Classifications

• • 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 materials, e.g. electroluminescent or chemiluminescent
  • C09K11/08—Luminescent materials, e.g. electroluminescent or chemiluminescent containing inorganic luminescent materials
  • C09K11/77—Luminescent materials, e.g. electroluminescent or chemiluminescent containing inorganic luminescent materials containing rare earth metals
  • C09K11/7766—Luminescent materials, e.g. electroluminescent or chemiluminescent containing inorganic luminescent materials containing rare earth metals containing two or more rare earth metals
  • C09K11/7781—Sulfates
• • A—HUMAN NECESSITIES
  • A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
  • A61B—DIAGNOSIS; SURGERY; IDENTIFICATION
  • A61B18/00—Surgical instruments, devices or methods for transferring non-mechanical forms of energy to or from the body
  • A61B18/18—Surgical instruments, devices or methods for transferring non-mechanical forms of energy to or from the body by applying electromagnetic radiation, e.g. microwaves
• • 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 materials, e.g. electroluminescent or chemiluminescent
  • C09K11/08—Luminescent materials, e.g. electroluminescent or chemiluminescent containing inorganic luminescent materials
  • C09K11/0805—Chalcogenides
  • C09K11/0822—Chalcogenides with rare earth metals
• • 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 materials, e.g. electroluminescent or chemiluminescent
  • C09K11/08—Luminescent materials, e.g. electroluminescent or chemiluminescent containing inorganic luminescent materials
  • C09K11/74—Luminescent materials, e.g. electroluminescent or chemiluminescent containing inorganic luminescent materials containing arsenic, antimony or bismuth
  • C09K11/7407—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 materials, e.g. electroluminescent or chemiluminescent
  • C09K11/08—Luminescent materials, e.g. electroluminescent or chemiluminescent containing inorganic luminescent materials
  • C09K11/77—Luminescent materials, e.g. electroluminescent or chemiluminescent containing inorganic luminescent materials containing rare earth metals
  • C09K11/7701—Chalogenides
• • 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 materials, e.g. electroluminescent or chemiluminescent
  • C09K11/08—Luminescent materials, e.g. electroluminescent or chemiluminescent containing inorganic luminescent materials
  • C09K11/77—Luminescent materials, e.g. electroluminescent or chemiluminescent containing inorganic luminescent materials containing rare earth metals
  • C09K11/7713—Sulfates
• • H—ELECTRICITY
  • H01—ELECTRIC ELEMENTS
  • H01J—ELECTRIC DISCHARGE TUBES OR DISCHARGE LAMPS
  • H01J61/00—Gas-discharge or vapour-discharge lamps
  • H01J61/02—Details
  • H01J61/38—Devices for influencing the colour or wavelength of the light
  • H01J61/40—Devices for influencing the colour or wavelength of the light by light filters; by coloured coatings in or on the envelope
• • H—ELECTRICITY
  • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
  • H05B—ELECTRIC HEATING; ELECTRIC LIGHT SOURCES NOT OTHERWISE PROVIDED FOR; CIRCUIT ARRANGEMENTS FOR ELECTRIC LIGHT SOURCES, IN GENERAL
  • H05B33/00—Electroluminescent light sources
  • H05B33/12—Light sources with substantially two-dimensional [2D] radiating surfaces
  • H05B33/14—Light sources with substantially two-dimensional [2D] radiating surfaces characterised by the chemical or physical composition or the arrangement of the electroluminescent material, or by the simultaneous addition of the electroluminescent material in or onto the light source
• • H—ELECTRICITY
  • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
  • H05B—ELECTRIC HEATING; ELECTRIC LIGHT SOURCES NOT OTHERWISE PROVIDED FOR; CIRCUIT ARRANGEMENTS FOR ELECTRIC LIGHT SOURCES, IN GENERAL
  • H05B33/00—Electroluminescent light sources
  • H05B33/12—Light sources with substantially two-dimensional [2D] radiating surfaces
  • H05B33/18—Light sources with substantially two-dimensional [2D] radiating surfaces characterised by the nature or concentration of the activator
• • A—HUMAN NECESSITIES
  • A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
  • A61L—METHODS OR APPARATUS FOR STERILISING MATERIALS OR OBJECTS IN GENERAL; DISINFECTION, STERILISATION OR DEODORISATION OF AIR; CHEMICAL ASPECTS OF BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES; MATERIALS FOR BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES
  • A61L2/00—Disinfection or sterilisation of materials or objects, in general; Accessories therefor
