TWI501039B - 感光性樹脂組成物、感光性樹脂組成物薄膜及使用其之半導體裝置 - Google Patents
感光性樹脂組成物、感光性樹脂組成物薄膜及使用其之半導體裝置 Download PDFInfo
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- TWI501039B TWI501039B TW100123255A TW100123255A TWI501039B TW I501039 B TWI501039 B TW I501039B TW 100123255 A TW100123255 A TW 100123255A TW 100123255 A TW100123255 A TW 100123255A TW I501039 B TWI501039 B TW I501039B
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Classifications
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Description
本發明關於感光性樹脂組成物及感光性樹脂組成物薄膜。更詳言之,係關於使用在半導體元件、多層結構的半導體裝置、影像感應器等之感光性組成物,尤其是具有接著機能的感光性樹脂組成物。
近年來,為了實現半導體裝置、電子構件的高性能化、低成本化,已提議各種的封裝形態。例如,為了形成如影像感應器或MEMS之類的中空狀封裝,已知用具有接著性的樹脂間隔材圍住元件周圍,在上面貼合玻璃等基板而形成中空構造的方法(例如,參照專利文獻1)。在如此用途中,尋求能夠藉光蝕刻法進行圖案化之接著劑。
又,尤其是隨著記憶體、系統LSI等半導體裝置的小型化、作動速度之高速化、高密度配線化,而進行3維構造之半導體封裝的實用化探討,以取代習知的利用銲線之連接,該3維構造之半導體封裝是利用貫穿孔在矽晶片的表裏兩面設置墊片(pad)或凸塊(bump)等之電極構造,並進行積層而確保晶片間之導通(參照非專利文獻1)。在此種構造的封裝中,係探討為積層晶片所使用之接著劑。在此所使用的接著劑除了以低應力性、接著性、絶緣性、可耐焊料回流之耐熱性等安裝可靠性為前提的特性之外,為使電極部分露出以確保晶片間的導通,較佳為亦具有能夠利用圖案化而去除電極上之接著劑的感光性。
作為具有感光性與高耐熱性之接著劑,已知使用聚醯亞胺樹脂前驅物的材料(例如,參照專利文獻2),此等材料為了醯亞胺之閉環反應,必須在300℃以上的高溫進行熱硬化。因此,隨著硬化收縮因而熱應力變大,會有發生基板翹屈、接著強度降低等擔憂。為解決此等課題,有提議一種使用可溶性聚醯亞胺作為基質樹脂,以降低硬化溫度之負型感光性材料(例如,參照專利文獻3)。又,同樣地,亦已知使用可溶性聚醯亞胺作為基質樹脂,而可低溫硬化的正型感光性材料(例如,參照專利文獻4、5)。
專利文獻1 日本特開2008-286877號公報
專利文獻2 日本特開平04-337380號公報
專利文獻3 日本特開2008-281597號公報
專利文獻4 日本特開2006-313237號公報
專利文獻5 日本特開2009-20246號公報
非專利文獻1 用以3維安裝之TSV技術,傳田精一著(2009)
然而,專利文獻3記載之樹脂設計其可溶性聚醯亞胺之熱應力大,而有對矽晶圓或玻璃基板等支撐基材之熱壓合性不足的情形。再者,此材料為負型感光性材料,圖案形狀容易成為倒錐狀。因此,產生圖案崩毀等缺陷,基於在圖案側壁形成配線等目的時,則有難以進行濺鍍膜等之成膜等問題。另一方面,專利文獻4、5記載之正型感光性材料不具有足夠的接著機能,溶媒乾燥後的膜為脆,因此亦難以B階段薄片化而使用。
本發明之目的為提供一種硬化後的應力小、接著性優異的正型感光性樹脂組成物及感光性樹脂組成物薄膜。
本發明為一種感光性樹脂組成物,其特徵為含有(a)具有下述通式(1)所表示之結構單位且在主鏈末端之至少一側具有通式(2)及/或(3)所表示之構造的鹼可溶性聚醯亞胺、(b)在分子內具有2個以上的環氧基及/或氧雜環丁烷基(oxetanyl)之化合物、(c)萘醌二疊氮化合物,且相對於100重量份(a)聚醯亞胺而言,(b)化合物的含量為20重量份以上。
根據本發明,可得一種感光性樹脂組成物及感光性樹脂組成物薄膜,其係能夠利用光蝕刻法形成正型圖案、硬化後的應力小、可得與半導體元件或支撐構材之高接著強度。
本發明之感光性樹脂組成物含有(a)具有下述通式(1)所表示之結構單位且在主鏈末端之至少一側具有通式(2)及/或(3)所表示之構造的鹼可溶性聚醯亞胺、(b)在分子內具有2個以上的環氧基及/或氧雜環丁烷基之化合物、(c)萘醌二疊氮化合物,且相對於100重量份(a)聚醯亞胺而言,(b)化合物的含量為20重量份以上。
(a)成分之聚醯亞胺為鹼可溶性聚醯亞胺。在此所謂鹼可溶性是指對2.38%四甲銨水溶液之溶解度為0.1g/100mL以上。在此所謂鹼可溶性是指對2.38%四甲銨水溶液之溶解度為0.1g/100mL以上。由於顯現此種鹼可溶性,且能夠進行良好的圖案加工,故(a)成分之聚醯亞胺係具有下述通式(1)所表示之結構單位,且在主鏈末端之至少一側具有通式(2)及/或(3)所表示之構造。
式中,X表示具有至少一個選自由羧基、酚性羥基、磺酸基及硫醇基所構成之群組的基團之1價有機基,Y表示具有至少一個選自由羧基、酚性羥基、磺酸基及硫醇基所構成之群組的基團之2價有機基。X較佳為芳香族基,Y較佳為芳香族基或具有碳-碳雙鍵的基。其中,X及Y較佳為具有酚性羥基或硫醇基。
又,R1
表示4~14價有機基,R2
表示2~12價有機基,R3
及R4
係各自獨立地表示至少一個選自由羧基、酚性羥基、磺酸基、及硫醇基所構成之群組的基團。又,α及β係各自獨立地表示0~10之整數。
在上述通式(1)中,R1
表示來自四羧酸二酐的結構成分。其中,較佳為含有芳香族基或環狀脂肪族基之碳原子數5~40的有機基。
