TWI580757B - 各向異性導電膜和由其連接的半導體裝置 - Google Patents

各向異性導電膜和由其連接的半導體裝置 Download PDF

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Publication number
TWI580757B
TWI580757B TW104119198A TW104119198A TWI580757B TW I580757 B TWI580757 B TW I580757B TW 104119198 A TW104119198 A TW 104119198A TW 104119198 A TW104119198 A TW 104119198A TW I580757 B TWI580757 B TW I580757B
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Taiwan
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conductive film
anisotropic conductive
weight
group
epoxy resin
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TW104119198A
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TW201610088A (zh
Inventor
申潁株
姜炅求
金智軟
朴憬修
朴永祐
孫秉勤
申炅勳
鄭光珍
韓在善
黃慈英
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三星Ｓｄｉ股份有限公司
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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L24/00—Arrangements for connecting or disconnecting semiconductor or solid-state bodies; Methods or apparatus related thereto
    • H01L24/01—Means for bonding being attached to, or being formed on, the surface to be connected, e.g. chip-to-package, die-attach, "first-level" interconnects; Manufacturing methods related thereto
    • H01L24/26—Layer connectors, e.g. plate connectors, solder or adhesive layers; Manufacturing methods related thereto
    • 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
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
    • C08J5/00—Manufacture of articles or shaped materials containing macromolecular substances
    • C08J5/18—Manufacture of films or sheets
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08G—MACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
    • C08G59/00—Polycondensates containing more than one epoxy group per molecule; Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups
    • C08G59/18—Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups ; e.g. general methods of curing
    • C08G59/20—Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups ; e.g. general methods of curing characterised by the epoxy compounds used
    • C08G59/22—Di-epoxy compounds
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08G—MACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
