JP7465365B2 - 銅箔積層板(ccl)用低誘電複合フィルムおよびこれを含む低誘電銅箔積層板(ccl) - Google Patents
銅箔積層板(ccl)用低誘電複合フィルムおよびこれを含む低誘電銅箔積層板(ccl) Download PDFInfo
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- JP7465365B2 JP7465365B2 JP2022553115A JP2022553115A JP7465365B2 JP 7465365 B2 JP7465365 B2 JP 7465365B2 JP 2022553115 A JP2022553115 A JP 2022553115A JP 2022553115 A JP2022553115 A JP 2022553115A JP 7465365 B2 JP7465365 B2 JP 7465365B2
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- polyimide
- porous substrate
- low dielectric
- core layer
- layer
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- 239000002131 composite material Substances 0.000 title claims description 53
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 title claims description 42
- 239000011889 copper foil Substances 0.000 title claims description 33
- 239000004642 Polyimide Substances 0.000 claims description 83
- 229920001721 polyimide Polymers 0.000 claims description 83
- 239000000758 substrate Substances 0.000 claims description 62
- 239000012792 core layer Substances 0.000 claims description 40
- 239000010410 layer Substances 0.000 claims description 40
- 239000011159 matrix material Substances 0.000 claims description 40
- 239000002245 particle Substances 0.000 claims description 30
- 239000012790 adhesive layer Substances 0.000 claims description 25
- 239000000919 ceramic Substances 0.000 claims description 20
- 239000011148 porous material Substances 0.000 claims description 18
- WKDNYTOXBCRNPV-UHFFFAOYSA-N bpda Chemical group C1=C2C(=O)OC(=O)C2=CC(C=2C=C3C(=O)OC(C3=CC=2)=O)=C1 WKDNYTOXBCRNPV-UHFFFAOYSA-N 0.000 claims description 16
- CBCKQZAAMUWICA-UHFFFAOYSA-N 1,4-phenylenediamine Chemical compound NC1=CC=C(N)C=C1 CBCKQZAAMUWICA-UHFFFAOYSA-N 0.000 claims description 13
- 229920000295 expanded polytetrafluoroethylene Polymers 0.000 claims description 12
- ANSXAPJVJOKRDJ-UHFFFAOYSA-N furo[3,4-f][2]benzofuran-1,3,5,7-tetrone Chemical compound C1=C2C(=O)OC(=O)C2=CC2=C1C(=O)OC2=O ANSXAPJVJOKRDJ-UHFFFAOYSA-N 0.000 claims description 12
- 238000000691 measurement method Methods 0.000 claims description 12
- VQVIHDPBMFABCQ-UHFFFAOYSA-N 5-(1,3-dioxo-2-benzofuran-5-carbonyl)-2-benzofuran-1,3-dione Chemical compound C1=C2C(=O)OC(=O)C2=CC(C(C=2C=C3C(=O)OC(=O)C3=CC=2)=O)=C1 VQVIHDPBMFABCQ-UHFFFAOYSA-N 0.000 claims description 11
- QQGYZOYWNCKGEK-UHFFFAOYSA-N 5-[(1,3-dioxo-2-benzofuran-5-yl)oxy]-2-benzofuran-1,3-dione Chemical compound C1=C2C(=O)OC(=O)C2=CC(OC=2C=C3C(=O)OC(C3=CC=2)=O)=C1 QQGYZOYWNCKGEK-UHFFFAOYSA-N 0.000 claims description 11
