CN107810551A - For encapsulating the granular epoxy resin constituent of semiconductor device and the semiconductor device using its encapsulation - Google Patents
For encapsulating the granular epoxy resin constituent of semiconductor device and the semiconductor device using its encapsulation Download PDFInfo
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- CN107810551A CN107810551A CN201680036870.1A CN201680036870A CN107810551A CN 107810551 A CN107810551 A CN 107810551A CN 201680036870 A CN201680036870 A CN 201680036870A CN 107810551 A CN107810551 A CN 107810551A
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L23/00—Details of semiconductor or other solid state devices
- H01L23/28—Encapsulations, e.g. encapsulating layers, coatings, e.g. for protection
- H01L23/29—Encapsulations, e.g. encapsulating layers, coatings, e.g. for protection characterised by the material, e.g. carbon
- H01L23/293—Organic, e.g. plastic
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08G—MACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
- C08G59/00—Polycondensates containing more than one epoxy group per molecule; Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
- C08J3/00—Processes of treating or compounding macromolecular substances
- C08J3/12—Powdering or granulating
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
- C08J5/00—Manufacture of articles or shaped materials containing macromolecular substances
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
- C08L63/00—Compositions of epoxy resins; Compositions of derivatives of epoxy resins
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08G—MACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
- C08G2190/00—Compositions for sealing or packing joints
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L2224/00—Indexing scheme for arrangements for connecting or disconnecting semiconductor or solid-state bodies and methods related thereto as covered by H01L24/00
- H01L2224/01—Means for bonding being attached to, or being formed on, the surface to be connected, e.g. chip-to-package, die-attach, "first-level" interconnects; Manufacturing methods related thereto
- H01L2224/10—Bump connectors; Manufacturing methods related thereto
- H01L2224/15—Structure, shape, material or disposition of the bump connectors after the connecting process
- H01L2224/16—Structure, shape, material or disposition of the bump connectors after the connecting process of an individual bump connector
- H01L2224/161—Disposition
- H01L2224/16151—Disposition the bump connector connecting between a semiconductor or solid-state body and an item not being a semiconductor or solid-state body, e.g. chip-to-substrate, chip-to-passive
- H01L2224/16221—Disposition the bump connector connecting between a semiconductor or solid-state body and an item not being a semiconductor or solid-state body, e.g. chip-to-substrate, chip-to-passive the body and the item being stacked
- H01L2224/16225—Disposition the bump connector connecting between a semiconductor or solid-state body and an item not being a semiconductor or solid-state body, e.g. chip-to-substrate, chip-to-passive the body and the item being stacked the item being non-metallic, e.g. insulating substrate with or without metallisation
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L2224/00—Indexing scheme for arrangements for connecting or disconnecting semiconductor or solid-state bodies and methods related thereto as covered by H01L24/00
- H01L2224/01—Means for bonding being attached to, or being formed on, the surface to be connected, e.g. chip-to-package, die-attach, "first-level" interconnects; Manufacturing methods related thereto
- H01L2224/42—Wire connectors; Manufacturing methods related thereto
- H01L2224/47—Structure, shape, material or disposition of the wire connectors after the connecting process
- H01L2224/48—Structure, shape, material or disposition of the wire connectors after the connecting process of an individual wire connector
- H01L2224/4805—Shape
- H01L2224/4809—Loop shape
- H01L2224/48091—Arched
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L2224/00—Indexing scheme for arrangements for connecting or disconnecting semiconductor or solid-state bodies and methods related thereto as covered by H01L24/00
- H01L2224/73—Means for bonding being of different types provided for in two or more of groups H01L2224/10, H01L2224/18, H01L2224/26, H01L2224/34, H01L2224/42, H01L2224/50, H01L2224/63, H01L2224/71
- H01L2224/732—Location after the connecting process
- H01L2224/73251—Location after the connecting process on different surfaces
- H01L2224/73265—Layer and wire connectors
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L2924/00—Indexing scheme for arrangements or methods for connecting or disconnecting semiconductor or solid-state bodies as covered by H01L24/00
- H01L2924/0001—Technical content checked by a classifier
- H01L2924/00012—Relevant to the scope of the group, the symbol of which is combined with the symbol of this group
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L2924/00—Indexing scheme for arrangements or methods for connecting or disconnecting semiconductor or solid-state bodies as covered by H01L24/00
- H01L2924/0001—Technical content checked by a classifier
- H01L2924/00014—Technical content checked by a classifier the subject-matter covered by the group, the symbol of which is combined with the symbol of this group, being disclosed without further technical details
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L2924/00—Indexing scheme for arrangements or methods for connecting or disconnecting semiconductor or solid-state bodies as covered by H01L24/00
- H01L2924/15—Details of package parts other than the semiconductor or other solid state devices to be connected
- H01L2924/181—Encapsulation
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- Chemical Kinetics & Catalysis (AREA)
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- Microelectronics & Electronic Packaging (AREA)
- Power Engineering (AREA)
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- Structures Or Materials For Encapsulating Or Coating Semiconductor Devices Or Solid State Devices (AREA)
- Epoxy Resins (AREA)
Abstract
A kind of semiconductor device for being used to encapsulate the granular epoxy resin constituent of semiconductor device, encapsulate the method for semiconductor device and encapsulated with the granular epoxy resin constituent disclosed herein.The average grain diameter of the granular epoxy resin constituent is about 500 microns to about 1200 microns, the average particle size is to be introduced into by 200 grams of epoxy resin components in sieve shaker, then after classifying 10 minutes under 80 revs/min, as calculated by equation 1, state that order stacks in the sieve that the sieve shaker split shed size is 150 microns, 250 microns, 355 microns, 500 microns, 600 microns, 850 microns, 1000 microns, 1700 microns and 2000 microns with this.
Description
Technical field
Half the present invention relates to a kind of granular epoxy resin constituent for being used to encapsulate semiconductor device and using its encapsulation
Conductor device.
