JP2010283244A - Semiconductor light emitting device, lighting device and image display - Google Patents

Abstract

<P>PROBLEM TO BE SOLVED: To provide a semiconductor light emitting device which has high luminance and light emission efficiency, and maintain them for a long period. <P>SOLUTION: The semiconductor light emitting device includes a semiconductor light emitting element and a substrate having a wiring pattern, and is characterized in that a surface of the substrate and/or wiring pattern right below the semiconductor light emitting element is covered with a light diffuse reflecting material-containing layer, the light diffuse reflecting material having a concentration of 30 to 70 wt.%. <P>COPYRIGHT: (C)2011,JPO&INPIT

Description

  The present invention relates to a semiconductor light emitting device, and an illumination device and an image display device using the same. Specifically, the present invention relates to a semiconductor light emitting device including a semiconductor light emitting element and a substrate having a wiring pattern.

  A semiconductor light-emitting device is widely used as a display device for home appliances and the like, a lighting device for indoor use, medical use and the like including a portable terminal. A semiconductor light emitting device is configured, for example, by providing a pair of positive and negative electrodes on a substrate provided with a predetermined wiring pattern, and bonding a semiconductor light emitting element (hereinafter also referred to as “LED chip” as appropriate) to the electrodes. Is done. In addition, for example, by including a phosphor in a sealing part such as a silicone resin and placing the phosphor on or around the semiconductor light emitting element, the wavelength of light emitted from the semiconductor light emitting element is converted, It is also possible to emit light having different wavelengths (for example, Patent Documents 1 to 3).

JP-A-11-168235 JP2003-110144A JP 2006-308859 A

However, in the conventional semiconductor light emitting device, the luminance of the semiconductor light emitting device may not be sufficiently increased due to poor reflection efficiency of the metal used for the wiring pattern on the electrode and the substrate. In addition, there are problems such as deterioration of the metal used in the electrodes and wiring patterns due to alkali ion outflow from the phosphor, etc., or deterioration in brightness due to discoloration, etc., and peeling of the sealing part due to these. there were.
In addition, when an insulating material such as ceramic is used as the substrate or the reflective portion, there is a problem that the luminance of the semiconductor light emitting device is not sufficiently increased.

  As a result of intensive studies to solve the above-mentioned problems, the present inventors have identified a substrate directly below the semiconductor light emitting element and the surface of the wiring pattern in a semiconductor light emitting device including a semiconductor light emitting element and a substrate having a wiring pattern. It has been found that the brightness of the semiconductor light-emitting device can be increased by covering with the light diffusive reflecting material-containing layer, and the brightness of the semiconductor light-emitting device can be maintained over a long period of time, and the present invention has been completed.

  That is, the gist of the present invention is that in a semiconductor light emitting device including a semiconductor light emitting element and a substrate having a wiring pattern, the substrate and / or the surface of the wiring pattern immediately below the semiconductor light emitting element has a concentration of a light diffusing reflector. Is coated with a light diffusive reflector-containing layer of 30 wt% or more and 70 wt% or less.

  Another aspect of the present invention is a semiconductor light emitting device including a semiconductor light emitting element and a substrate having a wiring pattern, wherein the substrate and / or the surface of the wiring pattern immediately below the semiconductor light emitting element is a light diffusing reflector. The semiconductor light emitting device is characterized in that it is coated with a light diffusing reflector containing layer having a concentration of 10 volume% or more and 40 volume% or less.

In any of the above semiconductor light emitting devices, the light diffusing reflector is preferably a metal oxide or a metal nitride.
Moreover, it is preferable that the average center particle diameter of this light-diffusion reflection material is 50 nm or more and 5000 nm or less, and it is preferable that the refractive index of this light-diffusion reflection material is 1.5 or more and 3.0 or less.
In addition, it is preferable that the semiconductor light emitting element is disposed on the substrate in a flip chip type.

  Moreover, it is preferable that this light-diffusion reflection material content layer contains a silicone resin. Furthermore, it is preferable that the reflectance of the light diffusing reflector containing layer covering the wiring pattern is 70% or more. Further, it is preferable that the semiconductor light emitting device has an emission wavelength between ultraviolet and near ultraviolet.

  Another gist of the present invention resides in an illumination device characterized by using the above-described semiconductor light emitting device as a light source.

  Furthermore, another gist of the present invention is an image display device comprising: a light source including the above-described semiconductor light-emitting device; and a display panel including an optical shutter that is irradiated with light from the light source. Exist.

  According to the present invention, the light diffusing and reflecting material-containing layer covers the substrate and the wiring pattern directly under the semiconductor light emitting element. Therefore, the light diffuse reflection material-containing layer can diffusely reflect light from the semiconductor light emitting element, and the light emission efficiency and luminance of the semiconductor light emitting device can be increased. Furthermore, the light-diffusing reflector-containing layer can provide a semiconductor light-emitting device in which the light emission efficiency and luminance do not decrease even when used for a long time, and it is possible to obtain a lighting device or an image display device that has high luminance over a long period of time. It becomes possible.

It is a schematic sectional drawing for demonstrating the structure of the semiconductor light-emitting device of this invention. It is a schematic sectional drawing for demonstrating the structure of the semiconductor light-emitting device of this invention. It is a schematic sectional drawing for demonstrating the structure of the semiconductor light-emitting device of this invention. It is a schematic sectional drawing for demonstrating the structure of the semiconductor light-emitting device of this invention. It is a graph which shows the relationship between the light-diffusion reflection material density | concentration in the light-diffusion reflection material content layer, and light extraction efficiency in the Example and comparative example of this invention. It is a graph which shows the brightness | luminance maintenance factor with time with respect to the initial stage brightness of Example 1 and Comparative Example 3. It is a simulation result of the relationship between the refractive index of the light diffusive reflector in the light diffusive reflector containing layer, and light extraction efficiency. It is a simulation result of the relationship between the particle size and refractive index of the light diffusion reflection material in the light diffusion reflection material containing layer, and the light extraction efficiency.

  Hereinafter, the present invention will be described in detail. However, the present invention is not limited to the following embodiments, and various modifications can be made without departing from the scope of the invention.

[1] Semiconductor Light-Emitting Device The semiconductor light-emitting device according to the present invention has at least one semiconductor light-emitting element, a substrate having a wiring pattern, a substrate directly under the light-emitting element and / or a light diffusing reflector-containing layer that covers the wiring pattern. Is.
That is, for example, as shown in FIG. 1, the semiconductor light emitting device 10 of the present invention covers a substrate 11 having a wiring pattern 12, a semiconductor light emitting element 13, and a substrate 11 and / or a wiring pattern 12 immediately below the semiconductor light emitting element 13. And a light diffusing and reflecting material containing layer 21.
The semiconductor light emitting device of the present invention may have members other than those described above as long as the objects and effects of the present invention are not impaired, and as shown in FIG. 15 is preferable. Moreover, you may have other layers, such as an insulating layer, for example between the board | substrate 11 and the semiconductor light-emitting element 13 as needed. The preferred structure of the semiconductor light emitting device of the present invention will be described in detail later.

Here, the semiconductor light emitting device of the present invention may be (A) one that uses the light emission color of the semiconductor light emitting element as it is, and (B) a member that contains a phosphor or a fluorescent component in the vicinity of the semiconductor light emitting element. The phosphor and the fluorescent component in the member may be excited by light from the semiconductor light emitting element, and light having a desired wavelength may be emitted using fluorescence. When the semiconductor light emitting device of the present invention emits light of a desired wavelength using (B) fluorescence, the sealing portion contains a phosphor that is excited by light from the semiconductor light emitting element. It is preferable.
Hereinafter, each member which comprises a semiconductor light-emitting device is demonstrated in detail.

[1-1] Semiconductor Light Emitting Element The semiconductor light emitting element in the semiconductor light emitting device of the present invention may emit light of any wavelength from the ultraviolet wavelength region to the infrared wavelength region. In the case of using the above-described (B) fluorescence, one that emits light that excites a phosphor or a fluorescent component (hereinafter also simply referred to as “phosphor”) is used. In this case, the emission wavelength of the semiconductor light emitting element is not particularly limited as long as it overlaps with the absorption wavelength of the phosphor, and a semiconductor light emitting element having a wide emission wavelength region can be used. In the present invention, it is particularly preferable to use a semiconductor light emitting element having an emission wavelength between blue and the near ultraviolet region, preferably between the ultraviolet and the near ultraviolet region.

  The specific numerical value of the peak emission wavelength of light emitted from the semiconductor light emitting device is usually 350 nm or more, preferably 380 nm or more, preferably 500 nm or less, more preferably 430 nm or less, and further preferably 420 nm or less. As the semiconductor light emitting element, specifically, a light emitting diode (hereinafter appropriately referred to as “LED”), a semiconductor laser diode (hereinafter appropriately referred to as “LD”), or the like can be used.

Among these, GaN-based LEDs and LDs in which a GaN-based compound semiconductor layer is formed on a substrate are preferable as the semiconductor light emitting device. This is because GaN-based LEDs and LDs have significantly higher light emission output and external quantum efficiency than SiC-based LEDs that emit light in this region, and are extremely bright with very low power when combined with the phosphor. This is because light emission can be obtained. For example, for a current load of 20 mA, GaN-based LEDs and LDs usually have a light emission intensity 100 times or more that of SiC-based. GaN-based LEDs and LDs preferably have an Al _X Ga _Y N light emitting layer, a GaN light emitting layer, or an In _X Ga _Y N light emitting layer. Among the GaN-based LEDs, those having an In _X Ga _Y N light emitting layer are particularly preferable because the light emission intensity is very strong. Of the GaN-based LDs, those having a multiple quantum well structure of an In _X Ga _Y N layer and a GaN layer are particularly preferred because the emission intensity is very strong.

  In the above, the value of X + Y is usually a value in the range of 0.8 to 1.2. In the GaN-based LED, those in which the light emitting layer is doped with Zn or Si or those without a dopant are preferable for adjusting the light emission characteristics.

As a GaN-based LED, these light emitting layer, p layer, n layer, electrode, and substrate for a semiconductor light emitting element can be used as basic components, and the light emitting layer is made of n-type and p-type Al _X. Those having a heterostructure sandwiched between Ga _Y N layers, GaN layers, In _X Ga _Y N layers, etc. have high luminous efficiency, and those having a hetero structure in a quantum well structure emit light. Higher efficiency and more preferable.

  In addition, the semiconductor light emitting device used in the present invention has a power consumption during operation of usually 5 W or less, preferably 4 W or less, more preferably 3 W or less, usually 0.060 W or more, preferably 0.065 W or more. More preferably, it is 0.070 W or more. If the amount of power during operation is too small, the light output tends to decrease overall, which tends to be disadvantageous in terms of cost, and if it is too large, heat dissipation becomes difficult, and phosphors, sealing parts, semiconductor light emitting elements, etc. are thermally deteriorated. Failure due to electrode migration may be induced. Moreover, the lifetime of the obtained semiconductor light-emitting device may be shortened by these.

  In the semiconductor light emitting device, when the semiconductor light emitting device substrate is made of a conductive material such as SiC or GaN, for example, a single electrode (single wire bonding) may be used. When the semiconductor light emitting element substrate is made of a low refractive index insulating material such as sapphire, for example, the light emitting layer is the upper surface and the semiconductor light emitting element substrate is the lower surface, and is bonded to the substrate to be described later. A structure in which n2 electrodes are provided and bonded to the substrate with a gold wire or the like (double wire bonding), or the light emitting layer is the lower surface and the substrate side for the semiconductor light emitting element is the upper surface, and is bonded to a substrate to be described later with a gold bump or the like (flip) Chip bonding) configuration and the like, and any configuration is preferable.

  Among them, the latter flip chip bonding is particularly preferable because it has high light extraction efficiency and is space-saving because it is directly bonded to the subpad, so that high integration is easy and a reflective member can be easily provided under the semiconductor light emitting element. Depending on the purpose of use of the semiconductor light emitting device, the ratio of light emitted toward the upper surface and side surface of the semiconductor light emitting device can be controlled by the cut shape of the upper surface and side surface of the semiconductor light emitting device. For example, by cutting the side surface of the semiconductor light emitting element into a shape that suppresses total reflection of light emitted from the light emitting layer, the ratio of the light emitted toward the side surface increases and the light extraction efficiency is improved.

[1-2] Substrate The substrate in the semiconductor light-emitting device of the present invention is not particularly limited as long as it has a wiring pattern. For example, a substrate in which printed wiring is applied on an insulating substrate. Can do. Further, for example, not only the wiring pattern but also a reflecting member, a heat radiating member, or the like may be formed on the substrate.

