WO2012090867A1

WO2012090867A1 - Method for manufacturing light emitting device

Info

Publication number: WO2012090867A1
Application number: PCT/JP2011/079844
Authority: WO
Inventors: 清司湯浅; 卓史波多野; 鈴木　洋介; 貴志鷲巣; 禄人田口
Original assignee: コニカミノルタオプト株式会社
Priority date: 2010-12-28
Filing date: 2011-12-22
Publication date: 2012-07-05
Also published as: JP2014135503A; JP5494830B2; JPWO2012090867A1

Abstract

This method for manufacturing a light emitting device comprises: a first mask disposition step for disposing a first mask on an LED element so as to cover part of that LED element; a phosphor mixture liquid application step for applying a phosphor mixture liquid in which phosphors are dispersed in a solvent to the LED element, part of which is covered by the first mask; a first mask removal step for removing the first mask from the LED element; a separation step for separating phosphor containing material that contains phosphors from the first mask; a fixing solution application step for applying a fixing solution that fixes the phosphors in the phosphor mixture liquid onto the LED element to which the phosphor mixture liquid has been applied; and a drying step for forming a wavelength conversion part by drying the fixing solution that has been applied onto the LED element.

Description

Method for manufacturing light emitting device

The present invention relates to a method for manufacturing a light emitting device.

2. Description of the Related Art Conventionally, in applications such as lighting, light emitting devices that obtain white light by emitting light from a phosphor using light from a light emitting element such as an LED element as excitation light have been developed.
As such a light emitting device, for example, a phosphor that emits yellow light by blue light emitted from the light emitting element is used, and a light emitting device that produces white light by mixing each light, or emitted from the light emitting element. There is known a light-emitting device that produces white light by using a phosphor that emits blue, green, and red light by ultraviolet light and mixing three colors of light emitted from the phosphor.

As a configuration of such a light emitting device, a light emitting element sealed with a phosphor layer has been developed. The phosphor layer is generally formed by applying and drying a solution in which the phosphor is dispersed, and the phosphor layer corresponds to a “wavelength conversion unit”.

In recent years, a spray coating method is known as a method of forming a phosphor layer (wavelength conversion unit) (see, for example, Patent Document 1).
The spray coating method is easy to apply the phosphor layer to a thin and uniform thickness, but the range applied by spray coating is wider than the size of the light emitting element. In addition, since the coating liquid used for coating usually contains a component for fixing (solidifying) the phosphor to the light emitting element, the coated phosphor is solidified to the light emitting element as it is. Therefore, when applying only to the portion of the light emitting element, it is necessary to cover the portion where the phosphor is not required to be coated with a mask having a predetermined shape.

International Publication Number WO03 / 034508 A1

However, even if it is covered with a mask, the phosphor is solidified on the mask, and in order to recover and reuse the solidified phosphor, separation of the solidified phosphor from the mask or separation from the solidified phosphor Impurities need to be separated, and complicated processing steps are required.
The present invention has been made in view of the above circumstances, and an object of the present invention is to provide a method for manufacturing a light-emitting device that does not require complicated processing steps and can easily collect and reuse phosphors.

In order to solve the above problems, according to the present invention, a light emitting element that emits light having a predetermined wavelength and a phosphor that emits fluorescence having a wavelength different from the excitation wavelength when excited by light emitted from the light emitting element are included. In a method for manufacturing a light emitting device having a wavelength conversion unit,
A first mask disposing step of disposing a first mask covering a part of the light emitting element on the light emitting element;
A phosphor mixture application step of applying a phosphor mixture in which the phosphor is dispersed in a solvent to the light emitting element partially covered with the first mask;
A first mask removing step of removing the first mask from the light emitting element;
A separation step of separating the phosphor-containing material containing the phosphor from the first mask;
A fixing solution applying step of applying a fixing solution for fixing the phosphor on the light emitting element to which the phosphor mixture solution is applied;
And a drying step of forming the wavelength conversion unit by drying the fixing solution applied on the light emitting element.

According to the present invention, the phosphor mixture is applied through the first mask, and then the first mask is removed to separate the phosphor-containing material from the first mask. Since the phosphor-containing material is separated before fixing, the phosphor-containing material can be easily recovered without going through complicated processing steps. As a result, the phosphor can be reused by further separating impurities from the separated phosphor-containing material.

It is sectional drawing which shows schematic structure of a light-emitting device. It is a schematic diagram for demonstrating schematically the manufacturing apparatus and manufacturing method of a light-emitting device. It is a schematic diagram for demonstrating schematically the manufacturing apparatus and manufacturing method of a light-emitting device. It is a schematic diagram for demonstrating schematically the manufacturing apparatus and manufacturing method of a light-emitting device. It is a schematic diagram for demonstrating schematically the manufacturing apparatus and manufacturing method of a light-emitting device. It is a schematic diagram for demonstrating schematically the manufacturing apparatus and manufacturing method of a light-emitting device. 2A to 2E are diagrams for easily explaining the manufacturing method of FIGS. 2A to 2E. 6 is a view showing a modification of the manufacturing method of FIGS. 2A to 2E. It is sectional drawing which shows schematic structure of a light-emitting device. It is a schematic diagram for demonstrating schematically the manufacturing apparatus and manufacturing apparatus of a light-emitting device. It is drawing for demonstrating the manufacturing method of FIG. 6 in detail. FIG. 7B is a perspective view of FIG. 7A. It is a modification of a mask, Comprising: It is a figure for demonstrating the manufacturing method of FIG. 6 in detail. It is a perspective view of FIG. 8A. It is the modification of a mask, Comprising: It is the top view which showed a part of mask. It is the modification of a mask, Comprising: It is the top view which showed a part of mask. It is the modification of a mask, Comprising: It is the top view which showed a part of mask. It is the modification of a mask, Comprising: It is the top view which showed a part of mask. It is a modification of a mask, Comprising: It is a figure for demonstrating the manufacturing method of FIG. 6 in detail. FIG. 10B is a perspective view of FIG. 10A. It is a modification of a mask, Comprising: It is a figure for demonstrating the manufacturing method of FIG. 6 in detail.

Hereinafter, preferred embodiments of the present invention will be described with reference to the drawings.
As shown in FIG. 1, the light emitting device 100 includes an LED substrate 1 having a concave cross section. A metal part 2 is provided in a recess (bottom part) of the LED substrate 1, and a rectangular parallelepiped LED element 3 is disposed on the metal part 2. The LED element 3 is an example of a light emitting element that emits light of a predetermined wavelength. A protruding electrode 4 is provided on the surface of the LED element 3 that faces the metal part 2, and the metal part 2 and the LED element 3 protrude. They are connected via electrodes 4 (flip chip type).

In the present embodiment, a blue LED element is used as the LED element 3. For example, a blue LED element is formed by laminating an n-GaN-based cladding layer, an InGaN light-emitting layer, a p-GaN-based cladding layer, and a transparent electrode on a sapphire substrate.

