WO2015033824A1 - Feuille de conversion de longueur d'onde, élément semi-conducteur optique fermé et dispositif à élément semi-conducteur optique - Google Patents

Feuille de conversion de longueur d'onde, élément semi-conducteur optique fermé et dispositif à élément semi-conducteur optique Download PDF

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WO2015033824A1
WO2015033824A1 PCT/JP2014/072343 JP2014072343W WO2015033824A1 WO 2015033824 A1 WO2015033824 A1 WO 2015033824A1 JP 2014072343 W JP2014072343 W JP 2014072343W WO 2015033824 A1 WO2015033824 A1 WO 2015033824A1
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optical semiconductor
wavelength conversion
semiconductor element
conversion sheet
group
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PCT/JP2014/072343
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English (en)
Japanese (ja)
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宗久 三谷
悠紀 江部
片山　博之
宏中 藤井
正路 山田
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日東電工株式会社
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Priority to KR1020167005624A priority Critical patent/KR20160055141A/ko
Priority to CN201480048721.8A priority patent/CN105518104A/zh
Publication of WO2015033824A1 publication Critical patent/WO2015033824A1/fr

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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
    • C09K11/77—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials containing rare earth metals
    • C09K11/7766—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials containing rare earth metals containing two or more rare earth metals
    • C09K11/7774—Aluminates
    • 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
    • C09K11/77—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials containing rare earth metals
    • C09K11/7728—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials containing rare earth metals containing europium
    • C09K11/7734—Aluminates
    • 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
    • C09K11/77—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials containing rare earth metals
    • C09K11/7728—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials containing rare earth metals containing europium
    • C09K11/77348—Silicon Aluminium Nitrides or Silicon Aluminium Oxynitrides
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F21—LIGHTING
    • F21V—FUNCTIONAL FEATURES OR DETAILS OF LIGHTING DEVICES OR SYSTEMS THEREOF; STRUCTURAL COMBINATIONS OF LIGHTING DEVICES WITH OTHER ARTICLES, NOT OTHERWISE PROVIDED FOR
    • F21V9/00—Elements for modifying spectral properties, polarisation or intensity of the light emitted, e.g. filters
    • F21V9/30—Elements containing photoluminescent material distinct from or spaced from the light source
    • F21V9/32—Elements containing photoluminescent material distinct from or spaced from the light source characterised by the arrangement of the photoluminescent material
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F21—LIGHTING
    • F21V—FUNCTIONAL FEATURES OR DETAILS OF LIGHTING DEVICES OR SYSTEMS THEREOF; STRUCTURAL COMBINATIONS OF LIGHTING DEVICES WITH OTHER ARTICLES, NOT OTHERWISE PROVIDED FOR
    • F21V9/00—Elements for modifying spectral properties, polarisation or intensity of the light emitted, e.g. filters
    • F21V9/30—Elements containing photoluminescent material distinct from or spaced from the light source
    • F21V9/38—Combination of two or more photoluminescent elements of different materials
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L33/00—Semiconductor devices with at least one potential-jump barrier or surface barrier 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 with at least one potential-jump barrier or surface barrier 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
    • H01L33/483—Containers
    • H01L33/486—Containers adapted for surface mounting
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L33/00—Semiconductor devices with at least one potential-jump barrier or surface barrier 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 with at least one potential-jump barrier or surface barrier 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 with at least one potential-jump barrier or surface barrier 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 with at least one potential-jump barrier or surface barrier 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
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L2224/00—Indexing scheme for arrangements for connecting or disconnecting semiconductor or solid-state bodies and methods related thereto as covered by H01L24/00
    • H01L2224/01—Means for bonding being attached to, or being formed on, the surface to be connected, e.g. chip-to-package, die-attach, "first-level" interconnects; Manufacturing methods related thereto
    • H01L2224/42—Wire connectors; Manufacturing methods related thereto
    • H01L2224/47—Structure, shape, material or disposition of the wire connectors after the connecting process
    • H01L2224/48—Structure, shape, material or disposition of the wire connectors after the connecting process of an individual wire connector
    • H01L2224/4805—Shape
    • H01L2224/4809—Loop shape
    • H01L2224/48091—Arched
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L2933/00—Details relating to devices covered by the group H01L33/00 but not provided for in its subgroups
    • H01L2933/0008—Processes
    • H01L2933/0033—Processes relating to semiconductor body packages
    • H01L2933/005—Processes relating to semiconductor body packages relating to encapsulations
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L2933/00—Details relating to devices covered by the group H01L33/00 but not provided for in its subgroups
    • H01L2933/0091—Scattering means in or on the semiconductor body or semiconductor body package
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L33/00—Semiconductor devices with at least one potential-jump barrier or surface barrier 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 with at least one potential-jump barrier or surface barrier 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

Definitions

  • the present invention relates to a wavelength conversion sheet, a sealed optical semiconductor element, and an optical semiconductor element device, and more particularly to a wavelength conversion sheet, a sealed optical semiconductor element, and an optical semiconductor element device used for optical applications.
  • white light semiconductor devices are known as light emitting devices capable of emitting high energy light.
  • the white light semiconductor device includes, for example, an optical semiconductor element that emits blue light, and a sealing material that seals the optical semiconductor element and converts blue light (wavelength) into yellow light.
  • White light emission is realized by mixing yellow and the like.
  • a sealing material for such a white light semiconductor device for example, a sheet-shaped optical semiconductor sealing material containing a silicone resin, a phosphor, and silica particles has been proposed (for example, see Patent Document 1 below). ).
  • the sheet-shaped optical semiconductor encapsulant has a problem that the chromaticity of light that has passed through the encapsulant has a large variation. As a result, color unevenness occurs in white light emitted from the optical semiconductor device.
  • An object of the present invention is to provide a wavelength conversion sheet, a sealed optical semiconductor element, and an optical semiconductor element device that can suppress variations in chromaticity.
  • the wavelength conversion sheet of the present invention is formed from a phosphor resin composition containing a silicone resin, organic particles, and a phosphor, and the organic particles have a refractive index of 1.45 to 1.60.
  • the content ratio of the organic particles in the wavelength conversion sheet is 10 to 25% by mass.
  • the total content of the organic particles and the phosphor in the wavelength conversion sheet is 15 to 70% by mass.
  • the organic particles are made of at least one material selected from the group consisting of acrylic resins, acrylic-styrene resins, and styrene resins.
  • the phosphor contains a CaAlSiN 3 : Eu phosphor.
  • the optical semiconductor element of the present invention is characterized by comprising an optical semiconductor element and the above-described wavelength conversion sheet disposed to face the optical semiconductor element.
  • an optical semiconductor device of the present invention is characterized by comprising a substrate, an optical semiconductor element mounted on the substrate, and the above-described wavelength conversion sheet disposed to face the optical semiconductor element.
  • the wavelength conversion sheet of the present invention contains organic particles having a refractive index of 1.45 to 1.60, it suppresses variation in chromaticity compared to the case of containing other additives. can do.
  • optical semiconductor element and the optical semiconductor device are provided with the wavelength conversion sheet of the present invention, they can emit uniform white light (with little color unevenness).
  • FIG. 1A to 1B are process diagrams showing a process for producing an embodiment of the wavelength conversion sheet of the present invention, wherein FIG. 1A is a process for preparing a release substrate, and FIG. 1B is a process for laminating a wavelength conversion sheet.
