CN1252210C - 连接材料和连接结构体 - Google Patents

连接材料和连接结构体 Download PDF

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CN1252210C
CN1252210C CNB011228016A CN01122801A CN1252210C CN 1252210 C CN1252210 C CN 1252210C CN B011228016 A CNB011228016 A CN B011228016A CN 01122801 A CN01122801 A CN 01122801A CN 1252210 C CN1252210 C CN 1252210C
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phenol
epoxy
resins
connection material
record
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CN1327020A (zh
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筱崎润二
武市元秀
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Dexerials Corp
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Sony Chemicals Corp
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Abstract

对于将半导体元件安装在半导体元件用电路基板上时所使用的连接材料，在所得连接结构体的保存中，不管连接材料是否吸湿，之后，装入240℃左右的焊接软熔炉内时，不会降低连接信赖性。将半导体元件安装在半导体元件用电路基板上时所使用的连接材料，含有以下成分(A)～(C)：(A)环氧树脂，(B)具有2个以上酚性羟基的酚系化合物，(C)潜在性硬化剂。连接材料中，成分(B)酚系化合物的酚性羟基当量数对环氧树脂的环氧当量数之比最好为0.2～1.0。

Description

连接材料和连接结构体
本发明是关于将LSI等半导体元件安装在半导体元件装配用的电路基板上时，特别是倒装片安装时有用的连接材料。
在将LSI等半导体元件安装在半导体元件装配用电路基板上时，在半导体元件的凸起(bump)电极和电路基板电极之间，夹入糊状或薄膜状绝缘性连接材料或者在其中分散了各向异性导电粒子的各向异性导电连接材料，一边加压一边热硬化，将两者连接起来，得到连接结构体。
作为这样的绝缘性连接材料，广泛使用由环氧树脂和咪唑系潜在性硬化剂形成的环氧系绝缘性连接材料。
然而，在将半导体元件安装在半导体元件装配用电路基板上时，使用以前的环氧系绝缘性连接材料或其中分散了各向异性导电粒子的各向异性导电连接材料时，所得到的连接结构体在保管中，有时连接材料吸湿，吸湿后装入240℃左右的焊接软熔炉内时，连接材料中浸入的水分会膨胀，随情况而破裂(像爆玉米花现象)，半导体元件和连接材料在界面处会产生剥离，存在连接的信赖性大大降低的问题。
本发明的目的是对将半导体元件安装在半导体元件用电路基板上时可使用的连接材料，在所得连接结构体保管中，不管连接材料是否吸湿，即使随后装入240℃左右的焊接软熔炉内，也不降低连接信赖性。
本发明者发现在使用连接材料将半导体元件和电路基板连接时，配合具有2个以上酚性羟基的酚系化合物，可抑制环氧系连接材料热硬化时收缩，即使在吸湿条件下保管连接结构体后，装入240℃左右的焊接软熔炉内也不降低连接信赖性，并由此完成本发明。
即，本发明提供的连接材料，其特征是含有以下成分(A)～(C)：
(A)环氧树脂，
(B)具有2个以上酚性羟基的酚系化合物
(C)潜在性硬化剂。
本发明提供的连接结构体，其特征是用这种连接材料连接对置电极间的结构体。
以下详细说明本发明。
本发明是连接材料，其特征是在含有环氧树脂(成分(A))和潜在性硬化剂(成分(C))的连接材料中，作为成分(B)，含有具有2个以上酚性羟基的酚系化合物。此处，成分(B)的具有2个以上酚性羟基的酚系化合物，在连接材料热硬化时与环氧树脂反应，可增大连接材料的硬度，提高粘接力，而且可抑制连接材料收缩。因此，即使在吸湿条件下保存连接结构体也能极大地抑制水分向连接材料浸入。因此，将连接结构体在焊接软熔炉内进行加热也能极大地抑制由水分引起的膨胀和破裂，从而提高了连接信赖性。