Background technology
Recently, as semiconductor device is used for the development trend of product of taking action, chip wafer (wafer in semiconductor device
Chip size increase), and the thickness of semiconductor device reduces.Therefore, the thickness of the encapsulant on semiconductor device has also connected
Amount with the encapsulant of per unit device reduces together.Herein, the thickness of the encapsulant on semiconductor device refers to be covered in
The thickness of the encapsulant of the apparent surface of the lead frame of face installation semiconductor device or the mounting plane of circuit board, or refer to and work as
When one or more semiconductor devices are stacked on lead frame or circuit board, in the installation of lead frame installed above or circuit board
The thickness of the encapsulant of the opposite side covering the superiors semiconductor device of plane.
Recently, in order that die cap (Mold cap) minimizes and solves to ask such as gate break (wire sweep)
Topic, energetically check the semiconductor packaging using compression molding (compression mold).Mainly use granular/powder
Encapsulant is compressed molding (compression mold).However, typical granular/powder encapsulation used in the art
In the situation of thing, if the amount of granular/powder encapsulant reduces, resin may be unevenly distributed in die cavity, thus cause
Surface molding defect, such as non-uniform spraying, lack of fill, space etc..Further, since the charging precision of oscillating feeder is bad
Change, resin weighing error and biased error occur, thus cause productivity ratio deterioration and encapsulant to waste.
In addition, there is also problems with:Granular/powder encapsulant attaches to feeder inner surface and deterioration continuous production
Rate, wherein the problems such as covering PCB identification marks by stain due to the fine powder of distribution.
Therefore, it is necessary to which a kind of granular epoxy resin constituent for being used to encapsulate semiconductor device, it can be solved as described above
The problem of.
One example of prior art is disclosed in Korean Patent Publication case the 2008-121003Ath.
The content of the invention
Technical problem
One embodiment of the present of invention is a kind of granular epoxy resin constituent for being used to encapsulate semiconductor device of offer, its
Can prevent weighing error, cover identification mark the problem of and continuous production rate deterioration.
Another embodiment of the present invention is a kind of using the granular epoxy for being used to encapsulate semiconductor device as described above to provide
The method that resin combination encapsulates semiconductor device.
One more embodiment of the present invention is used for the granular asphalt mixtures modified by epoxy resin for encapsulating semiconductor device as described above to provide a kind of use
The semiconductor device of fat composition encapsulation.
Technical scheme
According to one embodiment of present invention, there is provided a kind of granular epoxy resin composition for being used to encapsulate semiconductor device
Thing, wherein the average grain diameter of the granular epoxy resin constituent is about 500 microns to about 1200 microns, the average grain diameter is
It is introduced into by 200 grams of epoxy resin components in sieve shaker, it is such as logical after then classifying 10 minutes under 80 revs/min
Equation 1 is crossed to be calculated, the sieve shaker split shed size be 150 microns, 250 microns, 355 microns, 500 microns, it is 600 micro-
Rice, 850 microns, 1000 microns, the sieves (sieve) of 1700 microns and 2000 microns to be to state that order stacks.
<Equation 1>
In equation 1, IiTo remain in the weight (gram) of the epoxy resin component on i-th of stacking sieve, DiFor i-th
The individual opening size (micron) for stacking sieve, and Di+1The opening size (micron) of sieve is stacked for i+1.
As calculated by equation 1, the average grain diameter of epoxy resin component can be about 700 microns to about 1100 it is micro-
Rice.
The particle diameter that epoxy resin component can be included less than about 5 weight % (wt%), preferably less than 3wt% is less than about
150 microns of particle and about 60wt% or particle diameter more than 60wt%, more preferably about 65wt% or more than 65wt% are about 500
Micron or the particle more than 500 microns and less than about 1000 microns.
Epoxy resin component can be free of the particle that particle diameter is less than about 150 microns.
The particle diameter that epoxy resin component can be included less than about 20wt% is about 1000 microns or more than 1000 microns
Particle, and without particle diameter be preferably about 1000 microns or the particle more than 1000 microns.
Epoxy resin component is about 500 microns or more than 500 microns and less than about 1000 microns included in particle diameter
Particle among about 20% or less than 20%, preferably about 15% or the particle of the number percent less than 15% meet equation 2.
<Equation 2>
L/2≤H < L
In equation 2, L is the point extremely line (A) tangent with the both ends of the particle that connection forms particle exterior contour
Vertical line maximum length, and H is that connection forms the point of the inside particles profile to tangent with the both ends of the particle
The maximum length of the vertical line of line (A).
According to another embodiment of the present invention, there is provided a kind of method for encapsulating semiconductor device, including described in compression molding
For encapsulating the granular epoxy resin constituent of semiconductor device.
According to one more embodiment of the present invention, there is provided be used for the granular epoxy resin for encapsulating semiconductor device described in a kind of use
The semiconductor device of constituent encapsulation.
Beneficial effect
Using according to the present invention granular epoxy resin constituent can make weighing error, cover identification mark the problem of, even
Deterioration of continuous productivity ratio etc. minimize.
Brief description of the drawings
Fig. 1 is the example according to the shape of particle of granular epoxy resin constituent of the present invention for encapsulating semiconductor device
Figure.
Fig. 2 is the sectional view according to the semiconductor device of one embodiment of the present of invention.
Fig. 3 is the sectional view according to the semiconductor device of another embodiment of the present invention.
Fig. 4 is the sectional view according to the semiconductor device of one more embodiment of the present invention.
Fig. 5 is the sectional view according to the semiconductor device of another embodiment of the present invention.
Optimal mode
Hereinafter, embodiments of the invention are elaborated with reference to the accompanying drawings.
For encapsulating the granular epoxy resin constituent of semiconductor device
According to the present invention, such as pass through equation for encapsulating the average grain diameter of granular epoxy resin constituent of semiconductor device
Formula 1 is calculated, and can be about 500 microns to about 1200 microns, e.g., from about 700 microns to about 1100 microns, especially about 700 microns extremely
About 1000 microns.
