TWI833776B - 硬化性樹脂組成物及硬化性片材 - Google Patents
硬化性樹脂組成物及硬化性片材 Download PDFInfo
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- TWI833776B TWI833776B TW108124792A TW108124792A TWI833776B TW I833776 B TWI833776 B TW I833776B TW 108124792 A TW108124792 A TW 108124792A TW 108124792 A TW108124792 A TW 108124792A TW I833776 B TWI833776 B TW I833776B
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- epoxy resin
- curable
- resin composition
- curable resin
- resin
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- 125000000524 functional group Chemical group 0.000 claims abstract description 24
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- H01L21/04—Manufacture or treatment of semiconductor devices or of parts thereof the devices having potential barriers, e.g. a PN junction, depletion layer or carrier concentration layer
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Abstract
一種硬化性樹脂組成物,包含:第1環氧樹脂,其具有聚氧伸烷基鏈;第2環氧樹脂,其與前述第1環氧樹脂不同;熱塑性樹脂,其具有300,000以下之重量平均分子量且具有反應性官能基;選自於由硬化劑及硬化促進劑所構成群組中之至少一種;及無機充填劑。
Description
本發明是關於一種可經由熱等作用而硬化形成硬化物之硬化性樹脂組成物、及一種以硬化性樹脂組成物形成之硬化性片材,。
近年來,由於對半導體產品的薄型化、小型化的需求,所謂的晶圓級封裝(Wafer level package, WLP)之封裝技術倍受矚目。密封這種配備電路構件之安裝基板(亦稱作電路基板)時,會有使用片狀、粒子狀或液狀等密封材的情形。該等密封材可使用例如因熱等作用硬化之硬化性樹脂組成物。例如,於日本專利文獻1中,提案一種使用了含環氧樹脂之熱硬化性組成物的密封用片材。
先前技術文獻
專利文獻
專利文獻1:日本專利特開2016-175972號公報
發明欲解決之課題
例如,以密封用片材密封電路基板等基板時,係使片材密著於基板上後硬化。由於密封材之硬化物與基板之線膨脹係數不同,硬化物與基板的積層體容易產生翹曲。因對硬化物會要求一定程度的強度,若將硬化物之強度提高,彈性也會變高,積層體的翹曲會變大。抑制翹曲與確保強度間有消長關係,很難同時兼顧。
用以解決課題之手段
本發明的一態樣,是有關於一種硬化性樹脂組成物,包含:第1環氧樹脂,其具有聚氧伸烷基鏈;第2環氧樹脂,其與前述第1環氧樹脂不同;熱塑性樹脂,其具有300,000以下之重量平均分子量且具有反應性官能基;選自於由硬化劑及硬化促進劑所構成群組中之至少一種;及無機充填劑。
本發明的另一態樣,是有關於一種硬化性片材,係以前述之硬化性樹脂組成物所形成。
發明效果
根據本發明前述態樣,可提供一種既能確保硬化物強度同時還可抑制硬化物層與基板之積層體的翹曲之硬化性樹脂組成物及硬化性片材。
本發明之新穎特徵雖記述於附加的申請專利範圍內,但關於本發明之結構與內容兩方面,併同本發明之其他目的及特徵,藉由以下參酌圖式之詳細說明應可更加理解。
關於本發明一態樣之硬化性樹脂組成物,包含:第1環氧樹脂,其具有聚氧伸烷基鏈;第2環氧樹脂,其與前述第1環氧樹脂不同;熱塑性樹脂,其具有300,000以下之重量平均分子量且具有反應性官能基;選自於由硬化劑及硬化促進劑所構成群組中之至少一種;及無機充填劑。
在以硬化性樹脂組成物密封基板(電路基板等)的情況下,由於硬化性樹脂組成物與基板之線膨脹係數不同,在使硬化性樹脂組成物硬化時,容易於硬化性樹脂組成物與基板之積層體發生翹曲。特別是在密封大面積基板的情況下,會發生很大的翹曲。若產生翹曲會於之後的研磨步驟或單片化步驟中產生問題,故防止翹曲便成為很大的技術課題。例如,在將硬化性樹脂組成物所構成之片材利用於密封電路基板等基板的情況下,係藉由密著於基板上並硬化來進行基板之密封。就片材而言,特別容易在片材與基板之積層體發生翹曲。此外,對於硬化性樹脂組成物或片材會要求與基板之密著時或硬化後有一定程度的強度,若提高片材或硬化物的強度,則彈性也會提高,積層體的翹曲會變大。再者,一旦產生翹曲也會很難鬆弛。即使混合強度優異的材料與低彈性的材料,該等相反的特性還是很難同時兼顧。
根據本發明的前述態樣,藉由使用第1環氧樹脂與第2環氧樹脂,即可兼顧硬化物之強度與低彈性(或柔軟性)。此外,在使用第1環氧樹脂的同時,可使熱塑性樹脂以分散於第1及第2環氧樹脂附近之狀態共存,故能提高硬化物的柔軟性,並可確保較高的應力鬆弛性。因而認為可在硬化物剛硬化後減少硬化物與基板之積層體的翹曲。此外,由於能鬆弛應力,即使一時間產生翹曲,只要暫時靜置,便能鬆弛翹曲。
在此,本說明書中,所謂的基板指的是具備電子零件之基板、電子零件的集合體或電子零件本身。
在本發明的一態樣,亦包含以前述硬化性樹脂組成物形成之硬化性片材。若使用硬化性片材,既確保硬化物之高強度,且即使與基板等之線膨脹係數不同之構件作積層,還是能夠減少積層體的翹曲。此外,還可鬆弛已產生的翹曲。
以下,將更具體地說明硬化性樹脂組成物及硬化性片材之構成。
(硬化性樹脂組成物)
硬化性樹脂組成物包含第1環氧樹脂、第2環氧樹脂、前述熱塑性樹脂、硬化劑及/或硬化促進劑以及無機充填劑。在此,本說明書中,第1環氧樹脂、第2環氧樹脂及前述熱塑性樹脂一併(在使用其他樹脂的情況下也包括該樹脂)稱作硬化性樹脂。在此,前述態樣之硬化性樹脂是在加熱下硬化性樹脂會硬化之熱硬化性樹脂組成物。