在本发明的连接材料中，相对于环氧树脂的环氧当量数，酚系化合物的酚性羟基当量数的比，过小时(酚性羟基相对地过少时)，例如，在用连接材料连接半导体元件和电路基板时，在半导体元件界面的粘接力存在降低的趋势，反之，过大时(酚性羟基相对地过多时)，在电路基板界面的粘接力也会降低，所以最好调整为0.2～1.0，更好为0.3～0.6。具体讲是，在连接材料中使用400g的环氧当量为200g/eq的环氧树脂时，连接材料中的环氧树脂当量数为2。另一方面，在连接材料中使用400g的酚性羟基为100g/eq的成分(B)酚性化合物时，连接材料中的酚性羟基当量数为1。因此，这时相对于环氧树脂的环氧当量数，成分(B)酚系化合物的酚性羟基当量数的比为0.5。
此处，求得环氧当量时，在后述的潜在性硬化剂含有环氧树脂时，该部分环氧树脂的环氧当量也必须考虑在内。即，和酚系化合物的酚性羟基当量比较时的环氧当量，不仅成分(A)的环氧树脂，对于其他成分(例如成分(C)的潜在性硬化剂)中所含的环氧树脂也必须考虑，是指总的环氧当量。
作为本发明中所用成分(A)的环氧树脂，可使用公的最好能用作热固化型粘接剂(例如，各向异性导电粘接剂用的绝缘性熟固化型粘接剂)的成膜成分。特别是，考虑到成膜性和薄膜强度等时，最好并用2种以上，例如，可并用常温下固体的高分子量环氧树脂和常温下液体的环氧树脂。进而还可并用柔性的环氧树脂。作为这种固体的高分子量环氧树脂，有热塑酚型环氧树脂、热塑甲酚型环氧树脂、将二环戊二烯作主骨架的环氧树脂、双酚A型或双酚F型的高分子、或将它们变性的环氧树脂等。作为常温下为液体的环氧树脂，有双酚A型或双酚F型环氧树脂等。作为柔性环氧树脂，有二聚物酸变性环氧树脂、以丙二醇为主骨架的环氧树脂、尿烷变性环氧树脂等。
成分(A)的环氧树脂的环氧当量(g/eq)过小时，硬化收缩增大，会增加内部应力，反之，过大时，凝聚力降低，硬化物(连接结构体)的连接信赖性降低，所以最好100～500，更好为200～400。使用数种环氧树脂时的环氧当量，相当于各环氧树脂的环氧当量乘以各环氧树脂占总环氧树脂中的重量比所得值的和。
作为本发明中使用的具有2个以上酚性羟基的酚系化合物，可举出有双酚A、双酚F等的单量体、酚热塑树脂、甲酚热塑树脂等的低聚物、聚乙烯酚树脂等聚合物。其中，热塑型酚树脂最好。
这些具有2个以上酚性羟基的酚系化合物，其酚性羟基当量(q/eq)过小时，硬化收缩很大，内部应力增大，反之，过大是，凝聚力降低，硬化物(连接结构体)的连接信赖性降低，所以最好为50～500，更好为80～400。使用数种具有2个以上酚性羟基的酚系化合物时，其酚性羟基当量，相当于各酚系化合物的酚羟基当量乘以各酚系化合物占总酚系化合物中重量比之值的和。
作为本发明连接材料中使用的潜在性硬化剂，可单独或同时使用咪唑系潜在性硬化剂、胺系潜在性硬化剂等。其中，最好使用作用(硬化)湿度约为170℃的咪唑系潜在性硬化剂。通过使用显示这种硬化温度的咪唑系潜在性硬化剂，将本发明的连接材料适用于各向异性导电粘接剂时，能使电极端子间确实粘接，而且也能进行电连接。而且，将热压时的生产节拍时间可设定为数秒钟，也可对各向异性导电粘接剂付与良好的耐热性。
此处，作为咪唑系潜在性硬化剂，虽然可使用多年来公知的咪唑系潜在性硬化剂。但其中，最好使用微胶囊化的咪唑系潜在性硬化剂。作为这种微胶囊化咪唑系潜在性硬化剂，有用尿素和异氰酸酯使咪唑形成加合物，再用异氰酸酯化合物将其表面进行包复形成微胶囊化的咪唑系潜在性硬化剂，和用环氧化合物使咪唑形成加合物，再用异氰酸酯化合物将其表面进行包复形成微胶囊化的咪唑系潜在性硬化剂。
咪唑系潜在性硬化剂的使用量，咪唑系潜在性硬化剂过少时，耐热性降低，连接可靠性恶化，过多时，加热加压后的丸剂(ピ一ル)强度降低，保存稳定性恶化，对于100重量份环氧树脂最好5～30重量份，更好8～20重量份。
作为胺系潜在性硬化剂，可使用公知的聚胺系潜在性硬化剂、叔胺系潜在性硬化剂、烷尿系潜在性硬化剂。
使用胺系潜在性硬化剂时，其用量过少时加热加压后的丸剂(ピ一ル)的强度降低，连接可靠性恶化，过多时，保存稳定性恶化，所以，对于100重量份环氧树脂，最好2～40重量份，更好5～30重量份。
在将本发明的连接材料用作各向异性导电粘接剂时，可配合公知各向异性导电粘接剂中使用的导电粒子(例如，锡粒子、镍粒子等金属粒子、和表面形成镀金被覆膜的苯乙烯树脂粒子等复合粒子等)。作为配合量，在连接材料中最好为2～20容量％。
在本发明的连接材料中，可适当配合以前在各向异性导电粘接膜等中配合的公知添加剂，例如，异氰酸酯系交联剂、环氧硅烷化合物等的偶合剂、环氧变性硅酮树脂、或苯氧树脂等热硬化性绝缘树脂。根据需要也可使用甲苯或MEK等溶剂。