Average grain diameter refers to be introduced into sieve shaker by 200 grams of epoxy resin components, then classifies under 80 revs/min
After 10 minutes, such as the value calculated by equation 1, the sieve shaker split shed size be 150 microns, 250 microns,
355 microns, 500 microns, 600 microns, 850 microns, 1000 microns, 1700 microns and 2000 microns of sieve (sieve) is with old
Order is stated sequentially to stack.
<Equation 1>
In equation 1, IiTo remain in the weight (gram) of the epoxy resin component on i-th of stacking sieve, DiFor i-th
The individual opening size (micron) for stacking sieve, and Di+1The opening size (micron) of sieve is stacked for i+1.
Herein, it is Luo Taipu sieve shakers to sieve as JIS standard screens and sieve shaker.In addition, the sieve is stacked to be open
Sieve of the smallest size of sieve positioned at orlop position and opening size maximum is located at most upperstratum position.That is, opening is stacked first
Sieve that size is 150 microns, secondly to stack the sieve, the 3rd that opening size is 250 microns to stack opening size be 355 microns
Sieve, the 4th stack the sieve, the 5th that opening size is 500 microns and stack the stacking open-mouth ruler of sieve, the 6th that opening size is 600 microns
It is very little be 850 microns sieve, the 7th stack opening size be 1000 microns sieve, the 8th stack opening size be 1700 microns
Sieve, and the 9th stacks the sieve that opening size is 2000 microns.In this method, although existing with high length and width (aspect) ratio
Particle (with less than sieve opening short diameter and be more than sieve be open long diameter particle) by the possibility of each sieve, but
For convenience, the quality % for the component classified in a certain method is defined as the particle diameter distribution of granular resin constituent.
According to the present invention, when the average grain diameter of granular epoxy resin constituent meets scope as described above, due to suppression
Sticking between bad filling, particle is made or particle attaches to feeder inner surface and because what powder was spread covers identification mark
Note, therefore granular epoxy resin constituent can ensure stable productivity ratio and mouldability.
In one embodiment, included according to the granular epoxy resin constituent for being used to encapsulate semiconductor device of the present invention
Particle diameter less than about 5wt%, preferably less than about 3wt% is less than about 150 microns of particle.If particle diameter is less than about 150
The amount of the particle of micron is greater than about 5wt%, then can have machine error due to the fine powder in constituent, and can be due to distribution
The amount of encapsulant increases and the problem of covering identification mark be present.In addition, may occur in which feeder block and encapsulant attach into
Glassware.Particle diameter can be 0wt% less than about the lower limit of the amount of 150 microns of particle, but not limited to this.That is, according to this hair
Bright epoxy resin component can not include the particle that particle diameter is less than about 150 microns.
In addition, 60wt% can include about or more than 60wt% according to the epoxy resin component of the present invention, e.g., from about
65wt% or more than 65wt%, especially about 65wt% to about 90wt% particle diameter be about 500 microns or more than 500 microns and
Particle less than 1000 microns.Within this range, epoxy resin component can show more stable productivity ratio and mouldability.
If particle diameter is about 500 microns or is less than about 60wt% more than 500 microns and less than the amount of 1000 microns of particle, due to
Because resin weighing error occurs in the charging precision deterioration of oscillating feeder and deviates (deviation) error, therefore may occur in which for example
The problems such as surface molding defect, productivity ratio deterioration and encapsulant waste.
It is less than about in addition, being included according to the granular epoxy resin constituent for being used to encapsulate semiconductor device of the present invention
20wt%, preferably about 10wt% or the particle diameter less than 10wt%, more preferably about 3wt% or less than 3wt% are about 1000 microns
Or the particle more than 1000 microns.Within this range, it can prevent the charging port of feeder from blocking and good weighing essence can be realized
Degree.Particle diameter is about 1000 microns or the lower limit of the amount of particle (corase particles) more than 1000 microns can be 0wt%, but unlimited
In this.That is, can be free of particle diameter according to the epoxy resin component of the present invention is about 1000 microns or more than 1000 microns
Particle.
Meet that the percentage by weight of the particle of each above-mentioned particle diameter scope is calculated as follows.200 grams of epoxy resin are formed
Thing is introduced into sieve shaker, in the sieve that the sieve shaker split shed size is 150 microns, 500 microns and 1000 microns to state
Order sequentially stacks, and then classifies 10 minutes under 80 revs/min.Then, the epoxy resin component remained on sieve is measured
Weight or the epoxy resin component for passing through sieve weight, the weight of the subsequent epoxy resin component divided by introduced
The amount (200 grams) of epoxy resin component.Then, income value is multiplied by 100, thus calculates and meets each above-mentioned particle diameter scope
The percentage by weight of particle.Herein, it is Luo Taipu sieve shakers to sieve as JIS standard screens and sieve shaker.In addition, it is described sieve it is stacked with
So that the sieve that opening size is 150 microns is located at orlop position, opening size is that 500 microns of sieve is centrally located, and
Opening size is that 1000 microns of sieve is located at most upperstratum position.
Specifically, after sorting technique as described above, the epoxy by the sieve that opening size is 150 microns is measured
The weight of resin combination, the subsequent weight of the epoxy resin component divided by the amount of introduced epoxy resin component
(200 grams).Then, income value is multiplied by 100, thus calculates the percentage by weight of particle of the particle diameter less than about 150 microns.
In addition, after sorting technique as described above, the epoxy remained on the sieve that opening size is 500 microns is measured
The weight of resin combination, the weight of the epoxy resin component then measured divided by introduced epoxy resin component
Measure (200 grams).Then, income value is multiplied by 100, thus calculates particle diameter and is about 500 microns or more than 500 microns and is less than about
The percentage by weight of 1000 microns of particle.
In addition, after sorting technique as described above, the ring remained on the sieve that opening size is 1000 microns is measured
The weight of oxygen tree fat composition, the weight of the epoxy resin component then measured divided by introduced epoxy resin component
Amount (200 grams).Then, income value is multiplied by 100, and it is about 1000 microns or the grain more than 1000 microns thus to calculate particle diameter
The percentage by weight of son.
