TW202146233A - 金屬被覆液晶聚合物薄膜 - Google Patents

金屬被覆液晶聚合物薄膜 Download PDF

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TW202146233A
TW202146233A TW110113699A TW110113699A TW202146233A TW 202146233 A TW202146233 A TW 202146233A TW 110113699 A TW110113699 A TW 110113699A TW 110113699 A TW110113699 A TW 110113699A TW 202146233 A TW202146233 A TW 202146233A
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Taiwan
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metal layer
liquid crystal
metal
polymer film
crystal polymer
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TW110113699A
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English (en)
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有本紀久雄
澤田貴文
馬場雄一
長野秀司
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日商可樂麗股份有限公司
日商尾池工業股份有限公司
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Publication of TW202146233A publication Critical patent/TW202146233A/zh

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    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
    • H05K1/00—Printed circuits
    • H05K1/02—Details
    • H05K1/03—Use of materials for the substrate
    • H05K1/0313—Organic insulating material
    • H05K1/0353—Organic insulating material consisting of two or more materials, e.g. two or more polymers, polymer + filler, + reinforcement
    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
    • H05K1/00—Printed circuits
    • H05K1/02—Details
    • H05K1/09—Use of materials for the conductive, e.g. metallic pattern
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B15/00—Layered products comprising a layer of metal
    • B32B15/04—Layered products comprising a layer of metal comprising metal as the main or only constituent of a layer, which is next to another layer of the same or of a different material
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B15/00—Layered products comprising a layer of metal
    • B32B15/04—Layered products comprising a layer of metal comprising metal as the main or only constituent of a layer, which is next to another layer of the same or of a different material
    • B32B15/043—Layered products comprising a layer of metal comprising metal as the main or only constituent of a layer, which is next to another layer of the same or of a different material of metal
