CN105580133A - 半导体元件三维安装用填充材料 - Google Patents
半导体元件三维安装用填充材料 Download PDFInfo
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- CN105580133A CN105580133A CN201480052924.4A CN201480052924A CN105580133A CN 105580133 A CN105580133 A CN 105580133A CN 201480052924 A CN201480052924 A CN 201480052924A CN 105580133 A CN105580133 A CN 105580133A
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Classifications
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- C08G59/226—Mixtures of di-epoxy compounds
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Abstract
本发明提供一种在COW工艺中对制造厚度较薄且低外形化的三维半导体集成元件装置方面有用的填充材料、以及形成所述填充材料的固化性组合物。本发明的半导体元件三维安装用填充材料是在将多个半导体元件叠层并集成来制造三维半导体集成元件装置时填补横向邻接的半导体元件之间的空隙的填充材料,其特征在于,该填充材料是在填补了半导体元件之间的空隙的状态下从半导体元件的表面侧进行抛光和/或磨削而变得平坦的构件。
Description
技术领域
本发明涉及在通过将多个半导体元件叠层、贴合并集成来制造三维半导体集成元件装置的方法中使用的半导体元件三维安装用填充材料、以及作为该半导体元件三维安装用填充材料的原料而言有用的固化性组合物。本申请主张2013年9月27日在日本申请的日本特愿2013-201591号的优先权,且在此引用其内容。
背景技术
近年来,为了应对半导体装置的高度集成化,半导体元件的集成方法从平面集成转向立体集成,因而具有三维叠层结构的半导体集成电路装置备受关注。作为制造三维半导体集成电路装置的方法,已知有在第1半导体晶片上叠层切割了第2半导体晶片而得到的芯片的方法(COW工艺;ChipOnWaferProcess)(专利文献1等)。在芯片上制作贯通孔(TSV)的COW工艺的情况下,通过使用光致抗蚀剂进行蚀刻处理来制作。
现有技术文献
专利文献
专利文献1:日本特开2006-19429号公报
发明的内容
发明所要解决的课题
然而,将由第2半导体晶片切出的芯片叠层在第1半导体晶片上时,在横向邻接的芯片之间会产生空隙。如果存在该空隙,则难以在由第1半导体晶片和芯片构成的叠层体的整个面上以均匀的厚度涂布光致抗蚀剂,因此需要填补横向邻接的芯片之间产生的空隙。但是,仅通过涂布树脂等填补空隙会残留凹凸。另外,如果在芯片面上残留树脂,则会导致厚度的增大。因此,寻求一种填充材料,其在填补在横向邻接的芯片间的空隙时,可以通过涂布来容易地填补槽部,不会伴随固化而产生破裂、气泡,另外,即使实施平坦化或者薄化处理,也具有不会发生破裂、剥离的优异的加工性。
因此,本发明的目的在于,提供一种在COW工艺中对制造厚度薄且低外形化(lowprofile)的三维半导体集成元件装置方面有用的填充材料、以及形成所述填充材料的固化性组合物。
用于解决课题的技术方案
本发明人等为了实现上述目的而进行了深入研究,结果发现在通过COW工艺制造三维半导体集成元件装置(三维半导体集成电路装置等)的方法中,用填充材料填补在横向邻接的芯片之间的空隙,并在该状态下从芯片表面侧对所述填充材料进行抛光或磨削,则能够容易地使芯片表面侧变得平坦。本发明是基于上述见解而完成的。
即,本发明提供一种半导体元件三维安装用填充材料,其是在将多个半导体元件叠层并集成来制造三维半导体集成元件装置时,填补横向邻接的半导体元件之间的空隙的填充材料,其特征在于,该填充材料是在填补半导体元件之间的空隙的状态下,从半导体元件的表面侧被抛光和/或磨削而变得平坦的构件。
另外,本发明提供所述半导体元件三维安装用填充材料,其中,所述填充材料为固化性组合物的固化物,所述固化性组合物至少包含具有双酚骨架的环氧化合物和阳离子聚合引发剂。
