TW201625764A - 接著劑組成物、含其硬化物的半導體裝置及使用其的半導體裝置的製造方法 - Google Patents

接著劑組成物、含其硬化物的半導體裝置及使用其的半導體裝置的製造方法 Download PDF

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TW201625764A
TW201625764A TW104140874A TW104140874A TW201625764A TW 201625764 A TW201625764 A TW 201625764A TW 104140874 A TW104140874 A TW 104140874A TW 104140874 A TW104140874 A TW 104140874A TW 201625764 A TW201625764 A TW 201625764A
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adhesive composition
mass
semiconductor device
film
particle diameter
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TW104140874A
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TWI665279B (zh
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Kazuyuki Matsumura
Koichi Fujimaru
Daisuke Kanamori
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Toray Industries
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    • C09J11/00—Features of adhesives not provided for in group C09J9/00, e.g. additives
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Abstract

本發明的目的在於提供一種能夠識別對準標記、充分確保接合部的焊料的潤濕性、並且在抑制空隙產生的方面優異的接著劑組成物，本發明的接著劑組成物含有：（A）高分子化合物；（B）重量平均分子量為100以上且3,000以下的環氧化合物；（C）助焊劑；及（D）於表面具有含有苯基的烷氧基矽烷的、平均粒徑為30 nm～200 nm的無機粒子，所述接著劑組成物的特徵在於：（C）助焊劑含有酸改質松香。

Description

接著劑組成物、含其硬化物的半導體裝置及使用其的半導體裝置的製造方法
本發明是有關於一種在將半導體晶片電性接合或接著於電路基板上時、或將半導體晶片彼此接合或積層時所使用的接著劑組成物、含其硬化物的半導體裝置及使用其的半導體裝置的製造方法。
近年，伴隨著半導體裝置的小型化與高密度化，倒裝晶片（flip chip）安裝作為將半導體晶片安裝於電路基板的方法而受到注目，並極速普及。於倒裝晶片安裝中，對於半導體晶片的接著，採用如下方法作為一般方法，即，使環氧樹脂系接著劑介於形成在半導體晶片上的凸塊電極（bump electrode）與電路基板的墊電極之間。
於凸塊電極中具有焊料的倒裝晶片安裝中，提出有以去除存在於焊料表面或電極表面的氧化膜為目的而具有助焊劑（flux）功能的接著劑（例如參照專利文獻1及專利文獻2）。
另外，於倒裝晶片安裝中，要求隔著接著劑組成物而識別形成於基板或晶片上的對準標記（alignment mark）。即，接著劑組成物必須具有透明性。然而，在欲使用如所述般的接著劑組成物製作半導體裝置的情況下，透明性不足而不能識別對準標記，或因助焊劑性能不充分而使安裝後的接合部的焊料的潤濕性不良，有時在安裝後於半導體裝置內殘存空隙（void）。 現有技術文獻 專利文獻
