CN104508069A - 膜状粘接剂、半导体接合用粘接片、和半导体装置的制造方法 - Google Patents

膜状粘接剂、半导体接合用粘接片、和半导体装置的制造方法 Download PDF

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CN104508069A
CN104508069A CN201380040479.5A CN201380040479A CN104508069A CN 104508069 A CN104508069 A CN 104508069A CN 201380040479 A CN201380040479 A CN 201380040479A CN 104508069 A CN104508069 A CN 104508069A
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adhesive
film
chip
wafer
share
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CN104508069B (zh
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若山洋司
市川功
阿久津高志
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Lintec Corp
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Lintec Corp
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Abstract

本发明的膜状粘接剂是含有粘合剂树脂(A)、环氧树脂(B)、热固化剂(C)和填料(D)的膜状粘接剂，其中，D65标准光源的全光线透射率为70%以上，雾度值为50%以下。本发明提供在倒装安装方法中，可在规定位置正确地将半导体芯片进行小片键合，同时能够制造具有高的封装可靠性的半导体装置的膜状粘接剂和使用其的半导体接合用粘接片。

Description

膜状粘接剂、半导体接合用粘接片、和半导体装置的制造方法
技术领域
本发明涉及特别适于在将半导体芯片粘接(小片键合、die bonding)于有机基板、引线框或其它半导体芯片上的步骤中使用的膜状粘接剂、半导体接合用粘接片、以及使用了该膜状粘接剂、该粘接片的半导体装置的制造方法。
背景技术
硅、镓、砷等的半导体晶片(wafer)以大直径的状态被制造，该晶片在被切断分离(切割)为元件小片(半导体芯片)后转移至作为下一步骤的装配步骤。此时，半导体晶片通过背面研磨步骤薄化，然后在粘接片上贴合，施加切割、洗涤、干燥、膨胀、拾取(pick up)的各步骤后，移送至下一步骤的键合(bonding)步骤。
在键合步骤中，将半导体芯片安装在印刷线路基板上时，有时采用在半导体芯片的电路面侧的连接垫片部形成包含共晶焊锡、高温焊锡、金等的导通用突起物(凸块电极)，通过所谓倒装(face down)方式，使这些凸块电极与芯片搭载用基板上的相对应的端子部对面、接触，进行熔融/扩散接合的倒装安装方法。在这样的安装方法中，如果使用近年普及的被称为小片连接膜(die attachment film)的、以贴附于晶片的状态将晶片单片化(個片化)而得到芯片并供于在小片键合时将芯片和芯片搭载用基板粘接用的粘接膜，则比使用其它方式的底部填充(under fill)材料更为简便。
在小片连接膜在所述安装方法的适用中，显然具有如下的问题。即，在倒装安装方法中，通过光学读取在半导体芯片的电路面形成的定位标记，可在规定的位置正确地进行小片键合。因此，粘接膜不具有充分的透明性时，产生定位标记的读取变得困难的问题。
在专利文献1中，公开了波长440nm～770nm的光的透射率为74%以上的带有粘接膜的电子部件。其中公开的粘接膜不是含有填充材料的膜，但出于粘接膜的线性膨胀系数的调整、吸湿性的抑制等目的，有时添加填充材料。在倒装安装方法中，使用粘接膜作为小片连接膜时，由于在晶片的表面侧贴附粘接膜，粘接膜有时以没有被切割片覆盖、而露出的状态进行切割，该情况下，露出的粘接膜暴露于切割时的洗涤水中。因此，以吸湿性的控制为目的，要求在粘接膜中添加填充材料。通过控制吸湿性，可以提高切割时的粘接膜的耐水性、所得的半导体装置的封装可靠性。但是，由于构成粘接膜的其它成分与填充材料的光学特性的差异，导致有粘接膜的透明性降低的可能性。因此，由于贴附于半导体芯片的电路面上的粘接膜，导致定位标记读取性有时变得不充分。
现有技术文献
专利文献
专利文献1 : 日本特开2011-171688。
发明内容
因此，本发明的目的在于提供在倒装安装方法中，可在规定位置正确地将半导体芯片进行小片键合，同时能够制造具有高的封装可靠性的半导体装置的膜状粘接剂和使用该膜状粘接剂的半导体接合用粘接片。
解决上述课题的本发明含有以下的要点,
[1]膜状粘接剂，其含有粘合剂树脂(A)、环氧树脂(B)、热固化剂(C)和填料(D)，其中， 　D65标准光源的全光线透射率为70%以上，雾度值为50%以下；
[2]根据[1]所述的膜状粘接剂，其中，含有5质量%以上的填料(D)；
[3]根据[1]或[2]所述的膜状粘接剂，其中，填料(D)的平均粒径为50nm以下；
[4]根据[1]～[3]中任一项所述的膜状粘接剂，其中，粘合剂树脂(A)是含有5～30质量%的源于含环氧基的单体的结构单元的丙烯酸系聚合物；
[5]根据[1]～[4]中任一项所述的膜状粘接剂，其中，环氧树脂(B)的含量相对于粘合剂树脂(A)100质量份为50～1000质量份；
[6]半导体接合用粘接片，其中，将[1]～[5]中任一项所述的膜状粘接剂作为粘接剂层、可剥离地形成于支撑片上；
[7]根据[6]所述的半导体接合用粘接片，其中，支撑片含有“包含聚氨酯聚合物和乙烯基系聚合物的复合膜”或“聚氨酯丙烯酸酯固化物膜”作为结构层；
[8]半导体装置的制造方法，其是使用了上述[1]～[5]中任一项所述的膜状粘接剂、或者[6]或[7]所述的半导体接合用粘接片的半导体装置的制造方法，其中，包含：
在晶片上贴附膜状粘接剂或半导体接合用粘接片的粘接剂层的步骤、将晶片单片化而得到芯片的步骤、和经由膜状粘接剂或粘接剂层将芯片固定的步骤。
发明的效果