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B15/00—Layered products comprising a layer of metal
    • B32B15/04—Layered products comprising a layer of metal comprising metal as the main or only constituent of a layer, which is next to another layer of the same or of a different material
    • B32B15/08—Layered products comprising a layer of metal comprising metal as the main or only constituent of a layer, which is next to another layer of the same or of a different material of synthetic resin
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B15/00—Layered products comprising a layer of metal
    • B32B15/18—Layered products comprising a layer of metal comprising iron or steel
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B15/00—Layered products comprising a layer of metal
    • B32B15/20—Layered products comprising a layer of metal comprising aluminium or copper
    • 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
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09K—MATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
    • C09K19/00—Liquid crystal materials
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09K—MATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
    • C09K19/00—Liquid crystal materials
    • C09K19/02—Liquid crystal materials characterised by optical, electrical or physical properties of the components, in general
    • C—CHEMISTRY; METALLURGY
    • C23—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; CHEMICAL SURFACE TREATMENT; DIFFUSION TREATMENT OF METALLIC MATERIAL; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL; INHIBITING CORROSION OF METALLIC MATERIAL OR INCRUSTATION IN GENERAL
    • C23C—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL
    • C23C14/00—Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material
    • C23C14/06—Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material characterised by the coating material
    • C23C14/14—Metallic material, boron or silicon
    • C23C14/20—Metallic material, boron or silicon on organic substrates
    • C—CHEMISTRY; METALLURGY