  • A61L2/02—Disinfection or sterilisation of materials or objects, in general; Accessories therefor using physical processes
  • A61L2/08—Radiation
  • A61L2/10—Ultraviolet [UV] radiation
• • A—HUMAN NECESSITIES
  • A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
  • A61L—METHODS OR APPARATUS FOR STERILISING MATERIALS OR OBJECTS IN GENERAL; DISINFECTION, STERILISATION OR DEODORISATION OF AIR; CHEMICAL ASPECTS OF BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES; MATERIALS FOR BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES
  • A61L2103/00—Materials or objects being the target of disinfection or sterilisation
  • A61L2103/05—Living organisms or biological materials
• • A—HUMAN NECESSITIES
  • A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
  • A61N—ELECTROTHERAPY; MAGNETOTHERAPY; RADIATION THERAPY; ULTRASOUND THERAPY
  • A61N5/00—Radiation therapy
  • A61N5/06—Radiation therapy using light
  • A61N2005/0658—Radiation therapy using light characterised by the wavelength of light used
  • A61N2005/0661—Radiation therapy using light characterised by the wavelength of light used ultraviolet
• • 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
  • H01J—ELECTRIC DISCHARGE TUBES OR DISCHARGE LAMPS
  • H01J1/00—Details of electrodes, of magnetic control means, of screens, or of the mounting or spacing thereof, common to two or more basic types of discharge tubes or lamps
  • H01J1/54—Screens on or from which an image or pattern is formed, picked-up, converted, or stored; Luminescent coatings on vessels
  • H01J1/62—Luminescent screens; Selection of materials for luminescent coatings on vessels

Definitions

• the present invention relates to the field of UV emitting luminescent compounds e.g. for use in UV lamps. BACKGROUND OF THE INVENTION
• Fluorescent lamps which comprise an UV emitting phosphor are widely used for many applications, including disinfection and purification, skin tanning, medical treatments of the skin, polymer hardening, and semiconductor wafer processing.
• UV radiation sources are based on low- or medium-pressure mercury (Hg) discharge (also referred to as mercury- vapor lamps).
• Hg medium-pressure mercury
• the emission line spectrum of a low-pressure Hg discharge is dominated by the 185 nm and 245 nm lines. Increasing the pressure results in line broadening, increasing emission in the visible spectrum at the cost of UV emission.
• medium-pressure Hg discharge are less efficient as UV emitters.
• the efficiency of Hg discharge lamps is strongly dependent on temperature due to the change in Hg vapor pressure. Moreover, the spectrum changes with lamp drive conditions and temperature, which is undesirable.
• An excimer discharge lamp is a discharge lamp in which at least one component of the discharge-maintaining gas filling forms an excimer during operation of the lamp.
• Xenon (Xe) excimer discharge emits light mainly of 172 nm
• dielectric barrier driven quartz lamp comprising Xe as a filling gas shows a wall plug efficiency of more than 50 %.
• Xe as the excimer- forming gas filling component there are other well known excimer- forming filling components like Ne.
• Xe excimer discharge lamps using a fluorescent compound for conversion of discharge emission into visible light or into UV light have been described, e.g. in
• UV emitting wavelength converting materials also referred to as UV-emitting luminescent materials or UV-emitting phosphors
• drawbacks such as undesirably low conversion efficiency, low photochemical and/or chemical stability, Lewis alkalinity, undesirable chemical interaction with the discharge resulting in degradation of the UV-emitting luminescent material, and undesirably low disinfection efficiency due to spectral mismatch with the germicidal action curve.
• US 2008/02588601 in the presence of the excimer discharge may require a protective coating e.g. of alumina, which reduces the conversion efficiency.
• a wavelength converting material comprising a compound of the formula:
• the wavelength converting material provides intense and efficient conversion of UV light of the wavelength range of 100 to 200 nm into light of the wavelength range of 200 to 300 nm.
• the wavelength converting material thus has high quantum efficiency.
• the UV emission from the present wavelength converting material has a high degree of overlap with the germicidal action curve (GAC), for example an integral overlap of at least 70 %.
• GAC germicidal action curve
• the present wavelength converting material is also temperature stable and thus tolerates the high operating temperature of an excimer lamp. Additionally, the rare earth metal sulphates are easy to produce.