具體而言,作為四羧酸二酐,可列舉苯均四酸二酐、3,3’,4,4’-聯苯四羧酸二酐、2,3,3’,4’-聯苯四羧酸二酐、2,2’,3,3’-聯苯四羧酸二酐、3,3’,4,4’-二苯基酮四羧酸二酐、2,2’,3,3’-二苯基酮四羧酸二酐、2,2-雙(3,4-二羧基苯基)丙烷二酐、2,2-雙(2,3-二羧基苯基)丙烷二酐、1,1-雙(3,4-二羧基苯基)乙烷二酐、1,1-雙(2,3-二羧基苯基)乙烷二酐、雙(3,4-二羧基苯基)甲烷二酐、雙(2,3-二羧基苯基)甲烷二酐、雙(3,4-二羧基苯基)硫醚二酐(bis(3,4-dicarboxyphenyl) sulfide dianhydride)、雙(3,4-二羧基苯基)醚二酐、1,2,5,6-萘四羧酸二酐、9,9-雙(3,4-二羧基苯基)茀二酸酐、9,9-雙{4-(3,4-二羧基苯氧基)苯基}茀二酸酐、2,3,6,7-萘四羧酸二酐、2,3,5,6-吡啶四羧酸二酐、3,4,9,10-苝四羧酸二酐、2,2-雙(3,4-二羧基苯基)六氟丙烷二酐等之芳香族四羧酸二酐、或丁烷四羧酸二酐、1,2,3,4-環戊烷四羧酸二酐等之脂肪族四羧酸二酐、及下述所示構造之二酸酐等。此等係可單獨或組合2種以上使用。
在此,R9
表示選自氧原子、C(CF3
)2
、C(CH3
)2
、CO、COO及SO2
的基團,R10
及R11
係分別表示選自氫原子、羥基及硫醇基之基團。
在上述通式(1)中,R2
表示來自二胺之結構成分。其中,較佳為含有芳香族基或環狀脂肪族基之碳原子數5~40的有機基。
就二胺的具體例而言,可列舉3,3’-二胺基二苯基醚、3,4’-二胺基二苯基醚、4,4’-二胺基二苯基醚、3,3’-二胺基二苯基甲烷、3,4’-二胺基二苯基甲烷、4,4’-二胺基二苯基甲烷、3,3’-二胺基二苯基碸、3,4’-二胺基二苯基碸、4,4’-二胺基二苯基碸、3,4’-二胺基二苯基硫醚、4,4’-二胺基二苯基硫醚、1,4-雙(4-胺基苯氧基)苯、1,3-雙(4-胺基苯氧基)苯、1,3-雙(3-胺基苯氧基)苯、聯苯胺、m-苯二胺、p-苯二胺、1,5-萘二胺、2,6-萘二胺、雙(4-胺基苯氧基苯基)碸、雙(3-胺基苯氧基苯基)碸、雙(4-胺基苯氧基)聯苯、雙{4-(4-胺基苯氧基)苯基}醚、1,4-雙(4-胺基苯氧基)苯、2,2’-二甲基-4,4’-二胺基聯苯、2,2’-二乙基-4,4’-二胺基聯苯、3,3’-二甲基-4,4’-二胺基聯苯、3,3’-二乙基-4,4’-二胺基聯苯、2,2’,3,3’-四甲基-4,4’-二胺基聯苯、3,3’,4,4’-四甲基-4,4’-二胺基聯苯、2,2’-二(三氟甲基)-4,4’-二胺基聯苯、9,9-雙(4-胺基苯基)茀、或在此等之芳香族環以烷基或鹵素原子取代之化合物、或脂肪族之環己基二胺、亞甲基雙環己胺及下述所示構造之二胺等。此等係可單獨或組合2種以上使用。
在此,R9
表示選自氧原子、C(CF3
)2
、C(CH3
)2
、CO、COO、及SO2
的基團,R10
~R13
係分別表示選自羥基及硫醇基的基團。
此等之中,較佳為3,3’-二胺基二苯基醚、3,4’-二胺基二苯基醚、4,4’-二胺基二苯基醚、3,3’-二胺基二苯基甲烷、3,4’-二胺基二苯基甲烷、4,4’-二胺基二苯基甲烷、3,3’-二胺基二苯基碸、3,4’-二胺基二苯基碸、4,4’-二胺基二苯基碸、3,4’-二胺基二苯基硫醚、4,4’-二胺基二苯基硫醚、m-苯二胺、p-苯二胺、1,4-雙(4-胺基苯氧基)苯、9,9-雙(4-胺基苯基)茀及下述所示構造之二胺等。
R9
表示選自氧原子、C(CF3
)2
、C(CH3
)2
及SO2
的基團,R10
~R13
係分別表示選自羥基及硫醇基的基團。
在通式(1)中,R3
及R4
係各自獨立地表示選自由羧基、酚性羥基、磺酸基及硫醇基構成之群組的至少一個基團。藉由調整此R3
及R4
的量,聚醯亞胺相對於鹼水溶液之溶解速度改變,因此可得具有適度溶解速度之感光性樹脂組成物。
再者,為了提升與基板之接著性等,亦可在不使耐熱性降低的範圍內,在R2
共聚具有矽氧烷構造之脂肪族基。具體而言,作為二胺成分,可列舉共聚1~10莫耳%之雙(3-胺基丙基)四甲基二矽氧烷、雙(p-胺基-苯基)八甲基五矽氧烷等而成者。
通式(2)及(3)係表示具有通式(1)所表示之結構單位的聚醯亞胺之末端構造。聚醯亞胺雖具有2個末端,但只要此等之中1個以上為通式(2)及/或(3)所表示之構造即可。
在主鏈末端具有通式(2)及/或(3)所表示之構造的聚醯亞胺是把部分二胺用末端封裝劑之單胺取代,或把四羧酸二酐以末端封裝劑之二羧酸酐取代,可利用周知方法進行合成。例如,在低溫中使四羧酸二酐、二胺化合物與單胺反應之方法;在低溫中使四羧酸二酐、二羧酸酐與二胺化合物反應之方法;藉由四羧酸二酐與醇得到二酯,隨後在二胺、單胺與縮合劑的存在下使其進行反應之方法等,藉此可得聚醯亞胺前驅物。然後,將所得聚醯亞胺前驅物利用周知之醯亞胺化反應法予以醯亞胺化,而可合成聚醯亞胺。
在通式(2)中,X係來自末端封裝劑之1級單胺。就用作為末端封裝劑之1級單胺而言,較佳為5-胺基-8-羥基喹啉、1-羥基-7-胺基萘、1-羥基-6-胺基萘、1-羥基-5-胺基萘、1-羥基-4-胺基萘、2-羥基-7-胺基萘、2-羥基-6-胺基萘、2-羥基-5-胺基萘、1-羧基-7-胺基萘、1-羧基-6-胺基萘、1-羧基-5-胺基萘、2-羧基-7-胺基萘、2-羧基-6-胺基萘、2-羧基-5-胺基萘、2-胺基安息香酸、3-胺基安息香酸、4-胺基安息香酸、4-胺基水楊酸、5-胺基水楊酸、6-胺基水楊酸、2-胺基苯磺酸、3-胺基苯磺酸、4-胺基苯磺酸、3-胺基-4,6-二羥基嘧啶、2-胺基苯酚、3-胺基苯酚、4-胺基苯酚、2-胺基硫苯酚、3-胺基硫苯酚、4-胺基硫苯酚等。此等係可單獨或組合2種以上使用。
又,在通式(3)中,Y是來自末端封裝劑之二羧酸酐。就用作為末端封裝劑之酸酐而言,較佳為4-羧基酞酸酐、3-羥基酞酸酐、順式烏頭酸酐等。此等係可單獨或組合2種以上使用。
具有通式(1)所表示之結構單位且在主鏈末端之至少一側具有通式(2)及/或(3)所表示之構造的聚醯亞胺,其重複單位可為僅含通式(1)所表示之結構單位,亦可為與其他結構單位之共聚物,亦可含通式(1)所表示之結構單位之前驅物(聚醯胺酸構造)。此時,較佳為含有聚醯亞胺全體的50mol%以上之通式(1)所表示之結構單位。用於共聚或混合之結構單位的種類及量較佳為在無損藉最終加熱處理所得之聚醯亞胺的耐熱性之範圍內加以選擇。
(a)之聚醯亞胺的醯亞胺化率可利用例如以下方法容易地求得。在此,醯亞胺化率是指在如前述般經由聚醯亞胺前驅物合成聚醯亞胺時,在聚醯亞胺前驅物之中,多少莫耳%被轉換成聚醯亞胺的意思。首先,測定聚醯亞胺前驅物之紅外吸收光譜,確認起因於聚醯亞胺之醯亞胺構造的吸收波峰(1780cm-1
附近、1377cm-1
