JP2007217708A - Epoxy resin molding material for sealing and semiconductor device - Google Patents

Abstract

<P>PROBLEM TO BE SOLVED: To provide a sealing epoxy resin molding material having excellent filling properties suitable as an underfill material for flip chip mounting, and a flip chip mounted semiconductor device sealed with the material and having decreased molding failure such as void. <P>SOLUTION: The solid epoxy resin molding material for sealing to be used as an underfill material for flip chip mounting at least contains (A) an epoxy resin, (B) a curing agent and (C) an inorganic filler wherein the inorganic filler C has an average particle diameter of ≤12 μm and a specific surface area of ≥3.0 m<SP>2</SP>/g and satisfies at least one of the conditions that the content of the fraction having a particle diameter of ≤12 μm is ≥50 wt.%, the content of the fraction having a particle diameter of ≤24 μm is ≥70 wt.%, the content of the fraction having a particle diameter of ≤32 μm is ≥80 wt.%, and the content of the fraction having a particle diameter of ≤48 μm is ≥90 wt.%. <P>COPYRIGHT: (C)2007,JPO&INPIT

Description

The present invention relates to a sealing epoxy resin molding material and a semiconductor device.
More specifically, the present invention is an epoxy resin molding material for sealing excellent in fillability suitable as an underfill material for flip chip mounting, and molding defects such as voids sealed thereby, reflow resistance, moisture resistance, etc. The present invention relates to a flip chip mounting type semiconductor device with high reliability.

Conventionally, in the field of element sealing of electronic component devices such as transistors and ICs, resin sealing has been the mainstream in terms of productivity and cost, and epoxy resin molding materials have been widely used. This is because epoxy resins are balanced in various properties such as electrical properties, moisture resistance, heat resistance, mechanical properties, and adhesiveness with inserts. In recent years, high-density mounting of electronic components on printed wiring boards has been progressing. As a result, surface mount packages have become mainstream from conventional pin insertion packages. Surface-mount ICs, LSIs, etc. are thin and small packages in order to increase the mounting density and reduce the mounting height, and the volume occupied by the device package increases, resulting in a very thick package. It has become thinner. In addition, due to the increased functionality and capacity of the elements, the chip area is increased and the number of pins is increased, and further, the pad pitch is reduced and the pad size is reduced by increasing the number of pads (electrodes), so-called narrow pad pitch. Progress is also being made.
In addition, in order to cope with further reduction in size and weight, CSP (Quad Flat Package), SOP (Small Outline Package), etc. are also available for CSPs that can easily accommodate higher pins and can be mounted at higher density. (Chip Size Package
) And BGA (Ball Grid Array). In recent years, these packages have been developed with new structures such as a face-down type, a stacked (stacked) type, a flip chip type, and a wafer level type in order to realize high speed and multiple functions.
Flip chip mounting is a connection technique that replaces the conventional wire bonding, in which solder bumps are attached on the pads of a semiconductor chip and are connected to lands on a wiring board using the bumps. The chip to which the solder bumps are attached is aligned on the wiring board, and then the solder is melted by reflow, and an electrical and mechanical connection is formed through a self-alignment process. In the device mounted in this manner, an underfill material is injected into the gap between the chip / wiring board joined by solder bumps for the purpose of improving various reliability. In order to completely fill the narrow gaps in which the solder bumps are arranged without generating voids or the like, a high filling property is required for the underfill material.

  In order to solve this problem, conventionally, a solvent or solvent-free liquid type epoxy resin molding material for sealing, which is mainly composed of a bisphenol type epoxy resin, is used, and a chip / wiring board is utilized by utilizing a capillary phenomenon. A method of infiltrating and curing the gap has been taken (see, for example, Patent Documents 1 to 3 and Non-Patent Document 1).

JP 2000-260820 A JP 2000-273287 A Japanese Patent Application Laid-Open No. 2002-380483 Supervised by the Surface Mount Council “Practical Flip Chip and Related Chip Scale Technology” Published by Industrial Science Systems, Inc. September 30, 1998, p87

In recent years, from the viewpoint of cost reduction, a novel vacuum type molding technique using a solid-type sealing epoxy resin molding material has been developed for flip chip underfill. However, conventional solid-type molding materials have low filling properties and are difficult to seal without causing defects such as voids.
For example, in the production of next-generation flip-chip type semiconductor devices having fine pitch solder bumps and the like, when sealing using a conventional solid-type sealing epoxy resin, a slightly larger void having a diameter of about 0.1 mm is used. Due to the occurrence, the filling of the underfill part was not satisfactory.
In addition, finer flip-chip mounting semiconductor devices, that is, higher bumpability will be required in the future due to trends such as bump height and bump pitch reduction, and the number of bumps and chip area as the number of inputs and outputs increases. Is done.

Therefore, an epoxy resin molding material for sealing excellent in filling properties suitable as an underfill material for flip chip mounting has been demanded. Further, there has been a demand for a flip chip type semiconductor device having fine pitch solder bumps and the like, which has no molding defects and has high reliability such as reflow resistance and moisture resistance.
According to the first aspect of the present invention, there is provided an epoxy resin molding material for sealing suitable for sealing a flip-chip mounting type semiconductor device having fine pitch bumps and a large number of inputs / outputs (number of bumps). The

  According to the second aspect of the present invention, the flip-chip mounting type has fine pitch bumps sealed with the sealing epoxy resin molding material according to the present invention and has a large number of inputs / outputs (number of bumps). A semiconductor device is provided.

  As a result of intensive studies in order to solve the above-mentioned problems, the inventors have obtained an epoxy resin molding material for sealing for a specific semiconductor device, which contains a specific inorganic filler as an essential component, and has been sealed by this. It has been found that the above object can be achieved by a semiconductor device, and the present invention has been completed.

（ここで、Ｒ¹は水素原子、炭素数１〜６のアルキル基及び炭素数１〜２のアルコキシ基から選ばれ、Ｒ²は炭素数１〜６のアルキル基及びフェニル基から選ばれ、Ｒ³はメチル基又はエチル基を示し、ｎは１〜６の整数を示し、ｍは１〜３の整数を示す。）
９． （Ｅ）リン化合物をさらに含有する請求項１〜８のいずれかに記載の封止用エポキシ樹脂成形材料。
１０． （Ｅ）リン化合物がリン酸エステルを含有する請求項９記載の封止用エポキシ樹脂成形材料。
１１． リン酸エステルが下記一般式（II）で示される化合物を含有する請求項１０記載の封止用エポキシ樹脂成形材料。

（ここで、式中の８個のＲは炭素数１〜４のアルキル基を示し、全て同一でも異なっていてもよい。Ａｒは芳香族環を示す。）
１２． （Ｅ）リン化合物がホスフィンオキサイドを含有する請求項９〜１１のいずれかに記載の封止用エポキシ樹脂成形材料。
１３． ホスフィンオキサイドが下記一般式（III）で示される化合物を含有する請求項１２記載の封止用エポキシ樹脂成形材料。

（ここで、Ｒ^１、Ｒ^２及びＲ^３は炭素数１〜１０の置換又は非置換のアルキル基、アリール基、アラルキル基及び水素原子を示し、すべて同一でも異なってもよい。ただしすべてが水素原子である場合を除く。）
１４． （Ａ）エポキシ樹脂の１５０℃における溶融粘度が２ポイズ以下である請求項１〜１３のいずれかに記載の封止用エポキシ樹脂成形材料。
１５． （Ａ）エポキシ樹脂がビフェニル型エポキシ樹脂、ビスフェノールＦ型エポキシ樹脂、スチルベン型エポキシ樹脂、硫黄原子含有エポキシ樹脂、ノボラック型エポキシ樹脂、ジシクロペンタジエン型エポキシ樹脂、ナフタレン型エポキシ樹脂及びトリフェニルメタン型エポキシ樹脂の少なくとも１種を含有する請求項１〜１４のいずれかに記載の封止用エポキシ樹脂成形材料。
１６． （Ｂ）硬化剤の１５０℃における溶融粘度が２ポイズ以下である請求項１〜１５のいずれかに記載の封止用エポキシ樹脂成形材料。
１７． （Ｂ）硬化剤がビフェニル型フェノール樹脂、アラルキル型フェノール樹脂、ジシクロペンタジエン型フェノール樹脂、トリフェニルメタン型フェノール樹脂及びノボラック型フェノール樹脂の少なくとも１種を含有する請求項１〜１６のいずれかに記載の封止用エポキシ樹脂成形材料。
１８． （Ｆ）硬化促進剤をさらに含有する請求項１〜１７のいずれかに記載の封止用エポキシ樹脂成形材料。
１９． 請求項１〜１８のいずれかに記載の封止用エポキシ樹脂成形材料により封止された半導体装置。
２０． 以下の（ａ１）〜（ｆ１）の構成を１以上を備える請求項１９記載の半導体装置。
（ａ１）フリップチップのバンプ高さが１５０μｍ以下である
（ｂ１）フリップチップのバンプピッチが５００μｍ以下である
（ｃ１）半導体チップの面積が２５ｍｍ²以上である
（ｄ１）封止材の総厚さが２ｍｍ以下である
（ｅ１）フリップチップのバンプ数が１００個以上である
(ｆ１)成型時のエアベント厚みが４０μｍ以下である
２１． 以下の（ａ２）〜（ｆ２）の構成を１以上を備える請求項１９記載の半導体装置。
（ａ２）フリップチップのバンプ高さが１００μｍ以下である
（ｂ２）フリップチップのバンプピッチが４００μｍ以下である
（ｃ２）半導体チップの面積が５０ｍｍ²以上である
（ｄ２）封止材の総厚さが１.５ｍｍ以下である
（ｅ２）フリップチップのバンプ数が１５０個以上である
(ｆ２)成型時のエアベント厚みが３０μｍ以下である That is, the present invention relates to the following description items.
1. (A) an epoxy resin, (B) a curing agent and (C) an epoxy resin molding material for sealing containing at least an inorganic filler,
The said inorganic filler (C) is an epoxy resin molding material for sealing whose average particle diameter is 12 micrometers or less and whose specific surface area is 3.0 m < ² > / g or more.
2. The inorganic filler (C) has a particle size of 12 μm or less and 50 wt. % Or more and a particle size of 24 μm or less is 70 wt. % Or more and a particle diameter of 32 μm or less is 80 wt. % And a particle diameter of 48 μm or less are 90 wt. The epoxy resin molding material for sealing according to claim 1, wherein at least one of the conditions of% or more is satisfied.
3. (C) The epoxy resin molding material for sealing of Claim 1 or 2 whose average particle diameter of an inorganic filler is 10 micrometers or less.
4). (C) The epoxy resin molding material for sealing according to any one of claims 1 to 3, wherein the inorganic filler has a specific surface area of 3.5 to 5.5 m ² / g.
5). The epoxy resin molding material for sealing according to any one of claims 1 to 4, wherein the structure of (a1) to (f1) is used for a semiconductor device having one or more.
(A1) Bump height of flip chip is 150 μm or less (b1) Bump pitch of flip chip is 500 μm or less (c1) Area of semiconductor chip is 25 mm ² or more (d1) Total thickness of sealing material (E1) The number of flip chip bumps is 100 or more.
(f1) The air vent thickness during molding is 40 μm or less. The epoxy resin molding material for sealing according to claim 5, wherein the structure of (a2) to (f2) is used for a semiconductor device including one or more.
(A2) Bump height of flip chip is 100 μm or less (b2) Bump pitch of flip chip is 400 μm or less (c2) Area of semiconductor chip is 50 mm ² or more (d2) Total thickness of sealing material Is 1.5 mm or less (e2) The number of flip chip bumps is 150 or more
(f2) The air vent thickness during molding is 30 μm or less. (D) The epoxy resin molding material for sealing according to any one of claims 1 to 6, further comprising a silane coupling agent having a secondary amino group.
8). (D) The epoxy resin molding material for sealing according to claim 7, wherein the silane coupling agent having a secondary amino group contains a compound represented by the following general formula (I).

(Wherein, R ¹ is selected from a hydrogen atom, an alkyl group and alkoxy group having 1 to 2 carbon atoms of 1 to 6 carbon atoms, R ² is selected from alkyl group and a phenyl group having 1 to 6 carbon atoms, R ³ represents a methyl group or an ethyl group, n represents an integer of 1 to 6, and m represents an integer of 1 to ^3. )
9. (E) The epoxy resin molding material for sealing according to any one of claims 1 to 8, further comprising a phosphorus compound.
10. (E) The epoxy resin molding material for sealing according to claim 9, wherein the phosphorus compound contains a phosphate ester.
11. The epoxy resin molding material for sealing according to claim 10, wherein the phosphate ester contains a compound represented by the following general formula (II).

(Here, 8 R in the formula represent an alkyl group having 1 to 4 carbon atoms, and they may all be the same or different. Ar represents an aromatic ring.)
12 (E) The epoxy resin molding material for sealing in any one of Claims 9-11 in which a phosphorus compound contains a phosphine oxide.
13. The epoxy resin molding material for sealing according to claim 12, wherein the phosphine oxide contains a compound represented by the following general formula (III).