Can be included in particle diameter according to the granular epoxy resin constituent for being used to encapsulate semiconductor device of the present invention is
About 500 microns or more than 500 microns and less than about among 1000 microns of particle about 20% or less than 20%, e.g., from about 15% or
The particle of number percent less than 15% meets equation 2.It is preferred that the amount for meeting the particle of equation 2 is 0wt%.
<Equation 2>
L/2≤H < L
Wherein, reference picture 1, L are that connection forms the point of particle exterior contour to the line A's tangent with the both ends of the particle
The maximum length of vertical line, and H is the point extremely line A tangent with the both ends of the particle that connection forms the inside particles profile
Vertical line maximum length.Herein, term " particle exterior contour " refer to away from tangent line A distal side formed particle profile and
Term " inside particles profile " refers to the particle profile formed in the nearside away from tangent line A.
The number percent of particle is calculated as follows.10 grams of epoxy resin components are introduced into sieve shaker, then 80 turns/
Point lower classification 10 minutes, in the sieve that the sieve shaker split shed size is 150 microns, 500 microns and 1000 microns to state
Order sequentially stacks.Then, the quantity of the epoxy resin component particle remained on the sieve that opening size is 500 microns is measured
And meet the quantity of the particle of equation 2 among above particle, it is about 500 micro- to be calculated from there through equation 3 in particle diameter
Rice or more than 500 microns and less than about the number percent for the particle for meeting equation 2 among 1000 microns of particle.
<Equation 3>
Number percent={ among the epoxy resin component particle on the sieve that opening size is 500 microns is remained in
Meet the total of the epoxy resin component particle for the quantity of the particle of equation 2/remain on the sieve that opening size is 500 microns
Number } × 100
If as described above, be about 500 microns in particle diameter or more than 500 microns and less than about 1000 microns particle work as
The number percent of the middle particle for meeting equation 2 is about 20% or less than 20%, then epoxy resin component is because suppressing particle
Between coalescence and more efficiently prevent from feeder blocking.
For the component for the granular epoxy resin constituent for encapsulating semiconductor device
Epoxy resin, solidification can be included according to the granular epoxy resin constituent for being used to encapsulate semiconductor device of the present invention
At least one of agent, inorganic filler and curing catalysts.
Epoxy resin
Epoxy resin is included according to the granular epoxy resin constituent for being used to encapsulate semiconductor device of the present invention.
Epoxy resin is the epoxy resin with two or more epoxy radicals, and can be included usually used in technique
Any epoxy resin.For example, epoxy resin can include bisphenol A epoxide resin, bisphenol F epoxy resin, phenol novolac ring
Oxygen tree fat, tributyl catechol epoxy resin, naphthalene epoxy resins, glycidyl amine epoxy resins, cresol novolac epoxy tree
Fat, biphenyl epoxy resin, linear aliphatic epoxy resin, alicyclic ring epoxide resin, heterocyclic epoxy resin, the epoxy resin containing loop coil,
Cyclohexanedimethanol epoxy resin, trihydroxy methyl epoxy resin, halogenated epoxy resin etc..These epoxy resin can be individually or with it
Combining form uses.For example, epoxy resin can be the epoxy with two or more epoxy radicals and one or more hydroxyls
Resin.Epoxy resin can include at least one of solid epoxy and liquid epoxies, and preferably include solids epoxy
Resin.
Curing agent
Curing agent can be included according to the granular epoxy resin constituent for being used to encapsulate semiconductor device of the present invention.
Curing agent can include any curing agent usually used in technique.For example, curing agent can include:Phenol
It is aralkyl-phenol resin, phenol novolac phenol resin, new phenol phenol resin, cresol novolac phenol resin, naphthols phenol resin, terpene-phenolic resin, more
Function phenol resin, bicyclopentadiene phenol resin and the phenolic aldehyde phenol resin synthesized by bisphenol-A and fusible phenolic resin;Polynary phenolate
Compound, include three (hydroxy phenyl) methane and dihydroxybiphenyl;Acid anhydrides, include maleic anhydride and phthalic anhydride;Aromatic amine,
Such as m-phenylene diamine (MPD), two amido diphenyl-methanes and two amido diphenyl sulfones etc..These curing agent can combine shape individually or with it
Formula uses.It is preferred that curing agent is the phenol resin with one or more hydroxyls.
Inorganic filler
Inorganic filler can be included according to the granular epoxy resin constituent for being used to encapsulate semiconductor device of the present invention.
Inorganic filler can improved mechanical properties, while reduce the stress of constituent.The example of inorganic filler can include
Fused silica, crystalline silica, calcium carbonate, magnesium carbonate, aluminum oxide, magnesia, clay (clay), talcum (talc), silicon
At least one of sour calcium, titanium oxide, antimony oxide and glass fibre.
In order to reduce stress, inorganic filler can include the fused silica with low linear expansion coefficient.Melting two
Silica refers to that true specific gravity is 2.3 or the non-crystalline silica less than 2.3.Fused silica is by fusion-crystallization dioxy
SiClx is prepared or comprising the non-crystalline silica by various Material synthesis.Although the shape and particle of fused silica are straight
Footpath is not particularly limited, but fused silica is ideally with spherical.Epoxy resin component can include mean particle diameter
For 0.001 micron to 30 microns of spherical fused silica.In addition, according to the purpose of epoxy resin component, spherical melting
The maximum particle diameter of silica can tune at least one of 45 microns, 55 microns and 75 microns.Although conductive carbon
It can be included in as foreign substance on the surface of spherical fused silica, it is important that selection includes polarity as few as possible
The material of foreign substance.
Curing catalysts
Curing catalysts can be included according to the granular epoxy resin constituent for being used to encapsulate semiconductor device of the present invention.
Curing catalysts can Bao Han Phosphonium curing catalysts, Ji non-Phosphonium curing catalysts, include tertiary amine, Organometallic compounds
Thing, organic phosphorus compound, imidazoles, boride etc..