    • C23—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; CHEMICAL SURFACE TREATMENT; DIFFUSION TREATMENT OF METALLIC MATERIAL; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL; INHIBITING CORROSION OF METALLIC MATERIAL OR INCRUSTATION IN GENERAL
    • C23C—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL
    • C23C14/00—Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material
    • C23C14/06—Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material characterised by the coating material
    • C23C14/14—Metallic material, boron or silicon
    • C23C14/20—Metallic material, boron or silicon on organic substrates
    • C23C14/205—Metallic material, boron or silicon on organic substrates by cathodic sputtering
    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
    • H05K1/00—Printed circuits
    • H05K1/02—Details
    • H05K1/03—Use of materials for the substrate
    • H05K1/0313—Organic insulating material
    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
    • H05K3/00—Apparatus or processes for manufacturing printed circuits
    • H05K3/02—Apparatus or processes for manufacturing printed circuits in which the conductive material is applied to the surface of the insulating support and is thereafter removed from such areas of the surface which are not intended for current conducting or shielding
    • H05K3/022—Processes for manufacturing precursors of printed circuits, i.e. copper-clad substrates
    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
    • H05K1/00—Printed circuits
    • H05K1/02—Details
    • H05K1/03—Use of materials for the substrate
    • H05K1/0393—Flexible materials
    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
    • H05K2201/00—Indexing scheme relating to printed circuits covered by H05K1/00
    • H05K2201/01—Dielectrics
    • H05K2201/0104—Properties and characteristics in general
    • H05K2201/0129—Thermoplastic polymer, e.g. auto-adhesive layer; Shaping of thermoplastic polymer
    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
    • H05K2201/00—Indexing scheme relating to printed circuits covered by H05K1/00
    • H05K2201/01—Dielectrics
    • H05K2201/0137—Materials
    • H05K2201/0141—Liquid crystal polymer [LCP]
    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