(Here, R ¹ , R ² and R ³ represent a substituted or unsubstituted alkyl group having 1 to 10 carbon atoms, an aryl group, an aralkyl group and a hydrogen atom, which may all be the same or different. Except when it is an atom.)
14 (A) The epoxy resin molding material for sealing according to any one of claims 1 to 13, wherein the epoxy resin has a melt viscosity of 2 poises or less at 150 ° C.
15. (A) Epoxy resin is biphenyl type epoxy resin, bisphenol F type epoxy resin, stilbene type epoxy resin, sulfur atom-containing epoxy resin, novolac type epoxy resin, dicyclopentadiene type epoxy resin, naphthalene type epoxy resin and triphenylmethane type epoxy resin The epoxy resin molding material for sealing according to any one of claims 1 to 14, comprising at least one kind of resin.
16. (B) The epoxy resin molding material for sealing according to any one of claims 1 to 15, wherein the curing viscosity of the curing agent at 150 ° C is 2 poises or less.
17. (B) The curing agent contains at least one of biphenyl type phenol resin, aralkyl type phenol resin, dicyclopentadiene type phenol resin, triphenylmethane type phenol resin and novolak type phenol resin. The epoxy resin molding material for sealing as described.
18. (F) The epoxy resin molding material for sealing according to any one of claims 1 to 17, further comprising a curing accelerator.
19. A semiconductor device sealed with the sealing epoxy resin molding material according to claim 1.
20. 20. The semiconductor device according to claim 19, comprising one or more of the following configurations (a1) to (f1).
(A1) Flip chip bump height is 150 μm or less (b1) Flip chip bump pitch is 500 μm or less (c1) Semiconductor chip area is 25 mm ² or more (d1) Total thickness of sealing material (E1) The number of flip chip bumps is 100 or more.
(f1) The air vent thickness during molding is 40 μm or less. The semiconductor device according to claim 19, comprising one or more of the following configurations (a2) to (f2).
(A2) Bump height of flip chip is 100 μm or less (b2) Bump pitch of flip chip is 400 μm or less (c2) Area of semiconductor chip is 50 mm ² or more (d2) Total thickness of sealing material Is 1.5 mm or less. (E2) The number of flip chip bumps is 150 or more.
(f2) Air vent thickness during molding is 30 μm or less

Furthermore, according to the third aspect of the present invention, there is provided a method of manufacturing a flip-chip mounting type semiconductor device having fine pitch bumps and a large number of inputs / outputs (number of bumps), and a semiconductor device manufactured by the manufacturing method. Provided.
According to the fourth aspect of the present invention, there is provided a method (method) of using an epoxy resin molding material for sealing to a flip-chip mounting type semiconductor device having fine pitch bumps and a large number of inputs / outputs (number of bumps). Provided. That is, the present invention also relates to the following description items.
22. A step of arranging two or more solder bumps on the wiring board at a predetermined bump pitch, a step of providing a semiconductor chip on the wiring board at a predetermined bump height via the solder bumps, the wiring board and the semiconductor A method of manufacturing a semiconductor device having at least a step of sealing a portion including an underfill portion formed between chips using an epoxy resin molding material for sealing,
As the sealing material for sealing the underfill part, the first or second epoxy resin molding material for sealing is used,
The semiconductor device obtained by the manufacturing method includes the following (a1) to (f1):
(A1) Bump height at the time of flip chip mounting is 300 μm or less;
(B1) The bump pitch of the flip chip is 500 μm or less;
(C1) The area of the semiconductor chip is 25 mm ² or more;
(D1) the total thickness of the sealing material is 2 mm or less;
(E1) The flip chip has 100 or more bumps
(f1) A method of manufacturing a semiconductor device, which is a semiconductor device having one or more structures having an air vent thickness of 40 μm or less at the time of molding.
23. The following (a1) to (f1):
(A1) Bump height at the time of flip chip mounting is 300 μm or less;
(B1) The bump pitch of the flip chip is 500 μm or less;
(C1) The area of the semiconductor chip is 25 mm ² or more;
(D1) the total thickness of the sealing material is 2 mm or less;
(E1) The flip chip has 100 or more bumps;
(f1) The air vent thickness at the time of molding is 40 μm or less;
Use (method) of the above-mentioned 1 or 2 sealing epoxy resin molding material as a sealing material of a semiconductor device having one or more of the following structure

  The epoxy resin molding material for sealing for flip chip mounting according to the present invention has a high filling property required as an underfill material, and has few industrial defects such as voids.

(Epoxy resin)
The epoxy resin (A) used in the present invention is generally used for an epoxy resin molding material for sealing and is not particularly limited. For example, phenol novolac type epoxy resin, orthocresol novolac type epoxy resin, triphenyl Phenols such as epoxy resins having a methane skeleton, phenols such as phenol, cresol, xylenol, resorcin, catechol, bisphenol A, bisphenol F and / or naphthols such as α-naphthol, β-naphthol, dihydroxynaphthalene and formaldehyde, acetaldehyde Epoxidized novolak resin obtained by condensation or cocondensation with a compound having an aldehyde group such as propionaldehyde, benzaldehyde, salicylaldehyde, etc. under an acidic catalyst, Glycidyl obtained by reaction of polychlorobasic acid such as diol A, bisphenol F, bisphenol S, diglycidyl ether such as alkyl-substituted or unsubstituted biphenol, stilbene type epoxy resin, hydroquinone type epoxy resin, phthalic acid, dimer acid and epichlorohydrin Ester-type epoxy resin, diaminodiphenylmethane, isocyanuric acid and other polyamines obtained by reaction of epichlorohydrin, glycidylamine-type epoxy resin, epoxidized product of dicyclopentadiene and phenol co-condensation resin, epoxy resin having naphthalene ring, phenol -Epoxidized aralkyl type phenolic resin such as aralkyl resin, naphthol / aralkyl resin, trimethylolpropane type epoxy resin, terpene modified epoxy resin, olefin Examples include linear aliphatic epoxy resins, alicyclic epoxy resins, and sulfur atom-containing epoxy resins obtained by oxidizing a combination with a peracid such as peracetic acid. These may be used alone or in combination of two or more. It may be used.
Among them, biphenyl type epoxy resin, bisphenol F type epoxy resin, stilbene type epoxy resin and sulfur atom-containing epoxy resin are preferable from the viewpoint of filling property and reflow resistance, and novolak type epoxy resin is preferable from the viewpoint of curability, From the viewpoint of low hygroscopicity, dicyclopentadiene type epoxy resin is preferable, and from the viewpoint of heat resistance and low warpage, naphthalene type epoxy resin and triphenylmethane type epoxy resin are preferable, and contains at least one of these epoxy resins It is preferable.

（ここで、Ｒ¹〜Ｒ⁸は水素原子及び炭素数１〜１０の置換又は非置換の一価の炭化水素基から選ばれ、全てが同一でも異なっていてもよい。ｎは０〜３の整数を示す。）

（ここで、Ｒ¹〜Ｒ⁸は水素原子、炭素数１〜１０のアルキル基、炭素数１〜１０のアルコキシル基、炭素数６〜１０のアリール基、及び炭素数６〜１０のアラルキル基から選ばれ、全てが同一でも異なっていてもよい。ｎは０〜３の整数を示す。）

（ここで、Ｒ¹〜Ｒ⁸は水素原子及び炭素数１〜５の置換又は非置換の一価の炭化水素基から選ばれ、全てが同一でも異なっていてもよい。ｎは０〜１０の整数を示す。）

（ここで、Ｒ¹〜Ｒ⁸は水素原子、置換又は非置換の炭素数１〜１０のアルキル基及び置換又は非置換の炭素数１〜１０のアルコキシ基から選ばれ、全てが同一でも異なっていてもよい。ｎは０〜３の整数を示す。）
上記一般式（IV）で示されるビフェニル型エポキシ樹脂としては、たとえば、４，４’−ビス（２，３−エポキシプロポキシ）ビフェニル又は４，４’−ビス（２，３−エポキシプロポキシ）−３，３’，５，５’−テトラメチルビフェニルを主成分とするエポキシ樹脂、エピクロルヒドリンと４，４’−ビフェノール又は４，４’−（３，３’，５，５’−テトラメチル）ビフェノールとを反応させて得られるエポキシ樹脂等が挙げられる。なかでも４，４’−ビス（２，３−エポキシプロポキシ）−３，３’，５，５’−テトラメチルビフェニルを主成分とするエポキシ樹脂が好ましい。
上記一般式（V）で示されるビスフェノールＦ型エポキシ樹脂はとしては、例えば、Ｒ¹、Ｒ³、Ｒ⁶及びＲ⁸がメチル基で、Ｒ²、Ｒ⁴、Ｒ⁵及びＲ⁷が水素原子であり、ｎ＝０を主成分とするＹＳＬＶ−８０ＸＹ（新日鉄化学株式会社製商品名）が市販品として入手可能である。
上記一般式（VI）で示されるスチルベン型エポキシ樹脂は、原料であるスチルベン系フェノール類とエピクロルヒドリンとを塩基性物質存在下で反応させて得ることができる。この原料であるスチルベン系フェノール類としては、たとえば３−ｔ−ブチル−４，４′−ジヒドロキシ−３′，５，５′−トリメチルスチルベン、３−ｔ−ブチル−４，４′−ジヒドロキシ−３′，５′，６−トリメチルスチルベン、４，４’−ジヒドロキシ−３，３’，５，５’−テトラメチルスチルベン、４，４’−ジヒドロキシ−３，３’−ジ−ｔ−ブチル−５，５’−ジメチルスチルベン、４，４’−ジヒドロキシ−３，３’−ジ−ｔ−ブチル−６，６’−ジメチルスチルベン等が挙げられ、なかでも３−ｔ−ブチル−４，４′−ジヒドロキシ−３′，５，５′−トリメチルスチルベン、及び４，４’−ジヒドロキシ−３，３’，５，５’−テトラメチルスチルベンが好ましい。これらのスチルベン型フェノール類は単独で用いても２種以上を組み合わせて用いてもよい。 上記一般式（VII）で示される硫黄原子含有エポキシ樹脂のなかでも、Ｒ²、Ｒ³、Ｒ⁶及びＲ⁷が水素原子で、Ｒ¹、Ｒ⁴、Ｒ⁵及びＲ⁸がアルキル基であるエポキ
シ樹脂が好ましく、Ｒ²、Ｒ³、Ｒ⁶及びＲ⁷が水素原子で、Ｒ¹及びＲ⁸がｔ−ブチル基で、Ｒ⁴及びＲ⁵がメチル基であるエポキシ樹脂がより好ましい。このような化合物としては、ＹＳＬＶ−１２０ＴＥ(新日鐵化学社製)等が市販品として入手可能である。
これらのエポキシ樹脂はいずれか１種を単独で用いても２種以上を組合わせて用いてもよいが、その配合量は、その性能を発揮するためにエポキシ樹脂全量に対して合わせて２０重量％以上とすることが好ましく、３０重量％以上がより好ましく、５０重量％以上とすることがさらに好ましい。 Examples of the biphenyl type epoxy resin include an epoxy resin represented by the following general formula (IV). Examples of the bisphenol F type epoxy resin include an epoxy resin represented by the following general formula (V), and a stilbene type epoxy resin. Examples of the resin include an epoxy resin represented by the following general formula (VI), and examples of the sulfur atom-containing epoxy resin include an epoxy resin represented by the following general formula (VII).

(Here, R ^{1 to} R ⁸ are selected from a hydrogen atom and a substituted or unsubstituted monovalent hydrocarbon group having 1 to 10 carbon atoms, and all may be the same or different. N is 0 to 3. Indicates an integer.)

(Here, R ^{1 to} R ⁸ are a hydrogen atom, an alkyl group having 1 to 10 carbon atoms, an alkoxyl group having 1 to 10 carbon atoms, an aryl group having 6 to 10 carbon atoms, and an aralkyl group having 6 to 10 carbon atoms. All may be the same or different, and n represents an integer of 0 to 3.)

(Here, R ^{1 to} R ⁸ are selected from a hydrogen atom and a substituted or unsubstituted monovalent hydrocarbon group having 1 to 5 carbon atoms, and all may be the same or different. N is 0 to 10. Indicates an integer.)