本发明的连接材料可利用常法进行制造。例如，将环氧树脂、潜在性硬化剂和具有2个以上酚性羟基的酚系化合物在甲苯或MEK等溶剂中进行均匀混合制造。
本发明的连接材料通过形成薄膜化，可用作热硬化型连接薄膜。特别是在配合了各向异性导电连接用的导电粒子时，也可用作各向性导电连接薄膜。这些情况的制造，是在剥离片上(例如聚酯片)将连接材料涂布上薄膜状，在没有开始硬化反应的温度下使连接材料进行干燥。
本发明连接材料的使用形态，和过去的热硬化型粘接剂一样，将对置的一对电极进行连接。例如，将本发明的连接材料适用于对置的一对电极之间(例如，半导体元件的凸出(bump)电极和半导体元件装配用电路基板电极之间)，通过加压或加压加热使其热硬化，将两者牢固地连接在一起。得到的连接结构体，假使在高湿度环境下保存后装入焊接软熔炉内，与以前相比，不会降低连接信赖性。
以下根据实验例具体说明本发明。
实施例1～19
将环氧当量为140g/eq的环氧树脂(HP4032D、大日本インキ化学工业社制)、羟基当量为118q/eq的热塑型酚树脂(VH4170、大日本インキ化学工业社制)、环氧当量为244g/eq的咪唑系潜在性硬化剂(HX3941HP、旭チバ社制)、苯氧树脂(YP50、东都化成社制)、和导电粒子(镍被复丁苯乙烯的粒珠，直径50μm)、按照表1所示酚性羟基当量数与环氧当量数之比(OH/EPOXY)，调整各成分的配合量，并进行混合，利用薄膜化处理，制作成40μm厚的各向异性导电连接薄膜。使用的导电粒子为12容量％。
表1中，潜在性硬化剂的重量份是相对于100重量份环氧树脂的配合量。
将得到的各向异性导电连接薄膜贴付在具有18μm厚的铜图案(Line/Space＝100μm/50μm)的电路基板(FR5)上，在该贴付面上重叠上半导体芯片(外形6.3mm正方形、110μm正方形电镀凸起(凸起高度20μm)、150μm间距铝配线)、对每个凸起在150g的加压条件下以160℃，进行10秒钟的热压合操作，接着，对每个凸起在0.3g的加压条件下的200℃，进行5秒钟的热压合操作，制作成在电路基板上装配了半导体芯片的连接结构体。
对于得到的连接结构体，在制作后，前处理后(在85℃、85％RH的环境下放置24小时后、通过软熔炉(最高温度达240℃)2次处理后)、老化处理后(压煮试验(PCT(121℃、2.0265×102KPa、100％RH、100小时、200小时或300小时)))或热循环试验后(H/S(-55～125℃、250次、500次、1000次))、利用四端子法测定导通电阻值(Ω)。利用测得的导通电阻值，按以下基准评价连接信赖性。所得结果示于表2。
连接信赖性
等级标准
A：低于100Ω
B：100mΩ以上，1Ω以下
C：1Ω以上～无穷态
用显微镜观察老化处理(300小时)后连接处的剥离状态。在半导芯片和连接材料之间产生剥离时，以「I」表示。未产生剥离，以下「-」表示，结果示于表2。
[表1]
实验例   当量数比(OH/EPOXY)   潜在性硬化剂重量份
  12345678910111213141516171819   000.10.10.20.20.40.40.40.40.40.60.60.60.60.60.80.80.8   7156.514.56.514.561214172261214172261422
[表2]
  实验例   前处理后                 PCT后                           H/S后   剥离状态
  100   200   300   250   500   1000
  12345678910111213141516171819   BBBBBBAAAAAAAAAAAAA   CCBBBBAAAAAAAAAAAAA   --CCBBAAAAAAAAAAAAA   ----BBAAAABAAAABAAB   CCCBBABAAAAAAAAABAA   ---CBBBAAAABAAAABBA ---BBBAAAABAAAABBB IIII--------------
从实验例1～19的结果可知，在连接材料中并用具有2个以上酚性羟基的热塑型酚树脂时，改善了PCT特性。从整个实验例可知，酚性羟基当量数对环氧树脂的环氧当量数之比，最好范围为0.2～1.0。
从实验例7～19的结果可知，咪唑系潜在性硬化剂的配合量，对于100重量份环氧树脂，为5～30重量份为好。
根据本发明，对于将半导元件安装在半导体元件用电路基板上时所使用的连接材料，在所得连接结构体的保存中，不管连接材料是否吸湿，之后装入240℃左右的焊接软熔炉内时，不会降低连接的依赖性。