- 229910052802 copper Inorganic materials 0.000 claims description 9
- 239000010949 copper Substances 0.000 claims description 9
- YCKRFDGAMUMZLT-UHFFFAOYSA-N Fluorine atom Chemical compound [F] YCKRFDGAMUMZLT-UHFFFAOYSA-N 0.000 claims description 8
- 229910052731 fluorine Inorganic materials 0.000 claims description 8
- 239000011737 fluorine Substances 0.000 claims description 8
- YGYCECQIOXZODZ-UHFFFAOYSA-N 4415-87-6 Chemical compound O=C1OC(=O)C2C1C1C(=O)OC(=O)C12 YGYCECQIOXZODZ-UHFFFAOYSA-N 0.000 claims description 6
- -1 Dicarboxyphenyl hydroquinone Chemical compound 0.000 claims description 6
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- 239000013074 reference sample Substances 0.000 claims description 5
- VLDPXPPHXDGHEW-UHFFFAOYSA-N 1-chloro-2-dichlorophosphoryloxybenzene Chemical compound ClC1=CC=CC=C1OP(Cl)(Cl)=O VLDPXPPHXDGHEW-UHFFFAOYSA-N 0.000 claims description 4
- XUSNPFGLKGCWGN-UHFFFAOYSA-N 3-[4-(3-aminopropyl)piperazin-1-yl]propan-1-amine Chemical compound NCCCN1CCN(CCCN)CC1 XUSNPFGLKGCWGN-UHFFFAOYSA-N 0.000 claims description 4
- HHLMWQDRYZAENA-UHFFFAOYSA-N 4-[4-[2-[4-(4-aminophenoxy)phenyl]-1,1,1,3,3,3-hexafluoropropan-2-yl]phenoxy]aniline Chemical compound C1=CC(N)=CC=C1OC1=CC=C(C(C=2C=CC(OC=3C=CC(N)=CC=3)=CC=2)(C(F)(F)F)C(F)(F)F)C=C1 HHLMWQDRYZAENA-UHFFFAOYSA-N 0.000 claims description 4
- QHHKLPCQTTWFSS-UHFFFAOYSA-N 5-[2-(1,3-dioxo-2-benzofuran-5-yl)-1,1,1,3,3,3-hexafluoropropan-2-yl]-2-benzofuran-1,3-dione Chemical compound C1=C2C(=O)OC(=O)C2=CC(C(C=2C=C3C(=O)OC(=O)C3=CC=2)(C(F)(F)F)C(F)(F)F)=C1 QHHKLPCQTTWFSS-UHFFFAOYSA-N 0.000 claims description 4
- CHJAYYWUZLWNSQ-UHFFFAOYSA-N 1-chloro-1,2,2-trifluoroethene;ethene Chemical group C=C.FC(F)=C(F)Cl CHJAYYWUZLWNSQ-UHFFFAOYSA-N 0.000 claims description 3
- LJMPOXUWPWEILS-UHFFFAOYSA-N 3a,4,4a,7a,8,8a-hexahydrofuro[3,4-f][2]benzofuran-1,3,5,7-tetrone Chemical compound C1C2C(=O)OC(=O)C2CC2C(=O)OC(=O)C21 LJMPOXUWPWEILS-UHFFFAOYSA-N 0.000 claims description 3
- HLBLWEWZXPIGSM-UHFFFAOYSA-N 4-Aminophenyl ether Chemical compound C1=CC(N)=CC=C1OC1=CC=C(N)C=C1 HLBLWEWZXPIGSM-UHFFFAOYSA-N 0.000 claims description 3
- WUPRYUDHUFLKFL-UHFFFAOYSA-N 4-[3-(4-aminophenoxy)phenoxy]aniline Chemical compound C1=CC(N)=CC=C1OC1=CC=CC(OC=2C=CC(N)=CC=2)=C1 WUPRYUDHUFLKFL-UHFFFAOYSA-N 0.000 claims description 3
- JCRRFJIVUPSNTA-UHFFFAOYSA-N 4-[4-(4-aminophenoxy)phenoxy]aniline Chemical compound C1=CC(N)=CC=C1OC(C=C1)=CC=C1OC1=CC=C(N)C=C1 JCRRFJIVUPSNTA-UHFFFAOYSA-N 0.000 claims description 3