另外,本发明提供一种半导体元件三维安装用固化性组合物,其是用于形成所述半导体元件三维安装用填充材料的固化性组合物,其中,所述半导体元件三维安装用固化性组合物至少包含具有双酚骨架的环氧化合物和阳离子聚合引发剂,且在25℃下为液态。
本发明提供所述半导体元件三维安装用固化性组合物,其还含有脂环族环氧化合物。
本发明提供所述半导体元件三维安装用固化性组合物,其还含有平均粒径为0.05~1μm的无机和/或有机填料。
本发明提供所述半导体元件三维安装用固化性组合物,其还含有硅烷偶联剂。
即,本发明涉及以下方案。
[1]一种半导体元件三维安装用填充材料,其是在将多个半导体元件叠层并集成来制造三维半导体集成元件装置时,填补横向邻接的半导体元件之间的空隙的填充材料,其特征在于,该填充材料是在填补半导体元件之间空隙的状态下,从半导体元件的表面侧进行抛光和/或磨削而变得平坦的构件。
[2]根据[1]所述的半导体元件三维安装用填充材料,其中,所述填充材料是固化性组合物的固化物,所述固化性组合物至少包含具有双酚骨架的环氧化合物和阳离子聚合引发剂。
[3]根据[2]所述的半导体元件三维安装用填充材料,其中,所述固化性组合物的固化物的玻璃化转变温度为30℃以上。
[4]根据[2]或[3]所述的半导体元件三维安装用填充材料,其中,所述固化性组合物的固化物的热膨胀系数(ppm/K)为150以下。
[5]一种半导体元件三维安装用固化性组合物,其是用于形成[1]~[4]中任一项所述的半导体元件三维安装用填充材料的固化性组合物,其中,所述半导体元件三维安装用固化性组合物至少含有固化性化合物和阳离子聚合引发剂,且在25℃下为液态,所述固化性组合物包含具有双酚骨架的环氧化合物。
[6]根据[5]所述的半导体元件三维安装用固化性组合物,其中,具有双酚骨架的环氧化合物为选自式(1)~(3)所示的化合物中的至少一种。
[7]根据[5]或[6]所述的半导体元件三维安装用固化性组合物,其中,具有双酚骨架的环氧化合物的环氧当量为155~800g/eq。
[8]根据[5]~[7]中任一项所述的半导体元件三维安装用固化性组合物,其还含有脂环族环氧化合物。
[9]根据[8]所述的半导体元件三维安装用固化性组合物,其中,脂环族环氧化合物为式(4)所示的化合物。
[10]根据[8]所述的半导体元件三维安装用固化性组合物,其中,脂环族环氧化合物为选自式(4-1)~(4-6)所示的化合物中的至少一种。
[11]根据[5]~[10]中任一项所述的半导体元件三维安装用固化性组合物,其中,在固化性组合物总量(100重量%)中,含有30~99.99重量%的固化性化合物。
[12]根据[5]~[11]中任一项所述的半导体元件三维安装用固化性组合物,其中,具有双酚骨架的环氧化合物在固化性组合物所含的全部固化性化合物中所占的比例为30重量%以上。
[13]根据[5]~[12]中任一项所述的半导体元件三维安装用固化性组合物,其中,具有双酚骨架环氧化合物和脂环族环氧化合物的总量在固化性组合物中所含的全部固化性化合物中所占的比例为50重量%以上。
[14]根据[8]~[13]中任一项所述的半导体元件三维安装用固化性组合物,其中,固化性组合物中含有的具有双酚骨架的环氧化合物与脂环族环氧化合物的含量之比(前者︰后者(重量份))为55︰45~99︰1。
[15]根据[5]~[14]中任一项所述的半导体元件三维安装用固化性组合物,其中,相对于固化性组合物中所含的固化性化合物(优选为阳离子固化性化合物,特别优选为环氧化合物)100重量份,含有0.01~15重量份的阳离子聚合引发剂。
[16]根据[5]~[15]中任一项所述的半导体元件三维安装用固化性组合物,其中,所述固化性组合物还含有平均粒径为0.05~1μm的无机和/或有机填料。
[17]根据[16]所述的半导体元件三维安装用固化性组合物,其中,相对于固化性化合物(优选为阳离子固化性化合物,特别优选为环氧化合物)100重量份,含有0.1~70重量份的无机和/或有机填料。
[18]根据[5]~[17]中任一项所述的半导体元件三维安装用固化性组合物,其中,所述固化性组合物还含有硅烷偶联剂。
[19]根据[18]所述的半导体元件三维安装用固化性组合物,其中,相对于固化性化合物(优选为阳离子固化性化合物,特别优选为环氧化合物)100重量份,含有0.1~10重量份的硅烷偶联剂。