(Here, R ^{1 to} R ⁸ are selected from a hydrogen atom, a substituted or unsubstituted alkyl group having 1 to 10 carbon atoms, and a substituted or unsubstituted alkoxy group having 1 to 10 carbon atoms, all of which are the same or different. (N represents an integer of 0 to 3.)
Examples of the biphenyl type epoxy resin represented by the general formula (IV) include 4,4′-bis (2,3-epoxypropoxy) biphenyl or 4,4′-bis (2,3-epoxypropoxy) -3. , 3 ′, 5,5′-tetramethylbiphenyl as the main component, epichlorohydrin and 4,4′-biphenol or 4,4 ′-(3,3 ′, 5,5′-tetramethyl) biphenol An epoxy resin obtained by reacting is used. Among these, an epoxy resin mainly composed of 4,4′-bis (2,3-epoxypropoxy) -3,3 ′, 5,5′-tetramethylbiphenyl is preferable.
Examples of the bisphenol F-type epoxy resin represented by the general formula (V) include, for example, R ¹ , R ³ , R ⁶ and R ⁸ are methyl groups, and R ² , R ⁴ , R ⁵ and R ⁷ are hydrogen atoms. YSLV-80XY (trade name, manufactured by Nippon Steel Chemical Co., Ltd.) whose main component is n = 0 is available as a commercial product.
The stilbene type epoxy resin represented by the general formula (VI) can be obtained by reacting a stilbene phenol as a raw material with epichlorohydrin in the presence of a basic substance. Examples of the raw material stilbene phenols include 3-t-butyl-4,4′-dihydroxy-3 ′, 5,5′-trimethylstilbene, 3-t-butyl-4,4′-dihydroxy-3. ', 5', 6-trimethylstilbene, 4,4'-dihydroxy-3,3 ', 5,5'-tetramethylstilbene, 4,4'-dihydroxy-3,3'-di-t-butyl-5 , 5'-dimethylstilbene, 4,4'-dihydroxy-3,3'-di-t-butyl-6,6'-dimethylstilbene and the like, among others, 3-t-butyl-4,4'- Dihydroxy-3 ', 5,5'-trimethylstilbene and 4,4'-dihydroxy-3,3', 5,5'-tetramethylstilbene are preferred. These stilbene type phenols may be used alone or in combination of two or more. Among the sulfur atom-containing epoxy resins represented by the general formula (VII), R ² , R ³ , R ⁶ and R ⁷ are hydrogen atoms, and R ¹ , R ⁴ , R ⁵ and R ⁸ are alkyl groups. An epoxy resin is preferable, and an epoxy resin in which R ² , R ³ , R ⁶ and R ⁷ are hydrogen atoms, R ¹ and R ⁸ are t-butyl groups, and R ⁴ and R ⁵ are methyl groups is more preferable. As such a compound, YSLV-120TE (manufactured by Nippon Steel Chemical Co., Ltd.) and the like are commercially available.
Any one of these epoxy resins may be used alone or in combination of two or more, but the blending amount thereof is 20% in total with respect to the total amount of the epoxy resin in order to exhibit its performance. % Or more, preferably 30% by weight or more, and more preferably 50% by weight or more.

（ここで、Ｒは水素原子及び炭素数１〜１０の置換又は非置換の一価の炭化水素基から選ばれ、ｎは０〜１０の整数を示す。）
上記一般式（VIII）で示されるノボラック型エポキシ樹脂は、ノボラック型フェノール樹脂にエピクロルヒドリンを反応させることによって容易に得られる。なかでも、一般式（VIII）中のＲとしては、メチル基、エチル基、プロピル基、ブチル基、イソプロピル基、イソブチル基等の炭素数１〜１０のアルキル基、メトキシ基、エトキシ基、プロポキシ基、ブトキシ基等の炭素数１〜１０のアルコキシル基が好ましく、水素原子又はメチル基がより好ましい。ｎは０〜３の整数が好ましい。上記一般式（VIII）で示されるノボラック型エポキシ樹脂のなかでも、オルトクレゾールノボラック型エポキシ樹脂が好ましい。
ノボラック型エポキシ樹脂を使用する場合、その配合量は、その性能を発揮するためにエポキシ樹脂全量に対して２０重量％以上とすることが好ましく、３０重量％以上がより好ましい。 Examples of the novolac type epoxy resin include an epoxy resin represented by the following general formula (VIII).

(Here, R is selected from a hydrogen atom and a substituted or unsubstituted monovalent hydrocarbon group having 1 to 10 carbon atoms, and n represents an integer of 0 to 10.)
The novolak type epoxy resin represented by the general formula (VIII) can be easily obtained by reacting a novolak type phenol resin with epichlorohydrin. Among them, R in the general formula (VIII) is an alkyl group having 1 to 10 carbon atoms such as methyl group, ethyl group, propyl group, butyl group, isopropyl group, isobutyl group, methoxy group, ethoxy group, propoxy group. C1-C10 alkoxyl groups, such as a butoxy group, are preferable, and a hydrogen atom or a methyl group is more preferable. n is preferably an integer of 0 to 3. Among the novolak epoxy resins represented by the general formula (VIII), orthocresol novolac epoxy resins are preferable.
In the case of using a novolac type epoxy resin, its blending amount is preferably 20% by weight or more, more preferably 30% by weight or more, based on the total amount of the epoxy resin in order to exhibit its performance.

（ここで、Ｒ¹及びＲ²は水素原子及び炭素数１〜１０の置換又は非置換の一価の炭化水素基からそれぞれ独立して選ばれ、ｎは０〜１０の整数を示し、ｍは０〜６の整数を示す。）
上記式（IX）中のＲ¹としては、たとえば、水素原子、メチル基、エチル基、
プロピル基、ブチル基、イソプロピル基、ｔ−ブチル基等のアルキル基、ビニル基、アリル基、ブテニル基等のアルケニル基、ハロゲン化アルキル基、アミノ基置換アルキル基、メルカプト基置換アルキル基などの炭素数１〜５の置換又は非置換の一価の炭化水素基が挙げられ、なかでもメチル基、エチル基等のアルキル基及び水素原子が好ましく、メチル基及び水素原子がより好ましい。Ｒ²として
は、たとえば、水素原子、メチル基、エチル基、プロピル基、ブチル基、イソプロピル基、ｔ−ブチル基等のアルキル基、ビニル基、アリル基、ブテニル基等のアルケニル基、ハロゲン化アルキル基、アミノ基置換アルキル基、メルカプト基置換アルキル基などの炭素数１〜５の置換又は非置換の一価の炭化水素基が挙げられ、なかでも水素原子が好ましい。
ジシクロペンタジエン型エポキシ樹脂を使用する場合、その配合量は、その性能を発揮するためにエポキシ樹脂全量に対して２０重量％以上とすることが好ましく、３０重量％以上がより好ましい。 Examples of the dicyclopentadiene type epoxy resin include an epoxy resin represented by the following general formula (IX).

(Here, R ¹ and R ² are each independently selected from a hydrogen atom and a substituted or unsubstituted monovalent hydrocarbon group having 1 to 10 carbon atoms, n is an integer of 0 to 10, and m is Represents an integer of 0 to 6.)
R ¹ in the above formula (IX) is, for example, a hydrogen atom, a methyl group, an ethyl group,
Carbon such as alkyl groups such as propyl group, butyl group, isopropyl group and t-butyl group, alkenyl groups such as vinyl group, allyl group and butenyl group, halogenated alkyl group, amino group substituted alkyl group, mercapto group substituted alkyl group Examples thereof include substituted or unsubstituted monovalent hydrocarbon groups of 1 to 5, alkyl group such as methyl group and ethyl group and hydrogen atom are preferable, and methyl group and hydrogen atom are more preferable. Examples of R ² include a hydrogen atom, an alkyl group such as a methyl group, an ethyl group, a propyl group, a butyl group, an isopropyl group, and a t-butyl group, an alkenyl group such as a vinyl group, an allyl group, and a butenyl group, and an alkyl halide. Examples thereof include substituted or unsubstituted monovalent hydrocarbon groups having 1 to 5 carbon atoms such as a group, an amino group-substituted alkyl group, and a mercapto group-substituted alkyl group, and among them, a hydrogen atom is preferable.
When a dicyclopentadiene type epoxy resin is used, its blending amount is preferably 20% by weight or more, more preferably 30% by weight or more based on the total amount of the epoxy resin in order to exhibit its performance.

（ここで、Ｒ¹〜Ｒ³は水素原子及び置換又は非置換の炭素数１〜１２の一価の炭化水素基から選ばれ、それぞれ全てが同一でも異なっていてもよい。ｐは１又は０で、ｌ、ｍはそれぞれ０〜１１の整数であって、（ｌ＋ｍ）が１〜１１の整数でかつ（ｌ＋ｐ）が１〜１２の整数となるよう選ばれる。ｉは０〜３の整数、ｊは０〜２の整数、ｋは０〜４の整数を示す。）
上記一般式（X）で示されるナフタレン型エポキシ樹脂としては、ｌ個の構成単位及びｍ個の構成単位をランダムに含むランダム共重合体、交互に含む交互共重合体、規則的に含む共重合体、ブロック状に含むブロック共重合体が挙げられ、これらのいずれか１種を単独で用いても、２種以上を組み合わせて用いてもよい。

（ここで、Ｒは水素原子及び炭素数１〜１０の置換又は非置換の一価の炭化水素基から選ばれ、ｎは１〜１０の整数を示す。）
これらのエポキシ樹脂はいずれか１種を単独で用いても両者を組合わせて用いてもよいが、その配合量は、その性能を発揮するためにエポキシ樹脂全量に対して合わせて２０重量％以上とすることが好ましく、３０重量％以上がより好ましく、５０重量％以上とすることがさらに好ましい。 Examples of the naphthalene type epoxy resin include an epoxy resin represented by the following general formula (X), and examples of the triphenylmethane type epoxy resin include an epoxy resin represented by the following general formula (XI).

(Here, R ^{1 to} R ³ are selected from a hydrogen atom and a substituted or unsubstituted monovalent hydrocarbon group having 1 to 12 carbon atoms, all of which may be the same or different. P is 1 or 0. And l and m are each an integer of 0 to 11, wherein (l + m) is an integer of 1 to 11 and (l + p) is an integer of 1 to 12. i is an integer of 0 to 3, j represents an integer of 0 to 2, and k represents an integer of 0 to 4.)
As the naphthalene type epoxy resin represented by the general formula (X), a random copolymer containing 1 constituent unit and m constituent units at random, an alternating copolymer containing alternately, a copolymer containing regularly Examples thereof include block copolymers which are included in a combined or block form, and any one of these may be used alone, or two or more may be used in combination.

(Here, R is selected from a hydrogen atom and a substituted or unsubstituted monovalent hydrocarbon group having 1 to 10 carbon atoms, and n represents an integer of 1 to 10.)
These epoxy resins may be used alone or in combination of both, but the blending amount is 20% by weight or more in total with respect to the total amount of the epoxy resin in order to exhibit its performance. Preferably, it is 30% by weight or more, more preferably 50% by weight or more.

  The biphenyl type epoxy resin, stilbene type epoxy resin, sulfur atom-containing epoxy resin, novolac type epoxy resin, dicyclopentadiene type epoxy resin, naphthalene type epoxy resin and triphenylmethane type epoxy resin are used alone. It may be used or two or more types may be used in combination, but the blending amount is preferably 50% by weight or more, more preferably 60% by weight or more, and more preferably 80% by weight or more based on the total amount of the epoxy resin. Is more preferable.

The melt viscosity at 150 ° C. of the (A) epoxy resin used in the present invention is preferably 2 poise or less, more preferably 1 poise or less, and even more preferably 0.5 poise or less from the viewpoint of filling properties. Here, the melt viscosity is a viscosity measured with an ICI cone plate viscometer.

(Curing agent)
The (B) curing agent used in the present invention is generally used for an epoxy resin molding material for sealing and is not particularly limited. For example, phenol, cresol, resorcin, catechol, bisphenol A, bisphenol F, phenyl Phenols such as phenol and aminophenol and / or naphthols such as α-naphthol, β-naphthol, and dihydroxynaphthalene and compounds having an aldehyde group such as formaldehyde, benzaldehyde, and salicylaldehyde are condensed or co-condensed in an acidic catalyst. Aralkyls such as phenol / aralkyl resins and naphthol / aralkyl resins synthesized from novolak-type phenolic resins, phenols and / or naphthols and dimethoxyparaxylene or bis (methoxymethyl) biphenyl Kill-type phenol resin, dichloropentadiene-type phenol resin such as dichloropentadiene-type phenol novolak resin, naphthol novolak resin, terpene-modified phenol resin, etc. synthesized by copolymerization from phenol and / or naphthols and cyclopentadiene, etc. These may be used alone or in combination of two or more.
Among them, biphenyl type phenol resin is preferable from the viewpoint of flame retardancy, aralkyl type phenol resin is preferable from the viewpoint of reflow resistance and curability, and dicyclopentadiene type phenol resin is preferable from the viewpoint of low hygroscopicity, From the viewpoints of heat resistance, low expansion rate and low warpage, a triphenylmethane type phenol resin is preferable, and from the viewpoint of curability, a novolac type phenol resin is preferable, and contains at least one of these phenol resins. Is preferred.