根据本发明的膜状粘接剂和使用其的半导体接合用粘接片，可以适用于倒装安装方法，能够正确地确定位置而将芯片之间或芯片与基板相互地粘接。另外，即使在严苛的环境下，也可以得到显示高的封装可靠性的半导体装置。
具体实施方式
首先对于本发明的膜状粘接剂进行说明。
(膜状粘接剂)
本发明的膜状粘接剂含有粘合剂树脂(A)、环氧树脂(B)、热固化剂(C)和填料(D)作为必须成分，为了改良各种物性，根据需要可以含有其他成分。以下对于这些各成分具体地进行说明。
粘合剂树脂 (A)
粘合剂树脂只要是可赋予膜状粘接剂造膜性和挠性的聚合物成分，就没有限定，可以列举例如丙烯酸系聚合物、聚酯树脂、聚乙烯基醇树脂、聚乙烯醇缩丁醛、聚氯乙烯、聚苯乙烯、聚酰胺树脂、纤维素、聚乙烯、聚异丁烯、聚乙烯基醚、聚酰亚胺树脂、苯氧基树脂、苯乙烯-异戊二烯-苯乙烯嵌段共聚物、苯乙烯-丁二烯-苯乙烯嵌段共聚物等。这些粘合剂树脂可以单独使用，或将2种以上组合使用，但从避免由于不同种类的粘合剂树脂之间的相容性低而导致的膜状粘接剂的透明性降低的角度考虑，优选单独使用，将2种以上组合时，优选选择组成相似的粘合剂树脂等，以使相容性不会降低的方式选择。在上述列举的物质中，优选使用易于调节膜状粘接剂的各种特性、特别是粘合剂树脂与其它成分的相容性的丙烯酸系聚合物。
作为丙烯酸系聚合物，可以使用一直以来公知的丙烯酸系聚合物。丙烯酸系聚合物的重均分子量优选为1万～200万，更优选为10万～150万。丙烯酸系聚合物的重均分子量过低时，与在下述的半导体接合用粘接片中使用的支撑片的剥离力变高，有时产生包含膜状粘接剂的粘接剂层与支撑片的层间剥离不良。另外，丙烯酸系聚合物的重均分子量过高时，有时膜状粘接剂不能迎合基板的凹凸，成为孔隙等产生的主要原因。
丙烯酸系聚合物的玻璃化转变温度优选为-30～50℃，更优选为-10～40℃，特别优选为0～30℃的范围。玻璃化转变温度过低时，包含膜状粘接剂的粘接剂层与支撑片的剥离力变大，有时引起粘接剂层与支撑片的层间剥离的不良，过高时，有用于固定晶片的粘接力变得不充分的担心。
构成丙烯酸系聚合物的单体(原料单体)含有(甲基)丙烯酸酯单体作为必须成分。作为(甲基)丙烯酸酯单体的具体例，可以列举：(甲基)丙烯酸甲基酯、(甲基)丙烯酸乙基酯、(甲基)丙烯酸丙基酯、(甲基)丙烯酸丁基酯、(甲基)丙烯酸戊基酯、(甲基)丙烯酸己基酯、(甲基)丙烯酸庚基酯、(甲基)丙烯酸辛基酯、(甲基)丙烯酸2-乙基己酯、(甲基)丙烯酸壬基酯、(甲基)丙烯酸癸酯、(甲基)丙烯酸月桂基酯、(甲基)丙烯酸十四烷基酯、(甲基)丙烯酸十八烷基酯等烷基的碳数为1～18的(甲基)丙烯酸烷基酯；(甲基)丙烯酸环烷基酯、(甲基)丙烯酸苄酯、(甲基)丙烯酸异冰片基酯、(甲基)丙烯酸二环戊酯、(甲基)丙烯酸二环戊烯基酯、(甲基)丙烯酸二环戊烯基氧基乙酯、酰亚胺(甲基)丙烯酸酯等具有环状骨架的(甲基)丙烯酸酯；(甲基)丙烯酸羟基甲酯、(甲基)丙烯酸2-羟基乙酯、(甲基)丙烯酸2-羟基丙酯、(甲基)丙烯酸2-羟基丁酯等含有羟基的(甲基)丙烯酸酯；(甲基)丙烯酸缩水甘油基酯、(甲基)丙烯酸3,4-环氧环己基甲基酯等含有环氧基的(甲基)丙烯酸酯；一甲基氨基(甲基)丙烯酸酯、一乙基氨基(甲基)丙烯酸酯、二乙基氨基(甲基)丙烯酸酯等含有氨基的(甲基)丙烯酸酯；2-(甲基)丙烯酰氧基乙基邻苯二甲酸酯、2-(甲基)丙烯酰氧基丙基邻苯二甲酸酯等含有羧基的(甲基)丙烯酸酯。它们可以单独使用1种，也可以将2种以上并用。
另外，作为丙烯酸系聚合物的原料单体，可与(甲基)丙烯酸酯单体一起使用(甲基)丙烯酸、衣康酸等(甲基)丙烯酸酯以外的具有羧基的单体、乙烯基醇、N-羟甲基(甲基)丙烯酰胺等(甲基)丙烯酸酯以外的具有羟基的单体、(甲基)丙烯酰胺、醋酸乙烯酯、丙烯腈、苯乙烯等。
另外，作为构成丙烯酸系聚合物的单体，由于可得到与环氧树脂(B)的相容性好的丙烯酸系聚合物，因而至少优选使用含环氧基的单体。该情况下，在丙烯酸系聚合物中，源于含环氧基的单体的结构单元优选以5～30质量%的范围含有，更优选以10～25质量%的范围含有。通过使丙烯酸系聚合物以这样的范围含有含环氧基的单体作为结构单元，易于避免由于丙烯酸系聚合物与环氧树脂(B)的相容性的下降导致的膜状粘接剂透明性的降低。作为含环氧基的单体，除了上述列举的含环氧基的(甲基)丙烯酸酯以外，还可以列举缩水甘油基乙烯基醚、3,4-环氧环己基乙烯基醚、缩水甘油基(甲基)烯丙基醚、3,4-环氧环己基(甲基)烯丙基醚等。
另外，丙烯酸系聚合物可以含有源于含羟基的(甲基)丙烯酸酯、含氨基的(甲基)丙烯酸酯、(甲基)丙烯酸等具有活性氢基的单体的结构单元。由此，通过在膜状粘接剂中配合下述的交联剂(I)，可使丙烯酸系聚合物交联，能够控制膜状粘接剂的初期粘接力和凝集性。该情况下，在丙烯酸系聚合物中，源于具有活性氢基的单体的结构单元优选以1～30质量%左右的范围含有。
丙烯酸系聚合物可以使用上述原料单体，按照以往公知的方法来制造。
环氧树脂 (B)
作为环氧树脂(B)，可以使用目前公知的各种环氧树脂。环氧树脂可以列举双酚A型环氧树脂、双酚F型环氧树脂、亚苯基骨架型环氧树脂、线性酚醛清漆型环氧树脂、甲酚甲醛型环氧树脂、二环戊二烯型环氧树脂、联苯型环氧树脂、三酚基甲烷型环氧树脂、杂环型环氧树脂、均二苯乙烯型环氧树脂、稠合环芳香族烃改性环氧树脂、在这些的卤化物等的结构单元中含有2个以上的官能团的环氧树脂。另外，也可以使用具有不饱和烃基的环氧树脂。这样的环氧树脂例如在日本特开2008-133330中公开。环氧树脂的环氧当量没有特别限定，优选是150～250(g/eq)。环氧当量是根据JIS K7236；2001测定的值。这些环氧树脂可以单独使用1种，也可以将2种以上并用。
在本发明的膜状粘接剂中，环氧树脂(B)的含量相对于粘合剂树脂(A)100质量份优选为50～1000质量份、更优选为100～600质量份、进而优选为150～400质量份。通过使环氧树脂(B)的含量为上述范围，利用将倒装片安装在基板上的步骤中的焊锡加热时的热，环氧树脂(B)部分固化，膜状粘接剂形成乙阶段(B-stage)状态，容易防止焊锡流出。另外，如果环氧树脂(B)的含量高于上述范围，则膜状粘接剂与支撑片的剥离力过于变高，有时引起包含膜状粘接剂的粘接剂层与支撑片的层间剥离的不良。
热固化剂 (C)
热固化剂(C)作为对于环氧树脂(B)的热固化剂发挥功能。作为热固化剂(C)，可以列举在分子中具有2个以上可与环氧基反应的官能团的化合物。作为可与环氧基反应的官能团，可以列举源于酚羟基、醇性羟基、氨基、羧基、酸酐的官能团等，其中，优选是源于酚羟基、氨基和酸酐的官能团，更优选是酚羟基和氨基。