附近)的存在。接著,將此聚醯亞胺前驅物在350℃熱處理1小時後,再次測定紅外吸收光譜,比較熱處理前與熱處理後在1377cm-1
附近的波峰強度。把熱處理後之聚合物之醯亞胺化率當作100%,求出熱處理前之聚合物的醯亞胺化率。(a)之聚醯亞胺的醯亞胺化率較佳為90%以上。
導入(a)之聚醯亞胺的末端封裝劑能夠用以下方法檢測。例如,把已導入末端封裝劑之聚醯亞胺溶解在酸性溶液中,分解成聚醯亞胺之構成單位的胺成分與羧酸酐成分,將其以氣相層析法(GC)或NMR進行分析。也可以利用不同方法將已導入末端封裝劑之聚醯亞胺直接用熱分解層析法(PGC)或紅外光譜及13
CNMR光譜進行分析。
(a)之聚醯亞胺的重量平均分子量宜為10,000以上100,000以下。含有2種以上聚醯亞胺時,較佳為其中至少1種之重量平均分子量在上述範圍內。重量平均分子量小於10,000,則會有機械強度顯著降低且接著強度降低的情形。較佳為12,000以上。另一方面,重量平均分子量超過100,000時,會有對鹼顯影液的溶解性降低而產生顯影殘渣的情形。較佳為50,000以下。又,本發明中的重量平均分子量是利用凝膠滲透層析法(GPC法)測定且以聚苯乙烯換算而算出。
本發明之感光性樹脂組成物含有(b)在分子內具有2個以上的環氧基及/或氧雜環丁烷基之化合物,且(b)較佳為具有2個以上之環氧基之化合物。就在分子內具有2個以上之環氧基之化合物而言,可舉出雙酚A型環氧基化合物、雙酚F型環氧基化合物、酚醛清漆型環氧基化合物、聯苯酚型環氧基化合物、聯苯型環氧基化合物、縮水甘油胺型環氧基化合物、環狀脂肪族環氧基化合物等。具體而言,可舉出“jER(註冊商標)”828、834、1001、1002、1003、1004、1005、1007、1010、1100L、630、ESCN-220L、220F、220H、220HH、180H65、1032H60、YX4000H、152、157S70、1031(三菱化學(股))、“Epolight”40E、“Epolight”100E、“Epolight”200E、“Epolight”400E、“Epolight”70P、“Epolight”200P、“Epolight”400P、“Epolight”1500NP、“Epolight”80MF、“Epolight”4000、“Epolight”3002(共榮公司化學工業(股)製)、“ADEKA Resin(註冊商標)”EP-4000S、EP-4003S(ADEKA(股)製)、“Denacol”EX-212L、“Denacol”EX-214L、“Denacol”EX-216L、“Denacol”EX-850L、“Denacol”EX-321L(Nagase ChemteX(股)製)、“EPICLON(註冊商標)”850、EXA-850CRP、860、EXA-4701(DIC(股)製)“Tepic”S、“Tepic”G、“Tepic”P(日產化學工業(股)製)、GAN、GOT、EPPN502H、NC3000、NC6000(日本化藥(股)製)等。又,關於在分子內具有2個以上氧雜環丁烷基之化合物的具體例,可舉出OXT-121、OXT-221、OX-SQ-H、OXT-191、PNOX-1009、RSOX(東亞合成(股)製)、“Eternacoll”OXBP、同OXTP(宇部興產(股)製)等。
又,為了確保接著強度、熱壓合時之流動性、及硬化膜之低應力化,(b)化合物的含量相對於100重量份(a)之聚醯亞胺而言,必須為20重量份以上,更佳為40重量份以上。又,從耐熱性、顯影特性等觀點而言,相對於100重量份(a)之聚醯亞胺而言,較佳為100重量份以下。
本發明之感光性樹脂組成物含有(c)萘醌二疊氮化合物。所用之萘醌二疊氮化合物雖無特別限制,但可舉出一例為:在具有酚性羥基之化合物上以酯結合萘醌二疊氮磺酸而成之化合物。就具有酚性羥基之化合物而言,較佳為使用在分子內具有2個以上苯酚核之化合物。又,此等萘醌二疊氮化合物能夠利用具有酚性羥基之化合物與萘醌二疊氮磺酸氯化物之周知的酯化反應來合成。
就具有酚性羥基之化合物的具體例而言,可舉出以下化合物(皆為本州化學工業(股)製)。
由感度及解析度之觀點而言,此等具有酚性羥基的化合物之中,較佳為採用TekP-4HBPA、TrisP-HAP、TrisP-PA、Phcc-AP。
關於作為原料之萘醌二疊氮磺酸氯化物而言,可使用4-萘醌二疊氮磺酸氯化物或5-萘醌二疊氮磺酸氯化物。由於4-萘醌二疊氮磺酸酯化合物係在i線(波長365nm)領域具有吸收,所以適於i線曝光。又,由於5-萘醌二疊氮磺酸酯化合物是在廣範圍的波長領域存在著吸收,所以適於以廣範圍之波長的曝光。較佳為依照所曝光之波長選擇4-萘醌二疊氮磺酸酯化合物、5-萘醌二疊氮磺酸酯化合物。又,亦可混合使用4-萘醌二疊氮磺酸酯化合物和5-萘醌二疊氮磺酸酯化合物。又,從解析度方面來看,較佳為在分子內具有2個以上之萘醌二疊氮磺酸酯構造。
萘醌二疊氮化合物的添加量係無特別限制,較佳為相對於100重量份(a)之聚醯亞胺而言為5~40重量份,進一步更佳為10~30重量份。又,為獲得更良好的溶解對比,較佳為5重量份以上。另一方面,萘醌二疊氮化合物的添加量比40重量份多時,會有用感光性樹脂組成物形成的薄膜或硬化膜變脆的情形。
本發明之感光性樹脂組成物亦可含有丙烯酸樹脂。在此所稱丙烯酸樹脂是指不飽和羧酸或不飽和羧酸酯等之聚合物,日本特開2009-20246記載的丙烯酸樹脂等係與其相當。惟,多量含有丙烯酸樹脂時,在250℃以上的熱安定性降低,所以會損及可靠性。且,由於溶媒乾燥後的膜變脆,因此亦極難以B階段薄膜化而使用。從此等觀點而言,相對於100重量份(a)之聚醯亞胺而言,丙烯酸樹脂的含量較佳為小於10重量份,尤其是把本發明之感光性樹脂組成物用作為薄膜時,較佳為實質上不含丙烯酸樹脂。
本發明之感光性樹脂組成物亦可含界面活性劑、二氧化矽、二氧化鈦等之無機粒子、交聯劑、交聯促進劑、增感劑、溶解調整劑、安定劑、消泡劑等之添加劑、矽烷偶合劑、鈦螯合劑、氧化鋯螯合劑等。
較佳為在本發明之感光性樹脂組成物添加有機溶劑。就在此所使用之有機溶劑而言,只要是能夠溶解或分散各成分者即可。
