US20040096676A1 - Wet etchable laminated body, insulation film, and electronic circuit part using the laminated body and the film - Google Patents

Wet etchable laminated body, insulation film, and electronic circuit part using the laminated body and the film Download PDF

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Publication number
US20040096676A1
US20040096676A1 US10/468,115 US46811503A US2004096676A1 US 20040096676 A1 US20040096676 A1 US 20040096676A1 US 46811503 A US46811503 A US 46811503A US 2004096676 A1 US2004096676 A1 US 2004096676A1
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US
United States
Prior art keywords
layer
insulating layer
insulating
inorganic material
adhesive
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Abandoned
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US10/468,115
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English (en)
Inventor
Katsuya Sakayori
Terutoshi Momose
Tomoko Togashi
Shigeki Kawano
Michiaki Uchiyama
Kazuto Okamura
Kazutoshi Taguchi
Kazunori Ohmizo
Makoto Shimose
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Dai Nippon Printing Co Ltd
Nippon Steel Chemical and Materials Co Ltd
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Individual
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Assigned to NIPPON STEEL CHEMICAL CO., LTD., DAI NIPPON PRINTING CO., LTD. reassignment NIPPON STEEL CHEMICAL CO., LTD. ASSIGNMENT OF ASSIGNORS INTEREST (SEE DOCUMENT FOR DETAILS). Assignors: OHMIZO, KAZUNORI, OKAMURA, KAZUTO, SHIMOSE, MAKOTO, TAGUCHI, KAZUTOSHI, KAWANO, SHIGEKI, MOMOSE, TERUTOSHI, SAKAYORI, KATSUYA, TOGASHI, TOMOKO, UCHIYAMA, MICHIAKI
Publication of US20040096676A1 publication Critical patent/US20040096676A1/en
Priority to US11/543,812 priority Critical patent/US8066891B2/en
Abandoned legal-status Critical Current

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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
    • H05K3/00—Apparatus or processes for manufacturing printed circuits
    • H05K3/0011—Working of insulating substrates or insulating layers
    • H05K3/0017—Etching of the substrate by chemical or physical means
    • H05K3/002—Etching of the substrate by chemical or physical means by liquid chemical etching
    • G—PHYSICS
    • G11—INFORMATION STORAGE
    • G11B—INFORMATION STORAGE BASED ON RELATIVE MOVEMENT BETWEEN RECORD CARRIER AND TRANSDUCER
    • G11B5/00—Recording by magnetisation or demagnetisation of a record carrier; Reproducing by magnetic means; Record carriers therefor
    • G11B5/48—Disposition or mounting of heads or head supports relative to record carriers ; arrangements of heads, e.g. for scanning the record carrier to increase the relative speed
    • G11B5/4806—Disposition or mounting of heads or head supports relative to record carriers ; arrangements of heads, e.g. for scanning the record carrier to increase the relative speed specially adapted for disk drive assemblies, e.g. assembly prior to operation, hard or flexible disk drives
    • G11B5/484—Integrated arm assemblies, e.g. formed by material deposition or by etching from single piece of metal or by lamination of materials forming a single arm/suspension/head unit
    • 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
    • H05K1/05—Insulated conductive substrates, e.g. insulated metal substrate
    • H05K1/056—Insulated conductive substrates, e.g. insulated metal substrate the metal substrate being covered by an organic insulating layer
    • 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
    • H05K2201/0183—Dielectric layers
    • H05K2201/0195—Dielectric or adhesive layers comprising a plurality of layers, e.g. in a multilayer structure
    • 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
    • H05K2203/00—Indexing scheme relating to apparatus or processes for manufacturing printed circuits covered by H05K3/00
    • H05K2203/11—Treatments characterised by their effect, e.g. heating, cooling, roughening
    • H05K2203/1152—Replicating the surface structure of a sacrificial layer, e.g. for roughening
    • 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
    • H05K3/38—Improvement of the adhesion between the insulating substrate and the metal
    • H05K3/386—Improvement of the adhesion between the insulating substrate and the metal by the use of an organic polymeric bonding layer, e.g. adhesive
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
    • Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
    • Y10T428/00—Stock material or miscellaneous articles
    • Y10T428/31504—Composite [nonstructural laminate]
    • Y10T428/31678—Of metal
    • Y10T428/31681—Next to polyester, polyamide or polyimide [e.g., alkyd, glue, or nylon, etc.]