A wavelength converter 6 is formed in the recess of the LED substrate 1 so as to seal the periphery of the LED element 3. The wavelength conversion unit 6 is a part that converts light having a predetermined wavelength emitted from the LED element 3 into light having a longer wavelength different from the light having a wavelength different from the wavelength of the LED element 3. A phosphor that is excited to emit fluorescence having a wavelength different from the excitation wavelength is added.
Here, the wavelength conversion unit 6 is formed so as to seal the periphery of the LED element 3, but the wavelength conversion unit 6 may be provided only on the periphery (upper surface and side surface) of the LED element 3, and the LED substrate. The wavelength conversion unit 6 may not be provided in the concave portion 1.

Then, the manufacturing method of the light-emitting device 100 is demonstrated.
The method for manufacturing the light emitting device 100 includes the following steps (1) to (5).
(1) A first mask arrangement step of arranging a first mask 50 covering a part of the LED element 3 on the LED element 3 (see FIG. 2A).
(2) A phosphor mixed solution 40 in which a phosphor is dispersed in a solvent on the LED element 3 partially covered with the first mask 50 (a phosphor mixture not containing a fixing solution for fixing the phosphor). Phosphor mixed liquid coating process for coating (see FIG. 2B)
(3) First mask removing step for removing the first mask 50 from the LED element 3 (see FIG. 2C)
(4) Separation step of separating the phosphor-containing material containing the phosphor from the first mask 50 (see FIG. 2D)
(5) Fixing solution application step of applying a fixing solution 42 for fixing the phosphor in the phosphor mixture 40 onto the LED element 3 to which the phosphor mixture 40 is applied (see FIG. 2E).
(6) Drying step of drying the fixing solution 42 applied on the LED element 3

(1) First Mask Placement Step In the first mask placement step, as shown in FIG. 2A, a first mask 50 (hereinafter simply referred to as a mask 50) is pasted on the strip package 8. The mask 50 has a strip shape (tape shape) like the strip package 8, and a through hole 52 corresponding to the concave portion 8 a of the strip package 8 is formed.
(1.1) Mask The mask 50 is made of an alcohol-resistant material, specifically, polyamide, polyimide, polyether ketone, polyether ether ketone, polyamide imide, polyphenylene sulfide, polyester, polyether imide, Polysulfone, polyethersulfone, polycarbonate, polymethyl methacrylate, polycycloolefin, modified polyphenylene oxide, liquid crystal polymer, polyacetal, polyolefin, polystyrene, fluororesin, acrylonitrile-butadiene-styrene copolymer, triacetyl cellulose, silicone, epoxy, It is composed of at least one resin material such as acrylic and epoxy silicone. The mask 50 may be comprised from 1 type of resin materials among these resin materials, and may be comprised by the combination by 2 or more types of resin materials.
The thickness of the mask 50 is preferably 1.0 to 2.0 mm. If the thickness is less than 1.0 mm, the mask 50 itself may be warped (there is a possibility of peeling from the strip package 8). If the thickness exceeds 2.0 mm, the edge of the mask 50 is mixed with the phosphor. This is because it becomes an obstacle when the liquid 40 is applied and it is difficult to apply the liquid 40 in the design range.

A protective layer 54 (see FIG. 3) may be formed on the surface of the mask 50.
The protective layer 54 is preferably made of at least one material of chromium oxide, chromium, nickel, diamond-like carbon, diamond, SiC, silicon nitride, and fluorine compound. The protective layer 54 may be comprised from 1 type of resin materials among these materials, and may be comprised by the combination by 2 or more types of resin materials.
When the protective layer 54 is made of chromium oxide, chromium, nickel, diamond-like carbon, diamond, SiC, or silicon nitride, it can be formed by PVD processing such as vapor deposition, sputtering, or ion plating, or CVD processing.
When the protective layer 54 is made of nickel or chrome, it can be formed by plating. Although nickel and chromium are metals, they become hard when thinned (Vickers hardness of about 500 to 900). In particular, since these two materials have a high film formation rate per unit time and a relatively low film stress, it is possible to increase the film thickness to 1 μm or more. When it is desired to form the protective layer 54 in a short time, or when it is desired to form a thick protective layer 54 having a thickness of 1 μm or more, both are optimal materials.
Chromium oxide can be obtained by using chromium oxide itself as a film formation source or by a method of forming a film while doping oxygen in the process of forming chromium. Further, chromium oxide can also be obtained by heating and oxidizing the chromium film in the atmosphere. Chromium and chromium oxide are excellent in heat resistance, and are preferable when the mask 50 is used in a high temperature environment in the atmosphere of 100 ° C. or higher.
The diamond-like carbon film / diamond film can be formed by an ion plating method. A very hard film (Vickers 3000 or more) is obtained. Since the surface smoothness is good and the coating material adhered when cleaning the mask 50 can be easily removed, it is preferable when reducing the number of steps in the cleaning process.
SiC and silicon nitride films can also be formed on various materials such as CVD, sputtering, and ion plating on a material (Vickers 1000 to 3000) that has a hardness similar to that of diamond. It is possible to form a hard film on the mask 50 in accordance with existing equipment without additional investment. In addition, the acid / alkali / heat resistant performance is very good, and the range of selection of mask cleaning agents is expanded.
The necessary protective layer 54 can be selected according to the above various purposes.
When the protective layer 54 is made of a fluorine compound, a Teflon (registered trademark) fluorine resin dissolved in a solvent may be applied to the mask 50 as it is and dried.
A fluorine film can be obtained by a very simple manufacturing method and a chemically stable film having hardness and heat resistance can be obtained. The wettability with the coating solution on the film surface is small, and the attached coating agent can be easily removed.
By forming these protective layers 54 on the surface of the mask 50, in addition to improving the alcohol resistance performance of the mask 50, the protective layer 54 increases the hardness of the surface of the mask 50 and improves the strength. Therefore, even when a hard phosphor is sprayed in the phosphor mixture application process described later, it is possible to prevent the mask 50 from being scraped by the phosphor and generating minute dust.
Further, if the protective layer 54 made of a fluorine compound is formed on the mask 50, the protective layer 54 has water repellency. Therefore, after the phosphor mixed solution 40 is applied and dried, the phosphor is easily separated in the separation step. Can be recovered and reused.