• Me is at least one of trivalent praseodymium ions (Pr ), neodymium ions (Nd ) and bismuth ions (Bi ).
• Pr trivalent praseodymium ions
• Nd neodymium ions
• Bi bismuth ions
• the 4f-5d transitions of Pr and Nd 3+ provide fast luminescence, having a large absorption cross-section (high probability of an absorption process), and result in efficient wavelength converting materials. This is also true for the 6s-6p transition of Bi 3+
• a is in the range of 0.002 to 0.1, and typically is in the range of 0.01 ot 0.04 (corresponding to an Me content of 0.5 to 2 at. %).
• Such contents of the dopant (Me) provides particularly good absorption and avoids or reduces concentration quenching.
• Me comprises at least one of Pr 3+ , Nd 3+ and
• Bi 3+ and additionally at least one further trivalent cation.
• the present invention relates to a wavelength converting screen or a wavelength converting coating, comprising a wavelength converting material as defined above.
• a wavelength converting screen or a wavelength converting coating comprising a wavelength converting material as defined above.
• Such a screen or coating is typically used in an excimer discharge lamp, in which it is arranged to receive UV light resulting from the discharge.
• the invention provides an illumination device comprising a source of UV light to be converted, i.e. a source of unconverted light, and a wavelength converting material or a wavelength converting screen or coating as described above, for converting the UV light from said source.
• the illumination device may be a discharge lamp comprising a discharge vessel containing a gas comprising one or more of Ar, Kr, Xe, F 2 , Cl 2 , Br 2 , and I 2 , and means for creating an electrical discharge, and wherein at least part of a wall of the discharge vessel is provided with a wavelength converting material as described above, e.g. in the form of a coating.
• the illumination device may be or form part of a medical device or a cosmetic treatment device.
• the invention provides a cosmetic treatment device comprising a wavelength converting composition as defined above, a wavelength converting screen or coating as defined above, and/or an illumination device as defined above.
• the invention provides a medical device comprising a wavelength converting composition as defined above, a wavelength converting screen or coating as defined above, and/or an illumination device as defined above.
• the medical device may be a phototherapy device.
• the illumination device described above may form part of a system for UV illumination comprising e.g. optical components, such as lenses, waveguides etc, control circuitry and devices, cooling arrangements, mechanical support structures, etc.
• a system for UV illumination comprising e.g. optical components, such as lenses, waveguides etc, control circuitry and devices, cooling arrangements, mechanical support structures, etc.
• Such a system may be a system for sterilization, disinfection and/or purification by germicidal UV illumination.
• a system comprising said illumination device may be a medical device system.
• said system may be a chemical reactor, or a photoetching equipment.
• the present invention relates to the use of a wavelength converting composition as defined above for sterilization, disinfection or purification.
• the invention relates to the use of a wavelength converting composition as defined above in a cosmetic treatment method, typically tanning.
• the invention provides a method of producing a wavelength converting composition as defined above, comprising: reacting an oxide of Y, Lu, Sc La or Gd, with a sulphate or oxide of said trivalent cation in a sulphuric acid-containing medium; and removing said medium.
• steps are typically followed by a step of disintegrating, e.g. milling, the reaction product, and then by annealing the disintegrated reaction product, to obtain a crystal lattice of rare earth metal orthosulphate containing a dopant dispersed therein.
• Fig. 1 shows the emission spectrum of a Pr 3+ doped yttrium orthosulphates at various dopant concentrations.
• Fig. 2 shows the emission spectrum of a Pr 3+ doped yttrium orthosulphate and the germicidal action curve.
• Fig. 3 is a schematic cross-sectional view of a UV emitting discharge lamp according to embodiments of the invention.
• Fig. 4a shows the XRD pattern of a wavelength converting compound
• Fig. 4b shows the reflection, excitation and emission spectra of a wavelength converting compound according to an embodiment of the invention
• FIG. 5a-b show respectively the XRD pattern and the reflection (unbroken line), excitation (broken line) and emission (dotted line) spectra of another wavelength converting compound according to an embodiment of the invention (Lu 2 (S0 4 ) 3 :Pr).
• Fig. 6a-b show respectively the XRD pattern and the reflection (unbroken line), excitation (broken line) and emission (dotted line) spectra of another wavelength converting compound according to an embodiment of the invention (La 2 (S0 4 ) 3 :Pr).