具體而言,有機溶劑可舉出乙二醇單甲基醚、乙二醇單乙基醚、丙二醇單甲基醚、丙二醇單乙基醚、乙二醇二甲基醚、乙二醇二乙基醚、乙二醇二丁基醚等之醚類,乙二醇單乙基醚乙酸酯、丙二醇單甲基醚乙酸酯、丙基乙酸酯、丁基乙酸酯、異丁基乙酸酯、3-甲氧基丁基乙酸酯、3-甲基-3-甲氧基丁基乙酸酯、乳酸甲酯、乳酸乙酯、乳酸丁酯等之乙酸酯類,丙酮、甲基乙基酮、乙醯基丙酮、甲基丙基酮、甲基丁基酮、甲基異丁基酮、環戊酮、2-庚酮等之酮類,丁基醇、異丁基醇、戊醇、4-甲基-2-戊醇、3-甲基-2-丁醇、3-甲基-3-甲氧基丁醇、二丙酮醇等之醇類,甲苯、二甲苯等之芳香族烴類、其他N-甲基-2-吡咯啶酮、N-環己基-2-吡咯啶酮、N,N-二甲基甲醯胺、N,N-二甲基乙醯胺、二甲基亞碸、γ-丁內酯等。
又,亦可用濾紙或過濾器過濾感光性樹脂組成物。過濾方法係無特別限定,可舉出用保留粒徑0.2μm~10μm的薄膜過濾器(membrane filter)予以加壓過濾,藉此進行過濾之方法等。
本發明之感光性樹脂組成物其硬化前的形狀係無限定,可舉出例如清漆狀或薄膜狀等。薄膜狀的情況下亦可為形成在支撐體上的薄片狀。以清漆狀使用時,可使用將(a)~(c)成分及視需要所添加的成分溶解在上述有機溶媒而成者。又,感光性樹脂組成物薄膜係例如在支撐體上塗布本發明之感光性樹脂組成物,接著將其依照需要進行乾燥而得。
本發明之積層體係依序具有支撐體、本發明之感光性樹脂組成物薄膜及保護薄膜。又,本發明之感光性樹脂組成物薄膜較佳為形成在支撐體上。本發明之積層體所用的支撐體係無特別限定,可使用聚對苯二甲酸乙二酯(PET)薄膜、聚乙烯薄膜、聚丙烯(PP)薄膜、聚苯硫薄膜、聚醯亞胺薄膜等一般市售之各種薄膜。在支撐體的表面,為了調整與感光性樹脂組成物的濕潤性、密合性、剝離性,亦可實施聚矽氧、矽烷偶合劑、鋁螯合劑、聚尿素等之表面處理。又,支撐體的厚度係無特別限定,惟,從作業性的觀點來看,較佳為10~100μm之範圍。
又,本發明之感光性樹脂組成物薄膜為了保護表面,亦可在感光性樹脂組成物薄膜上具有保護薄膜。作為保護薄膜,可舉出聚乙烯薄膜、聚丙烯(PP)薄膜、聚酯薄膜等。保護薄膜較佳為與感光性接著薄膜的接著力小。
關於形成本發明之積層體的方法,可舉出在支撐體的薄膜上塗布本發明之感光性樹脂組成物,使其乾燥後,在感光性樹脂組成物薄膜的表面層合保護薄膜之方法。
關於將感光性樹脂組成物塗布在支撐體上的方法,可舉出使用旋塗機之旋轉塗布、噴灑塗布、輥塗覆、網版印刷、刮刀式塗法、模口塗法、簾幕式塗法、凹凸塗法(meniscus coat)、棒塗法、輥塗法、逗點輥塗法(knife roll coat)、凹版塗布、網版塗布、狹縫模口塗法等方法。又,塗布膜厚雖然依照塗布手法、組成物的固體含量濃度、黏度等而異,但通常乾燥後的膜厚較佳為0.5μm以上80μm以下。
乾燥可使用烘箱、加熱板、紅外線烘箱等。乾燥溫度及乾燥時間只要是能夠使有機溶媒揮發的範圍即可,較佳為適宜設定成使感光性樹脂組成物薄膜變成未硬化或半硬化狀態的條件。具體而言,宜在40℃~120℃的範圍內進行1分~數十分。又,亦可組合此等溫度而階段性昇溫,例如,在70℃、80℃、90℃各進行1分鐘熱處理。
接著,針對本發明之感光性樹脂組成物、及將使用其之感光性樹脂組成物薄膜進行圖案加工的方法、熱壓合於其他構材的方法,舉例加以說明。
首先,用本發明之感光性樹脂組成物、及使用它之感光性樹脂組成物薄膜,在基板上形成感光性樹脂組成物被膜。感光性樹脂組成物可在基板上塗布,且視需要進行乾燥,藉此形成被膜。就塗布方法而言,可舉出使用旋塗機之旋轉塗布、噴灑塗布、輥塗覆、網版印刷等方法。又,塗布膜厚雖然依塗布手法、樹脂組成物的固體含量濃度及黏度等而異,但通常較佳為以乾燥後之膜厚成為0.5μm以上80μm以下的方式進行塗布。乾燥可使用烘箱、加熱板、紅外線等。乾燥溫度及乾燥時間只要是可使有機溶媒揮發的範圍即可,較佳為適宜設定成使感光性樹脂組成物被膜變成未硬化或半硬化狀態的條件。具體而言,較佳為在50~150℃的範圍進行1分~數小時。
另一方面,感光性樹脂組成物薄膜為具有保護薄膜的情況下,是將其剝離,且使感光性樹脂組成物薄膜與基板相向,利用熱壓合進行貼合。熱壓合可藉由熱壓處理、熱層合處理、熱真空層合處理等來進行。從對基板凹凸的追隨性方面來看,貼合溫度宜為40℃以上。又,為了防止因貼合時感光性樹脂組成物薄膜的硬化導致圖案解析度變差,貼合溫度宜為150℃以下。
就基板的例子而言,可舉出矽晶圓、陶瓷類、砷化鎵、有機系電路基板、無機系電路基板、及在此等基板上配置電路的構成材料者,惟不限定於此等。就有機系電路基板的例子而言,可舉出玻璃布‧環氧基覆銅積層板等之玻璃基材覆銅積層板、玻璃不織布‧環氧基覆銅積層板等之複合覆銅積層板、聚醚醯亞胺樹脂基板、聚醚酮樹脂基板、聚碸系樹脂基板等之耐熱‧熱可塑性基板、聚酯覆銅薄膜基板、聚醯亞胺覆銅薄膜基板等之撓性基板。又,就無機系電路基板而言,氧化鋁基板、氮化鋁基板、碳化矽基板等之陶瓷基板、鋁基底基板、鐵基底基板等之金屬系基板。電路的構成材料之例子可舉出含有銀、金、銅、鋁等金屬的導體、含有無機系氧化物之電阻體、含有玻璃系材料及/或樹脂等之低介電體、含有樹脂或高介電常數無機粒子等之高介電體、含有玻璃系材料等之絶緣體等。
接著,在藉上述方法所形成的感光性樹脂組成物被膜上方,透過具有期望圖案的遮罩照射曝光光,並進行曝光。曝光光源較佳為使用水銀燈的i線(365nm)、h線(405nm)、g線(436nm)。在感光性樹脂組成物薄膜中,支撐體為對此等光線而言呈透明的材質時,亦可不從感光性樹脂組成物薄膜剝離支撐體而進行曝光。又,曝光裝置可使用縮小投影型曝光裝置、遮罩對準器、鏡式投影型曝光裝置等。
形成圖案方面,是在曝光後,以顯影液除去曝光部。就顯影液而言,較佳為四甲銨水溶液、二乙醇胺、二乙胺基乙醇、氫氧化鈉、氫氧化鉀、碳酸鈉、碳酸鉀、三乙胺、二乙胺、甲胺、二甲胺、醋酸二甲胺基乙酯、二甲胺基乙醇、二甲胺基乙基甲基丙烯酸酯、環己胺、乙二胺、六亞甲基二胺等之顯示鹼性的化合物之水溶液。又,視情況,亦可為在此等鹼水溶液中單獨含有下列或含有下列之數種組合:N-甲基-2-吡咯啶酮、N,N-二甲基甲醯胺、N,N-二甲基乙醯胺、二甲基亞碸、γ-丁內酯、二甲基丙烯醯胺等極性溶媒、甲醇、乙醇、異丙醇等醇類、乳酸乙酯、丙二醇單甲基醚乙酸酯等酯類、環戊酮、環己酮、異丁基酮、甲基異丁基酮等酮類等。
顯影可藉由對被膜面噴灑上述顯影液,在被膜面盛裝顯影液而浸漬在顯影液中、或浸漬而施加超音波等之方法進行。顯影時間或顯影步驟顯影液的溫度等顯影條件只要是能夠除去曝光部以形成圖案的條件即可。
較佳為顯影後以水進行清洗處理。在此亦可把乙醇、異丙基醇等醇類、乳酸乙酯、丙二醇單甲基醚乙酸酯等酯類加入水進行清洗處理。