The mask 50 may be made of at least one metal material of Al, SUS (Steel Use Stainless), Cu, and Ti. The metal mask 50 may be composed of one metal material among these metal materials, or may be composed of a combination (alloy) of two or more metal materials.
In particular, the type of SUS is preferably austenitic SUS such as SUS303, SUS304, SUS316, or SUS310 because rust is less likely to occur. In addition, stainless steel invar material having a low low thermal expansion coefficient although rust is somewhat generated can minimize the influence of the displacement and shape change of the mask 50 due to the environmental temperature change, and gives a thermal history with the mask 50 applied. At this time, when applying the temperature-adjusted coating liquid 40 to the strip package 8, it is most preferable because the positional deviation between the mask 50 and the strip package 8 can be suppressed. When using this stainless steel invar material, the above-mentioned protective layer 54 is preferably used on the surface of the mask 50 to prevent rust.
Since the Al material is easy to process, when a large amount of the mask 50 having a more complicated shape is required, it becomes a preferable material for reducing the processing cost.
Cu has a very high thermal conductivity, and is preferable when it is desired to follow the substrate in a high temperature environment or a change in the temperature of the outer periphery. The Cu mask 50 can also be used as a heat sink, and the temperature of the strip-shaped package 8 can be controlled through the mask 50 by bringing the Cu mask 50 into contact with a heat source or a cooling source.
Since Ti is a light and high-strength material, it is preferable when making a mask 50 having a larger area than SUS-based materials.
The thickness of the metal mask 50 is preferably 0.2 to 2.0 mm. If the thickness is less than 0.2 mm, the mask 50 itself may be warped. If the thickness exceeds 2.0 mm, the end of the mask 50 becomes an obstacle when the liquid mixture 40 is applied. This makes it difficult to apply.
A protective layer 54 may be formed on the surface of the metal mask 50 similarly to the resin mask 50.
When the metal mask 50 is used, it can be machined, rolled, pressed, or the like.
The metal mask 50 has a high cost merit (but not as much as a resin material) and is relatively easy to process. Therefore, the metal mask 50 can be processed into a complicated shape, and the shape of the package 1 and the LED element 3 is changed. Can also respond.
Furthermore, the metal mask 50 is superior in solvent resistance as compared to the case of resin, and can widely correspond to (use) the type of solvent used in the ceramic precursor solution.
In addition, since the hardness of the metal mask 50 is approximately the same as or inferior to the hardness of the phosphor, if the protective layer 54 is formed on the surface of the mask 50, the strength of the surface of the mask 50 is improved. Even when a strong jet is received, the mask 50 can be prevented from being damaged by the strong phosphor.

The mask 50 may be made of at least one ceramic material of alumina, silicon nitride, silicon carbide, or zirconia. The ceramic mask 50 may be composed of one ceramic material among these ceramic materials, or may be composed of a combination (alloy) of two or more ceramic materials.
Alumina is particularly excellent in workability and is preferable when a complex shape is required for the mask 50 with a ceramic material.
On the other hand, silicon nitride is also excellent in workability, but since its coefficient of thermal expansion is particularly low, the influence of displacement and shape change of the mask 50 due to environmental temperature changes can be minimized, and heat can be applied while the mask 50 is applied. When giving a history, the positional deviation between the mask 50 and the strip package 8 is most preferably suppressed.
Silicon carbide is a very hard material, and the mask 50 is hardly worn or damaged by the phosphor. It is preferable when you want to minimize the incidence of garbage.
Zirconia has a low thermal conductivity, and when there is an instantaneous change in ambient heat, when it is not desired to convey the change to the strip package 8, for example, when drying the temperature-controlled coating solution 40, a halogen light or the like is used. When the surface is instantaneously heated to dry the moisture and the solution, unnecessary heating of the strip package 8 can be prevented.
The thickness of the ceramic mask is preferably 0.5 to 2.0 mm. If the thickness is less than 0.5 mm, the mask 50 itself may be warped. If the thickness exceeds 2.0 mm, the end of the mask 50 becomes an obstacle when the liquid mixture 40 is applied. This makes it difficult to apply.
When the ceramic mask 50 is used, it can be produced by a method combining a sintering method and machining.
According to the ceramic mask 50, since the hardness itself is large, it is possible to prevent the mask 50 from being damaged by a strong phosphor without providing a member such as the protective layer 54.
Furthermore, according to the ceramic mask 50, as in the case of the metal mask 50, it is superior in solvent resistance compared to the case of the resin, and widely supports the types of solvents used in the ceramic precursor solution (use )can do.
When the metal or ceramic mask 50 is used, it is not attached to the strip package 8 like the resin mask 50 but is placed at a predetermined position of the strip package 8 or fixed to the strip package 8. What is necessary is just to arrange | position at intervals.

(2) Phosphor mixture liquid application process The phosphor mixture liquid 40 (phosphor or additive) and process used in the phosphor mixture application process will be described.
(2.1) Phosphor The phosphor is excited by the wavelength (excitation wavelength) of light emitted from the LED element 3 and emits fluorescence having a wavelength different from the excitation wavelength. In this embodiment, 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. Alternatively, 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. Mix to obtain a mixed raw material. Then, 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.
In this embodiment, the YAG phosphor is used. However, the type of the phosphor is not limited to this. For example, other phosphors such as non-garnet phosphors containing no Ce are used. You can also. In addition, the larger the particle size of the phosphor, the higher the light emission efficiency (wavelength conversion efficiency). On the other hand, the gap formed at the interface with the organometallic compound is increased, and the film strength of the formed ceramic layer is lowered. 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 μm or more and 50 μm or less. The average particle diameter of the phosphor can be measured, for example, by a Coulter counter method.

(2.2) Additive The method for adjusting the viscosity of the phosphor mixture liquid 40 includes a technique of adding swollen particles or inorganic particles to the solvent. Any technique can be used as long as the phosphor mixture liquid 40 can be thickened. However, the present invention is not limited to this.

(2.2.1) Swelled particles Examples of the swollen particles include layered silicate minerals.
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 by adding water to the mixed solution, a card house structure in which water enters and swells between layers of the smectite structure has an effect of greatly increasing the viscosity of the mixed solution.
When the content of the layered silicate mineral in the ceramic layer is less than 1% by weight, the effect of increasing the viscosity of the mixed solution cannot be obtained sufficiently. On the other hand, when the content of the layered silicate mineral exceeds 20% by weight, the strength of the ceramic layer after heating is lowered. Therefore, the content of the layered silicate mineral is preferably 1% by weight to 20% by weight, and more preferably 1% by weight to 10% by weight.
In consideration of compatibility with an organic solvent, a layered silicate mineral whose surface is modified (surface treatment) with an ammonium salt or the like can be used as appropriate.

(2.2.2) Inorganic particles Inorganic particles (oxide fine particles) fill not only the thickening effect that increases the viscosity of the phosphor mixture 40, but also the gap that occurs at the interface between the organometallic compound and the phosphor. It also has a filling effect and a film strengthening effect that improves the film strength of the ceramic layer after heating.
Examples of the inorganic particles used in the present invention include oxide fine particles such as silicon oxide, titanium oxide and zinc oxide, fluoride fine particles such as magnesium fluoride, and the like. In particular, when a silicon-containing organic compound such as polysiloxane is used as the organometallic compound, it is preferable to use silicon oxide fine particles from the viewpoint of stability with respect to the formed ceramic layer.
When the content of the inorganic particles in the ceramic layer is less than 1% by weight, the above-described effects cannot be sufficiently obtained. On the other hand, when the content of the inorganic particles exceeds 20% by weight, the strength of the ceramic layer after heating is lowered. Therefore, the content of the inorganic particles in the ceramic layer is preferably 1% by weight or more and 20% by weight or less, and more preferably 1% by weight or more and 10% by weight or less. The average particle diameter of the inorganic particles is preferably 0.001 μm or more and 50 μm or less in consideration of the above-described effects. The average particle diameter of the inorganic particles can be measured, for example, by a Coulter counter method.