  • the process to perform is shown.
  • 2A to 2D show a process of manufacturing an embodiment of the optical semiconductor device of the present invention using the wavelength conversion sheet shown in FIG. 1B
  • FIG. 2A shows a sealing layer lamination process
  • FIG. 2B shows an arrangement process
  • 2C shows a sealing process
  • FIG. 2D shows a peeling process.
  • 3A to 3E show a process for manufacturing a modified example of the optical semiconductor device using the wavelength conversion sheet shown in FIG. 1B.
  • FIG. 1A is a process for preparing a release substrate
  • FIG. 1B is a process for laminating a wavelength conversion sheet.
  • the process to perform is shown.
  • 2A to 2D show a process of manufacturing an embodiment of the optical
  • FIG. 3A shows a sealing layer lamination process
  • FIG. 3B shows an arrangement process
  • FIG. 3D shows the second peeling process
  • FIG. 3E shows the mounting process.
  • FIG. 4 shows another embodiment of the optical semiconductor device of the present invention (an embodiment in which the optical semiconductor device includes a housing).
  • FIG. 5 is a plan view illustrating a measurement method for evaluating chromaticity variation.
  • the upper side of the paper surface is the upper side (one side in the first direction, one side in the thickness direction), and the lower side of the paper surface is the lower side (the other side in the first direction, the other side in the thickness direction).
  • the direction of FIG. 1 is the upper side (one side in the first direction, one side in the thickness direction)
  • the lower side of the paper surface is the lower side (the other side in the first direction, the other side in the thickness direction).
  • the wavelength conversion sheet of the present invention is formed into a sheet shape from a phosphor resin composition containing a silicone resin, organic particles and a phosphor.
  • silicone resin examples include a transparent silicone resin used as a sealing material for sealing the optical semiconductor element, and a known or commercially available one can be used.
  • silicone resin examples include a two-stage reaction curable resin and a one-stage reaction curable resin.
  • the two-stage reaction curable resin has two reaction mechanisms. In the first stage reaction, the A stage state is changed to the B stage (semi-cured), and then in the second stage reaction, the B stage state is obtained. To C-stage (complete curing). That is, the two-stage reaction curable resin is a thermosetting resin that can be in a B-stage state under appropriate heating conditions. However, the two-stage reaction curable resin can be changed from the A-stage state to the C-stage state at a time without maintaining the B-stage state by intense heating.
  • the B stage state is a state between the A stage state in which the thermosetting resin is liquid and the C stage state in which the thermosetting resin is completely cured. It is a semi-solid or solid state smaller than the elastic modulus in the C-stage state.
  • the first-stage reaction curable resin has one reaction mechanism, and can be C-staged (completely cured) from the A-stage state by the first-stage reaction.
  • the first-stage reaction curable resin can be changed from the A-stage state to the B-stage state in the middle of the first-stage reaction. Is resumed, and includes a thermosetting resin that can be converted into a C stage (completely cured) from the B stage state. That is, such a thermosetting resin is a thermosetting resin that can be in a B-stage state.
  • the first-stage reaction curable resin cannot be controlled to stop in the middle of the first-stage reaction, that is, cannot enter the B stage state, and is changed from the A stage state to the C stage (completely cured).
  • A) thermosetting resin is a thermosetting resin that can be in a B-stage reaction.
  • the silicone resin include, for example, a condensation / addition reaction curable silicone resin composition, a heteroatom-containing modified silicone resin composition, an addition reaction curable silicone resin composition, an inorganic oxide-containing silicone resin composition, It consists of a silicone resin composition such as a thermoplastic / thermosetting silicone resin composition.
  • the silicone resin composition may be used alone or in combination.
  • silicone resin compositions from the viewpoint of transparency, durability, heat resistance, light resistance, and suppression of chromaticity variation, addition reaction curable silicone resin compositions, condensation / addition reaction curable silicone resin compositions are preferred. And more preferably, an addition reaction curable silicone resin composition.
  • the addition reaction curable silicone resin composition is a one-step reaction curable resin and contains, for example, an alkenyl group-containing polysiloxane, a hydrosilyl group-containing polysiloxane, and a hydrosilylation catalyst.
  • the alkenyl group-containing polysiloxane contains two or more alkenyl groups and / or cycloalkenyl groups in the molecule.
  • the alkenyl group-containing polysiloxane is specifically represented by the following average composition formula (1).
  • R 1 a R 2 b SiO (4-ab) / 2 (In the formula, R 1 represents an alkenyl group having 2 to 10 carbon atoms and / or a cycloalkenyl group having 3 to 10 carbon atoms. R 2 represents an unsubstituted or substituted monovalent carbon atom having 1 to 10 carbon atoms.
  • a hydrogen group (excluding an alkenyl group and a cycloalkenyl group); a is from 0.05 to 0.50, and b is from 0.80 to 1.80.
  • examples of the alkenyl group represented by R 1 include alkenyl having 2 to 10 carbon atoms such as vinyl, allyl, propenyl, butenyl, pentenyl, hexenyl, heptenyl, octenyl and the like. Groups.
  • examples of the cycloalkenyl group represented by R 1 include a cycloalkenyl group having 3 to 10 carbon atoms such as a cyclohexenyl group and a norbornenyl group.
  • R 1 is preferably an alkenyl group, more preferably an alkenyl group having 2 to 4 carbon atoms, and still more preferably a vinyl group.
  • the alkenyl groups represented by R 1 may be the same type or a plurality of types.
  • the monovalent hydrocarbon group represented by R 2 is an unsubstituted or substituted monovalent hydrocarbon group having 1 to 10 carbon atoms other than an alkenyl group and a cycloalkenyl group.
  • Examples of the unsubstituted monovalent hydrocarbon group include a methyl group, an ethyl group, a propyl group, an isopropyl group, a butyl group, an isobutyl group, a sec-butyl group, a tert-butyl group, a pentyl group, a hexyl group, and a pentyl group.
  • Alkyl groups having 1 to 10 carbon atoms such as heptyl group, octyl group, 2-ethylhexyl group, nonyl group and decyl group, for example, cyclohexane having 3 to 6 carbon atoms such as cyclopropyl, cyclobutyl group, cyclopentyl group and cyclohexyl group.
  • alkyl groups such as aryl groups having 6 to 10 carbon atoms such as phenyl, tolyl and naphthyl groups, and aralkyl groups having 7 to 8 carbon atoms such as benzyl and benzylethyl groups.
  • Preferred examples include an alkyl group having 1 to 3 carbon atoms and an aryl group having 6 to 10 carbon atoms, and more preferred examples include a methyl group and / or a phenyl group.
  • examples of the substituted monovalent hydrocarbon group include those obtained by substituting a hydrogen atom in the above-mentioned unsubstituted monovalent hydrocarbon group with a substituent.
  • substituents examples include a halogen atom such as a chlorine atom, such as a glycidyl ether group.
  • substituted monovalent hydrocarbon group examples include a 3-chloropropyl group and a glycidoxypropyl group.
  • the monovalent hydrocarbon group may be unsubstituted or substituted, and is preferably unsubstituted.
  • the monovalent hydrocarbon groups represented by R 2 may be of the same type or a plurality of types.
  • a methyl group and / or a phenyl group are mentioned, More preferably, combined use of a methyl group and a phenyl group is mentioned.
  • A is preferably 0.10 or more and 0.40 or less.
  • B is preferably 1.5 or more and 1.75 or less.
