TWI742362B - 用於半導體電路連接之黏著劑組成物及含彼之黏著膜 - Google Patents

用於半導體電路連接之黏著劑組成物及含彼之黏著膜 Download PDF

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TWI742362B
TWI742362B TW108113370A TW108113370A TWI742362B TW I742362 B TWI742362 B TW I742362B TW 108113370 A TW108113370 A TW 108113370A TW 108113370 A TW108113370 A TW 108113370A TW I742362 B TWI742362 B TW I742362B
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adhesive
resin
adhesive film
chemical formula
bonding
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TW108113370A
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TW201943821A (zh
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金柱賢
金丁鶴
南承希
李光珠
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南韓商Ｌｇ化學股份有限公司
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    • C—CHEMISTRY; METALLURGY
    • C07—ORGANIC CHEMISTRY
    • C07D—HETEROCYCLIC COMPOUNDS
    • C07D233/00—Heterocyclic compounds containing 1,3-diazole or hydrogenated 1,3-diazole rings, not condensed with other rings
    • C07D233/54—Heterocyclic compounds containing 1,3-diazole or hydrogenated 1,3-diazole rings, not condensed with other rings having two double bonds between ring members or between ring members and non-ring members
    • C07D233/56—Heterocyclic compounds containing 1,3-diazole or hydrogenated 1,3-diazole rings, not condensed with other rings having two double bonds between ring members or between ring members and non-ring members with only hydrogen atoms or radicals containing only hydrogen and carbon atoms, attached to ring carbon atoms
    • C07D233/58—Heterocyclic compounds containing 1,3-diazole or hydrogenated 1,3-diazole rings, not condensed with other rings having two double bonds between ring members or between ring members and non-ring members with only hydrogen atoms or radicals containing only hydrogen and carbon atoms, attached to ring carbon atoms with only hydrogen atoms or radicals containing only hydrogen and carbon atoms, attached to ring nitrogen atoms
