WO2011065322A1 - Procédé de fabrication d'unité de diodes électroluminescentes - Google Patents

Procédé de fabrication d'unité de diodes électroluminescentes Download PDF

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Publication number
WO2011065322A1
WO2011065322A1 PCT/JP2010/070786 JP2010070786W WO2011065322A1 WO 2011065322 A1 WO2011065322 A1 WO 2011065322A1 JP 2010070786 W JP2010070786 W JP 2010070786W WO 2011065322 A1 WO2011065322 A1 WO 2011065322A1
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Prior art keywords
phosphor
led chip
emitting diode
diode unit
glass
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PCT/JP2010/070786
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English (en)
Japanese (ja)
Inventor
卓史 波多野
修志 池永
禄人 田口
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コニカミノルタオプト株式会社
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Publication of WO2011065322A1 publication Critical patent/WO2011065322A1/fr

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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L33/00—Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
    • H01L33/48—Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by the semiconductor body packages
    • H01L33/50—Wavelength conversion elements
    • H01L33/508—Wavelength conversion elements having a non-uniform spatial arrangement or non-uniform concentration, e.g. patterned wavelength conversion layer, wavelength conversion layer with a concentration gradient of the wavelength conversion material
    • C—CHEMISTRY; METALLURGY
    • C03—GLASS; MINERAL OR SLAG WOOL
    • C03B—MANUFACTURE, SHAPING, OR SUPPLEMENTARY PROCESSES
    • C03B11/00—Pressing molten glass or performed glass reheated to equivalent low viscosity without blowing
    • C03B11/14—Pressing laminated glass articles or glass with metal inserts or enclosures, e.g. wires, bubbles, coloured parts
    • C—CHEMISTRY; METALLURGY
    • C03—GLASS; MINERAL OR SLAG WOOL
    • C03B—MANUFACTURE, SHAPING, OR SUPPLEMENTARY PROCESSES
    • C03B2215/00—Press-moulding glass
    • C03B2215/61—Positioning the glass to be pressed with respect to the press dies or press axis
    • 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
    • H01L2224/26—Layer connectors, e.g. plate connectors, solder or adhesive layers; Manufacturing methods related thereto
    • H01L2224/31—Structure, shape, material or disposition of the layer connectors after the connecting process
    • H01L2224/32—Structure, shape, material or disposition of the layer connectors after the connecting process of an individual layer connector
    • H01L2224/321—Disposition
    • H01L2224/32151—Disposition the layer connector connecting between a semiconductor or solid-state body and an item not being a semiconductor or solid-state body, e.g. chip-to-substrate, chip-to-passive
    • H01L2224/32221—Disposition the layer connector connecting between a semiconductor or solid-state body and an item not being a semiconductor or solid-state body, e.g. chip-to-substrate, chip-to-passive the body and the item being stacked
    • H01L2224/32245—Disposition the layer connector connecting between a semiconductor or solid-state body and an item not being a semiconductor or solid-state body, e.g. chip-to-substrate, chip-to-passive the body and the item being stacked the item being metallic
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L2924/00—Indexing scheme for arrangements or methods for connecting or disconnecting semiconductor or solid-state bodies as covered by H01L24/00
    • H01L2924/15—Details of package parts other than the semiconductor or other solid state devices to be connected
    • H01L2924/181—Encapsulation
    • 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
    • H01L33/00—Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
    • H01L33/48—Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by the semiconductor body packages
    • H01L33/52—Encapsulations
    • H01L33/56—Materials, e.g. epoxy or silicone resin

Definitions

  • the present invention relates to a method for manufacturing a light emitting diode unit, and more particularly to a method for manufacturing a light emitting diode unit in which a phosphor layer is sealed with a glass member.
  • White light-emitting diodes (hereinafter also referred to as white LEDs) have excellent features such as low power consumption, small size, light weight, low heat generation, mercury-free, easy adjustment of light quantity, etc., so incandescent bulbs, fluorescent lamps, It is expected as a next-generation energy-saving illumination light source that can replace high-pressure discharge lamps.
  • a method of emitting white light using an LED chip (1) a method of obtaining white light by combining three or more color LED chips (see Patent Document 1), or (2) blue light, blue-violet light, or near ultraviolet light A method of obtaining white light by combining an LED chip that emits light or the like and a phosphor (see Patent Documents 2 and 3) is known. Of these, the method (1) is difficult to balance the light emission intensity of each color LED chip, so the method of obtaining white light by combining the LED chip and the phosphor as in (2) is the focus. Has been.
  • gallium nitride-based substrates that are mainly used as LED chip materials that emit blue light and the like have a high refractive index. Therefore, if the surface of the LED chip is in contact with an air layer or the like, light extraction efficiency is achieved by total reflection. There is a problem that will be extremely lowered.
  • the LED chip Deterioration of the resin material that seals the surface is significant and becomes a problem.
  • the present invention has been made in view of the above technical problems, and an object of the present invention is a light-emitting diode unit that can be manufactured in a short time while suppressing deterioration and breakage of LED chips and phosphors. It is to provide a manufacturing method.
  • the present invention has the following features.
  • An LED chip that emits light of a predetermined wavelength from the surface; A phosphor for converting the wavelength of light emitted from the LED chip; A glass member for sealing the phosphor, and a manufacturing method of a light emitting diode unit comprising: Placing the LED chip on the lower mold; Supplying the phosphor to the surface of the LED chip; On the lower mold on which the LED chip supplied with the phosphor is mounted, a molten glass droplet having a temperature higher than that of the lower mold is dropped and solidified to seal the phosphor with a glass member. And a process for producing the light emitting diode unit.
  • the molten glass droplet dripped on the lower mold is solidified, the molten glass droplet is pressurized with an upper mold facing the lower mold, and the glass member is formed into a predetermined shape, The manufacturing method of the light emitting diode unit of said 1 which does.