硬化性樹脂組成物可為液狀、片狀、或是顆粒狀,亦可為半硬化狀態(所謂的B階段)。
(第1環氧樹脂)
第1環氧樹脂具有聚氧伸烷基鏈。藉由使用第1環氧樹脂及第2環氧樹脂,既可由第2環氧樹脂確保一定程度的強度,亦可由第1環氧樹脂確保柔軟性,並能鬆弛應力。第1環氧樹脂可於側鏈具有聚氧伸烷基鏈,但宜於主鏈具有聚氧伸烷基鏈。使用主鏈有聚氧伸烷基鏈的第1環氧樹脂,則容易確保高柔軟性,能進一步提高應力鬆弛性。
包含於聚氧伸烷基鏈上之伸烷基的碳數為例如2以上,宜為3以上,較佳為4以上。從較容易形成第1環氧樹脂與第2環氧樹脂之良好相分離狀態的觀點來看,伸烷基的碳數宜為4以上。從容易確保較高柔軟性的觀點來看,伸烷基的碳數宜設為16以下,較佳設為10以下或6以下。該等下限值與上限值可作任意組合。
伸烷基的碳數可為例如2~16、2~10、2~6、3~16、3~10、3~6、4~16、4~10或4~6。
伸烷基之具體例可舉例如:伸乙基、伸丙基、三亞甲基、伸丁基(1,2-伸丁基、1,3-伸丁基、1,4-伸丁基(或四亞甲基)等)、六亞甲基、八亞甲基及十亞甲基等。
伸烷基可為直鏈狀亦可為支鏈狀,但若以容易確保高度柔軟性的觀點來看,宜為直鏈狀。
於聚氧伸烷基鏈中氧伸烷基單元之重複數n為例如3以上,較佳為4以上或5以上,可為6以上或7以上,亦可設為8以上。重複數n在該範圍內時,既確保第1環氧樹脂與第2環氧樹脂良好的相分離狀態,亦容易提高柔軟性。因此可進一步提高應力鬆弛效果。從容易分散第1環氧樹脂、容易得到高應力鬆弛效果的觀點來看,氧伸烷基單元之重複數n為例如200以下,宜為100以下,可設為70以下,亦可設為30以下。該等下限值與上限值可作任意組合。
氧伸烷基單元之重複數n可為例如3~200、3~100、3~70、3~30、4~70、4~30、5~70、5~30、6~70、6~30、7~70或7~30等。
聚氧伸烷基鏈可具有一種氧伸烷基單元,亦可具有複數種種類不同之氧伸烷基單元。在第1環氧樹脂於具有複數種種類不同之氧伸烷基單元的情況下,各氧伸烷基單元之合計宜滿足前述重複數n的範圍。例如第1環氧樹脂具有一條依序鍵結有氧伸乙基單元、氧四亞甲基單元、氧伸丙基單元及氧四亞甲基單元各一個之鏈時,設定氧伸烷基單元之重複數n為4。又,在第1環氧樹脂具有非直接連結之複數個聚氧伸烷基鏈的情況下、及具有氧伸烷基單元互異之複數個聚氧伸烷基鏈的情況下,於各聚氧伸烷基鏈上之氧伸烷基單元重複數之合計宜滿足前述重複數n的範圍。在第1環氧樹脂具有複數個種類不同之氧伸烷基單元的情況下,可為聚氧伸烷基鏈上有種類不同之氧伸烷基單元無規配置的無規型,亦可為聚氧伸烷基鏈上有複數個種類不同之嵌段狀聚氧伸烷基鏈相連的嵌段型。
第1環氧樹脂只要具有聚氧伸烷基鏈,其種類沒有特別限定,環氧丙基醚型、環氧丙基酯型、環氧丙基胺型、脂環式環氧化合物等任一種均可。從容易取得的觀點來看,會使用具有聚氧伸烷基鏈的環氧丙基醚(具體為聚伸烷基二醇環氧丙基醚)等。
作為環氧丙基醚型之第1環氧樹脂可舉例如:聚乙二醇二環氧丙基醚、聚丙二醇二環氧丙基醚、聚三亞甲基二醇二環氧丙基醚、聚丁二醇二環氧丙基醚、聚六亞甲基二醇二環氧丙基醚及聚乙二醇聚丙二醇二環氧丙基醚等。
又,作為環氧丙基醚型之第1環氧樹脂,亦可使用多元醇之環氧烷加成物的環氧丙基醚。環氧烷加成的部分,相當於前述之聚氧伸烷基鏈。多元醇可列舉芳香族多元醇、脂環式多元醇等。芳香族多元醇可舉例如雙酚類(雙酚A、雙酚F、雙酚S等)。脂環式多元醇可舉例如芳香族多元醇的氫化物。
第1環氧樹脂可單獨使用一種,亦可二種以上作組合使用。
第1環氧樹脂之環氧當量可為例如200g/eq以上且800g/eq以下。環氧當量在該範圍內時,則容易與第2環氧樹脂形成相分離狀態,並可得到良好之應力鬆弛性。
第1環氧樹脂之漢森溶解度參數(HSP)值與第2環氧樹脂之HSP値的差為例如6以上,可為7以上,宜為9以上或10以上,更佳為11以上。HSP值的差在該範圍內時,則於硬化性樹脂組成物中較容易形成良好的相分離狀態,並可得到較高之應力鬆弛效果。從容易維持合適的相分離狀態的觀點來看,該等樹脂之HSP值的差為例如15以下。
在此,HSP是以分散項δD、極性項δP及氫鍵項δH三種參數表現物質溶解性的值。分散項δD、極性項δP及氫鍵項δH是物質固有的物性值,揭示於文獻例如「Hansen Solubility Parameters: A User’s Handbook, HSPiP 3rd
Edition ver.3.0.20」。在此,氫鍵項δH雖然可以使用前述文獻中記載的值,在沒有記載的情況下,可經由稱作Y-MB法之使用神經網絡方法的推算方法將氫鍵項δH算出。
(第2環氧樹脂)
第2環氧樹脂只要為與第1環氧樹脂不同之環氧樹脂即可。例如使用不具有聚氧伸烷基鏈之環氧樹脂作為第2環氧樹脂。第2環氧樹脂可使用在25℃下呈液狀、固體狀及半固形者等中之任一種。第2環氧樹脂可單獨使用一種,亦可二種以上組合使用。
(環氧樹脂2A)
第2環氧樹脂宜包含例如具有50℃以上玻璃轉移溫度(Tg)之環氧樹脂(稱作環氧樹脂2A)。使用此種環氧樹脂2A,可進一步提高硬化性樹脂組成物之硬化物的強度。環氧樹脂2A的Tg宜為50℃以上,亦可為100℃以上。Tg在該範圍內時,則容易賦予硬化物高強度。從容易取得與第1環氧樹脂之相分離結構之平衡的觀點來看,環氧樹脂2A的Tg為例如230℃以下。
此外,環氧樹脂2A的Tg是環氧樹脂2A之硬化物的Tg。環氧樹脂2A之硬化物的Tg,可使用以等量包含環氧樹脂2A與作為硬化劑的苯酚酚醛型樹脂之混合物製作2mm厚的膜且於175℃下硬化3小時製成樣品然後使用該樣品來作測定。使用該樣品,經由使用市售之動態黏彈性測定裝置的動態黏彈性測定(DMA),於頻率1Hz下一邊改變溫度一邊測定損耗正切tanδ,並將tanδ達頂峰的溫度設為Tg。
環氧樹脂2A之種類沒有特別限定。從容易確保硬化性的觀點來看,宜至少使用具有2個以上之環氧基的環氧樹脂。此外,從容易形成良好之相分離結構的觀點來看,宜為每分子平均環氧官能基數大於2之多官能環氧樹脂。每分子平均環氧官能基數大於2之多官能環氧樹脂,例如除了3官能以上之多官能環氧樹脂以外,亦包含混合3官能以上之多官能環氧樹脂與小於3官能之環氧樹脂(例如具有1個環氧基之單官能環氧樹脂及/或2官能環氧樹脂)這類的材料。又視其需要,可單獨使用單官能環氧樹脂,亦可併用單官能環氧樹脂與其他環氧樹脂。