Definitions

  • the present invention relates to a laminate which has a layer construction of first inorganic material layer (mainly metal layer)-insulating layer-second inorganic material layer (mainly metal layer) or a layer construction of inorganic material layer (mainly metal layer)-insulating layer and has high suitability for wet etching of a plurality of resin layers constituting the insulating layer in the laminate.
  • the present invention also relates to an insulating film and an electronic circuit component, for example, a wiring board such as a flexible printed board, a semiconductor related component such as CPS, a device such as a nozzle of a toner jet printer, particularly a suspension for a hard disk drive, produced by wet etching the laminate.
  • Pattern formation methods used in the formation of such wiring and circuits include: a method which comprises etching a metal layer, provided on a substrate in a layer construction of metal layer-insulating layer-metal layer, with an acidic solution, such as a ferric chloride solution, to form wirings, then subjecting the insulating layer to dry etching such as plasma etching or laser etching, or wet etching such as etching with hydrazine, to remove the insulating layer to form a desired shape for layer-to-layer continuity purposes (Japanese Patent Laid-Open No.
  • the warpage ⁇ of this substrate can be calculated according to the following equation (Miyaaki and Miki, NITTO TECHNICAL REPORT, 35 (3), 1 (1997)).
  • ⁇ 3 ⁇ l ⁇ ⁇ E 1 ⁇ E 2 2 ⁇ ⁇ h ⁇ ( E 1 2 + 14 ⁇ E 1 ⁇ E 2 2 + E 2 2 ) ⁇ ⁇ ⁇ ⁇ ⁇ ⁇ ⁇ ⁇ T
  • E 1 modulus of the metal
  • E 2 modulus of the insulating layer
  • ⁇ difference in coefficient of thermal expansion between the metal and the insulating layer
  • ⁇ T temperature difference
  • the coefficient of thermal expansion of the metal layer should be made identical to that of the insulating layer.
  • the use of a low-expansion polyimide as the insulating layer of the laminate has been proposed (U.S. Pat. No. 4,543,295 and Japanese Patent Laid-Open Nos. 18426/1980 and 25267/1977).
  • the low-expansion polyimide is not generally thermoplastic, the adhesion to metal layers is so low that it is difficult to provide adhesive strength high enough to withstand practical use.
  • a known method for overcoming this problem is to use a thermoplastic polyimide resin or epoxy resin having good adhesion to the metal layer as an adhesive insulating layer between the metal layer and the insulating layer (core layer) of the low-expansion polyimide (Japanese Patent Laid-Open No. 58428/1995).
  • the thickness of the low-expansion core insulating layer having a coefficient of thermal expansion close to that of the metal is made larger than the thickness of the adhesive layer to avoid the appearance of warpage of the whole laminate on the surface of the laminate. .
  • the smaller the thickness of the adhesive insulating layer the better the warpage preventive effect.
  • the thickness of the adhesive insulating layer is excessively small, however, the adhesion is deteriorated. At least when the total thickness of the adhesive layers respectively overlying and underlying the core layer is not more than the half of the thickness of the core layer, the warpage is less likely to occur.
  • the total thickness of adhesive insulating layers is not more than the half of the thickness of the core insulating layer.
  • the formation of the adhesive insulating layer in a smallest possible thickness, which can ensure the adhesion, is regarded as ideal (Japanese Patent Laid-Open No. 245587/1989).
  • the wireless suspension is mainly prepared using a laminate having a layer construction of first metal layer-adhesive insulating layer-core insulating layer-adhesive insulating layer-second metal layer.