專利文獻1：日本專利特開2013-173834號公報 專利文獻2：國際公開第2014/103637號
[發明所欲解決之課題]
鑒於所述狀況，本發明的目的在於提供一種能夠識別對準標記、充分確保接合部的焊料的潤濕性、並且在抑制空隙產生的方面優異的接著劑組成物。 [解決課題之手段]
即，本發明是一種接著劑組成物，其含有：（A）高分子化合物；（B）重量平均分子量為100以上且3,000以下的環氧化合物；（C）助焊劑；及（D）於表面具有含有苯基的烷氧基矽烷的、平均粒徑為30 nm～200 nm的無機粒子，且所述接著劑組成物的特徵在於：（C）助焊劑含有酸改質松香。 [發明的效果]
根據本發明，可獲得一種能夠識別對準標記、充分確保接合部的焊料的潤濕性、並且在抑制空隙產生的方面優異的接著劑組成物。
本發明的接著劑組成物含有：（A）高分子化合物；（B）重量平均分子量為100以上且3,000以下的環氧化合物；（C）助焊劑；及（D）於表面具有含有苯基的烷氧基矽烷的、平均粒徑為30 nm～200 nm的無機粒子，所述接著劑組成物的特徵在於：（C）助焊劑含有酸改質松香。
本發明的接著劑組成物藉由含有（A）高分子化合物，於製為膜狀時的製膜性優異。所謂高分子化合物，是指重量平均分子量為5,000以上且500,000以下的化合物。
作為（A）高分子化合物，可列舉：丙烯酸樹脂、苯氧基樹脂、聚酯樹脂、聚胺基甲酸酯樹脂、聚醯亞胺樹脂、矽氧烷改質聚醯亞胺樹脂、聚苯并噁唑樹脂、聚醯胺樹脂、聚碳酸酯樹脂、聚丁二烯等，但並不限定於該些。亦可將該些的兩種以上組合。該些中，就（D）於表面具有含有苯基的烷氧基矽烷的、平均粒徑為30 nm～200 nm的無機粒子的分散性良好，製成膜時膜的透明性高，容易識別對準標記的方面而言，較佳為苯氧基樹脂。另外，就抑制安裝後的空隙的方面而言，較佳為聚醯亞胺樹脂。
（A）高分子化合物的重量平均分子量的下限較佳為10,000以上，更佳為30,000以上。另外，重量平均分子量的上限較佳為100,000以下，更佳為80,000以下。於含有兩種以上（A）高分子化合物的情況下，只要其中至少一種的重量平均分子量為所述範圍即可。若重量平均分子量為10,000以上，則硬化膜的機械強度提高，熱循環試驗（thermal cycling test）中的龜裂產生等得到抑制，從而可獲得可靠性高的半導體裝置。另一方面，若重量平均分子量為100,000以下，則接著劑組成物的流動性變高，安裝後的接合部的焊料的潤濕性提高。此外，本發明中的（A）高分子化合物的重量平均分子量是利用凝膠滲透層析法（gel permeation chromatography，GPC法）來進行測定，並藉由聚苯乙烯換算而算出。
本發明的接著劑組成物含有（B）重量平均分子量為100以上且3,000以下的環氧化合物。環氧化合物藉由一般不伴隨收縮的開環反應而硬化，因而可減少接著劑組成物的硬化時的收縮。另外，藉由重量平均分子量為100以上且3,000以下，環氧化合物的反應性高，結果，硬化速度加快，從而可抑制安裝後的空隙。（B）重量平均分子量為100以上且3,000以下的環氧化合物較佳為具有兩個以上的環氧基、或環氧當量為100～500。藉由將環氧當量設為100以上，可提高硬化後的接著劑組成物的韌性。藉由將環氧當量設為500以下，硬化後的接著劑組成物的交聯密度變高，從而可提高耐熱性。此外，本發明中的（B）重量平均分子量為100以上且3,000以下的環氧化合物的重量平均分子量與（A）高分子化合物的重量平均分子量同樣地，利用凝膠滲透層析法（GPC法）來進行測定，並藉由聚苯乙烯換算而算出。
另外，（B）重量平均分子量為100以上且3,000以下的環氧化合物較佳為含有液狀環氧化合物與固體狀環氧化合物兩者。藉由含有液狀環氧化合物，能夠抑制在將接合劑組成物製成膜狀時膜的龜裂。藉由含有固體狀環氧化合物，能夠抑制安裝後的空隙的產生。