• Fig. 7a-b show respectively the XRD pattern and the reflection, excitation and emission spectra of another wavelength converting compound according to an embodiment of the invention (Y 2 (S0 4 ) 3 :Nd).
• Fig. 8 a-c show respectively the XRD pattern and the reflection (Fig. b) and emission (Fig. 8c) spectra of another wavelength converting compound according to the embodiment of the invention
• Fig. 9a-b show respectively the XRD pattern and the reflection, excitation and emission spectra of another wavelength converting compound according to an embodiment of the invention (Lu 2 (S0 4 ) 3 :Nd).
• the present inventors have found that certain rare earth metal oxide sulfates doped with Pr 3+ , Nd 3+ or Bi 3+ have excellent properties for use as VUV to UV-C converting compounds e.g. for use in excimer discharge lamps.
• the wavelength converting compounds according to the invention have the general formula Ln 2 (S0 4 ) 3 :Me, or more specifically Ln 2 - a (S0 4 ) 3 :Me a (which may also be written Ln 2 -aMe a (S0 4 ) 3 ), in which Ln is one or more of yttrium (Y), scandium (Sc), lanthanum (La), gadolinium (Ga) and lutetium (Lu), and Me is a trivalent cation, a being in the range from 0.0005 to 0.2.
• the wavelength converting compound has the formula
• w, x, y and z is in the range from 0.0 to 1.0 and w+x+y+z ⁇ 1.0, and wherein Me and a respectively are as defined above.
• a may be in the range from 0.001 to 0.1, typically from 0.002 to 0.1, or from 0.01 to 0.04.
• the sulfate of Sc, Y, La, Gd and/or Lu provides a host lattice which is activated by small amounts of Me as an activator, also referred to as a dopant.
• Me represents a trivalent cation, typically ions of bismuth (Bi 3+ ), praseodymium (Pr 3+ ) or neodymium (Nd 3+ ).
• the activator Me is capable of emitting UV light in the range of 200-300 nm.
• a wavelength converting compound refers to a compound which is capable of absorbing electromagnetic radiation of a particular wavelength or wavelength range and of emitting electromagnetic radiation of a different wavelength or wavelength range, typically of a longer wavelength.
• a wavelength converting material refers to a material having the same capability of absorption and emission as a wavelength converting compound.
• a wavelength converting material may be composed of a single type of wavelength converting compound or of a mixture of different types of wavelength converting compounds.
• activator or "dopant” refers to an impurity present in a host lattice, in particular trivalent ions, which is capable of emitting UV radiation upon excitation.
• Wavelength converting compounds according to the invention have been found to have intense and efficient emission of UV radiation in the wavelength range of 200- 300 nm, for example 200-280 nm or 220-300 nm.
• Fig. 1 shows the emission spectra of a wavelength converting compound according to embodiments of the invention having the formula Y 2 (S0 4 )3:Pr (Pr 3+ doped yttrium orthosulfate), at different concentrations of the dopant.
• the tested compounds contained Pr at a content of 0.2 atomic % (at.%), 0.5 at.%, 1 at.%, 2 at.% or 4 at.%, respectively.
• the dopant percentage refers to atomic %, i.e. the relative number of activator atoms (Me atoms) replacing atoms of the crystallographic site.
• the emission spectrum of the wavelength converting compounds according to the invention have a large overlap with the germicidal action curve (GAC), which shows the germicidal effect of UV light on E. coli.
• GAC germicidal action curve
• This effect is mainly achieved by radiation of 200-300 nm.
• the emission from a Pr 3+ doped yttrium orthosulphate according to embodiments of the invention has a large spectral overlap with the germicidal action curve, the integral overlap being of about 71 %.
• the wavelength converting compounds of the invention are useful as converters of very short wavelength UV radiation (typically VUV, having a wavelength of 100-200 nm) into UV light of 200-300 nm, for example 200- 280 nm (representing part of the UV-C spectrum) or 220-300 nm, or 220-280 nm.
• the wavelength converting compounds of the invention may have strong absorption in the range of 100-200 nm, in particular 150-180 nm.
• UV emission from the wavelength converting compounds according to embodiments of the invention may be useful in various applications.