  • An example of the laminate is such that the first metal layer is formed of a copper alloy foil, the second metal layer is formed of a stainless steel foil, and the insulating layer is comprised of a core insulating layer and an adhesive insulating layer stacked on both sides of the core insulating layer.
  • a wireless suspension using the laminate is scanned on a disk being rotated at a high speed and thus is a member to which fine vibration is applied. Therefore, the adhesive strength of wiring is very important. Accordingly, the wireless suspension using the laminate should satisfy strict specifications.
  • Hard disk drives are devices for recording information thereon. Therefore, a high level of data read/write reliability is required. To meet this requirement, the amount of refuse, such as dust, and outgas produced from the wireless suspension should be minimized.
  • a component called the “wireless suspension” is produced mainly by two methods, an additive method wherein wiring is formed by plating, and a subtractive method wherein wiring is formed by etching a copper foil.
  • the subtractive method only plasma etching by dry process is used for patterning of polyimide as the insulating layer.
  • a polyimide resin has been used as the adhesive for bonding between the insulating layer and the conductive inorganic material layer (metal layer) in the electronic circuit component, which satisfies the above strict specifications from the viewpoint of ensuring a high level of reliability of insulation.
  • adhesive properties In order to impart adhesive properties to the polyimide resin, it is common practice to impart thermoplasticity.
  • the introduction of a flexible structure, which can impart thermoplasticity, into a polyimide structure however, in many cases enhances chemical resistance. Therefore, the polyimide resin, to which the adhesive properties have been imparted, is likely to have poor suitability for wet etching and is more difficult to be etched by wet process than the core insulating layer. For this reason, the insulating layers have been simultaneously etched by dry process using plasma or laser.
  • the present inventors have found and aimed at the fact that, when the insulating layer in the laminate has been patterned by etching, irregularities (concaves and convexes) formed by the transfer of the shape of surface irregularities of the conductive inorganic material layer (metal layer) onto the adhesive insulating layer in the insulating layer affect the etching shape of the polyimide.
  • a generally adopted process for producing electronic circuit components such as hard disk suspensions and flexible printed boards is as follows.
  • An insulating layer is thermocompression bonded to and integrated with a conductive inorganic material (metal or the like) sheet to prepare a laminate.
  • an insulating layer may be formed by coating on a conductive inorganic material (metal or the like) sheet to prepare a laminate.
  • the laminate is then etched to produce the electronic circuit component.
  • Various methods have been proposed for improving the interfacial adhesion of the laminate. Among them, a method, which is very effective and is generally used, is to utilize anchor effect. In this method, fine irregularities are formed on the surface of the conductive inorganic material layer.
  • the insulating layer bites into the irregularities to develop the adhesion between the conductive inorganic material layer and the insulating layer.
  • the transfer of irregularities of the conductive inorganic material layer onto the insulating layer can be confirmed by removing the conductive inorganic material layer in the laminate by etching or the like.
  • the formation of the irregularities in the insulating layer means that the thickness of the insulating layer varies from portion to portion.
  • the adhesive insulating layer formed on the surface of the insulating layer has in many cases a lower wet etching rate than the low-expansion core insulating layer.
  • the thickness of the adhesive insulating layer is identical to that of the core insulating layer, the time necessary for etching the adhesive insulating layer is in many cases longer than that necessary for etching the core insulating layer. In this case, when the thickness of the adhesive insulating layer is uneven, the shape of the end face of the adhesive insulating layer becomes complicated.
  • the end face of the adhesive insulating layer is dropped, and this is causative of the occurrence of refuse.
  • the core insulating layer only in its portion corresponding to the smaller thickness portion of the adhesive insulating layer is etched in an earlier stage than the other portion. As a result, the whole insulating layer cannot be evenly etched, and the etching shape is unstable.
  • the thickness of the adhesive insulating layer is smaller than the average height of surface irregularities of the inorganic material layer in contact with the adhesive insulating layer, the irregularities of the inorganic material layer extend through some portions of the adhesive insulating layer and, consequently, disadvantageously, the adhesive insulating layer is partially absent.