上記式(XII)中のＲ¹〜Ｒ⁹は全てが同一でも異なっていてもよく、水素原子、メチル基、エチル基、プロピル基、ブチル基、イソプロピル基、イソブチル基等の炭素数１〜１０のアルキル基、メトキシ基、エトキシ基、プロポキシ基、ブトキシ基等の炭素数１〜１０のアルコキシル基、フェニル基、トリル基、キシリル基等の炭素数６〜１０のアリール基、及び、ベンジル基、フェネチル基等の炭素数６〜１０のアラルキル基から選ばれ、なかでも水素原子とメチル基が好ましい。ｎは０〜１０の整数を示す。
上記一般式(XII)で示されるビフェニル型フェノール樹脂としては、たとえば
Ｒ¹〜Ｒ⁹が全て水素原子である化合物等が挙げられ、なかでも溶融粘度の観点から、ｎが１以上の縮合体を５０重量％以上含む縮合体の混合物が好ましい。このような化合物としては、ＭＥＨ−７８５１（明和化成株式会社製商品名）が市販品として入手可能である。
ビフェニル型フェノール樹脂を使用する場合、その配合量は、その性能を発揮するために硬化剤全量に対して３０重量％以上とすることが好ましく、５０重量％以上がより好ましく、６０重量％以上がさらに好ましい。 Examples of the biphenyl type phenol resin include a phenol resin represented by the following general formula (XII).

R ^{1 to} R ⁹ in the above formula (XII) may all be the same or different and have 1 to 10 carbon atoms such as a hydrogen atom, a methyl group, an ethyl group, a propyl group, a butyl group, an isopropyl group, and an isobutyl group. An alkyl group, a methoxy group, an ethoxy group, a propoxy group, a butoxy group and the like, an alkoxyl group having 1 to 10 carbon atoms, a phenyl group, a tolyl group, an aryl group having 6 to 10 carbon atoms such as a xylyl group, and a benzyl group, It is selected from aralkyl groups having 6 to 10 carbon atoms such as phenethyl group, and among them, a hydrogen atom and a methyl group are preferable. n represents an integer of 0 to 10.
Examples of the biphenyl type phenol resin represented by the general formula (XII) include compounds in which R ^{1 to} R ⁹ are all hydrogen atoms, and in particular, from the viewpoint of melt viscosity, a condensate having n of 1 or more is used. A mixture of condensates containing 50% by weight or more is preferred. As such a compound, MEH-7851 (trade name, manufactured by Meiwa Kasei Co., Ltd.) is commercially available.
When a biphenyl type phenol resin is used, its blending amount is preferably 30% by weight or more, more preferably 50% by weight or more, and more preferably 60% by weight or more based on the total amount of the curing agent in order to exhibit its performance. Further preferred.

（ここで、Ｒは水素原子及び炭素数１〜１０の置換又は非置換の一価の炭化水素基から選ばれ、ｎは０〜１０の整数を示す。） Examples of the aralkyl-type phenol resin include phenol-aralkyl resins, naphthol-aralkyl resins, etc., and phenol-aralkyl resins represented by the following general formula (XIII) are preferred, and R in the general formula (XIII) is a hydrogen atom. , A phenol / aralkyl resin having an average value of n of 0 to 8 is more preferable. Specific examples include p-xylylene type phenol / aralkyl resins, m-xylylene type phenol / aralkyl resins, and the like. When using these aralkyl type phenol resins, the blending amount is preferably 30% by weight or more, more preferably 50% by weight or more, based on the total amount of the curing agent in order to exhibit the performance.

(Here, R is selected from a hydrogen atom and a substituted or unsubstituted monovalent hydrocarbon group having 1 to 10 carbon atoms, and n represents an integer of 0 to 10.)

（ここで、Ｒ¹及びＲ²は水素原子及び炭素数１〜１０の置換又は非置換の一価の炭化水素基からそれぞれ独立して選ばれ、ｎは０〜１０の整数を示し、ｍは０〜６の整数を示す。）
ジシクロペンタジエン型フェノール樹脂を用いる場合、その配合量は、その性能を発揮するために硬化剤全量に対して３０重量％以上とすることが好ましく、５０重量％以上がより好ましい。 As the dicyclopentadiene type phenol resin, for example, the following general formula (XIV)
The phenol resin etc. which are shown by are mentioned.

(Here, R ¹ and R ² are each independently selected from a hydrogen atom and a substituted or unsubstituted monovalent hydrocarbon group having 1 to 10 carbon atoms, n is an integer of 0 to 10, and m is Represents an integer of 0 to 6.)
When a dicyclopentadiene type phenol resin is used, its blending amount is preferably 30% by weight or more, more preferably 50% by weight or more, based on the total amount of the curing agent in order to exhibit its performance.

（ここで、Ｒは水素原子及び炭素数１〜１０の置換又は非置換の一価の炭化水素基から選ばれ、ｎは１〜１０の整数を示す。）
トリフェニルメタン型フェノール樹脂を用いる場合、その配合量は、その性能を発揮するために硬化剤全量に対して３０重量％以上とすることが好ましく、５０重量％以上がより好ましい。 Examples of the triphenylmethane type phenol resin include a phenol resin represented by the following general formula (XV).

(Here, R is selected from a hydrogen atom and a substituted or unsubstituted monovalent hydrocarbon group having 1 to 10 carbon atoms, and n represents an integer of 1 to 10.)
When using a triphenylmethane type phenol resin, the blending amount is preferably 30% by weight or more, more preferably 50% by weight or more, based on the total amount of the curing agent in order to exhibit its performance.

  Examples of the novolak type phenol resin include a phenol novolak resin, a cresol novolak resin, a naphthol novolak resin, and the like. Among these, a phenol novolak resin is preferable. In the case of using a novolac type phenol resin, the blending amount is preferably 30% by weight or more, more preferably 50% by weight or more based on the total amount of the curing agent in order to exhibit its performance.

  The above biphenyl type phenol resin, aralkyl type phenol resin, dicyclopentadiene type phenol resin, triphenylmethane type phenol resin and novolac type phenol resin may be used alone or in combination of two or more. However, the blending amount is preferably 60% by weight or more, more preferably 80% by weight or more, based on the total amount of the curing agent.

  The melt viscosity at 150 ° C. of the (B) curing agent used in the present invention is preferably 2 poises or less, more preferably 1 poise or less from the viewpoint of filling properties. Here, melt viscosity indicates ICI viscosity.

  The equivalent ratio of (A) epoxy resin and (B) curing agent, that is, the ratio of the number of hydroxyl groups in the curing agent to the number of epoxy groups in the epoxy resin (number of hydroxyl groups in the curing agent / number of epoxy groups in the epoxy resin) is: Although there is no restriction | limiting in particular, In order to suppress each unreacted part small, it is preferable to set to the range of 0.5-2, and 0.6-1.3 are more preferable. In order to obtain a sealing epoxy resin molding material excellent in moldability and reflow resistance, it is more preferably set in the range of 0.8 to 1.2.

(Inorganic filler)
The (C) inorganic filler used in the present invention is blended in the epoxy resin molding material for sealing in order to absorb moisture, reduce the coefficient of linear expansion, improve thermal conductivity, and improve strength. For example, fused silica , Crystalline silica, alumina, zircon, calcium silicate, calcium carbonate, potassium titanate, silicon carbide, silicon nitride, aluminum nitride, boron nitride, beryllia, zirconia, zircon, fosterite, steatite, spinel, mullite, titania, etc. Examples thereof include beads or glass fibers formed by spheroidizing these bodies. Furthermore, examples of the inorganic filler having a flame retardant effect include aluminum hydroxide, magnesium hydroxide, zinc borate, and zinc molybdate.
These inorganic fillers may be used alone or in combination of two or more. Of these, fused silica is preferable from the viewpoint of filling property and linear expansion coefficient, and alumina is preferable from the viewpoint of high thermal conductivity, and the shape of the inorganic filler is preferably spherical from the viewpoint of filling property and mold wear.

(C) Inorganic filler used in the present invention has an average particle size of 15 μm or less and a specific surface area of 3.0 to 6.0 m ² / g. It is necessary from the viewpoint of satisfying the filling property. The average particle size is more preferably 10 μm or less, and still more preferably 8 μm or less. When the thickness exceeds 15 μm, it becomes difficult to inject the epoxy resin molding material into the gap between the chip / wiring board bonded by the bump, and the filling property is lowered. The specific surface area is more preferably 3.5 to 5.5 m ² / g, and still more preferably 4.0 to 5.0 m ² / g. If it is less than 3.0 m ² / g or more than 6.0 m ² / g, voids are likely to be generated in the gap between the chip / wiring board bonded by the bump, and the filling property is lowered.
Further, from the viewpoint of filling properties, coarse particles of (C) inorganic filler may be cut with a sieve. At this time, the component (C) of 53 μm or more is preferably 0.5% by weight or less, the component (C) of 30 μm or more is more preferably 0.5% by weight or less, and the component (C) of 20 μm or more. Is more preferably 0.5% by weight or less.
(C) As for the compounding quantity of an inorganic filler, 60 to 95 weight% is preferable with respect to the epoxy resin molding material for sealing from a viewpoint of a filling property and reliability. 70 to 90% by weight is more preferable, and 75 to 85% by weight is more preferable. If it is less than 60% by weight, the reflow resistance tends to be lowered, and if it exceeds 95% by weight, the filling property tends to be lowered.

(Silane coupling agent having secondary amino group)
The (D) silane coupling agent having a secondary amino group used in the present invention is not particularly limited as long as it is a silane compound having a secondary amino group in the molecule. For example, γ-anilinopropyltrimethoxysilane, γ-anilinopropyltriethoxysilane, γ-anilinopropylmethyldimethoxysilane, γ-anilinopropylmethyldiethoxysilane, γ-anilinopropylethyldiethoxysilane, γ-anilinopropylethyldimethoxysilane, γ-aniline Linomethyltrimethoxysilane, γ-anilinomethyltriethoxysilane, γ-anilinomethylmethyldimethoxysilane, γ-anilinomethylmethyldiethoxysilane, γ-anilinomethylethyldiethoxysilane, γ-anilinomethylethyl Dimethoxysilane, N- (p-methoxyphenyl -Γ-aminopropyltrimethoxysilane, N- (p-methoxyphenyl) -γ-aminopropyltriethoxysilane, N- (p-methoxyphenyl) -γ-aminopropylmethyldimethoxysilane, N- (p-methoxyphenyl) ) -Γ-aminopropylmethyldiethoxysilane, N- (p-methoxyphenyl) -γ-aminopropylethyldiethoxysilane, N- (p-methoxyphenyl) -γ-aminopropylethyldimethoxysilane, γ- (N -Methyl) aminopropyltrimethoxysilane, γ- (N-ethyl) aminopropyltrimethoxysilane, γ- (N-butyl) aminopropyltrimethoxysilane, γ- (N-benzyl) aminopropyltrimethoxysilane, γ- (N-methyl) aminopropyltriethoxysilane, γ- (N-ethyl) ) Aminopropyltriethoxysilane, γ- (N-butyl) aminopropyltriethoxysilane, γ- (N-benzyl) aminopropyltriethoxysilane, γ- (N-methyl) aminopropylmethyldimethoxysilane, γ- (N -Ethyl) aminopropylmethyldimethoxysilane, γ- (N-butyl) aminopropylmethyldimethoxysilane, γ- (N-benzyl) aminopropylmethyldimethoxysilane, N-β- (aminoethyl) -γ-aminopropyltrimethoxy Examples include silane, γ- (β-aminoethyl) aminopropyltrimethoxysilane, N-β- (N-vinylbenzylaminoethyl) -γ-aminopropyltrimethoxysilane, and the like.

（ここで、Ｒ¹は水素原子、炭素数１〜６のアルキル基及び炭素数１〜２のアル
コキシ基から選ばれ、Ｒ²は炭素数１〜６のアルキル基及びフェニル基から選ば
れ、Ｒ³はメチル基又はエチル基を示し、ｎは１〜６の整数を示し、ｍは１〜３
の整数を示す。）
上記一般式（I）で示されるアミノシランカップリング剤としては、たとえばγ−アニリノプロピルトリメトキシシラン、γ−アニリノプロピルトリエトキシシラン、γ−アニリノプロピルメチルジメトキシシラン、γ−アニリノプロピルメチルジエトキシシラン、γ−アニリノプロピルエチルジエトキシシラン、γ−アニリノプロピルエチルジメトキシシラン、γ−アニリノメチルトリメトキシシラン、γ−アニリノメチルトリエトキシシラン、γ−アニリノメチルメチルジメトキシシラン、γ−アニリノメチルメチルジエトキシシラン、γ−アニリノメチルエチルジエトキシシラン、γ−アニリノメチルエチルジメトキシシラン、Ｎ−（ｐ−メトキシフェニル）−γ−アミノプロピルトリメトキシシラン、Ｎ−（ｐ−メトキシフェニル）−γ−アミノプロピルトリエトキシシラン、Ｎ−（ｐ−メトキシフェニル）−γ−アミノプロピルメチルジメトキシシラン、Ｎ−（ｐ−メトキシフェニル）−γ−アミノプロピルメチルジエトキシシラン、Ｎ−（ｐ−メトキシフェニル）−γ−アミノプロピルエチルジエトキシシラン、Ｎ−（ｐ−メトキシフェニル）−γ−アミノプロピルエチルジメトキシシラン等が挙げられる。特に好ましくは、γ−アニリノプロピルトリメトキシシランである。 Of these, aminosilane coupling agents represented by the following general formula (I) are preferred from the viewpoint of filling properties.