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    • C09J11/00—Features of adhesives not provided for in group C09J9/00, e.g. additives
    • C09J11/02—Non-macromolecular additives
    • C09J11/06—Non-macromolecular additives organic
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    • C09J7/10—Adhesives in the form of films or foils without carriers
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    • C09J133/04—Homopolymers or copolymers of esters
    • C09J133/06—Homopolymers or copolymers of esters of esters containing only carbon, hydrogen and oxygen, the oxygen atom being present only as part of the carboxyl radical
    • C09J133/062—Copolymers with monomers not covered by C09J133/06
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    • C09J133/08—Homopolymers or copolymers of acrylic acid esters
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    • C09J161/04—Condensation polymers of aldehydes or ketones with phenols only
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    • C09J179/00—Adhesives based on macromolecular compounds obtained by reactions forming in the main chain of the macromolecule a linkage containing nitrogen, with or without oxygen, or carbon only, not provided for in groups C09J161/00 - C09J177/00
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    • H01L24/00—Arrangements for connecting or disconnecting semiconductor or solid-state bodies; Methods or apparatus related thereto
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    • H01L24/12—Structure, shape, material or disposition of the bump connectors prior to the connecting process
    • H01L24/13—Structure, shape, material or disposition of the bump connectors prior to the connecting process of an individual bump connector
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    • H01L24/28—Structure, shape, material or disposition of the layer connectors prior to the connecting process