[20]根据[18]或[19]所述的半导体元件三维安装用固化性组合物,其中,环氧化合物、阳离子聚合引发剂、无机填料、有机填料、以及硅烷偶联剂的含量之和为固化性组合物总量的80重量%以上。
[21]根据[5]~[20]中任一项所述的半导体元件三维安装用固化性组合物,其中,固化性组合物的粘度(25℃下)为10~100000mPa·s。
[22]一种三维半导体集成元件装置的制造方法,该方法包括:利用[5]~[21]中任一项所述的半导体元件三维安装用固化性组合物的固化物对半导体元件之间进行填充,在填充了半导体元件之间的状态下从半导体元件的表面侧进行抛光和/或磨削而使所述固化物变得平坦的工序。
[23]一种三维半导体集成元件装置,其通过[22]所述的三维半导体集成元件装置的制造方法而得到。
发明的效果
根据本发明,用填充材料对横向邻接的变薄的半导体元件之间的空隙进行填补,并在该状态下从半导体元件的表面侧对填充材料进行抛光,由此,能够以良好地成品率制造芯片表面侧变得平坦、且厚度较薄的低外形化的三维半导体集成元件装置。
附图说明
图1是示出使用了本发明的半导体元件三维安装用填充材料的三维半导体集成元件装置的制造方法的一个例子的示意工序图。
图2是示出使用了本发明的半导体元件三维安装用填充材料的三维半导体集成元件装置的制造方法的一个例子的示意工序图(续图1)。
符号说明
1包含电路形成区域的硅晶片
2半导体元件三维安装用填充材料
3贯通孔
4贯通电极
20、20’半导体元件
30第1基底晶片
40具有两层配线层的半导体晶片
50具有三层配线层的半导体晶片
具体实施方式
[半导体元件三维安装用填充材料]
本发明的半导体元件三维安装用填充材料(以下,有时简称为“填充材料”)是在将多个半导体元件叠层并集成来制造三维半导体集成元件装置时,对横向邻接的半导体元件之间的空隙进行填补的填充材料(空隙填补材料)。该填充材料可以在填补半导体元件之间的空隙的状态下从半导体元件的表面侧进行抛光或磨削而变得平坦。
图1和图2是示出使用了本发明的半导体元件三维安装用填充材料的三维半导体集成元件装置(三维半导体集成电路装置)的制造方法的一个例子的示意工序图。在该工艺中,如下所述进行操作来制造三维半导体集成元件装置。
(a)准备第1基底晶片30,所述第1基底晶片30在包含电路形成区域的硅晶片1上叠层有半导体元件20。
(b)使邻接的半导体元件20之间的空隙处于用本发明的半导体元件三维安装用填充材料2填补的状态(使后面叙述的半导体元件三维安装用固化性组合物流入在上述空隙中并使其固化)。
(c)抛光和/或磨削上述填充材料2的表面,使其变得平坦/变薄。
(d)~(e)在半导体元件20内部或半导体元件三维安装用填充材料2中制作贯通孔3,在此形成贯通电极4而制作半导体晶片40。
(f)~(j)然后,在如上所述得到的具有2层配线层的半导体晶片40表面上叠层半导体元件20’,重复进行上述工序,由此可以得到具有3层配线层的半导体晶片50。
通过将这样的操作重复期望的次数并在期望的位置进行切割,能够得到三维半导体集成元件装置(三维半导体集成电路装置)。
优选通过在上述工序(c)中进行抛光和/或磨削使填充材料2的厚度为例如10~30μm。
如上所述,由于在用填充材料填补了横向邻接的元件之间的空隙的状态下从元件表面侧对填充材料进行抛光或磨削,因此元件表面侧变得平坦。因此,可以有效率地制造元件本身变薄且低外形化的三维半导体集成元件装置(三维半导体集成电路装置)。而且,这时不会发生破裂、产生气泡。
半导体元件20是使用了半导体的元件,例如可以是MEMS或图像传感器。另外,叠层的半导体元件20’可以与半导体元件20大小相同,也可以尺寸不同(长、宽、高)。
包含电路形成区域的硅晶片1可以是MEMS,也可以是图像传感器。
作为上述填充材料,优选至少包含具有双酚骨架的环氧化合物和阳离子聚合引发剂的固化性组合物的固化物。
[半导体元件三维安装用固化性组合物]
本发明的半导体元件三维安装用固化性组合物(以下,有时称为“本发明的固化性组合物”)至少包含具有双酚骨架的环氧化合物和阳离子聚合引发剂,且在25℃下为液态。本发明的固化性组合物可以用于形成上述半导体元件三维安装用填充材料。即,可以将本发明的固化性组合物注入横向邻接的元件之间的空隙并使其固化,由此形成上述填充材料。
(固化性化合物)