此處所謂液狀環氧化合物，是於25℃、1.013×105 N/m2 下表示出150 Pa･s以下的黏度者，所謂固體環氧化合物，是於25℃下表示出超過150 Pa･s的黏度者。作為液狀環氧化合物，例如可列舉：jER（註冊商標）YL980、jER（註冊商標）YL983U、jER（註冊商標）152、jER（註冊商標）630、jER（註冊商標）YX8000（以上為商品名，三菱化學（股）製造），艾比克隆（EPICLON）（註冊商標）HP-4032（以上為商品名，迪愛生（DIC）（股）製造）等，但並不限定於該些。亦可將該些的兩種以上組合。另外，作為固體環氧化合物，可列舉：jER（註冊商標）1002、jER（註冊商標）1001、jER（註冊商標）YX4000H、jER（註冊商標）4004P、jER（註冊商標）5050、jER（註冊商標）154、jER（註冊商標）157S70、jER（註冊商標）180S70、jER（註冊商標）1032H60（以上為商品名，三菱化學（股）製造），特皮科（TEPIC）（註冊商標）S（以上為商品名，日產化學工業（股）製造），艾普托妥（EPOTOHTO）（註冊商標）YH-434L（商品名，新日鐵化學（股）製造），EPPN502H、NC3000（以上為商品名，日本化藥（股）製造），EPICLON（註冊商標）N695、EPICLON（註冊商標）N865、EPICLON（註冊商標）HP-7200、EPICLON（註冊商標）HP-4700（以上為商品名，DIC（股）製造）等，但並不限定於該些。亦可將該些的兩種以上組合。
另外，就充分表現出接著力、提高安裝後的半導體裝置的連接可靠性的方面而言，相對於（A）高分子化合物100質量份，（B）重量平均分子量為100以上且3,000以下的環氧化合物的含量較佳為50質量份以上，更佳為100質量份以上。另一方面，就提高接合部的焊料的潤濕性的方面而言，較佳為500質量份以下，更佳為300質量份以下。
本發明的接著劑組成物含有（C）助焊劑，所述接著劑組成物的特徵在於：（C）助焊劑含有酸改質松香。（C）助焊劑是將金屬表面的氧化物去除而提高焊料的潤濕性的化合物。酸改質松香是使脂松香（Gum rosin）、木松香（Wood rosin）、浮油松香（Tall rosin）等原料松香類與(甲基)丙烯酸、(無水)馬來酸、富馬酸、(無水)檸康酸、(無水)衣康酸等不飽和羧酸進行狄耳士-阿德爾反應（Diels-Alder reaction）（加成反應）所得者。原料松香較佳為使用藉由蒸餾、再結晶、萃取等去除了金屬等雜質及為了提高樹脂色調而進行了純化者。另外，酸改質松香可藉由進行氫化而製成透明色調的酸改質松香。作為此種酸改質松香，可列舉：品新特（PINECRYSTAL）（註冊商標）KE-604、PINECRYSTAL（註冊商標）KR-120、瑪爾凱（MALKYD）（註冊商標）No.33（以上為商品名，荒川化學工業（股）製造）。該些酸改質松香含有兩個以上的羧基。因此，酸改質松香與環氧化合物反應，形成高密度的網眼結構，從而可提高耐熱性。此外，酸改質松香具有其化合物的大體積結構與藉由酸改質而生成的大體積的環結構，該些結構立體地阻礙環氧基對羧基的反應，從而提高接著劑組成物於室溫下的保存性。另一方面，於焊料熔點附近的200℃～250℃的溫度下，酸改質松香的分子運動性變高，從而去除焊料表面或接合金屬表面的氧化膜，接合部的焊料的潤濕性提高。
就提高接著劑組成物於室溫下的保存穩定性的方面或抑制安裝後的空隙的方面而言，（C）助焊劑中的酸改質松香的含量較佳為50質量%以上，更佳為90質量%以上，進而佳為95質量%以上。另外，上限是助焊劑全部為酸改質松香的100質量%。
就提高焊料的潤濕性的方面而言，相對於（D）於表面具有含有苯基的烷氧基矽烷的、平均粒徑為30 nm～200 nm的無機粒子100質量份，接著劑組成物中的（C）助焊劑的酸改質松香的含量較佳為5質量份以上，更佳為10質量份以上，進而佳為15質量份以上。另一方面，就抑制安裝後的空隙的方面而言，相對於（D）於表面具有含有苯基的烷氧基矽烷的、平均粒徑為30 nm～200 nm的無機粒子100質量份，（C）助焊劑的含量較佳為35質量份以下，更佳為30質量份以下，進而佳為25質量份以下。