  • An LED chip that emits light of a predetermined wavelength from the surface;
  • a glass member for sealing the phosphor, and a manufacturing method of a light emitting diode unit comprising: Temporarily fixing the upper surface of the LED chip with the surface facing downward; Supplying the phosphor to the surface of the LED chip; Dropping a molten glass droplet having a temperature higher than that of the lower mold on the lower mold facing the upper mold; Before the molten glass droplets dropped on the lower mold are solidified, pressurizing the molten glass drops with the upper mold on which the LED chip is temporarily fixed, and sealing the phosphor with a glass member;
  • a method for producing a light-emitting diode unit comprising:
  • the LED chip has an electrode part on the back side facing the surface, 4.
  • Step of electrically connecting the exposed portion of the electrode portion and the lead portion of the package substrate having a lead portion for supplying power to the LED chip through the electrode portion after the molten glass droplet is solidified.
  • the phosphor is supplied by applying a composition in which the phosphor is dispersed and heating to form a glass body containing the phosphor on the surface of the LED chip.
  • the manufacturing method of the light emitting diode unit of any one of 1-5.
  • the phosphor layer is sealed with the glass member by dripping and solidifying the molten glass droplet, it is not necessary to maintain the LED chip or the phosphor layer at a high temperature for a long time, Degradation due to temperature can be suppressed. Moreover, even when it is a case where a glass member is shape
  • the light emitting diode unit manufacturing method of this embodiment includes a step of placing an LED chip on the lower mold (LED chip placement step), and a step of supplying a phosphor layer on the surface of the LED chip (phosphor layer supply). Process) and a molten glass droplet having a temperature higher than that of the lower mold is dropped and solidified on the lower mold on which the LED chip supplied with the phosphor layer is placed, and the phosphor layer is sealed with a glass member. A process (sealing process).
  • FIG. 1 is a cross-sectional view schematically showing an LED chip placed on the lower die in the LED chip placing step
  • FIG. 2 is a state in which the phosphor layer is supplied to the surface of the LED chip in the phosphor layer supplying step.
  • FIG. 3 is a schematic view for explaining a sealing process.
  • 4 and 5 are cross-sectional views schematically showing a light emitting diode unit manufactured by the manufacturing method of the present embodiment.
  • FIG. 1A is a diagram illustrating an example of a state in which the LED chip 10 is placed on the lower mold 60.
  • the LED chip 10 is called a flip chip type having an electrode portion 11 on the back surface side, and emits light of a predetermined wavelength from the front surface 12.
  • a known LED chip such as one using a gallium nitride-based semiconductor (GaN, InGaN, AlInGaN, etc.) may be appropriately selected and used.
  • the emitted light may be blue light, blue-green light, near ultraviolet light, ultraviolet light, or the like.
  • the chip size is not limited, and may be 0.35 mm square (small chip) or 1 mm square (large chip).
  • the chip size is large, the amount of heat generation increases, but the phosphor layer and the like are sealed with a glass member having excellent heat resistance in the manufacturing method of this embodiment, so that even if a large 1 mm square chip is used, it is durable.
  • a light emitting diode unit having excellent properties can be manufactured.
  • a plurality of LED chips 10 are arranged and placed on one lower mold 60, and a light emitting diode unit in which the plurality of LED chips 10 are integrated with a glass member is manufactured. Is also preferable.
  • the light emitting diode unit having a configuration in which a plurality of LED chips 10 are integrated with a glass member is particularly suitable for applications requiring a high luminous flux.
  • the shape of the surface of the lower mold 60 on which the LED chip 10 is placed is not particularly limited, and may be a concave surface or a convex surface in addition to a flat surface. It is also preferable to provide an inclined surface 62 having a predetermined shape and use the surface formed on the glass member by the transfer of the inclined surface 62 as a positioning surface when the light emitting diode unit is fixed to the package substrate. It is also preferable to provide unevenness so that the LED chip 10 can be positioned at a predetermined position. If it is necessary to accurately position and place the LED chip, the LED chip may be temporarily fixed to the surface of the lower mold 60 using solder or the like.
  • the material of the lower mold 60 is preferably a material that has high heat resistance and hardly reacts with molten glass.
  • various heat-resistant alloys such as stainless steel
  • super hard materials mainly composed of tungsten carbide various ceramics (such as silicon carbide, silicon nitride, and aluminum nitride), composite materials containing carbon, and the like can be given.
  • various metals chromium, aluminum, titanium, etc.
  • nitrides chromium nitride, aluminum nitride, titanium nitride, boron nitride, etc.
  • oxides chromium oxide, aluminum oxide
  • FIG. 2A shows a state where the phosphor layer 30 is supplied to the surface 12 of the LED chip 10 of FIG. 1A
  • FIG. 2B shows the surface 12 of the three LED chips 10 of FIG. 1B. It is sectional drawing which shows typically the state to which the fluorescent substance layer 30 was supplied, respectively.
  • the phosphor used for the phosphor layer 30 to be supplied may be appropriately selected and used according to the application and type of the light emitting diode unit to be manufactured.
  • a blue LED chip + yellow is used by using a yellow phosphor that converts the wavelength of blue light into yellow light (excited by blue light and emits yellow light).
  • White light can be obtained by adopting a phosphor structure.
  • a configuration of blue LED chip + yellow phosphor + red phosphor or a configuration of blue LED chip + green phosphor + red phosphor can be used.
  • a configuration of near-ultraviolet LED chip + blue phosphor + yellow phosphor or a near-UV LED chip + blue phosphor + green phosphor + red phosphor With this configuration, white light can be obtained.
  • Suitable phosphors include YAG phosphors, silicate phosphors, nitride phosphors, oxynitride phosphors, sulfide phosphors, thiogallate phosphors, aluminate phosphors, and the like.
  • all the phosphors may be mixed and supplied, or may be supplied in layers for each type of phosphor.
  • loss due to so-called multistage excitation in which light emitted from the first phosphor excites another second phosphor, tends to be a problem. From the viewpoint of effectively reducing the loss due to such multi-stage excitation, it is preferable to supply the phosphors by dividing them into layers.
  • the phosphor layer 30 may be supplied to the surface 12 of the LED chip 10 by applying powder, or after being applied in a state of being dispersed in a liquid or gel binder, it is vaporized or thermally decomposed.
  • the binder may be removed.
  • a binder it is preferable to use a binder that can be removed at a low temperature from the viewpoint of suppressing deterioration of the phosphor layer 30 and the like.