Phosphonium curing catalysts include tetraphenylphosphoniphenolate, tetraphenylboronic acid tetraphenylphosphoniphenolate etc..
Tertiary amine includes benzyl dimethyl amine, triethanolamine, triethylenediamine, Diethylaminoethanol, three (dimethylamino first
Base) phenol, 2-2- (dimethylamino methyl) phenol, 2,4,6- tri- (two aminomethyls) phenol, -2- ethyl esters of caproic acid three etc..
Organo-metallic compound includes pentanedione acid chromium, pentanedione acid zinc, nickel acetylacetonate etc..
Organic phosphorus compound include three -4- methoxyl groups phosphines, triphenylphosphine, triphenylphosphine-triphenylborane, triphenylphosphine -
Isosorbide-5-Nitrae-benzoquinones adduct etc..Imidazoles includes 2-methylimidazole, 2- phenylimidazoles, 2- amidos imidazoles, 2- methyl isophthalic acids-vinyl miaow
Azoles, 2-ethyl-4-methylimidazole, 2- heptadecylimidazoles etc..Boride include tetraphenylboronic acid triphenylphosphine, tetraphenyl boron salt,
Trifluoroboranes-n-hexylamine, trifluoroboranes mono aminoethane, tetrafluoro borane triethylamine, tetrafluoro borine amine etc..
Curing catalysts can include 1,5- diazabicyclos [4.3.0] nonyl- 5- alkene (1,5-diazabicyclo [4.3.0]
non-5-ene:DBN), -7- alkene of 1,8- diazabicyclos [5.4.0] 11 (1,8-diazabicyclo [5.4.0] undec-7-
ene:DBU), phenol novolacs salt etc..It is preferred that curing catalysts are consolidated comprising organic phosphorus compound, boride, amine or imidazoles
Change catalyst.These curing catalysts can use individually or with its combining form.Curing catalysts can be by being catalyzed solidification
The adduct that agent obtains with epoxy resin or curing agent pre-reaction.
Additive
General additive can be included according to the granular epoxy resin constituent for being used to encapsulate semiconductor device of the present invention.
In one embodiment, additive can include coupling agent, releasing agent, stress elimination agent, crosslinking accelerator, leveling agent and colouring agent
At least one of.
Coupling agent can be included selected from least one of group consisted of:Epoxy silane, amino containing silane, sulfydryl silicon
Alkane, alkyl silane and alkoxy silane, but not limited to this.
Releasing agent can be included selected from least one of group consisted of:Paraffin, ester type waxes, higher fatty acids, height
Level fatty acid metal salts, natural acid and natural fat acid metal salt.
Stress elimination agent can be included selected from least one of group consisted of:Modify silicone oil, silicone elastomer,
Silicone powder and silicone resin, but not limited to this.
Colouring agent can include carbon black etc..
The method for preparing the granular epoxy resin constituent for encapsulating semiconductor device
Then, the method that will be apparent from preparing the granular epoxy resin constituent for being used to encapsulate semiconductor device.
Can be by mixing, melting and mediating asphalt mixtures modified by epoxy resin as described above according to the granular epoxy resin constituent of the present invention
Fat, curing agent, inorganic filler, curing catalysts and/or additive, then using for example crush, be granulated, extruding, cutting and/
Or the methods of screening, adjusts the average grain diameter of mixture and prepares.Herein, particle size adjustment can be by well known each in technique
Particle size adjustment method is planted to carry out, such as centrifugation grinding, crushing-screening, thermal cutting etc..
Centrifugation is ground to a kind of method that powder diameter is adjusted using grinder, and the grinder includes disc circulator
And the drum sieve (open mesh) on the upside of the circulator.Herein, grinder is included to have and is used for melting and mediating
Resin combination charging opening drum sieve.Circulator can be formed by the nonmagnetic substance with high thermal conductivity, and comprising
Open mesh with the net hole for cutting resin constituent.In addition, for rotating the instrument of circulator and being revolved for heating
Turning the heater of device can be provided to the upside of circulator and/or downside.Ground in addition, grinder optionally can be included also for cooling
The cooler of grinding machine.
Centrifugation grinding used according to the invention prepares the side for the granular epoxy resin constituent for being used to encapsulate semiconductor device
Method is as follows.First, the component of blending epoxy constituent, then melt and mediate the component, thus prepare epoxy resin
Constituent.Then, prepared epoxy resin component is fed into grinder via the opening of grinder, is then revolved in heating
Turn to rotate the circulator while device.Epoxy resin component because circulator rotate caused by centrifugal force pass through open mesh,
And the average grain diameter of epoxy resin component is adjusted in the process.The average grain diameter of epoxy resin component can be according to perforate silk
The temperature of the mesh size of net, the rotary speed of circulator and/or circulator is adjusted.When using centrifugation grinding, advantage exists
It can show that stabilised in size is distributed in epoxy resin component, and particle can have the surface of relative smooth.
Crushing-sieve as a kind of method using sieve regulation powder diameter.Prepared by crushing used according to the invention-screening uses
It is as follows in the method for the granular epoxy resin constituent of encapsulation semiconductor device.First, asphalt mixtures modified by epoxy resin is pre-mixed by blender
The component of fat composition, then heat and the component is mediated by roller, kneader, extruder etc., and then cooled down simultaneously
Crush, be consequently formed the epoxy resin component of crushing.Then, the epoxy resin component crushed using screening class, is thus moved
Except corase particles and fine powder.Herein, can be formed by suitably selecting screening condition to prepare the epoxy resin with required average grain diameter
Thing.Crushing-sieve to be desirable, because typical manufacturing line can be employed without additional separation equipment as former state.In addition, when molten
When melt resin forms thin slice before crushing, due to exist it is many can independent control factor, such as selection sheet thickness, selection
Pulverization conditions or screening, selection sieve etc. during screening during crushing, therefore in order to realize the particle diameter distribution according to the present invention, powder
It is broken-to sieve to be desirable, because there is many to be used to adjust epoxy resin component to required particle diameter distribution for crushing-screening
Option.