環氧樹脂2A可使用例如:雙酚型環氧樹脂(例如雙酚A型環氧樹脂、雙酚F型環氧樹脂、雙酚AD型環氧樹脂、雙酚S型環氧樹脂等)、雙酚型環氧樹脂經部分縮合之寡聚物混合物、聯苯型環氧樹脂(例如3,3’,5,5’-四甲基-4,4’-雙(環氧丙氧基)-1,1’-聯苯、3,3’,5,5’-四第三丁基-4,4’-雙 (環氧丙氧基)-1,1’-聯苯、4,4’-雙(環氧丙氧基)聯苯、3,3’–二甲基-4,4’-雙 (環氧丙氧基)聯苯等在聯苯環上可具有取代基(烷基(甲基、丁基等之C1-4
烷基等)等)之聯苯型環氧樹脂等)、酚醛型環氧樹脂(苯酚酚醛型環氧樹脂、三苯甲烷酚醛型環氧樹脂等)、茀型環氧樹脂(雙酚茀型環氧樹脂、雙甲酚茀型環氧樹脂等)、萘型環氧樹脂(1,6-雙(2,3-環氧丙氧基)萘等)、酚型環氧樹脂(鄰苯二酚二環氧丙基醚、間苯二酚二環氧丙基醚等)、酮型芳香族環氧樹脂(2,4-雙(環氧丙氧基)二苯基酮、4,4’-雙(環氧丙氧基)二苯基酮等)、或該等之加氫物(例如氫化雙酚A型環氧樹脂、氫化雙酚F型環氧樹脂、氫化雙酚S型環氧樹脂等)、醌型環氧樹脂(2,5-二異丙基氫醌二環氧丙基醚、氫醌二環氧丙基醚等)、脂環式環氧樹脂(例如二環氧薴烯)、二環戊二烯型環氧樹脂、環氧丙基酯型環氧樹脂、環氧丙基胺型環氧樹脂、乙炔脲型環氧樹脂(例如具有乙炔脲骨架之環氧樹脂)、酚酞型環氧樹脂等。環氧樹脂2A可為預聚物,亦可為聚醚改質環氧樹脂、聚矽氧改質環氧樹脂之類的環氧樹脂與其他聚合物之共聚物。環氧樹脂2A可單獨使用一種,亦可二種以上組合使用。
環氧丙基酯型環氧樹脂可舉例如:有機羧酸類之環氧丙基酯等(芳香族多羧酸之環氧丙基酯(鄰苯二甲酸二環氧丙基酯等)等)。環氧丙基胺型環氧樹脂可舉例如:胺苯酚型環氧樹脂(對胺苯酚型環氧樹脂(三環氧丙基-對胺苯酚等)等)、苯胺型環氧樹脂(二環氧丙基苯胺、4,4’-亞甲基雙[N,N-雙(環氧乙烷基甲基)苯胺]等)、甲苯胺型環氧樹脂(二環氧丙基鄰甲苯胺等)、二胺基二苯基甲烷型環氧樹脂(四環氧丙基二胺基二苯基甲烷等)、含氮雜環式環氧樹脂(異三聚氰酸三環氧丙基酯等)等。
從容易確保強度的觀點來看,環氧樹脂2A中,宜使用包含選自於由芳香環及5員環以上之雜環所構成群組中之至少一種環結構的環氧樹脂或其氫化物。從容易形成相分離結構的觀點來看,以雙酚型環氧樹脂(雙酚S型環氧樹脂等)、含氮雜環之環氧丙基胺等為佳。又,亦可併用環氧丙基胺型環氧樹脂與雙酚型環氧樹脂。在此情況下,能夠提升與被附著物(基板等)間之密著性。此外,從耐熱性和耐水性佳、便宜又經濟等觀點來看,宜為雙酚型環氧樹脂(雙酚A型環氧樹脂、雙酚F型環氧樹脂等)。又從耐溼性的觀點來看,宜為萘型環氧樹脂。
環氧樹脂2A之環氧當量宜為例如50g/eq以上且500g/eq以下。環氧當量在該範圍內時,容易得到高強度,並容易調節Tg。
(環氧樹脂2B)
第2環氧樹脂視需要可包含環氧樹脂2A以外的環氧樹脂(環氧樹脂2B)。環氧樹脂2B沒有特別限制,可為多官能,亦可為單官能。環氧樹脂2B的種類也沒有特別限制,可為環氧丙基醚型環氧樹脂、環氧丙基酯型環氧樹脂、環氧丙基胺型環氧樹脂及脂環式環氧樹脂中之任一種。環氧樹脂2B可單獨使用一種,亦可二種以上組合使用。
從調節硬化性樹脂組成物黏度的觀點來看,可與單官能環氧樹脂併用。所述單官能之環氧樹脂可舉例如:苯基環氧丙基醚、2-乙基己基環氧丙基醚、二環戊二烯環氧丙基醚及2-羥乙基環氧丙基醚等。
第1環氧樹脂與第2環氧樹脂之質量比為例如5:95~70:30,可為5:95~50:50、亦可為10:90~40/60或10:90~30:70。第1環氧樹脂與第2環氧樹脂之質量比在該範圍內時,則容易取得強度與柔軟性的平衡。
第1環氧樹脂與環氧樹脂2A於硬化性樹脂組成物所含環氧樹脂總量中所佔之合計比率例如為90質量%以上,亦可為95質量%以上。又,硬化性樹脂組成物所含之環氧樹脂,亦可只由第1環氧樹脂及環氧樹脂2A構成。在第1環氧樹脂及環氧樹脂2A之比率如此多的情況下,更容易確保因形成良好的相分離狀態所致之應力鬆弛效果。
(熱塑性樹脂)
作為熱塑性樹脂(第1熱塑性樹脂),只要是重量平均分子量(Mw)為300,000以下且具有反應性官能基者,則沒有特別限制,各種熱塑性樹脂皆可使用。
熱塑性樹脂之重量平均分子量(Mw)為300,000以下即可,宜為200,000以下、更佳為150,000以下或100,000以下。熱塑性樹脂之Mw在此範圍時,熱塑性樹脂之分散性提升,更容易得到高的應力鬆弛性。Mw宜為例如5,000以上。熱塑性樹脂之Mw在此範圍時,由於容易降低硬化物之彈性,故可更加提升抑制翹曲的效果。
另外,本說明書中,重量平均分子量Mw是使用凝膠滲透層析術(GPC)測定之聚苯乙烯換算的重量平均分子量。
熱塑性樹脂之Mw係依例如以下的順序求得。
將熱塑性樹脂溶解於溶劑中以調製測定用樣品。溶劑係對應熱塑性樹脂之種類自可溶解熱塑性樹脂的液狀溶劑中選擇。使用測定用樣品於下述條件下進行GPC測定,求出Mw。
裝置:SHODEX公司製、SYSTEM-21H
偵測器:RI偵測器
移動相:四氫呋喃
流量:1mL/分鐘
管柱:SHODEX公司製、KD-806M(×3支)
管柱溫度:40℃
基準物質:標準聚苯乙烯(Mw=3900000、650000、65000、5780、589)
另外,Mw通常是針對使用於硬化性樹脂組成物之熱塑性樹脂原料來測定。但在原料難以取得時,藉由眾所周知的分離方法及純化方法等將熱塑性樹脂從硬化性樹脂組成物中分離求出Mw即可。
熱塑性樹脂所具有之反應性官能基可例示如:環氧基、羧基、羥基、胺基(也包含亞胺基)、醯胺基、腈基、具有聚合性碳-碳不飽和鍵的基(例如乙烯基、烯丙基、丙烯醯基、甲基丙烯醯基等)等。熱塑性樹脂可具有該等反應性官能基之其中一種,亦可具有二種以上。熱塑性樹脂宜至少具有環氧基作為反應性官能基。在此情況下,能確保對第1環氧樹脂及第2環氧樹脂有適度的親和性。因此,熱塑性樹脂之分散性提升,可更加提高應力鬆弛性。熱塑性樹脂可為分子內具有1個反應性官能基之單官能聚合物,亦可為具有2個以上反應性官能基之多官能聚合物。
熱塑性樹脂在25℃下的性狀亦無特別限制,可使用在25℃下呈固體狀(例如橡膠狀、顆粒狀等)或液狀等各種性狀者。從容易確保較高柔軟性的觀點來看,熱塑性樹脂可使用於25℃下具有橡膠般彈性之高分子材料(包含橡膠)。熱塑性樹脂之Tg宜為40℃以下,且宜為25℃以下。熱塑性樹脂Tg之測定與環氧樹脂2A之Tg測定方式相同。