    • H01L24/29—Structure, shape, material or disposition of the layer connectors prior to the connecting process of an individual layer connector
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Abstract

本發明關於一種用於黏合半導體之黏著劑樹脂組成物，其包括：熱塑性樹脂；熱固性樹脂；固化劑；及具有特定結構之化合物，及含彼之用於半導體的黏著膜。

Description

用於半導體電路連接之黏著劑組成物及含彼之黏著膜
相關申請案之相互參照
本案請求於2018年4月17日向韓國智慧財產權局申請的韓國專利申請案第10-2018-0044654號及2019年4月15日申請的第10-2019-0043931號之權益，在此以引用的方式將其全文併入本文。
本發明關於用於半導體電路連接之黏著劑組成物及用於半導體之黏著膜。
近來，隨著電子裝置之小型化、高功能化和容量擴大的趨勢不斷擴展，及對半導體封裝之緻密化和高集成度的需求迅速提昇，半導體晶片的尺寸變得越來越大。就集成度之改進而言，逐漸使用晶片以多級式堆疊之堆疊封裝方法。
此外，已開發出使用TSV(矽通孔；Through Silicon Via)之半導體，並通過凸塊接合(bump bonding)傳輸信號。關於凸塊接合，一般應用熱壓黏合(thermo-compression bonding)技術。在此情況下，於熱壓黏合技術中黏著劑的熱固性影響封裝製造加工性及封裝可靠性。
已有人開發出糊形式之非導電糊(NCP)作為用於填充各個TSV層之間的黏著劑，但是凸塊之間距變窄且填充變得困難。為了克服此問題，正在開發膜形式之非導電膜(NCF)。
當進行凸塊接合的熱壓接合時，黏著劑應該於高溫下快速固化並且室溫的固化應被抑制，從而改善儲存安定性。觸媒在控制這些黏著劑之固化程度時扮演重要角色，為此目的已開發出熱潛伏型觸媒(thermally-latent catalyst)。
[技術問題]
本發明提供一種用於半導體電路連接之黏著劑組成物，其於熱壓黏合期間可於短時間內於高溫下固化，並於室溫下具有優良儲存安定性。
本發明也提供一種黏著膜，其包括用於半導體電路連接之黏著劑組成物。 [技術方案]
本發明提供一種用於黏合半導體之黏著劑樹脂組成物，其包括：熱塑性樹脂；熱固性樹脂；固化劑；及由以下化學式1所示之化合物。
Figure 02_image001
於化學式1中，R1 係氫、C1至C10烷基或C6至C20芳基，R2 係含有能形成氫鍵之官能基的有機官能基，R3 係氫、鹵素、C1至C10烷基或C6至C20芳基，且n係1至4，為R3 之取代數。
更明確地說，於化學式1中，R1 可為氫或苯基，且R2 係羥基、羧基、羰基、甲醯基或胺基。
該用於黏合半導體之黏著劑樹脂組成物，以100重量份的熱塑性樹脂；熱固性樹脂；固化劑；及化學式1之化合物的總量計，可包括0.1至15重量份的化學式1之化合物。
該熱塑性樹脂可包括至少一種選自由以下所組成的群組之聚合物樹脂：聚醯亞胺、聚醚醯亞胺、聚酯醯亞胺、聚醯胺、聚醚碸、聚醚酮、聚烯烴、聚氯乙烯、苯氧基、反應性丁二烯丙烯腈共聚物橡膠、及(甲基)丙烯酸酯系樹脂。
該熱固性樹脂可包括選自由固態環氧樹脂及液態環氧樹脂所組成的群組中之至少一者。
該固化劑可包括軟化點為70 ℃或更高的酚樹脂。
本發明也提供一種用於半導體的黏著膜，其包括用於黏合半導體之黏著劑樹脂組成物。 [有益之效果]
根據本發明，提供一種用於半導體電路連接之黏著劑組成物，其可於熱壓黏合期間於短時間內於高溫下固化並於室溫下具有優良儲存安定性，及用於半導體之電沉積膜(electrodeposited film)。
下文中，將更詳細地描述根據本發明示範性具體實例的用於半導體電路連接之黏著劑組成物及用於半導體之電沉積膜。然而，以下實施例僅為了例示本發明，且本發明之範疇不限於此。
根據本發明之具體實例，提供一種用於黏合半導體之黏著劑樹脂組成物，其包括：熱塑性樹脂；熱固性樹脂；固化劑；及以下化學式1所示之化合物。
Figure 02_image003
於化學式1中，R1 係氫、C1至C10烷基或C6至C20芳基，R2 係含有能形成氫鍵之官能基的有機官能基，R3 係氫、鹵素、C1至C10烷基或C6至C20芳基，且n係1至4，為R3 之取代數。