Then, earnestly it is segmented into a kind of method for adjusting particle diameter by cutting molten resin.Thermal cutting used according to the invention
The method for preparing the granular epoxy resin constituent for encapsulating semiconductor device is as follows.First, it is pre-mixed by blender
The component of epoxy resin component, the then extruding heating and using the mould comprising multiple apertures is provided in screw front end
While machine mediates the component, using being almost expelled from the multiple small of mould with the cutter cuts of die surface parallel sliding
The wire molten resin in hole.Herein, can be by suitably selecting kneading conditions and/or cutting condition to prepare with required average grain diameter
Epoxy resin component.Because device for thermally cutting is provided to the front end of extruder only in thermal cutting, thus earnestly be segmented into accordance with
Need, because typical manufacturing line can use as former state.
Can be in following broad range according to the granular epoxy resin constituent for being used to encapsulate semiconductor device of the present invention
Use:Need the application of the epoxy resin component encapsulation semiconductor device, stick together film, the insulating resin such as prepreg
Thin slice, circuit board, solder resist, underfill, crystal grain grafting material and component supplement resin, but not limited to this.
The encapsulation of semiconductor device
The granular asphalt mixtures modified by epoxy resin as described above for being used to encapsulate semiconductor device can be used according to the semiconductor device of the present invention
Fat composition encapsulates.
Fig. 2 is the section view according to the semiconductor device of one embodiment of the present of invention.Reference picture 2, according to the present invention
One embodiment semiconductor device (100) may include terminal plate (10), the projection (30) that is formed on terminal plate (10) with
And the semiconductor chip (20) formed on raised (30), wherein the gap between terminal plate (10) and semiconductor chip (20) and
The whole top surface of semiconductor chip (30) is encapsulated with epoxy resin component (40).Herein, epoxy resin component can include root
According to the granular epoxy resin constituent for being used to encapsulate semiconductor device of the present invention.
Fig. 3 is the section view according to the semiconductor device of another embodiment of the present invention.Reference picture 3, according to the present invention
Another embodiment semiconductor device (200) may include terminal plate (10), the projection (30) that is formed on terminal plate (10) with
And the semiconductor chip (20) formed on raised (30), wherein the gap between terminal plate (10) and semiconductor chip (20) and
Whole side available epoxy constituent (40) encapsulation of the semiconductor chip (30) in addition to its top surface.Herein, epoxy resin
Constituent can include the granular epoxy resin constituent for being used to encapsulate semiconductor device according to the present invention.
Fig. 4 is the section view according to the semiconductor device of one more embodiment of the present invention.Reference picture 4, according to this reality
In the semiconductor device (300) for applying example, semiconductor chip (20) is fastened to die pad via the crystal grain grafting material (60) of solidification
(50) upper face, semiconductor chip (20) are connected to lead frame (80) via wire (70).Semiconductor chip (20), punching
Die-cushion (50) and whole available epoxy constituent (40) encapsulation of the crystal grain grafting material (60) of solidification.Herein, asphalt mixtures modified by epoxy resin
Fat composition can include the granular epoxy resin constituent for being used to encapsulate semiconductor device according to the present invention.
Fig. 5 is the section view according to the semiconductor device of another embodiment of the present invention.Reference picture 5, according to this reality
In the semiconductor device (400) for applying example, semiconductor chip (20) is fastened to terminal plate via the crystal grain grafting material (60) of solidification
(10) upper face.Semiconductor chip (20) is connected to the electrode pad (90) on the upside of terminal plate (10) via wire (70).
Soldered ball (100) can be formed in the lower surface of terminal plate (10).Only in the terminal plate installed above for having semiconductor chip (20)
(10) surface available epoxy constituent (40) encapsulation.Herein, epoxy resin component can include the use according to the present invention
In the granular epoxy resin constituent of encapsulation semiconductor device.
In Fig. 2 into Fig. 5, each terminal plate, die pad, the size of projection and semiconductor chip, the crystal grain of solidification connect
The thickness of condensation material layer, raised quantity, the length of wire and lead frame are optional and can change.
It may include compression molding basis as described above using the method that semiconductor device is encapsulated according to the constituent of the present invention
The granular epoxy resin constituent for being used to encapsulate semiconductor device of the present invention.More specifically, compression molding may include for example
Granular epoxy resin constituent is supplied in die cavity, epoxy resin component is melted, semiconductor device is immersed to melting
In epoxy resin component, and the epoxy resin component encapsulation semiconductor device for passing through solidification of molten.
The pattern of invention
Then, the present invention will be explained in more detail with reference to some examples.It should be understood that these examples should not regard in any way
For the limitation present invention.
Example
The details of the component of epoxy resin component used and amount are as follows in example and comparative example.
(1) epoxy resin
Using 7.4wt% NC-3000 (Japanese chemical drug Co., Ltd), it is biphenyl novolac epoxy resin;And 1.8wt%
YX-4000 (Japanese epoxy resin Co., Ltd), it is biphenyl epoxy resin.
(2) curing agent
Using 3.3wt% DL-92 (bright and Co., Ltd), it is phenol novolacs;And 0.8wt% MEH-
7851S (bright and Co., Ltd), it is biphenyl phenolic resin.
(3) curing catalysts
Use 0.7wt% triphenylphosphine (Triphenyl phosphine) (Bei Xing Chemical Co., Ltd.s).
(4) inorganic filler
The spherical fused silica that mean particle diameter using 85wt% is 20 microns.
(5) coupling agent
Use 0.2wt% epoxy silane KBM-303 (Co., Ltd of SHIN-ETSU HANTOTAI) and 0.2wt% amino containing silane KBM-573
(Co., Ltd of SHIN-ETSU HANTOTAI).
(6) colouring agent
Use 0.3wt% carbon black MA-600B (Co., Ltd of Mitsubishi Chemical).
(7) releasing agent
Use 0.3wt% Brazil wax.