本發明的接著劑組成物含有（D）於表面具有含有苯基的烷氧基矽烷的、平均粒徑為30 nm～200 nm的無機粒子。若為如所述般於表面具有含有苯基的烷氧基矽烷、且平均粒徑為30 nm～200 nm，則無機粒子於接著劑樹脂組成物中的分散性優異，結果，接著劑組成物的透明性得以確保，從而能夠識別對準標記。進而，由於該無機粒子的分散性優異，故能夠將無機粒子高濃度地填充於接著劑組成物中，可於製成接著劑組成物時抑制安裝後的空隙的產生，進而，製成硬化物時的線膨脹係數降低，從而可提高半導體裝置的連接可靠性。另外，（D）於表面具有含有苯基的烷氧基矽烷的、平均粒徑為30 nm～200 nm的無機粒子的平均粒徑的下限較佳為50 nm以上，更佳為75 nm以上。另外，（D）於表面具有含有苯基的烷氧基矽烷的、平均粒徑為30 nm～200 nm的無機粒子的平均粒徑的上限較佳為175 nm以下，更佳為150 nm以下。
作為於表面具有含有苯基的烷氧基矽烷的、平均粒徑為30 nm～200 nm的無機粒子，可列舉藉由苯基矽烷偶合劑進行了表面處理的無機粒子，例如可列舉：Sciqas 0.15 μm苯基矽烷處理、Sciqas 0.1 μm苯基矽烷處理、Sciqas 0.05 μm苯基矽烷處理（以上為商品名，堺化學工業（股）製造），YA050C（商品名，亞都瑪科技（Admatechs）（股）製造）。
此外，所謂無機粒子的平均粒徑，表示無機粒子單獨存在的情況下的粒徑，是指所觀察到的粒徑的平均值。於形狀為球狀的情況下表示其直徑，於橢圓狀及扁平狀的情況下表示形狀的最大長度。進而，於輥狀或纖維狀的情況下表示長度方向的最大長度。作為測定接著劑組成物中的無機粒子的平均粒徑的方法，可利用掃描式電子顯微鏡（scanning electron microscope，SEM）直接對粒子進行觀察，並藉由計算100個粒子的粒徑的平均值的方法來進行測定。
作為（D）於表面具有含有苯基的烷氧基矽烷的、平均粒徑為30 nm～200 nm的無機粒子所使用的無機粒子，例如可列舉：滑石（talc）、煅燒黏土、未煅燒黏土、雲母、玻璃等矽酸鹽，氧化鈦、氧化鋁、二氧化矽等氧化物，碳酸鈣、碳酸鎂等碳酸鹽，氫氧化鋁、氫氧化鎂、氫氧化鈣等氫氧化物，硫酸鋇、硫酸鈣、亞硫酸鈣等硫酸鹽或亞硫酸鹽，硼酸鋅、偏硼酸鋇、硼酸鋁、硼酸鈣、硼酸鈉等硼酸鹽，氮化鋁、氮化硼、氮化矽等氮化物等。該些無機粒子亦可含有多種，就可靠性及成本的方面而言，較佳為二氧化矽或氧化鈦。
相對於去除了溶劑的接著劑組成物的有機物總量，（D）於表面具有含有苯基的烷氧基矽烷的、平均粒徑為30 nm～200 nm的無機粒子的含量較佳為45質量份以上，更佳為50質量份以上。若為45質量份以上，則可於製成接著劑組成物時抑制安裝後的空隙的產生，進而，製成硬化物時的線膨脹係數降低，從而可提高半導體裝置的連接可靠性。另外，就抑制無機粒子彼此的凝聚、接著劑組成物的流動性良好、提高安裝後的接合部的焊料的潤濕性的方面而言，較佳為70質量%以下，更佳為65質量份以下。
（D）於表面具有含有苯基的烷氧基矽烷的、平均粒徑為30 nm～200 nm的無機粒子的形狀可為球狀，橢圓狀、扁平狀、輥狀、纖維狀等非球狀的任一者，由於球狀的無機粒子容易於鹼可溶性接著劑膜中均勻分散，故可較佳地使用。
本發明的接著劑組成物較佳為含有（E）硬化促進劑。硬化促進劑因不溶解於接著劑組成物地存在而使環氧化合物的硬化反應變慢，就提高室溫下的保存性的方面而言，（E）硬化促進劑較佳為硬化促進劑粒子。另外，若使用咪唑系硬化促進劑粒子作為硬化促進劑粒子，則環氧樹脂的硬化速度快，能夠抑制安裝後的空隙，因而較佳。作為此種硬化促進劑粒子，可較佳地使用屈爾唑（CUREZOL）（註冊商標）2PZCNS、CUREZOL（註冊商標）2PZCNS-PW、CUREZOL（註冊商標）C11Z-CNS、CUREZOL（註冊商標）2MZ-A、CUREZOL（註冊商標）C11-A、CUREZOL（註冊商標）2E4MZ-A、CUREZOL（註冊商標）2MZA-PW、CUREZOL（註冊商標）2MAOK-PW、CUREZOL（註冊商標）2PHZ-PW（以上為商品名，四國化成工業（股）製造）等。