• the wavelength converting compounds may be particularly useful for ultraviolet germicidal irradiation to achieve sterilization, disinfection and/or purification, e.g. of food, air or water, such as drinking water, waste water, pool or pond water and the like, of objects such as laboratory or medical equipment, keyboards, personal care appliances such as tooth brushes and shavers, cosmetic tools, etc.
• the wavelength converting compounds of the invention may also be useful for UV irradiation for purposes other than sterilization, disinfection and/or purification.
• the UV emission of the present wavelength converting compounds may be used for medical or cosmetic treatment of humans or animals, e.g. cosmetic or medical treatment of the skin.
• cosmetic treatment by UV irradiation include tanning.
• medical treatment by UV irradiation include treatment of skin conditions and diseases, such as psoriasis, vitiligo, acne, and treatment of vitamin D deficiency.
• UV irradiation with the emission wavelengths of the present wavelength converting compounds may be useful to achieve chemical reactions such as crosslinking, photopolymerization, photooxidation, photoreduction, and photocatalysis, and other photochemical applications.
• UV irradiation with the emission wavelengths of the present wavelength converting compounds may be useful in the processing of semiconductor wafers, in particular for photoetching.
• the wavelength converting compounds of the invention may be applied in UV emitting illumination devices for a wide range of applications.
• a wavelength converting compound according to the invention may be applied in a UV emitting discharge lamp.
• the inner wall of the discharge vessel of a discharge lamp may be provided with a wavelength converting coating containing the wavelength converting compound.
• a discharge lamp according to embodiments of the invention is shown in cross-section in Fig. 3.
• the discharge lamp 30 has the general structure of a conventional discharge lamp and comprises a cylindrical glass tube 31 forming a discharge vessel.
• the glass tube 31 contains a gas comprising one or more of Ar, Kr, Xe, F 2 , Cl 2 , Br 2 , and I 2 , typically Xe .
• the inner surface of the glass tube 31 is provided with a wavelength converting coating 32 comprising a wavelength converting material comprising a wavelength converting compound according to the invention.
• the coating 32 may comprise more than one type of wavelength converting compound.
• the discharge lamp 30 is also provided with conventional electrodes 33 for providing an electrical field across the vessel 31 and the gas contained therein.
• the discharge lamp is an excimer discharge lamp, such as a xenon (Xe) excimer discharge lamp, a neon (Ne) excimer discharge lamo, or a xenon/neon excimer discharge lamp.
• Xe xenon
• Ne neon
• a discharge lamp in particular an Xe, Ne or Xe/Ne excimer discharge lamp may be applied in a medical device for phototherapy, in particular phototherapy of the skin; a cosmetic device for cosmetic treatment, in particular of the skins; a system for sterilization, disinfection and/or purification; a chemical reactor; and a system for processing, in particular photoetching, of semiconductor wafers.
• the wavelength converting compounds of the present invention may be produced by reacting an oxide of Y, Lu, Sc La or Gd, respectively, with a sulphate or oxide of the trivalent cation intended as activator (in particular Bi 3+ , Pr 3+ or Nd 3+ ) in an acid medium, typically containing sulphuric acid.
• the reaction product is then disintegrated, e.g. by milling or grinding, and annealed at high temperature, for example at a temperature in the range of from 500°C to 900°C, to obtain the host lattice and to distribute the activator therein by diffusion.
• said reacting can be achieved by dissolving said oxide of Y, Lu, Sc La or Gd, together with said sulphate or oxide in sulphuric acid, and heating the resulting solution to a temperature in the range of about 600°C to about 800°C for a time period of from 1 to 8 hours, such as from 2 to 6 hours, and typically about 4 hours, and removing said sulphuric acid medium e.g. by allowing it to evaporate.

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• 2011
  • 2011-12-13 US US13/977,800 patent/US20130289132A1/en not_active Abandoned
  • 2011-12-13 JP JP2013546784A patent/JP5897600B2/ja not_active Expired - Fee Related
  • 2011-12-13 WO PCT/IB2011/055626 patent/WO2012093298A1/en not_active Ceased
  • 2011-12-13 CN CN201180064126.XA patent/CN103328609B/zh not_active Expired - Fee Related
  • 2011-12-13 EP EP11807764.3A patent/EP2661474B1/en not_active Not-in-force
  • 2011-12-13 RU RU2013136489/05A patent/RU2581864C2/ru not_active IP Right Cessation

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