    • C08G59/00—Polycondensates containing more than one epoxy group per molecule; Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups
    • C08G59/18—Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups ; e.g. general methods of curing
    • C08G59/68—Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups ; e.g. general methods of curing characterised by the catalysts used
    • C08G59/687—Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups ; e.g. general methods of curing characterised by the catalysts used containing sulfur
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08G—MACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
    • C08G59/00—Polycondensates containing more than one epoxy group per molecule; Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups
    • C08G59/18—Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups ; e.g. general methods of curing
    • C08G59/68—Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups ; e.g. general methods of curing characterised by the catalysts used
    • C08G59/72—Complexes of boron halides
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    • C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
    • C09J7/00—Adhesives in the form of films or foils
    • C09J7/10—Adhesives in the form of films or foils without carriers
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    • C09J9/00—Adhesives characterised by their physical nature or the effects produced, e.g. glue sticks
    • C09J9/02—Electrically-conducting adhesives
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01B—CABLES; CONDUCTORS; INSULATORS; SELECTION OF MATERIALS FOR THEIR CONDUCTIVE, INSULATING OR DIELECTRIC PROPERTIES
    • H01B1/00—Conductors or conductive bodies characterised by the conductive materials; Selection of materials as conductors
    • H01B1/20—Conductive material dispersed in non-conductive organic material
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
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    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
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    • C09J2203/326—Applications of adhesives in processes or use of adhesives in the form of films or foils for bonding electronic components such as wafers, chips or semiconductors