  • the weight average molecular weight of the alkenyl group-containing polysiloxane is, for example, 100 or more, preferably 500 or more, and for example, 10,000 or less, preferably 5000 or less.
  • the weight average molecular weight of the alkenyl group-containing polysiloxane is a conversion value based on standard polystyrene measured by gel permeation chromatography.
  • the alkenyl group-containing polysiloxane is prepared by an appropriate method, and a commercially available product can also be used.
  • alkenyl group-containing polysiloxane may be of the same type or a plurality of types.
  • the hydrosilyl group-containing polysiloxane contains, for example, two or more hydrosilyl groups (SiH groups) in the molecule.
  • the hydrosilyl group-containing polysiloxane is represented by the following average composition formula (2).
  • composition formula (2) H c R 3 d SiO (4-cd) / 2 (Wherein R 3 represents an unsubstituted or substituted monovalent hydrocarbon group having 1 to 10 carbon atoms (excluding an alkenyl group and / or a cycloalkenyl group), and c is 0.30 or more) 1.0, and d is 0.90 or more and 2.0 or less.)
  • R 3 represents an unsubstituted or substituted monovalent hydrocarbon group having 1 to 10 carbon atoms (excluding an alkenyl group and / or a cycloalkenyl group), and c is 0.30 or more) 1.0, and d is 0.90 or more and 2.0 or less.
  • R 3 represents an unsubstituted or substituted monovalent hydrocarbon group having 1 to 10 carbon atoms (excluding an alkenyl group and / or a cycloalkenyl group), and c is 0.30 or more) 1.0, and d is 0.90 or more and 2.0 or less.)
  • an unsubstituted monovalent hydrocarbon group having 1 to 10 carbon atoms more preferably an alkyl group having 1 to 10 carbon atoms, and an aryl group having 6 to 10 carbon atoms, more preferably a methyl group. And / or a phenyl group.
  • C is preferably 0.5 or less.
  • D is preferably 1.3 or more and 1.7 or less.
  • the weight average molecular weight of the hydrosilyl group-containing polysiloxane is, for example, 100 or more, preferably 500 or more, and for example, 10,000 or less, preferably 5000 or less.
  • the weight average molecular weight of the hydrosilyl group-containing polysiloxane is a conversion value based on standard polystyrene measured by gel permeation chromatography.
  • the hydrosilyl group-containing polysiloxane is prepared by an appropriate method, and a commercially available product can also be used.
  • hydrosilyl group-containing polysiloxane may be of the same type or a plurality of types.
  • At least one of the hydrocarbon groups R 2 and R 3 preferably includes a phenyl group, more preferably, R 2 and R 3 Both hydrocarbons contain a phenyl group.
  • the addition reaction curable silicone resin composition is a phenyl silicone resin composition.
  • This phenyl silicone resin composition is a one-stage reaction curable resin that can be in a B-stage state.
  • the addition reaction curable silicone resin composition is a methyl silicone resin composition.
  • the methyl silicone resin composition is a one-stage reaction curable resin that cannot be in a B-stage state.
  • the blending ratio of the hydrosilyl group-containing polysiloxane is the ratio of the number of moles of alkenyl groups and cycloalkenyl groups of the alkenyl group-containing polysiloxane to the number of moles of hydrosilyl groups of the hydrosilyl group-containing polysiloxane (number of moles of alkenyl groups and cycloalkenyl groups). / Number of moles of hydrosilyl group) is adjusted to be, for example, 1/30 or more, preferably 1/3 or more, and for example, 30/1 or less, preferably 3/1 or less.
  • the hydrosilylation catalyst is a substance (addition catalyst) that improves the reaction rate of the hydrosilylation reaction (hydrosilyl addition) between the alkenyl group and / or cycloalkenyl group of the alkenyl group-containing polysiloxane and the hydrosilyl group of the hydrosilyl group-containing polysiloxane. If it exists, it will not specifically limit, For example, a metal catalyst is mentioned. Examples of the metal catalyst include platinum catalysts such as platinum black, platinum chloride, chloroplatinic acid, platinum-olefin complexes, platinum-carbonyl complexes, and platinum-acetyl acetate, such as palladium catalysts such as rhodium catalyst.
  • the blending ratio of the hydrosilylation catalyst is, for example, 1.0 ppm or more on a mass basis with respect to the alkenyl group-containing polysiloxane and the hydrosilyl group-containing polysiloxane as the metal amount of the metal catalyst (specifically, metal atom).
  • Yes for example, 10000 ppm or less, preferably 1000 ppm or less, and more preferably 500 ppm or less.
  • the addition reaction curable silicone resin composition is prepared by blending an alkenyl group-containing polysiloxane, a hydrosilyl group-containing polysiloxane, and a hydrosilylation catalyst in the above-described proportions.
  • the above addition reaction curable silicone resin composition is prepared and used in an A stage (liquid) state by blending an alkenyl group-containing polysiloxane, a hydrosilyl group-containing polysiloxane, and a hydrosilylation catalyst.
  • the phenyl-based silicone resin composition undergoes a hydrosilylation addition reaction between the alkenyl group and / or cycloalkenyl group of the alkenyl group-containing polysiloxane and the hydrosilyl group of the hydrosilyl group-containing polysiloxane by heating under a desired condition.
  • the hydroaddition reaction stops once.
  • the A stage state can be changed to the B stage (semi-cured) state.
  • the above-described hydrosilylation addition reaction is resumed and completed by heating under further desired conditions.
  • the B stage state can be changed to the C stage (fully cured) state.
  • the phenyl silicone resin composition When the phenyl silicone resin composition is in the B stage (semi-cured) state, it is solid.
  • the B-staged phenyl silicone resin composition can have both thermoplasticity and thermosetting properties. That is, the B-stage phenyl silicone resin composition is once cured by heating and then completely cured.
  • the above-described methyl silicone resin composition causes a hydrosilylation addition reaction between an alkenyl group and / or a cycloalkenyl group and a hydrosilyl group, and is accelerated and completed without stopping.
  • the A stage state can be changed to the C stage (fully cured) state.
  • a commercial item is used for the methyl silicone resin composition. Examples of commercially available products include the ELASTOSIL series (manufactured by Asahi Kasei Wacker Silicone Co., specifically, methyl silicone resin compositions such as ELASTOSIL LR7665), the KER series (manufactured by Shin-Etsu Silicone), and the like.
  • the condensation / addition reaction curable silicone resin composition is a two-stage reaction curable resin, and specifically, for example, those described in JP 2010-265436 A, JP 2013-187227 A, and the like. 1 to 8 condensation / addition reaction curable silicone resin compositions, for example, JP 2013-091705 A, JP 2013-001815 A, JP 2013-001814 A, JP 2013-001813 A, Examples thereof include a cage-type octasilsesquioxane-containing silicone resin composition described in JP2012-102167A.
  • the condensation / addition reaction curable silicone resin composition is solid and has both thermoplasticity and thermosetting properties.
  • the content ratio of the silicone resin in the phosphor resin composition is, for example, 25% by mass or more, preferably 35% by mass or more, and for example, 70% by mass or less, preferably 50% by mass or less.
  • the refractive index of the silicone resin is, for example, 1.35 or more, preferably 1.40 or more, and for example, 1.65 or less, preferably 1.60 or less.
  • the refractive index of the silicone resin is calculated by an Abbe refractometer.