  • organic solvents such as ethanol and acetone, and synthetic resins are suitable.
  • a glass body that is a phosphor layer 30 containing a phosphor on the surface 12 of the LED chip 10 by applying and heating a composition in which the phosphor is dispersed.
  • the composition may be applied by a known method such as spin coating, dip coating, or spray coating.
  • a bar coater according to the shape of the LED chip 10.
  • a dry oven or the like may be used to heat the applied composition.
  • the film thickness of the glass body formed after heating is preferably 10 ⁇ m to 80 ⁇ m.
  • the composition to be applied may be a gel (sol-gel solution) in which a transparent ceramic layer (glass body) is formed by further heating the gel after heating, and by volatilizing the solvent component.
  • the glass body may be formed directly without gelation.
  • sol-gel solution a solution containing a phosphor, a layered silicate mineral, and inorganic fine particles in a solution obtained by mixing an organometallic compound as a glass body component in an organic solvent can be used.
  • the organometallic compound serves as a binder for sealing the phosphor, the layered silicate mineral, and the inorganic fine particles.
  • organometallic compound used in the present invention include metal alcosides, metal acetylacetonates, metal carboxylates and the like, but metal alkoxides that are easily gelled by hydrolysis and polymerization reaction are preferable.
  • the metal alkoxide may be a single molecule such as tetraethoxysilane, or may be a polysiloxane in which an organic siloxane compound is linked in a chain or a ring, but a polysiloxane that increases the viscosity of the mixed solution is preferable.
  • a translucent glass body can be formed, but it is preferable to contain a silicon
  • the content of the organometallic compound in the glass body is less than 2% by mass, the organometallic compound as the binder is too small, and the strength of the glass body after heating and firing is lowered.
  • the content of the organometallic compound exceeds 50% by mass, the content of the layered silicate mineral is relatively decreased, so that the viscosity of the mixed solution before heating is decreased and the phosphor is easily precipitated. .
  • the content of the inorganic fine particles is relatively lowered, the strength of the glass body is also lowered. Therefore, the content of the organometallic compound in the glass body is preferably 2% by mass or more and 50 or less, and more preferably 2.5% by mass or more and 30% by mass or less.
  • the phosphor is excited by the wavelength (excitation wavelength) of light emitted from the LED chip 10 and emits fluorescence having a wavelength different from the excitation wavelength.
  • a YAG (yttrium, aluminum, garnet) phosphor that converts blue light (wavelength 420 nm to 485 nm) emitted from the blue LED element into yellow light (wavelength 550 nm to 650 nm) is used.
  • Such phosphors use oxides of Y, Gd, Ce, Sm, Al, La, and Ga, or compounds that easily become oxides at high temperatures, and are mixed well in a stoichiometric ratio.
  • a mixed raw material is obtained.
  • a coprecipitated oxide obtained by calcining a solution obtained by coprecipitation of a solution obtained by dissolving a rare earth element of Y, Gd, Ce, or Sm in an acid with a stoichiometric ratio with oxalic acid, and aluminum oxide or gallium oxide.
  • an appropriate amount of fluoride such as ammonium fluoride is mixed with the obtained mixed raw material as a flux and pressed to obtain a molded body.
  • the obtained molded body is packed in a crucible and fired in air at a temperature range of 1350 to 1450 ° C. for 2 to 5 hours to obtain a sintered body having the light emission characteristics of a phosphor.
  • the YAG phosphor is used.
  • the type of the phosphor is not limited to this.
  • other phosphors such as non-garnet phosphors containing no Ce are used. You can also.
  • the larger the particle size of the phosphor the higher the light emission efficiency (wavelength conversion efficiency), but the gap generated at the interface with the organometallic compound becomes larger, and the film strength of the formed glass body decreases. Accordingly, in consideration of the size of the gap generated at the interface between the light emission efficiency and the organometallic compound, it is preferable to use one having an average particle diameter of 1 ⁇ m or more and 50 ⁇ m or less.
  • the average particle diameter of the phosphor can be measured, for example, by a Coulter counter method.
  • the layered silicate mineral is preferably a swellable clay mineral having a structure such as a mica structure, a kaolinite structure, or a smectite structure, and particularly preferably a smectite structure rich in swellability. This is because, as will be described later, by adding water to the mixed liquid, it takes a card house structure in which water enters and swells between the layers of the smectite structure, so the viscosity of the mixed liquid is greatly increased. It is.
  • the content of the layered silicate mineral in the glass body is less than 0.5% by mass, the effect of increasing the viscosity of the mixed solution cannot be obtained sufficiently.
  • the content of the layered silicate mineral exceeds 20% by mass, the strength of the glass body after heating is lowered. Therefore, the content of the layered silicate mineral is preferably 0.5% by mass or more and 20% by mass or less, and more preferably 0.5% by mass or more and 10% by mass or less.
  • a layered silicate mineral whose surface is modified (surface treatment) with an ammonium salt or the like can be used as appropriate.
  • Inorganic fine particles include a filling effect that fills gaps formed at the interface between the organometallic compound, the phosphor and the layered silicate mineral, a thickening effect that increases the viscosity of the mixed liquid before heating, and a glass body film after heating. It has a film strengthening effect that improves strength.
  • Examples of the inorganic fine particles used in the present invention include oxide fine particles such as silicon oxide, titanium oxide and zinc oxide, and fluoride fine particles such as magnesium fluoride.
  • silicon oxide fine particles such as silicon oxide, titanium oxide and zinc oxide
  • fluoride fine particles such as magnesium fluoride.
  • silicon oxide fine particles such as silicon oxide, titanium oxide and zinc oxide
  • fluoride fine particles such as magnesium fluoride.
  • silicon oxide fine particles such as silicon-containing organic compound such as polysiloxane
  • the content of the inorganic fine particles in the glass body is less than 0.5% by mass, the above-described effects cannot be sufficiently obtained.
  • the content of the inorganic fine particles exceeds 50% by mass, the strength of the glass body after heating is lowered. Therefore, the content of the inorganic fine particles in the glass body is preferably 0.5% by mass or more and 50% by mass or less, and more preferably 1% by mass or more and 40% by mass or less.