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    • H05K2201/00—Indexing scheme relating to printed circuits covered by H05K1/00
    • H05K2201/03—Conductive materials
    • H05K2201/0332—Structure of the conductor
    • H05K2201/0335—Layered conductors or foils
    • H05K2201/0338—Layered conductor, e.g. layered metal substrate, layered finish layer or layered thin film adhesion layer
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Abstract

本發明提供一種金屬被覆液晶聚合物薄膜，其係具備可形成光學各向異性的熔融層之聚合物薄膜、積層在上述聚合物薄膜之至少單面的第1的金屬層，以及積層在上述第1的金屬層之上的第2的金屬層，在使用XPS之厚度方向上的氧濃度分析中，上述第1的金屬層的平均氧濃度為2.5原子%以下。

Description

金屬被覆液晶聚合物薄膜
本發明係有關一種在由可形成光學各向異性的熔融層之聚合物薄膜(以下，簡稱為熱塑性液晶聚合物薄膜、或液晶聚合物薄膜)所構成之基材表面上形成有金屬層的金屬被覆液晶聚合物薄膜、以及將其包含在積層構造中的覆金屬積層板。
對於行動電話、數位相機等攜帶式電子機器，車載電子零件、家用電器等電子機器，係要求小型化、輕量化。因此，企圖進行以樹脂薄膜為絕緣基材之撓性電路基板的利用、以及電路圖案的微細化。而且，在目前正開發中的第5代行動通訊系統(5G)中，為了對應10GHz以上的高頻，而要求減少電路基板中的傳輸損耗。
已知相較於以聚醯亞胺為絕緣基板之傳統的電路基板，以液晶聚合物薄膜為絕緣基板之撓性電路基板可減少傳輸損耗，而作為電路基板材料，已開發在各種液晶聚合物薄膜上積層有金屬層的覆金屬積層板。就覆金屬積層板而言，已開發且市售各種將銅箔等金屬箔隔著接著層或直接壓接到液晶聚合物薄膜上者。
作為覆金屬積層板之製造方法，亦研究藉由乾式鍍敷而在樹脂薄膜上將金屬薄膜予以成膜的方法。例如專利文獻1中記載一種2層撓性基板，其係直接在絕緣體薄膜之至少單面上形成基底金屬層，且在該基底金屬層上形成銅導體層的2層撓性基板，其特徵為基底金屬層主要含有固溶氧原子3.1～3.8原子%的鎳-鉻或鎳-鉻-鉬，並作為基底金屬層之製法而記載藉由真空蒸鍍法、濺鍍法、離子鍍法等乾式鍍敷法形成基底層。
亦研究一種在藉由乾式鍍敷而在樹脂薄膜上將金屬薄膜予以成膜時使用低氧環境的方法。專利文獻2中記載一種關於具有由樹脂薄膜/金屬層所構成的層構造之複合薄膜的製造方法，其係在對樹脂薄膜實施脫氣步驟、真空放電處理步驟之後，連續實施藉由濺鍍而形成金屬層之步驟，並且在氧氣濃度為0.01%以下之惰性氣體氣流中實施該等步驟的方法。 [先前技術文獻] [專利文獻]
專利文獻1：日本專利第4924843號 專利文獻2：日本專利第4646580號
[發明欲解決之課題]
在覆金屬積層板中，電路圖案係藉由蝕刻表面的金屬層而進行加工，然此時，金屬箔的膜厚成為電路之微細化上的限制。就在樹脂薄膜上形成微細電路的手法而言，亦研究使用金屬奈米粒子進行印刷加工的方法(印刷電子)，惟目前的情形係電阻比使用金屬箔的情況還大，無法承受在高頻下的使用。
專利文獻1係記載：藉由在乾式鍍敷的金屬化方法中，將固溶在基底金屬層的氧原子控制在3.1〜3.8原子%，而能夠提供銅導體層的密合性高，且具有絕緣信賴性高的2層撓性電路基板。在絕緣層之選項中，亦可列舉液晶聚合物薄膜，惟在實施例中，係使用傳輸損耗大於液晶聚合物薄膜之聚醯亞胺薄膜，且藉由濺鍍而進行基底與銅層的成膜，並未研究傳輸損耗的降低。
專利文獻2係記載：與在氧氣存在下進行輝光放電及濺鍍之傳統方法相比，藉由在極力排除氧氣的真空下進行樹脂薄膜之脫氣處理、藉由真空放電進行的表面處理、到藉由濺鍍之金屬層的形成為止之所有步驟，而樹脂薄膜與金屬層之間的剝離強度會被改善。然而，專利文獻2中並未記載抑制源自樹脂薄膜本身的氧與金屬層之間的反應。而且，實施例中，係使用聚醯亞胺薄膜作為樹脂薄膜，並未研究傳輸損耗的降低。
本發明之目的為提供一種金屬被覆液晶聚合物薄膜，其係藉由使於液晶聚合物薄膜表面形成的導體層(金屬層)薄層化，而適於微電路加工，並且可減少電路的傳輸損耗。 [用以解決課題之手段]
本發明之金屬被覆液晶聚合物薄膜，係具備由可形成光學各向異性的熔融相之聚合物(熱塑性液晶聚合物)所構成的聚合物薄膜主體、積層在上述聚合物薄膜主體之至少單面的第1的金屬層(第1金屬層)，以及積層在上述第1的金屬層之上的第2的金屬層(第2金屬層)，且在使用XPS之厚度方向上的氧濃度分析中，上述第1的金屬層之平均氧濃度為2.5原子%以下(較佳為2.0原子%以下)的金屬被覆液晶聚合物薄膜。
上述第1的金屬層在厚度方向之氧濃度的峰值係以4.5原子%以下(較佳為4.0原子%以下)為較佳。
上述第1的金屬層可包含選自包含鉻、錫、鐵、銅、鈷、鋅、鉬及鎳之群組的一種或二種以上。
上述第2的金屬層可為選自包含銅、金、銀及鋁之群組的一種、或者包含銅、金、銀、鋁之任一者的合金。