(2.3) Preparation of phosphor mixed solution As a preparation procedure of the phosphor mixed solution 40, lipophilic swelling particles or inorganic particles to which an organic cation is added or surface-treated are first premixed in an organic solvent. Thereafter, the phosphor or the phosphor and water are mixed. Thereby, swelling particle | grains or an inorganic particle can be mixed uniformly, and the thickening effect can be heightened more.
The viscosity of the phosphor mixture 40 is 10 to 1000 cP, preferably 12 to 500 cP, more preferably 20 to 400 cP, and most preferably 50 to 300 cP. These viscosities were measured using a vibration viscometer (VM-10A-L manufactured by CBC).
Note that the phosphor mixture liquid 40 may contain only swollen particles, may contain only inorganic particles, or may contain both swollen particles and inorganic particles.
Since the phosphor mixture liquid 40 prepared as described above does not contain a fixing solution (ceramic precursor) for fixing the phosphor, it contains a phosphor containing phosphor from the first mask 50 in the separation step described later. It is easy to separate matter, and since there is no substance fixed to the phosphor, it is easy to regenerate the phosphor.

(2.4) Coating device When apply | coating the fluorescent substance liquid mixture 40, the coating device 10 of FIG. 2B is used, for example.
The coating device 10 mainly includes a movable table 20 that can move up and down, left and right, and back and forth, and a spray device 30 that can spray the phosphor mixture 40 described above.

The spray device 30 is disposed above the movable table 20.
The spray device 30 has a nozzle 32 into which air is sent, and an air compressor (not shown) for sending air is connected to the nozzle 32. The hole diameter at the tip of the nozzle 32 is 20 μm to 2 mm, preferably 0.1 to 0.3 mm. The nozzle 32 is movable up and down, left and right, and front and rear, like the moving table 20.
For example, the spray gun W-101-142BPG manufactured by Anest Iwata is used as the nozzle 32, and the OFP-071C manufactured by Anest Iwata is used as the compressor.
The angle of the nozzle 32 can be adjusted, and the nozzle 32 can be tilted with respect to the movable table 20 (or the LED substrate 1 installed on the moving table 20). The angle of the nozzle 32 with respect to the injection target (LED substrate 1) is preferably in the range of 0 to 60 ° when the vertical direction from the injection target is 0 °.
A tank 36 is connected to the nozzle 32 via a connecting pipe 34. A fluorescent liquid mixture 40 is stored in the tank 36. The tank 36 contains a stirring bar, and the phosphor mixed solution 40 is constantly stirred. If the phosphor mixture liquid 40 is stirred, sedimentation of the phosphor having a large specific gravity can be suppressed, and a state in which the phosphor is dispersed in the phosphor mixture liquid 40 can be maintained.
For example, Anest Iwata PC-51 is used as the tank.

(2.5) Application of phosphor mixed solution When actually applying the phosphor mixed solution 40, a plurality of LED substrates 1 (on which the LED elements 3 are mounted in advance) are installed on the moving table 20, and the LED substrate 1 And the positional relationship between the nozzle 32 of the spray device 30 is adjusted.
Specifically, the LED substrate 1 is installed on the moving table 20, and the LED substrate 1 and the tip end portion of the nozzle 32 are arranged to face each other. The phosphor mixture liquid 40 can be uniformly applied as the distance between the LED substrate 1 and the nozzle 32 increases, but the film strength tends to decrease. It is suitable to keep the distance in the range of 3 to 30 cm.

Thereafter, while the LED substrate 1 and the nozzle 32 are moved relative to each other, the phosphor mixed solution 40 is sprayed from the nozzle 32 to apply the mixed solution 40 to the LED substrate 1 (phosphor applying step).
Specifically, on the other hand, the moving base 20 and the nozzle 32 are moved to move the LED substrate 1 and the nozzle 32 back and forth and right and left. Either one of the moving table 20 and the nozzle 32 may be fixed, and the other may be moved back and forth and left and right. A method of applying a plurality of LED elements 3 in a direction orthogonal to the moving direction of the moving table 20 and moving the nozzle 32 in a direction orthogonal to the moving direction of the moving table 20 is also preferably used. On the other hand, air is fed into the nozzle 32 and the mixed liquid 40 is sprayed from the tip of the nozzle 32 toward the LED substrate 1. The distance between the LED substrate 1 and the nozzle 32 can be adjusted in the above range in consideration of the pressure of the air compressor. For example, the pressure of the compressor is adjusted so that the pressure at the inlet (tip) of the nozzle 32 is 0.14 MPa.
By the above operation, the phosphor mixed solution 40 can be applied onto the LED element 3.

(3) First Mask Removal Step In the first mask removal step, the mask 50 is peeled from the strip package 8 as shown in FIG. 2C.

(4) Separation process (4.1) Separation means As shown in FIG. 2D, as the separation means, the phosphor-containing material is separated from the mask 50 by vibrating the mask 50, for example.
Further, the phosphor-containing material may be separated from the mask 50 by gravity. Specifically, the phosphor-containing material is separated by naturally drying the mask 50 so that the front and back surfaces are turned over or the mask 50 is tilted.
Alternatively, the phosphor-containing material may be separated from the mask 50 by scraping the phosphor-containing material.
Furthermore, a film (not shown) may be attached on the mask 50, and the phosphor-containing material attached to the film may be separated by peeling off the film.

(4.2) Impurity removal step An impurity removal step of removing impurities from the phosphor-containing material separated in the separation step of (4) may be performed. There are two methods for removing impurities, a method for removing everything other than phosphors as impurities and a method for removing only organic impurities. That is, there are a method of collecting and reusing only the phosphor, and a method of collecting and reusing a phosphor mixed with impurities (swelling particles and inorganic particles).
As a method of removing all impurities other than the former phosphor, only the phosphor is separated and recovered by dissolving the phosphor-containing material separated in the separation step with a solvent and filtering with a filter having a diameter smaller than 1 μm. be able to. This is because the particle size of the phosphor is larger than that of the swollen particles and inorganic particles, so that only the phosphor can be separated.
As a method for removing only the latter organic impurities, the phosphor and the swollen particles (and inorganic particles) are separated and recovered by baking the phosphor-containing material separated in the separation process at a high temperature of 100 ° C. to 120 ° C. be able to. In addition, it is more preferable to remove all impurities other than the phosphor because the purity can be increased when reused.
In addition, the phosphor obtained through the impurity removal step is then inspected for luminous efficiency (inspection step). Based on the luminous efficiency of the phosphor obtained in the inspection process, light emission in a predetermined color can be obtained by adjusting the ratio of the phosphor obtained in the collection and the unused phosphor that has not undergone the collection process. The phosphor mixed liquid 40 to be produced can be produced again. Or you may produce the fluorescent substance liquid mixture 40 again only using the fluorescent substance obtained by collection | recovery, without using an unused fluorescent substance.

(5) Fixing solution application process (5.1) Fixing solution The fixing solution 42 is a solution in which a metal compound as a ceramic precursor is dispersed in a solvent. If a translucent ceramic can be formed, the kind of metal is used. There is no limit.