本发明的固化性组合物至少包含具有双酚骨架的环氧化合物作为固化性化合物(特别是阳离子固化性化合物)。如果使用具有双酚骨架的环氧化合物作为固化性化合物,则在固化时不会产生裂纹,而且,即使在固化后进行抛光也不会产生裂纹或缺损,也不会引起抛光盘的堵塞。需要说明的是,在将现有的元件叠层用粘接剂转用作上述空隙填补剂的情况下,在固化时、固化后进行抛光时会产生裂纹、缺损,引起抛光盘的堵塞。另外,在仅使用脂环族环氧化合物作为固化性化合物的情况下,固化物变得过硬、发生固化收缩,从而容易在固化物中产生裂纹。
作为上述具有双酚骨架的环氧化合物,可以举出例如:具有双酚A骨架的环氧化合物(=双酚A型环氧树脂)、具有双酚F骨架的环氧化合物(=双酚F型环氧树脂)、具有双酚AD骨架的环氧化合物(=双酚AD型环氧树脂)、具有双酚S骨架的环氧化合物(=双酚S型环氧树脂)等。这些环氧化合物可以在分子内具有除了源自双酚和环氧氯丙烷的结构单元以外的结构单元。
作为具有双酚骨架的环氧化合物的代表例,可以列举下式(1)、(2)、(3)所示的化合物。
[化学式1]
上述式中,r表示0~8的数字。作为r,其中,优选0.01~3的范围,特别优选1~2的范围。
上述具有双酚骨架的环氧化合物的环氧当量例如为155~800g/eq,优选为155~500g/eq,特别优选为160~200g/eq,最优选为160~190g/eq。上述具有双酚骨架的环氧化合物优选为在室温(25℃)下呈现液态的化合物,但是即使为固体,只要通过与溶解具有双酚骨架的环氧化合物的其它液态(25℃下)的化合物(例如,其它的环氧化合物等)组合使用而使固化性化合物整体为液态(25℃)即可。
上述本发明的固化性组合物还可以含有具有双酚骨架的环氧化合物以外的环氧化合物。作为这样的环氧化合物,可以举出:在分子内具有由构成脂环且邻接的2个碳原子与氧原子构成的环氧基(=脂环环氧基)的环氧化合物(=脂环族环氧化合物);环氧基直接以单键键合于脂环的环氧化合物;具有脂环和缩水甘油醚基的缩水甘油醚型环氧化合物;其它的环氧化合物。
作为上述脂环,可以列举:环戊烷环、环己烷环、环辛烷环、环十二烷环等单环脂环(3~15元的环烷烃环,优选为5~6元的环烷烃环等);萘烷环(十氢萘环)、全氢茚环(双环[4.3.0]壬烷环)、全氢蒽环、全氢芴环、全氢菲环、全氢苊环、全氢非那烯环、降冰片烷环(双环[2.2.1]庚烷环)、异冰片烷环、金刚烷环、双环[3.3.0]辛烷环、三环[5.2.1.02,6]癸烷环、三环[6.2.1.02,7]十一烷环等多环(2~4环左右)的脂环(桥接碳环)等。另外,作为脂环环氧基,可以列举例如:环氧环戊基、3,4-环氧环己基、3,4-环氧三环[5.2.1.02,6]癸烷8-(或9)基(环氧化二环戊二烯基)等。在上述脂环中也可以键合有烷基(例如,甲基等碳原子数1~6的烷基)等取代基。
作为上述脂环族环氧化合物,可以举出下式(4)所示的化合物(2个脂环环氧基以单键或经由连结基团键合的化合物)。
[化学式2]
上述式中,Y1表示单键或连结基团。作为连结基团,可以列举例如:2价的烃基、羰基(-CO-)、醚键(-O-)、酯键(-COO-)、酰胺键(-CONH-)、碳酸酯键(-OCOO-)、以及多个这些基团键合而成的基团等。作为2价的烃基,可以例示出:亚甲基、乙叉基、异亚丙基、亚乙基、亚丙基、三亚甲基、四亚甲基等直链状或支链状的亚烷基(特别是C1-6亚烷基);1,2-亚环戊基、1,3-亚环戊基、环戊叉基、1,2-亚环己基、1,3-亚环己基、1,4-亚环己基、环己叉基等2价的脂环族烃基(特别是2价的亚环烷基);以及多个这些基团键合而成的基团等。
作为式(4)所示的化合物所包含的代表性化合物,可以列举:(3,4,3’,4’-二环氧基)联环己烷、双(3,4-环氧环己基甲基)醚、1,2-环氧基-1,2-双(3,4-环氧环己-1-基)乙烷、2,2-双(3,4-环氧环己烷-1-基)丙烷、1,2-双(3,4-环氧环己烷-1-基)乙烷等、下式(4-1)~(4-6)所示的化合物等。需要说明的是,下式中t为1~30的整数。
[化学式3]
除此以外,作为脂环族环氧化合物还可以列举:分子内具有脂环和2个以上的环氧基、且2个以上的环氧基中仅有1个为脂环环氧基的化合物。作为其代表化合物,可以举出下式(5)所示的柠檬烯二环氧化物等。
[化学式4]