作为热固化剂(C)的具体例，可以列举酚醛清漆型酚醛树脂、二环戊二烯系酚醛树脂、多官能系酚醛树脂、芳烷基酚醛树脂等酚系热固化剂；DICY(双氰胺)等胺系热固化剂。另外，可使用具有不饱和烃基的热固化剂。例如日本特开2008-248129中公开的、在1分子中具有可与环氧基反应的官能团和不饱和烃基的树脂可以用作具有不饱和烃基的热固化剂。热固化剂(C)可以单独使用1种，也可以将2种以上并用。
在本发明的膜状粘接剂中，热固化剂(C)的含量相对于环氧树脂(B)100质量份，通常为0.1～500质量份，优选为1～200质量份，进而优选为10～100质量份。热固化剂(C)的含量低于上述范围时，固化性不足，有时不能得到具有充分的粘接力的膜状粘接剂。
填料 (D)
通过在膜状粘接剂中配合填料(D)，有时可以调整膜状粘接剂的线性膨胀系数。另外，也可以更为减少膜状粘接剂的固化后的吸湿率。通过减少吸湿率，可以提高半导体封装的可靠性。填料可以是所谓的无机填充剂、有机填充剂的任一者，但从耐热性的角度考虑，优选使用无机填充剂。
作为填料的材质，可以列举二氧化硅、氧化铝、碳酸钙、硅酸钙、氢氧化镁、氢氧化铝、氧化钛、炭黑、滑石、云母或粘土等。其中，优选易于得到透明性、分散性良好，平均粒径小的物质的二氧化硅。填料可以单独使用1种，也可以将2种以上并用。作为填料的二氧化硅可以是利用有机化合物进行了表面修饰的二氧化硅。作为在填料(例如二氧化硅)的表面修饰中使用的有机化合物，可以列举具有(甲基)丙烯酰基等不饱和烃基的化合物。通过使表面修饰中使用的有机化合物具有不饱和烃基，在膜状粘接剂中含有具有不饱和烃基的其它成分时，可在填料与其它成分之间形成键，填料与其它成分的相容性提高。其结果是膜状粘接剂的全光线透射率、雾度值的控制变得容易，同时能够通过膜状粘接剂，以优异的粘接强度将半导体芯片接合在其它半导体芯片、基板上。
膜状粘接剂中填料(D)的含有比例，相对于构成膜状粘接剂的全部固体成分，优选为5质量%以上、更优选为5～50质量%、特别优选为10～30质量%。通过使填料(D)的含有比例为上述范围，可以进而使膜状粘接剂的固化后的吸湿减少，且膜状粘接剂中填料的比率不会过于变大，粘接性的损失少。
填料(D)的平均粒径优选为50nm以下。通过使填料(D)的平均粒径为上述范围，膜状粘接剂不损害与晶片等被粘物的贴附性而可以发挥粘接性。另外，易于将下述的膜状粘接剂的雾度值、全光线透射率调节为所需的范围。可得到所述效果的理由推测如以下所述。即使使用比可见光的波长(以360nm左右为下限)更小的平均粒径的填料，也不能避免由所述粒子导致的称为瑞利散射的可见光的散射。但是，通过使填料(D)的平均粒径为上述范围，可以将瑞利散射抑制为低的程度，将雾度值抑制为较低水平，将全光线透射率维持为较高水平。
填料(D)的平均粒径更优选为1～40nm、特别优选为10～30nm。通过使填料(D)的平均粒径在这样的范围，即使在膜状粘接剂的厚度较厚的情况下，也可以将雾度值抑制为较低水平，将全光线透射率维持为较高水平。
填料(D)的平均粒径表示为利用激光衍射-散射法测定的体积平均粒径。
其它成分
作为其它成分，可以列举下述成分。
(E) 固化促进剂
固化促进剂(E)用于调整膜状粘接剂的固化速度。作为优选的固化促进剂，可以列举三乙二胺、苄基二甲基胺、三乙醇胺、二甲基氨基乙醇、三(二甲基氨基甲基)苯酚等叔胺类；2-甲基咪唑、2-苯基咪唑、2-苯基-4-甲基咪唑、2-苯基-4,5-二羟基甲基咪唑、2-苯基-4-甲基-5-羟基甲基咪唑等咪唑类；三丁基膦、二苯基膦、三苯基膦等有机膦类；四苯基鏻四苯基硼酸盐、三苯基膦四苯基硼酸盐等四苯基硼盐等。它们可以单独使用1种，或将2种以上混合使用。
使用固化促进剂(E)时，固化促进剂(E)以相对于环氧树脂(B)100质量份，优选为0.01～10质量份、进而优选为0.1～1质量份的量含有。通过以上述范围的量含有固化促进剂(E)，即使暴露于高温高湿下也具有优异的粘接性，即使在暴露于严苛的回流焊条件的情况下，也可以实现高的封装可靠性。固化促进剂(E)的含量少时，固化不足，不能得到充分的粘接性，过量时，具有高极性的固化促进剂在高温高湿下，在固化后的膜状粘接剂中向粘接界面侧移动，偏析，由此使封装的可靠性降低。
(F) 偶联剂
通过使用具有与半导体晶片或芯片等无机物反应的官能团和与粘合剂树脂(A)或环氧树脂(B)等所具有的有机官能团反应的官能团的偶联剂(F)，可以使膜状粘接剂对于被粘物的粘接力提高。另外，在不损害将膜状粘接剂固化而得的固化物的耐热性的条件下，可以提高其耐水性。偶联剂(F)优选为硅烷偶联剂。
作为硅烷偶联剂，可以列举γ-环氧丙氧丙基三甲氧基硅烷、γ-环氧丙氧丙基甲基二乙氧基硅烷、β-(3,4-环氧环己基)乙基三甲氧基硅烷、γ-(甲基丙烯酰基丙基)三甲氧基硅烷、γ-氨基丙基三甲氧基硅烷、N-6-(氨基乙基)-γ-氨基丙基三甲氧基硅烷、N-6-(氨基乙基)-γ-氨基丙基甲基二乙氧基硅烷、N-苯基-γ-氨基丙基三甲氧基硅烷、γ-脲基丙基三乙氧基硅烷、γ-巯基丙基三甲氧基硅烷、γ-巯基丙基甲基二甲氧基硅烷、双(3-三乙氧基甲硅烷基丙基)四硫烷(スルファン)、甲基三甲氧基硅烷、甲基三乙氧基硅烷、乙烯基三甲氧基硅烷、乙烯基三乙酰氧基硅烷、咪唑硅烷等。硅烷偶联剂可以单独使用1种，也可以将2种以上并用。
偶联剂(F)的含量相对于粘合剂树脂(A)和环氧树脂(B)的合计100质量份，通常为0.1～20质量份、优选为0.2～10质量份、更优选为0.3～5质量份。偶联剂(F)的含量小于0.1质量份时，有时不能得到上述效果，超过20质量份时，有时成为排气的原因。
(G) 能量射线聚合性化合物
膜状粘接剂可含有能量射线聚合性化合物(G)。能量射线聚合性化合物(G)含有不饱和烃基，受到紫外线、电子束等能量射线的照射时，进行聚合固化。通过能量射线照射使能量射线聚合性化合物(G)聚合，可以使膜状粘接剂的粘接力降低。因此，容易进行支撑片与膜状粘接剂的层间剥离。
作为这样的能量射线聚合性化合物(G)，具体可以列举三羟甲基丙烷三丙烯酸酯、季戊四醇三丙烯酸酯、季戊四醇四丙烯酸酯、二季戊四醇单羟基五丙烯酸酯、二季戊四醇六丙烯酸酯或1,4-丁二醇二丙烯酸酯、1,6-己二醇二丙烯酸酯、聚乙二醇二丙烯酸酯、低聚酯丙烯酸酯、聚氨酯丙烯酸酯系低聚物、环氧改性丙烯酸酯、聚醚丙烯酸酯和衣康酸低聚物等丙烯酸酯系化合物。这样的化合物在分子内具有至少1个聚合性双键，通常重均分子量为100～30000、优选为300～10000左右。使用能量射线聚合性化合物(G)时，其配合量没有特别限定，但优选相对于构成膜状粘接剂的全部固体成分，以1～50质量%左右的比例使用。