  • the etching shape of the insulating layer is uneven.
  • FIG. 1 is a flow diagram of the production of a laminate for an electronic circuit component, for example, by pressing, shown for comparison with the present invention, wherein a laminate is produced based on common knowledge of the conventional technique wherein the adhesive resin layer in the insulating layer is made as thin as possible.
  • an insulating layer comprising a core insulating layer 1 , an adhesive insulating layer 2 provided on one side of the core insulating layer 1 and an adhesive insulating layer 3 provided on the other side of the core insulating layer 1 is sandwiched between a first inorganic material layer 4 and a second inorganic material layer 5 (FIG.
  • the laminate shown in FIG. 1 is an example of the case where the thickness of the adhesive insulating layer 3 in the insulating layer is equal to the average height of the surface irregularities of the second inorganic material layer 5 .
  • FIG. 2 is a typical diagram showing the laminate, shown in FIG. 1 ( 3 ) with the second inorganic material layer 5 being removed by etching, masked by coating a part of the adhesive insulating layer 3 with a masking agent 6 , wherein FIG. 2A is a cross-sectional view showing the layer construction of the laminate and FIG. 2B a top view of the laminate.
  • FIG. 3 is a schematic diagram illustrating an example of wet etching of the laminate shown in FIG. 2, wherein an etching process from the start of wet etching of the laminate, which has been partially masked with a masking agent 6 , to the removal of the masking agent 6 to complete the etching is shown in the order of FIGS. 3A to 3 D.
  • FIG. 3A shows such a state that, except for the site masked with the masking agent 6 , an etching liquid reaches the core insulating layer 1 and the core insulating layer 1 begins to be attacked by the etching liquid.
  • FIG. 3B shows such a state that, except for the site masked with the masking agent 6 , the core insulating layer 1 has been substantially completely attacked by the etching liquid.
  • FIG. 3C shows such a state that, except for the site masked with the masking agent 6 , the adhesive insulating layer 2 has been substantially completely attacked by the etching liquid.
  • FIG. 3D shows such a state that, after the completion of the wet etching, the masking agent 6 has been removed.
  • FIGS. 4A to 4 D are top views corresponding to FIGS. 3A to 3 D, respectively.
  • the laminate for an electronic circuit component shown in FIGS. 1 to 4 is an example of the laminate in which the adhesive insulating layer in the insulating layer having a thickness which has hitherto been considered to be ideal for suppressing the occurrence of warpage and has been determined by taking into consideration the adhesion to the metal layer.
  • the surface irregularities of the inorganic material such as the metal in the laminate contribute to an improvement in the adhesion of the inorganic material to the adhesive insulating layer. Since, however, the irregularities bite into the adhesive insulating layer to such an extent that is equal to the thickness of the adhesive insulating layer, when etching is carried out in this state, the etching shape after the removal of the masking agent is wavy (FIG. 4D). That is, a desired shape conforming to the mask cannot be provided, and the etching shape of the whole insulating layer is uneven. Thus, the accuracy is unreliable. The problem of the uneven complicated etching shape is likely to be led to dusting.
  • an object of the present invention is to provide a laminate comprising an insulating layer, which can realize an improvement in the shape of a patterned insulating layer, formed by patterning the insulating layer through wet etching, achieved by drawing attention to the state of irregularities transferred from the surface of the metal layer and, at the same time, is stable in the etching shape of the insulating layer and thus can suppress dusting, to provide an insulating film comprising the insulating layer, and to provide an electronic circuit component comprising a pattern of the insulating layer.
  • the present inventors have found that, in a laminate comprising: an insulating layer comprising a core insulating layer and an adhesive insulating layer provided on both surfaces of the core insulating layer; and an inorganic material layer formed of a metal or the like stacked on the insulating layer, when the shape of surface irregularities of the inorganic material layer has been transferred onto the adhesive insulating layer in the insulating layer and the thickness of the adhesive insulating layer is larger than the average height of the surface irregularities of the inorganic material layer, wet etching of the insulating layer can provide a good etching shape.