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    • C09J2301/00—Additional features of adhesives in the form of films or foils
    • C09J2301/30—Additional features of adhesives in the form of films or foils characterized by the chemical, physicochemical or physical properties of the adhesive or the carrier
    • C09J2301/312—Additional features of adhesives in the form of films or foils characterized by the chemical, physicochemical or physical properties of the adhesive or the carrier parameters being the characterizing feature
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
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    • C09J2301/00—Additional features of adhesives in the form of films or foils
    • C09J2301/30—Additional features of adhesives in the form of films or foils characterized by the chemical, physicochemical or physical properties of the adhesive or the carrier
    • C09J2301/314—Additional features of adhesives in the form of films or foils characterized by the chemical, physicochemical or physical properties of the adhesive or the carrier the adhesive layer and/or the carrier being conductive
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
    • C09J2301/00—Additional features of adhesives in the form of films or foils
    • C09J2301/40—Additional features of adhesives in the form of films or foils characterized by the presence of essential components
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    • C09J2463/00—Presence of epoxy resin
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Description

各向異性導電膜和由其連接的半導體裝置
本發明涉及一種各向異性導電膜，其包含氫化環氧樹脂、鋶(sulfonium)陽離子聚合催化劑和鋶穩定劑，以及由所述膜連接的半導體裝置。
近年來隨著通過製造小型和高度功能性電子裝置來減少元件的連接端子(connection terminal)之間的距離的趨勢增加，越來越多地使用能夠促進這類端子之間的連接的各種膜狀黏結劑將IC晶片和可撓性印刷電路(flexible printed circuit，FPC)板接合，將IC晶片和包含在其上形成的氧化銦錫(indium tin oxide，ITO)電極電路的玻璃基底接合等。
在作為膜狀黏結劑之一並且在樹脂組成物中含有導電粒子的各向異性導電膜(anisotropic conductive film，ACF)中，通過加熱和壓制使樹脂流體化以密封在連接目標上彼此面對的電極之間的間隙，同時電極之間的空隙經一些導電粒子填充，從而允 許電極之間的電連接。在電子產品中廣泛使用陽離子可聚合環氧樹脂黏結劑來將電線和LCD面板安裝或附接到基底。確切地說，應用於ACF的陽離子催化劑需要200℃或小於200℃的固化溫度和24小時或大於24小時的儲存穩定性。
儘管提議硼酸鋶催化劑(日本專利公開案第2010-132614A號)作為用於環氧樹脂固化的陽離子催化劑，但這種催化劑在環氧樹脂溶液中具有1小時或小於1小時的低儲存穩定性，並且因此需要改良儲存穩定性。此外，儘管可以添加穩定劑以改良儲存穩定性，但在固化之後穩定劑不向各向異性導電膜提供緻密結構。因此，需要一種展示較高耐濕性和耐熱性同時展示改良連接可靠性和膜特性的各向異性導電膜。
本發明的一個方面是提供一種各向異性導電膜，其就儲存穩定性、耐濕性、耐熱性以及膜可成形性來說具有改良特性，同時通過熱固化保證低溫快速固化。