(substrate)
Examples of the insulating substrate include a ceramic substrate, a resin substrate, a glass epoxy substrate, and the like. In particular, in order to efficiently dissipate heat generated by the semiconductor light emitting device, a high heat dissipation substrate is preferable. For example, a ceramic substrate such as alumina or aluminum nitride can be suitably used.
In addition, the shape of the substrate is not limited to a flat plate shape, and various shapes may be adopted according to the type and application of the semiconductor light emitting device, as will be described later in the section of the structure of the semiconductor light emitting device. Can do.

In addition, a reflective member for reflecting light emitted from the semiconductor light emitting element may be formed on the substrate. The reflecting member is not particularly limited in its formation position and shape as long as it does not impair the object and effect of the present invention. The reflective member may be, for example, a layer made of a metal printed at the same time as a wiring pattern described later, or a metal such as ceramic, silver, or aluminum, or Kovar, an alloy such as silver-platinum or silver-palladium, or white. It may be a layer made of a solder resist or the like. These may be used in combination.
Furthermore, a heat radiating member for radiating heat generated from the semiconductor light emitting element may be formed on the substrate. The heat radiating member may be, for example, a layer made of a metal such as copper or aluminum, or may be a resin in which a high heat radiating metal or a ceramic filler is dispersed at a high density.

  In the present invention, even if a ceramic or the like is used as a substrate or a reflection member, for example, a light diffusing reflective material-containing layer to be described later covers a base material or a wiring pattern. It becomes possible to make the brightness | luminance of an apparatus sufficient.

(Wiring pattern)
The wiring pattern is not particularly limited as long as it is formed on the substrate, and is appropriately selected according to the type and purpose of the semiconductor light emitting device. In the present invention, the wiring pattern includes electrodes, bumps, and the like formed on the substrate, and these may be covered with, for example, a light diffusing reflector containing layer described later.

In the present invention, it is preferable that the material used for the wiring pattern has a high reflectance. Specifically, the reflectance of light having a wavelength of 400 nm is preferably 70% or more, more preferably 75% or more, and further preferably 80% or more. Thereby, the brightness | luminance of a semiconductor light-emitting device can be made favorable. However, in the region covered with the light diffusing reflector-containing layer immediately below the semiconductor light emitting element, even if the reflectance of the wiring pattern material is below the above range, the light diffusing reflector-containing layer covering this will be described later. Since it has the reflectance of the range, the brightness | luminance of a semiconductor light-emitting device can be made favorable.
The method of measuring the reflectance is preferably a method that uses an integrating sphere or the like to include both regular reflection light and diffuse reflection light. For example, the reflectance can be measured using a spectrocolorimeter CM2600d manufactured by Konica Minolta Sensing Co., Ltd. I can do it.

  Moreover, as a material used for a wiring pattern, gold | metal | money, silver, copper, aluminum etc. are mentioned normally, Gold | metal | money, silver, copper are especially preferable from the surface that the brightness | luminance improvement by this invention and the maintenance effect of a brightness | luminance are easy to be obtained. These may use only 1 type and may use it in combination of 2 or more type.

[1-3] Light Diffuse Reflecting Material Containing Layer In the semiconductor light emitting device of the present invention, the substrate and / or the wiring pattern immediately below the semiconductor light emitting element is covered with a specific light diffusing reflecting material containing layer. That is, only one of the above-described substrate and wiring pattern may be covered with the light diffusing and reflecting material-containing layer, or both may be covered. Further, the light diffusing and reflecting material-containing layer may cover the entire region of the substrate or the wiring pattern, or may cover only a partial region. In particular, for the purpose of improving luminance by light diffuse reflection, it is preferable that all regions immediately below the semiconductor light emitting element are covered with a light diffuse reflector containing layer.

  Here, the substrate and / or wiring pattern immediately below the semiconductor light emitting element refers to a substrate and / or wiring pattern in a region where the semiconductor light emitting element is stacked. Note that even when another layer such as an insulating layer is formed between the semiconductor light emitting element and the substrate, or when there is a gap, a region where the semiconductor light emitting element is stacked, that is, other layers A region that is stacked with a semiconductor light emitting element through a layer or a gap is directly under the semiconductor light emitting element.

In the present invention, the light diffusive reflecting material-containing layer satisfies the following conditions (1) or (2), or both, in the content of the light diffusing reflective material.
(1) The concentration of the light diffusing reflector in the light diffusing reflector containing layer is 30% by weight or more and 70% by weight or less.
(2) The density | concentration of the light-diffusion reflection material in a light-diffusion reflection material content layer is 10 volume% or more and 40 volume% or less.

  The weight% concentration of the light diffusing reflector contained in the light diffusing reflector containing layer is usually 30% by weight or more, preferably 35% by weight or more, and more preferably 40% by weight or more. Moreover, it is 70 weight% or less normally, Preferably it is 60 weight% or less, More preferably, it is 50 weight% or less. If the concentration is higher than this value, the concealability is too high and the brightness may decrease or the viscosity may be high, making it difficult to apply. If the concentration is low, the effect of diffuse reflection may be too small to improve the brightness. There is sex.

  The volume% concentration of the light diffusing reflector contained in the light diffusing reflector containing layer is usually 10% by volume or more, and more preferably 15% by volume or more. Moreover, it is 40 volume% or less normally, More preferably, it is 30 volume% or less. If the concentration is higher than this value, the concealability is too high and the brightness may decrease or the viscosity may be high, making it difficult to apply. If the concentration is low, the effect of diffuse reflection may be too small to improve the brightness. There is sex.

(Light diffuse reflector)
The light diffusing reflector is not particularly limited as long as it diffuses and reflects the light incident on the light diffusing reflector containing layer and does not impair the object and effect of the present invention. It is preferable that the light emission wavelength is less absorbed.
Specifically, a metal oxide or a metal nitride is preferable as the light diffusing reflector. This is because the light extraction efficiency of the semiconductor light emitting device provided with the light diffusive reflecting material-containing layer can be improved because the refractive index is high and the reflectance is high. Furthermore, since these materials usually have a higher refractive index than a binder resin or the like, which will be described later, the above effects are easily obtained.

  Examples of the metal oxide include zirconium oxide, titanium oxide, aluminum oxide, zinc oxide, magnesium oxide, etc. Among them, zirconium oxide, titanium oxide, and aluminum oxide are preferable, and oxidation is possible because there is little absorption of ultraviolet to blue light. Zirconium and aluminum oxide are particularly preferred. Examples of the metal nitride include gallium nitride and silicon nitride. Among these, gallium nitride is preferable. Since these have a high refractive index and a high reflectance, the effects of the present invention are easily obtained. Metal oxynitrides are also preferred. These may use only 1 type and may use it in combination of 2 or more type.

  The average center particle diameter of the light diffusing reflector is usually 50 nm or more, preferably 70 nm or more, and more preferably 100 nm or more. Moreover, it is 5000 nm or less normally, Preferably it is 3000 nm or less, More preferably, it is 1000 nm or less. This is because, within the above range, the light diffusive reflection effect can be sufficiently secured. The average center particle size can be obtained from a weight-based particle size distribution curve. The weight-based particle size distribution curve is a value obtained by measuring the particle size distribution by a laser diffraction / scattering method.

  Further, the refractive index of the light diffusive reflector is preferably 1.5 or more, more preferably 1.7 or more, and further preferably 2.0 or more. Moreover, it is preferable that it is 3.0 or less, More preferably, it is 2.9 or less, More preferably, it is 2.8 or less. It is because a refractive index can be made higher than binder resin by being in the said range, and the reflectance of a light-diffusion reflection material can be made high. The refractive index can be measured using a sodium D-line wavelength (at 587.56 nm using an ellipsometer, Abbe refractometer, prism coupler refractometer, etc. If only a powder sample is obtained, the sodium D-line wavelength can be measured. It can also be measured by a liquid immersion method using a refractive liquid with a known refractive index valued by the refractive index at.

  In addition, there is no restriction | limiting in particular in the method of mixing a light-diffusion reflection material with the binder resin etc. which are mentioned later, For example, it can mix, defoaming using a planetary stirring mixer etc. Further, for example, when mixing a light scattering reflector of small particles, it may be mixed using a bead mill or a three roll as required after mixing the particles.

(Binder resin)
The light diffusive reflective material-containing layer can usually contain a binder resin in addition to the light diffusive reflective material. Examples of the binder resin include a thermosetting resin and a photocurable resin.

Specific examples of such binder resins include silicone resins, epoxy resins, (meth) acrylic resins such as poly (meth) methyl acrylate; styrene resins such as polystyrene and styrene-acrylonitrile copolymers; polycarbonate resins; polyester resins Phenoxy resin; butyral resin; polyvinyl alcohol; cellulose resin such as ethyl cellulose, cellulose acetate, cellulose acetate butyrate; phenol resin and the like. These may use only 1 type and may use it in combination of 2 or more type.
In the present invention, it is particularly preferable to include a silicone resin excellent in heat resistance and light resistance. Since the light diffusive reflective material-containing layer is disposed directly under the semiconductor light emitting device, the binder resin contains a silicone resin so that the binder resin can be colored, shrunk, cracked, and peeled by the high-density heat and light emitted from the light emitting device. It can be reduced.

  As a specific example of the silicone resin, a silicone resin used as a sealing member of a sealing portion to be described later can be given. The content of the silicone resin is preferably 30% by weight or more, more preferably 40% by weight or more, and still more preferably 50% by weight or more in the light diffusing / reflecting material-containing layer. Moreover, it is preferable that it is 70 weight% or less, More preferably, it is 65 weight% or less, More preferably, it is 60 weight% or less. If the binder resin is increased, the effect of diffuse reflection may be too small to improve the luminance. On the other hand, if the amount is less than this, the concealability may become too high, resulting in a decrease in luminance or a high viscosity that makes it difficult to apply.

(Glass)
The light diffusing and reflecting material-containing layer may be made of low-melting glass or sol-gel glass instead of the binder resin. By containing glass, the light diffusive reflector-containing layer can obtain high heat dissipation, light resistance, and the like. Among these, sol-gel glass is particularly preferable because it can be easily applied and cured at a temperature lower than the heat resistant temperature of the semiconductor light-emitting element, and can easily reduce the viscosity of the coating solution for forming a light diffusing reflector-containing layer. In addition, in order to adjust the degree of cross-linking and reduce brittleness, cracks, peeling, for example, a methyl group or a phenyl group may be introduced into the glass, and when these are introduced, from the viewpoint of heat resistance, light resistance, etc. It is preferable to introduce mainly a methyl group.
The content of the glass is usually 35% by weight or more, more preferably 45% by weight or more, and further preferably 55% by weight or more in the light diffusing / reflecting material-containing layer. Moreover, it is preferable that it is 75 weight% or less, More preferably, it is 70 weight% or less, More preferably, it is 65 weight% or less.

(Die bond agent)
Further, when the semiconductor light emitting element is of a wire bonding type, the light diffusing and reflecting material-containing layer may function as a white die bonding agent. The light diffusive reflective material-containing layer functions as a die bond agent, so that the semiconductor light emitting element is firmly adhered to the substrate and acts as a layer that diffusely reflects incident light, improving the brightness of the semiconductor light emitting element and maintaining the luminance over a long period of time. Can be maintained.

(Characteristics of light diffusive reflective material containing layer)
The film thickness of the light diffusing and reflecting material-containing layer is usually preferably 5 μm or more, more preferably 10 μm or more, and further preferably 15 μm or more. Moreover, it is 30 micrometers or less normally, More preferably, it is 25 micrometers or less, More preferably, it is 20 micrometers or less. By setting it to the lower limit value or more, the reflectance of the light diffusing reflector-containing layer can be made favorable. Moreover, by setting it as the upper limit value or less, the semiconductor light emitting device can be made thin, and the illumination and image display device using this as a light source can be miniaturized.

  Further, the reflectance of the light diffusing reflector-containing layer covering the wiring pattern formed on the substrate, that is, the reflectance of the light diffusing reflector-containing layer laminated with the wiring pattern is usually 70% or more. , Preferably 75% or more, more preferably 80% or more. By setting it within the above range, the luminance of the semiconductor light emitting device can be improved. The method for measuring the reflectance is preferably a method that uses an integrating sphere or the like to include diffusely reflected light as well as regular reflected light. For example, the reflectance can be measured using a spectrocolorimeter CM2600d manufactured by Konica Minolta Sensing Co., Ltd.

(Method for forming light diffusive reflective material-containing layer)
The method for forming the light diffusing reflector-containing layer is not particularly limited as long as the light diffusing reflector-containing layer can be formed so as to cover the surface of the substrate and / or the wiring pattern immediately below the semiconductor light emitting element. Absent. For example, a method of applying the light diffusion reflection material-containing coating solution for forming the light diffusion reflection material-containing layer containing the light diffusion reflection material or a binder resin by a general application method may be used.