(H) 光聚合引发剂
在膜状粘接剂中配合能量射线聚合性化合物(G)时，照射紫外线等能量射线，可以使包含膜状粘接剂的粘接剂层从支撑片的剥离性提高。通过在膜状粘接剂中含有光聚合引发剂(H)，可以减少聚合-固化时间和光线照射量。
作为光聚合引发剂(H)，具体地可以列举二苯甲酮、乙酰苯、苯偶姻、苯偶姻甲基醚、苯偶姻乙基醚、苯偶姻异丙基醚、苯偶姻异丁基醚、苯偶姻苯甲酸、苯偶姻苯甲酸甲酯、苯偶姻二甲基缩酮、2,4-二乙基噻吨酮、α-羟基环己基苯基酮、苄基二苯基硫化物、一硫化四甲基秋兰姆、偶氮双异丁腈、苄基、二苄基、二乙酰、1,2-二苯基甲烷、2-羟基-2-甲基-1-[4-(1-甲基乙烯基)苯基]丙酮、2,4,6-三甲基苯甲酰二苯基氧化膦和β-氯蒽醌等。光聚合引发剂(H)可以单独使用1种，或将2种以上组合使用。
光聚合引发剂(H)的含量相对于能量射线聚合性化合物(G)100质量份优选为0.1～10质量份，更优选为1～5质量份。如果光聚合引发剂(H)的含量低于上述范围，则有时由于光聚合的不足而不能得到满意的层间剥离性，如果高于上述范围，则生成对光聚合没有帮助的残留物，有时膜状粘接剂的固化性变得不充分。
(I) 交联剂
为了调节其初期粘接力和凝集力，也可以在膜状粘接剂中添加交联剂(I)。作为交联剂(I)，可以列举有机多元异氰酸酯化合物、有机多元亚胺化合物等。
作为有机多元异氰酸酯化合物，可以列举芳香族多元异氰酸酯化合物、脂肪族多元异氰酸酯化合物、脂环族多元异氰酸酯化合物和这些有机多元异氰酸酯化合物的三聚物、以及使这些有机多元异氰酸酯化合物与多元醇化合物反应而得的末端异氰酸酯聚氨酯预聚物等。
作为有机多元异氰酸酯化合物的进一步具体的例子，可以列举2,4-甲苯二异氰酸酯、2,6-甲苯二异氰酸酯、1,3-二甲苯二异氰酸酯、1,4-二甲苯二异氰酸酯、二苯基甲烷-4,4’-二异氰酸酯、二苯基甲烷-2,4’-二异氰酸酯、3-甲基二苯基甲烷二异氰酸酯、1,6-己二异氰酸酯、异佛尔酮二异氰酸酯、二环己基甲烷-4,4’-二异氰酸酯、二环己基甲烷-2,4’-二异氰酸酯、三羟甲基丙烷-甲苯二异氰酸酯加成物和赖氨酸异氰酸酯。
作为有机多元亚胺化合物的具体例子，可以列举N,N’-二苯基甲烷-4,4’-双(1-氮丙啶羧酰胺)、三羟甲基丙烷-三-β-氮杂环丙基丙酸酯、四羟甲基甲烷-三-β-氮杂环丙基丙酸酯和N,N’-甲苯-2,4-双(1-氮丙啶羧酰胺)三亚乙基三聚氰胺等。
交联剂(I)以相对于粘合剂树脂(A)100质量份，优选为1～40质量份、更优选为8～35质量份、特别优选为12～30质量份的比率使用。
(J) 通用添加剂
在膜状粘接剂中，除了上述以外，可以根据需要配合各种添加剂。作为各种添加剂，可以列举增塑剂、防静电剂、抗氧化剂、阻燃剂、吸气剂或链转移剂等。
包含上述各成分的膜状粘接剂的D65标准光源的全光线透射率为70%以上，雾度值为50%以下。
如果全光线透射率小于70%、或雾度值超过50%，则在半导体装置的制造步骤中，在将带有膜状粘接剂的芯片固定(小片键合)在基板或其他芯片等上时、或在带有膜状粘接剂的基板上固定半导体芯片等时，变得难以读取定位(位置确定)标记，不能正确地进行小片键合。
膜状粘接剂的D65标准光源的全光线透射率优选为75～100%，雾度值优选为1～40%。
膜状粘接剂的全光线透射率或雾度值可以通过调整填料(D)的平均粒径、或填料(D)以外的各成分的相容性来控制。
另外，膜状粘接剂的固化后的吸湿率优选为5%以下，更优选为3%以下，特别优选为0～2%。通过使膜状粘接剂的固化后的吸湿率为上述范围，可以使半导体封装的可靠性提高。应予说明，吸湿率是利用下述的实施例中的条件和方法测定的168小时后的吸湿率。
(半导体接合用粘接片)
本发明的半导体接合用粘接片通过将包含“含有上述各成分的膜状粘接剂”的粘接剂层叠层于支撑片上来制造。粘接剂层具有压敏粘接性或热粘接性和加热固化性。粘接剂层具有压敏粘接性时，能够以未固化状态按压在被粘物上来进行贴附。另外，粘接剂层具有热粘接性的情况下，在按压于被粘物上时，可以将粘接剂层加热来进行贴附。本发明中的热粘接性是指在常温下没有压敏粘接性，但通过热进行软化而可在被粘物上粘接。因此，本发明的半导体接合用粘接片中的粘接剂层具有在未固化状态下将各种被粘物暂时保持的功能。因此，可以在利用半导体接合用粘接片保持被粘物的状态下进行被粘物的没有被贴附在片上的面(背面)的加工、例如研磨加工。经过热固化，可以最终提供耐冲击性高的固化物，粘接强度也优异，即使在严酷的高温高湿条件下也可保持充分的粘接性。构成膜状粘接剂的粘接剂组合物可将上述各成分以适当的比例混合得到。混合时，可将各成分预先用溶剂稀释，另外可在混合时加入到溶剂中。
以下对于半导体接合用粘接片的合适方式和使用方式进行说明。在粘接剂层以可剥离的方式形成于支撑片上而成的半导体接合用粘接片的使用时，将粘接剂层粘接在晶片或基板等被粘物上，将支撑片剥离，将粘接剂层转印在被粘物上。本发明的半导体接合用粘接片的形状可采用带状、标签状等所有的形状。
支撑片可以是仅包含在表面不具有折缝(タック)的树脂膜的物质、或对树脂膜适当地进行了表面处理等的物质，或也可以是在树脂膜上具有粘着剂层的粘着片。另外，可在树脂膜上设置凹凸吸收层。
作为用作支撑片的树脂膜，可以使用例如聚乙烯膜、聚丙烯膜、聚丁烯膜、聚丁二烯膜、聚甲基戊烯膜、聚氯乙烯膜、氯乙烯基共聚物膜、聚对苯二甲酸乙二酯膜、聚萘二甲酸乙二酯膜、聚对苯二甲酸丁二酯膜、包含聚氨酯聚合物和乙烯基系聚合物的复合膜、聚氨酯丙烯酸酯固化物膜、乙烯醋酸乙烯酯共聚物膜、离聚物树脂膜、乙烯-(甲基)丙烯酸共聚物膜、乙烯-(甲基)丙烯酸酯共聚物膜、聚苯乙烯膜、聚碳酸酯膜、聚酰亚胺膜、氟树脂膜等膜。另外也可使用它们的交联膜。进而也可以是它们的叠层膜。另外，可以使用将它们着色了的膜等。粘接剂层具有能量射线固化性时，优选具有能量射线的透射性。另外，在要求在进行支撑片与粘接剂层的层间剥离之前可以目视确认被粘物的表面的情况下，优选具有可见光的透射性(透明或半透明)。