本發明的另一方面是提供一種甚至在150℃或小於150℃的連接溫度下允許連接並且展示極好的穩定性、黏結性以及可靠性的各向異性導電膜，一種製造其的方法，以及一種由其連接的半導體裝置。
根據本發明的一個實施例，提供一種各向異性導電膜的組成物或一種各向異性導電膜，其包含：包含氫化環氧樹脂的環 氧樹脂；由式1表示的陽離子聚合催化劑；以及由式2表示的化合物。
其中R1到R5各是氫原子、烷基、乙醯基、烷氧羰基、苯甲醯基或苯甲氧羰基；並且R6和R7各是烷基、苯甲基、鄰甲基苯甲基(o-methylbenzyl group)、間甲基苯甲基、對甲基苯甲基或萘甲基(naphthylmethyl group)。
其中R8到R12各是氫原子、烷基、乙醯基、烷氧羰基、苯甲醯基或苯甲氧羰基；R13和R14各是烷基、苯甲基、鄰甲基苯甲基、間甲基苯甲基、對甲基苯甲基或萘甲基；並且X1是鹵素原子或烷基硫酸。
根據本發明的另一實施例，提供一種各向異性導電膜，其在25℃下儲存170小時之後具有如由方程式1所表示的30%或小於30%的彈性模數變化率，並且具有60℃到85℃的差示掃描熱量計(differential scanning calorimeter，DSC)起始溫度。
[方程式1]彈性模數變化率(%)={(M1-M0)/M0}×100
其中M0是如在25℃下測量的所述各向異性導電膜的初始彈性模數(kgf/cm2)，並且M1是所述各向異性導電膜在25℃下單獨靜置170小時之後如在25℃下測量的所述膜的彈性模數(kgf/cm2)。具體而言，彈性模數變化為1%或大於1%至30%或少於30%。
根據本發明的另一實施例，提供一種包含以下各者的半導體裝置：具有第一電極的第一連接部件；具有第二電極的第二連接部件；以及安置在第一連接部件和第二連接部件之間以連接第一電極和第二電極的各向異性導電膜。
根據本發明的實施例，各向異性導電膜就儲存穩定性、耐濕性、耐熱性以及膜特性來說展示改良特性同時保證低溫快速固化，從而提供極好黏結性和連接可靠性的優勢。
3‧‧‧導電粒子
10‧‧‧黏結層
30‧‧‧半導體裝置
50‧‧‧第一連接部件
60‧‧‧第二連接部件
70‧‧‧第一電極
80‧‧‧第二電極
圖1是根據本發明的一個實施例的半導體裝置30的剖視圖，其包含具有第一電極70的第一連接部件50、具有第二電極80的第二連接部件60以及由安置在第一連接部件和第二連接部件之間以透過導電粒子3連接第一電極和第二電極的各向異性導電膜形成的黏結層10。
本發明的一個實施例涉及一種各向異性導電膜的組成物 或一種各向異性導電膜，其包含：包含氫化環氧樹脂的環氧樹脂；由式1表示的陽離子聚合催化劑；以及由式2表示的化合物。本發明的另一實施例涉及一種各向異性導電膜的組成物或一種各向異性導電膜，除如上文所闡述的組分外其更包含黏合劑樹脂。
其中R1到R5各是氫原子、烷基、乙醯基、烷氧羰基、苯甲醯基或苯甲氧羰基；並且R6和R7各是烷基、苯甲基、鄰甲基苯甲基、間甲基苯甲基、對甲基苯甲基或萘甲基。
其中R8到R12各是氫原子、烷基、乙醯基、烷氧羰基、苯甲醯基或苯甲氧羰基；R13和R14各是烷基、苯甲基、鄰甲基苯甲基、間甲基苯甲基、對甲基苯甲基或萘甲基；並且X1是鹵素原子或烷基硫酸。
根據本發明，氫化環氧樹脂特別包含氫化雙酚A型環氧樹脂和脂環族氫化環氧樹脂，例如環脂肪族(cycloaliphatic)環氧樹脂。環脂肪族環氧樹脂可以是具有結構的樹脂，例如脂環族二環氧乙縮醛(alicyclic diepoxy acetal)、脂環族二環氧己二酸酯(alicyclic diepoxy adipate)、脂環族二環氧羧酸酯(alicyclic diepoxy carboxylate)、二氧化乙烯環己烯(vinyl cyclohexene dioxide)等。
氫化雙酚A型環氧樹脂一般使用氫化雙酚A衍生物和表氯醇(epichlorohydrin)獲得，並且可以具有其中雙酚A分子中的雙鍵經氫分子取代的結構。
舉例來說，氫化雙酚A型環氧樹脂可以包含由式3表示的氫化雙酚A型環氧樹脂單體或由式4表示的氫化雙酚A型環氧樹脂寡聚物。
其中n在0.1到13範圍內。
氫化環氧樹脂可以具有150g/eq到1,200g/eq的環氧當量重量和900cps/25℃到12,000cps/25℃的黏度。
就固體含量來說，以各向異性導電組成物的總重量計，氫化環氧樹脂可以5重量%(wt%)到25重量%的量存在。此外，以100重量份環氧樹脂計，氫化環氧樹脂可以30重量份到60重量份，具體來說，35重量份到55重量份的量存在。在這個範圍內，就膜特性、耐濕性、耐熱性以及可靠性來說，各向異性導電膜可以具有優勢。具體來說，如果以100重量份環氧樹脂計，氫化環 氧樹脂的量大於60重量份，那麼由於其膜特性的劣化在初始階段和在可靠性評估之後各向異性導電膜可以展示增加的連接電阻。
根據本發明，可以另外使用除氫化環氧樹脂之外的另一環氧樹脂。環氧樹脂可以包含(但不限於)至少一種由以下所構成的族群中選出的環氧樹脂：雙酚型環氧樹脂、酚醛型環氧樹脂、縮水甘油基型(glycidyl type)環氧樹脂、脂肪族環氧樹脂、脂環族環氧樹脂以及芳香族環氧樹脂。
根據本發明，可以使用由式1表示的陽離子聚合催化劑。