  In the present invention, in particular, there is a method in which after the semiconductor light emitting element is flip-chip mounted at a predetermined position of the substrate, the above-described coating liquid for forming a light diffusing reflector containing layer is applied onto the substrate in the vicinity of the semiconductor light emitting element. preferable. As a result, the coating liquid for forming the light diffusive reflector-containing layer can enter between the substrate of the semiconductor light emitting element and the wiring pattern provided on the substrate by a capillary phenomenon, and light diffuse reflection can be easily performed. A material-containing layer can be formed. In addition, the coating liquid for forming the light diffusive reflecting material-containing layer is cured by heat, light, or the like as necessary. The curing method is appropriately selected according to the type of the binder resin described above. Curing of the coating liquid for forming the light diffusive reflecting material-containing layer may be performed before coating a coating liquid for forming a sealing portion described later, or may be cured simultaneously with the coating liquid. For example, when the binder resin is a UV curable type, it is preferably photocured before applying a coating liquid for forming a sealing portion, and when the binder resin is a thermosetting type, It may be cured before the coating solution, or may be cured at the same time.

  The coating liquid for forming a light diffusive reflecting material-containing layer may contain a solvent, an additive, or the like as necessary.

[1-4] Sealing Part The sealing part used in the semiconductor light emitting device of the present invention is a member for sealing the semiconductor light emitting element, and contains a sealing member.
In the present invention, the sealing portion may be a transparent light-guiding layer containing a thixotropic agent, a refractive index adjusting agent, or a light diffusing agent as necessary, and further absorbs the emission wavelength of the light-emitting element and converts it to an arbitrary wavelength. Or it is good also as a fluorescent substance containing layer for containing organic fluorescent substance and mixing the luminescent color of the light transmitted from a light source (semiconductor light emitting element), and the luminescent color of fluorescent substance, and obtaining a desired luminescent color.

  For example, as one embodiment of the sealing part, the sealing part can be a single-layer phosphor-containing layer containing at least one, preferably plural kinds of phosphors. These phosphors are contained in the phosphor-containing layer uniformly or with a continuous concentration distribution.

  In still another embodiment, the sealing portion contains substantially no phosphor, and the phosphor emits light emitted from the semiconductor light emitting device without changing the wavelength of light from the semiconductor light emitting device. It can be set as the multilayered structure which laminated | stacked the light guide layer led to a fluorescent substance containing layer and the above-mentioned fluorescent substance containing layer. Thus, by interposing the light guide layer between the semiconductor light-emitting element and the phosphor-containing layer, the phosphor is made to be a semiconductor compared to a semiconductor light-emitting device having a single layer structure in which the semiconductor light-emitting element is directly covered with the phosphor-containing layer. It can be arranged away from the light emitting element. As a result, deterioration of the phosphor due to ultraviolet rays can be reduced, and a semiconductor light emitting device having a stable function for a long time can be obtained. In addition, since the light guide layer substantially does not contain a phosphor, even if the temperature of the light guide layer rises due to heat generation of the semiconductor light emitting element, the influence on the phosphor is small. Therefore, deterioration of the phosphor due to temperature can also be suppressed.

  The phosphor-containing layer contains a plurality of types of phosphors having different emission colors (emission wavelength peaks), and in particular, the phosphors are unstable with respect to electricity, heat, and light under lighting use conditions. When the phosphor is included, a layer structure in which only the specific phosphor is separated from the semiconductor light emitting element and another stable phosphor is disposed in the vicinity of the semiconductor light emitting element may be employed.

(Sealing member)
The sealing member used for the sealing portion is not particularly limited, and a curable material that can be molded over the semiconductor light emitting element can be used. The curable material is a fluid material that is cured by performing some kind of curing treatment. Here, the fluid state means, for example, a liquid state or a gel state.
The sealing member is not particularly limited as long as it can seal the semiconductor light emitting device, but preferably has the following characteristics.

1) When the surface in contact with the semiconductor light emitting element and / or the sealing portion has a multilayer structure, it contains a polar group at the interface with other layers,
2) Hardness is 5 or more and 100 or less in Shore A, or 0 or more and 85 or less in Shore D, and 3) It has a siloxane bond.

  Hereinafter, these characteristics 1) to 3) will be described. As described above, when the sealing portion has a multilayer structure including the phosphor-containing layer and the light guide layer, the phosphor-containing layer is sealed in the same manner as the light guide layer, as will be described in detail later. Members can be included.

-Characteristic 1): Polar group The sealing member used in the present invention has a polar group at the surface in contact with the semiconductor light emitting element and / or the interface with other adjacent layers when the sealing part has a multilayer structure. It is preferable to contain. That is, it is preferable that the sealing member contains a compound having the polar group so that the adhesive interface has a polar group. Although there is no restriction | limiting in the kind of such a polar group, For example, a silanol group, an amino group, its derivative group, an alkoxy silyl group, a carbonyl group, an epoxy group, a carboxy group, a carbinol group (-COH), a methacryl group, cyano Group, sulfone group and the like. Note that the sealing member may contain only one of the above polar groups, or may contain two or more polar groups in any combination and ratio.

  Thus, when a sealing member has a polar group in an adhesion interface, a sealing member, a light-diffusion reflection material content layer, a semiconductor light emitting element, and a board | substrate adhere | attach strongly. When the sealing member has a laminated structure, the two layers are in close contact with each other, and it is advantageous that peeling on the laminated surface due to overcoating hardly occurs.

  The polar group contained in the sealing member according to the present invention is capable of hydrogen bonding with a predetermined functional group (for example, hydroxyl group, oxygen in a metalloxane bond, etc.) present on the surface of a resin such as polyphthalamide, ceramic or metal. And can exhibit high adhesion. As described above, the substrate is made of, for example, resin, ceramic, metal, or the like. Moreover, a hydroxyl group usually exists on the surface of ceramic or metal. On the other hand, the sealing member usually has a functional group capable of hydrogen bonding with the hydroxyl group. Therefore, the adhesion of the sealing portion to the substrate can be made excellent by the hydrogen bond.

The presence or absence of a substantial polar group in the sealing portion can be confirmed by IR (infrared spectroscopy) analysis and NMR (nuclear magnetic resonance).
These polar groups may be included in the sealing portion from the beginning, or may be added later to the surface of the sealing portion by primer application or surface treatment.

Characteristic 2): Hardness measurement value The hardness measurement value is an index for evaluating the hardness of the sealing member used in the present invention, and is measured by the following hardness measurement method.

  The sealing member used in the present invention is preferably a member having a relatively low hardness, preferably a member having an elastomeric shape. That is, in the present invention, a plurality of members having different thermal expansion coefficients, such as a semiconductor light emitting element, a substrate (mounting substrate), and a sealing portion composed of a plurality of layers, are used. When the hardness is low, and preferably exhibits an elastomeric shape, the sealing portion can relieve stress due to expansion and contraction of each member. Therefore, it is possible to provide a semiconductor light emitting device that is less likely to be peeled, cracked, disconnected, or the like during use and is excellent in reflow resistance and temperature cycle resistance.

Specifically, the sealing member has a durometer type A hardness measurement value (Shore A) of usually 5 or more, preferably 7 or more, more preferably 10 or more, and usually 100 or less, preferably 80 or less. Preferably it is 70 or less. By having the hardness measurement value in the above range, the semiconductor light-emitting device having the sealing portion is less likely to generate cracks, and has the advantage of being excellent in reflow resistance and temperature cycle resistance.
When the semiconductor light emitting device is used in a state where it is directly exposed, it is preferable that the material of the sealing portion has a mechanical strength sufficient to prevent the wire from being cut by an external force or the semiconductor light emitting element from being damaged. In this case, the hardness measurement value (Shore D) by durometer type D is usually 0 or more, preferably 7 or more, more preferably 10 or more, and usually 85 or less, preferably 70 or less, more preferably 60 or less. . However, such a high-hardness member may be inferior in reflow resistance and temperature cycle resistance compared to the above-mentioned low-hardness member, so low hardness near the semiconductor light emitting element and wiring, and high hardness in the outer periphery. It is good also as a layer structure using a member. For example, a condensation type silicone material having one or more of the above-described properties 1) to 3) is excellent in adhesiveness, and therefore can be used for a long period of time without delamination as a layer structure.
In addition, when the substrate (mounting substrate) to which the sealing member is applied is a thin substrate such as a flexible substrate, the substrate and the sealing portion may be warped due to curing shrinkage stress due to the lamination of the sealing portion. There is. For this reason, it is preferable that the sealing part is formed of a material having a rubber elasticity of Shore A of 5 or more and 80 or less.

[Hardness measurement method]
The hardness measurement value (Shore A) can be measured by the method described in JIS K6253. Specifically, the measurement can be performed using an A-type rubber hardness meter manufactured by Furusato Seiki Seisakusho.

  On the other hand, the hardness measurement value (Shore D) can be measured by the method described in JIS K6253. Specifically, the measurement can be performed using a D-type plastic hardness meter manufactured by Furusato Seiki Seisakusho.

-Characteristic 3): Siloxane bond In this invention, it is preferable that a sealing member contains a siloxane bond. That is, the sealing portion is preferably formed including a compound having a siloxane bond.

  Examples of the compound having a siloxane bond include a silicon-containing compound described later.

-Other characteristics It is preferable that a sealing part contains the layer (light guide layer) which guides the light emitted from the semiconductor light emitting element efficiently to a fluorescent substance content layer.

  For this reason, the resin contained in the sealing member forming the sealing portion preferably has a light transmittance of 80% or more, more preferably 85% or more at an emission wavelength of 350 nm to 500 nm at a film thickness of 1 mm. It is usually 98% or less.

  Moreover, it is preferable that a sealing member satisfy | fills the above-mentioned characteristics 1) -3). A curable material is preferably used for obtaining these characteristics. Moreover, when forming a sealing part, the above-mentioned curable material may use only 1 type, and may use 2 or more types together by arbitrary combinations and a ratio. As the curable material, any of an inorganic material, an organic material, and a mixture of both can be used.

  As the inorganic material, for example, a solution obtained by hydrolytic polymerization of a solution containing a metal alkoxide, a ceramic precursor polymer or a metal alkoxide by a sol-gel method, or a combination thereof is solidified (for example, a siloxane bond). Inorganic materials having

  On the other hand, examples of the organic material include a thermosetting resin and a photocurable resin. Specific examples include (meth) acrylic resins such as poly (meth) acrylic acid methyl; styrene resins such as polystyrene and styrene-acrylonitrile copolymer; polycarbonate resins; polyester resins; phenoxy resins; butyral resins; Cellulose resins such as cellulose acetate and cellulose acetate butyrate; epoxy resins; phenol resins; silicone resins and the like.

  Conventionally, as a phosphor dispersion material for a semiconductor light emitting device, an epoxy resin has been generally used. However, for example, a semiconductor light emitting device that emits white light excited by ultraviolet or near ultraviolet light when used as a high output semiconductor light emitting device. In the case of an apparatus, it is particularly preferable to use a silicon-containing compound that has little deterioration with respect to light emitted from the semiconductor light emitting element and is excellent in heat resistance.

  A silicon-containing compound is a compound having a silicon atom in the molecule, organic materials such as polyorganosiloxane (silicone-based materials), inorganic materials such as silicon oxide, silicon nitride, and silicon oxynitride, and borosilicates and phosphosilicates. Examples thereof include glass materials such as salts and alkali silicates. Among these, silicone materials are preferable from the viewpoint of transparency, adhesiveness, ease of handling, and the point that the cured product has stress relaxation force. Regarding silicone resins for semiconductor light emitting devices, for example, use as a sealant in JP-A-10-228249, JP-A-2927279, JP-A-2001-36147, etc., and JP-A 2000-123981 to wavelength adjustment coating. The use of is being tried.

[Silicone materials]
The silicone material generally refers to an organic polymer having a siloxane bond as a main chain, and examples thereof include a compound represented by the following formula (1) and / or a mixture thereof.
(R ¹ R ² R ³ SiO _1/2 ) _M (R ⁴ R ⁵ SiO _2/2 ) _D (R ⁶ SiO _3/2 ) _T (SiO _4/2 ) _Q Formula (1)

In the formula (1), R ¹ to R ⁶ represent those selected from the group consisting of an organic functional group, a hydroxyl group and a hydrogen atom. R ¹ to R ⁶ may be the same or different.

  In the formula (1), M, D, T, and Q represent a number of 0 or more and less than 1. However, the number satisfies M + D + T + Q = 1.

  When a silicone material is used as the curable material, the semiconductor light emitting element may be sealed using a liquid silicone material and then cured by heat or light.