硬化促進劑粒子的平均粒徑的下限較佳為0.1 μm以上，更佳為0.15 μm以上。另外，平均粒徑的上限較佳為2 μm以下，更佳為1 μm以下。此處所謂平均粒徑，表示硬化促進劑粒子單獨存在的情況下的平均粒徑。於硬化促進劑粒子的形狀為球狀的情況下表示其直徑，於橢圓狀及扁平狀的情況下表示形狀的最大長度。進而，於形狀為輥狀或纖維狀的情況下表示長度方向的最大長度。作為測定平均粒徑的方法，可利用掃描式電子顯微鏡（SEM）直接對粒子進行觀察，並藉由計算100個粒子的粒徑的平均值的方法來進行測定。若平均粒徑為0.1 μm以上，則接著劑膜的分散性良好，故製成膜時的膜的透明性高，對準標記的識別變得容易。若平均粒徑為2 μm以下，則硬化促進劑的比表面積增大，容易進行環氧化合物的硬化反應，接著劑組成物中所含的量減少，能夠抑制安裝後的空隙的產生。
另外，就使環氧化合物的硬化反應進行、表現出充分的接著力、提高安裝後的半導體裝置的連接可靠性的方面而言，相對於（B）重量平均分子量為100以上且3,000以下的環氧化合物100質量份，（E）硬化促進劑的含量較佳為1質量份以上，更佳為3質量份以上。另一方面，就抑制硬化反應，提高室溫下的保存穩定性，結果使接合部的焊料的潤濕性提高的方面而言，相對於（B）重量平均分子量為100以上且3,000以下的環氧化合物100質量份，（E）硬化促進劑的含量較佳為15質量份以下，更佳為10質量份以下。
本發明的接著劑組成物亦可進而含有離子補充劑、界面活性劑、矽烷偶合劑、有機染料、無機顏料等。
本發明的接著劑組成物可於溶媒中將各構成材料作為清漆（varnish）來使用，亦可將該清漆塗佈於剝離性基材上並進行脫溶媒而製成膜來使用。
作為溶媒，可將以下化合物單獨或混合兩種以上使用，但並不限定於該些：酮系溶劑中的丙酮、甲基乙基酮、甲基異丁基酮、環戊酮、環己酮；醚系溶劑中的1,4-二噁烷、四氫呋喃、二乙二醇二甲醚（diglyme）；二醇醚系溶劑中的甲基溶纖劑、乙基溶纖劑、丙二醇單甲醚、丙二醇單乙醚、丙二醇單丁醚、二乙二醇甲基乙基醚；此外，苄基醇、N-甲基吡咯啶酮、γ-丁內酯、乙酸乙酯、N,N-二甲基甲醯胺等。
作為剝離性基材，可列舉：聚丙烯膜、聚對苯二甲酸乙二酯膜、聚萘二甲酸乙二酯膜、聚酯膜、聚氯乙烯膜、聚碳酸酯膜、聚醯亞胺膜、聚四氟乙烯膜等氟樹脂膜、聚苯硫醚膜、聚丙烯膜、聚乙烯膜等，但並不限定於該些。另外，剝離性基材亦可藉由矽酮系脫模劑、長鏈烷基系脫模劑、氟系脫模劑、脂肪族醯胺系脫模劑等實施脫模處理。剝離性基材的厚度並無特別限定，通常較佳為5 μm～75 μm。另外，較佳為於接著劑的與具有脫模性基材的面相反側的面進而層壓另一剝離性基材，製成由剝離性基材上下夾持著的接著劑膜。另一剝離性基材的材質及厚度可使用與方才所說明的材質及厚度相同者。兩剝離性基材即便相同亦無妨。
另外，將各構成材料於溶媒中混合而製成清漆狀的接著劑組成物亦可塗佈於半導體晶圓或電路基板等並進行脫溶媒而使用。
本發明的接著劑組成物可適宜地用作半導體用接著劑組成物，所述半導體用接著劑組成物用於半導體裝置所使用的半導體元件、電路基板、金屬配線材料等電路構件彼此的接著或固定，或者半導體元件的密封。
本發明的半導體裝置包含所述接著劑組成物的硬化物或所述接著劑組成物膜的硬化物。所謂本發明的半導體裝置，是指可藉由利用半導體元件的特性而發揮功能的裝置整體。將半導體元件與基板連接而成者、將半導體元件彼此或基板彼此連接而成者、電光學裝置、半導體電路基板及電子設備全部包含於半導體裝置。
本發明的半導體裝置的製造方法的特徵在於：使所述接著劑組成物或所述接著劑組成物膜介於第一電路構件與第二電路構件之間，藉由加熱加壓而將所述第一電路構件與所述第二電路構件電性連接。