其中，作为树脂膜，优选使用23℃时的储能弹性模量(貯蔵弾性率)优选为1×107Pa以上、更优选为1×108～1×109Pa的树脂膜。另外，优选使用基于拉伸试验的23℃时的应力松弛率优选为40%以上、更优选为70～90%的树脂膜。通过使用储能弹性模量、应力松弛率为上述范围的树脂膜，可以在晶片的背面研磨步骤中，抑制晶片的翘曲、凹痕的发生。
其中，基于拉伸试验的23℃时的应力松弛率利用以下的方法测定。将树脂膜切成15mm×140mm而形成样品。在23℃、相对湿度50%的环境下，使用万能拉伸试验机(SHIMADZU社制オートグラフAG-10kNIS)，将该样品的两端20mm夹住，以每分钟200mm的速度拉伸，测定拉伸10%时的应力A(N/m2)、和从带状物的伸长停止起1分钟后的应力B(N/m2)。由这些应力A、B的值算出(A-B)/A×100(%)来作为应力松弛率。
这样的膜的特性用包含聚氨酯聚合物和乙烯基系聚合物的复合膜、或聚氨酯丙烯酸酯固化物膜易于得到。作为包含聚氨酯聚合物和乙烯基系聚合物的复合膜，例如可以使用日本特开2007-84722中公开的物质。作为聚氨酯丙烯酸酯固化物膜，例如可以使用日本特开平11-343469中公开的物质。
本发明的半导体接合用粘接片贴附在各种被粘物上，对被粘物施加所需的加工后，粘接剂层以在被粘物上固着残留的状态从支撑片上被剥离。即，在含有将粘接剂层从支撑片上转印至被粘物的步骤的工艺中使用。因此，支撑片的与粘接剂层相接的面的表面张力优选为40mN/m以下、进而优选为37mN/m以下、特别优选为35mN/m以下。下限值通常为25mN/m左右。这样的表面张力低的支撑片可以适当地选择树脂膜的材质来得到，或也可以通过在树脂膜的表面涂布剥离剂而实施剥离处理来得到。
作为在树脂膜的剥离处理中使用的剥离剂，可以使用醇酸系、有机硅系、氟系、不饱和聚酯系、聚烯烃系、蜡系等，特别是醇酸系、有机硅系、氟系的剥离剂具有耐热性，因此是优选的。
为了使用上述剥离剂对树脂膜的表面进行剥离处理，将剥离剂直接以无溶剂的状态、或进行溶剂稀释、乳化，利用凹版印刷涂布机、麦勒棒涂布器(メイヤーバーコーター)、气刀涂布机、辊涂机等进行涂布，将涂布了剥离剂的支撑片供于常温下或加热下、或利用电子束使其固化，形成剥离剂层即可。
另外，可以利用湿式层压或干式层压、热熔融层压、熔融挤出层压、共挤出加工等进行膜的叠层，由此调整支撑片的表面张力。即，制造将至少一面的表面张力作为与上述支撑片的粘接剂层相接的面的张力为优选的范围内的膜、以使该面为与粘接剂层相接的面的方式与其它膜叠层的叠层体，可形成支撑片。
支撑片可以是在上述这样的树脂膜上具有粘着剂层的粘着片。出于可将粘接剂层从粘着剂层剥离的目的，粘着剂层可以由具有再剥离性的公知粘着剂构成，通过选择紫外线固化型、加热发泡型、水溶胀型、弱粘型等粘着剂，可以使粘接剂层的剥离变得容易。特别地，使用包含聚氨酯聚合物和乙烯基系聚合物的复合膜或聚氨酯丙烯酸酯固化物膜作为树脂膜的构成层时，这些膜通常柔软，具有自粘性，因此它们为与粘接剂层直接接触的构成时，层间剥离有时变得困难。因此，为了避免这样的情况，优选使支撑片为粘着片。
粘着片的粘着力优选为10～10000mN/25mm，更优选为50～2000mN/25mm。粘着力是根据JIS Z 0237；2009，贴附在被粘物(SUS)上、经过30分钟后的粘着片由180°撕扯法得到的粘着力。通过使粘着片的粘着力在上述范围，从粘着剂层上剥离粘接剂层变得容易。
另外，粘着剂层的23℃时的储能弹性模量优选为1×104Pa以上、更优选为1×105～1×108Pa。通过使用储能弹性模量为上述范围的粘着剂层，可以在晶片的背面研磨步骤中，抑制晶片的翘曲、凹痕的发生。
另外，为了使树脂膜的上面、即设置粘着剂层的一侧的树脂膜表面与粘着剂层的密合性提高，可以实施电晕处理，或设置底漆层。另外，也可以在与粘着剂层相反的面上涂覆各种涂膜。
设置在树脂膜上的凹凸吸收层例如可利用一直以来公知的各种粘着剂形成，可以是兼具凹凸吸收层和粘着剂层的层。作为粘着剂，没有任何限定，可以使用例如橡胶系、丙烯酸系、有机硅系、聚乙烯基醚等粘着剂。另外，可以还使用能量射线固化型或加热发泡型、水溶胀型的粘着剂。另外，可以将包含聚氨酯聚合物和乙烯基系聚合物的复合膜或聚氨酯丙烯酸酯固化物膜作为凹凸吸收层使用。进而，可以在包括包含聚氨酯聚合物和乙烯基系聚合物的复合膜或聚氨酯丙烯酸酯固化物膜的凹凸吸收层上进而设置粘着剂层。应予说明，支撑片具有多层包含聚氨酯聚合物和乙烯基系聚合物的复合膜或聚氨酯丙烯酸酯固化物膜时，从粘着剂层除去处于最远位置的物质，包含聚氨酯聚合物和乙烯基系聚合物的复合膜或聚氨酯丙烯酸酯固化物膜视为凹凸吸收层。
作为包含聚氨酯聚合物和乙烯基系聚合物的复合膜或聚氨酯丙烯酸酯固化物膜，除了可以使用上述的物质以外，作为聚氨酯丙烯酸酯固化物膜，也可以是日本特开2011-068727中公开的、使片叠层于树脂膜上而形成凹凸吸收层，所述片是将含有聚氨酯丙烯酸酯系低聚物、和在分子内具有硫醇基的化合物的能量射线固化型组合物固化而成的片。
凹凸吸收层的23℃时的储能弹性模量优选为1×104Pa以上，更优选为3×105～3×106Pa。另外，凹凸吸收层的附加20%扭转应力的10秒后的应力松弛率优选为50%以上、更优选为80～99.9%。通过使用储能弹性模量、应力松弛率为上述范围的凹凸吸收层，可在晶片的半导体接合用粘接片被贴附的面上形成具有数十μm左右的高度的突起，凹凸吸收层吸收突起，能够平坦地保持半导体接合用粘接片的表面。另外，即使在粘接剂层的厚度比这样的突起的高度更薄的情况下，凹凸吸收层通过吸收贯穿粘接剂层的突起，粘接剂层也接近、到达晶片表面，也能够使粘接剂层与晶片表面粘接。
另外，对于半导体接合用粘接片，支撑片和粘接剂层可以是预先以与被粘物(半导体晶片等)相同的形状起模而成的形状。特别地，包含支撑片和粘接剂层的叠层体可以是在长的工程膜上连续地保持的形态。作为工程膜，可以使用作为上述支撑片例示的树脂膜。
支撑片的厚度通常为10～500μm、优选为15～300μm、特别优选为20～250μm左右。支撑片为粘着片时，通常在支撑片的厚度中，包含粘着剂的层的厚度占1～50μm左右。另外，设置凹凸吸收层时，通常在支撑片的厚度中，凹凸吸收层的厚度占10～450μm左右。另外，粘接剂层的厚度通常为2～500μm、优选为6～300μm、特别优选为10～150μm左右。粘接剂层的厚度优选与贴附的晶片中形成的凸部的高度大致相同。
对于半导体接合用粘接片，为了在使用前保护粘接剂层，可以在粘接剂层的上面预先叠层剥离膜。该剥离膜可使用在聚对苯二甲酸乙二酯膜、聚丙烯膜等塑料材料上涂布有机硅树脂等剥离剂的物质。