[Types of silicone materials]
When silicone materials are classified according to the curing mechanism, silicone materials such as an addition polymerization curing type, a condensation polymerization curing type, an ultraviolet curing type, and a peroxide vulcanization type can be generally cited. Among these, addition polymerization curing type (addition type silicone resin), condensation curing type (condensation type silicone resin), and ultraviolet curing type are preferable. Hereinafter, the addition type silicone material and the condensation type silicone material will be described.

(I) Addition-type silicone material The addition-type silicone material refers to a material in which a polyorganosiloxane chain is crosslinked by an organic addition bond. Typical examples include compounds having a Si—C—C—Si bond at the cross-linking point obtained by reacting vinylsilane and hydrosilane in the presence of an addition catalyst such as a Pt catalyst. As these, commercially available products can be used. Specific examples of addition polymerization curing type trade names include “LPS-1400”, “LPS-2410”, and “LPS-3400” manufactured by Shin-Etsu Chemical Co., Ltd.

  Specifically, the addition-type silicone material includes, for example, an alkenyl group-containing organopolysiloxane (A) represented by the following average composition formula (1a) and a hydrosilyl group-containing organo group represented by the following average composition formula (2a). The polysiloxane (B) is mixed with the total alkenyl group of (A) in an amount ratio such that the amount of the total hydrosilyl group of (B) is usually 0.5 to 2.0 times, and a catalytic amount of the addition reaction catalyst (C ) In the presence of.

(A) Alkenyl group-containing organopolysiloxane R _n SiO _{[(4-n) / 2]} (1a)
(In the formula (1a), R is the same or different substituted or unsubstituted monovalent hydrocarbon group, alkoxy group or hydroxyl group, and n is a positive number satisfying 1 ≦ n <2. And at least one of R is an alkenyl group.), An organopolysiloxane having an alkenyl group bonded to at least two silicon atoms in one molecule.

(B) Hydrosilyl group-containing polyorganosiloxane R ′ _a H _b SiO _{[(4-ab) / 2]} (2a)
(In the formula (2a), R ′ is the same or different substituted or unsubstituted monovalent hydrocarbon group excluding the alkenyl group, and a and b are 0.7 ≦ a ≦ 2.1, 0. (A positive number satisfying 001 ≦ b ≦ 1.0 and 0.8 ≦ a + b ≦ 2.6).) Organohydrogen poly having hydrogen atoms bonded to at least two silicon atoms in one molecule Siloxane.

Hereinafter, the addition type silicone resin will be described in more detail.
In R of the above formula (1a), the alkenyl group is an alkenyl group having 2 to 8 carbon atoms such as vinyl group, allyl group, butenyl group or pentenyl group. When R is a hydrocarbon group, it is selected from alkyl groups such as methyl group and ethyl group, monovalent hydrocarbon groups having 1 to 20 carbon atoms such as vinyl group and phenyl group. Preferably, they are a methyl group, an ethyl group, and a phenyl group. Each may be different, but when UV resistance is required, 80% or more of R is preferably a methyl group. R may be an alkoxy group having 1 to 8 carbon atoms or a hydroxyl group, but the content of the alkoxy group or hydroxyl group is preferably 3% or less of the weight of (A).

  n is a positive number satisfying 1 ≦ n <3. If this value is 3 or more, sufficient strength as a sealing portion may not be obtained. The synthesis of siloxane can be difficult.

Next, the organohydrogenpolysiloxane (2a) as the component (B) acts as a crosslinking agent for curing the composition by hydrosilylation reaction with the organopolysiloxane (1a) as the component (A). Composition formula (2a)
R ′ _a H _b SiO _{(4-ab) / 2} (2a)
(In the formula, R ′ is a monovalent hydrocarbon group excluding an alkenyl group, and a and b are 0.7 ≦ a ≦ 2.1, 0.001 ≦ b ≦ 1.0, and 0.8 ≦ a + b ≦ 2.6, preferably 0.8 ≦ a ≦ 2, 0.01 ≦ b ≦ 1, 1 ≦ a + b ≦ 2.4.) at least two in one molecule An organohydrogenpolysiloxane having 3 or more SiH bonds is preferred.

  Here, examples of R ′ include the same groups as R in formula (1a), but those having no alkenyl group are preferable. Further, when used for applications requiring UV resistance, at least 80% is preferably a methyl group.

  The molecular structure of the organohydrogenpolysiloxane may be any of linear, cyclic, branched, and three-dimensional network structures, but the number of silicon atoms in one molecule (or the degree of polymerization) is usually 3 to 3. One of about 1000, preferably about 3 to 300 can be used.

  The blending amount of the organohydropolysiloxane (2a) as the component (B) depends on the total alkenyl group amount of the organopolysiloxane (1a) as the component (A) and is based on the total alkenyl groups of the organopolysiloxane (1a). The total SiH amount is 0.5 times or more, preferably 0.8 times or more, and is usually 2.0 times or less, preferably 1.5 times or less.

  The addition reaction catalyst for component (C) is a catalyst for promoting the hydrosilylation addition reaction between the alkenyl group in component (A) and the SiH group in component (B). Black, platinum chloride, chloroplatinic acid, reaction product of chloroplatinic acid and monohydric alcohol, complex of chloroplatinic acid and olefins, platinum catalyst such as platinum bisacetoacetate, palladium catalyst, rhodium catalyst Platinum group metal catalysts such as In addition, although the compounding quantity of this addition reaction catalyst can be made into a catalytic quantity, it is normally 1 ppm or more normally with respect to the total weight of (A) and (B) component as a platinum group metal, Preferably it is 2 ppm or more. Preferably, it is usually 500 ppm or less, preferably 100 ppm or less.

  In addition to the above components (A) to (C), the addition-type silicone material has an addition reaction control agent for imparting curability and pot life as an optional component, and has, for example, an alkenyl group for adjusting hardness and viscosity. In addition to the linear diorganopolysiloxane, the linear non-reactive organopolysiloxane, the linear or cyclic low-molecular organopolysiloxane having about 2 to 10 silicon atoms, and the like are effective. You may mix in the range which does not impair.

  In addition, although the hardening conditions in particular of the said composition are not restrict | limited, It is preferable to set it as 120 to 180 degreeC and the conditions for 30 minutes to 180 minutes. If the resulting cured product is in a soft gel form after curing, it must be cured at a low temperature near room temperature for 10 to 30 hours because it has a larger coefficient of linear expansion than a rubber resin or hard plastic silicone resin. Therefore, generation of internal stress can be suppressed.

  As the addition-type silicone material, known materials can be used, and an additive or an organic group for improving adhesion to metal or ceramics may be further introduced. For example, silicone materials described in Japanese Patent No. 3909826, Japanese Patent No. 3910080, Japanese Patent Application Laid-Open No. 2003-128922, Japanese Patent Application Laid-Open No. 2004-221308, and Japanese Patent Application Laid-Open No. 2004-186168 are suitable.

(Ii) Condensation type silicone material Examples of the condensation type silicone material include a compound having a Si—O—Si bond obtained by hydrolysis and polycondensation of an alkylalkoxysilane at a crosslinking point. Specific examples include polycondensates obtained by hydrolysis and polycondensation of compounds represented by the following formula (2) and / or (3) and / or oligomers thereof.

M ^{m +} X _n Y ¹ _mn (2)
(In the formula (2), M represents at least one element selected from the group consisting of silicon, aluminum, zirconium, and titanium, X represents a hydrolyzable group, and Y ¹ represents a monovalent group. Represents an organic group, m represents an integer of 1 or more representing the valence of M, and n represents an integer of 1 or more representing the number of X groups, provided that m ≧ n.
_{^{(M s + X t Y 1}} st-1) u Y 2 (3)
(In Formula (3), M represents at least one element selected from the group consisting of silicon, aluminum, zirconium, and titanium, X represents a hydrolyzable group, and Y ¹ represents a monovalent group. Y ² represents an u-valent organic group, s represents an integer of 1 or more representing the valence of M, t represents an integer of 1 or more and s−1 or less, u represents Represents an integer of 2 or more.)

  The condensation type silicone material may contain a curing catalyst. Any curing catalyst can be used as long as the effects of the present invention are not significantly impaired. For example, a metal chelate compound can be suitably used. The metal chelate compound preferably contains one or more selected from the group consisting of aluminum, zirconium, tin, zinc, titanium, hafnium and tantalum, and more preferably contains Zr. In addition, only 1 type may be used for a curing catalyst and it may use 2 or more types together by arbitrary combinations and a ratio.

  Examples of such condensation-type silicone materials include, for example, JP-A-2006-77234, JP-A-2006-291018, JP-A-2006-316264, JP-A-2006-336010, and JP-A-2006-348284. And a member for a semiconductor light emitting device described in International Publication No. 2006/090804 pamphlet are suitable.

  In general, silicone materials often have low adhesion to semiconductor light emitting elements, substrates on which the elements are arranged, packages, and the like. Therefore, it is preferable to use a silicone material having high adhesion as the curable material used in the present invention, and in particular, a condensed silicone material having one or more of the following features <1> to <3>. More preferably, it is used.

<1> The silicon content is 20% by weight or more.
<2> The solid Si-nuclear magnetic resonance (NMR) spectrum measured by the method described in detail later has at least one peak derived from Si in the following (a) and / or (b).

  (A) A peak whose peak top position is in the region of chemical shift of −40 ppm or more and 0 ppm or less with respect to dimethylsilicone rubber, and the peak half-value width is 0.3 ppm or more and 3.0 ppm or less.

  (B) A peak whose peak top position is in a region where the chemical shift is −80 ppm or more and less than −40 ppm with respect to dimethylsilicone rubber, and the half width of the peak is 0.3 ppm or more and 5.0 ppm or less.

  <3> The silanol content is 0.01% by weight or more and 10% by weight or less.

  In the present invention, among the above features <1> to <3>, a silicone material having the feature <1> is preferable. More preferably, a silicone material having the above characteristics <1> and <2> is preferable. Particularly preferably, a silicone material having all of the above features <1> to <3> is preferable. Hereinafter, the features <1> to <3> will be described.

[Feature <1> (silicon content)]
The silicon content of the silicone material suitable in the present invention is usually 20% by weight or more, preferably 25% by weight or more, and more preferably 30% by weight or more. On the other hand, the upper limit is usually in the range of 47% by weight or less because the silicon content of the glass composed solely of SiO ₂ is 47% by weight.

  Note that the silicon content of the silicone-based material is calculated based on the results obtained by performing inductively coupled plasma spectroscopy (hereinafter abbreviated as “ICP” as appropriate), for example, using the following method. be able to.

Measurement of silicon content:
Silicone material is baked in a platinum crucible in the air at 450 ° C. for 1 hour, then at 750 ° C. for 1 hour, and at 950 ° C. for 1.5 hours to remove the carbon component, and then a small amount of residue is obtained. Add more than 10 times the amount of sodium carbonate and heat with a burner to melt, cool this, add demineralized water, and adjust the pH to neutral with hydrochloric acid to a few ppm as silicon. ICP analysis is performed.

[Characteristic <2> (Solid Si-NMR spectrum)]
When a solid Si-NMR spectrum of a silicone material suitable for the present invention is measured, at least one peak in the peak region of (a) and / or (b) derived from a silicon atom to which a carbon atom of an organic group is directly bonded, Preferably, a plurality of peaks are observed.

  When organized by chemical shift, in the silicone-based material suitable as the curable material used in the present invention, the half width of the peak described in (a) is generally the same as that in (b) above because the molecular motion is small. It is smaller than the peak described, and is usually 3.0 ppm or less, preferably 2.0 ppm or less, and usually 0.3 ppm or more.

  On the other hand, the half width of the peak described in (b) is usually 5.0 ppm or less, preferably 4.0 ppm or less, and usually 0.3 ppm or more, preferably 0.4 ppm or more.

  If the half-value width of the peak observed in the chemical shift region is too large, the molecular motion is constrained and strain is large, cracks are likely to occur, and the member may be inferior in heat resistance and weather resistance. For example, when a large amount of tetrafunctional silane is used, or when a large internal stress is accumulated by rapid drying in the drying process, the full width at half maximum may be larger than the above range.

  In addition, if the half width of the peak is too small, Si atoms in the environment will not be involved in siloxane crosslinking, and heat resistance is higher than substances formed mainly from siloxane bonds, such as examples where trifunctional silane remains in an uncrosslinked state. -It may be a member inferior in weather resistance.

  However, in a silicone material containing a small amount of Si component in a large amount of organic component, good heat resistance / light resistance and coating performance can be obtained even if the peak of the above-mentioned half width range is observed at -80 ppm or more. There may not be.

  The chemical shift value of the silicone material suitable in the present invention can be calculated based on the results of solid Si-NMR measurement using the following method, for example. In addition, analysis of measurement data (half-width or silanol amount analysis) is performed by a method of dividing and extracting each peak by, for example, waveform separation analysis using a Gaussian function or a Lorentz function.