- KMKWGXGSGPYISJ-UHFFFAOYSA-N 4-[4-[2-[4-(4-aminophenoxy)phenyl]propan-2-yl]phenoxy]aniline Chemical compound C=1C=C(OC=2C=CC(N)=CC=2)C=CC=1C(C)(C)C(C=C1)=CC=C1OC1=CC=C(N)C=C1 KMKWGXGSGPYISJ-UHFFFAOYSA-N 0.000 claims description 3
- MQAHXEQUBNDFGI-UHFFFAOYSA-N 5-[4-[2-[4-[(1,3-dioxo-2-benzofuran-5-yl)oxy]phenyl]propan-2-yl]phenoxy]-2-benzofuran-1,3-dione Chemical compound C1=C2C(=O)OC(=O)C2=CC(OC2=CC=C(C=C2)C(C)(C=2C=CC(OC=3C=C4C(=O)OC(=O)C4=CC=3)=CC=2)C)=C1 MQAHXEQUBNDFGI-UHFFFAOYSA-N 0.000 claims description 3
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- CXISKMDTEFIGTG-UHFFFAOYSA-N [4-(1,3-dioxo-2-benzofuran-5-carbonyl)oxyphenyl] 1,3-dioxo-2-benzofuran-5-carboxylate Chemical compound C1=C2C(=O)OC(=O)C2=CC(C(OC=2C=CC(OC(=O)C=3C=C4C(=O)OC(=O)C4=CC=3)=CC=2)=O)=C1 CXISKMDTEFIGTG-UHFFFAOYSA-N 0.000 claims description 3
- HQQADJVZYDDRJT-UHFFFAOYSA-N ethene;prop-1-ene Chemical group C=C.CC=C HQQADJVZYDDRJT-UHFFFAOYSA-N 0.000 claims description 3
- XUCNUKMRBVNAPB-UHFFFAOYSA-N fluoroethene Chemical group FC=C XUCNUKMRBVNAPB-UHFFFAOYSA-N 0.000 claims description 3
- 229920001343 polytetrafluoroethylene Polymers 0.000 claims 1
- 239000004810 polytetrafluoroethylene Substances 0.000 claims 1
- 229920005575 poly(amic acid) Polymers 0.000 description 14
- 238000000034 method Methods 0.000 description 7
- 150000004985 diamines Chemical class 0.000 description 6
- 238000010438 heat treatment Methods 0.000 description 6
- 238000005259 measurement Methods 0.000 description 6
- 238000010295 mobile communication Methods 0.000 description 6
- ZMXDDKWLCZADIW-UHFFFAOYSA-N N,N-Dimethylformamide Chemical compound CN(C)C=O ZMXDDKWLCZADIW-UHFFFAOYSA-N 0.000 description 5
- 238000005470 impregnation Methods 0.000 description 5
- 238000006116 polymerization reaction Methods 0.000 description 5
- 238000002360 preparation method Methods 0.000 description 5
- NVKGJHAQGWCWDI-UHFFFAOYSA-N 4-[4-amino-2-(trifluoromethyl)phenyl]-3-(trifluoromethyl)aniline Chemical compound FC(F)(F)C1=CC(N)=CC=C1C1=CC=C(N)C=C1C(F)(F)F NVKGJHAQGWCWDI-UHFFFAOYSA-N 0.000 description 4
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 4
- QIGBRXMKCJKVMJ-UHFFFAOYSA-N Hydroquinone Chemical compound OC1=CC=C(O)C=C1 QIGBRXMKCJKVMJ-UHFFFAOYSA-N 0.000 description 4
- WYURNTSHIVDZCO-UHFFFAOYSA-N Tetrahydrofuran Chemical compound C1CCOC1 WYURNTSHIVDZCO-UHFFFAOYSA-N 0.000 description 4
- 230000005540 biological transmission Effects 0.000 description 4
- 230000000052 comparative effect Effects 0.000 description 4
- 238000005516 engineering process Methods 0.000 description 4
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- ZWEHNKRNPOVVGH-UHFFFAOYSA-N 2-Butanone Chemical compound CCC(C)=O ZWEHNKRNPOVVGH-UHFFFAOYSA-N 0.000 description 3