使用本發明的接著劑組成物的半導體裝置的製造方法的一例為如下所述。首先，準備具有第一連接端子的第一電路構件、與具有第二連接端子的第二電路構件。此處，所謂電路構件，可列舉半導體晶片、電阻晶片、電容器晶片等晶片構件，具有矽通孔（Through Silicon Via，TSV）電極的半導體晶片或矽中介層（silicon interposer），玻璃環氧電路基板、膜電路基板等基板等。另外，作為連接端子，可列舉：鍍敷凸塊或柱形凸塊（stud bump）等凸塊電極、或者墊電極等。另外，亦可於第一電路構件及/或第二電路構件形成有貫通電極、於構件的單面及/或兩面形成有連接端子。
將第一電路構件與第二電路構件以第一連接端子與第二連接端子相向的方式配置。其次，使本發明的接著劑組成物介於所述相向配置的第一連接端子與第二連接端子之間。然後，對第一電路構件與第二電路構件加熱加壓，而使所述相向配置的第一連接端子與第二連接端子電性連接。藉由該步驟，第一電路構件與第二電路構件牢靠地電性連接，並且接著劑硬化，而使第一電路構件與第二電路構件物理固定。
此處，接著劑組成物可先僅賦予至任一電路構件的連接端子側的面，亦可賦予至第一電路構件及第二電路構件的連接端子側的兩個面。
作為更詳細的實施方式的例，對如下般製作半導體裝置的方法加以說明，即，使用具有第一電路構件與凸塊的半導體晶片，使用具有配線圖案的電路基板或半導體晶片作為第二電路構件，介隔本發明的接著劑組成物膜而將兩者連接，利用接著劑將第一電路構件與第二電路構件之間的空隙密封。
首先，將接著劑組成物膜貼付於作為第二電路構件的形成有配線圖案的電路基板或半導體晶片上。此時，接著劑組成物膜可於切取規定的大小後，貼付於形成有配線圖案的電路基板的配線圖案面或半導體晶片的凸塊形成面。另外，亦可於將接著劑膜貼付於半導體晶圓的凸塊形成面上後，對半導體晶圓進行切割（dicing）而使其單片化，藉此製作貼付有接著劑膜的半導體晶片。
其次，將作為第一電路構件的半導體晶片以第一電路構件的凸塊與第二電路構件的配線圖案相向的方式配置，使用黏合（bonding）裝置對兩者加熱加壓。加熱加壓的條件只要為可良好地獲得電性連接的範圍，則並無特別限定，為了進行接著劑的硬化，必需溫度100℃以上、壓力1 mN/凸塊以上、時間0.1秒以上的加熱加壓。於較佳為120℃以上且300℃以下、更佳為150℃以上且250℃以下的溫度，較佳為5 mN/凸塊以上且50000 mN/凸塊以下、更佳為10 mN/凸塊以上且10000 mN/凸塊以下的壓力，較佳為1秒以上且60秒以下、更佳為2秒以上且30秒以下的時間的黏合條件下進行。另外，亦可於黏合時，作為暫時壓接，藉由溫度50℃以上、壓力1 mN/凸塊以上、時間0.1秒以上的加熱加壓，而使半導體晶片上的凸塊與電路基板上的配線圖案接觸，然後以所述條件進行黏合。亦可在視需要進行黏合後，於50℃以上且200℃以下的溫度下將帶有半導體晶片的電路基板加熱10秒以上且24小時以下。
除此以外，本發明的接著劑亦可用作接著性樹脂材料，所述接著性樹脂材料用於製作黏晶膜（die attach film）、切晶黏晶膜（dicing die attach film）、引線框架（lead frame）固定帶、散熱板、強化板、遮蔽材的接著劑，阻焊劑（solder resist）等。 實施例
以下，基於實施例對本發明加以具體說明，但本發明並不限定於此。
＜高分子化合物、環氧化合物的重量平均分子量＞ 溶解於N-甲基-2-吡咯啶酮（以下稱為NMP）而調整濃度0.1重量%的溶液，作為測定樣品。使用以下所示構成的GPC裝置Waters2690（沃特世（Waters）（股）製造），算出聚苯乙烯換算的重量平均分子量。關於GPC測定條件，將移動層設為分別以濃度0.05 mol/L溶解有LiCl與磷酸的NMP，將流量設為0.4 mL/分。另外，使用管柱烘箱將管柱加溫至40℃。 檢測器：Waters996 系統控制器：Waters2690 管柱：東曹（TOSOH）TSK-GEL α-4000 管柱：東曹（TOSOH）TSK-GEL α-2500。