熱塑性樹脂可舉例如:二烯系熱塑性樹脂(異戊二烯橡膠、丁二烯橡膠、苯乙烯-丁二烯橡膠、氯丁二烯橡膠等)、丙烯酸系熱塑性樹脂(丙烯酸橡膠等)、腈系熱塑性樹脂(腈橡膠等)、胺甲酸乙酯系熱塑性樹脂(胺甲酸乙酯橡膠等)、聚矽氧系熱塑性樹脂(聚矽氧橡膠、環氧改質聚矽氧等)、聚酯系熱塑性樹脂(結晶性聚酯、非晶性聚酯、聚酯彈性體等)、聚醯胺系熱塑性樹脂(聚醚酯醯胺、聚醯胺彈性體等)、丁基橡膠、乙烯-丙烯橡膠等。聚矽氧系熱塑性樹脂於室溫(例如20~35℃)下可呈固體狀或液狀。聚矽氧油亦包含於前述聚矽氧系熱塑性樹脂。但,該等熱塑性樹脂不過是單純例示,並非以該等為限。
熱塑性樹脂可單獨使用一種,亦可二種以上組合使用。組合二種以上之熱塑性樹脂時,亦可組合反應性官能基數、反應性官能基種類及/或分類(例如二烯系、丙烯酸系等)等相異之二種以上熱塑性樹脂。
從容易控制分子量與分子量分布、亦容易導入反應性官能基且容易分散於硬化性樹脂組成物中的觀點來看,可使用丙烯酸系熱塑性樹脂。其中,對於片狀之硬化性樹脂組成物而言,使用丙烯酸系熱塑性樹脂較有利。又,亦可組合丙烯酸系熱塑性樹脂與其他熱塑性樹脂(例如腈系熱塑性樹脂、聚矽氧系熱塑性樹脂及/或二烯系熱塑性樹脂等)。
於丙烯酸系熱塑性樹脂(丙烯酸橡膠等)中,包含:含有具反應性官能基之單體單元(第1單體單元)與(甲基)丙烯酸酯單元(第2單體單元)等的熱塑性樹脂。丙烯酸系熱塑性樹脂視需要可包含該等單體單元以外之第3單體單元。另外,也有將丙烯酸酯(acrylate)(或丙烯酸酯(acrylic ester)與甲基丙烯酸酯(methacrylate)(或甲基丙烯酸酯(methacrylic ester))合併記載成(甲基)丙烯酸酯的情形。
(甲基)丙烯酸酯單元可舉例如(甲基)丙烯酸烷基酯單元等。(甲基)丙烯酸烷基酯單元可例示為:(甲基)丙烯酸C1-6
烷基酯單元((甲基)丙烯酸乙酯單元、(甲基)丙烯酸丙酯單元、(甲基)丙烯酸丁酯單元等),亦可為(甲基)丙烯酸C1-4
烷基酯單元。丙烯酸系聚合物可包含一種第2單體單元,亦可含二種以上第2單體單元。
第1單體單元可舉例如:和具有反應性官能基與聚合性碳-碳不飽和鍵(乙烯基、烯丙基、丙烯醯基、甲基丙烯醯基等)之單體相對應的單元。另外,反應性官能基為具有聚合性碳-碳不飽和鍵之基團時,為了形成在導入熱塑性樹脂後殘留未反應之反應性官能基的狀態,而利用多官能單體。若考慮與第2單體單元之聚合性,第1單體單元宜使用和具有丙烯醯基及/或甲基丙烯醯基之丙烯酸系單體相對應的單體單元。具有環氧基作為反應性官能基之丙烯酸系單體單元可舉例如(甲基)丙烯酸環氧丙酯單元等。丙烯酸系聚合物可包含一種第1單體單元,亦可包含二種以上第1單體單元。
第3單體單元沒有特別限制,可舉例如:氰乙烯(vinyl cyanide)單元(丙烯腈(acrylonitrile)單元等)、乙烯醚單元(2-氯乙基乙烯基醚單元等)、烯烴單元(乙烯單元等)等。丙烯酸系聚合物可包含一種第3單體單元,亦可包含二種以上第3單體單元。
又,亦宜使用聚矽氧系熱塑性樹脂。其中,對於液狀的硬化性樹脂組成物來說,使用聚矽氧系熱塑性樹脂會較有利。
相對於第1環氧樹脂及第2環氧樹脂之總量100質量份,熱塑性樹脂的量例如為5質量份以上,宜為10質量份以上或50質量份以上,亦可為100質量份以上。藉由熱塑性樹脂的量在此範圍,容易降低硬化物的彈性,較容易鬆弛翹曲。熱塑性樹脂的量例如為400質量份以下,也可為300質量份以下。在此情形下,較容易確保硬化物的強度。可將這些下限値與上限値任意作組合。片狀的硬化性樹脂組成物中,熱塑性樹脂的量宜為50質量份以上。液狀的硬化性樹脂組成物中,熱塑性樹脂的量可為150質量份以下,也可為100質量份以下,亦可為50質量份以下或40質量份以下。
相對於第1環氧樹脂及第2環氧樹脂之總量100質量份,熱塑性樹脂的量可為例如:5質量份以上且400質量份以下(或300質量份以下)、10質量份以上且400質量份以下(或300質量份以下)、50質量份以上且400質量份以下(或300質量份以下)、100質量份以上且400質量份以下(或300質量份以下)、5質量份以上且150質量份以下(或100質量份以下)、10質量份以上且150質量份以下(或100質量份以下)、50質量份以上且150質量份以下(或100質量份以下)、5質量份以上且50質量份以下(或40質量份以下)或是10質量份以上且50質量份以下(或40質量份以下)。
(硬化劑及硬化促進劑)
硬化性樹脂組成物包含硬化劑及/或硬化促進劑。硬化劑為能使前述環氧樹脂硬化及/或使前述熱塑性樹脂反應即可。硬化促進劑只要能促進前述環氧樹脂硬化及/或能促進前述熱塑性樹脂反應者即可。硬化劑及硬化促進劑各自在25℃下為固體時,宜分別使用例如熔點在30~130℃者。
硬化劑可使用酸酐、苯酚樹脂、胺化合物等。
酸酐沒有特別限定,可舉例如:酞酐、六氫酞酐、烷基六氫酞酐(例如甲基六氫酞酐)、四氫酞酐、烷基四氫酞酐(例如3-甲基四氫酞酐)、三烷基四氫酞酐、納迪克酸酐(himic anhydride)、丁二酸酐、甲基納迪克酸酐(methylnadic anhydride)、偏苯三甲酸酐、焦蜜石酸酐、甲基降莰烯-2,3-二羧基酸等。該等可單獨使用一種,亦可二種以上組合使用。
苯酚樹脂(酚系硬化劑)沒有特別限定,宜為苯酚酚醛樹脂。苯酚酚醛樹脂可為苯酚類或萘酚類(例如苯酚、甲酚、萘酚、烷基酚、雙酚、萜烯酚、萘酚等)與甲醛之縮合聚合物。更具體可舉如:苯酚酚醛樹脂、烷基酚酚醛樹脂(甲酚酚醛樹脂、丁基酚酚醛樹脂等)、聯苯苯酚酚醛樹脂、萜烯酚酚醛樹脂、α-萘酚酚醛樹脂、β-萘酚酚醛樹脂、二環戊二烯甲酚、聚對乙烯基苯酚、雙酚A型酚醛樹脂、伸茬基改質酚醛樹脂、十氫萘改質酚醛樹脂、聚(二-鄰羥苯基)甲烷、聚(二-間羥苯基)甲烷、聚(二-對羥苯基)甲烷等。該等中從耐水性的觀點來看宜為萘酚酚醛樹脂。該等可單獨使用一種,亦可二種以上組合使用。
胺化合物沒有特別限定,可使用例如:四甲基二胺基二苯基甲烷、四乙基二胺基二苯基甲烷、二乙基二甲基二胺基二苯基甲烷、二甲基二胺基甲苯、二胺基二丁基甲苯、二胺基二丙基甲苯、二胺基二苯基碸、二胺基二甲苯基碸、二乙基二胺基甲苯、雙(4-胺基-3-乙基苯基)甲烷、聚氧化四亞甲基-二-對胺基苯甲酸酯等。該等可單獨使用一種,亦可二種以上組合使用。
硬化劑宜使用會讓硬化劑官能基之當量數相對於環氧基1當量為0.05~1.5當量(例如0.1~1.5當量)、更佳為0.1~1.2當量的量。藉此,環氧樹脂組成物之硬化性會提升,硬化物的強度會提升。