- CSCPPACGZOOCGX-UHFFFAOYSA-N Acetone Chemical compound CC(C)=O CSCPPACGZOOCGX-UHFFFAOYSA-N 0.000 description 3
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- FXHOOIRPVKKKFG-UHFFFAOYSA-N N,N-Dimethylacetamide Chemical compound CN(C)C(C)=O FXHOOIRPVKKKFG-UHFFFAOYSA-N 0.000 description 3
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- GTDPSWPPOUPBNX-UHFFFAOYSA-N ac1mqpva Chemical compound CC12C(=O)OC(=O)C1(C)C1(C)C2(C)C(=O)OC1=O GTDPSWPPOUPBNX-UHFFFAOYSA-N 0.000 description 3
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- OZJPLYNZGCXSJM-UHFFFAOYSA-N 5-valerolactone Chemical compound O=C1CCCCO1 OZJPLYNZGCXSJM-UHFFFAOYSA-N 0.000 description 2
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- 150000008064 anhydrides Chemical class 0.000 description 2
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- MVPPADPHJFYWMZ-UHFFFAOYSA-N chlorobenzene Chemical compound ClC1=CC=CC=C1 MVPPADPHJFYWMZ-UHFFFAOYSA-N 0.000 description 2
- 238000010276 construction Methods 0.000 description 2
- JHIVVAPYMSGYDF-UHFFFAOYSA-N cyclohexanone Chemical compound O=C1CCCCC1 JHIVVAPYMSGYDF-UHFFFAOYSA-N 0.000 description 2
- 229910003460 diamond Inorganic materials 0.000 description 2
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- 238000001035 drying Methods 0.000 description 2
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Classifications
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- 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
- C08J9/00—Working-up of macromolecular substances to porous or cellular articles or materials; After-treatment thereof
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Description
380℃で60分の間イミド化させた基準試料のイミド化率を100%と想定し、ポリイミド系マトリックスに対して赤外線分光器を通じて波長1,700cm-1および1,615cm-1のピークの大きさを測定した後、下記の数学式1によりPI indexを計算した後、下記の数学式2によりイミド化率を計算する。
380℃で60分の間イミド化させた基準試料のイミド化率を100%と想定し、ポリイミド系マトリックスに対して赤外線分光器を通じて波長1,700cm-1および1,615cm-1のピークの大きさを測定した後、下記の数学式1によりPI indexを計算した後、下記の数学式2によりイミド化率を計算する。
まず、重合溶媒であるDMAcに窒素雰囲気下でpPDAおよびODAを投入した後、常温で完全に溶解させ、BPDAを30分かけて投入する。前記溶液を10分の間撹拌した後、PMDAを30分かけて投入する。その後20℃以下の温度で16時間の間反応させてポリアミック酸溶液を製造した。これを通じて固形分含量が15重量%で、25℃で粘度が3500cpsであるポリアミック酸溶液を収得した後、チョンステクノピルのMINIFLOWフィルタで(CTS-CAP10 A grade)フィルタリングし、最終的に固形分含量が15重量%である含浸溶液を製造した。
イミド化率はフーリエ変換赤外線分光器(FT-IR)を使って分析し、380℃で60分の間イミド化させた基準試料のイミド化率を100%と想定し、ポリイミド系マトリックスに対して赤外線分光器を通じて波長1,700cm-1および1,615cm-1のピークの大きさを測定した後、下記の数学式1によりPI indexを計算し、下記の数学式2によりイミド化率を計算した。