其中R1到R5各是氫原子、烷基、乙醯基、烷氧羰基、苯甲醯基或苯甲氧羰基；並且R6和R7各是烷基、苯甲基、鄰甲基苯甲基、間甲基苯甲基、對甲基苯甲基或萘甲基。具體來說，R1到R5可以各是氫原子或烷基，並且R6和R7可以各是烷基、苯甲基、鄰甲基苯甲基、間甲基苯甲基、對甲基苯甲基或萘甲基。更具體來說，R1到R5可以各是氫原子，並且R6和R7可以各是烷基、苯甲基、鄰甲基苯甲基、間甲基苯甲基、對甲基苯甲基或萘甲基。由式1表示的陽離子聚合催化劑可以防止大量氟離子在陽離子聚合時排放，並且因此防止金屬線、連接墊等的腐蝕。此外，由式1表示的陽離子聚合催化劑在較低溫度下產生陽離子，並且因此允許各向異性導電膜在例如150℃或低於150℃，具體來說140℃或低於 140℃，更具體來說130℃或低於130℃的低溫下快速固化。
以100重量份氫化環氧樹脂計，由式1表示的陽離子聚合催化劑可以5重量份到30重量份，具體來說10重量份到25重量份的量存在。在這個範圍內，就儲存穩定性和低溫快速固化來說，各向異性導電膜可以具有優勢。
根據本發明，可以使用由式2表示的化合物。
其中R8到R12各是氫原子、烷基、乙醯基、烷氧羰基、苯甲醯基或苯甲氧羰基；R13和R14各是烷基、苯甲基、鄰甲基苯甲基、間甲基苯甲基、對甲基苯甲基或萘甲基；並且X1是鹵素原子或烷基硫酸。
具體來說，R8到R12可以各是氫原子或烷基，並且R13和R14可以各是烷基、苯甲基、鄰甲基苯甲基、間甲基苯甲基、對甲基苯甲基或萘甲基。更具體來說，R8到R12可以各是氫原子，R13和R14可以各是烷基、苯甲基、鄰甲基苯甲基、間甲基苯甲基、對甲基苯甲基或萘甲基，並且X1可以是烷基硫酸。歸因於由式1表示的聚合催化劑所產生的陽離子，各向異性導電膜甚至在室溫下可以固化，並且因此遭受儲存穩定性劣化。由式2表示的化合物通過捕捉由式1表示的聚合催化劑所產生的陽離子來抑制各向異性導電膜在室溫下固化，並且因此促成各向異性導電膜的儲存 穩定性改良。
以100重量份由式1表示的聚合催化劑計，由式2表示的化合物可以0.1重量份到30重量份，具體來說3重量份到10重量份的量存在。在這個範圍內，各向異性導電膜可以在不抑制其低溫快速固化的情況下展示改良儲存穩定性。
根據本發明的實施例的各向異性導電組成物或各向異性導電膜包含由式1表示的陽離子聚合催化劑和由式2表示的化合物，並且因此可以在低溫下固化並且展示改良的儲存穩定性和連接可靠性。
本發明的另一實施例涉及一種各向異性導電膜的組成物或一種各向異性導電膜，除如上文所闡述的組分外其更包含黏合劑樹脂。黏合劑樹脂的實例可以包含聚醯亞胺樹脂、聚醯胺樹脂、苯氧基樹脂、環氧樹脂、聚甲基丙烯酸酯樹脂、聚丙烯酸酯樹脂、聚氨基甲酸酯樹脂、丙烯酸酯改性的氨基甲酸酯樹脂、聚酯樹脂、聚酯氨基甲酸酯樹脂、聚乙烯縮丁醛(polyvinyl butyral)樹脂、苯乙烯-丁烯-苯乙烯(styrene-butylene-styrene，SBS)樹脂和其環氧化改性物、苯乙烯-乙烯-丁烯-苯乙烯(styrene-ethylene-butylene-styrene，SEBS)樹脂和其改性物、丙烯腈丁二烯橡膠(acrylonitrile butadiene rubber，NBR)或其氫化化合物等。這些可以單獨使用或以其組合形式使用。儘管較高重量平均分子量的黏合劑樹脂准許較容易地成膜，但本發明不限於特定重量平均分子量的黏合劑樹脂。舉例來說，黏合劑樹脂可能 具有具體來說5,000g/mol到150,000g/mol，更具體來說10,000g/mol到80,000g/mol的重量平均分子量。如果黏合劑樹脂的重量平均分子量小於5,000g/mol，那麼成膜可能受抑制，並且如果黏合劑樹脂的重量平均分子量大於150,000g/mol，那麼可能存在與其他組分的相容性不佳的問題。此外，以100重量份各向異性導電膜的組成物計，黏合劑樹脂可以20重量份到60重量份，具體來說，30重量份到50重量份的量存在。
根據本發明的另一實施例，提供一種各向異性導電膜的組成物或一種各向異性導電膜，除如上文所闡述的組分外其更包含導電粒子。舉例來說，導電粒子可以包含：包含Au、Ag、Ni、Cu以及Pb的金屬粒子；碳粒子；通過用金屬塗布聚合物樹脂獲得的粒子；通過將用金屬塗布聚合物樹脂獲得的粒子的表面絕緣處理獲得的粒子等。聚合物樹脂包含(但不限於)聚乙烯、聚丙烯、聚酯、聚苯乙烯以及聚乙烯醇。塗布聚合物樹脂的金屬包含(但不限於)Au、Ag、Ni、Cu以及Pb。
具體來說，在外部引線接合(outer lead bonding，OLB)的情況下，因為黏著物是氧化銦錫(ITO)玻璃表面，所以可以使用包含由塑膠組分製成的核的導電粒子來防止在各向異性導電膜連接過程中產生的壓力對ITO的損害。在連接PCB基底的情況下，可以使用金屬粒子，例如Ni粒子。在電漿顯示面板(plasma display panel，PDP)的情況下，由於應用到電路的極高壓，可以使用通過用金(Au)電鍍金屬粒子(例如Ni粒子)而獲得的導電 粒子。在玻璃上置晶片(chip on glass，COG)或晶粒軟模封裝(chip on film，COF)的情況下，可以使用通過用熱塑性樹脂覆蓋導電粒子表面而獲得的絕緣導電粒子。在一個實施例中，根據本發明的各向異性導電膜的組成物或各向異性導電膜可能適用於COG接合。
取決於所應用的電路的間距和目的，導電粒子的尺寸經測定在1微米到30微米，較佳為3微米到20微米的範圍內。就固體含量來說，以各向異性導電膜的組成物的總重量計，導電粒子可以1重量%到30重量%，具體來說1重量%到15重量%的量存在。在這個範圍內，各向異性導電膜可以保證穩定連接可靠性，並且防止在熱壓制時由間距之間的導電粒子的附聚(agglomeration)引起的電短路。