(Here, R ¹ is selected from a hydrogen atom, an alkyl group having 1 to 6 carbon atoms and an alkoxy group having 1 to ² carbon atoms, R ² is selected from an alkyl group having 1 to 6 carbon atoms and a phenyl group; ³ represents a methyl group or an ethyl group, n represents an integer of 1 to 6, and m represents 1 to 3
Indicates an integer. )
Examples of the aminosilane coupling agent represented by the general formula (I) include γ-anilinopropyltrimethoxysilane, γ-anilinopropyltriethoxysilane, γ-anilinopropylmethyldimethoxysilane, and γ-anilinopropylmethyl. Diethoxysilane, γ-anilinopropylethyldiethoxysilane, γ-anilinopropylethyldimethoxysilane, γ-anilinomethyltrimethoxysilane, γ-anilinomethyltriethoxysilane, γ-anilinomethylmethyldimethoxysilane, γ-anilinomethylmethyldiethoxysilane, γ-anilinomethylethyldiethoxysilane, γ-anilinomethylethyldimethoxysilane, N- (p-methoxyphenyl) -γ-aminopropyltrimethoxysilane, N- (p -Methoxyphenyl) -γ-amino Propyltriethoxysilane, N- (p-methoxyphenyl) -γ-aminopropylmethyldimethoxysilane, N- (p-methoxyphenyl) -γ-aminopropylmethyldiethoxysilane, N- (p-methoxyphenyl) -γ -Aminopropylethyldiethoxysilane, N- (p-methoxyphenyl) -γ-aminopropylethyldimethoxysilane and the like. Particularly preferred is γ-anilinopropyltrimethoxysilane.

  (D) It is preferable that the compounding quantity of the silane coupling agent which has a secondary amino group is 0.037 to 4.75 weight% with respect to the epoxy resin molding material for sealing, and 0.088 to 2.3. More preferably, it is% by weight. If it is less than 0.037% by weight, the fluidity is lowered, and there is a tendency that molding defects such as voids are likely to occur, and the adhesion to the wiring board tends to be lowered. If it exceeds 4.75% by weight, the volatile matter increases, and there is a tendency that molding defects such as voids are likely to occur, and the moldability of the package tends to be lowered.

In order to improve the adhesiveness between the resin component and the filler, it is preferable to add a coupling agent to the sealing epoxy resin molding material of the present invention. As the coupling agent, (D) a silane coupling agent having a secondary amino group is preferable, but other coupling agents can be used in combination within the range in which the effects of the present invention can be achieved.
(D) Other coupling agents that can be used in combination with a silane coupling agent having a secondary amino group are generally used in epoxy resin molding materials for sealing and are not particularly limited. Various silane compounds such as silane compounds having epoxy groups and / or tertiary amino groups, epoxy silanes, mercapto silanes, alkyl silanes, phenyl silanes, ureido silanes, vinyl silanes, titanium compounds, aluminum chelates, aluminum / zirconium compounds, etc. Is mentioned. Examples of these are vinyltrichlorosilane, vinyltriethoxysilane, vinyltris (β-methoxyethoxy) silane, γ-methacryloxypropyltrimethoxysilane, β- (3,4-epoxycyclohexyl) ethyltrimethoxysilane, γ-glycol. Sidoxypropyltrimethoxysilane, γ-glycidoxypropylmethyldimethoxysilane, vinyltriacetoxysilane, γ-mercaptopropyltrimethoxysilane, γ-aminopropyltrimethoxysilane, γ-aminopropylmethyldimethoxysilane, γ-aminopropyl Triethoxysilane, γ-aminopropylmethyldiethoxysilane, γ- (N, N-dimethyl) aminopropyltrimethoxysilane, γ- (N, N-diethyl) aminopropyltrimethoxysilane, γ- (N, N Dibutyl) aminopropyltrimethoxysilane, γ- (N-methyl) anilinopropyltrimethoxysilane, γ- (N-ethyl) anilinopropyltrimethoxysilane, γ- (N, N-dimethyl) aminopropyltriethoxysilane , Γ- (N, N-diethyl) aminopropyltriethoxysilane, γ- (N, N-dibutyl) aminopropyltriethoxysilane, γ- (N-methyl) anilinopropyltriethoxysilane, γ- (N- Ethyl) anilinopropyltriethoxysilane, γ- (N, N-dimethyl) aminopropylmethyldimethoxysilane, γ- (N, N-diethyl) aminopropylmethyldimethoxysilane, γ- (N, N-dibutyl) aminopropyl Methyldimethoxysilane, γ- (N-methyl) anilinopropylmethyldimethoxysilane , Γ- (N-ethyl) anilinopropylmethyldimethoxysilane, N- (trimethoxysilylpropyl) ethylenediamine, N- (dimethoxymethylsilylisopropyl) ethylenediamine, methyltrimethoxysilane, dimethyldimethoxysilane, methyltriethoxysilane, Silane coupling agents such as γ-chloropropyltrimethoxysilane, hexamethyldisilane, vinyltrimethoxysilane, γ-mercaptopropylmethyldimethoxysilane, isopropyltriisostearoyl titanate, isopropyltris (dioctylpyrophosphate) titanate, isopropyltri ( N-aminoethyl-aminoethyl) titanate, tetraoctyl bis (ditridecyl phosphite) titanate, tetra (2,2-diallyloxime) Til-1-butyl) bis (ditridecyl) phosphite titanate, bis (dioctylpyrophosphate) oxyacetate titanate, bis (dioctylpyrophosphate) ethylene titanate, isopropyltrioctanoyl titanate, isopropyldimethacrylisostearoyl titanate, isopropyltridodecylbenzene Titanate coupling agents such as sulfonyl titanate, isopropyl isostearoyl diacryl titanate, isopropyl tri (dioctyl phosphate) titanate, isopropyl tricumyl phenyl titanate, tetraisopropyl bis (dioctyl phosphite) titanate, and the like. It may be used alone or in combination of two or more.

When these other coupling agents are used, the blending amount of the (D) silane coupling agent having a secondary amino group may be 30% by weight or more based on the total amount of the coupling agent in order to exhibit its performance. Preferably, 50 weight% or more is more preferable.
The total amount of the coupling agent including the (D) silane coupling agent having a secondary amino group is preferably 0.037 to 4.75% by weight based on the epoxy resin molding material for sealing, It is more preferable that it is 0.088-2.3 weight%. If it is less than 0.037% by mass, the adhesiveness to the wiring board tends to decrease, and if it exceeds 4.75% by mass, the volatile matter tends to increase, and there is a tendency that molding defects such as voids are likely to occur. There is a tendency for the moldability of the package to decrease. In addition, it is preferable that the compounding quantity of the said coupling agent is 0.05 to 5 weight% with respect to (C) inorganic filler, and 0.1 to 2.5 weight% is more preferable. The reason for defining the blending amount is the same as described above.
(Coupling agent coverage)
When using a coupling agent in this invention, it is preferable that the coverage of the coupling agent to an inorganic filler shall be 0.3-1.0, More preferably, it is 0.4-0.9, More preferably, it is 0. It is convenient to set it in the range of 0.5 to 0.8. When the coverage of the coupling agent is greater than 1.0, bubbles due to volatile components generated during molding tend to increase, and voids in the thin portion tend to be generated. Moreover, since the adhesive force of resin and a filler falls when the coverage of a coupling agent is smaller than 0.3, there exists a tendency for a molded article strength to fall.
The coupling agent coverage X of the epoxy resin molding material is defined as in the formula (xxx).
X (%) = S _c / S _f (xxx)
S _c and S _f represent the total minimum covering area of all coupling agents and the total surface area of all fillers in the epoxy resin molding material, respectively, and are defined by the equations (yyy) and (zzz).
_{S c = A 1 × W 1} + A 2 × W 2 + ... + A n × M n (n is used coupling agent number seed) (yyy)
S _f = B ₁ × W ₁ + B ₂ × W ₂ +... + B _l × W _l (l is the number of fillers used) (zzz)
Here, A and M represent the minimum coating area of each coupling agent and the amount of use thereof, and B and W represent the specific surface area of each filler and the amount of use thereof, respectively.
(Coupling agent coverage control method)
If the minimum coating area and specific surface area of each coupling agent and inorganic filler used in the epoxy resin molding material are known, the desired coupling agent can be obtained from the formula (xxx), (yyy) and (zzz). It is possible to calculate the amount of the coupling agent and the filler used for the coverage.

（ここで、式中の８個のＲは炭素数１〜４のアルキル基を示し、全て同一でも異なっていてもよい。Ａｒは芳香族環を示す。）
上記式（II）のリン酸エステルを例示すると、下記構造式（XVI）〜 （XX）で示されるリン酸エステル等が挙げられる。

(Phosphorus compound)
From the viewpoint of filling properties and flame retardancy, in the present invention, it is preferable to further blend (E) a phosphorus compound. Although there is no restriction | limiting in particular as (E) phosphorus compound used in this invention, Phosphate ester and a phosphine oxide are preferable from a moisture resistant reliability viewpoint.
The phosphate ester is not particularly limited as long as it is an ester compound of phosphoric acid and an alcohol compound or a phenol compound. For example, trimethyl phosphate, triethyl phosphate, triphenyl phosphate, tricresyl phosphate, trixylenyl phosphate, cresyl diphenyl phosphate, Examples include xylenyl diphenyl phosphate, tris (2,6-dimethylphenyl) phosphate, and aromatic condensed phosphate ester. Of these, an aromatic condensed phosphate represented by the following general formula (II) is preferred from the viewpoint of hydrolysis resistance.

(Here, 8 R in the formula represent an alkyl group having 1 to 4 carbon atoms, and they may all be the same or different. Ar represents an aromatic ring.)
Examples of the phosphate ester of the above formula (II) include phosphate esters represented by the following structural formulas (XVI) to (XX).

It is preferable that the addition amount of these phosphate ester exists in the range of 0.2-3.0 mass% in the quantity of a phosphorus atom with respect to all the other compounding components except a filler. When it is less than 0.2% by mass, the filling property is lowered, and molding defects such as voids are likely to occur. In addition, the flame retardant effect tends to be low. If it exceeds 3.0% by mass, the formability and moisture resistance may be deteriorated, and these phosphate esters may ooze out during molding, thereby impairing the appearance.

（ここで、Ｒ^１、Ｒ^２及びＲ^３は炭素数１〜１０の置換又は非置換のアルキル基、アリール基、アラルキル基及び水素原子を示し、すべて同一でも異なってもよい。ただしすべてが水素原子である場合を除く。）
上記一般式（Ｉ）で示されるリン化合物の中でも、耐加水分解性の観点からはＲ^１〜Ｒ^３が置換又は非置換のアリール基であることが好ましく、特に好ましくはフェニル基である。 As the phosphine oxide, a compound represented by the following general formula (III) is preferable.

(Here, R ¹ , R ² and R ³ represent a substituted or unsubstituted alkyl group having 1 to 10 carbon atoms, an aryl group, an aralkyl group and a hydrogen atom, which may all be the same or different. Except when it is an atom.)
Among the phosphorus compounds represented by the above general formula (I), R ^{1 to} R ³ are preferably substituted or unsubstituted aryl groups, particularly preferably phenyl groups, from the viewpoint of hydrolysis resistance.

    The amount of phosphine oxide is required to be 0.01 to 0.2% by weight of phosphorus atoms with respect to the epoxy resin molding material for sealing. Preferably it is 0.02 to 0.1 weight%, More preferably, it is 0.03 to 0.08 weight%. If it is less than 0.01% by weight, the flame retardancy is lowered, and if it exceeds 0.2% by weight, the moldability and moisture resistance are lowered.

(Curing accelerator)
From the viewpoint of curability, in the present invention, it is preferable to further blend (F) a curing accelerator. The (F) curing accelerator used in the present invention is not particularly limited as long as it is generally used in an epoxy resin molding material for sealing. For example, 1,8-diaza-bicyclo (5,4, 0) cycloamidine such as undecene-7, 1,5-diaza-bicyclo (4,3,0) nonene, 5,6-dibutylamino-1,8-diaza-bicyclo (5,4,0) undecene-7 Compounds and these compounds include maleic anhydride, 1,4-benzoquinone, 2,5-toluquinone, 1,4-naphthoquinone, 2,3-dimethylbenzoquinone, 2,6-dimethylbenzoquinone, 2,3-dimethoxy-5 Quinone compounds such as methyl-1,4-benzoquinone, 2,3-dimethoxy-1,4-benzoquinone, phenyl-1,4-benzoquinone, diazophenylmethane, Compounds having intramolecular polarization formed by adding a compound having a π bond such as a vinyl resin, tertiary amines such as benzyldimethylamine, triethanolamine, dimethylaminoethanol, tris (dimethylaminomethyl) phenol, and the like Derivatives, imidazoles such as 2-methylimidazole, 2-phenylimidazole, 2-phenyl-4-methylimidazole and their derivatives, tributylphosphine, methyldiphenylphosphine, triphenylphosphine, tris (4-methylphenyl) phosphine, diphenyl Organic phosphines such as phosphine and phenylphosphine, and intramolecular polarization formed by adding π-bonded compounds such as maleic anhydride, quinone compounds, diazophenylmethane, and phenolic resins to these phosphines Examples include phosphorus compounds, tetraphenylphosphonium tetraphenylborate, triphenylphosphine tetraphenylborate, tetraphenylboron salts such as 2-ethyl-4-methylimidazole tetraphenylborate, N-methylmorpholine tetraphenylborate, and derivatives thereof. These may be used alone or in combination of two or more. Among these, an adduct of an organic phosphine and a quinone compound is preferable from the viewpoint of filling property and reflow resistance.