Claims (11)

1.一种连接材料，其特征是含有以下成分(A)～(C)
(A)环氧树脂，
(B)具有2个以上酚性羟基的酚系化合物，
(C)由异氰酸酯化合物微胶囊化的潜在性硬化剂。
2.根据权利要求1记载的连接材料，其特征是在连接材料中，成分(B)酚系化合物的酚性羟基当量数对环氧树脂的环氧当量数之比为0.2～1.0。
3.根据权利要求1记载的连接材料，其特征是在连接材料中，成分(B)酚系化合物的酚性羟基当量数对环氧树脂的环氧当量数之比为0.3～0.6。
4.根据权利要求1～3中任一项记载的连接材料，其特征是成分(B)的具有2个以上酚性羟基的酚系化合物的酚性羟基当量为50～500g/eq。
5.根据权利要求1～3中任一项记载的连接材料，其特征是酚系化合物是热塑型酚树脂。
6.根据权利要求1～3中任一项记载的连接材料，其特征是成分(B)的具有2个以上酚性羟基的酚系化合物是热塑型酚树脂，并且该酚性羟基当量为50～500g/eq。
7.根据权利要求1～3中任一项记载的连接材料，其特征是成分(C)潜在性硬化剂是咪唑系潜在性硬化剂。
8.根据权利要求1～3中任一项记载的连接材料，其特征是成分(C)潜在性硬化剂的配合量，对于100重量份环氧树脂，为5～30重量份。
9.根据权利要求1～3中任一项记载的连接材料，其特征是进一步含有2～20容量％的各向异性导电连接用的导电粒子。
10.一种连接结构体，其特征是由对置的一对电极和在其之间被夹持的权利要求1～9任一项记载的连接材料组成，通过加压或加热加压，将它们连接在一起。
11.根据权利要求10记载的连接结构体，其特征是对置电极的一方是半导体元件的凸起电极，另一方是装配半导体元件用的电路基板的电极。
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EP1160857B1 (en) 2014-10-08
KR100776554B1 (ko) 2007-11-16
US20020009597A1 (en) 2002-01-24
KR20010109159A (ko) 2001-12-08
US6475641B2 (en) 2002-11-05
EP1160857A3 (en) 2004-01-02
TWI282353B (en) 2007-06-11
JP3711842B2 (ja) 2005-11-02
EP1160857A2 (en) 2001-12-05
JP2001345349A (ja) 2001-12-14

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