根據本發明的又一實施例，各向異性導電膜的組成物或各向異性導電膜除如上文所闡述的組分外可以更包含矽烷偶合劑。
矽烷偶合劑可以包含(但不限於)至少一種由以下所構成的族群中選出的物質：可聚合含氟基的矽化合物，例如乙烯基三甲氧基矽烷、乙烯基三乙氧基矽烷(vinyltriethoxysilane)以及(甲基)丙烯醯氧基丙基三甲氧基矽烷((meth)acryloxypropyltrimethoxysilane)；環氧基化矽化合物，例如3-縮水甘油氧基丙基三甲氧基矽烷(3-glycidoxypropyltrimethoxysilane)、3-縮水甘油氧基丙基甲基二 甲氧基矽烷(3-glycidoxypropylmethyldimethoxysilane)以及2-(3,4-環氧環己基)乙基三甲氧基矽烷(2-(3,4-epoxycyclohexyl)ethyltrimethoxysilane)；含氨基的矽化合物，例如3-氨基丙基三甲氧基矽烷(3-aminopropyltrimethoxysilane)、N-(2-氨基乙基)-3-氨基丙基三甲氧基矽烷(N-(2-aminoethyl)-3-aminopropyltrimethoxysilane)以及N-(2-氨基乙基)-3-氨基丙基甲基二甲氧基矽烷(N-(2-aminoethyl)-3-aminopropylmethyldimethoxysilane)；以及3-氯丙基三甲氧基矽烷(3-chloropropyltrimethoxysilane)。
就固體含量來說，以各向異性導電膜的組成物的總重量計，矽烷偶合劑可以1重量%到10重量%的量存在。
根據本發明的又一實施例，各向異性導電膜可以更包含添加劑，例如聚合抑制劑、抗氧化劑以及熱穩定劑，以在其基本特性不劣化的情況下展示額外特性。就固體含量來說，添加劑可以(但不限於)0.01重量%到10重量%的量存在於各向異性導電膜的組成物中。
聚合抑制劑的實例可以包含氫醌、氫醌單甲醚(hydroquinone monomethyl ether)、對苯醌、吩噻嗪以及其混合物。抗氧化劑可以包含酚類(phenolic)化合物、羥基肉桂酸酯(hydroxycinnamate)化合物等。抗氧化劑的實例可以包含四-(亞甲基-(3,5-二-叔丁基-4-羥基肉桂酸酯)甲烷(tetrakis-(methylene-(3,5-di-t-butyl-4-hydroxycinnamate)methane) 、3,5-雙(1,1-二甲基乙基)-4-羥基苯丙酸巰基二-2,1-乙烷二酯(3,5-bis(1,1-dimethylethyl)-4-hydroxybenzenepropanoic acid thioldi-2,1-ethanediyl ester)等。
根據本發明，各向異性導電膜可以包含由各向異性導電膜的組成物形成的各向異性導電黏結層，和離型膜。在將各向異性導電膜初步壓制到第一連接部件或第二連接部件時可以移除離型膜。因此，各向異性導電膜和各向異性導電黏結層可以在本文中相容地使用。
根據本發明，各向異性導電膜可能具有：包含一個各向異性導電黏結層的單層結構；其中不含有導電粒子的不導電黏結層和含有導電粒子的導電黏結層依序堆疊的雙層結構；或不導電黏結層堆疊於導電黏結層的兩個表面上的三層結構。本文所公開的各向異性導電膜的組成物可以用於不導電黏結層、導電黏結層或不導電黏結層和導電黏結層兩者。
本發明的又一實施例涉及一種各向異性導電膜，其在25℃下儲存170小時之後具有如由方程式1所表示的30%或小於30%的彈性模數變化率，並且具有60℃到85℃的差示掃描熱量計(DSC)起始溫度。
[方程式1]模數變化率(%)={(M1-M0)/M0}×100
其中M0是如在25℃下測量的所述各向異性導電膜的初始彈性模數(kgf/cm2)，並且M1是所述各向異性導電膜在25℃下單獨 靜置170小時之後如在25℃下測量的所述膜的彈性模數(kgf/cm2)。
30%或小於30%的彈性模數變化率與各向異性導電膜的儲存穩定性改良相關聯，並且60℃到85℃的DSC起始溫度與其低溫快速固化特性相關聯。如本文所用，DSC起始溫度是指在使用DSC測量各向異性導電膜的熱量以及溫度變化時，歸因於放熱反應，DSC曲線的斜率首次增加的時間點下的溫度。各向異性導電膜的初始彈性模數M0可以是100kgf/cm2到1200kgf/cm2，具體來說250kgf/cm2到750kgf/cm2。在這個初始彈性模數範圍內，各向異性導電膜可以展示改良的膜特性。
根據本發明的實施例，各向異性導電膜如上所述可以包含環氧樹脂，其包含氫化環氧樹脂；由式1表示的陽離子聚合催化劑以及由式2表示的化合物，並且可以更包含黏合劑樹脂或導電粒子。因此，細節(例如氫化環氧樹脂、由式1表示的陽離子聚合催化劑以及由式2表示的化合物的量和類型)也可以適用於本發明的這些實施例。此外，根據實施例的各向異性導電膜可以具有10倍到60倍的連接電阻增加比率，如由方程式2表示：[方程式2]連接電阻增加比率=T1/T0
其中T0是如在各向異性導電膜在150℃和70MPa下經受壓制5秒之後測量的連接電阻，並且T1是如在各向異性導電膜在85℃和85% RH下單獨靜置500小時之後測量的連接電阻。
本發明的又一實施例涉及一種包含以下各者的半導體裝置：具有第一電極的第一連接部件；具有第二電極的第二連接部件；以及本文所公開並且安置在第一連接部件和第二連接部件之間以連接第一電極和第二電極的各向異性導電膜。