  • the refractive index of the silicone resin is calculated as a refractive index in a cured state (fully cured state).
  • organic particle material examples include thermoplastic resins. Specific examples include acrylic resins, styrene resins, acrylic-styrene resins, silicone resins, polycarbonate resins, benzoguanamine resins, polyolefin resins, polyester resins, polyamide resins, and polyimide resins. .
  • Such organic particles may be used alone or in combination.
  • acrylic resins styrene resins, and acrylic-styrene resins are preferable from the viewpoint of light diffusibility and availability.
  • the acrylic resin is a poly (meth) acrylic acid ester obtained by polymerizing a monomer containing a (meth) acrylic acid ester (acrylic acid ester and / or methacrylic acid ester).
  • a monomer containing a (meth) acrylic acid ester acrylic acid ester and / or methacrylic acid ester.
  • the styrene resin is, for example, a styrene polymer obtained by polymerizing a monomer containing a styrene monomer.
  • examples of the styrene resin include polystyrene and poly- ⁇ -methylstyrene.
  • the acrylic-styrene resin is an acrylic-styrene copolymer obtained by polymerizing a monomer containing a (meth) acrylic acid ester and a styrene monomer.
  • examples of the acrylic-styrene resin include (meth) methyl acrylate-styrene copolymer, (meth) ethyl acrylate-styrene copolymer, (meth) ethyl acrylate-styrene copolymer, and the like.
  • the acrylic resin, styrene resin, and acrylic-styrene resin may be a copolymer containing a copolymerizable monomer other than the acrylic monomer and the styrene monomer.
  • Preferred examples of the copolymerizable monomer include (meth) acrylic acid, acrylonitrile, ethylene, and butadiene. These copolymerizable monomers can be used alone or in combination of two or more.
  • These organic particles may be cross-linked. That is, preferably, a crosslinked acrylic resin, a crosslinked acrylic-styrene resin, and a crosslinked styrene resin are used.
  • the organic particles are in the form of particles, and the shape thereof is not particularly limited, and examples thereof include a substantially spherical shape, a substantially flat plate shape, and a substantially needle shape.
  • the average particle diameter (average of the maximum length) of the organic particles is, for example, 1 ⁇ m or more, preferably 5 ⁇ m or more, and for example, 100 ⁇ m or less, preferably 20 ⁇ m or less, more preferably 10 ⁇ m or less, and further preferably Is 9 ⁇ m or less.
  • the average particle diameter of particularly preferable organic particles is 6 ⁇ m or more and 9 ⁇ m or less, and is most preferable. Is 7 ⁇ m or more and 9 ⁇ m or less.
  • the average particle diameter of particularly preferable organic particles is 5 ⁇ m or more and 7 ⁇ m or less.
  • the average particle diameter of the organic particles is within the above range, the chromaticity variation of the wavelength conversion sheet can be further suppressed.
  • the average particle diameter of the organic particles is measured by a particle size distribution measuring device.
  • the refractive index of the organic particles is 1.45 or more, preferably 1.48 or more.
  • the refractive index is 1.60 or less, preferably 1.55 or less, more preferably 1.53 or less, and still more preferably 1.50 or less.
  • the refractive index of the organic particles is calculated by an Abbe refractometer.
  • the refractive index of the organic particles When the refractive index of the organic particles is not more than the above lower limit, the effect of light diffusion by the organic particles is low, and it is insufficient to suppress variation in chromaticity of the wavelength conversion sheet. On the other hand, when the refractive index of the organic particles exceeds the above upper limit, the refractive index difference between the silicone resin and the organic particles becomes large, and the translucency may be lowered. *
  • SSX series (refractive index 1.49, crosslinked polymethyl methacrylate particles), SBX series (refractive index 1.59, crosslinked polystyrene particles), MSX series from Sekisui Plastics Co., Ltd. (Refractive index 1.495 to 1.595, methyl methacrylate-styrene copolymer crosslinked particles), MB series (refractive index 1.49, polymethyl methacrylate particles), BMX series (refractive index 1.49, crosslinked poly) Butyl methacrylate particles).
  • the difference between the refractive index of the silicone resin and the refractive index of the organic particles is, for example, 0.04 or more, preferably 0.05 or more, and for example, 0.20 or less, preferably 0.12 or less. More preferably, it is 0.10 or less. Thereby, the dispersion
  • the true specific gravity of the organic particles is, for example, 1.00 or more, preferably 1.10 or more, and for example, 1.50 or less, preferably 1.30 or less.
  • the content ratio of the organic particles in the phosphor resin composition is, for example, 5% by mass or more, preferably 10% by mass or more, more preferably 15% by mass or more, and for example, 30% by mass or less, preferably 25% by mass or less, and more preferably 20% by mass or less.
  • the phosphor is a particle having a wavelength conversion function and may be any known phosphor used in an optical semiconductor device, for example, a yellow phosphor capable of converting blue light into yellow light, and blue light as red.
  • a yellow phosphor capable of converting blue light into yellow light
  • blue light as red.
  • Known phosphors such as a red phosphor that can be converted into light and a green phosphor that can convert blue light into green light can be used.
  • the yellow phosphor for example, Y 3 Al 5 O 12: Ce (YAG ( yttrium aluminum garnet): Ce), Tb 3 Al 3 O 12: Ce (TAG ( terbium-aluminum-garnet): Ce), etc.
  • Garnet-type phosphors having a garnet-type crystal structure such as oxynitride phosphors such as Ca- ⁇ -SiAlON.
  • YAG: Ce is mentioned.
  • red phosphor examples include nitride phosphors such as CaAlSiN 3 : Eu (CASN) and CaSiN 2 : Eu. From the viewpoint of availability, CASN is preferable.
  • the green phosphor for example, Lu 3 Al 5 O 12: Ce: garnet phosphors (LuAG ruthenium aluminum garnet) and the like.
  • a yellow phosphor alone or a combination of a red phosphor and a green phosphor is used.
  • Such phosphors may be used alone or in combination.
  • the phosphor is in the form of particles, and the shape thereof is not particularly limited, and examples thereof include a substantially spherical shape, a substantially flat plate shape, and a substantially needle shape.
  • the average particle diameter (average of the maximum length) of the phosphor is, for example, 0.1 ⁇ m or more, preferably 0.2 ⁇ m or more, more preferably 1 ⁇ m or more, and for example, 500 ⁇ m or less, preferably 200 ⁇ m or less, more preferably 50 ⁇ m or less.
  • the average particle diameter of the phosphor particles is measured by a particle size distribution measuring device.
  • the composition of the phosphor is appropriately adjusted so that the light passing through the wavelength conversion sheet becomes white corresponding to the optical semiconductor element, and the phosphor content in the phosphor resin composition is, for example, 5% by mass or more. , Preferably, it is 10 mass% or more, for example, 65 mass% or less, Preferably, it is 50 mass% or less.
  • the content ratio is, for example, 1 part by mass or more, preferably 5 parts by mass with respect to 100 parts by mass of the green phosphor. Part or more, and for example, 50 parts by mass or less, preferably 30 parts by mass or less.
  • the total content ratio of the organic particles and the phosphor in the phosphor resin composition is, for example, 15% by mass or more, preferably 20% by mass or more, and for example, 70% by mass or less, preferably 60% by mass or less.
  • the phosphor resin composition can also contain inorganic particles.
  • the inorganic particles are blended in the phosphor resin composition as necessary in order to improve the film formability.