另外,作为脂环族环氧化合物,也可以使用如下式(6)~(9)所示的化合物那样的、具有3个以上的脂环环氧基的脂环族环氧化合物、仅具有1个脂环环氧基且没有其它环氧基的脂环族环氧化合物。需要说明的是,在下式中,a、b、c、d、e、f为0~30的整数。
[化学式5]
作为上述环氧基直接以单键键合于脂环的环氧化合物,可以举例如下式(10)所示的化合物。
[化学式6]
在上述式中,R表示从q元醇[R-(OH)q]中除去了q个OH的基团,p表示1~30的整数,q表示1~10的整数。在q个括号内的基团中,p可以分别相同,也可以不同。作为q元醇[R-(OH)q],可以列举:甲醇、乙醇、1-丙醇、异丙醇、1-丁醇等一元醇;乙二醇、1,2-丙二醇、1,3-丙二醇、1,4-丁二醇、新戊二醇、1,6-己二醇、二乙二醇、三乙二醇、四乙二醇、二丙二醇、聚丙二醇等二元醇;甘油、双甘油、赤藓醇、三羟甲基乙烷、三羟甲基丙烷、季戊四醇、二季戊四醇、山梨糖醇等三元以上的醇。上述醇也可以是聚醚多元醇、聚酯多元醇、聚碳酸酯多元醇、聚烯烃多元醇等。作为上述醇,优选碳原子数1~10的脂肪族醇(特别是三羟甲基丙烷等脂肪族多元醇)。
作为上述具有脂环和缩水甘油醚基的缩水甘油醚型环氧化合物,可以举出脂环族醇(特别是脂环族多元醇)的缩水甘油醚。该化合物也可以是上述具有双酚骨架的环氧化合物[例如上式(1)、(2)、(3)所示的化合物]的芳香环进行了核加氢的化合物。
作为上述其它环氧化合物,可以列举例如:上述q元醇[R-(OH)q]的缩水甘油醚;乙酸、丙酸、丁酸、硬脂酸、己二酸、癸二酸、马来酸、衣康酸等一元或多元羧酸的缩水甘油酯;环氧化亚麻籽油、环氧化大豆油、环氧化蓖麻油等具有双键的油脂的环氧化物;环氧化聚丁二烯等聚烯烃(包含聚链二烯)的环氧化物等。
在除了上述具有双酚骨架的环氧化合物以外的环氧化合物中,优选脂环族环氧化合物。通过组合使用具有双酚骨架的环氧化合物和脂环族环氧化合物,能够提高固化物(填充材料2)的耐热性,可以抑制固化物在高温环境下的硬度发生变化。
本发明的固化性组合物除了环氧化合物以外还可以含有其它固化性化合物,环氧化合物在本发明的固化性组合物所含的全部固化性化合物(特别是全部阳离子固化性化合物)中所占的比例为例如50重量%以上,优选为70重量%以上,特别优选为85重量%以上,最优选为90重量%以上,环氧化合物的比例的上限为100重量%。
上述本发明的固化性组合物中的固化性化合物含量(在含有两种以上的情况下为其总量),例如为30~99.99重量%,优选为50~99.9重量%,进一步优选为60~99.5重量%。
上述本发明的固化性组合物中的环氧化合物含量(在含有两种以上的情况下为其总量),例如为30~99.99重量%,优选为50~99.9重量%,进一步优选为60~99.5重量%。
具有双酚骨架的环氧化合物在本发明的固化性组合物的全部固化性化合物中所占的比例为例如30重量%以上,优选为40重量%以上,进一步优选为50重量%以上,特别优选为70重量%以上。
具有双酚骨架的环氧化合物在本发明的固化性组合物的全部环氧化合物中所占的比例为例如30重量%以上,优选为40重量%以上,进一步优选为50重量%以上,特别优选为70重量%以上。
具有双酚骨架的环氧化合物和脂环族环氧化合物的总量在本发明的固化性组合物的全部固化性化合物中所占的比例为例如50重量%以上,优选为70重量%以上,进一步优选为90重量%以上。
具有双酚骨架的环氧化合物和脂环族环氧化合物的总量在本发明的固化性组合物的全部环氧化合物中所占的比例为例如50重量%以上,优选为70重量%以上,进一步优选为90重量%以上。
本发明的固化性组合物中的具有双酚骨架的环氧化合物与脂环族环氧化合物的含量之比(前者︰后者(重量份))为例如55︰45~99︰1,优选为60︰40~95︰5,更优选为70︰30~90︰10。
(阳离子聚合引发剂)
本发明的固化性组合物含有阳离子聚合引发剂(固化催化剂)。阳离子聚合引发剂是通过光照射或加热而释放出引发阳离子聚合的物质的化合物。
在阳离子聚合引发剂中,作为通过光照射而产生阳离子种的阳离子聚合引发剂,可以列举例如:三芳基锍盐(例如六氟锑酸盐、五氟羟基锑酸盐、六氟磷酸盐、六氟砷酸盐)等,可以优选使用商品名“CPI-100P”、“CPI-101A”、“LW-S1”(以上为San-Apro公司制造)、商品名“CD-1010”、“CD-1011”、“CD-1012”(以上为美国Sartomer公司制造)、商品名“IRGACURE264”(BASF公司制造)、商品名“CIT-1682”(日本曹达株式会社制造)等市售品。