Example 1 is to example 5 and comparative example 1 to comparative example 3
Weighing component as listed in Table 1 and equably mixed using Henschel blender to prepare the first powder constituent
Thing.Then, each first constituent is mediated in extruder and is supplied in centrifugal grinder and formed with preparing granular epoxy resin
Thing.Herein, temperature and centrifugation grinding condition are mediated as outlined below in table 1.
By the following method with regard to average grain diameter, particle size classification, shape and each epoxy resin component of characteristic evaluation.
(1) average grain diameter (micron):200 grams of epoxy resin components are introduced into sieve shaker, then under 80 revs/min
Classification 10 minutes, the sieve shaker split shed size be 150 microns, 250 microns, 355 microns, 500 microns, 600 microns,
850 microns, 1000 microns, 1700 microns and 2000 microns of sieve (sieve) with state order stack.Then, equation is passed through
Formula 1 calculates the average grain diameter of each epoxy resin component.
<Equation 1>
In equation 1, IiTo remain in the weight (gram) of the epoxy resin component on i-th of stacking sieve, DiFor i-th
The individual opening size (micron) for stacking sieve, and Di+1The opening size (micron) of sieve is stacked for i+1.
(2) particle size classification (wt%):200 grams of epoxy resin components are introduced into sieve shaker, then under 80 revs/min
Classification 10 minutes, in the sieve that the sieve shaker split shed size is 150 microns, 500 microns and 1000 microns to state order
Stack.Then, measure the weight of the epoxy resin component for the sieve for respectively passing through that opening size is 150 microns, remain in open-mouth ruler
It is very little be 500 microns sieve on epoxy resin component weight and the ring that remaines on the sieve that opening size is 1000 microns
The weight of oxygen tree fat composition.Then, the weight divided by the amount of introduced epoxy resin component that respectively measure and it is multiplied by 100,
Thus the percentage by weight for the particle for meeting each particle diameter scope is calculated.
(3) style characteristic (%):10 grams of epoxy resin components are introduced into sieve shaker, then at 80 revs/min lower point
Class 10 minutes, in the sieve that the sieve shaker split shed size is 150 microns, 500 microns and 1000 microns to state order heap
It is folded.Then, measure the quantity of the epoxy resin component particle remained on the sieve that opening size is 500 microns and meet equation
The quantity of the particle of formula 2, calculated from there through equation 3 among the particle on the sieve that opening size is 500 microns is remained in
Meet the number percent of the particle of equation 2.
<Equation 2>
L/2≤H < L
In equation 2, L is the point extremely line (A) tangent with the both ends of the particle that connection forms particle exterior contour
Vertical line maximum length, and H is that connection forms the point of the inside particles profile to tangent with the both ends of the particle
The maximum length of the vertical line of line (A).
<Equation 3>
Number percent={ among the epoxy resin component particle on the sieve that opening size is 500 microns is remained in
Meet the total of the epoxy resin component particle for the quantity of the particle of equation 2/remain on the sieve that opening size is 500 microns
Number } × 100
(4) machine error (weighing and biased error):Each epoxy resin component of example and comparative example uses compression mould
Molding machine (east and Co., Ltd) is moulded to 110 microns of thickness 20 times.By weighing error at least once and resin biased error shadow
The epoxy resin component that loud epoxy resin component is classified as X and do not influenceed by weighing error and resin biased error is classified as.
(5) fillable:By compression molding machine (east and Co., Ltd) by each epoxy resin group of example and comparative example
It is molded into thing on the semiconductor chip of PKG assemblies, wherein size is that 12 millimeters × 12 millimeters of chip wafer is pacified using paste
Mounted in the FBGA substrate (sizes with 56 units:15 millimeters × 15 millimeters) on.Herein, the molding of each epoxy resin component
Thickness is 110 microns, and molding temperature is 165 DEG C and molding cycle is 60 seconds.As the PKG as packaged by naked eye after molding
Outward appearance when so that overall cell molds good epoxy resin component, causes the asphalt mixtures modified by epoxy resin for being less than 5 unit filling defects
Fat composition, and cause 5 or the epoxy resin component more than 5 unit filling defects is classified as X.
(6) feeder blocks:Each epoxy resin component of example and comparative example uses compression molding machine (eastern and limited public affairs
Department) it is moulded to 110 microns of thickness 20 times.The epoxy resin component for causing feeder to block at least once is classified as X and not led
The epoxy resin component for causing feeder to block is classified as O.
(7) epoxy resin component attaches to the inner surface of feeder:Repeated using the oscillating feeder of mould machine with 0.2
The feed rate of Grams Per Second introduces each epoxy resin component of 3.3 grams of examples and comparative example to compression molding machine (eastern and limited public affairs
Department) in operation 20 times.Complete feed after, separating feed device and measurement attach to feeder inwall epoxy resin composition
The weight of thing.(in this case, sticked when the gross weight for the epoxy resin component for attaching to feeder is less than 150 milligram hours
The epoxy resin component for investing feeder inner surface is barely perceivable), it is allowed to epoxy resin component is classified as O.When glutinous
The gross weight of the epoxy resin component of feeder is invested for 150 milligrams or more than 150 milligram hours (due to asphalt mixtures modified by epoxy resin significantly occurs
Fat composition sticks, therefore by the inner surface blackening of naked eye to feeder), epoxy resin component is classified as X.
(8) the defects of covering identification mark
It is micro- that each epoxy resin component of example and comparative example uses compression molding machine (east and Co., Ltd) to be moulded to 20
The thickness of rice 20 times.When the every PCB average for interspersing among the stain on identification marked region is 1 or during more than 1, asphalt mixtures modified by epoxy resin
Fat composition is classified as X.When the every PCB average for interspersing among the stain on identification marked region is less than 1.
Table 1
For the example 1 with the particle diameter distribution according to the present invention to the epoxy resin component of example 5, meet equation
The ratio of 2 particle is 20% or less than 20%, and such as machine error, bad filling, feeder does not occur and block, encapsulate
The problems such as thing attaches to feeder inner surface and covers identification mark.