又,視需要亦可在顯影前進行烘烤處理。藉此,有時會提高顯影後圖案的解析度、增大顯影條件的容許寬。此烘烤處理溫度較佳為50~180℃之範圍,特佳為60~120℃之範圍。時間宜為5秒~數小時。
圖案形成後,在感光性樹脂組成物被膜中係殘存醌二疊氮化合物。因此,於熱壓合或硬化之際,此等有時會熱分解而產生氮。為避免此情形,較佳為在圖案形成後之感光性樹脂組成物被膜的整面照射上述曝光光,並預先使醌二疊氮化合物分解。此製程稱為去色(bleaching)曝光。
圖案形成後或去色曝光後,為了減低殘存在感光性樹脂組成物被膜中的溶媒、揮發成分、水、氮等,較佳為在60~200℃之範圍進行加熱乾燥。時間較佳為1分~數小時。
把形成有圖案的感光性樹脂組成物被膜所形成之基板熱壓合在基板或其他構材以暫時固定。熱壓合溫度較佳為100~150℃的溫度範圍。且壓合時的壓力較佳為0.01~10MPa之範圍。時間較佳為1秒~數分鐘。熱壓合可在常壓下進行,為防止氣泡之進入等,亦可在真空中實施。
熱壓合後,施加120℃至400℃的溫度以成為硬化膜。此加熱處理係選擇溫度、進行階段性昇溫,或者選擇某溫度範圍連續地昇溫同時實施5分至5小時實施。其一例係在130℃、200℃各熱處理30分。或可舉出從室溫至250℃費2小時直線地進行昇溫等方法。此時,加熱溫度較佳為150℃以上300℃以下的溫度,更佳為180℃以上250℃以下。該加熱處理可在常壓下進行、亦可在真空中實施。
硬化後接著體的接著強度,從接著可靠性的觀點來看,宜為30MPa以上。更宜為45MPa以上。
硬化膜的膜厚雖可任意地設定,但較佳為0.5μm以上80μm以下。
接著,就本發明之感光性樹脂組成物及感光性樹脂組成物薄膜之用途,針對具有感光性樹脂組成物硬化膜之半導體裝置加以說明。又,近年來有提案各種構造之半導體裝置,本發明之感光性樹脂組成物的用途係不限定於下。
本發明之感光性樹脂組成物及感光性樹脂組成物薄膜可適合用於作為接著、固定或封裝半導體元件、半導體裝置、電路基板、金屬配線材料的半導體用接著劑。又,本發明之感光性樹脂組成物及感光性樹脂組成物薄膜亦可作為半導體元件、半導體裝置、電路基板等之絶緣膜使用。又,本發明所稱半導體裝置是指把半導體元件連接在基板上而成者,不只是連接半導體元件彼此或基板彼此者,而是指所有利用半導體元件之特性而可機能化之裝置,含電光學裝置、半導體電路基板及此等之電子構件係全部包括在半導體裝置中。
使用本發明之感光性樹脂組成物及感光性樹脂組成物薄膜的半導體裝置之製造方法的一例子係如下所述。使第一連接端子與第二連接端子相向,來配置具有第一連接端子的第一電路構材與具有第二連接端子的第二電路構材。接著,在前述相向配置的第一連接端子與第二連接端子之間隔著本發明之感光性樹脂組成物薄膜形成感光性樹脂組成物被膜。或在第一連接端子面或第二連接端子面的任一面或兩者上塗布感光性樹脂組成物的清漆並乾燥,藉此形成感光性樹脂組成物被膜。接著,將感光性樹脂組成物被膜圖案化,使第一連接端子與第二連接端子之欲導通的部分開口。然後,將第一電路構材與第二電路構材加熱加壓,以使此等電連接。
電連接可以首先在僅任一電路構材的連接端子側的面上形成上述感光性樹脂組成物被膜後而進行,也可在第一及第二電路構材的連接端子側的兩面上形成上述感光性樹脂組成物被膜後而進行。又,也可在第一電路構材及/或第二電路構材形成貫穿電極並在構材之單面及/或兩面上形成連接端子。就此種電路構材而言,可用形成有鍍覆凸塊或釘頭凸塊(stud bump)等凸塊之半導體晶片、電阻體晶片、電容器晶片等之晶片構件、具有TSV(through silicon via)電極之半導體晶片或矽插入物(silicon interposer)、環氧玻璃電路基板、薄膜電路基板等之基板等。藉由使用在兩面具有連接端子之電路構材而重複進行如上連接,能獲得電路構材為3維積層之半導體裝置。
在上述半導體裝置之製造方法中,藉由使用本發明之感光性樹脂組成物及感光性樹脂組成物薄膜,而可得硬化後的接著劑端部存在於比電路構材的端部更內側之半導體裝置,亦即,在加熱加壓第一電路構材與第二電路構材後,可獲得抑制接著劑朝電路構材外周滲出(修邊,fillet)發生的半導體裝置。藉由抑制修邊之發生,能減小半導體裝置之安裝面積,可提供半導體裝置之輕薄短小化。即使在不使用本發明之感光性樹脂組成物的情況下,藉由預先在電路構材的周邊部不形成樹脂組成物被膜,而能夠與上述同樣地抑制修邊之發生。然而,此方法係難以使位置吻合,再者,加工在1片晶圓時,非常難以在特定位置形成樹脂組成物被膜。相對於此,使用本發明之感光性樹脂組成物及感光性樹脂組成物薄膜的方法是利用圖案化除去電路構材周邊部的感光性樹脂組成物被膜,因而可容易獲得抑制修邊發生之半導體裝置。
抑制修邊發生之半導體裝置的製造方法之一例係如下所示。與上述半導體裝置之製造方法同樣地,在第一電路構材與第二電路構材之間形成感光性樹脂組成物被膜。接著,藉由將感光性樹脂組成物被膜圖案化,以除去第一電路構材及/或第二電路構材之周邊部的感光性樹脂組成物被膜。然後,加熱加壓第一電路構材與第二電路構材,以接著此等。其結果,可得感光性樹脂組成物被膜的硬化物不會從第一電路構材及第二電路構材滲出之半導體裝置。
又,關於其他用途,在形成有由光電二極體、彩色濾光片、微鏡片陣列所成之CCD或CMOS影像感應器的矽晶圓上,貼合感光性樹脂組成物薄膜、或塗布感光性樹脂組成物之清漆並乾燥,藉此形成感光性樹脂組成物被膜。將其圖案化後,在殘留圖案上積層作為支撐基板之玻璃基板並進行熱壓合。將其加熱以使感光性樹脂組成物被膜硬化。如此進行,將已圖案化之感光性樹脂組成物被膜的硬化物作為分隔壁而使半導體元件與玻璃基板接著,而可得具有中空構造之影像感應器。
以下,針對本發明之感光性樹脂組成物的調製方法、感光性樹脂組成物薄片之製造方法、及其物性評估方法與結果更具體地說明,惟本發明係不限於此等。
把聚醯亞胺溶解於NMP,而調製固體含量濃度0.1重量%之溶液,利用下示結構之GPC裝置Waters2690(Waters(股)製),算出聚苯乙烯換算之重量平均分子量。GPC測定條件為:移動層是以LiCl與磷酸各自濃度為0.05mol/L溶解之NMP、展開速度為0.4ml/分。又,管柱是用管柱烘箱加溫至40℃。
檢測器:Waters996
系統控制器:Waters2690
管柱:TOSOHTSK-GELα-4000
管柱:TOSOHTSK-GELα-2500
首先,測定聚醯亞胺之紅外吸收光譜,確認來自聚醯亞胺中之醯亞胺構造讀吸收波峰(1780cm-1