(5.1.1) Sol-gel solution The fixing solution 42 may be a solution (sol-gel solution) in which ceramics are formed by heating the gel after gelation by a reaction such as hydrolysis. Further, by volatilizing the solvent component, the ceramic may be directly formed without gelation.
In the former case (sol-gel solution), the metal compound may be an organic compound or an inorganic compound. Examples of preferable metal compounds include metal alkoxides, metal acetylacetonates, metal carboxylates, nitrates, and oxides. Of these, metal alkoxides are preferred because they are easily gelled by hydrolysis and polymerization reaction, and tetraethoxysilane is particularly preferred. A plurality of types of metal compounds may be used in combination. As the fixing solution, it is preferable to appropriately contain water for hydrolysis, a solvent, a catalyst and the like in addition to the metal compound.
Examples of the solvent include alcohols such as methanol, ethanol, propanol, and butanol.
Examples of the catalyst include hydrochloric acid, sulfuric acid, nitric acid, acetic acid, hydrofluoric acid, ammonia and the like.
When tetraethoxysilane is used as the metal compound, it is preferable to use 138 parts by mass of ethyl alcohol and 52 parts by mass of pure water with respect to 100 parts by mass of tetraethoxysilane.

(5.1.2) Polysilazane Polysilazane can also be used as a ceramic precursor.
The polysilazane used in the present invention is represented by the following general formula (i).
(R ¹ R ² SiNR ³ ) _n (i)
In formula (i), 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 One is a hydrogen atom, 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.
Polysilazane represented by the above formula (i) and a reaction accelerator as required are dissolved in an appropriate solvent and cured by heating, excimer light treatment, UV light treatment, and excellent heat resistance and light resistance. A ceramic film can be produced. In particular, 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.
As the reaction accelerator, an acid, a base, or the like is preferably used, but it may not be used. Examples of 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.
Particularly preferred when a reaction accelerator is used is a metal carboxylate, and the addition amount is preferably 0.01 to 5 mol% based on polysilazane.
As the solvent, aliphatic hydrocarbons, aromatic hydrocarbons, halogen hydrocarbons, ethers, and esters can be used. 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 preferably higher, but since the increase in concentration leads to a shortening of the polysilazane storage period, the polysilazane is preferably dissolved in the solvent at 5% by mass or more and 50% by mass or less.

(5.2) Application of Fixing Solution As shown in FIG. 2E, when the fixing solution 42 is applied, the same application apparatus 10 as in FIG. 2B is used in the same manner as when the phosphor mixed solution 40 is applied. A fixing solution 42 can be applied on the LED element 3 to which the phosphor mixed solution 40 is applied. In addition, when apply | coating the fixing liquid 42 on the LED element 3 to which the fluorescent substance mixed liquid 40 was apply | coated, the state which the fluorescent substance mixed liquid 40 may be dried may be sufficient. When the fixing liquid 42 is applied after the phosphor mixed liquid 40 is dried, the movement of the phosphor on the LED element 3 due to the application pressure when the fixing liquid 42 is applied onto the LED element 3 is reduced. Therefore, the chromaticity uniformity of the LED element 3 can be improved.
As in the case of applying the phosphor mixture liquid 40 when the fixing liquid 42 is applied, a second part of the LED element 3 covering the LED element 3 to which the phosphor mixture liquid 40 is applied is covered. The fixing solution 42 may be applied onto the LED element 3 by arranging the mask 60. Thereafter, the second mask 60 may be removed from the LED element 3 to separate a metal compound or the like as a ceramic precursor in the fixing solution 42 attached from the second mask 60. Note that the second mask 60 can be the same as the first mask 50.

(6) Drying Step In the drying step, the wavelength conversion section 6 can be formed (completed) by drying the fixing solution 42 by heating after applying the fixing solution.
The heating temperature is preferably 120 ° C. to 500 ° C., and more preferably 120 ° C. to 200 ° C. from the viewpoint of further suppressing deterioration of the LED element 3 and the like.

As described above, according to the embodiment of the present invention, the phosphor mixture liquid 40 is applied through the first mask 50, and then the first mask 50 is removed from the LED element 3, and the first mask 50. Since the phosphor-containing material is separated from the phosphor, and the phosphor-containing material is separated before fixing the phosphor, the phosphor-containing material can be easily recovered without going through complicated processing steps. As a result, the phosphor can be reused by further separating impurities from the separated phosphor-containing material. That is, in the present invention, since the phosphor mixture liquid 40 does not contain a fixing solution for fixing the phosphor, the phosphor-containing material can be easily separated from the first mask 50, and the phosphor mixture liquid 40 is not fluorescent. Since there is no substance that adheres to the body, the effect of easily regenerating the separated phosphor-containing material is obtained.
Further, since the phosphor-containing material is separated from the first mask 50 by vibrating the first mask 50, using gravity, or scraping off, it can be easily separated by a simple method. .
Further, since impurities are further removed from the phosphor-containing material separated from the first mask 50, only the phosphor can be recovered and reused. Further, by removing the impurities by heating the phosphor-containing material, the impurities can be easily removed.
Further, since the emission efficiency of the collected phosphor is inspected, it is possible to sort out phosphors with good emission efficiency and reuse them.
Since the second mask 60 is disposed on the LED element 3 and the fixing solution 42 is applied onto the LED element 3, the second mask 60 is recovered and the second mask 60 is used to fix the solution in the fixing solution 42. By separating the metal compound or the like, the metal compound or the like can also be reused.
Further, as in the prior art, for example, in the case of Japanese Patent No. 4450547 and Japanese Patent Application Laid-Open No. 2005-311395, if the coating liquid is continuously applied using a mask, dust adheres to the wavelength conversion section obtained after drying. May have. When the present inventor examined the phenomenon for such a problem, when the coating solution contains an organic solvent such as isopropyl alcohol (IPA), a part of the mask is dissolved and peeled off by the alcohol solvent. However, it has been found that the fragments are mixed in the coating solution. In particular, in the case of direct application by a spray method including a phosphor, in addition to the generation of dust due to the dissolution, the mask is shaved by spraying a hard phosphor, so that minute dust is scattered and adheres to the wavelength conversion unit. There was a problem. Therefore, as described above, when the mixed solution 40 is applied, by using the alcohol-resistant resin mask 50, dissolution by the alcohol solvent in the mixed solution 40 is suppressed, and the wavelength conversion unit 6. On the other hand, it is possible to prevent dust from being dissolved in the mask 50 from being mixed.
When the resin mask 50 is used, it can be mass-produced by press molding or the like.
The resin mask 50 is cost-effective and can be disposable, and can be processed into a complicated shape. Therefore, even if the shape of the package 1 or the LED element 3 changes in the future, it becomes possible to cope with it.
Further, when the protective layer 54 is formed on the surface of the mask 50, the strength of the surface of the mask 50 is improved, so that the mask 50 is damaged by the strong phosphor even when the liquid mixture 40 is strongly jetted. Can be prevented.