＜無機粒子的平均粒徑＞ 利用掃描式電子顯微鏡（SEM，日本電子公司製造的JSM-6510A）對100個粒子的粒徑進行觀察，將其平均值作為平均粒徑。觀察中，以圓形觀察到粒子的情況下，將其直徑作為粒徑，以橢圓等形狀觀察到粒子的情況下，將粒子的輪廓中距離最長的區間的長度作為粒徑。
＜對準標記的識別＞ 接著劑組成物的對準標記的識別的評價如下般進行。自各實施例及比較例中製作的接著劑膜剝離保護膜後，使用層壓裝置（名機製作所（股）製造，MVLP600）將該接著劑組成物膜貼合於帶有銅柱凸塊的TEG晶片（沃爾茨（WALTS）（股）製造，WALTS-TEG CC80-0101JY）的銅柱凸塊形成面上。然後，將基材膜剝離，從而製作帶有接著劑組成物的評價晶片。製作10個該評價晶片。之後，利用倒裝晶片黏合裝置（東麗工程（Toray Engineering）（股）製造，FC-3000WS）的相機進行晶片上的圖案識別性評價。記錄10個所製作的評價晶片中能夠自動識別的個數。
＜空隙的評價＞ 如所述般進行了對準標記的識別評價後，於成為被著體的基板（WALTS（股）製造，WALTS-KIT CC80-0102JY[MAP]_模式（Model）I（Cu+OSP規格））進行倒裝晶片黏合。關於倒裝晶片黏合的條件，將基板放置於加熱至140℃的黏合台上，於溫度140℃、壓力150 N/晶片、時間1秒的條件下臨時壓接後，於溫度250℃、壓力150N的條件下將時間設為5秒而進行正式壓接。使用超音波影像裝置（日立電力解決方案（Hitachi Power Solutions）（股）製造，FS300III）對所得的半導體裝置進行空隙的觀察。作為空隙的評價，記錄晶片面積中空隙所佔的比例。此外，結果的下限設為1%以下，結果的上限設為10%以上。
＜接合部的焊料潤濕性評價＞ 如所述般進行了空隙的評價後，對半導體裝置進行剖面研磨而使接合處露出。之後，利用光學顯微鏡對接合形狀進行觀察。如圖1般，將銅柱凸塊100的焊料101在基板的銅配線102的側面的兩側潤濕的情況評價為A，將僅單側潤濕的情況評價為B，將任一側面均未潤濕、但配線上濕潤的情況評價為C，將任一側面均未潤濕、配線上亦存在接著劑組成物103的咬入的情況評價為D（圖1）。
各實施例及比較例中所用的（A）成分的聚醯亞胺如下般合成。
合成例1 聚醯亞胺的合成 於乾燥氮氣流下，將1,3-雙(3-胺基苯氧基)苯4.82 g（0.0165莫耳）、3,3'-二胺基-4,4'-二羥基二苯基碸3.08 g（0.011莫耳）、1,3-雙(3-胺基丙基)四甲基二矽氧烷4.97 g（0.02莫耳）、及作為封端劑的苯胺0.47 g（0.005莫耳）溶解於NMP 130 g中。向其中同時添加2,2-雙{4-(3,4-二羧基苯氧基)苯基}丙烷二酐26.02 g（0.05莫耳）與NMP 20 g，於25℃下反應1小時，繼而於50℃下攪拌4小時。之後，於180℃下攪拌5小時。攪拌結束後，將溶液投入至水3 L中，進行過濾並回收沈澱，利用水進行3次洗滌後，使用真空乾燥機於80℃下進行20小時乾燥。對所得的聚合物固體的紅外吸收光譜進行測定，結果，於1780 cm-1 附近、1377 cm-1 附近檢測到由聚醯亞胺所引起的醯亞胺結構的吸收峰值。另外，所得的聚醯亞胺的重量平均分子量為18000。
除此以外，各實施例及比較例所使用的（A）成分～（F）成分如下所述。 （A）成分 1256（商品名，苯氧基樹脂，重量平均分子量為50000，三菱化學（股）製造） 4250（商品名，苯氧基樹脂，重量平均分子量為60000，三菱化學（股）製造） （B）成分 YL-980（商品名，液狀環氧化合物，重量平均分子量370，三菱化學（股）製造） N-865（商品名，固體狀環氧化合物，重量平均分子量850，DIC（股）製造） 1032H60（商品名，固體狀環氧化合物，重量平均分子量525，三菱化學（股）製造） （C）成分 KR-120（商品名，酸改質松香100%，荒川化學工業（股）製造） （D）成分 Sciqas 0.15 