附近、1377cm-1
附近)存在。接著,對上述聚醯亞胺在350℃熱處理1小時後,再度測定紅外吸收光譜,比較熱處理前與熱處理後在1377cm-1
附近之波峰強度。把熱處理後之聚醯亞胺之醯亞胺化率設為100%,求出熱處理前之聚醯亞胺之醯亞胺化率。
用旋轉塗布機在矽晶圓上旋轉塗布各實施例及比較例所製作之感光性樹脂組成物。旋轉時間為10秒鐘、旋轉數係在500~700rpm左右調整,使得乾燥後膜厚成為約25μm。塗布後,在100℃之加熱板上乾燥3分鐘。
剝離各實施例及比較例所製作之感光性樹脂組成物薄膜的保護薄膜,且用層合裝置(Takatori(股)製、VTM-200M)、階段溫度80℃、輥溫度80℃、真空度150Pa、貼付速度5mm/秒、貼付壓力0.2Mpa之條件,將該剝離面層合在矽晶圓上,並剝離支撐體薄膜。
用具有L/S=70/70、60/60、50/50、40/40、30/30、25/25、20/20μm之圖案的遮罩,對旋轉塗布或層合後之矽晶圓進行圖案曝光。遮罩與感光性樹脂組成物薄膜之曝光間隙設為100μm,照射400mJ/cm2
(以h線之測光值)超高壓水銀燈之L39過濾器透射光。圖案曝光後,藉由浸漬顯影,用氫氧化四甲銨之2.38%水溶液除去曝光部,並以水進行清洗處理。顯影時間是設為完全溶解曝光部之時間的1.5倍。以光學顕微鏡觀察所得圖案,以圖案的線沒有阻塞等異常時的最小尺寸作為解析度之評估。
如上述般進行,對已在矽晶圓上進行層合或旋轉塗布之矽晶圓用超高壓水銀燈、以曝光量1000mJ/cm2
(以i線之測光值)進行曝光處理,然後藉由惰性烘箱(光洋THERMO SYSTEMS(股)製、INL-60)、N2
氣體環境下、以200℃熱處理60分鐘,而獲得硬化膜。把所得矽晶圓上的硬化膜用47%氟化氫酸在室溫下浸泡7分鐘後,以自來水洗淨,並從矽晶圓剝離硬化膜。將剝離之硬化膜用熱重量測定裝置(SII奈米科技(股)製、TG/DTA6200),在氮氣體環境下、以昇溫速度10℃/分之條件測定熱重量減少,將相對於測定開始時之重量而言重量減少1%時的溫度當作耐熱性指標。
對如上述在矽晶圓上進行層合或旋轉塗布後之矽晶圓以曝光量400mJ/cm2
(以h線之測光值)進行曝光。將曝光後之矽晶圓裁切成50×50mm,使感光性樹脂組成物薄膜在上方載置於150℃之加熱板上預加熱1分鐘後,將矽晶片(2×2mm、厚度525μm)以壓力0.2MPa熱壓合30秒鐘以暫時固定。然後,用氮氣體環境下之惰性烘箱在250℃以60分之條件進行熱硬化,在矽晶圓上隔著感光性樹脂組成物接著矽晶片而得樣品。依照以下條件測定該樣品之矽晶片的剪切強度,並當作接著強度。
裝置:Dage公司製晶圓剪切測試機系列4000
測定溫度:30℃
樣品尺寸:2mm×2mm
測試速度:200μm/s
測試高度:300μm
用KLA-Tencor公司製應力測定裝置FLX-2908,依照以下順序進行測定。首先,以應力測定裝置測定6吋矽晶圓之翹曲,在此晶圓依照上述順序層合感光性樹脂組成物薄膜或以旋轉塗布進行感光性樹脂組成物之塗布。用超高壓水銀燈、以曝光量1000mJ/cm2
(以i線之測光值)對此矽晶圓進行曝光處理後,藉由惰性烘箱(光洋THERMO SYSTEMS(股)製、INL-60)在N2
氣體環境下、在200℃熱處理60分鐘,以獲得硬化膜。再次以應力測定裝置測定硬化後的基板翹曲,由硬化膜形成前後之矽晶圓翹曲算出在室溫下之應力。
在各實施例及比較例所用之聚醯亞胺、醌二疊氮化合物係依照以下方法合成。
在乾燥氮氣流下,將16.41g(0.082莫耳)4,4’-二胺基二苯基醚(4,4’-DAE)、1.24g(0.005莫耳)1,3-雙(3-胺基丙基)四甲基二矽氧烷(SiDA)、作為末端封裝劑之2.73g(0.025莫耳)3-胺基苯酚(MAP)溶解在100gN-甲基-2-吡咯啶酮(NMP)中。於其中同時加入31.02g(0.1莫耳)4,4’-氧基二酞酸二酐(ODPA)與30g NMP,在20℃攪拌1小時,接著在50℃攪拌4小時。然後,在180℃攪拌5小時而得樹脂溶液。接著,將樹脂溶液投入3L的水中,並收集白色沈澱。將此沈澱過濾集中,以水洗淨3次後,以80℃之真空乾燥機乾燥5小時而得聚醯亞胺A。所得樹脂粉體之醯亞胺化率為95%。
在乾燥氮氣流下,將30.95g(0.0845莫耳)2,2-雙(3-胺基-4-羥基苯基)六氟丙烷(BAHF)、1.24g(0.005莫耳)SiDA溶解在100g NMP中。於其中同時加入31.02g(0.1莫耳)ODPA與30gNMP,在20℃攪拌1小時,接著在50℃攪拌4小時。於其中加入2.5g(0.02莫耳)MAP,在50℃攪拌2小時後,在180℃攪拌5小時而得樹脂溶液。接著,將樹脂溶液投入3L的水中,並收集白色沈澱。將此沈澱過濾集中,以水洗淨3次後,以80℃之真空乾燥機乾燥5小時而得聚醯亞胺B。所得樹脂粉體之醯亞胺化率為94%。
在乾燥氮氣流下,將30.03g(0.082莫耳)BAHF、1.24g(0.005莫耳)SiDA、作為末端封裝劑之3.13g(0.025莫耳)4-胺基硫苯酚溶解在100gNMP中。於其中同時加入29.42g(0.1莫耳)3,3’,4,4’-聯苯四羧酸二酐(BPDA)與30gNMP,在20℃攪拌1小時,接著在50℃攪拌4小時。然後,在180℃攪拌5小時而得樹脂溶液。接著,將樹脂溶液投入3L的水中,並收集白色沈澱。將此沈澱過濾集中,以水洗淨3次後,以80℃之真空乾燥機乾燥5小時而得聚醯亞胺C。所得樹脂粉體之醯亞胺化率為94%。
在乾燥氮氣流下,將30.03g(0.082莫耳)BAHF、1.24g(0.005莫耳)SiDA、作為末端封裝劑之4.1g(0.025莫耳)3-羥基酞酸酐溶解在100gNMP中。於其中同時加入31.02g(0.1莫耳)ODPA與30g NMP,在20℃攪拌1小時,接著在50℃攪拌4小時。然後,在180℃攪拌5小時。攪拌結束後,將溶液投入3L水中而獲得白色沈澱。將此沈澱過濾集中,以水洗淨3次後,以80℃之真空乾燥機乾燥5小時而得聚醯亞胺D。所得聚合物粉體之醯亞胺化率為96%。
在乾燥氮氣流下,將17.60g(0.088莫耳)4,4’-DAE、1.24g(0.005莫耳)SiDA及作為末端封裝劑之1.64g(0.015莫耳)MAP溶解在80gNMP中。於其中同時加入31.02g(0.1莫耳)ODPA與20gNMP,在20℃攪拌1小時,接著在50℃攪拌4小時。然後,添加15g二甲苯,邊使水與二甲苯同時共沸邊在180℃攪拌5小時。攪拌結束後,將溶液投入3L水中而獲得白色沈澱。將此沈澱過濾集中,以水洗淨3次後,以80℃之真空乾燥機乾燥20小時而得聚醯亞胺E。所得聚合物粉體之醯亞胺化率為95%。