半导体接合用粘接片的制造方法没有特别限定，支撑片为树脂膜时，可以通过在树脂膜上将粘接剂组合物涂布干燥，形成粘接剂层来进行制造。另外也可以通过将粘接剂层设置在剥离膜上，将其转印到上述树脂膜或粘着片上来进行制造。另外，半导体接合用粘接片可以以形成与贴附在粘接剂层上的晶片的形状相同的形状或比晶片更大的同心圆的形状等的方式、利用冲裁加工等进行切断。
接着，对于本发明的半导体接合用粘接片的利用方法，采用例子说明将该粘接片贴附在晶片上、适用于半导体装置的制造的情况。
(半导体装置的制造方法)
本发明的半导体装置的制造方法包含将上述半导体接合用粘接片的粘接剂层贴附在晶片上的步骤、将晶片单片化而得到芯片的步骤、和经由粘接剂层将芯片固定的步骤。
以下对于本发明的半导体装置的制造方法的一部分例子进行详述。
在本发明的半导体装置的第1制造方法中，首先在表面形成了电路的半导体晶片的电路面上贴附半导体接合用粘接片。在进行贴附时，可以将半导体晶片的电路面载置于半导体接合用粘接片的粘接剂层上，轻轻按压，根据情况加热，一边使粘接剂层软化一边将半导体晶片固定。接着根据需要，在利用半导体接合用粘接片将半导体晶片的电路面保护的状态下，将晶片的背面研磨，形成规定厚度的晶片。
半导体晶片可以是硅晶片，另外也可以是镓-砷等的化合物半导体晶片。在晶片表面上的电路的形成可以利用包含蚀刻法、剥离法(lift off method)等一直以来普遍使用的方法的各种方法进行。在半导体晶片的电路形成步骤中，形成规定的电路。这样的晶片的研磨前的厚度没有特别限定，通常为500～1000μm左右。另外，半导体晶片的表面形状没有特别限定，但可形成突起状电极。作为突起状电极，可以列举圆柱型电极、球状电极等。另外，可以是具有贯通电极的半导体晶片。半导体接合用粘接片在半导体晶片上的贴附方法没有特别限定。
背面研磨可在贴附了半导体接合用粘接片的状态通过使用研磨机和用于晶片步骤的吸附台(吸着テーブル)等的公知方法进行。背面研磨步骤之后，可进行除去由研磨生成的破碎层的处理。背面研磨后的半导体晶片的厚度没有特别限定，优选为10～400μm，特别优选为25～300μm左右。根据本发明的半导体接合用粘接片，可以在晶片的背面研磨时可靠地保持晶片，另外能够防止切削水向电路面的侵入，同时可以防止晶片翘曲、凹痕的发生。
背面研磨步骤后，在晶片的背面贴附所谓的称作切割片的粘着片。切割片的贴附一般利用称作贴片机的装置进行，没有特别限定。接着，在晶片的电路面上残留粘接剂层，仅剥离支撑片。将支撑片剥离的方法没有特别限定。
然后，进行贴附于切割片上的晶片的切割，将晶片单片化而得到芯片。
半导体晶片的切断手段没有特别限定。作为一个例子，可以列举在晶片的切断时将切割片的周边部利用环形框架(ring frame)固定后，通过使用切割机等旋转圆刃等公知手法进行晶片的芯片化的方法等。此时的切断深度为加入了粘接剂层的厚度和半导体晶片的厚度的合计和切割锯片的磨损部分的深度。另外，可以利用激光将粘接剂层和晶片切断。
接着根据需要，进行切割片的膨胀时，半导体芯片间隔扩张，可进而容易地进行半导体芯片的拾取。此时，在芯片与切割片之间产生偏移，芯片与切割片之间的粘接力减少，半导体芯片的拾取性提高。这样，进行半导体芯片的拾取时，使切断的粘接剂层在半导体芯片电路面固着残留，可以从切割片上剥离。
接着，进行半导体芯片的键合步骤(小片键合)。在键合步骤中，介由粘接剂层将半导体芯片载置于引线框的晶片焊垫(die pad)上或其它的半导体芯片(下段芯片)表面上(以下将搭载芯片的晶片焊垫或下段芯片表面记为“芯片搭载部”)。在本发明中，由于固着在半导体芯片的表面上的粘接剂层的全光线透射率、雾度值为规定的范围，因此在小片键合时可以容易地读取芯片表面的定位标记。其结果是能够将半导体芯片正确地在芯片搭载部进行小片键合。芯片搭载部可在载置半导体芯片之前进行加热，另外，也可以在刚刚载置芯片后进行加热。加热温度通常为80～200℃，优选为100～180℃，加热时间通常为0.1秒～5分钟，优选为0.5秒～3分钟，载置时的压力通常为1kPa～200MPa。
将半导体芯片载置于芯片搭载部后，根据需要与利用了下述树脂密封中的加热的粘接剂层的固化不同，可进行用于粘接剂层的固化的加热。此时的加热条件在上述加热温度的范围，加热时间通常为1～180分钟，优选为10～120分钟。
另外，不进行载置后的加热处理而形成临时粘接状态，可利用在封装制造中通常进行的树脂密封的加热，使粘接剂层固化。通过经历这样的步骤，粘接剂层固化，将半导体芯片与芯片搭载部牢固地粘接，可将芯片固定。粘接剂层在小片键合条件下流动化，因此可充分填埋芯片搭载部的凹凸中，能够防止孔隙的发生，封装的可靠性变高。
在本发明的半导体装置的第2制造方法中，与上述第1制造方法同样地，在半导体晶片的电路面上贴附半导体接合用粘接片，将晶片的背面进行研磨。背面研磨步骤之后，可进行除去由研磨生成的破碎层的处理。
背面研磨后，从晶片的背面侧向晶片内部照射激光。激光由激光源进行照射。激光源是使波长和相位一致的光产生的装置，作为激光的种类，可以列举产生脉冲激光的Nd-YAG激光器、Nd-YVO激光器、Nd-YLF激光器、Ti-sapphire激光器等产生多光子吸收的设备。激光的波长优选为800～1100nm，进而优选为1064nm。
激光向晶片内部照射，沿着预定切断线在晶片内部形成改性部。激光扫描一个预定切断线的次数可以为1次或多次。优选监测激光的照射位置以及电路间的预定切断线的位置，一边进行激光的对位，一边进行激光的照射。应予说明，预定切断线是将在晶片表面形成的各电路间区分开来的假想的线。
改性部形成后，在晶片背面贴附切割片。接着，使粘接剂层残留在晶片的电路面上，仅剥离支撑片。
接着，进行贴附于切割片上的晶片的切割，将晶片单片化而得到芯片。半导体晶片通过将切割片进行膨胀而芯片化。即，如果通过激光照射在晶片内部形成改性部后，进行膨胀，则切割片伸长，半导体晶片以晶片内部的改性部为起点，被切断分离成一个一个的芯片。此时，粘接剂层也切断分离成一个一个的芯片大小。另外，在膨胀的同时使用夹具等抓住(ひっかく)切割片，也可以将切割片伸长而将粘接剂层和晶片切断分离成每个芯片。膨胀优选在-20～40℃的环境下、以5～600mm/分钟的速度进行。另外，膨胀步骤后，为了消除膨胀了的切割片的松弛，也可以进行热收缩。然后，在表面具有粘接剂层的芯片被拾取，经过键合步骤来制造半导体装置。键合步骤与上述第1制造方法同样。