  The blending amount of the curing accelerator is not particularly limited as long as the curing acceleration effect is achieved, but is preferably 0.005 to 2% by weight, more preferably based on the epoxy resin molding material for sealing. Is 0.01 to 0.5% by weight. If it is less than 0.005% by weight, the curability in a short time tends to be inferior, and if it exceeds 2% by weight, the curing rate tends to be too high and it tends to be difficult to obtain a good molded product.

(Flame retardants)
Various flame retardants may be further added to the present invention from the viewpoint of flame retardancy. The flame retardant is generally used for an epoxy resin molding material for sealing and is not particularly limited. For example, a brominated epoxy resin such as a diglycidyl etherified product of tetrabromobisphenol A or a brominated phenol novolac epoxy resin. Phosphorus compounds such as antimony oxide, red phosphorus and the above-mentioned phosphate esters, melamine, melamine cyanurate, nitrogen-containing compounds such as melamine-modified phenol resin and guanamine-modified phenol resin, phosphorus / nitrogen-containing compounds such as cyclophosphazene, zinc oxide, Examples thereof include metal compounds such as iron oxide, molybdenum oxide, ferrocene, the above aluminum hydroxide, magnesium hydroxide, and composite metal hydroxide.
Non-halogen and non-antimony flame retardants are preferable from the viewpoint of environmental problems in recent years and high temperature storage characteristics. Among these, phosphate esters are preferable from the viewpoint of filling properties, and composite metal hydroxides are preferable from the viewpoints of safety and moisture resistance.

The composite metal hydroxide is preferably a compound represented by the following composition formula (XXI).
p (M ¹ aOb) · q (M ² cOd) · r (M ³ cOd) · mH ₂ O (XXI)
(Here, M ¹ , M ² and M ³ represent different metal elements, and a, b, c, d, p,
q and m are positive numbers, and r is 0 or a positive number. )
Especially, the compound whose r in the said composition formula (XXI) is 0, ie, the compound shown by the following composition formula (XXIa), is further more preferable.
m (M ¹ aOb) · n (M ² cOd) · l (H ₂ O) (XXIa)
(Here, M ¹ and M ² represent different metal elements, and a, b, c, d, m, n, and l represent positive numbers.)
M ¹ and M ^{2 in the} above composition formulas (XXI) and (XXIa) are not particularly limited as long as they are different metal elements, but from the viewpoint of flame retardancy, M ¹ and M ² should not be the same. M ¹ is selected from metal elements belonging to the third period, Group IIA alkaline earth metal elements, Group IVB, Group IIB, Group VIII, Group IB, Group IIIA and Group IVA, and M ² is selected from IIIB to IIB. Is preferably selected from the group transition metal elements, M ¹ is selected from magnesium, calcium, aluminum, tin, titanium, iron, cobalt, nickel, copper and zinc, and M ² is iron, cobalt, nickel, copper and zinc More preferably, it is chosen from. From the viewpoint of fluidity, M ¹ is preferably magnesium and M ² is preferably zinc or nickel, more preferably M ¹ is magnesium and M ² is zinc. The molar ratio of p, q, and r in the composition formula (XXI) is not particularly limited as long as the effect of the present invention can be obtained, but r = 0, and the molar ratio p / q of p and q is 99/1 to Preferably it is 50/50. That is, the molar ratio m / n of m and n in the composition formula (XXIa) is preferably 99/1 to 50/50.
In addition, the classification of metal elements is a long-period type periodic rate table in which the typical element is the A subgroup and the transition element is the B subgroup (Source: Kyoritsu Shuppan Co., Ltd., “Chemical Dictionary 4”, February 15, 1987) (Reduced plate 30th printing).
The shape of the composite metal hydroxide is not particularly limited, but from the viewpoint of fluidity and filling properties, a polyhedral shape having an appropriate thickness is preferable to a flat plate shape. Compared to metal hydroxides, complex metal hydroxides tend to give polyhedral crystals.
Although the compounding quantity of a composite metal hydroxide does not have a restriction | limiting in particular, 0.5-20 weight% is preferable with respect to the epoxy resin molding material for sealing, 0.7-15 weight% is more preferable, 1.4- 12% by weight is more preferred. If it is less than 0.5% by weight, the flame retardancy tends to be insufficient, and if it exceeds 20% by weight, the filling property and reflow resistance tend to be lowered.

(Heating loss rate)
The heat loss rate of the epoxy resin molding material is essentially 0.25% by mass or less, preferably 0.22% by mass or less, and more preferably 0.20% by mass or less. When the heating weight loss rate exceeds 0.25% by mass, bubbles due to volatile matter generated during molding increase, and voids in the thin portion are likely to occur.
(Definition of heating loss rate)
A weight W ₀ obtained by adding the resin composition to a heat-resistant container of weight A is measured. This is left to stand at 200 ° C. for 1 hour, and then the total weight W of the container and the resin composition is measured. At this time, the heating loss rate Y is obtained by the following equation.
Y = 100 × (W ₀ −W) / (W ₀ −A)
(Control method of heating loss rate)
Volatile components generated at the time of measuring the heating loss rate are mainly moisture and alcohols. Therefore, it is effective to reduce the moisture content of the pre-molded epoxy resin molding material, optimize the coupling agent to the minimum required amount, use a coupling agent that hardly generates volatile components, and the like.

The sealing epoxy resin molding material according to the present invention will be further described with some preferred embodiments.
(First aspect)
As a first preferred embodiment of the epoxy resin molding material for sealing according to the present invention, (A) an epoxy resin, (B) a curing agent, (C) an average particle size of 12 μm or less, and a specific surface area of 3.0 m ² / An epoxy resin molding material for sealing containing an inorganic filler that is at least g is mentioned. In this case, other additives may be added as desired. By adjusting the combination and blending amount of each component, a flip chip mounting type epoxy resin molding material for sealing underfill can be obtained. Of these, (A) an epoxy resin, (B) a curing agent, (C) selection of an inorganic filler having an average particle size of 12 μm or less and a specific surface area of 3.0 m ² / g or more and its blending amount are particularly important. is there.
(Second aspect)
As a second preferred embodiment of the epoxy resin molding material for sealing according to the present invention, (A) an epoxy resin, (B) a curing agent, (C) an average particle size of 12 μm or less, and a specific surface area of 3.0 m ² / Examples include an epoxy resin molding material for sealing containing an inorganic filler that is g or more, and (D) a silane coupling agent having a secondary amino group. In this case, other additives may be added as desired. By adjusting the combination and blending amount of each component, a flip chip mounting type epoxy resin molding material for sealing underfill can be obtained. Among them, (A) an epoxy resin, (B) a curing agent, (C) an inorganic filler having an average particle size of 12 μm or less, a specific surface area of 3.0 m ² / g or more, and (D) a secondary amino group. The selection and blending amount of the silane coupling agent is particularly important.
(Third aspect)
As a third preferred embodiment of the epoxy resin molding material for sealing according to the present invention, (A) an epoxy resin, (B) a curing agent, (C) an average particle size of 12 μm or less, and a specific surface area of 3.0 m ² / Examples include an inorganic filler that is g or more, (D) a silane coupling agent having a secondary amino group, and (E) an epoxy resin molding material for sealing containing a curing accelerator. In this case, other additives may be added as desired. By adjusting the combination and blending amount of each component, a flip chip mounting type epoxy resin molding material for sealing underfill can be obtained. Among them, (A) an epoxy resin, (B) a curing agent, (C) an inorganic filler having an average particle size of 12 μm or less, a specific surface area of 3.0 m ² / g or more, and (D) a secondary amino group. The selection and blending amount of the silane coupling agent and (E) curing accelerator are particularly important.

(Fourth aspect)
As a fourth preferred embodiment of the epoxy resin molding material for sealing according to the present invention, (A) an epoxy resin, (B) a curing agent, and (C) a maximum particle size of 63 μm or less and a particle size of 20 μm or more are 5 wt. An epoxy resin molding material for sealing containing at least% inorganic filler can be mentioned. In this case, other additives may be added as desired. By adjusting the combination and blending amount of each component, a flip chip mounting type epoxy resin molding material for sealing underfill can be obtained. Among them, (A) an epoxy resin, (B) a curing agent, (C) a maximum particle size of 63 μm or less, and a particle size of 20 μm or more is 5 wt. It is particularly important to select an inorganic filler of at least% and its blending amount.

(5th aspect)
As a fifth preferred embodiment of the epoxy resin molding material for sealing according to the present invention, (A) an epoxy resin, (B) a curing agent, (C) a maximum particle size of 63 μm or less, and a particle size of 20 μm or more is 5 wt. . An epoxy resin molding material for sealing containing at least% inorganic filler and (D) a silane coupling agent having a secondary amino group. In this case, other additives may be added as desired. By adjusting the combination and blending amount of each component, a flip chip mounting type epoxy resin molding material for sealing underfill can be obtained. Among them, (A) an epoxy resin, (B) a curing agent, (C) a maximum particle size of 63 μm or less, and a particle size of 20 μm or more is 5 wt. It is particularly important to select and compound the amount of inorganic fillers of at least% and (D) a silane coupling agent having a secondary amino group.

(Sixth aspect)
As a sixth preferred embodiment of the sealing epoxy resin molding material according to the present invention, (A) an epoxy resin, (B) a curing agent, (C) a maximum particle size of 63 μm or less, and a particle size of 20 μm or more is 5 wt. . % Or more inorganic filler, (D) a silane coupling agent having a secondary amino group, and (E) an epoxy resin molding material for sealing containing a curing accelerator. In this case, other additives may be added as desired. By adjusting the combination and blending amount of each component, a flip chip mounting type epoxy resin molding material for sealing underfill can be obtained. Among them, (A) an epoxy resin, (B) a curing agent, (C) a maximum particle size of 63 μm or less, and a particle size of 20 μm or more is 5 wt. The selection and blending amount of the inorganic filler of at least%, (D) a silane coupling agent having a secondary amino group, and (E) a curing accelerator are particularly important.

(Seventh aspect)
As a seventh preferred embodiment of the epoxy resin molding material for sealing according to the present invention, in the first to sixth embodiments, the (C) inorganic filler has a particle diameter of 12 μm or less and 50 wt. % Or more and a particle size of 24 μm or less is 70 wt. % Or more and a particle diameter of 32 μm or less is 80 wt. % And a particle diameter of 48 μm or less are 90 wt. An epoxy resin molding material for sealing that satisfies at least one of the conditions of% or more is mentioned. In this case, the (C) inorganic filler has a particle diameter of 12 μm or less and 50 wt. % Or more and a particle size of 24 μm or less is 70 wt. % Or more and a particle diameter of 32 μm or less is 80 wt. % And a particle diameter of 48 μm or less are 90 wt. It is preferable to satisfy all the conditions of at least%.
In particular, a particle size of 12 μm or less is 50 wt. % And a particle diameter of 48 μm or less are 90 wt. % Or more is preferable, and it is more preferable that all the above conditions are satisfied.

(Eighth aspect)
As a seventh preferred embodiment of the epoxy resin molding material for sealing according to the present invention, in the first to seventh embodiments, the (C) inorganic filler satisfies the following conditions (1) and (2): An epoxy resin molding material for sealing that can be filled at the same time can be used.
(1) The average particle size is 12 μm or less and the specific surface area is 3.0 m ² / g or more;
(2) An inorganic filler having a maximum particle size of 63 μm or less and a particle size of 20 μm or more is 5 wt. % Or more;

  In the production of next-generation flip-chip type semiconductor devices equipped with fine-pitch solder bumps, etc., when sealing with a conventional solid-type sealing epoxy resin, a slightly larger void with a diameter of about 0.1 mm is generated. As a result, the filling of the underfill part was not satisfactory. However, by using the sealing epoxy resin of the present invention represented by the first to eighth aspects as a sealing material, the above problem has been solved.