硬化促進劑沒有特別限定,可舉如:咪唑系硬化促進劑、磷系硬化促進劑(磷系觸媒等)、胺系硬化促進劑、有機金屬化合物、鏻鹽系硬化促進劑、雙環式脒類與其衍生物、有機金屬化合物或有機金屬錯合物、多胺之脲化合物等。硬化促進劑宜具有潛伏性。潛伏性硬化促進劑可舉例如:咪唑系促進劑、磷系促進劑、胺系硬化促進劑、微膠囊型硬化促進劑等。使用硬化促進劑時,摻混量宜相對於硬化性樹脂100質量份為0.1~40質量份,較佳為1~30質量份。
咪唑系硬化促進劑可舉如:咪唑、2-取代咪唑化合物(2-甲基咪唑、2-乙基咪唑、1-異丁基-2-甲基咪唑、2-乙基-4-甲基咪唑、2-苯基咪唑、2-苯基-4-甲基咪唑、1-苯甲基-2-甲基咪唑、1-苯甲基-2-苯基咪唑、1,2-二甲基咪唑、1-氰乙基-2-甲基咪唑、1-氰乙基-2-乙基-4-甲基咪唑、1-氰乙基-2-十一基咪唑、1-氰乙基-2-苯基咪唑等)、偏苯三甲酸鹽(1-氰乙基-2-十一基咪唑鎓偏苯三甲酸鹽、1-氰乙基-2-苯基咪唑鎓偏苯三甲酸鹽等)、三加成物(2,4-二胺基-6-[2’-甲基咪唑基-(1’)]-乙基-對稱三、2,4-二胺基-6-[2’-十一基咪唑基-(1’)]-乙基-對稱三、2,4-二胺基-6-[2’-甲基-4’-甲基咪唑基-(1’)]-乙基-對稱三等)、2,4-二胺基-6-[2’-甲基咪唑基-(1’)]-乙基-對稱三異三聚氰酸加成物、2-苯基咪唑異三聚氰酸加成物、2-甲基咪唑異三聚氰酸加成物、2-苯基-4,5-羥甲基咪唑及2-苯基-4-甲基-5-二羥甲基咪唑。
磷系硬化促進劑可舉如:三烷基膦化合物(三丁基膦等)、三芳基膦化合物(三苯基膦等)。
胺系硬化促進劑可舉如:2,4,6-參(二甲基胺甲基)酚、二乙基胺、三乙基胺、二伸乙四胺、三伸乙四胺及4,4-二甲基胺吡啶等。胺系硬化促進劑亦可為胺加成物。
有機金屬化合物或有機金屬錯合物可舉如:環烷酸鋅、環烷酸鈷、辛酸錫、辛酸鈷、雙乙醯丙酮鈷(II)及參乙醯丙酮鈷(III)等。
微膠囊型硬化促進劑可使用例如已將胺化合物粉末分散於環氧樹脂中的微粒子組成物等。胺化合物基於所欲的增黏倍率來選擇即可。胺化合物可舉如:脂肪族第一胺、脂環式第一胺、芳香族第一胺、脂肪族第二胺、脂環式第二胺、芳香族第二胺、咪唑化合物、咪唑啉化合物及該等化合物與碳酸、磺酸、異氰酸酯或環氧化合物之反應生成物等。該等可取用1種或將2種以上併用。例如:可將脂肪族第一胺、脂環式第一胺、芳香族第一胺、脂肪族第二胺、脂環式第二胺、芳香族第二胺、咪唑化合物或咪唑啉化合物與上記反應生成物併用。胺化合物粉末之平均粒徑宜為50µm以下,較佳為10µm以下。
在此,本說明書中的平均粒徑,是以使用雷射繞射-散射式粒度分布測定裝置測定之體積基準的粒徑分布於累計體積50%之粒徑(D50)求得。使用胺化合物粉末時,從抑制於室溫或25℃下之增黏的觀點來看,胺化合物的熔點或軟化點宜為60℃以上。
硬化促進劑可單獨使用一種,亦可二種以上組合使用。硬化促進劑宜作為與樹脂(環氧樹脂等)之反應生成物(加成物)使用。
硬化促進劑的量相對於硬化性樹脂100質量份例如為0.1質量份以上且20質量份以下,亦可為1質量份以上且10質量份以下。在此,硬化促進劑作為加成物使用時,硬化促進劑的量指的是扣除了硬化促進劑以外成分之硬化促進劑本身的量。
(無機充填劑)
無機充填劑可舉如:金屬氧化物、金屬氫氧化物(例如氫氧化鎂等)、金屬鹽(例如無機酸鹽(碳酸鈣、白雲石(特別是碳酸鹽)等))、其他的礦物系充填劑(滑石、矽灰石等)等。又,亦可以使用紅丹、碳化矽、氮化硼(BN)等。金屬氧化物可例示如:氧化矽(熔融氧化矽等)、氧化鋁、氧化鈦等。無機充填劑可為經過表面處理(例如藉由矽烷化合物等進行表面處理)者。該等無機充填劑可單獨使用一種或將二種以上組合使用。
無機充填劑通常是已分散或混合於硬化性樹脂組成物中之狀態。因此,無機充填劑係以可分散或混合於硬化性樹脂組成物中之形態來使用。無機充填劑之形態宜為例如粒狀或短纖維狀。
無機充填劑之平均粒徑(D50)為例如0.01µm以上且100µm以下。
無機充填劑的量相對於硬化性樹脂100質量份為例如1質量份以上且5000質量份以下(或1質量份以上且3000質量份以下),若從兼具低翹曲與應力鬆弛的觀點來看,宜為10質量份以上且3000質量份以下。
(其他)
硬化性樹脂組成物視需要亦可包含其他成分。其他成分可舉如:第2熱塑性樹脂、聚合起始劑(自由基產生劑、酸產生劑、鹼產生劑等)、聚合觸媒(磷系觸媒(三苯膦等)、核殼觸媒等)、離子捕捉劑、阻燃劑、顏料、碳黑、耦合劑(矽烷耦合劑等)、流變減黏性賦予劑、預膠化劑等。
硬化性樹脂組成物亦可包含上述第1熱塑性樹脂以外的熱塑性樹脂(第2熱塑性樹脂)。第2熱塑性樹脂的種類可舉例如:丙烯酸樹脂、苯氧樹脂、聚烯烴、聚胺甲酸酯、聚醚、聚酯、聚醯亞胺、聚醋酸乙烯酯或其膠化物(亦包含聚乙烯醇)、丁醛樹脂、聚醯胺、聚氯乙烯、聚二氯亞乙烯、纖維素、熱塑性環氧樹脂、熱塑性苯酚樹脂等。其中,以對片材之成形性優異的優點來看,宜為丙烯酸樹脂。硬化性樹脂每100質量份,第2熱塑性樹脂的量可為5質量份以上且200質量份以下,亦可為10質量份以上且100質量份以下。
添加進樹脂組成物時之第2熱塑性樹脂的形態沒有特別限定。第2熱塑性樹脂可為例如平均粒徑0.01µm以上且200µm以下(較佳為0.01µm以上且100µm以下)之粒子。前述粒子亦可具有核-殼結構。在這種情形下,核例如可為包含源自選自於由(甲基)丙烯酸正、異及第三丁酯所構成群組中至少一種單體之單元的聚合物,亦可為包含源自其他(甲基)丙烯酸酯之單元的聚合物。殼層可為例如單官能單體((甲基)丙烯酸甲酯、(甲基)丙烯酸正、異或第三丁酯、(甲基)丙烯酸等)與多官能單體(1,6-己二醇二丙烯酸酯等)之共聚物。此外,亦可於調製硬化性樹脂組成物時添加已分散或溶解於溶劑中之高純度的第2熱塑性樹脂。
硬化性樹脂組成物可藉由例如按預定比率混合各成分來調製。例如可按預定比率摻合各成分,並視需要邊加熱邊混合。此外,亦可將各成分的混合物攪拌例如60分鐘~480分鐘然後於減壓下進行脫泡。
依據前述態樣,藉由使用第1環氧樹脂、第2環氧樹脂與第1熱塑性樹脂,即使只單純混合構成成分,仍可使各樹脂分散於硬化性樹脂組成物中。若調節混合時的旋轉條件(剪率、剪切速度等),則容易獲得第1環氧樹脂與第2環氧樹脂之良好的相分離狀態。