  • examples of the inorganic particles include silica (SiO 2 ), talc (Mg 3 (Si 4 O 10 ) (HO) 2 ), alumina (Al 2 O 3 ), boron oxide (B 2 O 3 ), calcium oxide (CaO).
  • inorganic particles such as nitrides such as (AlN) and silicon nitride (Si 3 N 4 ).
  • an oxide is mentioned, More preferably, a silica is mentioned.
  • the average particle diameter (average of the maximum length) of the inorganic particles is, for example, 1 nm or more, preferably 5 nm or more, and for example, 30 ⁇ m or less, preferably 10 ⁇ m or less, more preferably 5 ⁇ m or less, even more preferably. Is 0.1 ⁇ m or less.
  • the average particle size of the inorganic particles is measured by a particle size distribution measuring device.
  • the refractive index of the inorganic particles is, for example, 1.35 or more, preferably 1.40 or more, and for example, 1.65 or less, preferably 1.60 or less.
  • the refractive index of the inorganic particles is calculated by an Abbe refractometer.
  • the phosphor composition when the phosphor composition contains a phenyl silicone resin composition, it preferably contains inorganic particles.
  • the viscosity of the phosphor composition can be increased and the film formability can be improved, so that a phenyl silicone resin-containing wavelength conversion sheet in which variations in chromaticity are suppressed can be obtained more reliably. .
  • the content ratio of the inorganic particles in the phosphor resin composition is, for example, 0.1% by mass or more, preferably 0.5% by mass or more. It is 10 mass% or less, preferably 5 mass% or less.
  • the above-mentioned phosphor resin composition may contain known additives such as a silane coupling agent, an anti-aging agent, a modifier, a surfactant, a dye, a pigment, a discoloration inhibitor, and an ultraviolet absorber as necessary. Can be added at an appropriate ratio.
  • the silicone resin, the organic particles, the phosphor, and, if necessary, the inorganic particles and additives are blended in the above blending ratio and mixed.
  • the temperature is, for example, 10 ° C. or higher, preferably 15 ° C. or higher, and for example, 40 ° C. or lower, preferably 35 ° C. or lower.
  • the phosphor resin composition is defoamed after its preparation, if necessary.
  • Examples of the defoaming method include known defoaming methods such as stirring defoaming, vacuum defoaming (vacuum defoaming), centrifugal defoaming, and ultrasonic defoaming.
  • the viscosity of the phosphor resin composition is, for example, at 25 ° C., for example, 1000 mPa ⁇ s or more, preferably 2000 mPa ⁇ s or more, preferably 50000 mPa ⁇ s or less, preferably 30000 mPa ⁇ s or less.
  • the viscosity of the phosphor resin composition is less than the lower limit, moldability or processability may be insufficient.
  • the above upper limit is exceeded, before the silicone resin composition is laminated and formed into a sheet, bubbles do not escape in the defoaming step of the phosphor resin composition (coating liquid) by stirring or the like, and bubbles are generated in the optical semiconductor device. In some cases, a color shift of the optical semiconductor device or a defect in the reliability test may occur.
  • the method for manufacturing the wavelength conversion sheet 1 includes, for example, a preparation process (see FIG. 1A) and a wavelength conversion sheet stacking process (see FIG. 1B). Hereinafter, each process is explained in full detail.
  • a release substrate 2 is prepared.
  • the peeling substrate 2 is used as a protective sheet for covering and protecting the surface of the wavelength conversion sheet 1 or a coating substrate for the wavelength conversion sheet 1.
  • the release substrate 2 is detachably attached to the back surface of the wavelength conversion sheet 1 in order to protect the wavelength conversion sheet 1 until the optical semiconductor element 5 is sealed with the wavelength conversion sheet 1. That is, the peeling substrate 2 is laminated so as to cover the back surface of the wavelength conversion sheet 1 at the time of shipping, transporting, and storing the wavelength conversion sheet 1, and the back surface of the wavelength conversion sheet 1 immediately before use of the wavelength conversion sheet 1. It is the flexible film formed from resin which can be peeled off so that it may curve in a substantially U shape. That is, the peeling base material 2 consists only of a flexible film. Moreover, the sticking surface of the flexible film is peeled off as necessary.
  • a polyester film for example, a polyethylene terephthalate film
  • a polycarbonate film for example, a polyolefin film (for example, a polyethylene film, a polypropylene film), a polystyrene film, an acrylic film, a silicone resin film, fluorine
  • a resin sheet such as a resin film, for example, a peeling plate such as a glass plate can be used.
  • the peeling process is performed to the surface (surface on the side in which the wavelength conversion sheet 1 is formed) of the peeling base material 2 as needed.
  • the thickness of the release substrate 2 is not particularly limited, but in the case of a resin sheet, for example, from the viewpoint of handleability and cost, it is, for example, 20 to 100 ⁇ m, and in the case of a release plate, for example, 0.5 to 10 mm. It is.
  • the wavelength conversion sheet 1 is laminated on the upper surface of the release substrate 2 as shown in FIG. 1B.
  • the phosphor resin composition is applied to the upper surface of the release substrate 2, for example, and then the phosphor resin composition is cured.
  • Examples of the application method include known application methods such as an applicator, cast, spin, and roll.
  • the method for curing the phosphor resin composition is appropriately determined according to the type of the silicone resin, and examples thereof include heating.
  • the temperature is, for example, 70 ° C. or higher, preferably 90 ° C. or higher, and for example, 150 ° C. or lower, preferably 130 ° C. or lower.
  • the time is, for example, 1 minute or more, preferably 3 minutes or more, and for example, 30 minutes or less, preferably 15 minutes or less.
  • the wavelength conversion sheet 1 is laminated on the upper surface of the peeling substrate 2.
  • the wavelength conversion sheet 1 is manufactured.
  • the wavelength conversion sheet 1 is preferably formed as a phosphor resin composition in a C stage state (fully cured state).
  • the C-stage state may be obtained after temporarily maintaining the B-stage state by two-stage heating. By the step heating, the C stage state may be set without maintaining the B stage state.
  • the wavelength conversion sheet 1 has a flat plate shape, specifically, has a predetermined thickness, extends in a predetermined direction orthogonal to the thickness direction, and has a flat surface and a flat back surface.
  • the wavelength conversion sheet 1 is not a light emitting device but a component of the light emitting device, that is, a component for producing the light emitting device, does not include an LED and a substrate on which the LED is mounted, and specifically, a phosphor. It is a device that is formed from a resin composition, circulates by itself, and is industrially usable.
  • C-staging reaction involves the alkenyl group and / or cycloalkenyl group of the alkenyl group-containing polysiloxane, hydrosilyl
  • hydrosilyl addition reaction with the hydrosilyl group of the group-containing polysiloxane is further accelerated. Thereafter, the alkenyl group and / or the cycloalkenyl group or the hydrosilyl group of the hydrosilyl group-containing polysiloxane disappears, and the hydrosilyl addition reaction is completed, whereby a C-staged phenyl silicone resin composition, that is, a cured product ( Product).
  • the above cured product is represented by the following average composition formula (3).
  • R 5 e SiO (4-e) / 2 (Wherein R 5 represents an unsubstituted or substituted monovalent hydrocarbon group having 1 to 10 carbon atoms, including a phenyl group (excluding alkenyl groups and cycloalkenyl groups); 3 or less.)