Here, selection of (A) epoxy resin, (B) curing agent, and (C) inorganic filler is preferably performed from the following viewpoints.
(A) In selecting an epoxy resin, it is preferable to select a resin having a melt viscosity at 150 ° C. of 2 poises or less, and more preferable to select a resin having a melt viscosity of 1 poise or less. (C) This selection is particularly effective when the blending ratio of the inorganic filler is high. Of these, biphenyl type epoxy resin, bisphenol F type epoxy resin, stilbene type epoxy resin and sulfur atom-containing epoxy resin are preferably selected from the viewpoint of reliability.
(B) In the selection of the curing agent, it is preferable to select a curing viscosity at 150 ° C. of 2 poises or less, and it is more preferable to select a melt viscosity of 1 poises or less. (C) This selection is particularly effective when the blending ratio of the inorganic filler is high. In addition, from the viewpoint of moldability (A) When novolac type epoxy resin is selected as the epoxy resin, when dicyclopentadiene type epoxy resin is selected from the viewpoint of low hygroscopicity, naphthalene type epoxy from the viewpoint of heat resistance and low warpage The above selection is particularly effective when a resin and a triphenylmethane type epoxy resin are selected.
(C) In selecting an inorganic filler having an average particle size of 12 μm or less and a specific surface area of 3.0 m ² / g or more, the average particle size is in the range of 12 μm or less. It is necessary to select a size that can be injected in consideration of the height and the bump pitch, but selecting a size smaller than necessary should be avoided because it causes a decrease in fluidity. In addition, it is effective to select a specific surface area within the range of 3.0 m ² / g or more and the smallest possible one among the average particle diameters that can be injected. In order to satisfy both the average particle diameter and the specific surface area within the above ranges, it is effective to combine two or more commercially available inorganic fillers.
Further, if necessary, the coarse particles of the inorganic filler (C) may be cut with a sieve. The component (C) of 53 μm or more is preferably 0.5% by weight or less, the component (C) of 30 μm or more is more preferably 0.5% by weight or less, and the component (C) of 20 μm or more is 0%. More preferably, it is not more than 0.5% by weight.

In addition, an anion exchanger can be added to the sealing epoxy resin molding material of the present invention from the viewpoint of improving the moisture resistance and high temperature storage characteristics of a semiconductor element such as an IC. The anion exchanger is not particularly limited, and conventionally known anion exchangers can be used. Examples thereof include hydrotalcites and hydrated oxides of elements selected from magnesium, aluminum, titanium, zirconium, bismuth, and the like. These may be used alone or in combination of two or more. Of these, hydrotalcite represented by the following composition formula (XXI) is preferable.
Mg _1-X Al _X (OH) ₂ (CO ₃ ) _{X / 2} · mH ₂ O (XXI)
(0 <X ≦ 0.5, m is a positive number)

  Furthermore, in the sealing epoxy resin molding material of the present invention, as other additives, higher fatty acids, higher fatty acid metal salts, ester waxes, polyolefin waxes, polyethylene, release agents such as polyethylene oxide, carbon black, etc. If necessary, a coloring agent, a stress relaxation agent such as silicone oil or silicone rubber powder, and the like can be blended.

(Preparation and usage)
The epoxy resin molding material for sealing of the present invention can be prepared by any method as long as various raw materials can be uniformly dispersed and mixed. As a general method, a raw material having a predetermined blending amount is mixed with a mixer or the like. Examples thereof include a method of sufficiently mixing, melt mixing and kneading with a mixing roll, an extruder, a raking machine, a planetary mixer, etc., then cooling, and defoaming and pulverizing as necessary. Moreover, you may tablet into the dimension and weight which meet molding conditions as needed.
As a method for sealing a semiconductor device by using the epoxy resin molding material for sealing of the present invention as a sealing material, a low-pressure transfer molding method is the most common, but examples include an injection molding method and a compression molding method. It is done. A dispensing method, a casting method, a printing method, or the like may be used. From the viewpoint of filling properties, a molding method capable of molding in a reduced pressure state is preferable.

(Semiconductor device)
Next, the semiconductor device of the present invention will be described. Moreover, the suitable use and usage method of the epoxy resin molding material of this invention are demonstrated through description of this semiconductor device.
As a semiconductor device of the present invention, a wired member such as a tape carrier, a wiring board, a supporting member such as glass, or a mounting substrate, an active element such as a semiconductor chip, a transistor, a diode, or a thyristor, a passive element such as a capacitor, a resistor, or a coil Etc.
Examples thereof include a flip chip mounting type semiconductor device sealed with an epoxy resin molding material for sealing.
Here, as the epoxy resin molding material for sealing, the epoxy resin molding material for sealing of the present invention can be used. That is, containing (A) an epoxy resin, (B) a curing agent, and (C) an inorganic filler that satisfies at least one of the following conditions (1) and (2):
(1) The average particle size is 12 μm or less and the specific surface area is 3.0 m ² / g or more;
(2) An inorganic filler having a maximum particle size of 63 μm or less and a particle size of 20 μm or more is 5 wt. % Or more;
If desired, an epoxy resin molding material for sealing containing (D) a silane coupling agent having a secondary amino group and (E) a curing accelerator is used.
As said (C) inorganic filler, the inorganic filler which satisfy | fills the conditions of said (1) from a viewpoint of a fillability improvement is preferable, and the inorganic emphasis agent which satisfy | fills the said (2) from a viewpoint of a burr | flash improvement From the viewpoint of both, a filler satisfying the conditions (1) and (2) is preferable.
The mounting substrate is not particularly limited, and examples thereof include an organic substrate, an organic film, a ceramic substrate, an interposer substrate such as a glass substrate, a liquid crystal glass substrate, an MCM (Multi Chip Module) substrate, and a hybrid IC substrate. Can be mentioned.

As the semiconductor device of the present invention, (a) flip chip bump height, (b) flip chip bump pitch, (c) semiconductor chip area, (d) sealing material defined to predetermined values, respectively. It is preferable to have one or more configurations of total thickness, (e) the number of flip chip bumps, and (f) air vent thickness during molding.
Specifically, it is preferable to have one or more of the following configurations (a1) to (f1).
(A1) Bump height during flip chip mounting is 300 μm or less (b1) Bump pitch of flip chip is 500 μm or less (c1) Area of semiconductor chip is 25 mm ² or more (d1) Total sealing material The thickness is 2 mm or less (e1) The flip chip has 100 or more bumps
(f1) The air vent thickness at the time of molding is 40 μm or less. A semiconductor device including one or more of the following configurations (a2) to (f2) is more preferable.
(A2) Bump height during flip chip mounting is 200 μm or less (b2) Bump pitch of flip chip is 400 μm or less (c2) The area of the semiconductor chip is 50 mm ² or more (d2) Total sealing material The thickness is 1.5 mm or less. (E2) The number of flip chip bumps is 150 or more.
(f2) The air vent thickness at the time of molding is 30 μm or less A semiconductor device including one or more of the following configurations (a3) to (f3) is more preferable.
(A3) Bump height during flip chip mounting is 150 μm or less (b3) Bump pitch of flip chip is 300 μm or less (c3) The area of the semiconductor chip is 80 mm ² or more (d3) Total sealing material The thickness is 1.0 mm or less. (E3) The number of flip chip bumps is 200 or more.
(f3) The air vent thickness at the time of molding is 20 μm or less The semiconductor device has been described with reference to a preferred embodiment, and among them, a semiconductor device including the configurations (a) to (f) in the following combinations is particularly preferable.
From the viewpoint of filling properties, a semiconductor device having at least one of the configuration (a) and the configuration (b) is preferable. More specifically, a semiconductor device having configurations (a1) and (b1), a semiconductor device having configurations (a1) and (d1), a semiconductor device having configurations (a1) and (c1), configurations (b) and ( A semiconductor device provided with d) and a semiconductor device provided with configurations (b1) and (c1) are preferred. Further, a semiconductor device having configurations (a2) and (b2), a semiconductor device having configurations (a2) and (d2), a semiconductor device having configurations (a2) and (c2), and configurations (b2) and (d2) A semiconductor device and a semiconductor device having configurations (b2) and (c2) are preferable. Furthermore, a semiconductor device having configurations (a3) and (b3), a semiconductor device having configurations (a3) and (d3), a semiconductor device having configurations (a3) and (c3), and configurations (b3) and (d3) The semiconductor device provided and the semiconductor device provided with configurations (b3) and (c3) are preferable.

  As such a semiconductor device, for example, a COB (Chip On Board) in which a semiconductor chip connected to a wiring formed on a wiring board or glass by flip chip bonding is sealed with the epoxy resin molding material for sealing of the present invention. ), Semiconductor devices mounted on bare chips such as COG (Chip On Glass), semiconductor chips connected to wiring formed on a wiring board or glass, flip chip bonding, active elements such as transistors, diodes, thyristors and / or capacitors, A hybrid IC in which passive elements such as resistors and coils are sealed with the sealing epoxy resin molding material of the present invention, and a semiconductor chip mounted on an interposer substrate on which MCM (Multi Chip Module) motherboard connection terminals are formed, After connecting the semiconductor chip and the wiring formed on the interposer substrate by bumps, the present invention Examples include BGA (Ball Grid Array), CSP (Chip Size Package), and MCP (Multi Chip Package) in which the semiconductor chip mounting side is sealed with an epoxy resin molding material for sealing. In addition, these semiconductor devices are epoxy resin molding materials for sealing two or more elements at a time, even in a stacked type package in which two or more elements are mounted on a mounting substrate. It may be a batch mold type package sealed with.

A preferred embodiment of the semiconductor device of the present invention will be described with reference to FIGS.
The semiconductor device of the present invention is not limited to these.
FIG. 1 shows a cross-sectional view of an underfill type flip-chip type BGA, and FIG. 2 shows a cross-sectional view of an overmold type flip-chip type BGA. FIG. 3 shows a top view (partially perspective view) when the semiconductor chip 3 is disposed on the wiring board 1 of the flip chip type BGA via the solder bumps 2.
The underfill type flip-chip type BGA semiconductor device 10 shown in FIG. 1 has solder bumps 2 arranged on a wiring board 1 at a predetermined bump pitch b as shown in FIG. The semiconductor chip 3 is connected and fixed on the wiring board 1 at the bump height a; and the underfill portion 5 formed between the wiring board 1 and the semiconductor chip 3 is sealed with an epoxy resin molding material (sealing material). 4 is used for sealing. The overmolded flip-chip type BGA semiconductor device 20 shown in FIG. 2 is the above except that the underfill portion 5 is sealed and the entire semiconductor chip 3 is covered in the sealing step. It is manufactured in the same manner.
Here, in manufacturing the semiconductor device of the present invention, it is preferable to set the bump height a, bump pitch b, semiconductor chip area d, and total thickness e of the sealing material as follows.
The height a of the solder bump 2 is preferably 300 μm or less, more preferably 200 μm or less, and even more preferably 150 μm or less.
The pitch b of the solder bumps 2, that is, the center distance between the solder bumps is preferably 500 μm or less, more preferably 400 μm or less, and even more preferably 300 μm or less.
The number of solder bumps 2 is preferably 100 or more, more preferably 150 or more, and even more preferably 200 or more.
The area d of the semiconductor chip 3 is preferably 25 mm ² or more, more preferably 50 mm ² or more, and further preferably 80 mm ² or more.
The total thickness e of the sealing material 4 is preferably 2 mm or less, more preferably 1.5 mm or less, and even more preferably 1.0 mm or less.
In the underfill type, the total thickness and the bump height a have the same value.

（ここで、ｎは０〜８の正の数を示す。）

（ここで、ｎは０〜８の正の数を示す。） Examples of the present invention are shown below, but the scope of the present invention is not limited to these examples. The evaluation of each sealing epoxy resin molding material and semiconductor device was performed based on an evaluation method described later unless otherwise specified.
(Examples 1-7, Comparative Examples 1-6)
In each of the compositions shown in Tables 1 to 3, each material was premixed (dry blended), then kneaded with a biaxial roll having a roll surface temperature of about 80 ° C. for 10 minutes, then cooled and pulverized, and Examples 1 to 7 and Each sealing epoxy resin molding material 1-13 of Comparative Examples 1-6 was manufactured. In addition, the composition in a table | surface is shown by a weight part.
(A) Epoxy resin Japan Epoxy Resin product name Epicoat YH-4000H (epoxy equivalent 196, melting point 106 ° C.) as biphenyl type epoxy resin, Sumitomo Chemical product name ESB-400 (epoxy equivalent 400, containing bromine) as brominated epoxy resin An epibis type epoxy resin having a rate of 49%, diglycidyl etherification modified product of 2,2′-bis (4-hydroxy-3,5-dibromophenyl) propane with epichlorohydrin was used.
(B) Curing agent (B) As the curing agent, a phenol / benzaldehyde / xylylene methoxide polycondensate represented by the following structural formula (XXII) having a hydroxyl equivalent weight of 156 and a softening point of 73 ° C. (product name of Sumikin Chemical Co., Ltd.) HE510-05), a phenol-hydroxybenzaldehyde resin (Maywa Kasei Co., Ltd. product name MEH-7500-3S) represented by the following structural formula (XXIII) having a hydroxyl group equivalent of 100 and a softening point of 83 ° C. was used.

(Here, n represents a positive number from 0 to 8.)

(Here, n represents a positive number from 0 to 8.)