上述聚合物薄膜主體可為平面方向之線膨脹係數成為0～24ppm/℃者。
本發明之覆金屬積層板係在積層構造中包含上述金屬被覆液晶聚合物薄膜者。覆金屬積層板可具備上述金屬被覆液晶聚合物薄膜、與進一步積層在上述第2的金屬層上的第3的金屬層(第3金屬層)。
上述金屬被覆液晶聚合物薄膜的製造方法，可包含藉由在上述聚合物薄膜主體之至少單面(單面或兩面)進行濺鍍，而將上述第1的金屬層之薄膜予以成膜的步驟。
依據本發明，則可提供一種傳輸損耗降低，可形成線寬更細的電路之撓性電路基板。
另外，申請專利範圍及/或說明書及/或圖式所揭示之至少2個構成的任意組合亦包含在本發明中。尤其是申請專利範圍之各請求項的2個以上之任意組合亦包含在本發明中。
[用以實施發明的形態]
本發明之金屬被覆液晶聚合物薄膜，係具備積層在由可形成光學各向異性的熔融層之聚合物(熱塑性液晶聚合物)所構成的薄膜主體(熱塑性液晶聚合物薄膜)之至少單面之第1金屬層、與積層在上述第1金屬層之上的第2金屬層，在使用XPS之厚度方向上的氧濃度分析中，上述第1金屬層之平均氧濃度為2.5原子%以下。上述第1金屬層之厚度方向的氧濃度之峰值係以4.5原子%以下為較佳。如此的金屬被覆液晶聚合物薄膜，可為第1的金屬層係藉由濺鍍形成，且第2的金屬層係藉由乾式鍍敷或濕式鍍敷形成的金屬鍍敷液晶聚合物薄膜。例如，金屬被覆液晶聚合物薄膜可為具備在熱塑性液晶聚合物薄膜之表面上以濺鍍形成的第1金屬層(第1之濺鍍膜)、與在上述第1金屬層之表面上以濺鍍形成的第2金屬層(第2之濺鍍膜)者。
在成為絕緣基材之樹脂薄膜表面以乾式鍍敷法形成成為基底層之金屬層，且在基底層上積層有成為導體層之金屬層的金屬被覆樹脂薄膜，係如專利文獻1所例示地已為先前習知，惟本發明者等發現藉由使用熱塑性液晶聚合物薄膜作為樹脂薄膜，並將基底層之氧濃度限制在預定值以下，即可降低在電路加工成導體層時之在高頻區域的傳輸損耗。而且，本發明者等發現為了抑制基底層中的氧濃度，在乾式鍍敷時僅使用無氧環境並不足，有必要抑制源自樹脂薄膜本身之氧的污染。在此處，如果藉由濺鍍等乾式鍍敷而形成成為基底的第1金屬層與第2金屬層，則可使在絕緣基材上形成的金屬層成為具有亞微米量級厚度之極薄的金屬層，且可藉由蝕刻等已知方法而進行微細的電路加工。因此，可同時達成撓性電路基板之電路圖案的精細化以及傳輸損耗的降低之二個課題。
(基材) 本發明中，係使用熱塑性液晶聚合物薄膜作為絕緣基材。已知相較於使用聚醯亞胺作為絕緣基材者，使用熱塑性液晶聚合物薄膜作為絕緣基材之撓性電路基板可降低在電路加工時之傳輸損耗。亦可因應需要，而使用以習知方法在熱塑性液晶聚合物薄膜的單面上形成金屬層的單面覆金屬積層板作為基材，並在另一面(薄膜面)形成下述第1金屬層。
(液晶聚合物薄膜) 本發明中使用之液晶聚合物薄膜，係由可形成光學各向異性之熔融相的聚合物所形成。此聚合物只要是可熔融成形的液晶聚合物即可，對於該聚合物的化學構成，並無特別限定，惟例如以由熱塑性液晶聚合物所構成為較佳。就熱塑性液晶聚合物而言，可列舉例如：熱塑性液晶聚酯、或於該等中導入有醯胺鍵之熱塑性液晶聚酯醯胺等。
而且，熱塑性液晶聚合物可為在芳香族聚酯或芳香族聚酯醯胺中進一步導入有醯亞胺鍵、碳酸酯鍵、碳二亞胺鍵或三聚異氰酸酯鍵等源自異氰酸酯之鍵等的聚合物。
就本發中使用之熱塑性液晶聚合物之具體例而言，可列舉自以下所例示之被分類為(1)至(4)的化合物及其衍生物所導出的習知熱塑性液晶聚酯以及熱塑性液晶聚酯醯胺。然而，為了形成可形成光學各向異性的熔融相之聚合物，各種原料化合物的組合無疑係在適當的範圍內。
(1)芳香族或脂肪族二醇(代表例係參照表1) [表1]
Figure 02_image001
(2)芳香族或脂肪族二羧酸(代表例係參照表2) [表2]
Figure 02_image003
(3)芳香族羥基羧酸(代表例係參照表3) [表3]
Figure 02_image005
(4)芳香族二胺、芳香族羥基胺或芳香族胺基羧酸(代表例係參照表4) [表4]
Figure 02_image007
作為由該等原料化合物所得之熱塑性液晶聚合物之代表例係可列舉如：具有表5及6所示之構造單元的共聚物。
[表5]
Figure 02_image009
[表6]
Figure 02_image011
該等共聚物中，以至少包含對羥基苯甲酸及/或6-羥基-2-萘甲酸作為重複單元之聚合物為較佳，尤其以(i)包含對羥基苯甲酸與6-羥基-2-萘甲酸之重複單元的共聚物、或(ii)包含至少一種選自包含對羥基苯甲酸及6-羥基-2-萘甲酸之群組的芳香族羥基羧酸、至少一種芳香族二醇、及至少一種芳香族二羧酸之重複單元的共聚物為較佳。
例如，在(i)之共聚物中，熱塑性液晶聚合物至少包含對羥基苯甲酸與6-羥基-2-萘甲酸之重複單元之情形，重複單元(A)之對羥基苯甲酸與重複單元(B)之6-羥基-2-萘甲酸的莫耳比(A)/(B)，係在熱塑性液晶聚合物中，期望為(A)/(B)=10/90～90/10左右，更佳可為(A)/(B)=15/85～85/15左右，進一步較佳可為(A)/(B)= 20/80～80/20左右。