  • the average particle diameter of the inorganic fine particles is preferably 0.001 ⁇ m or more and 50 ⁇ m or less in consideration of the above-described effects.
  • the average particle diameter of the inorganic fine particles can be measured, for example, by a Coulter counter method. In consideration of compatibility with an organic metal compound or an organic solvent, a material obtained by treating the surface of inorganic fine particles with a silane coupling agent or a titanium coupling agent can be used as appropriate.
  • the precursor solution is a mixture of an organometallic compound in an organic solvent, and a translucent glass body can be obtained by heating the precursor solution.
  • a glass body is formed by heating a mixed solution in which the precursor solution is mixed with a phosphor, a layered silicate mineral, and inorganic fine particles.
  • water enters between the layers of the layered silicate mineral and the viscosity of the mixed solution increases, so that the phosphor can be prevented from settling.
  • the organic solvent alcohols such as methanol, ethanol, propanol and butanol having excellent compatibility with added water are preferable. Further, when the amount of the organic metal compound mixed with the organic solvent is less than 5% by mass, it becomes difficult to increase the viscosity of the mixed solution, and when the amount of the organic metal compound exceeds 50% by mass, the polymerization reaction is faster than necessary. Proceed. Therefore, the mixing amount of the organometallic compound with respect to the organic solvent is preferably 5% by mass or more and 50% by mass or less, and more preferably 8% by mass or more and 40% by mass or less.
  • the layered silicate mineral when using a surface-treated lipophilic layered silicate mineral, the layered silicate mineral is first added to a solution (precursor solution) in which an organometallic compound is mixed in an organic solvent. Premixing is performed, and then phosphor, inorganic fine particles, and water are mixed.
  • a hydrophilic layered silicate mineral that has not been surface-treated is used, first the layered silicate mineral and water are premixed, and then the phosphor, inorganic fine particles, and precursor solution are mixed. Thereby, a layered silicate mineral can be mixed uniformly and the thickening effect can be heightened more.
  • the preferred viscosity of the mixed solution is 0.025 to 0.8 Pa ⁇ s, and the most preferred viscosity is 0.03 to 0.5 Pa ⁇ s.
  • the ratio of water to the total amount of the solvent obtained by adding water to the organic solvent is less than 5% by mass, the above thickening effect cannot be sufficiently obtained, and when the ratio of water exceeds 60% by mass, the thickening effect is achieved.
  • the effect of reducing the viscosity due to excessive mixing of water is greater than that. Therefore, the ratio of water is preferably 5% by mass or more and 60% by mass or less, and more preferably 7% by mass or more and 55% by mass or less with respect to the total amount of solvent.
  • the most preferable composition of the mixed solution is that using polysiloxane as the organometallic compound.
  • composition range of each of the above components contained in the mixed solution is that the polysiloxane dispersion is 4 to 30% by mass, and the layered silica is used.
  • the acid salt mineral is 1 to 10% by mass
  • the inorganic fine particles are 1 to 40% by mass
  • the water is 10 to 50% by mass.
  • a predetermined amount of the mixed liquid obtained as described above is applied onto the surface 12 of the LED chip 10, and heated and baked to form a glass body having a predetermined film thickness.
  • the method for applying the mixed solution is not particularly limited, and various conventionally known methods such as spin coating, dip coating, spray coating, and bar coating can be used.
  • the heating temperature is less than 50 ° C., the polymerization reaction of the organometallic compound does not proceed.
  • the heating temperature exceeds 1000 ° C. the layered silicate mineral is thermally decomposed and the layered structure is destroyed. Therefore, the heating temperature of the mixed solution needs to be 50 ° C. or higher and 1000 ° C. or lower, and preferably 100 ° C. to 600 ° C. However, it is necessary to set the temperature at which the LED chip 10 does not deteriorate.
  • the thickness of the formed glass body is less than 5 ⁇ m, the wavelength conversion efficiency is lowered and sufficient fluorescence cannot be obtained, and when the thickness of the glass body exceeds 500 ⁇ m, the film strength is reduced and cracks and the like are generated. It tends to occur. Therefore, the thickness of the glass body is preferably 5 ⁇ m or more and 500 ⁇ m or less.
  • the particle size of the phosphor and inorganic fine particles contained in the glass body is larger than the thickness of the glass body to be formed, a part of the phosphor or inorganic fine particles protrudes from the surface of the glass body and the surface is smooth. Sex is lost. Therefore, phosphors and inorganic fine particles having a maximum particle size smaller than the thickness of the glass body are used.
  • the phosphor layer 30 is formed of a translucent glass body, heat resistance and light resistance can be improved as compared with the case where the phosphor layer 30 is formed of a resin material.
  • the phosphor is less likely to settle when the glass body is formed and the phosphor is uniformly dispersed in the glass body, the occurrence of color unevenness can be effectively reduced.
  • the film strength of the glass body is improved by adding inorganic fine particles.
  • examples of the latter in which a glass body is directly formed without being gelled by volatilizing a solvent component
  • examples of the latter include, for example, a composition containing an inorganic polymer and an organic solvent.
  • Polysilazane can be used as the inorganic polymer.
  • the polysilazane used in the present invention is represented by the following general formula (1).
  • R 1 , R 2 and R 3 each independently represent a hydrogen atom or an alkyl group, an aryl group, a vinyl group or a cycloalkyl group, and at least one of R 1 , R 2 and R 3 Are hydrogen atoms, preferably all are hydrogen atoms, and n represents an integer of 1 to 60.
  • the molecular shape of polysilazane may be any shape, for example, linear or cyclic.
  • the polysilazane represented by the above formula (1) and a reaction accelerator as required are dissolved in an appropriate solvent and then cured by heating, excimer light treatment, UV light treatment, and excellent heat resistance and light resistance.
  • a ceramic film can be made.
  • the effect of preventing penetration of moisture can be further improved by heat curing after irradiation with UVU radiation (eg, excimer light) containing a wavelength component in the range of 170 to 230 nm.
  • reaction accelerator it is preferable to use an acid, a base or the like, but it is not necessary to use it.