実施例1と同様に実施して製造するものの、多孔性基材の重量%、体積%、ポリイミド系層の体積%、ポリイミド系層の総厚さと多孔性基材の厚さの厚さ比、ポリイミド系マトリックスのイミド化率、多孔性基材を含むか否かおよびポリイミド系マトリックスを含むか否かなどを変更して表1~表3のような低誘電複合フィルムを製造した。
実施例および比較例により製造したそれぞれの低誘電複合フィルムに対して、下記の物性を評価して表1~表3に示した。
それぞれの低誘電複合フィルムに対してネットワークアナライザー(E8364A(45MHz~50GHz)、Agilent Technologies社)を使って共振空胴(Resonant cavity)を通じてフィルム形態のサンプルをギガヘルツ(GHz)領域で誘電率および誘電損失を測定した。
それぞれの低誘電複合フィルムに対して万能材料試験機(Universal Testing Machine、UTM)を使ってASTM-D882規格に基づいて引張強度を測定した。
それぞれの低誘電複合フィルムに対して熱機械的分析装置(Pyris Diamond TMA、Perkin Elmer instrument)を通じて熱膨張係数を測定した。窒素気流下で昇温条件10℃/minで30~400℃範囲で測定した後、50~250℃間での平均値を算出した。
実施例1と同様に実施して製造するものの、実施例1のジアンハイドライドであるBPDAとPMDAを、BPDAとODPA(実施例14)、BPDAとBTDA(実施例15)、BPDAと6FDA(実施例16)、PMDAとODPA(実施例17)、PMDAとBTDA(実施例18)、PMDAと6FDA(実施例19)に変更して低誘電複合フィルムを製造した。
実施例1と同様に実施して製造するものの、実施例1のジアミンであるpPDAとODAを、pPDAとTFDB(実施例20)および、ODAとTFDB(実施例21)に変更して低誘電複合フィルムを製造した。
実施例1と同様に実施して製造するものの、実施例1のジアンハイドライドであるBPDAとPMDAを、6FDA(実施例22)および、ODPA(実施例23)、BTDA(実施例24)に変更してそれぞれ単独で適用されたポリアミック酸を製造して低誘電複合フィルムを製造した。
実施例1と同様に実施して製造するものの、実施例1のジアミンであるpPDAとODAを、TFDB(実施例25)および、BAPP(実施例26)に変更してそれぞれ単独で適用されたポリアミック酸を製造して低誘電複合フィルムを製造した。
実施例14~26により製造したそれぞれの低誘電複合フィルムに対して、下記の物性を評価して表4および表5に示した。
それぞれの低誘電複合フィルムに対してネットワークアナライザー(E8364A(45MHz~50GHz)、Agilent Technologies社)を使って共振空胴(Resonant cavity)を通じてフィルム形態のサンプルをギガヘルツ(GHz)領域で誘電率および誘電損失を測定した。
それぞれの低誘電複合フィルムに対して万能材料試験機(Universal Testing Machine、UTM)を使ってASTM-D882規格に基づいて引張強度を測定した。
それぞれの低誘電複合フィルムに対して熱機械的分析装置(Pyris Diamond TMA、Perkin Elmer instrument)を通じて熱膨張係数を測定した。窒素気流下で昇温条件10℃/minで30~400℃範囲で測定した後、50~250℃間での平均値を算出した。
実施例1により製造した低誘電複合フィルムの上部面に、潜在性硬化剤およびアクリル樹脂が含まれた1液型のエポキシ溶液をコーティングした後、温度100℃で乾燥して厚さが6μmである接着層を具備する低誘電複合フィルムを製造した。ここで1液型エポキシ100重量部に対して潜在性硬化剤であるDICY(dicyandiamide)およびアクリル樹脂10重量部を含む。この時、製造された低誘電複合フィルム全体体積に対して接着層が6体積%であった。
製造例1と同様に実施して製造するものの、低誘電複合フィルム全体体積に対する接着層の体積%を変更して下記の表6のような低誘電複合フィルムを製造した。
前記製造例1~6により製造した低誘電複合フィルムに対して下記の物性を評価して下記の表6に示した。
それぞれの低誘電複合フィルムに対してネットワークアナライザー(E8364A(45MHz~50GHz)、Agilent Technologies社)を使って共振空胴(Resonant cavity)を通じてフィルム形態のサンプルをギガヘルツ(GHz)領域で誘電率および誘電損失を測定した。
製造例に係るそれぞれの低誘電複合フィルムに対してIPC-TM-650 2.4.9.1の評価規格に基づいて90度方向で引き上げて銅層が剥離される時点を測定して評価した。
Claims (12)
- 拡張型ポリテトラフルオロエチレン(ePTFE)を含み、多数個の気孔を具備する多孔性基材および、ポリイミド系化合物を含んで形成され、前記多孔性基材の気孔に充填されるポリイミド系マトリックスを具備するコア層を含み、
前記コア層は前記多孔性基材の上面および下面のうちいずれか一面以上に備えられ、前記ポリイミド系マトリックスから由来したポリイミド系層をさらに含み、
前記コア層全体重量に対して、前記多孔性基材が20~85重量%であり、
前記コア層全体体積に対して、前記多孔性基材が15~80体積%であり、
前記コア層全体体積に対して、前記ポリイミド系層が8~40体積%であり、
前記ポリイミド系マトリックスは下記の測定方法1により測定したイミド化率が90%以上である、銅箔積層板(CCL)用低誘電複合フィルム:
[測定方法1]
380℃で60分の間イミド化させた基準試料のイミド化率を100%と想定し、前記ポリイミド系マトリックスに対して赤外線分光器を通じて波長1,700cm -1 および1,615cm -1 のピークの大きさを測定した後、下記の数学式1によりPI indexを計算した後、下記の数学式2によりイミド化率を計算する。
- 前記多孔性基材は、