  • the present inventors have further found that, when the thickness of the adhesive insulating layer is larger, the degree of influence of the surface irregularities of the inorganic material layer on the etching shape of the insulating layer is smaller.
  • the present inventors have attempted to prevent the formation of through-holes in the adhesive insulating layer by making the thickness of the adhesive insulating layer larger than the average height of surface irregularities of the inorganic material layer and thus to prevent the core insulating layer from being exposed and, as a result, could have realized a laminate that comprises an adhesive insulating layer having a larger thickness than the mean roughness Rz (JIS (Japanese Industrial Standards) C 6515) of the surface of an inorganic material layer in contact with the insulating layer and, upon wet etching, can provide a good etching shape and has suppressed dusting properties.
  • Rz JIS (Japanese Industrial Standards) C 6515
  • the laminate of the present invention has a layer construction of first inorganic material layer-insulating layer-second inorganic material layer or a layer construction of inorganic material layer-insulating layer, characterized in that the insulating layer comprises a laminate of two or more wet etchable insulating unit layers and, at the interface between the inorganic material layer and the insulating layer, surface irregularities of the inorganic material layer have been transferred onto the insulating layer, and the average height of the irregularities transferred onto at least one layer in the insulating layer is less than the thickness of the outermost insulating unit layer in the insulating layer.
  • the insulating film of the present invention is characterized by comprising a laminate of two or more wet etchable insulating unit layers, said insulating film being adaptable for stacking on an inorganic material layer, said inorganic material layer having surface irregularities of which the average height is less than the thickness of the outermost insulating unit layer in the insulating layer.
  • the thickness of the adhesive insulating layer is 1.1 to 3 times Rz. Further, the thickness of the adhesive insulating layer is preferably not more than the half of the thickness of the low-expansion core insulating layer from the viewpoint of reducing the warpage of the substrate and preventing dusting.
  • Rz referred to in the present invention is as specified in JISC 6515.
  • Rz may be measured by providing a profile curve of irregularities and determining the difference between the average value of the distances of five highest profile peaks from a reference line in a reference length and the average value of the distances of five deepest profile valleys from the reference line in a reference length and expressing this difference in micrometer ( ⁇ m).
  • the electronic circuit component according to the present invention is an electronic circuit component produced by wet etching the laminate, particularly preferably a suspension for a hard disk drive, produced by wet etching.
  • FIG. 1 is a flow diagram of an example of the production of a laminate for an electronic circuit component by pressing, shown for comparison with the present invention, wherein a laminate is produced based on common knowledge of the conventional technique wherein the adhesive resin layer in the insulating layer is made as thin as possible;
  • FIGS. 2A and 2B are typical diagrams showing the laminate, shown in FIG. 1 ( 3 ) with the second inorganic material layer being removed by etching, masked by coating a part of the adhesive insulating layer with a masking agent, wherein FIG. 2A is a cross-sectional view showing the layer construction of the laminate and FIG. 2B a top view of the laminate;
  • FIGS. 3A, 3B, 3 C, and 3 D are cross-sectional views illustrating wet etching wherein an etching process from the start of wet etching of the laminate shown in FIG. 2, which has been partially masked with a masking agent, to the removal of the masking agent to complete the etching is shown in the order of FIGS. 3A to 3 D;
  • FIGS. 4A, 4B, 4 C, and 4 D are top views corresponding to FIGS. 3A to 3 D, respectively;
  • FIG. 5 is a schematic flow diagram of an embodiment of a production process of the laminate according to the present invention wherein the laminate is produced by pressing;
  • FIGS. 6A and 6B are typical diagrams showing the laminate, shown in FIG. 5 ( 3 ) with the second inorganic material layer being removed by etching, masked by coating a part of the adhesive insulating layer with a masking agent, wherein FIG. 6A is a cross-sectional view showing the layer construction of the laminate and FIG. 6B a top view of the laminate;
  • FIGS. 7A, 7B, 7 C, and 7 D are diagrams illustrating wet etching wherein an etching process from the start of wet etching of the laminate shown in FIG. 6, which has been partially masked with a masking agent, to the removal of the masking agent to complete the etching is shown in the order of FIGS. 7A to 7 D;
  • FIGS. 8A, 8B, 8 C, and 8 D are top views corresponding to FIGS. 7A to 7 D, respectively;
  • FIG. 9 is a schematic cross-sectional view showing an example of etching of a laminate, illustrating an unfavorable phenomenon wherein, when the etching rate of the adhesive insulating layer is excessively low, the etching shape is such that the upper adhesive insulating layer and the lower adhesive insulating layer are left in a projected form;
  • FIG. 10 is an SEM photograph (scanning electron photomicrograph) of sample A.