發明人對可用於黏合或封裝半導體裝置之組件進行研究。結果，通過實驗發現，當包括化學式1之化合物的組成物或黏著膜用作半導體電路連接之材料時，其可於熱壓黏合期間於短時間內於高溫下固化，並於室溫下具有優良儲存安定性，從而完成本發明。
明確地說，化學式1之化合物包括含有能於R2 處形成氫鍵之官能基的有機官能基，其可藉由在進行形成氫鍵之室溫下使觸媒去活化而延遲固化反應，並可於熱壓黏合期間藉由於高於固化溫度之溫度下打斷氫鍵而將觸媒活化。因此，此具體實例的用於黏合半導體之黏著劑樹脂組成物可於高溫下快速固化，並可於室溫下長時間儲存。
如上所述，於化學式1中，R1 可為氫、C1至C10烷基或C6至C20芳基，R2 可為含有能形成氫鍵之官能基的有機官能基，R3 可為氫、鹵素、C1至C10烷基或C6至C20芳基，且n可為1至4，為R3 之取代數。更明確地說，於化學式1中，R1 可為氫或苯基，且R2 可為羥基、羧基、羰基、甲醯基或胺基。
用於黏合半導體之黏著劑樹脂組成物，以100重量份的熱塑性樹脂；熱固性樹脂；固化劑；及化學式1之化合物的總量計，可包括0.1至15重量份或0.5至10重量份的化學式1之化合物。
當以100重量份的熱塑性樹脂；熱固性樹脂；固化劑；及化學式1之化合物的總量計化學式1之化合物的重量太低時，固化反應便難以進行。因此，不能確保固化度(degree of cure)或反應溫度範圍變寬，導致於特定溫度之快速固化性質喪失。
當以100重量份的熱塑性樹脂；熱固性樹脂；固化劑；及化學式1之化合物的總量計化學式1之化合物的重量太高時，一些觸媒甚至可於室溫下被活化，所以可能無法確保膜之儲存安定性。
根據本發明之具體實例，除了化學式1之化合物之外，用於半導體電路連接之黏著劑組成物可另外包括熱塑性樹脂、熱固性樹脂及無機填料。
此外，除了化學式1之化合物之外，用於半導體電路連接之黏著劑組成物可另外包括熱固性樹脂、熱塑性樹脂、固化劑及無機填料。
關於該具體實例的用於黏合半導體之黏著劑樹脂組成物中所含的熱固性樹脂、熱塑性樹脂及固化劑，可使用供半導體電路連接用之黏著劑組成物的領域中習知之組分。
熱固性樹脂之實例沒有特別限制，例如，可較佳地使用環氧樹脂。
明確地說，環氧樹脂可為選自由以下所組成之群組中的至少一者：雙酚系環氧樹脂、聯苯系環氧樹脂、萘系環氧樹脂、茀系環氧樹脂、酚酚醛清漆系環氧樹脂、甲酚酚醛清漆系環氧樹脂、參(羥苯基)甲烷系環氧樹脂、四苯基甲烷系環氧樹脂、二環戊二烯型環氧樹脂、及二環戊二烯改質之酚型環氧樹脂。
雙酚系環氧樹脂之實例包括雙酚A型環氧樹脂、雙酚F型環氧樹脂、雙酚S型環氧樹脂、氫化雙酚A型環氧樹脂及雙酚AF型環氧樹脂。
舉例來說，當使用兩種類型之環氧樹脂作為熱固性樹脂時，可使用於10至35℃為液相的環氧樹脂及於10至35℃為固相的環氧樹脂之重量比為1:0.1至1:5的混合物。
當固體環氧樹脂之含量以液體環氧樹脂為基準計低於0.1重量份時，過量之樹脂可能於晶粒附著製程(die attachment process)期間流出而造成污染，且黏著層可能非常黏而造成撿拾性質(pick-up property)衰退。另一方面，當固態環氧樹脂之含量以液態環氧樹脂為基準計超過5.0重量份時，就與熱塑性樹脂之相容性及反應性而言可能是不利的。
此外，環氧樹脂也可包括至少一種選自由軟化點為50℃至100℃之甲酚酚醛清漆型環氧樹脂及軟化點為50℃至100℃之雙酚A環氧樹脂所組成的群組之環氧樹脂，以及軟化點為50℃至100℃之聯苯系環氧樹脂。
本文中，環氧樹脂，以軟化點為50℃至100℃之聯苯系環氧樹脂為基準計，可包括0.25至1.25或0.3至1.1重量份之至少一種選自由軟化點為50℃至100℃之甲酚酚醛清漆型環氧樹脂及軟化點為50℃至100℃之雙酚A環氧樹脂所組成的群組之環氧樹脂。
環氧樹脂之平均環氧當量可為100至1000。平均環氧當量可根據環氧樹脂中所含之每種環氧樹脂與環氧當量的重量比而獲得。
熱塑性樹脂的類型沒有特別限制，例如，選自由聚醯亞胺、聚醚醯亞胺、聚酯醯亞胺、聚醯胺、聚醚碸、聚醚酮、聚烯烴、聚氯乙烯、苯氧基、反應性丁二烯丙烯腈共聚物橡膠及(甲基)丙烯酸酯系樹脂所組成之群組中的至少一種聚合物樹脂皆可使用。
較佳地，熱塑性樹脂可為玻璃轉移溫度為 -10至30℃且重量平均分子量為200,000至1,000,000 g/mol之(甲基)丙烯酸酯系樹脂。
丙烯酸酯系樹脂係含有環氧基之丙烯酸系共聚物，並可含有1至25重量%、2至20重量%或2.5至15重量%之量的丙烯酸縮水甘油酯或甲基丙烯酸縮水甘油酯。
在此，當環氧基團於(甲基)丙烯酸酯系樹脂中之含量低於1重量%時，與環氧樹脂之相容性及黏著劑強度可能不足。當該量超過25重量%時，由於固化導致黏度的上升速率變得太快，因此在半導體裝置的熱壓黏合製程中可能無法充分地進行焊料凸塊的黏合及填充。