在乾燥氮氣流下,將16.40g(0.082莫耳)4,4’-DAE、1.24g(0.005莫耳)SiDA、作為末端封裝劑之1.64g(0.025莫耳)MAP溶解在120gNMP。於其中同時加入31.02g(0.1莫耳)ODPA與30g NMP,在20℃攪拌1小時,接著在50℃攪拌4小時。然後,在180℃攪拌5小時而得樹脂溶液。接著,將樹脂溶液投入3L的水中,並收集白色沈澱。將此沈澱過濾集中,以水洗淨3次後,以80℃之真空乾燥機乾燥5小時而得聚醯亞胺F。所得樹脂粉體之醯亞胺化率為95%。
在乾燥氮氣流下,將16.41g(0.082莫耳)4,4’-二胺基二苯基醚(4,4’-DAE)、1.24g(0.005莫耳)1,3-雙(3-胺基丙基)四甲基二矽氧烷(SiDA)、作為末端封裝劑之2.73g(0.025莫耳)3-胺基苯酚(MAP)溶解在100gN-甲基-2-吡咯啶酮(NMP)中。於其中同時加入31.02g(0.1莫耳)4,4’-氧基二酞酸二酐(ODPA)與30gNMP,在20℃攪拌1小時,接著在50℃攪拌4小時。然後,在180℃攪拌2.5小時而得樹脂溶液。接著,將樹脂溶液投入3L的水中,並收集白色沈澱。將此沈澱過濾集中,以水洗淨3次後,以80℃之真空乾燥機乾燥3小時而得聚醯亞胺G。所得樹脂粉體之醯亞胺化率為83%。
在乾燥氮氣流下,將11.41g(0.057莫耳)4,4’-DAE、1.24g(0.005莫耳)SiDA及作為末端封裝劑之6.98g(0.075莫耳)苯胺溶解在80g NMP中。於其中同時加入、31.02g(0.1莫耳)ODPA與20gNMP,在20℃攪拌1小時,接著在50℃攪拌4小時。然後,在180℃攪拌5小時而得樹脂溶液。接著,將樹脂溶液投入3L的水中,並收集白色沈澱。將此沈澱過濾集中,以水洗淨3次後,以80℃之真空乾燥機乾燥5小時而得聚醯亞胺H。所得樹脂粉體之醯亞胺化率為95%。
在乾燥氮氣流下,將21.22g(0.05莫耳)TrisP-PA(商品名、本州化學工業(股)製)與26.8g(0.1莫耳)5-萘醌二疊氮磺酸氯化物(東洋合成(股)製、NAC-5)溶解在450g 1,4-二烷,並使成為室溫。於其中滴入與50gl,4-二烷混合之12.65g三乙胺,使系統內不得成為35℃以上。滴下後在40℃攪拌2小時。過濾三乙胺鹽,並將濾液投入水中。然後,過濾收集所析出之沈澱,進一步以1L之1%鹽酸水洗淨。然後,進一步以2L水洗淨2次。將該沈澱用真空乾燥機乾燥,獲得下述式所表示之醌二疊氮化合物A。
在乾燥氮氣流下,將12.25g(0.04莫耳)Phcc-AP(商品名、本州化學工業(股)製)與26.8g(0.1莫耳)5-萘醌二疊氮磺酸氯化物(東洋合成(股)製、NAC-5)溶解在450g 1,4-二烷中,使成為室溫。於其中滴入與50g1,4-二烷混合之12.65g三乙胺,使系統內不得成為35℃以上。滴在下後40℃攪拌2小時。過濾三乙胺鹽,並將濾液投入水中。然後,過濾收集所析出之沈澱,進一步以1L之1%鹽酸水洗淨。然後,進一步以2L水洗淨2次。將此沈澱以真空乾燥機乾燥,獲得下述式所表示之醌二疊氮化合物B。
在乾燥氮氣流下,將12.78g(0.056莫耳)雙酚A與26.8g(0.1莫耳)5-萘醌二疊氮磺酸氯化物(東洋合成(股)製、NAC-5)溶解在450g 1,4-二烷中,使其成為室溫。於其中滴入與50g1,4-二烷混合之12.65g三乙胺,使系統內不得成為35℃以上。滴下後在40℃攪拌2小時。過濾三乙胺鹽,並將濾液投入水中。然後,過濾收集所析出之沈澱進一步以1L之1%鹽酸水洗淨。然後,進一步以2L水洗淨2次。將此沈澱以真空乾燥機乾燥,獲得下述式所表示之醌二疊氮化合物C。
在500ml的燒瓶中裝入5g 2,2’-偶氮雙(異丁腈)、5g t-十二烷硫醇、150g丙二醇單甲基醚乙酸酯(以下簡稱為PGMEA)。然後,裝入30g甲基丙烯酸、35g甲基丙烯酸苄酯、35g八氫-1H-4,7-甲橋茚-5-基甲基丙烯酸酯,在室溫攪拌片刻,將燒瓶內進行氮取代後,在70℃加熱攪拌5小時。接著,於所得溶液添加15g甲基丙烯酸縮水甘油酯、1g二甲基苄胺、0.2g p-甲氧基苯酚,並在90℃加熱攪拌4小時,獲得丙烯酸樹脂溶液。所得丙烯酸樹脂溶液之固體含量濃度為43重量%,又,所得樹脂的重量平均分子量(Mw)為10600、酸價為118mgKOH/g。
將(a)10g合成例1所得之聚醯亞胺A、(b)2.0g OXT-191(商品名、東亞合成(股))、(c)2.0g醌二疊氮化合物A溶解在二丙酮醇/乳酸乙基=40/60之比率的溶媒中。溶媒之添加量是把溶媒以外之成分當作固體含量,將固體含量濃度調整成為45重量%。然後,以保留粒徑2μm之過濾器加壓過濾,獲得感光性樹脂組成物(表1)。
用逗點式輥塗布機塗布將所得感光性接著劑在厚度38μm之PET薄膜上,在75℃進行乾燥6分鐘後,層合作為保護薄膜之厚度10μm之PP薄膜,而獲得感光性樹脂組成物薄膜。進行塗覆使得感光性樹脂組成物薄膜的膜厚成為約25μm。用所得感光性接著劑薄膜如前述般進行解析度、耐熱性、接著強度及應力之評估。
與實施例1同樣地進行,以表1所示混合比製作感光性樹脂組成物薄膜,如前述般進行解析度、耐熱性、接著強度及應力之評估。
將實施例1之感光性樹脂組成物以上述方法旋轉塗布在矽晶圓上,以形成塗膜。用其進行解析度、耐熱性、接著強度及應力之評估。
將實施例3之感光性樹脂組成物以上述方法旋轉塗布在矽晶圓,以形成塗膜。用其進行解析度、耐熱性、接著強度及應力之評估。
與實施例1同樣地進行,以表2所示混合比製作感光性樹脂組成物薄膜,如前述般進行解析度、耐熱性、接著強度及應力之評估。
依表2記載的組成調製感光性樹脂組成物,與實施例1同樣地進行,試著形成感光性樹脂組成物薄膜,但由於膜太脆故在薄膜狀態發生龜裂,無法評估解析度、接著強度、應力。針對硬化後的膜,僅實施耐熱性評估。
將參考例1之感光性樹脂組成物以上述方法旋轉塗布在矽晶圓,以形成塗膜。用其進行解析度、耐熱性、接著強度及應力之評估。
在L/S=10μm/10μm的銅梳狀電極上利用真空層合貼合實施例2所得之感光性樹脂組成物薄膜。然後,以丙酮拭除電極部之被膜。接著,用超高壓水銀燈以曝光量1000mJ/cm2