  • the unsubstituted or substituted monovalent hydrocarbon group having 1 to 10 carbon atoms represented by R 5 includes an unsubstituted or substituted monovalent carbon group having 1 to 10 carbon atoms represented by R 2 in the formula (1). Examples thereof are the same as the hydrogen group and the unsubstituted or substituted monovalent hydrocarbon group having 1 to 10 carbon atoms represented by R 3 in the formula (2).
  • an unsubstituted monovalent hydrocarbon group more preferably an alkyl group having 1 to 10 carbon atoms, and an aryl group having 6 to 10 carbon atoms, and more preferably a combined use of a phenyl group and a methyl group is used.
  • an unsubstituted monovalent hydrocarbon group more preferably an alkyl group having 1 to 10 carbon atoms, and an aryl group having 6 to 10 carbon atoms, and more preferably a combined use of a phenyl group and a methyl group.
  • E is preferably 1 or more and 3 or less.
  • the proportion of the phenyl groups in R 5 in the average composition formula of the cured product (3) is 30 mol% or more, preferably is 35 mol% or more, and 55 mol% or less, preferably 50 mol% It is as follows.
  • the thickness of the wavelength conversion sheet 1 is, for example, 10 ⁇ m or more, preferably 50 ⁇ m or more, and for example, 1000 ⁇ m or less, preferably 500 ⁇ m or less.
  • the variation of the chromaticity CIEx of the wavelength conversion sheet 1, that is, the difference R between the maximum value and the minimum value of the chromaticity CIEx is, for example, 0.0150 or less, preferably in the range where the film thickness of the wavelength conversion sheet 1 is 5 ⁇ m or less. 0.0100 or less, more preferably 0.0070 or less. A method for measuring variation in chromaticity will be described later in Examples.
  • the wavelength conversion sheet 1 is formed of a phosphor resin composition containing a silicone resin, organic particles having a refractive index of 1.45 to 1.60, and a phosphor. Therefore, the organic particles can diffuse light incident from the optical semiconductor element 5 into the wavelength conversion sheet 1 efficiently and uniformly inside the wavelength conversion sheet 1. As a result, the chromaticity of light passing through the wavelength conversion sheet 1 can be made uniform, and variations in chromaticity can be suppressed.
  • the manufacturing method of the optical semiconductor device 8 includes, for example, a sealing layer stacking step (see FIG. 2A), an arranging step (see FIG. 2B), a sealing step (see FIG. 2C), and a peeling step (see FIG. 2D). .
  • a sealing layer stacking step see FIG. 2A
  • an arranging step see FIG. 2B
  • a sealing step see FIG. 2C
  • a peeling step see FIG. 2D.
  • sealing layer stacking step first, as shown in FIG. 2A, the sealing layer 3 is stacked on one surface (the surface on which the release substrate 2 is not stacked) of the wavelength conversion sheet 1 manufactured in FIG. .
  • the sealing layer 3 is formed from a sealing resin composition, and such a sealing resin composition includes a known transparent resin used for embedding and sealing an optical semiconductor element, as a transparent resin.
  • a sealing resin composition includes a known transparent resin used for embedding and sealing an optical semiconductor element, as a transparent resin.
  • thermosetting resins such as silicone resins (described above), epoxy resins, and urethane resins
  • thermoplastic resins such as acrylic resins, styrene resins, polycarbonate resins, and polyolefin resins.
  • silicone resins are preferable from the viewpoints of durability, heat resistance, and light resistance.
  • a method of forming the sealing layer 3 on the wavelength conversion sheet for example, a method of directly forming the sealing layer 3 on the wavelength conversion sheet 1, a sealing layer 3 on another release substrate, or the like. After forming, the method of transferring the sealing layer 3 from the peeling base material to the wavelength conversion sheet 1 by a laminator, thermocompression bonding, etc. is mentioned.
  • the sealing layer 3 is heated to bring the sealing layer 3 made of the sealing resin composition into a B-stage state (semi-cured state).
  • the temperature is, for example, 50 ° C. or more, preferably 80 ° C. or more, and for example, 150 ° C. or less, preferably 140 ° C. or less
  • the heating time is, for example, 1 minute or more, Preferably, it is 5 minutes or more, and for example, 100 minutes or less, preferably 15 minutes or less. Note that whether or not the sealing layer 3 is in the B-stage state can be appropriately set according to the type of the thermosetting resin.
  • the wavelength conversion sheet 1 and the wavelength conversion sealing sheet 4 including the sealing layer 3 laminated thereon are obtained.
  • the substrate 7 on which the optical semiconductor element 5 is mounted and the wavelength conversion sealing sheet 4 are arranged to face each other. That is, the substrate 7 and the wavelength conversion sealing sheet 4 are arranged to face each other so that the optical semiconductor element 5 and the sealing layer 3 face each other.
  • the substrate 7 is made of an insulating substrate, for example.
  • a conductive pattern (not shown) including electrodes is formed on the surface of the substrate 7.
  • the optical semiconductor element 5 is, for example, an element that emits blue light (specifically, a blue LED), and is mounted on the substrate 7.
  • the optical semiconductor element 5 is connected to an electrode (not shown) of the substrate 7 by wire bonding.
  • a terminal (not shown) provided on the upper surface of the optical semiconductor element 5 and an electrode (not shown) provided on the upper surface of the substrate 7 are connected via a wire 6 (see a virtual line). Electrically connected.
  • the optical semiconductor element 5 may be flip-chip mounted on the substrate 7 (see solid line).
  • the optical semiconductor element 5 is embedded by the sealing layer 3 of the wavelength conversion sealing sheet 4.
  • the optical semiconductor element 5 and the wire 6 are embedded.
  • the sealing layer 3 is thermocompression bonded to the substrate 7.
  • the wavelength conversion encapsulating sheet 4 and the substrate 7 are pressed flat.
  • the temperature is, for example, 80 to 220 ° C.
  • the pressure is, for example, 0.01 to 1 MPa
  • the press time is, for example, 1 to 10 minutes.
  • the upper surface and side surfaces of the optical semiconductor element 5 and the wire are covered with the sealing layer 3 by this thermocompression bonding. That is, the optical semiconductor element 5 and the wire are embedded in the sealing layer 3.
  • the upper surface of the substrate 7 exposed from the optical semiconductor element 5 is covered with the sealing layer 3.
  • the wavelength conversion sealing sheet 4 is bonded to the optical semiconductor element 5 and the substrate 7.
  • the sealing layer 3 is in a C stage state (fully cured state).
  • peeling process In the peeling step, the peeling substrate 2 is peeled from the wavelength conversion sealing sheet 4 as shown in the phantom line of FIG. 2C and FIG. 2D.
  • the optical semiconductor device 8 is obtained as a white light emitting device.
  • the optical semiconductor device 8 includes the substrate 7, the optical semiconductor element 5 mounted on the substrate 7, the sealing layer 3 formed on the substrate 7 and encapsulating the optical semiconductor element 5, and the optical semiconductor element 5. And a wavelength conversion sheet 1 formed on the sealing layer 3.
  • the optical semiconductor element 5 mounted on the substrate 7 is sealed with the wavelength conversion sealing sheet 4 as shown in FIG. 2C.
  • the wavelength conversion sealing sheet 4 As shown in FIG. 2C, it is also possible to seal the optical semiconductor element 5 that is not yet mounted on 7 but supported by the support sheet 9.