[Solid Si-NMR spectrum measurement]
When performing a solid Si-NMR spectrum about a silicone type material, a solid Si-NMR spectrum measurement and waveform separation analysis are performed on condition of the following. Further, from the obtained waveform data, the half width of each peak is determined for the silicone material.

[Equipment conditions]
Equipment: Chemagnetics Infinity CMX-400 Nuclear Magnetic Resonance Spectrometer
²⁹ Si resonance frequency: 79.436 MHz
Probe: 7.5 mmφ CP / MAS probe Measurement temperature: room temperature Sample rotation speed: 4 kHz
Measurement method: Single pulse method
¹ H decoupling frequency: 50 kHz
²⁹ Si flip angle: 90 °
²⁹ Si 90 ° pulse width: 5.0μs
Repeat time: 600s
Integration count: 128 Observation width: 30 kHz
Broadening factor: 20Hz
Reference sample: Dimethyl silicone rubber

[Feature <3> (silanol content)]
A silicone material suitable as a curable material used in the present invention has a silanol content of usually 0.01% by weight or more, preferably 0.1% by weight or more, more preferably 0.3% by weight or more, and usually It is 10% by weight or less, preferably 8% by weight or less, more preferably 5% by weight or less. By reducing the silanol content, the silanol-based material has excellent performance with little change over time, excellent long-term performance stability, and low moisture absorption and moisture permeability. However, since a member containing no silanol is inferior in adhesion, there exists an optimum range for the silanol content as described above.

  The silanol content of the silicone-based material is measured, for example, by measuring the solid Si-NMR spectrum using the method described in the above section [Measurement of solid Si-NMR spectrum], and the ratio of the peak area derived from silanol to the total peak area. Thus, the ratio (%) of silicon atoms which are silanols in all silicon atoms can be obtained and calculated by comparing with the silicon content analyzed separately.

  In addition, since the silicone material suitable as the curable material used in the present invention contains an appropriate amount of silanol, silanol is hydrogen-bonded to the polar portion present on the surface of the light emitting element or package, and adhesion is exhibited. To do. Examples of the polar part include a hydroxyl group and a metalloxane-bonded oxygen.

  Furthermore, a silicone material suitable in the present invention forms a covalent bond by dehydration condensation with a light-emitting element or a hydroxyl group on the surface of a package by heating in the presence of an appropriate catalyst, thereby further strengthening the adhesion. Sex can be expressed.

  On the other hand, if there is too much silanol, the inside of the system will thicken and it will be difficult to apply, or it will become more active and solidify before the light-boiling components volatilize by heating, leading to increased foaming and internal stress. It may occur and induce cracks.

[Other ingredients]
As long as the effects of the present invention are not significantly impaired, the curable material may be used by further mixing other components with the above-described inorganic material and / or organic material. In addition, only 1 type may be used for another component and it may use 2 or more types together by arbitrary combinations and ratios.

[Inorganic particles]
The curable material may further contain inorganic particles for the purpose of improving optical characteristics and workability and for the purpose of obtaining any of the following effects [1] to [5]. In addition, inorganic particle | grains may use only 1 type and may use 2 or more types together by arbitrary combinations and a ratio.
[1] By making the curable material contain inorganic particles as a light scattering agent, a layer formed of the curable material is used as a scattering layer. Thereby, the light transmitted from the light source can be scattered in the scattering layer, and the directivity angle of the light emitted from the light guide member to the outside can be widened. In particular, by including a light scattering agent in the light guide layer, irradiation from the light emitting element is mitigated in the phosphor-containing layer, so that deterioration of the phosphor can be suppressed.
[2] By containing inorganic particles as a binder in the curable material, it is possible to prevent the occurrence of cracks in the layer formed of the curable material.
[3] By containing inorganic particles as a viscosity modifier in the curable material, the viscosity of the curable material can be increased.
[4] By containing inorganic particles in the curable material, shrinkage of the layer formed of the curable material can be reduced.
[5] By incorporating inorganic particles in the curable material, the refractive index of the layer formed of the curable material can be adjusted, and the light extraction efficiency can be improved.

  However, when inorganic particles are included in the curable material, the effect obtained depends on the type and amount of the inorganic particles.

  For example, ultrafine silica particles having a particle size of about 10 nm, fumed silica (dry silica, such as “manufactured by Nippon Aerosil Co., Ltd., trade names: AEROSIL # 200, RX200, RY200”, “manufactured by Tokuyama Corporation, In the case of “trade name: Leoloseal” etc.), the thixotropic property of the curable material is increased, so that the effect [3] is great.

  In addition, for example, when the inorganic particles are crushed silica or true spherical silica having a particle size of about several μm, there is almost no increase in thixotropic property, and the function as an aggregate of the layer containing the inorganic particles is the center. The effects [2] and [4] are great.

  In addition, for example, when inorganic particles having a particle size of about 1 μm, which has a refractive index different from those of other compounds (such as the inorganic material and / or organic material) used in the curable material, Since the light scattering at the interface increases, the effect [1] is great.

  In addition, for example, the median particle size is usually 1 nm or more, preferably 3 nm or more, and usually 10 nm or less, preferably 5 nm or less, specifically, the emission wavelength or less, having a larger refractive index than other compounds used in the curable material. When the inorganic particles having a particle size of are used, the refractive index can be improved while maintaining the transparency of the layer containing the inorganic particles, and thus the effect [5] is great.

  Accordingly, the type of inorganic particles to be mixed may be selected according to the purpose. Moreover, the kind may be single and may combine multiple types. Moreover, in order to improve dispersibility, it may be surface-treated with a surface treatment agent such as a silane coupling agent.

-Types of inorganic particles Examples of the types of inorganic particles used include inorganic oxide particles such as silica, barium titanate, titanium oxide, zirconium oxide, niobium oxide, aluminum oxide, cerium oxide, yttrium oxide, diamond particles, and nitriding Examples include inorganic nitride particles such as gallium, but other materials can be selected according to the purpose, and the present invention is not limited to these.

  The form of the inorganic particles may be any form such as powder, slurry, etc. depending on the purpose, but if it is necessary to maintain transparency, the refractive index of other materials contained in the layer containing the inorganic particles is set. It is preferable that they are equivalent or added to the curable material as a water-based or solvent-based transparent sol.

-Median particle size of inorganic particles The median particle size of these inorganic particles (primary particles) is not particularly limited, but is usually about 1/10 or less of phosphor particles. Specifically, those having the following median particle diameter are used according to the purpose. For example, if inorganic particles are used as the light scattering material, the median particle size is usually 0.05 μm or more, preferably 0.1 μm or more, and usually 50 μm or less, preferably 20 μm or less. For example, if inorganic particles are used as the aggregate, the median particle diameter is preferably 1 μm to 10 μm. For example, if inorganic particles are used as a thickener (thixotropic agent), the median particle size is preferably 10 to 100 nm. For example, if inorganic particles are used as the refractive index adjuster, the median particle size is preferably 1 to 10 nm.
In the present invention, the inorganic fine particles in the light guide layer act as a light scattering agent in the sealing portion.

-Mixing method of inorganic particles The method of mixing inorganic particles is not particularly limited. Usually, it is recommended to mix while defoaming using a planetary stirring mixer or the like in the same manner as the phosphor. For example, when mixing small particles that tend to aggregate, such as Aerosil, the aggregated particles are crushed using a bead mill or three rolls as necessary after mixing the particles and then large particles that can be easily mixed such as phosphors. You may mix an ingredient.

-Content rate of inorganic particle The content rate of the inorganic particle in a curable material is arbitrary unless the effect of this invention is impaired remarkably, and can be freely selected by the application form. However, the content of the inorganic particles in the layer containing the inorganic particles is preferably selected according to the application form. For example, when inorganic particles are used as the light scattering agent, the content in the layer is preferably 0.01 to 10% by weight. Even when the same light scattering agent is used, when inorganic particles are used to provide a diffuse reflection layer as in the present invention, the content is preferably 10% by weight or more, more preferably 30%, in order to ensure concealment. % By weight or more. Moreover, 70 weight% or less is preferable, More preferably, it is 50 weight% or less.

  For example, when inorganic particles are used as an aggregate, the content in the layer is preferably 1% by weight to 50% by weight. For example, when using inorganic particles as a thickener (thixotropic agent), the content in the layer is preferably 0.1% by weight to 20% by weight. Further, for example, when inorganic particles are used as a refractive index adjusting agent, the content in the layer is preferably 10% by weight to 80% by weight. If the amount of inorganic particles is too small, the desired effect may not be obtained, and if it is too large, various properties such as adhesion, transparency and hardness of the cured product may be adversely affected. Moreover, what is necessary is just to set the content rate of the inorganic particle in a fluid curable material so that the content rate of the inorganic particle in each layer may be settled in the said range. Therefore, when the fluid curable material does not change in weight in the drying step, the content of inorganic particles in the curable material is the same as the content of inorganic particles in each layer to be formed. Also, when the curable material changes in weight in the drying process, such as when the fluid curable material contains a solvent, the content of inorganic particles in the curable material excluding the solvent, What is necessary is just to make it become the same as the content rate of the inorganic particle in each layer formed.

  In addition, the content rate of an inorganic particle can be measured similarly to the content rate of the below-mentioned fluorescent substance.

Further, the sealing portion may be a layer containing a phosphor (phosphor-containing layer).
Examples of the phosphor used in the semiconductor light emitting device of the present invention include the following red, yellow, green, and blue phosphors excited by ultraviolet to blue light, and one or more selected from these are used alone. Or 2 or more types can be used in arbitrary combinations and arbitrary ratios.

但し、上記の母体結晶及び付活元素又は共付活元素は、元素組成には特に制限はなく、同族の元素と一部置き換えることもでき、得られた蛍光体は近紫外から可視領域の光を吸収して可視光を発するものであれば用いることが可能である。 There is no particular limitation on the composition of the phosphor, but a metal oxide represented by Y ₂ O ₃ , YVO ₄ , Zn ₂ SiO ₄ , Y ₃ Al ₅ O ₁₂ , Sr ₂ SiO _4, etc., which becomes a base crystal, Metal nitrides typified by (Ca, Sr) AlSiN _{3 and the} like, phosphates typified by Ca ₅ (PO ₄ ) ₃ Cl and the like, sulfides typified by ZnS, SrS, CaS and the like, Y ₂ O ₂ Rare earth metal ions such as Ce, Pr, Nd, Pm, Sm, Eu, Tb, Dy, Ho, Er, Tm, Yb, Ag, Cu, and the like such as oxysulfides represented by S, La ₂ O ₂ S, etc. , Au, Al, Mn, Sb, and other metal ions may be combined as activators or coactivators. Table 1 shows specific examples of preferred crystal matrixes.
In the illustration of the present invention, phosphors that are different only in part of the structure are omitted as appropriate. For example, “Y ₂ SiO ₅ : Ce ³⁺ ”, “Y ₂ SiO ₅ : Tb ³⁺ ” and “Y ₂ SiO ₅ : Ce ³⁺ , Tb ³⁺ ” are changed to “Y ₂ SiO ₅ : Ce ³⁺ , Tb ³⁺ ”, “ “La ₂ O ₂ S: Eu”, “Y ₂ O ₂ S: Eu” and “(La, Y) ₂ O ₂ S: Eu” are collectively shown as “(La, Y) ₂ O ₂ S: Eu”. ing. Omitted parts are separated by commas (,).

However, the matrix crystal and the activator element or coactivator element are not particularly limited in element composition, and can be partially replaced with elements of the same family, and the obtained phosphor is light in the near ultraviolet to visible region. Any material that absorbs and emits visible light can be used.

  Specifically, the following phosphors can be used, but these are merely examples, and phosphors that can be used in the present invention are not limited to these. In the following examples, as described above, phosphors that differ only in part of the structure are omitted as appropriate.

[Orange to red phosphor]
Any orange or red phosphor that can be used in combination with the phosphor of the present invention can be used as long as the effects of the present invention are not significantly impaired.
At this time, the emission peak wavelength of the orange to red phosphor, which is the same color combination phosphor, is usually 570 nm or more, preferably 580 nm or more, more preferably 585 nm or more, and usually 780 nm or less, preferably 700 nm or less, more preferably 680 nm. It is preferable to be in the following wavelength range.
Table 2 shows phosphors that can be used as orange to red phosphors.

Among these, as red phosphors, (Ca, Sr, Ba) ₂ Si ₅ (N, O) ₈ : Eu, (Ca, Sr, Ba) Si (N, O) ₂ : Eu, (Ca, Sr , Ba) AlSi (N, O) ₃ : Eu, (Sr, Ba) ₃ SiO ₅ : Eu, (Ca, Sr) S: Eu, (La, Y) ₂ O ₂ S: Eu, Eu (dibenzoylmethane) ) ₃ · 1,10-phenanthroline complexes of β- diketone Eu complex, a carboxylic acid Eu _complex, K 2 _SiF 6: Mn is _{preferred, (Ca, Sr, Ba)} 2 Si 5 (N, O) 8: Eu, (Sr, Ca) AlSi (N, O): Eu, (La, Y) ₂ O ₂ S: Eu, and K ₂ SiF ₆ : Mn are more preferable.