又，(ii)之共聚物之情形，至少一種選自包含對羥基苯甲酸及6-羥基-2-萘甲酸之群組的芳香族羥基羧酸(C)、至少一種選自包含4,4'-二羥基聯苯、氫醌、苯基氫醌以及4,4'-二羥基聯苯醚之群組的芳香族二醇(D)、及至少一種選自包含對苯二甲酸、間苯二甲酸以及2,6-萘二甲酸之群組的芳香族二羧酸(E)的在熱塑性液晶聚合物中的各重複單元之莫耳比，可為芳香族羥基羧酸(C)：上述芳香族二醇(D)：上述芳香族二羧酸(E)=(30～80)：(35～10)：(35～10)左右，可更佳為(C)：(D)：(E)=(35～75)：(32.5～12.5)：(32.5～12.5)左右，可進一步較佳為(C)：(D)：(E)=(40～70)：(30～15)：(30～15)左右。
芳香族羥基羧酸(C)中，源自6-羥基-2-萘甲酸之重複單元的莫耳比率，係例如可為85莫耳%以上，可較佳為90莫耳%以上，更佳為95莫耳%以上。芳香族羥基羧酸(E)中，源自2,6-萘二羧酸之重複單元的莫耳比率，係例如可為85莫耳%以上，可較佳為90莫耳%以上為較佳，更佳為95莫耳%以上。
而且，芳香族二醇(D)可為源自二種互為相異之選自包含氫醌、4,4'-二羥基聯苯、苯基氫醌以及4,4'-二羥基二苯醚之群組的芳香族二醇之重複單元(D1)與(D2)，此情形，二種芳香族二醇之莫耳比可為(D1)/(D2)=23/77～77/23，可更佳為25/75～75/25，進一步較佳為30/70～70/30。
而且，源自芳香族二醇(D)之重複構造單元與源自芳香族二羧酸(E)之重複構造單元的莫耳比，係以(D)/(E)=95/100～100/95為較佳。如超出此範圍，則聚合度不會增加而有機械強度降低之傾向。
另外，可形成本發明中所謂的光學各向異性之熔融相，係例如藉由將試料放在熱台上，在氮氣環境下升溫加熱並觀察試料的透射光，而可認定。
作為熱塑性液晶聚合物而較佳者，係融點(以下稱為Tm0 )在例如200～360℃之範圍者，更佳為240～350℃之範圍者，進一步較佳為Tm0 在260～330℃之範圍者。另外，融點係可使用示差掃描熱析儀觀察熱塑性液晶聚合物試樣的熱行為來獲得。亦即，求出將熱塑性液晶聚合物試樣以10°C/分鐘之速度升溫使其完全熔化後，將熔融物以10°C/分鐘之速度冷卻至50°C，再以10°C/分鐘之速度升溫後呈現的吸熱峰位置，作為熱塑性液晶聚合物試樣之融點。
上述熱塑性液晶聚合物中，在無損本發明之效果的範圍內，可添加聚對苯二甲酸乙二酯、改質聚對苯二甲酸乙二酯、聚烯烴、聚碳酸酯、聚芳酯、聚醯胺、聚苯硫醚、聚醚醚酮、氟樹脂等熱塑性聚合物、各種添加劑、填充劑等。
本發明之製造方法中使用的熱塑性液晶聚合物薄膜，係例如可將上述熱塑性液晶聚合物之熔融捏合物擠出成形而得。擠出成形法係使用任意方法者，然以習知的T模法、充氣法等在工業上為有利。尤其在充氣法中，由於不僅在熱塑性液晶聚合物薄膜之機械軸方向(以下簡稱為MD方向)，而且在與該方向正交的方向(以下，簡稱為TD方向)上亦施加應力，可在MD方向、TD方向均勻地拉伸，因此可得到在MD方向與TD方向上分子配向性、介電特性等得到控制的熱塑性液晶聚合物薄膜。
例如，在藉由T模法進行的擠出成形中，不僅可將從T模擠出的熔融體片材在熱塑性液晶聚合物薄膜的MD方向拉伸，而且可同時對於此與TD方向拉伸而製膜，或可將從T模擠出的熔融體片材先在MD方向拉伸，然後在TD方向拉伸而製膜。
在藉由充氣法的擠出成形中，亦可對於從環形模熔融擠出的圓筒狀片材，以預定的拉伸比(相當於MD方向的延伸倍率)以及吹塑比(相當於TD方向的延伸倍率)進行延伸而製膜。
如此的擠出成形的延伸倍率，係作為MD方向的延伸倍率(或拉伸比)，而例如可為1.0〜10左右，且可較佳為1.2〜7左右，進一步較佳為1.3〜7左右。而且，作為TD方向的延伸倍率(或拉伸比)，而例如可為1.5〜20左右，且可較佳為2〜15左右，進一步較佳為2.5〜14左右。
此外，亦可因應所需，而進行習知或慣用的熱處理以調整熱塑性液晶聚合物薄膜之融點及/或熱膨脹係數。熱處理條件可根據目的而適當地設定，例如可藉由以相對於熱塑性液晶聚合物之融點(Tm0 )溫度為(Tm0 -10)℃以上(例如：(Tm0 -10)〜(Tm0 +30)℃左右，較佳為(Tm0 )〜(Tm0 +20)℃左右)加熱數小時，而使熱塑性液晶聚合物薄膜之融點(Tm )上升。
熱塑性液晶聚合物薄膜之融點(Tm )，係例如可為270〜380℃，可較佳為280〜370℃之範圍者。另外，熱塑性液晶聚合物薄膜之融點(Tm )，係可使用示差掃描熱析儀觀察熱塑性液晶聚合物薄膜的熱行為來獲得。亦即，求出將熱塑性液晶聚合物薄膜以10°C/分鐘之速度升溫時呈現的吸熱峰位置，作為熱塑性液晶聚合物薄膜之融點(Tm )。
熱塑性液晶聚合物薄膜，可為在薄膜的平面方向之線膨脹係數經調整為0～24ppm/℃左右者。在電路基板製造商，係使用具有大致在該範圍內的線膨脹係數之液晶聚合物薄膜作為絕緣基材。線膨脹係數，係例如可藉由TMA方法測定。
熱塑性液晶聚合物薄膜之厚度，係可因應用途而適當地設定，例如若考慮到在多層電路基板之絕緣層材料中使用，則可為10〜500μm，可較佳為15〜250μm，更佳為25至180μm。
(單面覆金屬積層板) 本發明之金屬液晶被覆聚合物薄膜可為將上述熱塑性液晶聚合物薄膜作為基材，而在單面或雙面形成有下述第1金屬層與第2金屬層者。或者，亦可將經由習知方法而在熱塑性液晶聚合物薄膜之單面上形成有金屬層的單面覆金屬積層板作為基材，並且在露出有熱塑性液晶聚合物的另一表面上形成下述第1金屬層與第2金屬層。作為此基材之單面覆金屬積層板，可為直接或隔著接著層將金屬箔熱壓在熱塑性液晶聚合物薄膜之表面者。