顧及黏著膜製造期間之組成物的流量控制，熱塑性樹脂之含量以100重量份之熱固性樹脂為基準計可為10至1500重量份。
作為固化劑，已知能用作熱固性樹脂之固化劑的化合物皆可使用。更明確地說，固化劑可包括至少一種選自由胺系固化劑及酸酐系固化劑所組成之群組的化合物。
作為固化劑，較佳可運用酚醛清漆系酚樹脂。
酚醛清漆系酚樹脂具有環位於反應性官能基之間的化學結構。由於此結構特徵，酚醛清漆系酚樹脂可進一步降低黏著劑組成物之吸濕性，並可進一步改善於高溫下IR回焊製程(reflow process)的穩定性，從而防止黏著膜的剝離及回焊龜裂(reflow cracking)。
酚醛清漆系酚樹脂的具體實例包括選自由酚醛清漆酚樹脂、木酚酚醛清漆酚樹脂、甲酚酚醛清漆酚樹脂、聯苯酚醛清漆酚樹脂、雙酚A酚醛清漆酚樹脂及雙酚F酚醛清漆酚樹脂所組成之群組中的至少一者。
酚醛清漆系酚樹脂的軟化點可為60℃或更高、60℃至150℃、105℃至150℃、或70℃至120℃。軟化點為60℃或更高的酚醛清漆系酚樹脂確保在黏著劑組成物固化之後具有充分的耐熱性、強度及黏著性。然而，當酚醛清漆系酚樹脂之軟化點太高時，黏著劑組成物之流動性可能降低，並且可能於實際半導體製造過程中於黏著劑內部形成空隙，從而顯著降低最終產物之可靠性或品質。
酚醛清漆系酚樹脂可較佳地具有80 g/eq.至300 g/eq. 之羥基當量及60℃至150℃之軟化點。
固化劑之含量可考量最終製造之黏著膜的物質而適當地選擇。例如，固化劑之用量以100重量份之熱固性樹脂為基準計可為10至700重量份或30至300重量份。
用於黏合半導體之黏著劑樹脂組成物可另外包括固化催化劑。
固化觸媒之作用是促進固化劑的作用或促進用於黏合半導體之黏著劑樹脂組成物的固化，並且可運用在用於半導體之黏著膜的領域中已知之任何固化觸媒，而沒有特別限制。
例如，作為固化觸媒，可使用選自由磷系化合物、硼系化合物、磷-硼系化合物及咪唑系化合物所組成之群組中的至少一者。固化觸媒之用量可考慮最終生成之黏著膜的性質等而加以適當選擇。
同時，具體實例之用於黏合半導體之黏著劑樹脂組成物可另外包括無機填料。
無機填料可為至少一種選自由氧化鋁、二氧化矽、硫酸鋇、氫氧化鎂、碳酸鎂、矽酸鎂、氧化鎂、矽酸鈣、碳酸鈣、氧化鈣、氫氧化鋁、氮化鋁及硼酸鋁所組成之群組的無機顆粒。
能吸附離子雜質並改進可靠性之離子吸附劑可用作無機填料。離子吸附劑可為至少一種選自由氫氧化鎂、碳酸鎂、矽酸鎂、氧化鎂、矽酸鈣、碳酸鈣、氧化鈣、氧化鋁、氫氧化鋁、氮化鋁、硼酸鋁晶鬚(aluminum borate whisker)、鋯系無機物質及銻-鉍系無機物質所組成之群組的無機顆粒。
無機填料之平均粒徑(以最長外徑為基準計)較佳為0.01至10μm、0.02至5.0μm或0.03至2.0μm。當無機填料之粒徑太小時，其可能輕易地聚集於黏著劑組成物中。另一方面，當無機填料之粒徑太大時，半導體電路可能被無機填料損壞，並且黏著膜之黏附性可能劣化。
無機填料之含量以100重量份之熱固性樹脂及熱塑性樹脂的總量為基準計可為10至300重量份或15至250重量份。
用於半導體電路連接之黏著劑組成物以100重量份之熱固性樹脂、熱塑性樹脂及無機填料的總量為基準計可包括10至90重量份之有機溶劑。有機溶劑之含量可考量黏著劑組成物和最終生成之黏著膜的物性及製程而加以適當選擇。
有機溶劑可為選自由酯、醚、酮、芳族烴及亞碸所組成之群組的至少一種化合物。
酯溶劑之實例包括乙酸乙酯、乙酸正丁酯、乙酸異丁酯、甲酸戊酯、乙酸異戊酯、乙酸異丁酯、丙酸丁酯、丁酸異丙酯、丁酸乙酯、丁酸丁酯、乳酸甲酯、乳酸乙酯、γ-丁內酯、ε-己內酯、δ-戊內酯、氧基乙酸烷酯，例如氧基乙酸甲酯、氧基乙酸乙酯、氧基乙酸丁酯(例如，甲氧基乙酸甲酯、甲氧基乙酸乙酯、甲氧基乙酸丁酯、乙氧基乙酸甲酯、乙氧基乙酸乙酯等等)、3-氧基丙酸烷酯，例如3-氧基丙酸甲酯、3-氧基丙酸乙酯(例如，3-甲氧基丙酸甲酯、3-甲氧基丙酸乙酯、3-乙氧基丙酸甲酯、3-乙氧基丙酸乙酯等等)、2-氧基丙酸烷酯，例如2-氧基丙酸甲酯、2-氧基丙酸乙酯、2-氧基丙酸丙酯(例如，2-甲氧基丙酸甲酯、2-甲氧基丙酸乙酯、2-甲氧基丙酸丙酯、2-乙氧基丙酸甲酯、2-乙氧基丙酸乙酯等等)、2-氧基-2-甲基丙酸甲酯、2-氧基-2-甲基丙酸乙酯(例如，2-甲氧基-2-甲基丙酸甲酯、2-乙氧基-2-甲基丙酸乙酯等等)、丙酮酸甲酯、丙酮酸乙酯、丙酮酸丙酯、乙醯乙酸甲酯、乙醯乙酸乙酯、2-酮基丁酸甲酯、2-酮基丁酸乙酯等。