In addition, this invention is not limited to the said embodiment, In the range which does not deviate from the summary, it can change suitably.
For example, in the fixing solution application process of the above embodiment, the spray device 30 used in the phosphor mixed solution application step is used. However, as shown in FIG. The liquid 42 may be applied to the LED element 3. The configuration of the fixing liquid spray device 80 is the same as that of the phosphor mixed liquid spray device 30. Also in this case, as described above, after the phosphor mixture liquid 40 is applied by the spray device 30 through the mask 50, the fixing solution 42 may be applied by the spray device 80 through the mask 60. In this way, by applying the phosphor mixture liquid 40 and the fixing liquid 42 with

different spray devices

30 and 80, the fixing liquid 42 and the phosphor mixture liquid 40 are more optimal in terms of ejection amount, ejection pressure, viscosity, etc., respectively. And each solution can be uniformly applied to the LED element 3 in a dispersed state.

Here, the variation of the shape of the

masks

50 and 60 will be described.
When the following mask is used, as shown in FIGS. 5, 6, and 7A, the inner wall surface 81 that forms the concave portion 8a of the package 1 becomes a tapered surface so as to increase in diameter upward. It is preferable.
The mask 50F has a belt-like shape (tape shape) like the belt-like package 8, and as shown in FIG. 7B, a through-hole 52 having a rectangular shape in plan view is formed at a position corresponding to the concave portion 8a of the belt-like package 8. Yes. A cover portion 51 is formed at a position corresponding to the upper side of the LED element 3 in the through hole 52 so as to cover the entire upper surface of the LED element 3. In this case, the cover 51 has a rectangular shape that is slightly larger than the planar shape of the LED element 3.
The cover portion 51 is supported by a support portion 55 that spans the surfaces of the inner peripheral surface 53 that forms the through hole 52 that face each other.
Therefore, the cover 51 covers the entire upper surface of the LED element 3, so that the mixed liquid 40 sprayed from the nozzle 32 of the spray device 30 flows so as to flow around the LED element 3 near the ridge line of the cover 51. The jet of the liquid 40 changes. As a result, the mixed solution 40 is uniformly attached to the side surface and the upper surface of the LED element 3.

The mask 50F may have a shape other than those shown in FIGS. 7A and 7B, and other mask shapes will be described below.
The mask 50A shown in FIGS. 8A and 8B has a band shape (tape shape) like the band package 8, and a rectangular through hole 52A in a plan view is formed at a position corresponding to the concave portion 8a of the band package 8. ing. Then, the inner peripheral surface 53A that forms the through hole 52A of the mask 50A has a taper having the same inclination angle so as to be substantially flush with the tapered surface that is the inner wall surface 81 that forms the concave portion 8a of the band-shaped package 8. It is a surface.
Therefore, the liquid mixture 40 sprayed from the nozzle 32 of the spray device 30 flows smoothly along the tapered surface (inner peripheral surface 53A) and the tapered surface which is the inner wall surface 81 forming the recess 8a, and the side surface of the LED element 3 Go around to the side. As a result, the jet can be collected around the LED element 3, and the mixed liquid 40 is uniformly attached to the side surface and the upper surface of the LED element 3.

The mask 50 B shown in FIG. 9A also has a strip shape (tape shape) like the strip package 8. The mask 50 B has a mesh shape including a large number of meshes 56 B (through holes) at positions corresponding to the recesses 8 a of the strip-shaped package 8. A large number of meshes 56B have a rectangular shape with a substantially uniform size.
A mask 50C shown in FIG. 9B is different from the mask 50B shown in FIG. 9A, and a lot of meshes 56C are meshes whose centers are dense and whose outer periphery is sparse.
On the other hand, the mask 50D shown in FIG. 9C differs from the mask 50B shown in FIG. 9A in that many meshes 56D have a sparse center and a dense outer periphery.
In the

masks

50C and 50D shown in FIGS. 9B and 9C, the

meshes

56C and 56D are formed. Therefore, the mixed liquid 40 ejected from the nozzles 32 of the spray device 30 flows between the

numerous meshes

56C and 56D, and the flow rate of the jet flows. Due to the difference, the jet changes.
Although the fine settings differ depending on various conditions such as the size of the nozzle mouth, the position of the nozzle and the tip, the viscosity of the liquid to be sprayed, the density and weight of the phosphor to be mixed, the general tendency is as shown in FIG. 9A When the uniform mesh mask 50B is used, it is used when the density of the phosphor is relatively small and the liquid has a low viscosity and is easily diffused by a nozzle. The jet flow after passing through the mask tends to be mist-like and tends to adhere uniformly to the side surface.
9B and 9C, in the case where it is desired to have a mesh density difference between the center and the outer edge, the density of the phosphor is high and the straightness of the sprayed particles is strong, and the angle of the nozzle Or when the arrangement is adjusted.
In the case of a mesh mask with a dense center and a sparse outer periphery, such as the mask 50C, when a nozzle is placed and sprayed in the vicinity of almost the top of the chip, the jet that reaches the mask flows in a sparse to dense direction of the mesh 56C. Diffuses, and the mixed liquid 40 is uniformly attached to the side surface and the upper surface of the LED element 3.
On the other hand, the mask 50D has an effect of making the film thickness of the side surface and the upper surface of the chip uniform when the nozzle is arranged at an oblique position of the chip or when the nozzle is sprayed at an angle. In this case, since the jet is inclined obliquely, it is easy to hit the side and not to the top. If the mask 50D is used in such a case, the thickness of the phosphor can be uniformly attached.
Thus, even if the conditions and arrangement of the nozzle and the liquid are changed, the phosphor can be uniformly attached to the side surface of the chip only by changing the shape of the mask to be covered.
Of the mesh-

like masks

50B, 50C, and 50D shown in FIGS. 9A to 9C, the mesh-

like masks

50C and 50D shown in FIGS. 9B and 9C have a difference in flow rate in the jet flow than the mesh-like mask 50B shown in FIG. 9A. It is preferable in that it is easily generated.
The mesh masks 50B, 50C, and 50D shown in FIGS. 9A to 9C describe only mask portions at positions corresponding to the concave portions 8a of the strip package 8, and the outside of the mesh portions is as follows. This is a mesh-free portion that is affixed to the upper surface of the strip package 8.
Further, the shape of the

meshes

56B, 56C, and 56D can be appropriately changed to a rectangular shape, a diamond shape, a circular shape, and the like depending on the spray conditions, the size shape of the LED element 3, and the like (for example, refer to the mask 50Da in FIG. 9D).
In the case of this mesh-structured mask, since the entrainment of the jet is larger than the others, the thickness of the phosphor can be uniformly attached even if the inner wall surface of the package is not enlarged upward. .