阳离子聚合引发剂中,作为通过加热而产生阳离子种的阳离子聚合引发剂,可以列举例如:芳基重氮鎓盐、芳基碘鎓盐、芳基锍盐、丙二烯-离子络合物等,可以优选使用商品名“PP-33”、“CP-66”、“CP-77”(以上为ADEKA公司制造)、商品名“FC-509”(3M制造)、商品名“UVE1014”(G.E.公司制造)、商品名“San-aidSI-60L”、“San-aidSI-80L”、“San-aidSI-100L”,“San-aidSI-110L”(以上为三新化学工业株式会社制造),商品名“CG-24-61”(BASF公司制造)等市售品。而且,也可以是铝、钛等金属和乙酰乙酸或二酮类的螯合物与三苯基硅烷醇等硅烷醇的化合物、或者铝、钛等金属和乙酰乙酸或二酮类的螯合化合物与双酚S等酚类的化合物。
本发明的固化性组合物含有阳离子聚合引发剂,因此,可以通过热或光进行阳离子固化而形成上述填充材料。
阳离子聚合引发剂的配合量没有特别限定,相对于上述固化性组合物中的全部固化性化合物(优选为全部阳离子固化性化合物,特别优选为全部环氧化合物)100重量份,优选为0.01~15重量份,更优选为0.05~10重量份,进一步优选为0.1~8重量份,特别优选为0.1~5重量份,最优选为0.1~3重量份。通过在上述范围内进行配合,可以得到耐热性、透明性、耐候性等良好的固化物(填充材料)。
(添加剂)
本发明的固化性组合物可以含有无机和/或有机填料。通过含有无机和/或有机填料,可以抑制固化物(填充材料2)的热膨胀,提高耐热性。
作为无机填料,可以列举例如:二氧化硅、氧化铝、氧化镁、氧化钛、氧化锑、滑石、粘土、蒙脱石、水滑石、合成云母、碳酸钙、氢氧化铝、氢氧化镁等。这些填料可以单独使用一种或组合使用两种以上。其中,优选二氧化硅(特别是球状二氧化硅)、氧化铝。
无机填料的平均粒径为例如0.05~1μm,优选为0.1~1μm。
相对于本发明的固化性组合物中的全部固化性化合物(优选为全部阳离子固化性化合物,特别优选为全部环氧化合物)100重量份,无机填料的配合量为例如70重量份以下(例如0.1~70重量份),优选为50重量份以下(例如1~50重量份),进一步优选为40重量份以下(例如5~40重量份)。
作为有机填料,可以列举例如:聚酰亚胺、聚醚醚酮、芳族聚酰胺、纤维素等。这些填料可以单独使用一种或组合使用两种以上。其中,优选聚酰亚胺(特别是球状聚酰亚胺)、聚醚醚酮(特别是球状聚醚醚酮)。
相对于本发明的固化性组合物中的全部固化性化合物(优选为全部阳离子固化性化合物,特别优选为全部环氧化合物)100重量份,有机填料的配合量为例如70重量份以下(例如0.1~70重量份),优选为50重量份以下(例如1~50重量份),进一步优选为40重量份以下(例如5~40重量份)。
本发明的固化性组合物还可以含有硅烷偶联剂。通过含有硅烷偶联剂,可以提高固化物(填充材料2)对于硅晶片的密合性。
作为硅烷偶联剂,可以列举例如:(甲基)丙烯酸3-三甲氧基甲硅烷基丙酯、(甲基)丙烯酸3-三乙氧基甲硅烷基丙酯、(甲基)丙烯酸3-二甲氧基甲基甲硅烷基丙酯、(甲基)丙烯酸3-二乙氧基甲基甲硅烷基丙酯等。在使用官能团为(甲基)丙烯酰氧基的硅烷偶联剂的情况下,可以少量添加自由基聚合引发剂。需要说明的是,虽然也可以使用官能团为环氧基的硅烷偶联剂[2-(3,4-环氧环己基)乙基三甲氧基硅烷、3-环氧丙氧基丙基甲基二甲氧基硅烷、3-环氧丙氧基丙基三甲氧基硅烷、3-环氧丙氧基丙基甲基二乙氧基硅烷、3-环氧丙氧基丙基三乙氧基硅烷等],但是这样的偶联剂属于上述其它环氧化合物。
相对于本发明的固化性组合物中的全部固化性化合物(优选为全部阳离子固化性化合物,特别优选为全部环氧化合物)100重量份,硅烷偶联剂的配合量为例如10重量份以下(例如0.1~10重量份),优选为5重量份以下(例如0.2~5重量份),进一步优选为3重量份以下(例如0.3~3重量份)。
在本发明的固化性组合物中,可以在不损害本发明的效果的范围内进一步根据需要添加一种或两种以上的各种添加剂(例如,聚硅氧烷类或氟类的消泡剂、流平剂、表面活性剂、有机类的橡胶粒子、阻燃剂、着色剂、增塑剂、防静电剂、抗氧化剂、紫外线吸收剂、光稳定剂、离子吸附体、颜料、染料、荧光体等)。相对于固化性组合物整体,上述各种添加剂的配合量为例如5重量%以下。本发明的固化性组合物可以含有溶剂,但是在溶剂的量过多时,固化物中有时会产生气泡,因此,优选相对于固化性组合物整体,为例如20重量%以下,更优选为10重量%以下,特别优选为5重量%以下,最优选为1重量%以下。