(以i線之測光值)進行曝光處理後,用惰性烘箱、在N2
氣體環境下、以200℃熱處理60分鐘,製作評估用樣品。在溫度85℃、相對濕度85%之氣體環境下,於所得評估用樣品之電極間施加50V電壓進行持續1000小時之絶緣可靠性試験。電阻值是在1000小時為止持續保持在1010
Ω以上,所以絶緣可靠性為合格。銅梳狀電極係使用:在形成有厚度0.4μm之熱氧化膜與在其上之厚度0.8μm之氮化矽膜之矽晶圓上,將厚度0.08μm之鉻基底電極與其上厚度10μm之銅電極圖案加工而成者。
用第1圖說明本實施例。首先,在矽晶圓100上利用濺鍍形成作為密合層101之Ni層(10nm)與其上之作為導體層102的無電解銅鍍覆層(10μm)。
然後,在該基板上以旋轉塗布機旋轉塗布實施例2所得之感光性接著劑清漆,並乾燥,藉此形成感光性樹脂組成物被膜。然後,利用曝光、顯影在感光性樹脂組成物被膜上形成貫穿孔,並以惰性烘箱進行加熱處理,藉此進行感光性樹脂組成物被膜之硬化,而獲得具有貫穿孔層102之基板(第1圖(a))。
接著,在該基板上以旋轉塗布機旋轉塗布實施例2所得之感光性樹脂組成物清漆,並藉由乾燥、曝光、顯影形成配線孔層之圖案(空間部),以惰性烘箱進行加熱處理,而硬化配線孔層103,獲得具有貫穿孔/配線孔之基板(第1圖(b))。
接著,在該基板利用濺鍍形成作為密合層之Ni層(厚度10nm)後,進行電解銅鍍覆,將貫穿孔、配線孔以銅鍍覆料充填。然後,藉化學機械研磨(CMP)去除不要部分的銅鍍覆料,及進行絶緣膜表面之平坦化,獲得具有貫穿層/配線層104之基板(第1圖(c))。
然後,將上述方法之貫穿層/配線層的形成當作一個循環,重複3次,製作貫穿層、配線層分別積層4層之合計8層的多層配線基板。確認所製作之多層配線基板的絶緣層有無剝離或破裂等異常,但沒發現此等異常。又,用測試機確認所製作之多層配線基板的任意最外部配線層與最下層之導體層間的導通時,任一配線間皆有導通,及可確認沒有引起相鄰配線間之短路。
實施例及比較例所用之(b)化合物係如以下所示。
jER828:BisA型環氧基化合物(三菱化學(股)製)
OXT-191:氧雜環丁烷化合物(東亞合成(股)製)
EP4003S:環氧丙烷改性BisA型環氧樹脂(ADEKA(股)製)
jER152:苯酚酚醛清漆型環氧樹脂(三菱化學(股)製)
jER630:縮水甘油胺型環氧樹脂(三菱化學(股)製)
NC3000:聯苯型環氧樹脂(日本化藥(股)製)
“EPICLON(註冊商標)”850S:BisA型環氧樹脂(DIC(股)製)
根據本發明可得一種感光性樹脂組成物及感光性樹脂組成物薄膜,其係可藉由光蝕刻法形成正型圖案、硬化後的應力小、與可得半導體元件或支撐構材之高接著強度。
100...矽晶圓
101...密合層
102...導體層
103...貫穿孔層
104...配線孔層
105...貫穿層/配線層
第1圖(a)~(c)係用本發明之感光性樹脂組成物所作成之多層配線基板。
Claims (15)
- 一種感光性樹脂組成物,其特徵為含有(a)具有下述通式(1)所表示之結構單位且在主鏈末端之至少一側具有通式(2)及/或(3)所表示之構造的鹼可溶性聚醯亞胺、(b)在分子內具有2個以上的環氧基及/或氧雜環丁烷基(oxetanyl)之化合物、及(c)醌二疊氮化合物,且相對於100重量份(a)聚醯亞胺而言,(b)化合物的含量為20重量份以上,
- 如申請專利範圍第1項之感光性樹脂組成物,其中(b)為具有2個以上之環氧基之化合物。
- 如申請專利範圍第1或2項之感光性樹脂組成物,其中(a)之聚醯亞胺之醯亞胺化率為90%以上。
- 如申請專利範圍第1或2項之感光性樹脂組成物,其中相對於100重量份(a)之聚醯亞胺而言,(b)化合物的含量為40重量份以上。
- 如申請專利範圍第1或2項之感光性樹脂組成物,其進一步含有丙烯酸樹脂,其中相對於100重量份(a)之聚醯亞胺而言,所含丙烯酸樹脂的含量為小於10重量份。
- 一種感光性樹脂組成物薄膜,其特徵為含有(a)具有下述通式(1)所表示之結構單位且在主鏈末端之至少一側具有通式(2)及/或(3)所表示之構造的鹼可溶性聚醯亞胺、(b)在分子內具有2個以上的環氧基及/或氧雜環丁烷基之化合物、及(c)醌二疊氮化合物,且相對於100重量份(a)之聚醯亞胺而言,(b)化合物的含量為20重量份以上,
- 如申請專利範圍第6項之感光性樹脂組成物薄膜,其中(b)之化合物為在分子內具有2個以上之環氧基的化合物。
- 如申請專利範圍第6或7項之感光性樹脂組成物薄膜,其中相對於100重量份(a)之聚醯亞胺而言,(b)之 化合物的含量為40重量份以上。
- 如申請專利範圍第6或7項之感光性樹脂組成物薄膜,其進一步含有丙烯酸樹脂,其中相對於100重量份(a)之聚醯亞胺而言,所含丙烯酸樹脂的含量為小於10重量份。
- 一種積層體,其特徵為依序具有支撐體、如申請專利範圍第6至9項中任一項之感光性樹脂組成物薄膜及保護薄膜。
- 一種硬化物,其係如申請專利範圍第1至5項中任一項之感光性樹脂組成物或如申請專利範圍第6至9項中任一項之感光性樹脂組成物薄膜之硬化物。
- 一種半導體裝置,其具有如申請專利範圍第1至5項中任一項之感光性樹脂組成物或如申請專利範圍第6至9項中任一項之感光性樹脂組成物薄膜之硬化物。
- 一種半導體裝置,其係在電路構材之間具有如申請專利範圍第1至5項中任一項之感光性樹脂組成物或如申請專利範圍第6至9項中任一項之感光性樹脂組成物薄膜之硬化物,且該硬化物的端部是位於比電路構材之端部更為內側。
- 一種半導體裝置,其係在第1電路構材與第2電路構材之間隔著如申請專利範圍第1至5項中任一項之感光性樹脂組成物或如申請專利範圍第6至9項中任一項之感光性樹脂組成物薄膜,利用圖案化在所希望的位置開口後,藉由加熱加壓而將該第1電路構材與第2電路構材予以電連接而得之半導體裝置,其中該感光性樹脂組成物或感光性樹脂組成物薄膜的硬化物之端 部係位於比該第1電路構材及第2電路構材的端部更為內側。
- 一種半導體裝置之製造方法,其特徵為使第1電路構材與第2電路構材之間隔著如申請專利範圍第1至5項中任一項之感光性樹脂組成物或如申請專利範圍第6至9項中任一項之感光性樹脂組成物薄膜,藉由加熱加壓而將該第1電路構材與該第2電路構材予以電連接。
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