(第1金屬層) 第1金屬層可為包含選自包含鉻、錫、鐵、銅、鈷、鋅、鉬及鎳之群組的一種或二種以上者。例如，可為該等金屬之二種以上之合金，亦可為進一步添加有其它金屬之合金。第1金屬層可為包含不可避免之雜質者，惟需要將氧控制在預定濃度以下。
第1金屬層係可藉由使用要積層之金屬作為靶的濺鍍而予以成膜。濺鍍所使用的氣體係以無氧之氬氣為較佳。此時，金屬層中所含的氧被認為是來自要濺鍍之液晶聚合物薄膜者。可藉由使用習知的濺鍍方法，且調整濺鍍時的輸出(電流、電壓)以及通電間隔(負載比：duty ratio)等條件，而抑制來自液晶聚合物薄膜的污染，且將第1金屬層中之氧濃度抑制在預定值內。 濺鍍時之輸出(電流、電壓)並無特別限制，但例如以10～1000kW為較佳，以50～800kW為更佳，以100～700kW為進一步較佳。而且，通電之間隔(負載比)亦無特別限制，但例如以1.1～50%為較佳，以1.5～30%為更佳，以2.0～20%為進一步較佳。
第1金屬層係以在使用XPS(X射線光電子分光分析儀)之厚度方向上的氧濃度分析中，平均氧濃度成為2.5原子%以下為較佳。藉此，而在將形成在第1金屬層上之第2金屬層作為導體層進行電路加工之情形，可顯著地降低高頻區域中的傳輸損耗。進而，平均氧濃度係以2.0原子%以下為更佳。第1金屬層係以在厚度方向之氧濃度的峰值為4.5原子%以下為較佳。進而，氧濃度之峰值係以4.0原子%以下為更佳。
第1金屬層之厚度並無特別限定，惟以5nm以上為較佳，以50nm以下為較佳。若厚度過薄，則無法得到提升第2金屬層之密合性之效果，且亦難以將平均氧濃度控制的很低。另一方面，於使用與第2金屬層的導電性不同的金屬作為第1金屬層之情形，若使第1金屬層成為過厚，則將難以抑制傳輸損耗。第1金屬層厚度係以30nm以下為更佳，以20nm以下為進一步較佳。
(第2金屬層) 第2金屬層係積層在上述第1金屬層之上。第2金屬層可為選自包含銅、金、銀及鋁之群組的一種。可為由包含銅、金、銀及鋁之任一者的合金所構成者。第2金屬層之製法並無特別限制，惟以經由鍍敷形成為鍍敷層者為較佳。鍍敷法可為濺鍍、離子鍍、真空蒸鍍、CVD等乾式鍍敷，亦可為濕式鍍敷(電鍍)。例如，可將第2金屬層與第1金屬層同樣地藉由濺鍍來形成。
第2金屬層之厚度並無特別限定，惟例如以50nm以上400nm以下為較佳，以300nm以下為更佳。藉由將金屬箔(例如軋製銅箔)在液晶聚合物薄膜等基材進行熱壓接而形成的覆金屬積層板中，金屬箔的厚度成為限制，而無法得到一定以下之厚度的導體層，惟在第1金屬層上藉由鍍敷形成第2金屬層時，能以任意厚度形成導體層。在以化學蝕刻等之習知方法進行電路加工之情形，若導體層薄，則亦可進行精細的電路加工。
(覆金屬積層板) 本發明之覆金屬積層板係由上述金屬被覆液晶聚合物薄膜所構成者、或包含上述金屬被覆液晶聚合物薄膜者。為了說明，將覆金屬積層板30之構成的一部分之示意剖面圖呈示於圖1A、1B、1C中。另外，該圖僅係用於說明積層構造之示意圖，圖的寬度及各部分的厚度比非為實際比例。於一實施型態中，本發明之金屬被覆液晶聚合物薄膜20係可藉由將第2金屬層2製成所要的厚度，而作為電路基板材料使用。因此，本發明所提供之覆金屬積層板30可為包含熱塑性液晶聚合物薄膜10、第1金屬層1與第2金屬層2者(圖1A)。
於其它實施型態中，覆金屬積層板30可為在第2金屬層2上進一步積層有第3金屬層3(以下稱為第3金屬層)者(圖1B)。第3金屬層3可用乾式鍍敷法或濕式鍍敷法之任一種方法形成。例如在藉由濺鍍等乾式鍍敷之方法積層有第1金屬層1與第2金屬層2之後，可在第2金屬層2上藉由電鍍形成第3金屬層3。在此，第3金屬層3係與第2金屬層2相同，可為選自銅、金、銀、鋁之一種，亦可為由包含銅、金、銀、鋁之任一者的合金所構成者。此時，可由與第2金屬層2相同的金屬形成第3金屬層3。藉此，而可得到上述金屬被覆液晶聚合物薄膜20之導體層(第2金屬層)2被增厚的覆金屬積層板30。在熱塑性液晶聚合物薄膜10的兩面上形成有第1金屬層與第2金屬層(無圖示)之情形，可僅在單面的第2金屬層2上形成第3金屬層3，亦可在兩面之第2金屬層2上分別形成第3金屬層3。第3金屬層之厚度並無特別限定，但可為1～20μm，以1～5μm為更佳。
作為其它實施型態，在熱塑性液晶聚合物薄膜之單面形成第1金屬層1、第2金屬層2以及因應必要之第3金屬層3，且將金屬箔4熱壓接在另一面等，以習知方法設置金屬層者，亦包含在本發明之覆金屬積層板30中(圖1C)。此時，亦可將如上所述以金屬箔4的熱壓接等之習知方法製造的單面覆金屬積層板作為基材，而在另一面設置第1金屬層1、第2金屬層2、以及因應必要之第3金屬層3，或者，亦可將第1金屬層1、第2金屬層2、以及因應必要之第3金屬層3設置在熱塑性液晶聚合物薄膜10之單面之後，在另一面，藉由金屬箔4之熱壓接等習知方法設置金屬層。
根據本發明，可提供一種金屬被覆液晶聚合物薄膜，其係在熱塑性液晶聚合物薄膜之單面或雙面，相較於使用金屬箔，顯著地降低傳輸損耗，且具有比金屬箔更薄的金屬層。例如，藉由化學蝕刻等習知方法形成電路之情形，在薄的導體層則能夠進行微細的電路加工，因此，可藉由使用本發明之金屬被覆液晶聚合物薄膜，而提供一種傳輸損耗降低(高頻特性優異)，且亦抑制尺寸的撓性電路基板。 [實施例]