以上详述的第1制造方法和第2制造方法终究只不过表示本发明制造方法的一部分的例子，本发明的制造方法也可以采用其他的方式。例如，可以不使用半导体接合用片，而在晶片上单独贴附膜状粘接剂，将用于晶片的背面研磨的保护片另外贴附在膜状粘接剂上。
另外，也可以是在将膜状粘接剂或半导体接合用粘接片贴附在晶片上之前的阶段，完成晶片的背面研磨，膜状粘接剂或半导体接合用粘接片的贴附后不进行晶片的背面研磨的制造方法。
另外，晶片的单片化方法可以是基于从晶片的表面侧形成深度比晶片的厚度更小的沟，将晶片的背面研磨、直至到达沟，由此进行单片化的所谓先切割法的方法，或可以是如日本特开2004-111428中记载那样的、在使激光从晶片的表面与芯片的形状一致而进行入射，在晶片内部形成改性区域的步骤中，附加了将晶片的背面研磨的步骤的晶片的分割方法。
由上述半导体装置的制造方法可知，本发明的半导体接合用粘接片，能够用作可适用于从晶片的背面研磨步骤至芯片的键合步骤的背面研磨-小片键合片。
实施例
以下通过实施例说明本发明，但本发明不限于这些实施例。应予说明，在以下的实施例和比较例中，各评价如以下这样进行。
＜雾度值和全光线透射率＞
使用粘接剂组合物(1)～(5)，将各粘接剂组合物涂布于剥离膜(リンテック社制SP-PET381031)上后，使其干燥(在烘箱中100℃、1分钟)，制作厚度为20μm的膜状粘接剂。另外，制作其它的厚度20μm的膜状粘接剂，将膜状粘接剂叠层，由此得到厚度为40μm、60μm、80μm、100μm的膜状粘接剂。接着，将剥离膜剥离，制成评价用样品。使用雾度仪(日本电色工业社制　NDH-5000)，根据JIS K7136：2000，测定评价用样品的膜状粘接剂的雾度值(%)。另外，根据JIS K7361：2000，测定评价用样品的膜状粘接剂的D65标准光源的全光线透射率(%)。
＜吸湿率＞
将使用粘接剂组合物(1)～(5)制作的膜状粘接剂(50mm见方)叠层为200μm的厚度，得到叠层片，形成评价用样品。将评价用样品在140℃的烘箱中进行1小时的加热固化后，投入到湿热条件(85℃、相对湿度85%)下规定的时间(24小时和168小时)，测定投入前后的固化物的重量变化(%)，得到24小时后和168小时后的吸湿率。
＜定位＞
准备ウォルツ社制8英寸晶片“WALTS-TEG MB50-0101JY_TYPE-B(具有聚酰亚胺膜)、厚度725μm”。在形成于该晶片上的各单片化预定区域上存在544个垫片。对于这些的各垫片，制作30μm高度的Cu柱，进而在这些Cu柱上以15μm的高度设置SnAg焊锡，形成合计高度为45μm的凸块。按照以上的顺序，准备模仿倒装型晶片的评价用晶片。
对于评价用晶片的凸块设置面，使用全自动背面研磨带用带式层压机(リンテック株式会社制RAD-3510F/12)将实施例和比较例中得到的半导体接合用粘接片层压。
接着，使用晶片背面研磨装置(株式会社ディスコ制DGP8760)进行研磨和干式抛光处理，得到300μm厚的晶片。然后，使用全自动多晶片贴片机(リンテック株式会社制RAD-2700F/12)，在干式抛光面贴附紫外线(UV)固化型切割带(リンテック株式会社制 Adwill D-678)，固定于环形框架上。
接着，利用相同装置将半导体接合用粘接片的支撑片剥离，使粘接剂层暴露。然后，使用全自动切割锯(株式会社ディスコ制DFD651)进行切割，将各芯片单片化(7.3mm×7.3mm)。
对于附着了定向的芯片的切割带，使用半自动UV照射装置(リンテック株式会社制RAD-2000m/12)进行UV照射(照度230mW/cm2、光量180mJ/cm2、氮氛围下)，使切割带的粘着力降低。接着，通过手工作业将附着了粘接剂层的芯片由切割带剥离，为了防止固着，以粘接剂层侧向下的方式收纳于在芯片收纳部底面贴附了剥离膜(リンテック株式会社制 SP-PET381031)的芯片载盘。
使用倒装式接合器(flip-chip bonder)(九州松下株式会社制、商品名“FB30T-M”)，将单片化了的带有粘接剂层的芯片从芯片载盘取出，对其凸块设置面(贴附了粘接剂层的面)的能否识别图案进行评价。进行10个芯片的试验，将10个都可识别图案的情况设为“A”、将6～9个的情况设为“B”、将5个以下的情况设为“C”。
[膜状粘接剂的制造例]
构成膜状粘接剂的粘接剂组合物(1)～(5)的各成分如下述和表1所述。按照下述成分和表1的配合量，配合各成分，制备粘接剂组合物(1)～(5)。在表1中，各成分的数值表示固体成分换算的质量份，在本发明中，固体成分是指溶剂以外的全部成分。
(A)丙烯酸系聚合物：包含正丁基丙烯酸酯55质量份、甲基丙烯酸酯10质量份、甲基丙烯酸缩水甘油酯20质量份和2-羟基乙基丙烯酸酯15质量份的丙烯酸系聚合物(重均分子量：90万、玻璃化转变温度：-28℃)
(B1)环氧树脂：双酚A型环氧树脂(ジャパンエポキシレジン社制　jER828、环氧当量：235g/eq)
(B2)环氧树脂：酚醛清漆型环氧树脂(日本化药社制　EOCN-104S、环氧当量：218g/eq)
(C)热固化剂：酚醛清漆型酚醛树脂(DIC社制　TD-2131、酚羟基当量：103g/eq)
(D1)填料：二氧化硅填料(日产化学社制　MEK-ST、平均粒径：10～15nm)
(D2)填料：二氧化硅填料(アドマテックス制　YA050C-MJE、平均粒径：50nm)
(D3)填料：二氧化硅填料(アドマテックス制　アドマファインSC2050、平均粒径：500nm)
(D4)填料：炭黑(三菱化学社制 ＃MA650、平均粒径：28nm)
(E)固化促进剂：2-苯基-4,5-二羟基甲基咪唑(四国化成工业社制 キュアゾール2PHZ-PW)
(F)偶联剂：硅烷偶联剂(信越化学社制　KBE-403)。
[表1]
。
使用上述的粘接剂组合物(1)～(5)形成膜状粘接剂，进行各评价。结果示于表2。
[表2]
。
(实施例1)
将重均分子量5000的聚氨酯丙烯酸酯系低聚物(荒川化学社制)50质量份、丙烯酸异冰片基酯50质量份、光聚合引发剂(イルガキュア184、チバ・ガイギー社制)2.0质量份、和酞菁系颜料0.2质量份配合，得到光固化型树脂组合物。将所得的树脂组合物利用喷水模头(ファウンテンダイ)方式以厚度达到110μm的方式涂覆到作为浇铸用工程片的经过了剥离处理的PET膜(リンテック株式会社制、SP-PET381031)上，形成树脂组合物层。刚涂覆后，在树脂组合物层上进而层压进行了相同剥离处理的PET膜，然后，使用高压水银灯(160W/cm、高度10cm)，以光量为250mJ/cm2 的条件进行紫外线照射，由此使树脂组合物层交联、固化，得到夹在2张剥离膜中的厚度为110μm的树脂膜。