在本发明的固化性组合物中,相对于固化性组合物整体,环氧化合物、阳离子聚合引发剂、无机填料、有机填料、以及硅烷偶联剂的总含量为例如80重量%以上,优选为90重量%以上,特别优选为95重量%以上,最优选为99重量%以上。
本发明的固化性组合物在25℃下呈现液态,其粘度(25℃)为例如10~100000mPa·s,优选为100~10000mPa·s,特别优选为500~10000mPa·s,最优选为500~3000mPa·s。本发明的固化性组合物优选为常温下具有流动性的糊状。如果本发明的固化性组合物的粘度过大,则不容易除去气泡,并且操作性、处理性等容易变差。需要说明的是,粘度可以使用B型粘度计、D型粘度计等来测定。
本发明的固化性组合物可以为单液型、双液型中的任一种。
本发明的固化性组合物可以通过对具有双酚骨架的环氧化合物和阳离子聚合引发剂、以及根据需要的脂环族环氧化合物、无机或有机填料、硅烷偶联剂、其它的添加剂进行搅拌混合来制备。搅拌混合可以使用通用的混合机、混练机等。
如上所述制备的半导体元件三维安装用固化性组合物可以在制造三维半导体集成元件装置时注入横向邻接的半导体元件之间的空隙中,在给定的条件下进行固化(光固化或加热固化),作为上述填充材料2发挥作用。
在使本发明的固化性组合物发生光固化(光阳离子固化)的情况下,作为照射的活性能量线(光),可以列举例如:紫外线、电子束等,其中,可以优选使用紫外线。上述紫外线的波长可以根据阳离子聚合引发剂的种类等而适当选择。另外,活性能量线的照射条件可以根据所配合的环氧化合物的种类、膜厚、阳离子聚合引发剂的种类、量等而适当选择,例如,在使用紫外线的情况下,其照射量(剂量)优选为10~30000mJ/cm2,特别优选为50~25000mJ/cm2。作为上述紫外线的照射源,可以列举例如:高压水银灯、超高压水银灯、氙灯、碳弧灯、金属卤化物灯、太阳光、LED灯等。
如上所述,在对本发明的固化性组合物照射活性能量线而使其光固化后,可以根据需要进一步进行加热(后固化)。通过后固化,能够得到降低固化物中的未反应物、提高固化物的固化度,缓和应变等的效果。另外,有时也可以获得提高固化物的硬度、密合性的效果。上述加热通常可以在100~200℃的温度、1~300分钟的条件下进行。
另外,使本发明的固化性组合物加热固化(热阳离子固化)时的固化温度为例如45~200℃左右,固化时间为例如1~60分钟左右。加热固化还可以通过多步来进行。
需要说明的是,在加热固化的情况下,将固化性组合物注入上述邻接的半导体元件之间的空隙时,由于热使固化性组合物的流动性增加而在中央聚集(由于与硅晶片的润湿性较小),面内膜厚分布有时并不恒定,因此更优选光固化。
对本发明的固化性组合物进行固化而得到的固化物的坚韧性优异,即使进行抛光处理也不会产生裂纹、缺损。另外,对本发明的固化性组合物进行固化而得到的固化物的耐热性优异,玻璃化转变温度(Tg:℃)为例如30℃以上,优选为50℃以上,特别优选为80℃以上。而且,热膨胀系数(ppm/K)为例如150以下,优选为100以下。
实施例
以下,基于实施例对本发明进行更详细的说明,但是本发明并不限定于这些实施例。
实施例1
将双酚F型环氧树脂100重量份和阳离子聚合引发剂“CPI-100P”2重量份在自转/公转搅拌机(Thinky公司制造,商品名“脱泡练太郎”)中搅拌混合,得到了填充材料用的固化性组合物。
实施例2~24、比较例1~4
如表1中记载那样更该配方,除此以外,与实施例1同样地得到了填充材料用的固化性组合物。
评价试验
作为涂布基板,准备了在8英寸硅晶片上对模拟芯片的凸凹形状进行切削加工而制作成的基板(模拟COW基板:晶片厚度725μm,芯片部9mm×9mm×0.2mm厚,槽部2mm宽度×0.1mm厚)。即,在8英寸硅晶片的表面上,在纵向和横向分别以10mm间隔制作了宽2mm×深0.2mm的槽。
使用刮桨板(NewlongSeimitsuKogyo公司制造的J刮桨板)在该模拟COW基板的表面上涂布上述实施例和比较例中得到的填充材料用固化性组合物,从而形成了涂膜。
肉眼观察得到的涂膜,并根据下述基准对填充性进行评价。
<评价基准>
芯片部、槽部均被填充,槽部完全未残留气泡的情况:◎