將本發明之前述態樣之硬化性樹脂組成物應用在基板等被附著物上使其硬化,形成硬化物之層與被附著物的積層體時,因硬化物與被附著物間之線膨脹係數通常會不相同,而會發生積層體翹曲的現象。然而,硬化性樹脂組成物之硬化物之應力鬆弛性很優異的緣故,暫時放置後積層體的翹曲即會鬆弛。更具體說明如下:首先,於直徑300mm及厚度200µm之圓盤狀基板的一主面,形成厚度200µm之硬化性樹脂組成物之硬化物層而得到積層體。於此情況下,對於硬化物層剛形成時積層體的翹曲,在硬化物層形成經過24小時後的積層體的翹曲可降低為50%以下,較佳的為40%以下(更佳為20%以下)。因此於本發明中,可有效地鬆弛翹曲。一般來說,基板是以無機系材料形成的基板(玻璃基板、矽基板、藍寶石基板、化合物半導體基板、陶瓷基板等)與硬化物層之積層體容易產生翹曲。於本發明中,即使在使用該等無機系材料所形成的基板的情況下,還是可有效地鬆弛翹曲。
另外,這裡所謂的硬化物層,係設為在基板上之一主面形成硬化性樹脂組成物層並將塗膜於150℃下加熱處理3小時所形成者。硬化物層剛形成後之積層體的翹曲,指的是於3小時的加熱處理結束然後冷卻至室溫(例如20~35℃)後的初始階段(例如加熱處理結束然後冷卻至室溫後又經過5分鐘的階段)之積層體的翹曲。翹曲的測定方法可使用雷射位移計測定基板的中心與端部兩點之高低差的平均,並以該值為翹曲量。硬化物層形成經過24小時後之積層體的翹曲,是在3小時的加熱處理結束後經過24小時之階段測定的。
這種硬化性樹脂組成物,即使應用在基板等被附著物上使其硬化,仍可有效地鬆弛所得積層體的應力。此外,硬化性樹脂組成物亦適於片材成形,可作為硬化性片材利用。以硬化性樹脂組成物的硬化物可有效地鬆弛應力。因此,即使將硬化性樹脂組成物應用在具備電路構件的基板上使其硬化,仍可鬆弛所得積層體的翹曲。故硬化性樹脂組成物及硬化性片材作為用以密封具備電路構件之基板(安裝構件等)、電子零件等之密封材亦甚是有用。此外,硬化性樹脂組成物及硬化性片材,適合形成例如稱為晶圓級封裝(WLP)或面板級封裝(PLP)的封裝體,也可利用於扇出型面板級封裝(FOPLP)及扇出型晶圓級封裝(FOWLP)。硬化性樹脂組成物及硬化性片材,也適用於密封大面積之電子零件或基板。此外,硬化性樹脂組成物,也適合作為對搭載半導體元件等之電子零件或基板一併進行底部填充(underfill)與包覆成型(overmold)時之密封材(模封底部填充材)。
(硬化性片材)
硬化性片材是由前述硬化性樹脂組成物所形成。硬化性片材亦可為半硬化狀態(所謂的B階段)。
硬化性片材可利用眾所周知之片材成形方法由硬化性樹脂組成物形成。硬化性片材是藉由使用例如模具、輥塗機、刮刀等將硬化性樹脂組成物進行片材成形而形成。從使片材成形易於進行的觀點來看,可將利用於片材成形之糊狀硬化性樹脂組成物的黏度調整為10mPa.s以上且10000mPa.s以下。使用溶劑糊的情況下,之後可於70~150℃下乾燥1~10分鐘以除去溶劑。此外,硬化性片材可使用擠製成形、壓縮成形、印刷成形、轉注成形等成形方法形成,亦可利用藉由分配器等進行之塗布成形來形成。此外,糊液包含第2熱塑性樹脂時,亦可於使用糊液形成薄膜之後進行加熱處理。加熱處理是例如藉由以下方式進行:將糊液薄膜化之後,在小於硬化性樹脂之硬化溫度(例如70~150℃)下,對薄膜加熱例如1~10分鐘。
硬化性片材可為單層片材,亦可為具有2層以上之多層片材。多層片材可藉由分別作成各層之後再積層(積層法)而形成,亦可藉由依序塗佈各層之材料(塗佈法)來形成。就多層片材而言,可為至少相鄰2層的組成(構成成分的種類及/或含量等)互異者。各層可依前述之片材成形方法形成。
硬化性片材的厚度為例如50µm以上且1000µm以下,亦可為100µm以上且700µm以下。厚度在此範圍時,對於硬化性片材與基板等被附著物之積層體而言,就容易確保高的應力鬆弛效果,可更有效地鬆弛翹曲。
(使用硬化性片材之密封)
本發明前述態樣之硬化性片材,特別適用於密封配備電路構件之基板(安裝構件等)或電子零件等。關於使用硬化性片材之密封,以下將舉例說明密封安裝構件(或安裝結構體)之情形。
圖1與圖2是安裝構件之剖面示意圖,為了說明使用硬化性片材之安裝構件的密封。圖3是經硬化性片材之硬化物密封之安裝構件的剖面示意圖。經硬化性片材4P之硬化物4密封之安裝構件10是藉由例如具備以下步驟之方法製造的:準備安裝構件10之第1準備步驟、準備硬化性片材4P之第2準備步驟、將硬化性片材4P配置於安裝構件之配置步驟、及以硬化性片材4P密封第2電路構件2之密封步驟。
(第1準備步驟)
準備安裝構件10,其具備如圖1所示之第1電路構件1與搭載於第1電路構件1上之複數個第2電路構件2。
第1電路構件1是選自於由以下構件所構成群組中之至少1種:例如半導體元件、半導體封裝體、玻璃基板、樹脂基板、矽基板、藍寶石基板、化合物半導體基板及陶瓷基板。該等第1電路構件,亦可為其表面形成有ACF(各向異性導電膜)或ACP(各向異性導電糊)之類的導電材料層者。樹脂基板可為剛性樹脂基板亦可為可撓曲性樹脂基板,可舉例如:環氧樹脂基板(例如玻璃環氧基板)、雙馬來醯亞胺三基板、聚醯亞胺樹脂基板、氟樹脂基板等。第1電路構件1亦可為於內部配備半導體晶片等之內建零件基板。
本發明之上述面向的樹脂組成物與硬化性片材,也適用於大面積的樹脂密封。因此,第1電路構件可為大面積基板(晶圓或面板等)。此種基板的面積可為例如30,000mm2
以上。若為晶圓,則例如晶圓直徑為200mm(8吋)以上。此種晶圓可舉例如直徑200mm(8吋)之晶圓、直徑300mm(12吋)之晶圓等。晶圓例如具有圓盤狀或與其類似之形狀,但並不限定於該等形狀。此外,所謂的晶圓直徑,指的是圓盤狀晶圓之平面形狀的圓的直徑,若晶圓非圓盤狀,則指的是與晶圓平面形狀具有相同面積的圓(等效圓)之直徑。若為面板,例如,面板的一邊長度可為250mm以上,或可為300mm以上。面板通常具有矩形或是與其類似的形狀,但並不限定於該等形狀。此種面板可舉例如:250mm×350mm、320mm×320mm之面板,370mm×470mm、410mm×515mm之面板,508mm×610mm之面板,500mm×510mm之面板及610mm×457mm之面板等。