  • the method for manufacturing the optical semiconductor device 8 includes, for example, a sealing layer stacking step (see FIG. 3A), a placement step (see FIG. 3B), a sealing step (see FIG. 3C), and a first peeling step (see FIG. 3C), a second peeling step (see FIG. 3D), and a mounting step (FIG. 3E).
  • a sealing layer stacking step see FIG. 3A
  • a placement step see FIG. 3B
  • a sealing step see FIG. 3C
  • a first peeling step see FIG. 3C
  • a second peeling step see FIG. 3D
  • a mounting step FIG. 3E
  • the sealing layer stacking step is the same as the sealing layer stacking step of the above-described embodiment.
  • the support sheet 9, the optical semiconductor element 5 supported by the support sheet 9, and the wavelength conversion sealing sheet 4 are disposed to face each other. That is, the support sheet 9 and the wavelength conversion sealing sheet 4 are arranged to face each other so that the optical semiconductor element 5 and the sealing layer 3 face each other.
  • the support sheet 9 includes a support plate 10 and an adhesive layer 11 laminated on the upper surface of the support plate 10.
  • the support plate 10 has a plate shape extending in the surface direction, is provided at a lower portion of the support sheet 9, and is formed in substantially the same shape as the support sheet 9 in plan view.
  • the support plate 10 is made of a hard material that cannot be stretched in the plane direction. Specifically, examples of such a material include silicon oxide (such as quartz), oxides such as alumina, metals such as stainless steel, An example is silicon.
  • the thickness of the support plate 10 is, for example, 0.1 to 2 mm.
  • the adhesive layer 11 is formed on the entire upper surface of the support plate 10.
  • the pressure-sensitive adhesive material that forms the pressure-sensitive adhesive layer 11 include pressure-sensitive adhesives such as acrylic pressure-sensitive adhesives and silicone-based pressure sensitive adhesives.
  • the adhesive layer 11 may be formed by, for example, an active energy ray irradiation release sheet whose adhesive strength is reduced by irradiation with an active energy ray (specifically, an active energy ray irradiation release sheet described in JP 2005-286003 A or the like). ) Or the like.
  • the thickness of the adhesive layer 11 is, for example, 0.1 to 1 mm.
  • the support plate 10 and the adhesive layer 11 are bonded together.
  • a support plate 10 is prepared, and then a varnish prepared from the above-mentioned adhesive material and a solvent blended as necessary is applied to the support plate 10, and then, if necessary, an application method in which the solvent is distilled off.
  • the pressure-sensitive adhesive layer 11 can be directly laminated on the support plate 10.
  • the thickness of the support sheet 9 is, for example, 0.2 to 6 mm.
  • the optical semiconductor element 5 is laminated on the support sheet 9. Specifically, the lower surface of the optical semiconductor element 5 is brought into contact with the upper surface of the adhesive layer 11.
  • the optical semiconductor element 5 is disposed (placed) on the support sheet 9. That is, the optical semiconductor element 5 is supported on the support sheet 9.
  • each of the sealing step and the first peeling step is the same as each of the sealing step and the peeling step of the above-described embodiment.
  • a sealed optical semiconductor element 12 including the conversion sheet 1 is obtained.
  • the sealing layer 3 covers the upper surface and side surfaces of the optical semiconductor element 5.
  • the lower surface of the optical semiconductor element 5 is exposed from the sealing layer 3 and is in contact with the upper surface of the adhesive layer 11.
  • the sealed optical semiconductor element 12 is peeled off from the upper surface of the adhesive layer 11 as indicated by an arrow in FIG. 3D. Specifically, when the adhesive layer 11 is an active energy ray irradiation release sheet, the active energy ray is irradiated to the adhesive layer 11.
  • the optical semiconductor element 5, the sealing layer 3 that seals the optical semiconductor element 5, and the wavelength conversion sheet 1 that is disposed opposite to the optical semiconductor element 5 and is formed on the sealing layer 3 are sealed.
  • the light-stopping semiconductor element 12 is obtained.
  • the sealed optical semiconductor element 12 is mounted on the substrate 7 as shown in FIG. 3E. Specifically, a terminal (not shown) provided on the lower surface of the optical semiconductor element 5 and an electrode (not shown) of the substrate 7 are connected, and the sealed optical semiconductor element 12 is flip-chip mounted on the substrate 7. .
  • the optical semiconductor device 8 including the substrate 7, the optical semiconductor element 5, the sealing layer 3, and the wavelength conversion sheet 1 is manufactured.
  • the optical semiconductor device 8 is formed on the substrate 7, the optical semiconductor element 5 mounted on the substrate 7, and the substrate 7, and the optical semiconductor element 5 is sealed.
  • the optical semiconductor device 8 is mounted on the substrate 7 and the substrate 7, for example, although not shown, although the sealing layer 3 to be formed and the wavelength conversion sheet 1 formed on the sealing layer 3 are provided.
  • the wavelength conversion sheet 1 which is formed on the optical semiconductor element 5 and the substrate 7 and seals the optical semiconductor element 5 can also be provided. That is, the optical semiconductor device 8 may not include the sealing layer 3.
  • This optical semiconductor device 8 is, for example, known in the art that a phosphor resin composition is formed on a substrate 7 on which an optical semiconductor element 5 is mounted so that the optical semiconductor element 5 (and the wire 6) is sealed. It can manufacture by apply
  • the sealed optical semiconductor element 12 is formed on the optical semiconductor element 5, the sealing layer 3 that seals the optical semiconductor element 5, and the sealing layer 3.
  • the sealed optical semiconductor element 12 may include the optical semiconductor element 5 and the wavelength conversion sheet 1 that seals the optical semiconductor element 5. That is, the optical semiconductor device 8 may not include the sealing layer 3.
  • the sealing optical semiconductor element 12 may be formed by applying a phosphor resin composition to a support sheet 9 on which the optical semiconductor element 5 is supported so that the optical semiconductor element 5 is sealed. It can manufacture by peeling the support sheet 9 after apply
  • the optical semiconductor device 8 does not include a housing disposed on the substrate 7 so as to surround the optical semiconductor element 5, but for example, as shown in FIG.
  • the optical semiconductor device 8 may include a housing 13.
  • the optical semiconductor device 8 of the embodiment of FIG. 4 includes a substrate 7, an optical semiconductor element 5 mounted on the substrate 7, a housing 13 formed on the substrate 7, and a sealing for sealing the optical semiconductor element 5.
  • a layer 3 and a wavelength conversion sheet 1 formed on the sealing layer 3 are provided.
  • the housing 13 has a substantially frame shape in a plan view, and is formed in a substantially trapezoidal cylindrical shape that becomes gradually narrower upward. Further, the housing 13 is disposed so as to surround the optical semiconductor element 5 and spaced from the optical semiconductor element 5.
  • the sealing layer 3 is filled in the housing 13.
  • the wavelength conversion sheet 1 is also formed on the entire upper surface of the sealing layer 3 and the inner end of the upper surface of the housing 13.
  • Example 1 In a disposable cup, 4.0 g of a silicone resin (LR7665, addition reaction curable silicone resin composition, manufactured by Asahi Kasei Wacker Silicone), 4.0 g of YAG phosphor (Y468, average particle size of 17 ⁇ m, manufactured by Nemoto Lumi Materials), 4.0 g And 2.0 g of cross-linked polymethyl methacrylate particles (SSX-108, organic particles, refractive index 1.49, average particle size 8 ⁇ m, manufactured by Sekisui Plastics Co., Ltd.) and stirred for 5 minutes with a spatula, Stirring and defoaming were carried out for 3 minutes using a stirrer / deaerator (Mazerustar, Kurabo Industries). Thereby, the composition (varnish) for wavelength conversion sheets was prepared. The viscosity of the wavelength conversion sheet composition was 19000 mPa ⁇ s to 25000 mPa ⁇ s.