  • reaction accelerators include triethylamine, diethylamine, N, N-diethylethanolamine, N, N-dimethylethanolamine, triethanolamine, triethylamine, hydrochloric acid, oxalic acid, fumaric acid, sulfonic acid, acetic acid, nickel, iron, palladium , Metal carboxylates including iridium, platinum, titanium, and aluminum, but are not limited thereto.
  • a metal carboxylate is particularly preferable, and the addition amount is preferably 0.01 to 5 mol% based on polysilazane.
  • aliphatic hydrocarbons aliphatic hydrocarbons, aromatic hydrocarbons, halogen hydrocarbons, ethers, and esters
  • Preferred are methyl ethyl ketone, tetrahydrofuran, benzene, toluene, xylene, dimethyl fluoride, chloroform, carbon tetrachloride, ethyl ether, isopropyl ether, dibutyl ether, and ethyl butyl ether.
  • the polysilazane concentration is high.
  • the polysilazane is preferably dissolved in the solvent at 5 to 50% by mass or less.
  • the heating temperature at the time of firing is preferably 100 ° C. to 350 ° C. from the viewpoint of suppressing deterioration of the material used for the substrate and the metal of the wiring. More preferably, the temperature is 150 ° C to 300 ° C.
  • the composition contains inorganic fine particles. Since the viscosity of the composition is increased by containing inorganic fine particles, the precipitation rate of the phosphor when the phosphor is dispersed in the composition is reduced, and it is easy to uniformly disperse the phosphor in the composition. Become.
  • inorganic fine particles of various oxides such as silica and inorganic fine particles of magnesium fluoride are suitable. From the viewpoint of stability with a glass body formed from polysilazane, it is preferable to contain inorganic fine particles of silica.
  • the inorganic fine particles preferably have a 50% particle diameter (median diameter) of 1 nm to 500 nm.
  • the shape of the inorganic fine particles is not particularly limited, but preferably spherical fine particles are used.
  • the particle size distribution is not particularly limited, but from the viewpoint of uniformly dispersing the phosphor, those having a relatively narrow distribution are preferably used rather than those having a wide distribution.
  • the shape and particle size distribution of the inorganic fine particles can be confirmed using SEM and TEM.
  • the content of the inorganic fine particles is preferably 0.1% by mass to 25% by mass with respect to the entire composition including the phosphor. In order to further uniformly disperse the phosphors of the inorganic fine particles, it is also preferable to apply ultrasonic waves to the composition in which the phosphors are mixed and disperse them.
  • the phosphor layer 30 may be supplied by placing the glass plate 31 having the phosphor layer 30 on the surface 12 of the LED chip 10.
  • FIG.2 (c) is a figure which shows the state which mounted the glass plate 31 which has the fluorescent substance layer 30 so that it might straddle the surface 12 of the three LED chips 10 of FIG.1 (b).
  • the phosphor layer 30 can be supplied more easily by placing one glass plate 31 across the surface of the arrayed LED chips 10. Can do.
  • the glass plate 31 having the phosphor layer 30 As the glass plate 31 having the phosphor layer 30, (A) a kneaded glass in which the phosphor is dispersed inside, or (B) a glass plate in which the phosphor layer 30 is coated on at least one surface is suitably used. Can be used.
  • the phosphor layer 30 may be applied and formed on the surface of the glass plate by the same method as that for applying the phosphor layer 30 to the surface 12 of the LED chip 10 described above.
  • the kneaded glass in which the phosphor is dispersed is preferably produced by pressure-molding a mixed material in which glass powder and phosphor powder are mixed.
  • a mixed material in which glass powder and phosphor powder are mixed.
  • a resin binder may be added, but in that case, a step of removing the resin binder after pressure molding is required. Therefore, it is preferable to perform pressure molding by mixing glass powder and phosphor powder without using a resin binder.
  • the glass powder to be mixed preferably has a maximum particle size of 160 ⁇ m or more and a median diameter d50 of 5 ⁇ m or more.
  • kneaded glass in which the phosphor is uniformly dispersed can be obtained without using a resin binder.
  • bubbles are more easily removed when the maximum particle size is 160 ⁇ m or more. If the maximum particle size is less than 160 ⁇ m, bubbles are difficult to escape.
  • the median diameter d50 is less than 5 ⁇ m, when the powder is put into the mold, dust rises and handling becomes difficult. In addition, the work environment may be harmed.
  • the upper limit of the maximum particle diameter should just be a range from which favorable scattered light is obtained, and can be suitably determined according to the combination of a LED chip and fluorescent substance.
  • the median diameter d50 is a particle diameter (cumulative average diameter) at a point where the cumulative curve becomes 50% when the total curve of one group of particle bodies is 100%, and the maximum particle The diameter is the particle diameter at which the cumulative curve becomes 100%.
  • the median diameter d50 and the maximum particle diameter can be measured using a general laser diffraction / scattering particle size measuring device. Specifically, HELOS (manufactured by JEOL), Microtrac HRA (manufactured by Nikkiso) And SALD series (manufactured by Shimadzu Corporation). Particularly preferred is the SALD series (manufactured by Shimadzu Corporation).
  • the particle diameter of the glass powder As described above, by setting the particle diameter of the glass powder to a predetermined size, it becomes possible to obtain a kneaded glass in which the phosphor is uniformly dispersed. Thereby, primary light emitted from the LED chip can be satisfactorily scattered, and generation of bubbles that emulsify the glass in white can be suppressed, and the primary light and secondary light emitted from the phosphor can be mixed well and mixed.
  • a kneaded glass capable of emitting light with such mixed color light (third light) can be manufactured.
  • the glass powder does not precipitate crystals under the heating environment during pressure molding, or does not precipitate in a large amount even if slightly precipitated. Therefore, a glass having a crystal precipitation temperature higher than the heating temperature is preferable.
  • the heating temperature is set to 150 ° C. to 200 ° C. higher than the glass yield point
  • the crystal precipitation temperature is preferably 200 ° C. or higher than the glass yield point.