In the case of FIGS. 10A and 10B, a reflective member 82 such as Al or Ag is provided on the inner wall surface 81 that forms the recess 8 a of the strip package 8. The reflective member 82 is provided in the same taper shape along the inner wall surface 81 which forms the recessed part 8a. The mask 50 E has a band shape (tape shape) similarly to the band-shaped package 8, and a through hole 52 E having a rectangular shape in plan view is formed so as to correspond to the concave portion 8 a of the band-shaped package 8. The inner peripheral surface 53E that forms the through hole 52E of the mask 50E is a tapered surface that covers a part of the reflecting member 82 along the shape of a part of the reflecting member 82. That is, the taper surface (inner peripheral surface 53A) of the mask 50A shown in FIGS. 8A and 8B further has a shape extending along the inner wall surface 81 that forms the recess 8a.
The inner peripheral surface 53E may have a shape that covers the entire reflecting member 82.
Therefore, such a tapered surface (inner peripheral surface 53E) of the mask 50E covers the whole or a part of the reflecting member 82, so that the mixed liquid 40 ejected from the nozzle 32 of the spray device 30 becomes the tapered surface of the mask 50E. It flows along the (inner peripheral surface 53E) and turns around to the side surface side of the LED element 3. As a result, the jet can be collected around the LED element 3, and the mixed liquid 40 is uniformly attached to the side surface and the upper surface of the LED element 3.
Further, when the size of the bottom surface forming the concave portion 8a of the strip-shaped package 8 is large and the distance from the inner wall surface 81 forming the concave portion 8a to the LED element 3 is far, the LED element 3 is located along the mask 50E. This is particularly effective because the mixed liquid 40 is led to
Further, since the mask 50E has a shape extending so as to cover a part or all of the reflecting member 82, the positioning of the mask 50E with respect to the strip package 8 is easy.
Note that the inner peripheral surface 53E that forms the through hole 52E of the mask 50E may contact the inner wall surface 81 that forms the recess 8a as shown in FIGS. 10A and 10B, or as shown in FIG. 10C. A space may be provided between the inner peripheral surface 53E and the inner wall surface 81.
The mask 50E can be used for the flip-chip type LED element 3.

Although not shown in the drawings, the outer peripheral portions of the

masks

50F and 50A to 50D shown in FIGS. 7 to 9 are provided with at least one of at least one of positioning notches, bosses, and holes for the band-shaped package 8. preferable.
However, in the case of the mask 50E shown in FIG. 10, since it has a shape that can be positioned with respect to the strip package 8, as described above, it is not necessary to provide positioning notches, bosses, holes, and the like.

The mask 50F can be made of the same material as the mask 50 described above.
The thickness of the mask 50F varies slightly depending on the material, but is preferably 0.2 to 2.0 mm. More preferably, it is 0.5 to 1.0 mm. If the thickness is less than 0.2 mm, jet flow rectification, entrainment, reflection, etc. will not occur, and it will not be possible to uniformly apply to the side surface of the LED element, and the mask 50F itself may be warped. (There is a possibility of peeling from the strip package 8). If the thickness exceeds 2.0 mm, the end of the mask 50F becomes an obstacle when the mixed liquid 40 is applied, and it becomes difficult to apply the liquid within the design range.
The masks 50A to 50E are the same as the thickness of the mask 50F, and the material is also the same.

A conductive member 57 is preferably provided on the back surface of the mask 50F. Specifically, it is preferable to provide a frame shape around the through hole 52 on the back surface of the mask 50F (see FIG. 7A). As the conductive member 57, for example, a member made of metal, conductive resin, carbon, or the like is preferable.
It is necessary to dispose the mask 50F on the belt-like package 8 and make it adhere to it, and spray the mixed solution 40, and then release the mask 50F. In particular, the mask 50F is made of a nonconductive material (nonmetal) such as resin or ceramic. When configured, the mask 50F and the strip-shaped package 8 are brought into close contact with each other due to static electricity, and are not easily peeled off. Therefore, by attaching the conductive member 57 to the back surface of the mask 50F, the mask 50F can be easily peeled off from the strip package 8 by grounding and releasing static electricity.
As a method of providing the conductive member 57 on the mask 50F, for example, there are a film forming process by a sputtering method, a vapor deposition method or the like, or a method of directly attaching a thin member to the mask 50F by an adhesive or an insert.

As described above, the inner wall surface 81 that forms the concave portion 8a of the band-shaped package 8 is a tapered surface that expands upward, and the band-shaped package 8 is between the LED element 3 and the nozzle 32 of the spray device 30. Since the mask 50F that exposes at least a part of the concave portion 8a of the strip-shaped package 8 is disposed on the upper surface, the mixed liquid 40 sprayed from the nozzle 32 is a taper that is an inner wall surface 81 that forms the concave portion 8a of the strip-shaped package 8. It flows along the surface and adheres to the side surface and the upper surface of the LED element 3. As a result, the mixed liquid 40 can be uniformly applied to the side surface and the upper surface of the LED element 3. In addition, since the mask 50F exposes at least a part of the concave portion 8a of the strip-like package 8, the wraparound due to the jet of the mixed liquid 40 occurs between the portion covered with the mask 50F and the exposed portion. It can apply | coat reliably and uniformly to the side surface and upper surface of the element 3. FIG.
Therefore, as in the prior art, for example, in Japanese Patent No. 445047, by rotating the nozzle, the flow of the liquid mixture and gas is ejected in a spiral shape, so that the liquid mixture is sprayed on the upper surface and side surfaces of the LED element. However, there is a problem that a drive mechanism for rotating the nozzle is required, and the manufacturing apparatus is complicated and increases in size. However, by using the mask 50F as described above, the nozzle that ejects the mixed liquid is used. There is no need to rotate the LED in a spiral, and no rotational drive mechanism is required, so that the manufacturing apparatus can be reduced in size, and the light emitting device 100 can be easily manufactured by applying the liquid mixture 40 to the side surface of the LED element 3. .

Moreover, since the mask 50F has the cover part 51 which covers the whole upper surface of the LED element 3, the liquid mixture 40 flows so that it may wrap around the LED element 3 side in the vicinity of the ridgeline of the cover part 51, and a jet flow changes. ing. As a result, the mixed liquid 40 can be more uniformly attached to the side surface and the upper surface of the LED element 3. As described above, the mask 50F is provided with the cover portion 51 that covers the entire upper surface of the LED element 3, and the jet of the mixed liquid 40 can be changed only by improving the shape of the mask 50F. The mixed liquid 40 can be uniformly attached to the upper surface. In this respect as well, manufacturing can be facilitated.
More specifically, since the jet state changes depending on the density of the phosphor, the diameter of the nozzle, and the viscosity of the solution, the size and shape of the cover portion 51 of the mask 50F are adjusted depending on the condition of the phosphor after application. go. This delicate adjustment is also performed when other mask shapes are used. In the mask 50A, the angle of the inner peripheral surface 53A that forms the through hole 52A is slightly changed to adjust the coating condition, and in the masks 50B to 50D, the mesh is adjusted. Adjust by changing the size and shape. In the mask 50E, the angle of the inner peripheral surface 53E that forms the through hole 52E and the distance from the LED element 3 to the inner peripheral surface 53E are slightly changed and adjusted. Methods for examining the coating condition include a method of obtaining a film thickness distribution by applying a sample to a dummy sample, cutting it, and observing a cross section, and a method of actually illuminating the LED with the phosphor after application to observe the color. After fine adjustment of the mask shape, a final mask shape suitable for the shape and characteristics of the target LED element is determined.

Although the inner peripheral surface 53 that forms the through hole 52 of the mask 50F shown in FIG. 7 is not a tapered surface, it is flush with the inner wall surface 81 that forms the recess 8a as in the mask 50A shown in FIG. It is good also as such a taper surface.