複數個第2電路構件2可各自為相同構件,亦可為相異構件。圖示例中,複數個第2電路構件2任一個皆為隔著凸塊3搭載於第1電路構件1之半導體元件。第1電路構件1與第2電路構件2之間的間隙S,是以底部填充材5進行樹脂密封。以底部填充材5對該間隙S進行樹脂密封的方法有以下幾種:於第2電路構件2之與第1電路構件1相對的面預先塗佈底部填充材5的方法(例如將經底部填充材5樹脂密封之第2電路構件2搭載於第1電路構件1上的方法);於第1電路構件1上塗佈底部填充材5之後搭載第2電路構件2以進行樹脂密封的方法;及於第1電路構件1上搭載第2電路構件2後於間隙S中填入底部填充材5來進行樹脂密封的方法等。此外,亦可使用本發明前述態樣之硬化性片材4P對間隙S作底部填充來進行樹脂密封。例如,亦可於第1電路構件1上搭載第2電路構件2之後,藉由以硬化性片材4P模封的同時進行間隙S之底部填充的模封底部填充(molded underfill)來樹脂密封間隙S。此外,根據電路構件間的連接方法或方式,亦有第1電路構件1與第2電路構件2之間不存在間隙、不需藉由底部填充材5作樹脂密封的情形。再者第2電路構件2亦可為不配置底部填充材5、需要以維持間隙S的狀態進行密封(中空密封)的電子零件(中空構件)。中空構件可舉例如:RFIC、SAW、感測器晶片(加速度感測器等)、壓電振盪器晶片、晶體振盪器晶片、MEMS裝置等。中空構件以外之第2電路構件2可舉例如:半導體元件、FBAR、BAW、多層晶片LC濾波器、電介質濾波器、積層陶瓷電容器(MLCC)等。
換言之,安裝構件可具有各種第1電路構件1上搭載有第2電路構件2之結構,例如:晶片接合基板(Chip-on-Board, CoB)結構(包含晶片接合晶圓(Chip-on-Wafer, CoW)、晶片接合薄膜(Chip-on-Film, CoF)、晶片接合玻璃(Chip-on-Glass, CoG))、晶片接合晶片(Chip-on-Chip, CoC)結構、晶片接合封裝體(Chip-on-Package, CoP)結構及封裝體接合封裝體(Package-on-Package, PoP)結構。安裝構件亦可為於搭載有第2電路構件2之第1電路構件1上再積層第1電路構件1及/或第2電路構件2這樣的多層安裝構件。
凸塊3具有導電性,第1電路構件1與第2電路構件2可藉由凸塊3作電性連接。凸塊3的材料只要具有導電性即無特別限定,可舉例如:銅、金、焊球等。
底部填充材沒有特別限制,可使用環氧樹脂(或樹脂組成物)等眾所周知的底部填充材。
(第2準備步驟)
準備如圖1所示之硬化性片材4P。
硬化性片材4P是如上述方式所製成。
(配置步驟)
以硬化性片材4P之一主面與第2電路構件2相對向之方式,將硬化性片材4P配置於安裝構件10(圖1)。此時,是以一片硬化性片材4P覆蓋複數個第2電路構件2。在密封面積較大等情況下,視需要亦可用複數個硬化性片材覆蓋第2電路構件2。
另外,圖示例中,係顯示密封第1電路構件1單面側之態樣,但亦可為兩面側都密封之態樣。
(密封步驟)
以硬化性片材4P密封第2電路構件2。密封步驟中,以按壓構件6將硬化性片材4P對安裝構件10(更具體地說,是隔著第2電路構件2對第1電路構件1)進行按壓(圖2),同時加熱硬化性片材4P使其硬化。藉此,使用硬化性片材4P密封安裝構件的第2電路構件2。藉由密封,形成安裝構件之第2電路構件2被硬化性片材4P硬化所形成之硬化物4包覆的狀態(圖3)。在第2電路構件2包含中空構件的情況下,於密封步驟中,亦可於維持間隙S的同時密封第2電路構件2。
硬化性片材4P對第1電路構件1之押壓,係於例如以小於硬化性片材4P所含硬化性樹脂之硬化溫度加熱硬化性片材4P的同時進行(熱壓)。藉此,硬化性片材4P將密著於第2電路構件2表面,且容易伸展到第2電路構件2彼此間之第1電路構件1的表面,能夠提升第2電路構件2之密封可靠性。熱壓可於大氣壓力下進行,亦可於減壓環境下(例如0.001~0.05MPa)進行。按壓時之加熱條件沒有特別限定,對應按壓方式或硬化性樹脂的種類適當地設定即可。前述加熱是在例如40~200℃(較佳為50~180℃)下進行1秒~300分鐘(較佳為3秒~300分鐘)。
然後,於前述硬化溫度下加熱硬化性片材4P,使硬化性片材4P中的硬化性樹脂硬化,形成硬化物4。藉此,第2電路構件2被密封,可得如圖3所示之經硬化物4密封之安裝構件10。硬化性片材4P之加熱(硬化性樹脂之硬化)條件對應硬化性樹脂的組成適當設定即可。硬化性樹脂之硬化在例如50~200℃(較佳為120~180℃)下進行1秒~300分鐘(較佳為60分鐘~300分鐘)。
熱壓與硬化性樹脂的硬化可個別施行,亦可同時施行。例如,可於減壓環境下且在小於硬化性片材4P所含硬化性樹脂之硬化溫度下熱壓之後,解除減壓,於大氣壓力下進一步以高溫加熱,使硬化性樹脂硬化。或是,可於大氣壓力下且在小於硬化性片材4P所含硬化性樹脂之硬化溫度下熱壓之後,進一步以高溫加熱,使硬化性樹脂硬化。此外,亦可於減壓環境下且在硬化溫度下熱壓,藉以於減壓中使硬化性樹脂硬化。
密封步驟亦可藉由壓縮成型工法進行。壓縮成型工法可使用眾所周知的壓縮成形機等。成型壓力宜為例如0.5MPa~10MPa,較佳為1MPa~5MPa。硬化條件以進行前硬化(亦稱成形時加熱)與後硬化的方式為佳。
對於前硬化的溫度與時間,可以適當地作設定。前硬化的溫度宜為50~200℃,較佳為70~180℃。前硬化的時間宜為3秒~30分鐘,較佳為2分鐘~15分鐘。更進一步地說,也可以將加熱(成形時加熱)分成多階段來進行硬化,例如,亦可於80~130℃下進行前硬化8分鐘~12分鐘後,再於140~160℃下進行後硬化2分鐘~5分鐘。
後硬化會因成形時的加熱條件等而有所不同,宜於80~200℃下進行,較佳於100~180℃下進行。後硬化的時間會因成形時的加熱條件等而有所不同,宜為10分鐘~300分鐘,較佳為30分鐘~180分鐘。
實施例
以下依據實施例及比較例具體說明本發明,但本發明並不限定於底下的實施例。
《實施例1~116、比較例1~2及參考例1》
(1)硬化性樹脂組成物之調製
於容器中,以表1~表11所示的質量比放入表1~表11所示的成分,藉著於110℃下攪拌20分鐘調製硬化性樹脂組成物。
(2)硬化性片材之製作
將前述(1)所得之硬化性樹脂組成物以T模具熔融擠出予以片材化而製作厚度200µm之片材(硬化性片材)。
(3)積層體之製作
使用(2)所製作之硬化性片材密封基板。基板使用圓盤狀之矽基板(直徑300mm及厚度200µm)。硬化性片材以硬化後之厚度為200µm之方式作配置。密封是藉由將硬化性片材配置於半導體晶片上,於減壓環境下(4hPa)以125℃對硬化性片材進行前硬化10分鐘後、再以150℃加熱3小時同時壓縮成型來進行。