醚溶劑之實例包括二乙二醇二甲醚、四氫呋喃、乙二醇單甲醚、乙二醇單***、甲基溶纖素乙酸酯(methyl cellosolve acetate)、乙基溶纖劑乙酸酯、二乙二醇單甲醚、二乙二醇單***、二乙二醇單丁醚、丙二醇單甲醚、丙二醇單甲醚乙酸酯、丙二醇單***乙酸酯、丙二醇單丙醚乙酸酯等。
酮溶劑之實例包括甲基乙基酮、環己酮、環戊酮、2-庚酮、3-庚酮、N-甲基-2-吡咯烷酮等。
芳族烴溶劑之實例包括甲苯、二甲苯、苯甲醚、檸檬烯(limonene)等。
亞碸溶劑之實例包括二甲基亞碸等。
用於黏合半導體之黏著劑樹脂組成物可另外包括偶合劑。偶合劑沒有特別限制，但是較佳為2-(3,4-環氧環己基)-乙基三甲氧基矽烷、3-環氧丙氧基丙基三甲氧基矽烷、3-環氧丙氧基丙基甲基-二乙氧基矽烷、3-環氧丙氧基丙基三乙氧基矽烷、N-(2-胺基乙基)-3-胺基丙基甲基二甲氧基矽烷、N-(2-胺基乙基)-3-胺基丙基三甲氧基矽烷、N-(2-胺基乙基)-3-胺基丙基三乙氧基矽烷、3-胺基丙基三甲氧基矽烷、3-胺基丙基三乙氧基矽烷、3-三乙氧基矽基-N-(1,3-二甲基-亞丁基)丙胺、N-苯基-3-胺基丙基三甲氧基矽烷、含巰基之3-巰基丙基甲基二甲氧基矽烷、3-巰基丙基三甲氧基矽烷等。
根據另一個本發明之具體實例，提供一種包括該黏著劑組成物之用於半導體電路連接的黏著膜。
由於用於半導體電路連接之黏著膜包括上述具體實例的用於半導體電路連接之黏著劑組成物，因此其不僅於室溫下顯現出優良儲存安定性，還可在熱壓黏合期間於高溫下於短時間內固化。
黏著膜可於5 rad/s之剪切速率下具有3000至6000Pa·s之熔體黏度(melt viscosity)。
在此，熔體黏度定義為可於黏著膜之整個範圍內獲得的最小黏度，而不是於特定溫度下之黏度。例如，使用TA進階流變擴展系統(ARES)以10℃/min之速率和5 rad/s之剪切速率下測得的最低黏度值可定義為熔體黏度。
熔體黏度可根據樹脂之類型、丙烯酸系樹脂之含量、填料之類型和含量等而變化。由於黏著膜包括上述具體實例的用於半導體電路連接之黏著劑組成物，因此與習知的黏著膜相比，該黏著膜可具有相對低之熔體黏度值。
這是因為黏著劑組成物包括能於分子結構中形成氫鍵的化學式1之化合物。化學式1之化合物含有有機官能基，該有機官能基包括能形成氫鍵以延遲反應的起始溫度之官能團，使得反應的起始點隨之移動，並使其與習知的黏著膜相比，變成可具有相對低之熔體黏度。在不包括能於分子結構中形成氫鍵的上述化學式1之觸媒的情況下，反應沒有延遲效應，因此反應在較低溫度下開始並使熔體黏度提高，從而具有相對高之熔體黏度。
此熔體黏度之變化可能影響整個膜之性質，例如與非導電膜(NCF)黏合之可能性及導電之可能性。
黏著膜於25℃下靜置4週之後，與初始反應峰相比，具有20%或更小的峰值變化(△H)，或可於25℃下靜置4週之後，與初始熔體黏度相比，於5 rad/s之剪切率下具有50%或更小的熔體黏度變化。
在此，峰值變化(△H)可藉由示差熱分析儀(DSC)測量之反應峰值變化來計算。熔體黏度之變化可藉由使用上述最小熔體黏度測量方法測量的熔體黏度之變化來計算。
當黏著膜之峰值變化(△H)為20%或更小時，或當熔體黏度變化為50%或更小時，室溫下之變化小，因此儲存安定性優良。因此，即使於室溫下長時間放置之後也可進行常規處理。
作為用於支撐膜之支撐基材，可使用具有優異耐熱性和耐化學性之樹脂膜；藉由使構成樹脂膜之樹脂交聯所獲得的交聯膜；或藉由將聚矽氧樹脂等塗覆於樹脂膜表面上並剝離該膜所獲得之膜。
構成樹脂膜之樹脂的實例包括聚烯烴，例如聚酯、聚乙烯、聚丙烯、聚丁烯和聚丁二烯、氯乙烯、乙烯-甲基丙烯酸共聚物、乙烯-乙酸乙烯酯共聚物、聚酯、聚醯亞胺、聚對苯二甲酸乙二酯、聚醯胺、聚胺酯等。
支撐基材之厚度沒有特別限制，但是可為3至400μm，5至200μm或10至150μm。
黏著劑層係由上述黏著劑組成物構成。黏著劑組成物之描述如上所述。
再者，必要的話，可在支撐基材與黏著層之間插置黏性層(tacky layer)。作為黏性層，此技藝已知者皆可運用而沒有特別限制。
保護膜之種類沒有特別限制，此技藝已知之塑料膜皆可運用。例如，保護膜可為包括例如以下樹脂之塑料膜：低密度聚乙烯、線性聚乙烯、中密度聚乙烯、高密度聚乙烯、超低密度聚乙烯、聚丙烯的無規共聚物、聚丙烯的嵌段共聚物、均聚丙烯、聚甲基戊烯、乙烯-乙酸乙烯酯共聚物、乙烯-甲基丙烯酸共聚物、乙烯-甲基丙烯酸甲酯共聚物、乙烯-離子聚合物(ionomer)共聚物、乙烯-乙烯醇共聚物、聚丁烯和苯乙烯。