第一連接部件和第二連接部件各包含需要電連接的電極。具體來說，第一連接部件和第二連接部件可以包含玻璃基底、塑膠基底、印刷電路板、陶瓷電路板、可撓性電路板、半導體矽晶片、IC晶片、驅動器IC晶片等，其上形成有電極，例如氧化銦錫(ITO)和氧化銦鋅(indium zinc oxide，IZO)。更具體來說，第一連接部件和第二連接部件中的一個可以是IC晶片或驅動器IC晶片，並且另一個可以是玻璃基底。
參考圖1，在半導體裝置30中，具有第一電極70的第一連接部件50和具有第二電極80的第二連接部件60可以借助安置在第一連接部件和第二連接部件之間以連接第一電極和第二電極的根據本發明實施例的各向異性導電層彼此接合。
本發明提供一種由各向異性導電膜組成物形成的各向異性導電膜。不需要特別設備或裝備來形成各向異性導電膜。舉例來說，包含各向異性導電黏結層和離型膜的各向異性導電膜可以通過以下方式獲得：將根據本發明的各向異性導電組成物溶解於有機溶劑(例如甲苯)中，在防止導電粒子粉碎的速度下以預定時間段攪拌所獲得的溶液，將溶液以某一厚度(例如10微米到50微米的厚度)塗布到離型膜上，並且以預定時間段乾燥溶液以蒸 發甲苯等。
離型膜可以包含例如聚烯烴膜，例如聚乙烯、聚丙烯、乙烯/丙烯共聚物、聚丁烯-1、乙烯/乙酸乙烯酯共聚物、聚乙烯/苯乙烯丁二烯橡膠的混合物、聚氯乙烯等。此外，離型膜可以包含：聚合物，例如聚對苯二甲酸乙二酯、聚碳酸酯、聚(甲基丙烯酸甲酯)等；熱塑性彈性體，例如聚氨基甲酸酯、聚醯胺-多元醇(polyamide-polyol)共聚物等；以及其混合物。離型膜可以具有任何適合厚度。舉例來說，離型膜的厚度可以是10微米到50微米。
隨後，將參考一些實例更詳細地描述本發明。應理解提供這些實例僅為了說明，並且不應以任何方式解釋為限制本發明。
為清楚起見，將省略對本領域的技術人員顯而易見的細節描述。
實例1：製造各向異性導電膜
將35重量%黏合劑(YP50，國都化學株式會社(Kukdo Chemical Co.,Ltd.))、20重量%氫化環氧樹脂(ST-3000，國都化學株式會社)、20.8重量%環氧丙烷系環氧樹脂(EP-4000S，艾迪科株式會社(Adeka Co.,Ltd.))、4重量%固化催化劑(SI-B3A，三信化學株式會社(Sanshin Chemical Co.,Ltd.))、0.2重量%穩定劑(SI-S，三信化學株式會社)、20重量%導電粒子(AUL704F，積水株式會社(Sekisui Co.,Ltd.))以及作為溶劑的丙二醇單甲醚乙酸酯(propylene glycol monomethyl ether acetate，PGMEA)混 合。將所獲得的混合液體塗布到離型膜上，隨後在乾燥器中在60℃下乾燥以使溶劑揮發，從而獲得各向異性導電膜(塗層厚度：10微米)。
實例2：製造各向異性導電膜
以與實例1中相同的方式製造各向異性導電膜，但其中改為使用SI-B2A(三信化學株式會社)代替SI-B3A作為固化催化劑。
實例3：製造各向異性導電膜
以與實例1中相同的方式製造各向異性導電膜，但其中改為使用S-ME(三信化學株式會社)代替SI-S作為穩定劑。
比較例1：製造各向異性導電膜
以與實例1中相同的方式製造各向異性導電膜，但其中改為使用縮水甘油胺型(glycidyl amine-type)環氧樹脂(SE-300P，西納T和C有限公司(SHINA T&C Co.,Ltd.))代替ST-3000的氫化環氧樹脂。
比較例2：製造各向異性導電膜
以與實例1中相同的方式製造各向異性導電膜，但其中改為不使用穩定劑並且以4.2重量%的量使用固化催化劑。
比較例3：製造各向異性導電膜
以與實例1中相同的方式製造各向異性導電膜，但其中改為使用亞甲基雙(methylenebis)(苯胺)(MDA-220，國都化學株式會社)代替SI-S作為穩定劑。
實驗實例：各向異性導電膜的特性評估
使用關於DSC起始溫度、在25℃下170小時之後的彈性模數變化率、連接電阻以及在可靠性評估之後的連接電阻的以下方法評估在實例1到實例3和比較例1到比較例3中製造的每一各向異性導電膜中。結果顯示於表1中。
DSC起始溫度
DSC起始溫度定義為在使用差示掃描式熱量計型號Q20(TA儀器(TA Instruments))以10℃/min的速率在0℃到300℃的溫度範圍內在氮氣環境下測量各向異性導電膜黏結層的熱量時，歸因於產熱，DSC曲線的斜率首次增加的時間點下的溫度。
在25℃下170小時之後的彈性模數變化率
通過使用UTM設備在室溫(25℃)下以5mm/min的速度在兩末端以180°的方向拉動來測量尺寸是2毫米×10毫米×10微米(寬度×長度×厚度)的各向異性導電膜的黏結層在25℃下的初始彈性模數(M0)。此處，使用100N UTM夾具進行測量，並由最大應力的一半的點的斜率來計算初始彈性模數，亦即，(最大應力的一半應力值-初始應力值)/(最大應力的一半的點的應變值)。隨後，在膜於25℃下靜置170小時之後以上述相同方式測量在25℃下的彈性模數(M1)。隨後，以百分比形式計算在170小時之後相對於初始彈性模數的彈性模數變化率。
連接電阻和在可靠性評估之後的連接電阻
為了評估各向異性導電膜的連接電阻，將包含具有1200 平方微米的凸塊區域和2000埃的厚度的氧化銦錫(ITO)電路的玻璃基底和具有1200平方微米的凸塊區域和1.5毫米的厚度的IC晶片放置在各向異性導電膜的上表面和下表面上，隨後在150℃和70Mpa的條件下壓制並且加熱5秒，從而每個樣品製造5個樣本。測量各樣本中的初始連接電阻(T0)。