  • LR7665 addition reaction curable silicone resin composition, manufactured by Asah
  • the glass slide was placed on a hot plate and heated at 105 ° C. for 5 minutes to cure the wavelength conversion sheet composition to produce a wavelength conversion sheet (C stage, film thickness 170 to 210 ⁇ m) ( (See FIG. 5 described later).
  • Examples 2 to 13 and Comparative Examples 1 to 3 A wavelength conversion sheet (C stage, film thickness: 170 to 210 ⁇ m) was produced in the same manner as in Example 1 except that the formulation of the wavelength conversion sheet was changed to the formulation shown in Tables 1 and 2.
  • Examples 14 to 22 and Comparative Example 4 A phenyl silicone resin composition A was prepared according to the following synthesis examples and preparation examples. Using this phenyl-based silicone resin composition A in place of LR7665, the wavelength conversion sheet (C stage, C stage, etc.) was used in the same manner as in Example 1 except that the formulation of the wavelength conversion sheet was changed to the formulation shown in Table 3. A film thickness of 170 to 210 ⁇ m was manufactured.
  • the weight average molecular weight in terms of polystyrene of the alkenyl group-containing polysiloxane A was measured by gel permeation chromatography and found to be 2300.
  • polystyrene equivalent weight average molecular weight of the alkenyl group-containing polysiloxane B was measured by gel permeation chromatography and found to be 1000.
  • the average unit formula and average composition formula of the hydrosilyl group-containing polysiloxane C are as follows.
  • polystyrene equivalent weight average molecular weight of the hydrosilyl group-containing polysiloxane C was measured by gel permeation chromatography and found to be 1000.
  • Comparative Example 5 After adding 6.0 g of silicone resin (LR7665) and 4.0 g of YAG phosphor (Y468) to the disposable cup and stirring for 5 minutes with a spatula, further stirring and defoaming with a stirrer / deaerator 3 Conducted for a minute. Thereby, the composition (varnish) for wavelength conversion layers was prepared.
  • the prepared composition for wavelength conversion layer was applied on a slide glass with an applicator.
  • the slide glass was placed on a hot plate and heated at 105 ° C. for 5 minutes to cure the wavelength conversion layer composition, thereby forming a wavelength conversion sheet (film thickness 200 ⁇ m).
  • Comparative Example 6 To the disposal cup, 9.0 g of silicone resin (LR7665) and 1.0 g of crosslinked polymethyl methacrylate particles (SSX-108) are added and stirred for 5 minutes with a spatula, and further with a stirrer / deaerator. Stirring and degassing were carried out for 3 minutes. This prepared the composition for diffusion layers (varnish).
  • the prepared composition for the diffusion layer was applied to the surface of the wavelength conversion sheet of Comparative Example 5 using an applicator.
  • the wavelength conversion sheet coated with the diffusion layer composition is placed on a hot plate and heated at 105 ° C. for 5 minutes to cure the diffusion layer composition, and the diffusion layer (film thickness 100 ⁇ m) is formed. Formed.
  • each of LR7665 and phenyl-based silicone resin composition A is allowed to react (ie, completely cured, C stage) at 100 ° C. for 1 hour without containing particles and phosphors.
  • a cured product was obtained.
  • the obtained cured product was measured with an Abbe refractometer.
  • Both LR7665 and the cured product of phenyl silicone resin composition A had a refractive index of 1.42.
  • the A-stage phenyl-based silicone resin composition A is reacted (completely cured, C-staged) at 100 ° C. for 1 hour without adding an inorganic filler to obtain a cured product (fully cured state).
  • the chromaticity CIEx was measured with a chromaticity measuring instrument (DF-1000A, manufactured by Otsuka Electronics Co., Ltd.), and the film thickness was measured with a laser displacement meter (LT-9030M, manufactured by Keyence Corporation).
  • the measured film thickness was plotted on the x-axis and the chromaticity CIEx was plotted on the y-axis. In order to eliminate the influence of the protruding light, the measurement data of 15 mm at both ends in the length direction was deleted.
  • the difference (the length in the y-axis direction) between the maximum value and the minimum value of the chromaticity CIEx was calculated for each width unit (x-axis direction) having a film thickness of 5 ⁇ m.
  • the width of the film thickness of 5 ⁇ m that minimizes the difference between the maximum value and the minimum value is selected (for example, the film thickness in the range of 195 to 200 ⁇ m in Example 1), and the maximum value of the chromaticity CIEs in this film thickness range.
  • Tables 1 to 3 show the difference R between the minimum value and the minimum value.
  • the difference R in Comparative Example 5 was 0.0170, and the difference R in Comparative Example 6 was 0.0190.
  • LR7665 trade name “ELASTOSIL LR7665”, addition reaction curable silicone resin composition (methyl silicone resin composition, one-stage reaction curable resin that cannot be in B-stage state), manufactured by Asahi Kasei Wacker Silicone Co., Ltd., crosslinked methacrylic Acid methyl particles: “SSX-108”, organic particles, refractive index 1.49, average particle size 8 ⁇ m, manufactured by Sekisui Plastics Co., Ltd./crosslinked methyl methacrylate particles: “SSX-105”, organic particles, refractive index 1.
  • Methyl laurate particles “SSX-108LXE”, organic particles, refractive index 1.545, average particle size 8 ⁇ m, manufactured by Sekisui Plastics Co., Ltd., crosslinked methyl methacrylate particles: “XX-227AA”, organic particles, refractive index 1 525, average particle size 8 ⁇ m, Sekisui Plastics Co., Ltd., silica particles: “3 sdc”, refractive index 1.45, average particle size 3.4 ⁇ m, Denki Kagaku Kogyo Co., Ltd., silicone particles: “Tospearl 2000B”, refraction 1.42, average particle size 6.0 ⁇ m, manufactured by Momentive Performance Materials Japan, Aerosil particles: “R976S”, refractive index 1.46, average particle size 7 nm, manufactured by Evonik, YAG phosphor: “ Y468 ”, YAG: Ce, average particle size 17 ⁇ m, manufactured by Nemoto Lumimaterial, LuAG phosphor:“ LP
  • the wavelength conversion sheet, the sealed optical semiconductor element and the optical semiconductor element device of the present invention can be applied to various industrial products, and can be used for optical applications such as a white light semiconductor device.

Abstract

Une feuille de conversion de longueur d'onde est caractérisée en ce qu'elle est formée d'une composition de résine à luminophore qui contient une résine de silicone, des particules organiques et un luminophore. Cette feuille de conversion de longueur d'onde est également caractérisé en ce que les particules organiques ont un indice de réfraction de 1,45 à 1,60.
PCT/JP2014/072343 2013-09-06 2014-08-26 Feuille de conversion de longueur d'onde, élément semi-conducteur optique fermé et dispositif à élément semi-conducteur optique WO2015033824A1 (fr)

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CN201480048721.8A CN105518104A (zh) 2013-09-06 2014-08-26 波长转换片、封装光半导体元件及光半导体元件装置

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