  A total of 13 types of molding materials thus prepared were molded using a transfer molding machine under conditions of a mold temperature of 180 ° C., a molding pressure of 6.9 MPa, and a curing time of 90 seconds, and evaluated by spiral flow and gel time tests.

[Fabrication of Semiconductor Device 1 (Flip Chip BGA)]
Next, semiconductor devices of Examples 1 to 7 and Comparative Examples 1 to 6 were produced using the epoxy resin molding materials 1 to 13 for sealing. In addition, sealing with an epoxy resin molding material for sealing is performed using a transfer molding machine after molding at a mold temperature of 180 ° C., a molding pressure of 6.9 MPa, and a curing time of 90 seconds, and after curing at 180 ° C. for 5 hours. It was done by doing.
Examples 1 to 7 (Table): A fine wiring pattern is formed on an insulating base substrate (glass cloth-epoxy resin laminate, manufactured by Hitachi Chemical Co., Ltd., product name E-679), and a gold-plated terminal on the semiconductor element mounting side and the opposite side A semiconductor element mounting substrate having an outer dimension of 22 mm long × 14 mm wide × 0.3 mm thick coated with an insulating protective resist (product name: PSR4000AUS5, manufactured by Taiyo Ink) on the surface excluding external connection terminals is dried at 120 ° C. for 2 hours. After that, a semiconductor element having a length of 9 mm × width of 8 mm × thickness of 0.4 mm (area 72 mm ² ), a bump diameter of 145 μm, a bump pitch of 200 μm, and a bump number of 160 is subjected to a reflow process by IR reflow at 260 ° C. for 10 seconds. Went and implemented. The bump height after mounting was 100 μm. Next, using the epoxy resin molding materials 1 to 7 for sealing, the semiconductor element mounting surface was vacuum transfer molded to the dimensions of 22 mm long × 14 mm wide × 0.7 mm thick under the above conditions. A flip chip BGA device was fabricated.
Comparative Examples 1 to 6 (Table): Semiconductor devices of Comparative Examples 1 to 6 were produced in the same manner as in Examples 1 to 7, except that the epoxy resin molding materials 8 to 13 for sealing were used.

[Fabrication of Semiconductor Device 2 (Flip Chip BGA)]
Next, semiconductor devices of Examples 1 to 7 and Comparative Examples 1 to 6 were produced using the epoxy resin molding materials 1 to 13 for sealing. In addition, sealing with an epoxy resin molding material for sealing is performed using a transfer molding machine after molding at a mold temperature of 180 ° C., a molding pressure of 6.9 MPa, and a curing time of 90 seconds, and after curing at 180 ° C. for 5 hours. It was done by doing.
Examples 1 to 7 (Table): A fine wiring pattern is formed on an insulating base substrate (glass cloth-epoxy resin laminate, manufactured by Hitachi Chemical Co., Ltd., product name E-679), and a gold-plated terminal on the semiconductor element mounting side and the opposite side A semiconductor element mounting substrate having an outer dimension of 22 mm long × 14 mm wide × 0.3 mm thick coated with an insulating protective resist (product name: PSR4000AUS5, manufactured by Taiyo Ink) on the surface excluding external connection terminals is dried at 120 ° C. for 2 hours. After that, a semiconductor element having a length of 6 mm, a width of 5 mm, a thickness of 0.4 mm (area 30 mm ² ), a bump diameter of 300 μm, a bump pitch of 490 μm, and 120 bumps is subjected to a reflow process at 260 ° C. for 10 seconds by IR reflow. Went and implemented. The bump height after mounting was 260 μm. Next, using the epoxy resin molding materials 1 to 7 for sealing, the semiconductor element mounting surface was vacuum transfer molded to the dimensions of 22 mm long × 14 mm wide × 1.2 mm thick under the above conditions, and the flip chip of Examples A BGA device was fabricated.
Comparative Examples 1 to 6 (Table): Semiconductor devices of Comparative Examples 1 to 6 were produced in the same manner as in Examples 1 to 7, except that the epoxy resin molding materials 8 to 13 for sealing were used.

[Fabrication of Semiconductor Device 3 (Flip Chip BGA)]
Next, semiconductor devices of Examples 1 to 7 and Comparative Examples 1 to 6 were manufactured using the epoxy resin molding materials 1 to 13 for sealing. In addition, sealing with an epoxy resin molding material for sealing is performed using a transfer molding machine after molding at a mold temperature of 180 ° C., a molding pressure of 6.9 MPa, and a curing time of 90 seconds, and after curing at 180 ° C. for 5 hours. It was done by doing.
Examples 1 to 7 (Table): A fine wiring pattern is formed on an insulating base substrate (glass cloth-epoxy resin laminate, manufactured by Hitachi Chemical Co., Ltd., product name E-679), and a gold-plated terminal on the semiconductor element mounting side and the opposite side A semiconductor element mounting substrate having an outer dimension of 22 mm long × 14 mm wide × 0.3 mm thick coated with an insulating protective resist (product name: PSR4000AUS5, manufactured by Taiyo Ink) on the surface excluding external connection terminals is dried at 120 ° C. for 2 hours. After that, a semiconductor element having a length of 5 mm × width of 4 mm × thickness of 0.4 mm (area 20 mm ² ), a bump diameter of 390 μm, a bump pitch of 700 μm, and a bump number of 40 is subjected to a reflow process by IR reflow at 260 ° C. for 10 seconds. Went and implemented. The bump height after mounting was 350 μm. Next, using the epoxy resin molding materials 1 to 7 for sealing, the semiconductor element mounting surface was vacuum transfer molded to the dimensions of 22 mm long × 14 mm wide × 2.5 mm thick under the above conditions. A flip chip BGA device was fabricated.
Comparative Examples 1 to 6 (Table): Semiconductor devices of Comparative Examples 1 to 6 were produced in the same manner as in Examples 1 to 7, except that the epoxy resin molding materials 8 to 13 for sealing were used.

  The manufactured semiconductor devices of Examples 1 to 7 and Comparative Examples 1 to 6 were evaluated by the following test. The evaluation results are shown in Tables 1 to 3.

〔Evaluation methods〕
(1) Spiral flow (fluidity index)
Molding was performed using a spiral flow measurement mold according to EMMI-1-66, and the flow distance was determined.
(2) Gel time Using a JSR curast meter, the time (s) to the rise of the torque curve was measured at a sample of 3 g and a temperature of 180 ° C.
(3) Void generation amount Using an ultrasonic exploration imaging device (HYE-HOCUS type manufactured by Hitachi Construction Machinery Co., Ltd.), the semiconductor device is observed through a fluoroscopic observation to observe whether voids having a diameter of 0.1 mm or more are generated. Evaluation was performed by the number of void-generating semiconductor devices / the number of test semiconductor devices.
(4) A burr pot was molded using a mold provided with a slit having a thickness of 10 μm, and the length of the burr that flowed through the slit was obtained with a caliper. The burr length in the slit was good when it was less than 10 μm, and NG was 10 μm or more.

FIG. 1 shows a cross-sectional view of a flip chip type BGA (underfill type) sealed with an epoxy resin molding material (sealing material) for sealing. FIG. 2 shows a cross-sectional view of a flip chip type BGA (overmold type) sealed with an epoxy resin molding material (sealing material) for sealing. FIG. 3 shows a top view (partially perspective view) when the semiconductor chip 3 is arranged on the wiring board 1 via the solder bumps 2.

Explanation of symbols

1: Wiring board 2: Solder bump 3: Semiconductor chip 4: Sealing material 5: Underfill part a: Bump height b: Bump pitch d: Area of semiconductor chip e: Total thickness of sealing material

Claims (20)

(A) an epoxy resin, (B) a curing agent and (C) an epoxy resin molding material for sealing containing at least an inorganic filler,
The inorganic filler (C) has an average particle diameter of 12 μm or less and a specific surface area of 3.0 m ² / g or more, and the inorganic filler (C) has a particle diameter of 12 μm or less and 50 wt. % Or more and a particle size of 24 μm or less is 70 wt. % Or more and a particle diameter of 32 μm or less is 80 wt. % And a particle diameter of 48 μm or less are 90 wt. Satisfy at least one of the above conditions,
A solid epoxy resin molding material for sealing, which is used as an underfill material for flip chip mounting. (C) The solid epoxy resin molding material for sealing according to claim 1, wherein the inorganic filler has an average particle size of 10 μm or less. (C) The specific surface area of an inorganic filler is 3.5-5.5 m < ² > / g, The solid epoxy resin molding material for sealing of Claim 1 or 2. The solid epoxy resin molding material for sealing in any one of Claims 1-3 which uses the structure of (a1)-(f1) for a semiconductor device provided with one or more.
(A1) Flip chip bump height is 150 μm or less (b1) Flip chip bump pitch is 500 μm or less (c1) Semiconductor chip area is 25 mm ² or more (d1) Total thickness of sealing material (E1) The number of flip chip bumps is 100 or more.
(f1) The air vent thickness at the time of molding is 40 μm or less The solid epoxy resin molding material for sealing according to claim 4, wherein the structure of (a2) to (f2) is used for a semiconductor device having one or more.
(A2) Bump height of flip chip is 100 μm or less (b2) Bump pitch of flip chip is 400 μm or less (c2) Area of semiconductor chip is 50 mm ² or more (d2) Total thickness of sealing material Is 1.5 mm or less. (E2) The number of flip chip bumps is 150 or more.
(f2) Air vent thickness during molding is 30 μm or less (D) The solid epoxy resin molding material for sealing according to any one of claims 1 to 5, further comprising a silane coupling agent having a secondary amino group. (D) The solid epoxy resin molding material for sealing according to claim 6, wherein the silane coupling agent having a secondary amino group contains a compound represented by the following general formula (I).

(Wherein, R ¹ is selected from a hydrogen atom, an alkyl group and alkoxy group having 1 to 2 carbon atoms of 1 to 6 carbon atoms, R ² is selected from alkyl group and a phenyl group having 1 to 6 carbon atoms, R ³ represents a methyl group or an ethyl group, n represents an integer of 1 to 6, and m represents an integer of 1 to ^3. ) (E) The solid epoxy resin molding material for sealing according to any one of claims 1 to 7, further comprising a phosphorus compound. (E) The solid epoxy resin molding material for sealing according to claim 8, wherein the phosphorus compound contains a phosphate ester. The solid epoxy resin molding material for sealing according to claim 9, wherein the phosphoric ester contains a compound represented by the following general formula (II).

(Here, 8 R in the formula represent an alkyl group having 1 to 4 carbon atoms, and they may all be the same or different. Ar represents an aromatic ring.) (E) The solid epoxy resin molding material for sealing in any one of Claims 8-10 in which a phosphorus compound contains a phosphine oxide. The solid epoxy resin molding material for sealing according to claim 11, wherein the phosphine oxide contains a compound represented by the following general formula (III).

(Here, R ¹ , R ² and R ³ represent a substituted or unsubstituted alkyl group having 1 to 10 carbon atoms, an aryl group, an aralkyl group and a hydrogen atom, which may all be the same or different. Except when it is an atom.) (A) The epoxy resin has a melt viscosity at 150 ° C. of 2 poises or less, and the solid epoxy resin molding material for sealing according to claim 1. (A) Epoxy resin is biphenyl type epoxy resin, bisphenol F type epoxy resin, stilbene type epoxy resin, sulfur atom-containing epoxy resin, novolac type epoxy resin, dicyclopentadiene type epoxy resin, naphthalene type epoxy resin and triphenylmethane type epoxy resin The solid epoxy resin molding material for sealing according to any one of claims 1 to 13, comprising at least one kind of resin. (B) The melt viscosity at 150 ° C. of the curing agent is 2 poises or less. The solid epoxy resin molding material for sealing according to claim 1. (B) The curing agent contains at least one of biphenyl type phenol resin, aralkyl type phenol resin, dicyclopentadiene type phenol resin, triphenylmethane type phenol resin and novolac type phenol resin. The solid epoxy resin molding material for sealing as described. (F) The solid epoxy resin molding material for sealing according to any one of claims 1 to 16, further comprising a curing accelerator. A semiconductor device sealed with the sealing solid epoxy resin molding material according to claim 1. 19. The semiconductor device according to claim 18, comprising one or more of the following configurations (a1) to (f1).
(A1) Flip chip bump height is 150 μm or less (b1) Flip chip bump pitch is 500 μm or less (c1) Semiconductor chip area is 25 mm ² or more (d1) Total thickness of sealing material (E1) The number of flip chip bumps is 100 or more.
(f1) The air vent thickness at the time of molding is 40 μm or less 19. The semiconductor device according to claim 18, comprising at least one of the following configurations (a2) to (f2).
(A2) Bump height of flip chip is 100 μm or less (b2) Bump pitch of flip chip is 400 μm or less (c2) Area of semiconductor chip is 50 mm ² or more (d2) Total thickness of sealing material Is 1.5 mm or less. (E2) The number of flip chip bumps is 150 or more.
(f2) Air vent thickness during molding is 30 μm or less

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