  • P 2 O 5 —BaO glass, P 2 O 5 —ZnO glass, P 2 O 5 —Nb 2 O 5 glass, P 2 O 5 —B 2 O 3 glass, SiO 2 glass B 2 O 3 —ZnO—La 2 O 3 glass, SiO 2 —B 2 O 3 —ZnO glass, and the like can be preferably used.
  • the phosphor content in the kneaded glass is preferably 0.02 to 12%, more preferably 0.05 to 5% in volume ratio. If the phosphor content is less than 0.02%, the amount of fluorescent light is too small, and if it exceeds 12%, the phosphor itself shields the light. Thus, if the phosphor content is 0.02 to 12%, the amount of light to be converted is not too low, and the amount of light that does not hinder the light transmission can be obtained. A kneaded glass capable of emitting mixed color light can be manufactured. In addition, when the phosphor content is 0.05 to 5%, the balance between the converted light and the light transmission is further improved, and a kneaded glass capable of emitting a better color mixture light is manufactured. Can do.
  • the order of the LED chip mounting process and the phosphor layer supplying process is not limited thereto.
  • the LED chip mounting step may be performed after the phosphor layer supplying step.
  • FIGS. 3A to 3C are schematic views sequentially showing the states in the sealing process.
  • the dropping of the molten glass droplet 44 is performed by heating a pipe-shaped dropping nozzle 41 connected to a melting tank (not shown) containing molten glass to a predetermined temperature by a heater 42.
  • a pipe-shaped dropping nozzle 41 connected to a melting tank (not shown) containing molten glass to a predetermined temperature by a heater 42.
  • the molten glass 43 is supplied to the tip of the dripping nozzle 41 by its own weight and accumulates in a droplet shape by the surface tension (FIG. 3A).
  • the molten glass 43 collected at the tip of the dropping nozzle 41 reaches a certain mass, it is separated from the dropping nozzle 41 by gravity and becomes a molten glass droplet 44 that drops downward (FIG. 3B).
  • the mass of the molten glass droplet 44 dropped from the dropping nozzle 41 can be adjusted by the outer diameter of the tip of the dropping nozzle 41 and the like, and depending on the type of glass, the molten glass droplet 44 of about 0.1 to 2 g is dropped. Can be made.
  • a method of pressurizing and extruding the molten glass 43 or a method of separating by applying an external force such as airflow or vibration may be used. Compared with the method of pouring glass directly, the glass mass can be reduced, the mass can be easily adjusted, and the glass temperature to be sealed at the time of dropping is lowered, so that damage to the LED chip due to glass heat can be alleviated.
  • the molten glass droplet 44 dropped from the dropping nozzle 41 is once collided with a member provided with a through-hole, and a part of the collided molten glass droplet 44 is passed through the through-pore, thereby miniaturizing.
  • the molten glass droplet 44 may be dropped.
  • a diode unit can be manufactured.
  • the lower mold 60 is preferably heated to a predetermined temperature in advance. Thereby, the shape of the surface of the glass member formed by the transfer of the lower mold 60 is stabilized.
  • the predetermined temperature is lower than the temperature of the molten glass droplet 44 to be dropped and is a temperature at which the dropped molten glass droplet 44 is cooled and solidified, and may be appropriately selected according to the type of glass to be used. If the temperature of the lower mold 60 is too low, the shape of the surface of the glass member formed by transfer becomes unstable, and wrinkles are likely to occur. On the other hand, if the temperature is set higher than necessary, the life of the lower mold 60 tends to be shortened due to fusion with the glass, surface oxidation, or the like.
  • the temperature of the lower mold 60 is preferably set in the range of Tg-100 ° C. to Tg + 100 ° C., where Tg is the glass transition temperature of the glass used, and the range of Tg ⁇ 100 ° C. to Tg + 50 ° C. It is more preferable to set to.
  • a known heating means can be appropriately selected and used. For example, an infrared heating device, a high frequency induction heating device, a cartridge heater used by being embedded in the lower die 60, a sheet heater used by contacting the outside of the lower die 60, and the like are suitable.
  • the molten glass droplet 44 dropped on the lower mold 60 is rapidly cooled and solidified by heat conduction to the lower mold 60 and the like, and the phosphor layer 30 is sealed with the glass member 40 to form the light emitting diode unit 50. (FIG. 3C).
  • the solidification is usually completed several seconds to several tens of seconds after the molten glass droplet 44 is dropped.
  • the phosphor layer 30 can be sealed with the glass member 40 without applying a high pressure simply by dropping the molten glass droplet 44, damage to the member due to pressure can be suppressed.
  • glass there is no particular limitation on the type of glass that can be used, and a known glass can be selected and used depending on the application. Examples thereof include optical glasses such as borosilicate glass, silicate glass, phosphate glass, and lanthanum glass. From the viewpoint of suppressing light reflection on the surface 12 of the LED chip 10 and further improving the light extraction efficiency, it is preferable to use glass having a small difference in refractive index from the LED chip 10.
  • (Modification of sealing process) 4A to 4C are schematic views showing a modification of the sealing process in the first embodiment.
  • the sealing step shown in FIG. 4 is different from the sealing step shown in FIG. 3 in that the lower mold 60 is inclined by an angle ⁇ , and the molten glass droplet 44 having a temperature higher than that of the inclined lower mold 60 is It is dropped on the lower mold 60.
  • Others are the same as those described in FIG.
  • the tilt angle ⁇ of the lower mold 60 when the molten glass droplet 44 is dropped is preferably 0.1 ° to 10 ° with respect to the horizontal. In this manner, by configuring the molten glass droplet 44 to be dropped while the lower die 60 is inclined, the occurrence of air pockets in the lower die 60 at the time of dropping can be suppressed.
  • the inclination angle ⁇ is greater than 10 °, the dropped molten glass may be inclined or protruded, which may adversely affect the surface accuracy of the glass member 40 after solidification.
  • the inclination angle ⁇ of the lower mold 60 when the molten glass droplet 44 is dropped is more preferably 3 ° to 7 °. If it is this angle range, the inclination of the dripped molten glass does not generate
  • FIG. 5 is a cross-sectional view of the light emitting diode unit 50 manufactured by the method of the present embodiment.