用於半導體電路連接之黏著膜可藉由以下方式製造：混合黏著劑組成物之組分，將其塗覆於支撐基材上至預定厚度以形成黏著層，並使黏著層乾燥。
黏著膜可藉由將黏著層形成於支撐基材上，然後將保護膜層壓於黏著層上而製造。
黏著膜可藉著將黏性層形成於支撐基材上，然後將黏著層和保護膜依次層壓於黏性層上而製造。
黏著層可藉由以下方法形成於支撐基材上：將黏著劑組成物直接地或用適當溶劑稀釋之後藉由已知裝置如缺角輪塗佈機(comma coater)、凹版塗佈機(gravure coater)、模具塗佈機(die coater)、往復塗佈機(reverse coater)等塗覆於支撐基材上或離形膜上，然後接著於60℃至200℃之溫度下乾燥10秒至30分鐘。
必要的話，可進一步進行老化製程以充份促進黏著層的交聯。
黏著層之厚度可於1至500μm、5至100μm或5至50μm之範圍中適當地調節。
下文中，將參考以下實施例詳細說明本發明。然而，這些實施例僅為了例示本發明，且本發明之範疇不限於此。 實施例1：用於黏合半導體之樹脂組成物和黏著膜的製備 (1) 用於半導體電路連接之黏著劑組成物的製備
將40 g之酚醛樹脂(KH-6021，由DIC製造，雙酚A酚醛清漆樹脂，羥基當量121 g/eq.，軟化點133℃)作為環氧樹脂之固化劑；40 g之高黏度液態環氧樹脂(RE-310S，由Nippon Kayaku Co.製造，雙酚A環氧樹脂，環氧當量為180 g/eq.)；40 g熱塑性丙烯酸酯樹脂(KG-3015，Mw為900,000，玻璃轉移溫度為10℃)；1.5 g之2-(1H-咪唑-2-基)苯甲酸(Sigma-Aldrich製造)；及80 g之無機填料(SC-2050，由Admatech製造，球形二氧化矽，平均粒徑約400 nm)與甲基乙基酮混合，以獲得用於半導體電路連接之黏著劑組成物(固體含量為40重量%)。 (2) 黏著膜之製備
使用缺角輪塗佈機(comma coater)將黏著劑組成物塗佈於經離形處理之聚對苯二甲酸乙二酯膜(厚度：38μm)上，並於110℃下乾燥3分鐘，以獲得具有厚度約20μm之黏著層的黏著膜。 (3) 半導體裝置之製備
製備包括凸塊晶片(4.5 mm×4.5 mm)的晶圓作為半導體元件，其中於高度為15μm且間距為50μm之銅填料上形成高度為3μm之無鉛焊料。
將黏著膜之黏著層配置於晶圓之凸塊表面上之後，於50℃下進行真空層壓，切割(individualized)各個晶片。
使用熱壓接合器(thermo-compression bonder)將切割後的凸塊晶片在具有50μm間距連接墊之6 mm×8 mm基材晶片上進行熱壓黏合。明確地說，於100℃之頭部溫度在100 N下預黏合2秒，於100℃靜置10分鐘，瞬間加熱至260℃之頭部溫度，並於100 N下熱壓黏合4秒。 實施例2至3及比較例1至4
除了運用表1和2所示之組分和含量之外，以與實施例1相同的方式製備用於半導體電路連接之黏著劑組成物及使用該黏著劑組成物之黏著膜。此後，藉由使用彼製造半導體裝置。
Figure 02_image005
Figure 02_image007
* KH-6021：酚樹脂(DIC，羥基當量121 g/eq.，軟化點133℃) * RE-310S：環氧樹脂(由Nippon Kayaku Co.製造，環氧當量為180 g/eq) * KG-3015：丙烯酸系樹脂(含3重量%之甲基丙烯酸縮水甘油酯系重複單元，玻璃轉移溫度10℃，重量平均分子量900,000) * 化學式1-1：2-(1H-咪唑-2-基)苯甲酸 * 化學式1-2：2-(4,5-二氫-1H-咪唑-2-基)酚 * 化學式1-3：2-(1H-咪唑-2-基)苯甲酸甲酯 * 2MZ-H：咪唑固化劑(Curezol 2MZ-H，由SHIKOKU製造) * 2PZ：咪唑固化劑(Curezol 2PZ，由SHIKOKU製造) * 2-(2-甲基苯基)-1H-咪唑：咪唑固化劑(由Aldrich製造) * 3-(1H-咪唑-2-基)苯甲酸：咪唑固化劑(化學式1-1之異構物，由Aldrich製造) * KBM-403：偶合劑(環氧系，3-環氧丙氧基丙基三甲氧基矽烷，由Shin-Etsu Chemical Co., Ltd.製造) * SC-2050：填料(由Admatech製造，球形二氧化矽，平均粒徑約400nm) [實驗例：物性之評估] 實驗例 (1) 熔體黏度之測量
將每個實施例和比較例所獲得之黏著層堆疊至厚度變為320μm，然後使用輥式層壓機於60℃層壓。在每個試片形成直徑為8mm之圓形之後，將使用TA進階流變擴展系統(ARES)以10℃/min之速率和5 rad/s之剪切速率測量的最低黏度值界定為熔體黏度。 (2) DSC起效點之評估