作為液晶聚合物薄膜，係將Kuraray股份有限公司製造之「Vecstar」(註冊商標)(DSC的熔點310℃，厚度50μm，依TMA法之線膨脹係數15ppm/℃)作為絕緣基材使用，將其安裝在卷對卷濺鍍裝置中並抽真空，並使用無氧的高純度氬氣，藉由NiCr靶(Ni 80wt%，Cr 20wt%)之濺鍍，而在膜上將膜厚為15nm的濺鍍膜(第1金屬層)予以成膜。接著，將靶變更為Cu，並在第1金屬層上將厚度為120nm的Cu膜(第2金屬層)予以成膜。針對如此操作而得的金屬被覆液晶聚合物薄膜，藉由X射線光電子分光分析裝置(XPS)(ULVAC-PHI股份有限公司製造/PHI5000 VersaProbe2)，在以(Ar)離子從第2金屬層的表面蝕刻至基材薄膜表面的同時，在深度方向上進行分析，求出第1金屬層中的平均氧濃度與氧濃度的最大值(峰值)。將平均氧濃度定義為存在鎳合金的區域定義為鎳合金層，並將鎳合金層內的氧存在比率加以平均者。
僅變更NiCr靶的濺鍍條件而以四種方式進行上述過程，將其作為實施例1、實施例2、比較例1及比較例2。其中，在實施例1、2與比較例1中，以高輸出間歇地進行濺鍍，在比較例2中，以低輸出恆定地進行濺鍍。該等結果呈示於表7。
針對各金屬被覆液晶聚合物薄膜，藉由電鍍而將Cu層增厚至12μm以製成覆金屬積層板，並且藉由化學蝕刻將寬度為100～120μm的微帶線進行加工，使用微波網絡分析儀(由安捷倫股份有限公司製造，商品名稱：8722ES)及探針(由Cascade Microtech股份有限公司製造，商品名稱：ACP40-250)在0.05～67 GHz的條件下測定傳輸損耗，比較在60 GHz之損耗。此時，對各微帶線的寬度進行比較，由於在所有情況下均顯示出相同傾向，因此使用微帶線寬為110μm之數值作為代表。
[表7]
　 實施例1 實施例2 比較例1 比較例2
NiCr層成膜時的最大輸出 (kW) 675 105 1275 5 (穩定)
負載比(%) 2.0 16.0 1.0 100
NiCr層平均氧濃度 (原子%) 1.8 1.6 2.8 2.7
NiCr層波峰氧濃度 (原子%) 3.4 3.4 6.6 4.8
傳輸損耗(dB/100mm) 60GHz -9.4 -9.6 -9.9 -10.1
在以低輸出恆定地進行濺鍍之比較例2中，第1金屬層的氧濃度超出本發明的範圍。在比較例1中，由於最大輸出過大，因此在濺鍍開始時產生來自液晶聚合物薄膜的污染，第1金屬層的氧濃度並未降低，相較於比較例2，於傳輸損耗並未觀察到顯著差異。另一方面，在實施例1和2中，確認了傳輸損耗減少之效果。 [產業上利用之可能性]
若根據本發明之金屬被覆液晶聚合物薄膜，則可減少撓性電路基板的傳輸損耗，可使線寬微細化，作為高頻電路基板材料之利用性高。
如上所述，已參照圖式說明本發明之較佳實施例，惟在該技術領域中具有一般知識者可查看本說明書容易地在不言而喻的範圍內進行各種變更及修正。因此，如此變更及修正被解釋為在申請專利範圍所限定的本發明之範圍內者。
1:第1金屬層 2:第2金屬層 3:第3金屬層 4:金屬箔層 10:液晶聚合物薄膜 20:金屬被覆液晶聚合物薄膜 30:覆金屬積層板
從參考附圖對以下較佳之實施型態的說明，應更清楚地理解本發明。然而，實施型態及圖式僅為圖示以及用於說明者，不應被用於限定本發明之範圍。本發明之範圍係藉由所附的請求項決定。 圖1A係用以說明本發明之金屬被覆液晶聚合物薄膜以及覆金屬積層板之積層構造的一實施型態之示意截面圖。 圖1B係用以說明本發明之覆金屬積層板之積層構造的其它實施型態之示意截面圖。 圖1C係用以說明本發明之覆金屬積層板之積層構造的其它實施型態之示意截面圖。
1:第1金屬層
2:第2金屬層
10:液晶聚合物薄膜
20:金屬被覆液晶聚合物薄膜
30:覆金屬積層板

Claims (7)

  1. 一種金屬被覆液晶聚合物薄膜，其係具備由可形成光學各向異性的熔融相之聚合物所構成的聚合物薄膜主體、積層在該聚合物薄膜主體之至少單面的第1的金屬層、以及積層在該第1的金屬層之上的第2的金屬層， 在使用XPS之厚度方向上的氧濃度分析中，該第1的金屬層的平均氧濃度為2.5原子%以下。
  2. 如請求項1之金屬被覆液晶聚合物薄膜，其中在該第1的金屬層之厚度方向的氧濃度之峰值為4.5原子%以下。
  3. 如請求項1或2之金屬被覆液晶聚合物薄膜，其中該第1的金屬層係包含選自包含鉻、錫、鐵、銅、鈷、鋅、鉬及鎳之群組的一種或二種以上。
  4. 如請求項1至3中任一項之金屬被覆液晶聚合物薄膜，其中該第2的金屬層係由選自包含銅、金、銀及鋁之群組的一種、或包含銅、金、銀、鋁之任一者的合金所構成。
  5. 如請求項1至4中任一項之金屬被覆液晶聚合物薄膜，其中該聚合物薄膜主體在平面方向之線膨脹係數為0～24ppm/℃。
  6. 一種覆金屬積層板，其具備如請求項1至5中任一項之金屬被覆液晶聚合物薄膜，與積層在該第2的金屬層上的第3的金屬層。
  7. 一種如請求項1至5中任一項之金屬被覆液晶聚合物薄膜的製造方法，其包含藉由在該聚合物薄膜主體之至少單面進行濺鍍而將該第1的金屬層之薄膜予以成膜的步驟。
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