  • 5A to 5C show a light emitting diode unit 50 manufactured by dropping a molten glass droplet 44 on the LED chip 10 or the like shown in FIGS. 2A to 2C, respectively.
  • the phosphor layer 30 is sealed with the glass member 40 in the light emitting diode unit 50 manufactured by the method of the present embodiment, deterioration of the sealing material due to heat generation of the LED chip 10 is suppressed. In addition, high extraction efficiency can be ensured. Further, deterioration of the phosphor layer 30 due to the influence of the external environment is suppressed, and the durability is excellent.
  • the surface 45 of the glass member 40 has a gentle convex shape, but the degree of convexity of the surface 45 can be adjusted by changing the temperature and size of the molten glass droplet 44 to be dropped. For example, when the temperature of the molten glass droplet 44 to be dropped is increased, the viscosity is lowered, and the surface 45 of the glass member 40 has a flatter shape (the curvature is reduced). On the contrary, when the temperature of the molten glass droplet 44 is lowered, the viscosity increases, and the surface 45 of the glass member 40 has a shape with a larger convexity (the curvature increases). Thus, the surface 45 of the glass member 40 can be made into an appropriate shape according to the required condensing characteristic by changing the conditions for dropping the molten glass droplet 44.
  • the lower mold 60 of the electrode unit 11 is dropped by dropping the molten glass droplet 44 in a state where the electrode unit 11 on the back surface side of the LED chip 10 is in contact with the lower mold 60.
  • the contact surface can be exposed without being sealed by the glass member 40 (FIG. 4A).
  • the electrical connection for supplying electric power to the LED chip 10 can be easily performed by sealing with the glass member 40 so that at least a part of the electrode portion 11 is exposed.
  • FIG. 6 is a cross-sectional view of the light emitting diode unit 50 connected to the package substrate 20.
  • FIGS. 6A to 6C show cases where the package substrate 20 is connected to the light emitting diode unit 50 shown in FIGS. 5A to 5C.
  • the package substrate 20 has a lead portion 21 for supplying power to the LED chip 10 via the electrode portion 11.
  • the material of the package substrate 20 is preferably a highly insulating ceramic material such as aluminum nitride or aluminum oxide. Further, a heat resistant resin or a metal material may be used. In the case of a conductive material, an insulating film is preferably provided on the surface.
  • a normal flip chip bonding method may be used for the connection between the electrode portion 11 of the LED chip 10 and the lead portion 21 of the package substrate 20.
  • bumps (protrusions) made of a conductive material are provided on the lead portion 21, the package substrate 20 is fixed on a high-temperature heater, and the load is adjusted while adjusting the position of the LED chip 10 and the package substrate 20 by image processing.
  • the method of connecting by adding.
  • the slope 46 formed on the glass member is used as a positioning surface, thereby eliminating the need for image processing or the like for position adjustment. You can also.
  • the manufacturing method of the light emitting diode unit of this embodiment is a lower mold in which the LED chip supplied with the phosphor layer is placed after the LED chip placing step and the phosphor layer supplying step described in the first embodiment.
  • a molten glass droplet having a temperature higher than that of the lower mold is dropped on the upper mold, and the molten glass droplet is pressed with the upper mold facing the lower mold before the molten glass drop is solidified, so that the glass member has a predetermined shape. It has the process (sealing process) which shape
  • FIGS. 7A to 7D are schematic views sequentially showing the sealing process in the second embodiment.
  • a molten glass droplet 44 having a temperature higher than that of the lower die 60 is dropped on the lower die 60 on which the LED chip 10 supplied with the phosphor layer 30 is placed.
  • the molten glass droplet 44 is dropped by heating the dropping nozzle 41 to a predetermined temperature by the heater 42.
  • the details of the dropping method of the molten glass droplet 44 are the same as in the case of the first embodiment.
  • the sealing step in the second embodiment after dropping the molten glass droplet 44, the lower mold 60 is moved to a position facing the upper mold 70, and the molten glass droplet 44 is pressurized before being cooled and solidified, The glass member 40 is formed into a predetermined shape (FIG. 7C).
  • the molten glass droplet 44 is rapidly cooled by heat conduction to the lower mold 60 and the upper mold 70 and solidifies in a short time to become the glass member 40.
  • the upper mold 70 After releasing the pressure, the upper mold 70 is moved upward, and the obtained light emitting diode unit 50 is recovered (FIG. 7D).
  • the pressure load is much higher than when the glass sheet is heated and pressurized together with the members such as the LED chip 10. It can be kept small, and can be sufficiently deformed in a very short pressurization time. Therefore, the light emitting diode unit 50 can be manufactured in a short time while sufficiently suppressing deterioration due to temperature and damage due to pressure of each member.
  • the preferred material of the upper mold 70 is the same as that of the lower mold 60 described above. Further, like the lower mold 60, the upper mold 70 is preferably preheated to a predetermined temperature. The heating temperature of the lower mold 60 and the upper mold 70 may be the same or different.
  • the load applied to deform the molten glass droplet 44 and the pressurizing time may be appropriately set according to the size of the molten glass droplet 44, etc.
  • a load in the range of several tens to several hundreds N is from several seconds to In many cases, it is sufficient to apply pressure for several tens of seconds. Further, the applied load may be changed with time.
  • the means for applying the load is not particularly limited, and known driving means such as an air cylinder, a hydraulic cylinder, a servo motor, etc. may be appropriately selected and used.
  • FIG. 8 is a cross-sectional view of the light emitting diode unit 50 manufactured by the method of the present embodiment.
  • FIG. 8A shows a light emitting diode unit 50 having one LED chip 10.
  • 8B and 8C show a light emitting diode unit 50 in which three LED chips 10 are integrated by a glass member 40.
  • FIG. 8A shows a light emitting diode unit 50 having one LED chip 10.
  • 8B and 8C show a light emitting diode unit 50 in which three LED chips 10 are integrated by a glass member 40.
  • the shape of the surface 45 of the glass member 40 is formed by forming the molten glass droplet 44 dropped on the lower mold 60 with the upper mold 70, so that a desired shape corresponding to the application is formed. It can be formed easily.