MD方向の引張強度およびTD方向の引張強度の比が1:0.4~2.5である、請求項1に記載の銅箔積層板(CCL)用低誘電複合フィルム。 - 前記ポリイミド系層の総厚さと前記多孔性基材の厚さは厚さ比が1:0.2~12である、請求項1に記載の銅箔積層板(CCL)用低誘電複合フィルム。
- 前記コア層は前記多孔性基材の上面および下面にそれぞれ第1ポリイミド系層および第2ポリイミド系層を含み、
前記第1ポリイミド系層と第2ポリイミド系層は厚さ比が1:0.5~1.5である、請求項1に記載の銅箔積層板(CCL)用低誘電複合フィルム。 - 前記コア層の一面または両面に接着層をさらに含む、請求項1に記載の銅箔積層板(CCL)用低誘電複合フィルム。
- 前記ポリイミド系マトリックスは、
BPDA(3,3’,4,4’-Biphenyltetracarboxylic dianhydride)、PMDA(Pyromellitic dianhydride)、ODPA(4,4’-oxydiphthalic anhydride)、BTDA(3,3’,4,4’-benzophenone tetracarboxylic dianhydride)、BPADA(2,2-Bis[4-(3,4-Dicarboxyphenoxy)Phenyl]Propane Dianhydride)、TAHQ(Ditricarboxylic anhydride hydroquinone ester)、6FDA(2,2-bis(3,4-anhydrodicarboxyphenyl)hexafluoropropane)、CBDA(cyclobutane-1,2,3,4-tetracarboxylic dianhydride)およびCHDA(1,2,4,5-Cyclohexanetetracarboxylic Dianhydride)からなる群から選択された1種以上を含むジアンハイドライドおよび、
pPDA(paraphenylene diamine)、ODA(4,4’-Oxydianiline)、TPE-R(1,3-Bis(4-aminophenoxy)benzene)、TPE-Q(1,4-Bis(4-aminophenoxy)benzene)、BAPP(2,2-Bis[4-(4-aminophenoxy)Phenyl]Propane)、M-Tolidine(2,2’-Dimethyl-4,4’-diaminobiphenyl)、O-Tolidine(3,3’-Dimethyl-4,4’-diaminobiphenyl)、TFDB(2,2’-bis(trifluoromethyl)-[1,1’-biphenyl]-4,4’-diamine)およびHFBAPP(2,2-Bis[4-(4-aminophenoxy)phenyl] hexafluoropropane)からなる群から選択された1種以上を含むジアミンの重合を通じて形成されたポリアミック酸がイミド化されて形成されている、請求項1に記載の銅箔積層板(CCL)用低誘電複合フィルム。 - 前記コア層および接着層全体体積に対して、前記接着層が2~40体積%である、請求項5に記載の銅箔積層板(CCL)用低誘電複合フィルム。
- 前記ポリイミド系マトリックスはフッ素系粒子およびセラミック粒子のうちいずれか一つ以上を含む、請求項1に記載の銅箔積層板(CCL)用低誘電複合フィルム。
- 前記フッ素系粒子は、
フルオロエチレン(PTFE)、ペルフルオロアルコキシ共重合体(PFA、MFA、perfluoroalkoxy copolymer)、フッ素化エチレンプロピレン共重合体(FEP、fluorinated ethylene propylene copolymer)、エチレン-テトラフルオロエチレン共重合体(ETFE、ethylene tetrafluoroethylene copolymer)およびエチレン-クロロトリフルオロエチレン共重合体(ECTFE、ethylene chlorotrifluoroethylene copolymer)からなる群から選択された1種以上を含む、請求項8に記載の銅箔積層板(CCL)用低誘電複合フィルム。 - 前記セラミック粒子は、
B、Na、Mg、Al、Si、P、K、CaおよびTiからなる群から選択された1種以上の元素を含むセラミック粒子である、請求項8に記載の銅箔積層板(CCL)用低誘電複合フィルム。 - 前記セラミック粒子は中空型セラミック粒子および非中空型セラミック粒子のうちいずれか一つ以上を含む、請求項8に記載の銅箔積層板(CCL)用低誘電複合フィルム。
- 拡張型ポリテトラフルオロエチレン(ePTFE)を含み、多数個の気孔を具備する多孔性基材および、ポリイミド系化合物を含んで形成され、前記多孔性基材の気孔に充填されるポリイミド系マトリックスを具備するコア層と、
前記コア層の一面または両面に備えられる銅箔と、
前記コア層と銅箔の間に介在される接着層とを含み、
前記コア層は前記多孔性基材の上面および下面のうちいずれか一面以上に備えられ、前記ポリイミド系マトリックスから由来したポリイミド系層をさらに含み、
前記コア層全体重量に対して、前記多孔性基材が20~85重量%であり、
前記コア層全体体積に対して、前記多孔性基材が15~80体積%であり、
前記コア層全体体積に対して、前記ポリイミド系層が8~40体積%であり、
前記ポリイミド系マトリックスは下記の測定方法1により測定したイミド化率が90%以上である、低誘電銅箔積層板(CCL):
[測定方法1]
380℃で60分の間イミド化させた基準試料のイミド化率を100%と想定し、前記ポリイミド系マトリックスに対して赤外線分光器を通じて波長1,700cm -1 および1,615cm -1 のピークの大きさを測定した後、下記の数学式1によりPI indexを計算した後、下記の数学式2によりイミド化率を計算する。
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