantity with the unit Kelvin familiar to the person skilled in the art. The higher the numerical value, the colder the viewer sees the white light of an artificial radiation source.
  • the CCT follows the concept of
  • Black light emitter whose color temperature is the so-called Planckian curve in the CIE diagram.
  • the lumen equivalent is a photometric quantity familiar to the person skilled in the art with the unit Im W, which describes how large the photometric luminous flux in lumens of a light source at a given wavelength
  • radiometric radiant power with the unit watts is.
  • the lumen is a photometric one familiar to those skilled in the art
  • photometric quantity which describes the luminous flux of a light source, which is a measure of the total visible radiation emitted by a radiation source. The larger the luminous flux, the brighter the light source appears to the observer.
  • CIE x and CIE y represent the coordinates in the familiar CIE standard color diagram (in this case normal observer 1931), which describes the color of a light source.
  • a further subject of the present invention is the use of the compounds according to the invention or the emission-converting material according to the invention described above in a light source.
  • the light source is an LED, in particular a phosphor-converted LED, in short pc-LED.
  • the emission-converting material comprises, in addition to the conversion luminescent material according to the invention, at least one further conversion luminescent material, in particular such that the light source emits white light or light with a specific color point (color-on-demand principle).
  • color-on-demand principle is meant the realization of light of a particular color point with a pc-LED using one or more conversion phosphors.
  • Another object of the present invention is thus a light source comprising a primary light source and the emission-converting material.
  • the emission-converting material comprises, in addition to the conversion luminescent material according to the invention, at least one further conversion luminescent substance, so that the Light source preferably emits white light or light with a certain color point.
  • the light source according to the invention is preferably a pc-LED.
  • a pc-LED typically includes a primary light source and an emission converting material.
  • the emission-converting material according to the invention can either be dispersed in a resin (for example epoxy or silicone resin) or with suitable proportions directly on the primary light source or remotely located therefrom, depending on the application (the latter arrangement also includes "Remote Phosphor Technology " with a).
  • the primary light source may be a semiconductor chip, a luminescent one
  • Light source such as ZnO, a so-called TCO (Transparent Conducting Oxide), a ZnSe or SiC based arrangement, an organic light-emitting layer based arrangement (OLED) or a plasma or discharge source, most preferably a semiconductor chip.
  • the primary light source is a semiconductor chip, it is preferably a luminescent indium-aluminum-gallium nitride (InAIGaN), as known in the art.
  • InAIGaN luminescent indium-aluminum-gallium nitride
  • lasers as a light source.
  • the emission-converting material according to the invention can be converted for use in light sources, in particular pc LEDs, into any external forms such as spherical particles, platelets and structured materials and ceramics. These forms are summarized under the term "shaped body”. Consequently, it is in the
  • Another subject of the invention is a lighting unit which contains at least one light source according to the invention.
  • Such lighting units are mainly used in display devices, in particular liquid crystal display devices (LC display) with a backlight. Therefore, such a display device is the subject of the present invention.
  • the optical display unit according to the invention the optical display unit according to the invention.
  • Coupling between the emission-converting material and the primary light source preferably by a light-conducting arrangement.
  • emission-converting material is optically coupled. In this way, the lighting requirements adapted lights consisting of one or more different
  • Conversion phosphors which may be arranged to a fluorescent screen, and a light guide, which is coupled to the primary light source implement. This makes it possible to place a strong primary light source in a convenient location for the electrical installation and to install without additional electrical wiring, only by laying fiber optics at random locations, lights of emission-converting materials that are coupled to the light guide.
  • 0.9539 g (9000 mmol) of a2CO3, 0.0739 g (1000 mmol) of U2CO3, 1.0453 g (9990 mmol) of GeO2, 1.08025 g (30.000 mmol) of S1O2 and 0.0018 g (0.010 mmol) of ⁇ 2 ⁇ 4 ⁇ 2 ⁇ 2 ⁇ are carried in an agate mortar Thoroughly rub acetone.
  • the powder is dried, transferred to a covered porcelain crucible and calcined at 600 ° C for 1 hour.
  • the calcined powder is thoroughly rubbed with acetone together with 2.5% by weight of NaF and 2.5% by weight of LiF in an agate mortar.
  • the dried powder is transferred to a covered porcelain crucible and heated at 800 ° C for 4 hours.
  • the blue LEDs used in this example for LED characterization have one
  • the light-technical characterization of the LED is carried out with a spectrometer from the company Instrument Systems - spectrometer CAS 140 and an associated integrating sphere ISP 250.
  • the LED is characterized by determining the wavelength-dependent spectral power density.
  • the spectrum thus obtained of the light emitted by the LED is used to calculate the color point coordinates CIE x and y.

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Abstract

La présente invention concerne des composés de formule (I) : (A2‑2nBn)x(Ge1‑mMm)yO(x+2y)Mn4+, où les paramètres A, B, M, m, n, x, et y ont l'une des significations indiquées dans la revendication 1. L'invention concerne en outre un procédé de préparation des composés de formule (I), l'utilisation de ces composés en tant que substances luminescentes de conversion, ainsi qu'un matériau convertisseur d'émission contenant au moins un composé de formule (I). Un autre objet de la présente invention concerne un dispositif émetteur de lumière qui contient au moins un composé de formule (I) selon l'invention.
EP15720907.3A 2014-04-28 2015-04-01 Substances luminescentes Withdrawn EP3137576A1 (fr)

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PCT/EP2015/000704 WO2015165567A1 (fr) 2014-04-28 2015-04-01 Substances luminescentes

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TWI589036B (zh) * 2016-07-25 2017-06-21 林孝正 用於發光晶體的覆晶螢光鏡片、具有其的發光模組、生物培養裝置及發光模組改造方法
TWI589035B (zh) * 2016-07-25 2017-06-21 林孝正 生物培養裝置及其發光模組改造方法
EP3541891B1 (fr) 2016-11-17 2023-04-26 Current Lighting Solutions, LLC Luminophores revêtus émettant une ligne rouge
KR102048678B1 (ko) * 2016-12-29 2019-11-26 중앙대학교 산학협력단 산화물계 형광체, 그의 제조 방법, 및 상기 형광체를 포함하는 발광 다이오드
KR102486988B1 (ko) * 2017-09-22 2023-01-10 삼성디스플레이 주식회사 발광 소자 및 이를 포함하는 표시 장치
CN108102648B (zh) * 2017-12-25 2020-03-10 广东工业大学 一种颜色可调的长余辉材料及其制备方法
CN109054830B (zh) * 2018-07-17 2021-06-18 延边大学 用于白光led的多种钛锗酸盐的荧光材料及制备方法
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US20220403450A1 (en) 2021-06-03 2022-12-22 Illumina Software, Inc. Systems and methods for sequencing nucleotides using two optical channels
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US20170051201A1 (en) 2017-02-23
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WO2015165567A1 (fr) 2015-11-05
CN106459752A (zh) 2017-02-22
KR20160147936A (ko) 2016-12-23

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