As the orange phosphor, (Sr, Ba) ₃ SiO ₅ : Eu, (Sr, Ba) ₂ SiO ₄ : Eu, (Ca, Sr, Ba) ₂ Si ₅ (N, O) ₈ : Eu, ( Ca, Sr, Ba) AlSi (N, O) ₃ : Ce is preferred.

[Blue phosphor]
When using blue fluorescent substance, the said blue fluorescent substance can use arbitrary things, unless the effect of this invention is impaired remarkably. At this time, the emission peak wavelength of the blue phosphor is usually 420 nm or more, preferably 430 nm or more, more preferably 440 nm or more, and usually less than 500 nm, preferably 490 nm or less, more preferably 480 nm or less, more preferably 470 nm or less, It is particularly preferable that the wavelength range is 460 nm or less. When the emission peak wavelength of the blue phosphor used is within this range, it overlaps with the excitation band of the phosphor suitable for the present invention, and the phosphors of other colors are efficiently excited by the blue light from the blue phosphor. Because you can.

以上の中でも、青色蛍光体としては、（Ｃａ，Ｓｒ，Ｂａ）ＭｇＡｌ_１０Ｏ_１７：Ｅｕ、（Ｓｒ，Ｃａ，Ｂａ，Ｍｇ）_１０（ＰＯ_４）_６（Ｃｌ，Ｆ）_２：Ｅｕ、（Ｂａ，Ｃａ，Ｍｇ，Ｓｒ）_２ＳｉＯ_４：Ｅｕ、（Ｓｒ，Ｃａ，Ｂａ，Ｍｇ）_１０（ＰＯ_４）_６（Ｃｌ，Ｆ）_２：Ｅｕ、（Ｂａ，Ｃａ，Ｓｒ）_３ＭｇＳｉ_２Ｏ_８：Ｅｕが好ましく、（Ｂａ，Ｓｒ）ＭｇＡｌ_１０Ｏ_１７：Ｅｕ、（Ｃａ，Ｓｒ，Ｂａ）_１０（ＰＯ_４）_６（Ｃｌ，Ｆ）_２：Ｅｕ、Ｂａ_３ＭｇＳｉ_２Ｏ_８：Ｅｕがより好ましく、Ｓｒ_１０（ＰＯ_４）_６Ｃｌ_２：Ｅｕ、ＢａＭｇＡｌ_１０Ｏ_１７：Ｅｕが特に好ましい。 Table 3 shows phosphors that can be used as such blue phosphors.

Among these, as the blue phosphor, (Ca, Sr, Ba) MgAl ₁₀ O ₁₇ : Eu, (Sr, Ca, Ba, Mg) ₁₀ (PO ₄ ) ₆ (Cl, F) ₂ : Eu, (Ba , Ca, Mg, Sr) ₂ SiO ₄ : Eu, (Sr, Ca, Ba, Mg) ₁₀ (PO ₄ ) ₆ (Cl, F) ₂ : Eu, (Ba, Ca, Sr) ₃ MgSi ₂ O ₈ : Eu is preferred, (Ba, Sr) MgAl ₁₀ O ₁₇ : Eu, (Ca, Sr, Ba) ₁₀ (PO ₄ ) ₆ (Cl, F) ₂ : Eu, Ba ₃ MgSi ₂ O ₈ : Eu is more preferred, Sr ₁₀ (PO ₄ ) ₆ Cl ₂ : Eu, BaMgAl ₁₀ O ₁₇ : Eu are particularly preferable.

[Green phosphor]
When the green phosphor is used, any green phosphor can be used as long as the effect of the present invention is not significantly impaired. At this time, the emission peak wavelength of the green phosphor is preferably in the range of usually 500 nm or more, particularly 510 nm or more, more preferably 515 nm or more, and usually less than 550 nm, especially 542 nm or less, more preferably 535 nm or less. If this emission peak wavelength is too short, it tends to be bluish, while if it is too long, it tends to be yellowish, and the characteristics as green light may deteriorate.

Table 4 shows phosphors that can be used as such green phosphors.

Among these, as the green phosphor, Y ₃ (Al, Ga) ₅ O ₁₂ : Ce, CaSc ₂ O ₄ : Ce, Ca ₃ (Sc, Mg) ₂ Si ₃ O ₁₂ : Ce, (Sr, Ba) ₂ SiO ₄ : Eu, (Si, Al) ₆ (O, N) ₈ : Eu (β-sialon), (Ba, Sr) ₃ Si ₆ O ₁₂ : N ₂ : Eu, SrGa ₂ S ₄ : Eu, BaMgAl ₁₀ O ₁₇ : Eu, Mn is preferred.

When the semiconductor light emitting device of the present invention is used for a lighting device, Y ₃ (Al, Ga) ₅ O ₁₂ : Ce, CaSc ₂ O ₄ : CeCa ₃ (Sc, Mg) ₂ Si ₃ O ₁₂ : Ce, (Sr , Ba) ₂ SiO ₄ : Eu, (Si, Al) ₆ (O, N) ₈ : Eu (β-sialon), (Ba, Sr) ₃ Si ₆ O ₁₂ : N ₂ : Eu are preferable.

When the semiconductor light emitting device of the present invention is used for an image display device, (Sr, Ba) ₂ SiO ₄ : Eu, (Si, Al) ₆ (O, N) ₈ : Eu (β-sialon), ( Ba, Sr) ₃ Si ₆ O ₁₂ : N ₂ : Eu, SrGa ₂ S ₄ : Eu, and BaMgAl ₁₀ O ₁₇ : Eu, Mn are preferable.

[Yellow phosphor]
When a yellow phosphor is used, any yellow phosphor can be used as long as the effects of the present invention are not significantly impaired. At this time, the emission peak wavelength of the yellow phosphor is usually in the wavelength range of 530 nm or more, preferably 540 nm or more, more preferably 550 nm or more, and usually 620 nm or less, preferably 600 nm or less, more preferably 580 nm or less. Is preferred.

The phosphors that can be used as such yellow phosphors are shown in Table 5 below.

More in even, as the yellow _{phosphor, Y 3 Al 5 O 12:} Ce, (Y, Gd) 3 Al 5 O 12: Ce, (Sr, Ca, Ba, Mg) 2 SiO 4: Eu, (Ca, Sr) Si ₂ N ₂ O ₂ : Eu is preferred.

[Other phosphors]
As the phosphor, it is possible to contain a phosphor other than those described above. For example, the phosphor-containing layer itself can be formed of a fluorescent resin in which an ionic fluorescent material or an organic / inorganic fluorescent component is dissolved and dispersed uniformly and transparently.

[Particle size of phosphor]
The particle size of the phosphor is not particularly limited, but is the median particle size (D ₅₀ ) and is usually 0.1 μm or more, preferably 2 μm or more, more preferably 5 μm or more. Moreover, it is 100 micrometers or less normally, Preferably it is 50 micrometers or less, More preferably, it is 20 micrometers or less. When the median particle diameter (D ₅₀ ) of the phosphor is in the above range, the light transmitted from the light source is sufficiently scattered in the phosphor-containing layer. In addition, since the light transmitted from the light source is sufficiently absorbed by the phosphor particles, wavelength conversion is performed with high efficiency, and light emitted from the phosphor is irradiated in all directions. Thereby, primary light from a plurality of types of phosphors can be mixed to obtain a desired color (for example, white), and uniform color and illuminance can be obtained. On the other hand, when the median particle diameter (D ₅₀ ) of the phosphor is larger than the above range, the phosphor cannot sufficiently fill the space of the phosphor-containing layer, so that the light transmitted from the light source is sufficiently contained in the phosphor. It may not be absorbed. Moreover, when the median particle diameter (D ₅₀ ) of the phosphor is smaller than the above range, the luminous efficiency of the phosphor is lowered, and the illuminance may be lowered.

  The particle size distribution (QD) of the phosphor particles is preferably smaller in order to align the dispersion state of the particles in the phosphor-containing layer, but in order to reduce the particle size, the classification yield is lowered and the cost is increased. 0.03 or more, preferably 0.05 or more, more preferably 0.07 or more. Moreover, it is 0.4 or less normally, Preferably it is 0.3 or less, More preferably, it is 0.2 or less.

The median particle size (D ₅₀ ) and particle size distribution (QD) can be determined from a weight-based particle size distribution curve. The weight-based particle size distribution curve is obtained by measuring the particle size distribution by a laser diffraction / scattering method, and specifically, for example, can be measured as follows.

[Measurement method of weight-based particle size distribution curve]
(1) A phosphor is dispersed in a solvent such as ethylene glycol in an environment of a temperature of 25 ° C. and a humidity of 70%.
(2) The particle size distribution is measured in a particle size range of 0.1 μm to 600 μm with a laser diffraction particle size distribution measuring device (LA-300 manufactured by Horiba, Ltd.).
(3) the integrated value in the measured weight particle size distribution curve is denoted a particle size value when the 50% and median particle diameter D _50. Further, the particle diameter values when the integrated values are 25% and 75% are expressed as D ₂₅ and D ₇₅ , respectively, and defined as QD = (D ₇₅ −D ₂₅ ) / (D ₇₅ + D ₂₅ ). A small QD means a narrow particle size distribution.

  Also, the shape of the phosphor particles is arbitrary as long as it does not affect the formation of the phosphor-containing layer, such as the fluidity of the curable material.

[Surface treatment of phosphor]
The phosphor may be subjected to a surface treatment for the purpose of improving water resistance or preventing unnecessary aggregation of the phosphor in the phosphor-containing layer. Examples of such surface treatment include surface treatment using an organic material, an inorganic material, a glass material and the like described in JP-A-2002-223008, and coating with a metal phosphate described in JP-A-2000-96045 and the like. Examples thereof include known treatments such as treatment, coating treatment with metal oxide, and silica coating.

As specific examples of the surface treatment, for example, the following surface treatments (i) to (iii) are performed in order to coat the surface of the phosphor with the metal phosphate.
(I) a predetermined amount of a water-soluble phosphate such as potassium phosphate or sodium phosphate, and at least one of alkaline earth metals such as calcium chloride, strontium sulfate, manganese chloride and zinc nitrate, Zn and Mn The water-soluble metal salt compound is mixed in the phosphor suspension and stirred.
(Ii) The phosphate of at least one metal among alkaline earth metals, Zn and Mn is generated in the suspension, and the generated metal phosphate is deposited on the phosphor surface.
(Iii) Remove moisture.

Moreover, a silica coat is mentioned as a suitable example among the other examples of surface treatment. Silica coating includes a method of precipitating SiO ₂ by neutralizing water glass, a method of surface treating a hydrolyzed alkoxysilane (for example, JP-A-3-231987), etc., and improving dispersibility. In terms of the point, a method of surface-treating a hydrolyzed alkoxysilane is preferable.

[Phosphor mixing method]
There is no particular limitation on the mixing method used when the phosphor particles are contained in the curable material. For example, if the dispersed state of the phosphor particles is good, it only needs to be post-mixed with the above curable material. That is, a layer may be formed by mixing a curable material and a phosphor, preparing a curable material containing the phosphor, and coating the curable material containing the phosphor. Further, for example, when hydrolysis / polycondensation of alkylalkoxysilane is used as a curable material, if the phosphor particles are likely to aggregate in the curable material, a reaction solution containing a raw material compound before hydrolysis ( If appropriate, the phosphor particles are mixed in advance in a “pre-hydrolysis solution” below) and subjected to hydrolysis and polycondensation in the presence of the phosphor particles, and the surface of the phosphor particles is partially silane-coupled, The dispersed state of the phosphor particles is improved.

  Some phosphors are hydrolyzable, but when the above-mentioned alkylalkoxysilane hydrolyzate / polycondensate is used as a curable material, the moisture in the fluid state before coating is silanol. Since it exists potentially as a body and there is almost no free water, such a phosphor can be used without being hydrolyzed. Further, if the curable material after hydrolysis / polycondensation is used after being subjected to dehydration / dealcoholation treatment, there is also an advantage that the combined use with such a phosphor becomes easy.