此外，針對可靠性評估，將電路連接產品在85℃和85% RH下於高溫高濕度箱中靜置500小時，隨後以與上述相同的方式測量在可靠性評估之後的連接電阻(T1)。
使用電阻測試儀型號2000萬用表(multimeter)(吉時利有限公司(Keithley Co.,Ltd.))通過4點探針法(4-point probe method)測量連接電阻，其中使用與測試儀(ASTM F43-64T)連接的四個探針測量四點之間的電阻。使用通過應用1mA的測試電流測量的電壓來計算電阻，其又展現在測試儀上。
如表1中所示，實例1到實例3的各向異性導電膜的DSC起始溫度是60℃到85℃並且因此允許在低溫下固化。此外，實例1到實例3的各向異性導電膜在初始階段和在可靠性評估之後當在低溫快速固化條件下經受初步和主要壓制時展示極好的連 接電阻，並且展示極好的儲存穩定性，因為固化反應由於在25℃下170小時之後的小於30%的彈性模數變化率而未出現。另一方面，未使用氫化環氧樹脂的比較例1的各向異性導電膜在可靠性評估之後在低溫快速固化條件下初步並且主要壓制時連接失敗。此外，不含有穩定劑的比較例2的各向異性導電膜展示儲存穩定性劣化。另外，對於比較例3的各向異性導電膜來說，認為因陽離子聚合催化劑產生的路易士酸(Lewis acid)所致的環氧樹脂的聚合延遲，歸因於具有未共用電子對(例如N和O)的化合物與陽離子聚合催化劑的反應。因此，比較例3的各向異性導電膜在初始階段展示不佳的連接電阻和在可靠性評估之後在低溫接合時連接失敗。
3‧‧‧導電粒子
10‧‧‧黏結層
30‧‧‧半導體裝置
50‧‧‧第一連接部件
60‧‧‧第二連接部件
70‧‧‧第一電極
80‧‧‧第二電極

Claims (10)

  1. 一種各向異性導電膜，其在25℃下儲存170小時之後具有如由方程式1所表示的30%或小於30%的模數變化率以及具有60℃到85℃的差示掃描熱量計起始溫度，[方程式1]彈性模數變化率(%)={(M1-M0)/M0}×100其中M0是如在25℃下測量的所述各向異性導電膜的初始彈性模數，以及M1是所述各向異性導電膜在25℃下單獨靜置170小時之後如在25℃下測量的所述各向異性導電膜的彈性模數，且其中所述各向異性導電膜包括：包括氫化環氧樹脂的環氧樹脂；由式1表示的陽離子聚合催化劑；以及由式2表示的化合物， 其中R1到R5各是氫原子、烷基、乙醯基、烷氧羰基、苯甲醯基或苯甲氧羰基；以及R6以及R7各是烷基、苯甲基、鄰甲基苯甲基、間甲基苯甲基、對甲基苯甲基或萘甲基， 其中R8到R12各是氫原子、烷基、乙醯基、烷氧羰基、苯 甲醯基或苯甲氧羰基；R13以及R14各是烷基、苯甲基、鄰甲基苯甲基、間甲基苯甲基、對甲基苯甲基或萘甲基；以及X1是鹵素原子或烷基硫酸，其中所述各向異性導電膜具有10倍到60倍的連接電阻增加比率，如由方程式2表示：[方程式2]連接電阻增加比率=T1/T0其中T0是如在各向異性導電膜在150℃和70MPa下經受壓制5秒之後測量的連接電阻，並且T1是如在各向異性導電膜在85℃和85% RH下單獨靜置500小時之後測量的連接電阻。
  2. 如申請專利範圍第1項所述的各向異性導電膜，其中R1到R5各是氫原子，以及R6以及R7各是烷基、苯甲基、鄰甲基苯甲基、間甲基苯甲基、對甲基苯甲基或萘甲基。
  3. 如申請專利範圍第1項所述的各向異性導電膜，其中R8到R12各是氫原子，R13以及R14各是烷基、苯甲基、鄰甲基苯甲基、間甲基苯甲基、對甲基苯甲基或萘甲基；以及X1是烷基硫酸。
  4. 如申請專利範圍第1項至第3項中任一項所述的各向異性導電膜，其中以100重量份所述環氧樹脂計，所述氫化環氧樹脂以30重量份到60重量份的量存在。
  5. 如申請專利範圍第1項至第3項中任一項所述的各向異性導電膜，其中所述氫化環氧樹脂是由式3表示的氫化雙酚A型環氧樹脂單體或由式4表示的氫化雙酚A型環氧樹脂寡聚物，[式3] 其中n在0.1到13範圍內。
  6. 如申請專利範圍第1項所述的各向異性導電膜，其中所述各向異性導電膜更包括黏合劑樹脂以及導電粒子。
  7. 如申請專利範圍第6項所述的各向異性導電膜，其中所述各向異性導電膜包括：就固體含量來說以所述各向異性導電膜的組成物的總重量計，20重量%到50重量%所述環氧樹脂；以100重量份所述環氧樹脂計，30重量份到60重量份所述氫化環氧樹脂；以100重量份所述氫化環氧樹脂計，5重量份到30重量份由式1表示的所述陽離子聚合催化劑；以100重量份由式1表示的所述陽離子聚合催化劑計，0.1重量份到30重量份由式2表示的所述化合物；25重量%到60重量%所述黏合劑樹脂；以及1重量%到30重量%所述導電粒子。
  8. 如申請專利範圍第1項至第3項中任一項所述的各向異性導電膜，其中所述各向異性導電膜的初始彈性模數M0是100kgf/cm2到1200kgf/cm2。
  9. 一種半導體裝置，包括：第一連接部件，具有第一電極； 第二連接部件，具有第二電極；以及如申請專利範圍第1項至第3項中任一項所述的各向異性導電膜，安置在所述第一連接部件以及所述第二連接部件之間以連接所述第一電極以及所述第二電極。
  10. 如申請專利範圍第9項所述的半導體裝置，其中所述第一連接部件以及所述第二連接部件中的一個包括IC晶片或驅動器IC晶片，以及另一個包括玻璃基底。
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