(4)評價
按已述之方法求出前述(3)所得之積層體之初始及硬化24小時後的翹曲,並評價應力鬆弛性。
A:24小時後的翹曲為初始之20%以下
B:24小時後的翹曲大於初始之20%且在40%以下
C:24小時後的翹曲大於初始之40%且在50%以下
D:24小時後的翹曲大於初始之50%且在60%以下
E:24小時後的翹曲大於初始之60%
此外,按已述之方法求出所使用的第1環氧樹脂與第2環氧樹脂之HSP值,並算出差值。
求出無機充填劑於構成成分總量中所佔之質量比率(質量%)作為填料充填率。
《實施例117~128》
(1)硬化性樹脂組成物之調製
除了以表12所示之質量比使用表12所示的成分以外,以與實施例1同樣方式於室溫下調製液狀的硬化性樹脂組成物。
(2)積層體之製作
使用(1)所調製之液狀硬化性樹脂組成物將基板密封。基板是使用與實施例1同樣之矽基板。硬化性樹脂組成物是以硬化後之厚度為200µm之方式塗佈於基板上。硬化是藉由以125℃對硬化性樹脂組成物之塗膜進行前硬化10分鐘後,於150℃下加熱3小時來進行。
(3)評價
除了使用前述(2)所得之積層體以外,以與實施例1同樣方式進行評價。
實施例、比較例及參考例之結果示於表1~表12。
表1
如表1所示,不含第1環氧樹脂之比較例1及2在經過24小時後翹曲還是很大,得到應力鬆弛性很低的結果。使用Mw為350,000之熱塑性樹脂之參考例1儘管併用第1環氧樹脂與第2環氧樹脂,應力鬆弛性還是很低。
表2A
表2B
表3A
表3B
表4
表5
表6
表7
表8A
表8B
表9
表10
表11
表12
與前述比較例及參考例之結果相較之下,實施例可將經過24小時後的翹曲降低至50%以下、40%以下或20%以下,得到高的應力鬆弛性。即使變更第1環氧樹脂、第2環氧樹脂、熱塑性樹脂或硬化劑的種類仍可獲得這樣的效果。
雖就有關目前較佳之實施態樣來說明本發明,但不能將此種揭示作限定解釋。本發明所屬技術領域中具有通常知識者經由閱讀前述揭示應能通曉各種變形或改變無虞。因此,所列申請專利範圍在不脫離本發明本質精神及範圍下,應解釋為包含所有的變形與改變。
產業上之可利用性
根據本發明前述態樣之硬化性樹脂組成物或硬化性片材,即使與基板等被附著物積層並使其硬化,仍可確保硬化物層之強度同時鬆弛積層體的翹曲。因此,硬化性樹脂組成物及硬化性片材在作為用以密封包含基板等之安裝結構體、電子零件等的密封材上相當有用。此外,硬化性樹脂組成物及硬化性片材亦適於作為扇出型晶圓級封裝(FOWLP)及扇出型面板級封裝(FOPLP)之密封材。
10:安裝構件
1:第1電路構件
2:第2電路構件
3:凸塊
4:硬化性片材之硬化物
4P:硬化性片材
5:底部填充材
6:按壓構件
S:間隙
圖1為剖面示意圖,用以說明使用本發明一實施形態之硬化性片材對包含基板之的安裝結構體(安裝構件)進行密封時,將硬化性片材配置於安裝構件上之步驟。
圖2為剖面示意圖,用以說明使用本發明一實施形態之硬化性片材對包含基板之安裝構件進行密封時,以硬化性片材密封電路構件之步驟。
圖3係經使用本發明一實施形態之硬化性片材密封後的安裝構件之剖面示意圖。
10:安裝構件
1:第1電路構件
2:第2電路構件
3:凸塊
4:硬化性片材之硬化物
5:底部填充材
S:間隙
Claims (16)
- 一種硬化性樹脂組成物,包含:第1環氧樹脂,其具有聚氧伸烷基鏈;第2環氧樹脂,其與前述第1環氧樹脂不同;熱塑性樹脂,其具有5000以上且200,000以下之重量平均分子量且具有反應性官能基;選自於由硬化劑及硬化促進劑所構成群組中之至少一種;及無機充填劑;並且,前述第1環氧樹脂與前述第2環氧樹脂之質量比為5:95至40:60;前述第2環氧樹脂包含環氧樹脂或其加氫物,該環氧樹脂包含選自於由芳香環及五員環以上之雜環所構成群組中之至少一種環結構;相對於前述第1環氧樹脂與前述第2環氧樹脂之總量100質量份,前述熱塑性樹脂的量為10質量份以上且300質量份以下。
- 如請求項1之硬化性樹脂組成物,其中前述聚氧伸烷基鏈所含伸烷基之碳數為2以上。
- 如請求項1或2之硬化性樹脂組成物,其中前述聚氧伸烷基鏈上之氧伸烷基單元之重複數為3以上。
- 如請求項1或2之硬化性樹脂組成物,其中前述第1環氧樹脂包含聚伸烷基二醇環氧丙基醚。
- 如請求項1或2之硬化性樹脂組成物,其中 前述第1環氧樹脂包含:選自於由芳香族多元醇之環氧烷加成物之環氧丙基醚及脂環式多元醇之環氧烷加成物之環氧丙基醚所構成群組中之至少一種。
- 如請求項1或2之硬化性樹脂組成物,其中前述第1環氧樹脂之漢森溶解度參數值與前述第2環氧樹脂之漢森溶解度參數值的差為6以上。
- 如請求項1或2之硬化性樹脂組成物,其中前述熱塑性樹脂包含丙烯酸系熱塑性樹脂。
- 如請求項1或2之硬化性樹脂組成物,其中前述熱塑性樹脂包含聚矽氧系熱塑性樹脂。
- 如請求項1或2之硬化性樹脂組成物,其中前述熱塑性樹脂至少具有環氧基作為前述反應性官能基。
- 如請求項1或2之硬化性樹脂組成物,其中前述熱塑性樹脂的量為50質量份以上且300質量份以下。
- 如請求項1或2之硬化性樹脂組成物,在直徑300mm及厚度200μm之圓盤狀基板一主面形成厚度200μm之前述硬化性樹脂組成物之硬化物層所得的積層體中,相對於剛形成前述硬化物層後之前述積層體的翹曲,自形成前述硬化層至經過24小時後之前述積層體的翹曲為40%以下。
- 如請求項1或2之硬化性樹脂組成物,前述硬化性樹脂組成物包含前述硬化劑,前述硬化劑具有與環氧基反應之官能基,並且,前述官能基之當量數相對於環氧基1當量為0.1~1.5當量。
- 如請求項12之硬化性樹脂組成物,前述硬化性樹脂組成物更包含前述硬化促進劑。
- 如請求項1或2之硬化性樹脂組成物,其為液狀。
- 一種硬化性片材,係以如請求項1至14中任一項之硬化性樹脂組成物所形成。
- 如請求項15之硬化性片材,係用以密封配備電路構件之安裝構件。
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US20210403765A1 (en) | 2021-12-30 |
KR20210090183A (ko) | 2021-07-19 |
CN113056519A (zh) | 2021-06-29 |
US11718770B2 (en) | 2023-08-08 |
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