  In addition, when the hydrolyzate / polycondensate of the above alkylalkoxysilane is used as a curable material and phosphor particles or inorganic particles are contained in the curable material, an organic coating is used on the particle surface to improve dispersibility. It is also possible to perform modification with a ligand. Other addition-type silicone resins are susceptible to curing inhibition by such organic ligands, and there are cases where particles subjected to such surface treatment cannot be mixed and cured. This is because platinum-based curing catalysts used in addition-reactive silicone resins have a strong interaction with these organic ligands, tend to lose hydrosilylation ability and cause poor curing. . Such poisonous substances include organic compounds containing multiple bonds, such as organic compounds containing N, P, S, etc., ionic compounds of heavy metals such as Sn, Pb, Hg, Bi, As, acetylene groups, etc. Amines, vinyl chloride, sulfur vulcanized rubber) and the like. On the other hand, the hydrolysis / polycondensation product of the alkylalkoxysilane is based on a condensation-type curing mechanism that hardly causes inhibition of curing by these poisoning substances. For this reason, the hydrolysis / polycondensation products of the above alkylalkoxysilanes have a high degree of freedom in mixing with fluorescent components such as phosphor particles and inorganic particles whose surface has been modified by organic ligands, and complex phosphors. It is large and has excellent characteristics as a phosphor binder and a transparent material with high refractive index nanoparticles.

[Phosphor content]
The content of the phosphor in the curable material is arbitrary as long as the effects of the present invention are not significantly impaired, and can be freely selected depending on the application form. However, the total amount of the phosphor in the phosphor-containing layer is usually 5% by weight or more, preferably 6% by weight or more, more preferably 7% by weight or more, and usually 30% by weight or less, preferably 25% by weight or less, more Preferably it is 20 weight% or less. The phosphor content in the fluid curable material may be set so that the phosphor content in the phosphor-containing layer falls within the above range. Therefore, when the fluid curable material does not change in weight in the curable material curing step, the phosphor content in the curable material is the same as the phosphor content in the phosphor-containing layer. In addition, when the curable material changes in weight in the curable material curing process, such as when the fluid curable material contains a solvent, the phosphor content in the curable material excluding the solvent, etc. May be the same as the phosphor content in the phosphor-containing layer. In addition, when not only a fluorescent substance content layer but a light guide layer contains a fluorescent substance, the above-mentioned fluorescent substance content rate is a value of the average fluorescent substance content rate in the whole sealing part.

The phosphor content and concentration distribution in the phosphor-containing layer can be calculated from the preparation, and the phosphor-containing layer cured product is chemically dissolved to perform ICP analysis of elements unique to the phosphor, or the cross-section of the cured product It can be obtained by manufacturing and performing image processing after taking a picture. An example of obtaining the density distribution by image processing is shown below.
(1) The phosphor-containing layer is peeled off from the LED and cut with a cutter knife or the like to produce a cross section that can be observed in the depth direction.
(2) The cross section of the phosphor-containing layer is irradiated with black light, and a photograph is taken in a state where the phosphor emits light in each color.
(3) The cross-sectional photograph is processed by image processing software, the image is decomposed for each RGB component to obtain an image in which each phosphor is emphasized, and the number of phosphor particles is counted.
(4) A concentration distribution in the depth direction is obtained.

  When all the light transmitted from the light source is converted into the phosphor emission color to obtain the desired emission color, the emission color of the light transmitted from the light source and the emission color of the phosphor are suppressed in order to suppress excitation light omission. A higher phosphor content is preferred than when obtaining a desired luminescent color by mixing colors. In addition, when multiple small light emitting elements with a high horizontal light distribution ratio are used, the phosphor-containing layer immediately above the light emitting element has a higher density than the single light emitting element with an upward light distribution. The excitation light is difficult to be irradiated. In this case, since it becomes difficult for the light emitting device to pass through the excitation light, the phosphor content immediately above the light emitting element can be made lower than in the case of a single upward light distribution and high output light emitting element. Deterioration of the stop can be reduced. When multiple light-emitting elements with a high lateral emission ratio are installed, the phosphors between the light-emitting elements are exposed to high-density light by the light-emitting elements adjacent to each other. The phosphor arrangement in which the phosphor concentration on the near side is high can reduce the thermal quenching of the phosphor between the light emitting elements and the deterioration due to heat and light. If the phosphor content is more than the above range, the coating performance may be deteriorated, or the utilization efficiency of the phosphor may be lowered due to optical interference action, and the luminance may be lowered. On the other hand, if the phosphor content is less than the above range, wavelength conversion by the phosphor becomes insufficient, and the target emission color may not be obtained.

  However, the content ratio of the phosphor is particularly suitable for obtaining white light. Accordingly, the specific phosphor content varies depending on the target color, the luminous efficiency of the phosphor, the color mixture format, the specific gravity of the phosphor, the coating film thickness, and the shape of the optical member, and is not limited thereto.

[1-5] Configuration of Semiconductor Light-Emitting Device As described above, the semiconductor light-emitting device of the present invention includes a substrate having a wiring pattern, a semiconductor light-emitting element, and a light that covers the substrate and / or the wiring pattern immediately below the semiconductor light-emitting element. The structure is not particularly limited as long as it has at least the diffuse reflection material-containing layer, and can have, for example, a sealing portion.
Hereinafter, preferred structural examples of the semiconductor light emitting device according to the present invention will be described with reference to FIGS. 1 to 4, but the present invention is not limited thereto. 1 to 4 are diagrams for explaining the structure of the semiconductor light emitting device of the present invention, and do not accurately show the scales of the respective members.

  For example, the semiconductor light emitting device 10 shown in FIG. 1 has a wiring pattern 12 formed on a flat substrate 11. The semiconductor light emitting element 13 has an electrode (not shown) arranged on the substrate 11 side. In such a configuration, after the wiring pattern 12 on the substrate 11 and the semiconductor light emitting element 13 are mounted so as to be electrically connected, the light diffusing reflector containing layer 21 containing the light diffusing reflector 22 is made to emit semiconductor light. It can be manufactured by forming between the element 13 and the substrate 11. In such a configuration, it may be mounted using a submount, and the electrode of the semiconductor light emitting element 13 can be electrically connected directly on the wiring pattern 12.

  2 is an example in which a substrate 11 having a shape surrounding the semiconductor light emitting element 13 is used as the substrate 11. In such a configuration, the semiconductor light emitting element 13 is mounted at a predetermined position of the substrate 11 to form the light diffusing and reflecting material containing layer 21. The light diffusing reflector containing layer 21 may be formed before mounting the semiconductor light emitting element 13, but in the case of the flip chip type, as described above, the light diffusing reflector containing layer 21 is utilized by utilizing the capillary phenomenon. The layer 21 is preferably formed. In this case, the light diffusing reflector containing layer 21 is formed after the semiconductor light emitting element 13 is mounted. Thereafter, a curable material for forming the sealing portion 15 is poured into the substrate 11, and the poured curable material is cured to form the sealing portion 15.

  As shown in FIG. 3, the semiconductor light emitting device 10 ″ may include a phosphor 16 in the sealing portion 15 of the semiconductor light emitting device 10 ′ shown in FIG. 2. Further, as shown in FIG. 4, the semiconductor light emitting device 10 ″ ″ includes the sealing portion 15 of the semiconductor light emitting device 10 ′ shown in FIG. 2 including a layer not containing the phosphor 16 and a layer containing the phosphor 16. It can also be used. In addition, the layer containing the phosphor 16 may include a plurality of phosphors in a single layer, and although not illustrated, a plurality of layers may be laminated for each color.

  Moreover, the shape of the sealing portion 15 of the semiconductor light emitting device shown in FIGS. 2 to 4 as described above may be, for example, a dome shape. Further, the sealing portion 15 may be further covered with a visible light transmitting resin (not shown) in a dome shape so as to have a lens function. As the visible light translucent resin, for example, an epoxy resin, a urethane resin, a silicone resin or the like can be used, and among them, an epoxy resin is particularly preferable. These can be used alone or in combination of two or more. Furthermore, you may make visible light translucent resin contain 1 type, or 2 or more types of additives, such as a viscosity modifier, a diffusing agent, and an ultraviolet absorber, in arbitrary ratios and combinations as needed.

[1-6. Characteristics of semiconductor light emitting device]
The semiconductor light emitting device of the present invention can emit light in an arbitrary color by appropriately determining the type and amount of the phosphor used. When using a semiconductor light-emitting device for an illumination device, a semiconductor light-emitting device that emits white light is useful. The light emitting efficiency of the semiconductor light emitting device of the present invention is usually 20 lm / W or more, preferably 22 lm / W or more, more preferably 25 lm / W or more, and particularly preferably 28 lm / W or more. The average color rendering index Ra is 80 or more, preferably 85 or more, more preferably 88 or more.

  The average color rendering index Ra is a numerical value of how much color misregistration occurs when viewed with the reference light defined by JIS. The average value of the color rendering index of the color chart for color rendering evaluation It is represented by The smaller the color shift, the larger the Ra value, and the closer to 100, the better the color rendering. The average color rendering index Ra is calculated according to JIS Z 8726.

  The luminous efficiency is calculated by dividing the total luminous flux (lm) of the semiconductor light emitting device by the power consumption (W) of the device.

  First, in order to maintain the measurement accuracy of the semiconductor light emitting device to be measured, the parts other than the semiconductor light emitting device facing the inside of the integrating sphere (wiring board, heat sink, etc.) are colored with high reflection efficiency, such as white, and integrated. Attach to a spectrophotometer with a sphere. Examples of the spectrophotometer include “USB2000” manufactured by Ocean Optics Co., Ltd. The reason why the integrating sphere is used is to measure and integrate light in all directions emitted from the semiconductor light emitting device, that is, to eliminate light leaking out of the measurement system without being measured.

  Next, this semiconductor light emitting device is turned on, and its emission spectrum and total luminous flux (lm) are measured. The measured spectrum is usually observed when light from the semiconductor light emitting element for excitation leaked from the phosphor-containing layer (hereinafter simply referred to as “excitation light”) and light that has been wavelength-converted by the phosphor overlap. Is done.

  The total luminous flux (lm) can be obtained by integrating the luminous flux for each wavelength in the entire wavelength region where the emission spectrum is observed. The power consumption (W) can be obtained by taking the product of the current (A) flowing through the semiconductor light emitting device and the voltage (V).

  The luminous efficiency defined in the present invention can be obtained by dividing the total luminous flux (lm) obtained as described above by the power consumption (W).

  Today's semiconductor light emitting devices have been devised in various ways for the purpose of increasing the size, increasing the brightness, and reducing the cost. For example, a gold-plated electrode that suppresses electrode migration may be used on the substrate, a heat sink such as copper may be provided to improve heat dissipation, or a substrate material such as aluminum nitride may be used. In order to achieve the above objectives, such as using a resin package that cannot avoid coloring with heat and light in order to reduce costs, it is necessary to select a member with low reflectivity or a member whose reflectivity decreases with time. There are many. The semiconductor light emitting device having the light diffusive reflecting material-containing layer of the present invention can maintain a high luminance and achieve a long life even when a low reflectance member is used in the semiconductor light emitting device.

[2] Illumination device and image display device The application of the semiconductor light-emitting device of the present invention is not particularly limited, and can be used in various fields in which ordinary light-emitting devices are used. Specific examples of uses of the semiconductor light emitting device of the present invention include light sources for various illumination devices such as illumination lamps and thin illuminations, and light sources for image display devices such as liquid crystal displays (backlights, front lights, etc.). Can be mentioned.
The image display device may include a light source including a semiconductor light emitting device and a display panel including an optical shutter such as a liquid crystal panel that receives light from the light source. When the image display device displays a color image, the semiconductor light emitting device of the present invention may be used in combination with a color filter. Moreover, when using the semiconductor light-emitting device of this invention as a light source of an illuminating device or an image display apparatus, a semiconductor light-emitting device may be used independently and you may use it combining several semiconductor light-emitting devices.

  EXAMPLES Hereinafter, although this invention is demonstrated in detail using an Example, this invention is not limited to a following example, unless it deviates from the summary.

[Synthesis Example 1] (Manufacture of sealing member)
Momentive Performance Materials Japan G.K. both ends silanol dimethyl silicone oil XC96-723 385g, methyltrimethoxysilane 10.28g, and zirconium tetraacetylacetonate powder 0.791g as a catalyst, The solution was weighed in a 500 ml three-necked Kolben equipped with a fractionating tube, a Dimroth condenser and a Liebig condenser, and stirred at room temperature for 15 minutes until the coarse particles of the catalyst were dissolved. Thereafter, the temperature of the reaction solution was raised to 100 ° C. to completely dissolve the catalyst, and initial hydrolysis was performed while stirring at 500 rpm for 30 minutes at 100 ° C. under total reflux.