接着，另外准备其他的剥离膜(リンテック株式会社制、SP-PET381031)。制备粘着剂层形成用涂覆液，其是在将2-乙基己基丙烯酸酯、甲基丙烯酸甲酯、丙烯酸2-羟基乙酯以80：10：10的质量比聚合而得的重均分子量70万的丙烯酸酯共聚物的、浓度为40质量%的甲苯溶液100质量份(含有溶剂的量)中添加了异氰酸酯系交联剂(ポリウレタン工业株式会社制、コロネートL)20质量份(含有溶剂的量)而得的涂覆液。将该粘着剂层形成用涂覆液以干燥后的厚度为10μm的方式涂布在其它剥离膜的剥离处理面上，在80℃进行2分钟的干燥且接着在100℃进行1分钟的干燥，得到在其它剥离膜上形成的粘着剂层。
将该粘着剂层转印至树脂膜，除去浇铸用工程片，在23℃、相对湿度50%的环境下保管14天，由此进行养护，得到粘着片(支撑片1)。
将粘接剂组合物(1)利用甲基乙基酮稀释，以使固体成分浓度为50质量%，在进行了有机硅处理的剥离膜(リンテック株式会社制　SP-PET381031)上进行涂布、干燥(干燥条件：在烘箱中100℃、1分钟)，以使干燥后厚度为20μm，得到在剥离膜上形成的膜状粘接剂。反复该操作，得到在其它的剥离膜上形成的、干燥后的厚度为20μm的膜状粘接剂。接着，将所得的膜状粘接剂叠层，制作厚度为40μm的膜状粘接剂。
然后，使膜状粘接剂与从上述粘着片除去其它的剥离膜而露出的粘着片的粘着剂层贴合，将膜状粘接剂转印至粘着片上，由此得到所需的半导体接合用粘接片。各评价结果示于表3。
(实施例2)
使重均分子量4000的聚丙二醇(以下记为PPG4000)33g与异佛尔酮二异氰酸酯5g聚合而得到末端异氰酸酯基聚氨酯预聚物，使该末端异氰酸酯基聚氨酯预聚物与季戊四醇三丙烯酸酯10g反应，得到重均分子量为17350的聚氨酯丙烯酸酯系低聚物。
添加所得的聚氨酯丙烯酸酯系低聚物100g(固体成分)、作为稀释单体的丙烯酸异冰片基酯66.7g、和作为光聚合引发剂的2-羟基-2-甲基-1-苯基-丙烷-1-酮(チバスペシャルティケミカルズ社制：ダロキュア1173、固体成分浓度100质量%)0.83g、作为具有硫醇基的化合物的季戊四醇四(3-巯基丙酸酯)(堺化学工业社制：PEMP、固体成分浓度100质量%)39.2g(80.2mmol)，得到常温液体的能量射线固化型组合物。
在作为浇铸用工程片的经过了剥离处理的PET膜(リンテック株式会社制：SP-PET381031)上，用喷水模头方式以厚度达到90μm的方式涂布上述能量射线固化型组合物，形成固化型组合物层，然后，从固化型组合物层侧进行紫外线照射。作为紫外线照射装置，使用传送带式紫外线照射装置(アイグラフィクス社制：ECS-401GX)，紫外线源使用高压水银灯(アイグラフィクス社制：H04-L41)｛照射条件：灯高度150mm、灯功率3kW(换算功率120mW/cm)、光线波长365nm的照度271mW/cm2、光量177mJ/cm2(オーク制作所社制紫外线光量计：UV-351)｝。然后，刚照射后在固化型组合物层上贴合实施例1的树脂膜，从树脂膜侧进而进行2次紫外线照射，使组合物交联、固化｛照射条件：灯高度150mm、灯功率3kW(换算功率120mW/cm)、光线波长365nm的照度271mW/cm2、光量600mJ/cm2(オーク制作所社制紫外线光量计：UV-351)｝。然后，将经过了剥离处理的PET膜剥离，得到厚度90μm的凹凸吸收层叠层了的树脂膜。
在该叠层体的凹凸吸收层上转印实施例1的粘着剂层，在23℃、相对湿度50%的环境下保管14天，由此进行养护，得到带有凹凸吸收层的粘着片(支撑片2)。
接着，得到除了将厚度为20μm的膜状粘接剂叠层、使膜状粘接剂的厚度达到100μm以外、其它用与实施例1同样的顺序形成的膜状粘接剂，转印至带有凹凸吸收层的粘着片的粘着剂层上，由此得到半导体接合用粘接片。各评价结果示于表3。
(实施例3)
除了使用粘接剂组合物(2)以外，其它与实施例1同样地得到半导体接合用粘接片。各评价结果示于表3。
(实施例4)
除了使用粘接剂组合物(2)以外，其它与实施例2同样地得到半导体接合用粘接片。各评价结果示于表3。
(实施例5)
除了使用厚度100μm的低密度聚乙烯膜(支撑片3)作为支撑片以外，其它与实施例1同样地得到半导体接合用粘接片。各评价结果示于表3。
(比较例1)
除了使用粘接剂组合物(3)以外，其它与实施例1同样地得到半导体接合用粘接片。各评价结果示于表3。
(比较例2)
除了使用粘接剂组合物(4)以外，其它与实施例1同样地得到半导体接合用粘接片。各评价结果示于表3。
[表3]
。
由上述结果可知，对于本发明的半导体接合用粘接片，小片键合时的定位优异。另外，没有配合填料(D)的粘接剂组合物(5)与其它粘接剂组合物相比，吸湿性差。

Claims (8)

1.膜状粘接剂，其含有粘合剂树脂(A)、环氧树脂(B)、热固化剂(C)和填料(D)，其中，
D65标准光源的全光线透射率为70%以上，
雾度值为50%以下。
2.根据权利要求1所述的膜状粘接剂，其中，含有5质量%以上的填料(D)。
3.根据权利要求1或2所述的膜状粘接剂，其中，填料(D)的平均粒径为50nm以下。
4.根据权利要求1～3中任一项所述的膜状粘接剂，其中，粘合剂树脂(A)是含有5～30质量%的源于含环氧基的单体的结构单元的丙烯酸系聚合物。
5.根据权利要求1～4中任一项所述的膜状粘接剂，其中，环氧树脂(B)的含量相对于粘合剂树脂(A)100质量份为50～1000质量份。
6.半导体接合用粘接片，其中，将权利要求1～5中任一项所述的膜状粘接剂作为粘接剂层以可剥离的方式形成于支撑片上。
7.根据权利要求6所述的半导体接合用粘接片，其中，支撑片含有下述膜作为结构层：
包含聚氨酯聚合物和乙烯基系聚合物的复合膜、或
聚氨酯丙烯酸酯固化物膜。
8.半导体装置的制造方法，其是使用了权利要求1～5中任一项所述的膜状粘接剂、或者权利要求6或7所述的半导体接合用粘接片的半导体装置的制造方法，其中，包含：
在晶片上贴附膜状粘接剂或半导体接合用粘接片的粘接剂层的步骤、
将晶片单片化而得到芯片的步骤、和
经由膜状粘接剂或粘接剂层将芯片固定的步骤。
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