芯片部、槽部虽然均被填充,但是在槽部残留有气泡的情况:○
仅槽部被填充的情况:△
用UV照射机(牛尾电机株式会社制造,商品名“UVC-02516S1AA02”)对上述涂膜以3600mJ/cm2照射(光固化)UV光(UV-A),然后,使用加热板在120℃下加热10分钟(后固化)而形成填充材料。
通过肉眼观察和光学显微镜对得到的填充材料有无裂纹进行确认,根据下述基准进行评价。
<评价基准>
没有裂纹的情况:○
有裂纹的情况:×
对于没有裂纹的样品而言,使用抛光机(MusashinoDenshi公司制造,商品名“MA-200D”)和抛光盘(三井研削砥石株式会社制造,商品名“CBNDIA#400”),在转数100rpm、抛光时间10分钟、砝码500g的条件下实施了抛光试验。需要说明的是,由于在比较例1~4中得到的填充材料中确认到了裂纹,因此未进行抛光试验。
在抛光之后,通过肉眼观察和光学显微镜确认填充材料、硅晶片中有无裂纹、缺损,以及有无抛光盘的堵塞,根据下述基准对抛光性进行评价。
<评价基准>
填充材料、硅晶片中没有裂纹、缺损、没有抛光盘堵塞的情况:○
填充材料、硅晶片中有裂纹、缺损和/或有抛光盘堵塞的情况:×
另外,对于用固化性组合物对实施例和比较例中得到的填充材料进行固化(固化条件与上述试验相同)而得到的填充材料(大小:500mm×10mm)的耐热性而言,使用SeikoInstruments公司制造的DSC(差示扫描量热仪)测定了玻璃化转变温度(Tg)。并且,使用热机械分析装置(商品名“EXSTARTMA/SS7100”、SIINanoTechnology公司制造),用压缩模式测定了热膨胀系数(ppm/K)。
※实施例和比较例中使用的化合物如下所述。
<固化性化合物>
双酚F型环氧树脂:双酚F·环氧氯丙烷的二缩水甘油醚,环氧当量:168g/eq,商品名“RE-303S”,日本化药株式会社制造
双酚A型环氧树脂:双酚A·环氧氯丙烷的二缩水甘油醚,环氧当量:185g/eq,商品名“RE-410S”,日本化药株式会社制造
2021P:3,4-环氧环己基甲基(3,4-环氧基)环己烷羧酸酯,商品名“Celloxide2021P”,株式会社大赛璐制造
PB3600:环氧化聚丁二烯,商品名“EPOLEADPB3600”,株式会社大赛璐制造
<阳离子聚合引发剂>
CPI-100P:二苯基-4-(苯硫基)苯基锍六氟磷酸酯,商品名“CPI-100P”,San-Apro公司制造
CPI-101A:二苯基-4-(苯硫基)苯基锍六氟锑酸盐,商品名“CPI-101A”,San-Apro公司制造
LW-S1:锍化合物,商品名“LW-SI”,San-Apro公司制造
<其它>
二氧化硅:商品名“SC4050-SEJ”,平均粒径1μm,Admatechs公司制造
硅烷偶联剂:丙烯酸3-三甲氧基甲硅烷基丙酯
工业实用性
根据本发明的半导体元件三维安装用填充材料,用填充材料对横向邻接的变薄了的半导体元件之间的空隙进行填补,并在该填补的状态下从半导体元件的表面侧对填充材料进行抛光,由此,能够以良好的成品率制造芯片表面侧变得平坦、且厚度较薄的、低外形化的三维半导体集成元件装置。
Claims (6)
1.一种半导体元件三维安装用填充材料,其是在将多个半导体元件叠层并集成来制造三维半导体集成元件装置时填补横向邻接的半导体元件之间的空隙的填充材料,其中,该填充材料是在填补半导体元件之间的空隙的状态下从半导体元件的表面侧进行抛光和/或磨削而变得平坦的构件。
2.根据权利要求1所述的半导体元件三维安装用填充材料,其中,所述填充材料是固化性组合物的固化物,所述固化性组合物至少包含具有双酚骨架的环氧化合物和阳离子聚合引发剂。
3.一种半导体元件三维安装用固化性组合物,其是用于形成权利要求1或2所述的半导体元件三维安装用填充材料的固化性组合物,其中,所述固化性组合物至少包含具有双酚骨架的环氧化合物和阳离子聚合引发剂,且在25℃下为液态。
4.根据权利要求3所述的半导体元件三维安装用固化性组合物,其还含有脂环族环氧化合物。
5.根据权利要求3或4所述的半导体元件三维安装用固化性组合物,其还含有平均粒径为0.05~1μm的无机和/或有机填料。
6.根据权利要求3~5中任一项所述的半导体元件三维安装用固化性组合物,其还含有硅烷偶联剂。
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