Although the embodiment of the present invention has been described above, the following contents 1 to 18 are also incorporated. 1. A light emitting element that is disposed in a recess recessed below the package and emits light of a predetermined wavelength, and a phosphor that is excited by light emitted from the light emitting element and emits fluorescence having a wavelength different from the excitation wavelength In a method for manufacturing a light emitting device having a wavelength conversion unit,
The inner wall surface forming the concave portion of the package is a tapered surface that expands upward.
In the step of spraying a mixed liquid in which the phosphor is dispersed in a solvent from a spray injection port and applying the mixed liquid on the light emitting element to form the wavelength conversion unit, the light emitting element and the spray injection port A mask for exposing at least a part of the recess of the package is disposed on the upper surface of the package.
2. 2. The method for manufacturing a light-emitting device according to claim 1, wherein the mask has a cover that covers the entire upper surface of the light-emitting element.
3. The mask has a through hole that exposes a recess of the package;
2. The method for manufacturing a light-emitting device according to claim 1, wherein the inner peripheral surface forming the through hole is a tapered surface that is substantially flush with the inner wall surface forming the recess of the package.
4). 2. The method of manufacturing a light emitting device according to claim 1, wherein the mask has a mesh shape in which positions corresponding to the recesses of the package are formed of a large number of meshes.
5. 5. The method of manufacturing a light emitting device according to claim 4, wherein the plurality of meshes are meshes having a dense center and a sparse outer periphery.
6). 5. The method for manufacturing a light emitting device according to claim 4, wherein the plurality of meshes are meshes having a sparse center and a dense outer periphery.
7. A reflective member is disposed on the inner wall surface forming the concave portion of the package,
The mask has a through hole that exposes a recess of the package;
The inner peripheral surface that forms the through hole is a tapered surface that covers the whole or a part of the reflecting member along the shape of the whole or a part of the reflecting member. Manufacturing method of light-emitting device.
8). The method for manufacturing a light-emitting device according to any one of items 1 to 7, wherein the mask has a thickness of 0.2 to 2.0 mm.
9. 9. The method for manufacturing a light emitting device according to claim 1, wherein a conductive member is provided on a back surface of the mask.

10. A method for manufacturing a light-emitting device, comprising: a light-emitting element that emits light of a predetermined wavelength; and a wavelength conversion unit that includes a phosphor that is excited by light emitted from the light-emitting element and emits fluorescence having a wavelength different from the excitation wavelength. In
Applying a coating liquid in which the phosphor is dispersed in an alcohol solvent onto the light emitting element;
Heating and baking the coating solution after coating to form the wavelength conversion section;
With
In the step of applying the coating liquid, an alcohol-resistant mask is disposed on the light-emitting element.
11. In the method for manufacturing the light emitting device according to item 10,
The mask is polyamide, polyimide, polyetherketone, polyetheretherketone, polyamideimide, polyphenylene sulfide, polyester, polyetherimide, polysulfone, polyethersulfone, polycarbonate, polymethyl methacrylate, polycycloolefin, modified polyphenylene oxide, Light emission characterized by being composed of at least one resin material of liquid crystal polymer, polyacetal, polyolefin, polystyrene, fluororesin, acrylonitrile-butadiene-styrene copolymer, triacetyl cellulose, silicone, epoxy, acrylic, epoxy silicone Device manufacturing method.
12 In the method for manufacturing the light emitting device according to item 11,
A protective layer is formed on the surface of the mask,
The method for manufacturing a light emitting device, wherein the protective layer is made of at least one material of chromium oxide, chromium, nickel, diamond-like carbon, diamond, SiC, silicon nitride, and fluorine compound.
13. In the method for manufacturing a light emitting device according to item 11 or 12,
A method of manufacturing a light-emitting device, wherein the mask has a thickness of 0.5 to 2.0 mm.
14 In the method for manufacturing the light emitting device according to item 10,
The method of manufacturing a light emitting device, wherein the mask is made of at least one metal material of Al, SUS, Cu, and Ti.
15. In the method for manufacturing the light emitting device according to item 14,
A protective layer is formed on the surface of the mask,
The method for manufacturing a light emitting device, wherein the protective layer is made of at least one material of chromium oxide, chromium, nickel, diamond-like carbon, diamond, SiC, silicon nitride, and fluorine compound.
16. In the method for manufacturing a light emitting device according to item 14 or 15,
A method for manufacturing a light-emitting device, wherein the mask has a thickness of 0.2 to 2.0 mm.
17. In the method for manufacturing the light emitting device according to item 10,
The method for manufacturing a light emitting device, wherein the mask is made of at least one ceramic material of alumina, silicon nitride, silicon carbide, or zirconia.
18. In the method for manufacturing the light emitting device according to Item 17,
A method of manufacturing a light-emitting device, wherein the mask has a thickness of 0.5 to 2.0 mm.

3 LED elements (light emitting elements)
6 Wavelength conversion unit 40 Phosphor mixture liquid 42 Fixing liquid 50 First mask 60 Second mask 100 Light emitting device

Claims

A method of manufacturing a light-emitting device, comprising: a light-emitting element that emits light of a predetermined wavelength; and a wavelength conversion unit that includes a phosphor that is excited by light emitted from the light-emitting element and emits fluorescence having a wavelength different from the excitation wavelength. In
A first mask disposing step of disposing a first mask covering a part of the light emitting element on the light emitting element;
A phosphor mixture application step of applying a phosphor mixture in which the phosphor is dispersed in a solvent to the light emitting element partially covered with the first mask;
A first mask removing step of removing the first mask from the light emitting element;
A separation step of separating the phosphor-containing material containing the phosphor from the first mask;
A fixing solution applying step of applying a fixing solution for fixing the phosphor on the light emitting element to which the phosphor mixture solution is applied;
And a drying step of drying the fixing solution applied onto the light emitting element to form the wavelength conversion section.
The method for manufacturing a light emitting device according to claim 1, wherein the separating step separates the phosphor-containing material from the first mask by vibrating the first mask.
The method of manufacturing a light emitting device according to claim 1, wherein the separating step separates the phosphor-containing material from the first mask by gravity.
The method for manufacturing a light emitting device according to claim 1, wherein the separating step separates the phosphor-containing material from the first mask by scraping the phosphor-containing material.
The method for manufacturing a light emitting device according to any one of claims 1 to 4, further comprising an impurity removal step of removing impurities from the phosphor-containing material separated in the separation step.
6. The method for manufacturing a light emitting device according to claim 5, wherein the impurity removing step removes impurities from the phosphor-containing material by heating the phosphor-containing material.
The method for manufacturing a light emitting device according to claim 5 or 6, further comprising an inspection step of inspecting the light emission efficiency of the phosphor obtained by the impurity removal step.
The fixing liquid application step includes disposing a second mask covering a part of the light emitting element on the light emitting element, and applying the fixing liquid onto the light emitting element. 8. A method for manufacturing a light-emitting device according to claim 7.
The method for manufacturing a light emitting device according to any one of claims 1 to 8, wherein the phosphor has a volume average particle diameter of 1 µm or more and 50 µm or less.
The method for manufacturing a light emitting device according to any one of claims 1 to 9, wherein the phosphor mixture liquid includes swollen particles.