使用示差熱分析儀(DSC)以10℃/min之速率於30至300℃範圍中進行示差熱分析。將初始反應峰開始形成之部分與外插基線(extrapolated baseline)之交點處的溫度指定為起效點(onset)。 (3) 孔隙之評估
對於實施例和比較例所獲得之每個半導體裝置，當藉由超音波掃描顯微鏡(SAT)得到於凸塊晶片與基材晶片之間被孔隙佔據之面積為1%或更小時，將其評定為合格(○)。當超過1%時，將其評定為不合格(×)。 (4) 傳導性之評估
對於實施例和比較例所獲得之每個半導體裝置，當可確認菊花鏈連接(daisy chain connection)時評估為合格(○)，且當不能確認菊花鏈連接時評估為不合格(×)。 (5) 連接狀態之評估
對於在實施例和比較例所獲得之每個半導體裝置，使連接部分藉由單面拋光暴露出來並用光學顯微鏡觀察。當黏著劑組成物沒被截留於連接部分且焊料在佈線過程中充分潤濕時，將其評定為合格(○)，否則評定為不合格(×)。 (6) 於室溫下之老化性質的評估
將實施例和比較例所獲得之黏著膜於25℃下靜置，且每天使用示差熱分析儀(DSC)計算峰值變化(△H)。藉由上述最小熔體黏度測量方法測量最小熔體黏度之變化。當峰值變化(△H)大於20%且最小熔體黏度之變化大於50%時，評定為隨時間變化。當在4週內未觀察到隨時間變化時，將其評定為合格(○)。當4週內隨時間發生變化時，將其評估為不合格(×)。
Figure 02_image009
Figure 02_image011
如表3和4所示，確認實施例1至3所提供之用於半導體的黏著膜具有相對低的熔體黏度及高的DSC起效溫度。
這可能是因為實施例1至3之組成物具有高的DSC起效溫度，使得於塗佈期間的乾燥製程之溫度下實質上不發生微反應(micro-reaction)，因此可具有相對低之黏度。因此，於運用實施例1至3之黏著膜的半導體裝置中，孔隙實質上沒有殘留，並於100℃預黏合之後令該膜靜置10分鐘的期間峰值變化(△H)很小。結果，確認沒有發生隨時間之變化，且沒發生傳導性缺陷或差的連接狀態。
相反地，由於比較例所提供之黏著劑組成物的起效點較低，因此於塗佈期間的乾燥製程之溫度下進行微反應而形成高黏度。結果，確認孔隙可能殘留於運用比較例之黏著膜的半導體裝置中，且由於於100℃預黏合之後令該膜靜置10分鐘的期間發生隨時間之變化，而發生傳導性缺陷及差的連接狀態。此外，確認比較例之黏著膜即使於室溫下儲存也會快速反應，因此隨時間之變化發生於4週內。

Claims (9)

  1. 一種用於黏合半導體之黏著劑樹脂組成物，其包含：熱塑性樹脂；熱固性樹脂；固化劑；及以下化學式1所示之化合物，其中以100重量份的熱塑性樹脂、熱固性樹脂、固化劑、及化學式1之化合物的總量計，該黏著劑樹脂組成物包含0.1至15重量份的化學式1之化合物：
    Figure 108113370-A0305-02-0027-1
     其中於化學式1中，R1係氫、C1至C10烷基或C6至C20芳基，R2係羧基、羰基、甲醯基或胺基，R3係氫、鹵素、C1至C10烷基或C6至C20芳基，且n係1至4，為R3之取代數。
  2. 如請求項1之用於黏合半導體之黏著劑樹脂組成物，其中於化學式1中，R1係氫或苯基，且R2係羧基。
  3. 如請求項1之用於黏合半導體之黏著劑樹脂組成物，其中該熱塑性樹脂包含至少一種選自由以下所組成的群組之聚合物樹脂：聚醯亞胺、聚醚醯亞胺、聚酯 醯亞胺、聚醯胺、聚醚碸、聚醚酮、聚烯烴、聚氯乙烯、苯氧基、反應性丁二烯丙烯腈共聚物橡膠、及(甲基)丙烯酸酯系樹脂。
  4. 如請求項1之用於黏合半導體之黏著劑樹脂組成物，其中該熱固性樹脂包含選自由固態環氧樹脂及液態環氧樹脂所組成的群組中之至少一者。
  5. 如請求項1之用於黏合半導體之黏著劑樹脂組成物，其中該固化劑包含軟化點為70℃或更高的酚樹脂。
  6. 一種用於半導體的黏著膜，其包含請求項1之用於黏合半導體之黏著劑樹脂組成物。
  7. 如請求項6之用於半導體的黏著膜，其中該黏著膜於5rad/s之剪切率下具有3000至6000Pa．s的熔體黏度。
  8. 如請求項6之黏著膜，其中該黏著膜於25℃下靜置4週之後，與初始反應峰相比，具有20%或更小的峰值變化(△H)。
  9. 如請求項6之用於半導體的黏著膜，其中該黏著膜於25℃下靜置4週之後，與初始熔體黏度相比，於5rad/s之剪切率下具有50%或更小的熔體黏度變化。
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