For the comparative example 1 without the particle diameter distribution according to the present invention to the epoxy resin component of comparative example 3, compare
The epoxy resin component of example 1 produces the problem of machine error, bad filling and feeder block, the asphalt mixtures modified by epoxy resin of comparative example 2
The problem of fat composition produces machine error, bad filling and covers identification mark, and the epoxy resin component of comparative example 3
Produce the problem of encapsulant attaches to feeder inner surface and covers identification mark.Therefore, it was demonstrated that comparative example 1 to comparative example 3
Epoxy resin component can not realize the effect of the present invention.
Although some embodiments have been described, it should be understood that previous embodiment provides and not merely for illustrative purpose
It should be regarded as limiting the invention in any way, and those who familiarize themselves with the technology can be in without departing from the spirit and category situation
It is lower to obtain various retouchings, change, change and equivalent embodiment.
Claims (11)
1. a kind of granular epoxy resin constituent for being used to encapsulate semiconductor device, wherein the granular epoxy resin constituent
Average grain diameter is 500 microns to 1200 microns, and the average grain diameter is that 200 grams of epoxy resin components are being introduced into reciprocating gird
(seive) in machine, after then classifying 10 minutes under 80 revs/min, calculated by equation 1, opened in the sieve shaker
Mouthful size be 150 microns, 250 microns, 355 microns, 500 microns, 600 microns, 850 microns, 1000 microns, 1700 microns and
2000 microns of sieve with state order stack;
<Equation 1>
Wherein Ii is the weight in grams of the epoxy resin component remained on i-th stacking sieve, DiFor described i-th
The individual opening size in units of micron for stacking sieve, and Di+1The open-mouth ruler in units of micron of sieve is stacked for i+1
It is very little.
2. granular epoxy resin constituent according to claim 1, wherein the epoxy resin component is described average
Particle diameter is calculated by equation 1, is 700 microns to 1100 microns.
3. granular epoxy resin constituent according to claim 1, including:It is micro- that particle diameter less than 5wt% is less than 150
The particle of rice, and 60wt% or the particle diameter more than 60wt% are 500 microns or more than 500 microns and less than 1000 microns
Particle.
4. granular epoxy resin constituent according to claim 1, including:It is micro- that particle diameter less than 3wt% is less than 150
The particle of rice, and 65wt% or the particle diameter more than 65wt% are 500 microns or more than 500 microns and less than 1000 microns
Particle.
5. granular epoxy resin constituent according to claim 1,150 microns of particle is less than without particle diameter.
6. granular epoxy resin constituent according to claim 1, including:Particle diameter less than 20wt% is micro- for 1000
Rice or the particle more than 1000 microns.
7. granular epoxy resin constituent according to claim 1, it is 1000 microns or more than 1000 without particle diameter
The particle of micron.
8. granular epoxy resin constituent according to claim 1, including:It it is 500 microns or more than 500 in particle diameter
Micron and less than among 1000 microns of particle 20% or the particle less than 20% meets equation 2;
<Equation 2>
L/2≤H < L
Wherein L forms the vertical line of the point extremely line (A) tangent with the both ends of the particle of particle exterior contour for connection most
Long length, and H is point the hanging down to the line (A) tangent with the both ends of the particle that connection forms the inside particles profile
The maximum length of straight line.
9. granular epoxy resin constituent according to claim 8, including:It it is 500 microns or more than 500 in particle diameter
Micron and less than among 1000 microns of the particle 15% or the particle less than 15% meets equation 2.
10. a kind of method for encapsulating semiconductor device, including:Compression molding use according to any one of claim 1 to 9
In the granular epoxy resin constituent of encapsulation semiconductor device.
11. a kind of semiconductor device, it is used to encapsulate semiconductor device with according to any one of claim 1 to 9
Granular epoxy resin constituent encapsulates.
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KR10-2016-0056686 | 2016-05-09 | ||
PCT/KR2016/004988 WO2017003087A1 (en) | 2015-06-30 | 2016-05-12 | Granular epoxy resin composition for semiconductor device encapsulation, and semiconductor device encapsulated by using same |
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JP3134791B2 (en) * | 1996-06-28 | 2001-02-13 | 松下電工株式会社 | Granular semiconductor sealing material, method for manufacturing the same, and semiconductor device using the material |
JP4973325B2 (en) | 2007-06-11 | 2012-07-11 | 住友ベークライト株式会社 | Manufacturing method of epoxy resin composition for semiconductor encapsulation and manufacturing method of semiconductor device |
JP2008303368A (en) * | 2007-06-11 | 2008-12-18 | Sumitomo Bakelite Co Ltd | Epoxy resin composition for sealing semiconductor and semiconductor device using the same |
WO2010067538A1 (en) * | 2008-12-10 | 2010-06-17 | 住友ベークライト株式会社 | Granulated epoxy resin composition for semiconductor encapsulation, semiconductor device using same, and method for manufacturing semiconductor device |
JP5090404B2 (en) * | 2009-06-25 | 2012-12-05 | 日東電工株式会社 | Manufacturing method of resin tablet for optical semiconductor sealing, resin tablet for optical semiconductor sealing obtained thereby, and optical semiconductor device using the same |
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JP2000178414A (en) * | 1998-12-16 | 2000-06-27 | Tokuyama Corp | Spherical silica for semiconductor encapsulant |
JP2000313733A (en) * | 1999-04-30 | 2000-11-14 | Sanyo Chem Ind Ltd | Production of spherical resin particle dispersion and spherical resin particle |
CN102246296A (en) * | 2008-12-10 | 2011-11-16 | 住友电木株式会社 | Semiconductor-sealing resin composition, method for producing semiconductor device, and semiconductor device |
CN102325724A (en) * | 2008-12-22 | 2012-01-18 | 电气化学工业株式会社 | Powder, method for producing same, and resin composition containing same |
CN103492483A (en) * | 2011-05-02 | 2014-01-01 | 陶氏环球技术有限责任公司 | Trimethyl borate in epoxy resins |
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KR20170003379A (en) | 2017-01-09 |
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