Subsequently, the distillate was connected to the Liebig condenser side, nitrogen was blown into the liquid with SV20, and methanol, water, and low-boiling silicon components of by-products were distilled off with nitrogen accompanying at 100 ° C. and 500 rpm for 1 hour. Stir. While nitrogen was blown into the liquid with SV20, the polymerization reaction was continued for 5.5 hours while the temperature was further raised and maintained at 130 ° C. to obtain a reaction liquid having a viscosity of 120 mPa · s. Here, “SV” is an abbreviation for “Space Velocity” and refers to the volume of blown volume per unit time. Therefore, SV20 refers to blowing N ₂ in a volume 20 times that of the reaction solution in one hour.

  Nitrogen blowing was stopped and the reaction solution was once cooled to room temperature, then transferred to an eggplant-shaped flask, and methanol and moisture remaining in a trace amount at 120 ° C. and 1 kPa for 30 minutes on an oil bath using a rotary evaporator. The low boiling silicon component was distilled off to obtain a solvent-free sealing member (semiconductor device member forming liquid) having a viscosity of 200 mPa · s.

<Examples and Comparative Examples>
<1-1. Fabrication of semiconductor light emitting device>
As a semiconductor light emitting device (hereinafter referred to as a chip), a plurality of GaN-based light emitting diodes (LEDs) having a peak wavelength of 405 nm, a half width of 30 nm, and a size of 350 μm × 350 μm and having a light emitting layer formed on a sapphire substrate Using. More specifically, ten flip chip type GaN-based light emitting elements having a light emission wavelength of 405 nm are flip-bond mounted with gold bumps on a gold-plated electrode on the bottom surface of a surface-mount type alumina package having a diameter of 8 mm, and the first light emission A device was made.
A second semiconductor light-emitting device is manufactured in the same manner except that a surface-mount type alumina package (same material as the first light-emitting device package) having a diameter of 6 mm is used and the number of semiconductor light-emitting elements is three. did.

<1-2. Preparation of phosphor-containing layer forming solution>
After using the sealing member synthesized in Synthesis Example 1 described above and mixing the thixotropic agent and phosphor shown in Table 6 with the sealing member, the stirring deaerator “Awatake Rentaro ARV-200” manufactured by Shinky Corp. Mixing was performed to obtain a phosphor-containing layer forming solution.

<1-3. Preparation of coating solution for forming light diffusive reflective material-containing layer>
Alumina fine particles (AO-502 manufactured by Admatechs Co., Ltd.) having a particle size of 0.7 μm were mixed with the sealing member synthesized in Synthesis Example 1 so as to have the following concentration, and then stirred and deaerated by “Sinky Corporation” The mixture was mixed with “Rentaro ARV-200” to obtain a white light-diffusing reflector-containing layer forming coating solution.
In addition, as described below, the concentration of the alumina fine particles in the coating solution for forming the light diffusing / reflecting material-containing layer was changed to 0 wt%, 10 wt%, 30 wt%, and 50 wt%, and the first light emitting device was used. Thus, four types of light emitting devices having different alumina fine particle contents in the light diffusing and reflecting material containing layer were produced.
<Alumina fine particle content>
Example 1 50% by weight
Example 2 30% by weight
Comparative Example 1 10% by weight
Comparative Example 2 0% by weight

<1-4. Filling with coating solution for forming light diffusive reflective material-containing layer>
In both the first and second semiconductor light emitting devices, there was a gap of about 20 μm between the GaN-based semiconductor light emitting element and the bottom surface (substrate) of the alumina package. Using a dispenser for the first light-emitting device, about 0.04 mg of a coating solution for forming a light diffusing reflector containing layer per chip was dispensed in the vicinity of the chip and filled under the chip (semiconductor light-emitting element) by capillary action. At this time, the coating liquid for forming the light diffusing reflector containing layer does not adhere to the surface of the semiconductor light emitting element, and the adhesion to the side surface of the light emitting layer is negligible. It was in a position.

<1-5. Production of sealing part>
Using a dispenser, 30 μl of the phosphor-containing layer forming solution obtained in 1-2 was injected into each semiconductor light-emitting device on which the light diffusing reflector-containing layer was formed. Next, the semiconductor light emitting device is held at 90 ° C. for 2 hours, at 110 ° C. for 1 hour, and then at 150 ° C. for 3 hours to cure the phosphor-containing layer forming solution and the light diffusing reflector-containing layer forming coating solution. The semiconductor light emitting devices of the examples and the comparative examples were obtained.

<1-6. Measurement of brightness>
The brightness is measured using a spectroscope “USB2000” (integrated wavelength range: 355-800 nm, light receiving method: 100 mmφ integrating sphere) manufactured by Ocean Optics. Measurement was carried out by holding in a constant temperature bath at 25 ° C. During the measurement, in order to prevent the temperature rise of the semiconductor light emitting device, heat was radiated using the aluminum heat radiating substrate, the heat conductive sheet and the heat sink used in the continuous lighting test as they were.

FIG. 5 shows data when only the transparent silicone resin is sealed. The horizontal axis represents the concentration (% by weight) of alumina in the light diffusing reflector containing layer, and the vertical axis represents the light extraction efficiency. It can be seen that the light extraction efficiency decreases when the alumina concentration is 0% to 10%, but the light extraction efficiency increases as the alumina concentration increases from 10% to 30% to 50%. In particular, the light extraction efficiency was improved at 30% to 50%, compared with the case where the light diffusing reflector-containing layer was not formed (0%). The light diffusing reflector in the layer containing the light diffusing reflector is added with a light diffusing reflector having a large specific gravity to the low-viscosity binder resin, so that the concentration of the light diffusing reflector is higher on the side closer to the substrate. It seems that a gentle concentration gradient occurs. As a result, light emission from the side surface of the light emitting element is not hindered, and it is considered to have a strong diffuse reflection effect directly under the semiconductor light emitting element.
Further, although not shown in the graph, when the light diffusion reflector containing layer having an alumina concentration of 50% by weight was sealed with a sealing member containing a phosphor, the light extraction efficiency was improved by about 10%. .

<Continuous lighting test>
For the purpose of comparing the luminance maintenance ratio with the semiconductor light-emitting device of Example 1, the phosphor-containing layer obtained in 1-2 above using the second semiconductor light-emitting device and not providing the light diffusing reflector-containing layer The forming liquid was applied from the upper edge of the package without any dents or rises, and the phosphor-containing layer was cured under the same temperature conditions as in 1-5 above to obtain a semiconductor light emitting device of Comparative Example 3.
That is, in Example 1, a light diffusing reflector-containing layer was provided as an underfill directly under the light emitting element, and a phosphor-containing layer was provided thereon, but in Comparative Example 3, a light diffusing reflector-containing layer was not formed, and direct fluorescence The body-containing layer forming solution was applied and cured.
The semiconductor light emitting devices of Example 1 and Comparative Example 3 were mounted on an aluminum heat dissipation substrate, and a heat sink was attached under the heat dissipation substrate via a heat conductive sheet, and the heat dissipation substrate and the heat sink were fixed with screws. While maintaining the temperature of the light emitting surface of the chip (semiconductor light emitting element) at 100 ± 10 ° C., a driving current of 360 mA was applied to the semiconductor light emitting device of Example 1 and 120 mA was applied to the semiconductor light emitting device of Comparative Example 3. Continuous lighting was performed at a temperature of 60 ° C. and a relative humidity of 90%. Taking out at regular intervals, the percentage of luminance over time (luminance maintenance rate) with respect to the initial luminance (Lumen) was measured by the luminance measuring method described later. The results are shown in FIG.

Since the semiconductor light emitting device of Example 1 has a larger number of light emitting elements and higher luminance than the light emitting device of Comparative Example 3, the light emitting device of Comparative Example 3 originally has less degradation of the phosphor and the sealant and has a higher luminance. Although the maintenance factor should be higher, Example 1 showed a higher luminance maintenance factor in the continuous lighting test. The reason is considered as follows.
(1) Since the phosphor in the semiconductor light emitting device of Comparative Example 3 also exists directly under the semiconductor light emitting element, the phosphor immediately under the semiconductor light emitting element deteriorates due to high-density light and heat from the light emitting element, and the luminance decreases. did.
(2) Since the semiconductor light emitting device of Example 1 is provided with a light diffusing reflector containing layer as an underfill directly under the semiconductor light emitting element, the concealing property and the light diffusing reflectivity are high. Since the agent (binder resin in the light diffusive reflector-containing layer in Example 1) and the substrate are not irradiated with strong light, these members are less likely to be colored, modified, or peeled off by light or heat, resulting in a decrease in luminance. Was suppressed.

  From the above, it can be seen that the light diffusive reflecting material-containing layer of the present invention not only improves the luminance of the semiconductor light emitting device, but also improves the luminance maintenance rate in continuous lighting. Furthermore, by combining with a highly reliable package, substrate, or sealant, it can be suitably used as a light source for various lighting applications and image display devices.

<Optical simulation>
For the light emitting device having the same optical arrangement as that of Example 1, optical simulation was performed in order to examine the influence of the refractive index and particle diameter of the fine particles dispersed in the light diffusing and reflecting material-containing layer.
Prerequisite:
Light-emitting element substrate Sapphire (n = 1.76, k = 0)
Light emitting part GaN layer (n = 2.55, k = 0)
Element bottom surface ITO (n = 2.12, k = 4.35 × 10 ⁻² )
Package electrode surface Au (n = 1.65, k = 1.96)
Sealing member Resin of Synthesis Example 1 (n = 1.41, k = 0)
Light Diffuse Reflector Al ₂ O ₃ (n = 1.76, k = 0)

FIG. 7 and Table 7 below show the simulation results when the horizontal axis represents the refractive index of the light diffusing reflector contained in the light diffusing reflector containing layer, and the vertical axis represents the light extraction efficiency. When the refractive index was changed from 1.5 to 2.75, which is slightly higher than that of the silicone resin, the extraction efficiency increased monotonously with respect to the refractive index, the refractive index was 2.0 or more, and the light extraction efficiency was almost constant. became. This shows that particles of zirconia (2.1), titania (2.2), GaN (2.55), etc. having a higher refractive index than alumina (1.7) are better.

8 and Table 8 show the simulation results when the horizontal axis represents the particle diameter of the particles to be contained in the light diffusive reflector-containing layer, and the vertical axis represents the light extraction efficiency. The change in light extraction efficiency when the refractive index is changed from 1.5 to 2.75 is shown. It can be seen that the particle diameter that maximizes the light extraction efficiency varies depending on the refractive index. In the table, n represents the refractive index.

  The application of the semiconductor light-emitting device of the present invention is not particularly limited, but can be suitably used in a wide range of fields such as lighting devices, image display devices, and light sources for liquid crystal backlights such as thin televisions. In particular, since it is excellent in luminance and luminous efficiency and can be maintained over a long period of time, its industrial applicability is extremely high in each field such as a lighting device and an image display device.

DESCRIPTION OF SYMBOLS 10, 10 ', 10 ", 10"' ... Semiconductor light-emitting device 11 ... Board | substrate 12 ... Wiring pattern 13 ... Semiconductor light-emitting element 15 ... Sealing part 16 ... Phosphor 21 ... Light-diffusion reflection material containing layer 22 ... Light diffusion Reflective material

Claims (11)

In a semiconductor light emitting device including a semiconductor light emitting element and a substrate having a wiring pattern,
The surface of the substrate and / or the wiring pattern immediately below the semiconductor light emitting element is coated with a light diffusing reflector containing layer having a light diffusing reflector concentration of 30 wt% or more and 70 wt% or less. A semiconductor light emitting device. In a semiconductor light emitting device including a semiconductor light emitting element and a substrate having a wiring pattern,
The surface of the substrate and / or the wiring pattern immediately below the semiconductor light emitting element is covered with a light diffusing reflector containing layer having a light diffusing reflector concentration of 10% by volume to 40% by volume. A semiconductor light emitting device. The semiconductor light emitting device according to claim 1, wherein the light diffusive reflecting material is a metal oxide or a metal nitride. 4. The semiconductor light-emitting device according to claim 1, wherein an average center particle size of the light diffusive reflector is 50 nm or more and 5000 nm or less. 5. The semiconductor light emitting device according to claim 1, wherein a refractive index of the light diffusive reflecting material is 1.5 or more and 3.0 or less. The semiconductor light-emitting device according to claim 1, wherein the semiconductor light-emitting element is disposed on the substrate in a flip chip type. The semiconductor light-emitting device according to claim 1, wherein the light diffusing and reflecting material-containing layer includes a silicone resin. 8. The semiconductor light emitting device according to claim 1, wherein a reflectance of the light diffusing reflective material-containing layer covering the wiring pattern is 70% or more. 9. The semiconductor light-emitting device according to claim 1, wherein the semiconductor light-emitting element has an emission wavelength between ultraviolet and near ultraviolet. An illumination device using the semiconductor light-emitting device according to claim 1 as a light source. An image, comprising: a light source including the semiconductor light emitting device according to claim 1; and a display panel including an optical shutter that receives irradiation of light from the light source. Display device.

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