μm苯基矽烷處理（商品名，二氧化矽，平均粒徑150 nm，苯基矽烷偶合表面處理、即於表面具有含有苯基的烷氧基矽烷，堺化學工業（股）製造） YA050C（商品名，二氧化矽，平均粒徑50 nm，苯基矽烷偶合表面處理、即於表面具有含有苯基的烷氧基矽烷，Admatechs（股）製造） （E）成分 2MAOK-PW（商品名，咪唑系硬化促進劑粒子，四國化成工業（股）製造） （F）其他 己二酸（助焊劑） Sciqas 0.15 μm（商品名，二氧化矽，平均粒徑150 nm，未表面處理，堺化學工業（股）製造） 實施例1～實施例9及比較例1～比較例3 （1）接著劑組成物膜的製作方法 以表1所記載的組成比將表1所示的（A）成分～（F）成分混合，而製作接著劑組成物清漆。使用環己酮作為有機溶劑，並將溶媒以外的添加物作為固體成分，而製成固體成分濃度為53%的接著劑組成物清漆。使用狹縫模塗佈機（塗敷機）將所製作的接著劑組成物清漆塗佈於作為剝離性基材的厚度38 μm的聚對苯二甲酸乙二酯膜的表面處理面，於100℃下進行10分鐘乾燥。藉此獲得乾燥後的厚度為30 μm的接著劑膜，將切割帶（T1902-90，聚烯烴基材，古河電氣工業（股）製造）的黏著面貼合於該接著劑膜上，獲得由基材膜與保護膜夾持的結構的接著劑組成物膜。此時，切割帶作為基材膜而發揮功能，聚對苯二甲酸乙二酯膜作為保護膜而發揮功能。使用所得的接著劑組成物膜，如所述般實施對準標記的識別、空隙的評價、接合部的潤濕性評價。將結果示於表1。
【表1】 [產業上之可利用性]
本發明的接著劑組成物可用作如下接著劑，所述接著劑可用於電腦、可攜式終端機中所使用的電子構件或散熱板與印刷基板或可撓性基板的接著、以及基板彼此的接著。進而，本發明的接著劑組成物可適宜地用作如下半導體用接著劑，所述半導體用接著劑可於將IC、LSI等半導體晶片接著或直接電性接合於可撓性基板、玻璃環氧基板、玻璃基板、陶瓷基板等電路基板時使用。
100‧‧‧銅柱凸塊 101‧‧‧焊料 102‧‧‧銅配線 103‧‧‧接著劑組成物
圖1是表示使用本發明的接著劑組成物所製作的半導體裝置的接合部的焊料潤濕性的示意圖。
100‧‧‧銅柱凸塊
101‧‧‧焊料
102‧‧‧銅配線
103‧‧‧接著劑組成物

Claims (8)

  1. 一種接著劑組成物，其含有：（A）高分子化合物；（B）重量平均分子量為100以上且3,000以下的環氧化合物；（C）助焊劑；及（D）於表面具有含有苯基的烷氧基矽烷的、平均粒徑為30 nm～200 nm的無機粒子，且所述接著劑組成物的特徵在於：（C）助焊劑含有酸改質松香。
  2. 如申請專利範圍第1項所述的接著劑組成物，其中所述（A）高分子化合物為重量平均分子量10,000以上且100,000以下的苯氧基樹脂。
  3. 如申請專利範圍第1項或第2項所述的接著劑組成物，其中所述（C）助焊劑中的酸改質松香的含量為50質量%以上且100質量%以下。
  4. 如申請專利範圍第1項至第3項中任一項所述的接著劑組成物，其中，相對於所述（D）於表面具有含有苯基的烷氧基矽烷的、平均粒徑為30 nm～200 nm的無機粒子100質量份，所述（C）助焊劑的酸改質松香的含量為5質量份～35質量份。
  5. 如申請專利範圍第1項至第4項中任一項所述的接著劑組成物，其更含有（E）硬化促進劑。
  6. 如申請專利範圍第1項至第5項中任一項所述的接著劑組成物，其中，相對於接著劑組成物的總量，所述（D）於表面具有含有苯基的烷氧基矽烷的、平均粒徑為30 nm～200 nm的無機粒子的含量為45質量%～70質量%。
  7. 一種半導體裝置，其包含如申請專利範圍第1項至第6項中任一項所述的接著劑組成物的硬化物。
  8. 一種半導體裝置的製造方法，其使如申請專利範圍第1項至第6項中任一項所述的接著劑組成物介於第一電路構件與第二電路構件之間，將所述第一電路構件與所述第二電路構件電性連接。
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