  • FIG. 11 is an SEM photograph (scanning electron photomicrograph) of sample B.
  • FIG. 5 is a typical schematic flow diagram of an embodiment of a production process of a laminate according to the present invention, wherein the laminate is produced by pressing.
  • an insulating layer comprising a core insulating layer 11 , an adhesive insulating layer 12 provided on one side of the core insulating layer 11 and an adhesive insulating layer 13 provided on the other side of the core insulating layer 11 is sandwiched between a first inorganic material layer 14 and a second inorganic material layer 15 (FIG. 5 ( 1 )), the assembly is pressed to produce a laminate according to the present invention (FIG. 5 ( 2 )), and the second inorganic material layer 15 is removed by etching (FIG. 5 ( 3 )).
  • the thickness of the adhesive insulating layer 13 shown in FIG. 5 is larger than the average height of surface irregularities of the second inorganic material layer 15 .
  • FIG. 6 is a typical diagram showing the laminate, shown in FIG. 5 ( 3 ) with the second inorganic material layer 15 being removed by etching, masked by coating a part of the adhesive insulating layer 13 with a masking agent 16 , wherein FIG. 6A is a cross-sectional view showing the layer construction of the laminate and FIG. 6B a top view of the laminate.
  • FIG. 7 is a schematic diagram illustrating wet etching of the laminate shown in FIG. 6, wherein an etching process from the start of wet etching of the laminate, which has been partially masked with a masking agent 16 , to the removal of the masking agent 16 to complete the etching is shown in the order of FIGS. 7A to 7 D.
  • FIG. 7A shows such a state that, except for the site masked with the masking agent 16 , the adhesive insulating layer 13 is being attacked by an etching liquid.
  • FIG. 7B shows such a state that, except for the site masked with the masking agent 16 , the core insulating layer 11 has been substantially completely attacked by the etching liquid. Irregularities formed by the residual core insulating layer 11 are also very gentle, indicating that the influence of gentle irregularities of the adhesive insulating layer 13 in FIG. 7A is further reduced.
  • FIG. 7B shows such a state that, except for the site masked with the masking agent 16 , the core insulating layer 11 has been substantially completely attacked by the etching liquid. Irregularities formed by the residual core insulating layer 11 are also very gentle, indicating that the influence of gentle irregularities of the adhesive insulating layer 13 in FIG. 7A is further reduced.
  • FIG. 7C shows such a state that, except for the site masked with the masking agent 16 , the adhesive insulating layer 12 has been completely attacked by the etching liquid.
  • An etching pattern of the insulating layer thus formed is linear and is substantially free from wavy uneven or other irregular shapes.
  • FIG. 7D shows such a state that, after the completion of the wet etching, the masking agent 16 has been removed.
  • FIGS. 8A to 8 D are top views corresponding to FIGS. 7A to 7 D, respectively.
  • the thickness of the adhesive insulating layer 13 is larger than the average height of surface irregularities of the second inorganic material layer 15 .
  • the insulating layer in the laminate or the insulating film according to the present invention comprises two or more insulating unit layers stacked on top of each other or one another and preferably has a layer construction of adhesive insulating layer-core insulating layer-adhesive insulating layer.