  • the surface 45 of the glass member 40 can have a convex shape with a very large curvature, or like the light emitting diode unit 50 of FIG. 8C.
  • a plurality of convex portions corresponding to the plurality of LED chips 10 may be arranged.
  • a step of electrically connecting the electrode portion 11 of the LED chip 10 and the lead portion 21 of the package substrate 20 is provided, and the package It is also preferable to manufacture the light emitting diode unit 50 integrated with the substrate 20.
  • FIGS. 9A to 9D are schematic views showing a modification of the sealing process in the second embodiment. 9 differs from the sealing process shown in FIG. 7 in FIGS. 9A and 9B in the modification of the sealing process according to the first embodiment shown in FIG. Similarly to the example, the lower mold 60 is inclined by the angle ⁇ , and a molten glass droplet 44 having a temperature higher than that of the inclined lower mold 60 is dropped on the lower mold 60. This is the same as that described in.
  • a molten glass droplet 44 having a temperature higher than that of the package substrate 20 is dropped on the lower mold 60 inclined by the angle ⁇ .
  • the lower mold 60 on which the molten glass droplet 44 is dropped is returned to a horizontal position, the lower mold 60 is moved to a position facing the upper mold 70, and the molten glass droplet 44 is added by the upper mold 70 before being cooled and solidified.
  • the glass member 40 is molded into a predetermined shape (FIG. 9C).
  • the upper mold 70 is moved upward, and the obtained light emitting diode unit 50 is recovered (FIG. 9D).
  • the inclination angle ⁇ of the lower mold 60 when the molten glass droplet 44 is dropped is preferably 0.1 ° to 10 ° with respect to the horizontal.
  • the molten glass droplet 44 is dropped, the lower mold 60 is returned to the horizontal, and the molten glass droplet 44 is pressurized with the upper mold 70 before being cooled and solidified.
  • type 60 at the time of dripping can be suppressed.
  • the dropped molten glass may be inclined or protruded, which may adversely affect the surface shape accuracy of the glass member transferred by the molding surface 74 of the upper mold 70.
  • the inclination angle ⁇ of the lower mold 60 when the molten glass droplet is dropped is more preferably 3 ° to 7 °. With this angle range, there is no tilt of the dropped molten glass, no air pool in the lower mold 60 is dropped, and the surface shape accuracy of the glass member transferred by the molding surface 74 is more preferable. State.
  • the manufacturing method of the light emitting diode unit according to the present embodiment includes a step of temporarily fixing the surface of the LED chip downward (LED chip mounting step) and a step of supplying a phosphor layer to the surface of the LED chip ( A phosphor layer supplying step), and a molten glass droplet having a temperature higher than that of the lower die is dropped on the lower die, and the LED chip is temporarily fixed before the molten glass droplet dropped on the lower die is solidified. And a step of sealing the phosphor with a glass member by pressurizing the molten glass droplet with the upper mold (sealing step).
  • the surface of the LED chip 10 is temporarily fixed to the upper mold 70 with the surface facing downward. Solder or the like may be used for temporary fixing. Other details are the same as those in the first embodiment.
  • the phosphor layer supplying step is the same as in the first embodiment.
  • FIGS. 10A to 10D are schematic views sequentially showing the sealing process in the third embodiment.
  • a molten glass droplet 44 having a temperature higher than that of the lower mold 60 is dropped on the molding surface 64 of the lower mold 60 having the molding surface 64 of a predetermined shape (FIGS. 10A and 10B).
  • the molten glass droplet 44 is dropped by heating the dropping nozzle 41 to a predetermined temperature by the heater 42.
  • the details of the dropping method of the molten glass droplet 44 are the same as in the case of the first embodiment.
  • the molten glass droplet 44 is pressurized with the upper mold 70 to which the LED chip 10 supplied with the phosphor layer 30 is temporarily fixed. (FIG. 10 (c)).
  • the molten glass droplet 44 is rapidly cooled by heat conduction to the lower mold 60 and the upper mold 70 and solidifies in a short time to become the glass member 40.
  • the upper mold 70 is moved upward, the temporary fixing is removed, and the light emitting diode unit 50 is recovered (FIG. 10D).
  • the timing for pressurizing the molten glass droplet 44 with the upper die 70 on which the LED chip 10 is placed is preferably slower from the viewpoint of suppressing deterioration of the phosphor layer 30 and the like due to heat, but if too late, the phosphor layer The pressure required for sealing 30 etc. will become high. From such a viewpoint, it is preferable to pressurize several seconds to several tens of seconds after dropping the molten glass droplet 44 on the lower mold 60. What is necessary is just to set suitably the load and pressurization time to apply similarly to 2nd Embodiment. Moreover, it is preferable that the lower mold
  • the glass member 40 can be formed in a desired shape without applying high pressure.
  • the LED chip 10 and the phosphor layer 30 are sealed in the molten glass droplet 44 at a predetermined timing after the dropped molten glass droplet 44 is cooled to some extent. The influence of heat can be minimized. Accordingly, the light emitting diode unit 50 can be manufactured in a short time while sufficiently suppressing deterioration due to temperature and damage due to pressure of each member.

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Abstract

La présente invention concerne un procédé de fabrication d'unité de diodes électroluminescentes, comprenant les étapes suivantes: une étape lors de laquelle une puce LED est placée sur une matrice de moulage inférieure ; une étape lors de laquelle un matériau de phosphore est déposé à la surface de la puce LED ; et une étape lors de laquelle le matériau de phosphore est encapsulé au moyen d'un élément de verre par la chute d'une gouttelette de verre fondu à une température supérieure à celle de la matrice de moulage inférieure et la solidification de la gouttelette sur la matrice de moulage inférieure, sur laquelle est placée la puce LED recouverte du matériau de phosphore qui y a été fournie. Ainsi, l'unité de diodes électroluminescentes peut être fabriquée dans un court laps de temps, tout en supprimant la détérioration et la rupture de la puce LED, de la couche de matériau de phosphore et analogues.
PCT/JP2010/070786 2009-11-30 2010-11-22 Procédé de fabrication d'unité de diodes électroluminescentes WO2011065322A1 (fr)

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