  • the insulating unit layers constituting the insulating layer or the insulating film are generally formed of an organic material. However, at least one of the insulating unit layers constituting the insulating layer or the insulating film may contain an inorganic material. Inorganic materials usable herein include, for example, colloidal silica, glass fiber, and other inorganic fillers.
  • the coefficient of linear thermal expansion of at least one of the insulating unit layers constituting the insulating layer or the insulating film is preferably not more than 30 ppm from the viewpoint of rendering the coefficient of linear thermal expansion close to that of the inorganic material layer. More preferably, the difference in coefficient of linear thermal expansion between at least one of the insulating unit layers constituting the insulating layer or the insulating film and the inorganic material layer is not more than 15 ppm.
  • the core insulating layer is particularly preferably formed of a material, which has the same coefficient of thermal expansion as the inorganic material layer, for example, a low-expansion polyimide from the viewpoint of preventing the warpage of the laminate.
  • the adhesive insulating layer is mainly formed of a thermoplastic resin from the viewpoint of imparting adhesive properties.
  • the coefficient of thermal expansion of the adhesive insulating layer is larger than that of the metal layer, and this large coefficient of thermal expansion of the adhesive insulating layer is causative of warpage of the laminate. Therefore, preferably, the warpage is prevented by rendering the thickness of the adhesive insulating layer smaller than the thickness of the core insulating layer.
  • the expression “adhesion of the adhesive insulating layer” means that the strength of adhesion to the inorganic material layer is not less than 100 g/cm.
  • Thermoplastic polyimides may be mentioned as specific suitable materials having the above property.
  • materials having the above property are not particularly limited to the thermoplastic polyimides only, and any resin may be used independently of the presence or absence of an imide bond so far as the resin has a combination of adhesive properties, heat resistance, and insulating properties. Since the adhesive strength of the adhesive insulating layer developed sometimes varies depending upon the relationship with the adhesion to the inorganic material layer as the adherend, the optimal material should be properly selected according to the type of the adherend or according to properties required of the laminate. Therefore, it is not always necessary to use an identical material, for example, polyimide resins having an identical composition. In some cases, however, an identical material is used.
  • the core insulating layer is sandwiched between two adhesive insulating layers, warpage of the laminate does not occur when the total thickness of the two adhesive insulating layers is smaller than the thickness of the core insulating layer.
  • the total thickness of the two adhesive insulating layers is not more than the half of the thickness of the core insulating layer. Therefore, the thickness of one adhesive insulating layer is preferably not more than a quarter of the thickness of the core insulating layer.
  • the weight average molecular weight of the resin usable in the adhesive insulating layer is generally preferably not less than 6,000 and not more than 500,000 although the preferred molecular weight varies depending upon the molecular structure.
  • the weight average molecular weight is particularly preferably not less than 8,000 and not more than 100,000.
  • the molecular weight is not less than 500,000, the formation of an even coating is difficult, while, when the molecular weight is not more than 6,000, the film formability is poor making it difficult to form an even adhesive coating.
  • the material for the adhesive insulating layer may be shaped by coating a solution of the material, or alternatively may be shaped by other methods. Further, the material may be shaped in the form of a precursor or a derivative thereof followed by treatment to provide a desired structure.
  • the inorganic material used in the laminate according to the present invention broadly refers to materials which are not organic materials.
  • examples of inorganic materials include, but are not particularly limited to, metals, single-crystal silicon, and metal oxides.
  • Metals include, but are not particularly limited to, copper, iron, and alloys such as stainless steel.
  • metals subjected to surface treatment that is, metals having on their surface a nonmetallic inorganic material layer, for example, a ceramic layer, may also be used.
  • a laminate of a highly elastic metal, such as stainless steel, and a copper foil or an alloy copper foil for wiring is preferred.
  • Examples of a combination of a material for the first inorganic material layer with a material for the second inorganic material layer include:
  • any one of the first inorganic material layer and the second inorganic material layer is formed of stainless steel or surface treated stainless steel while the other is formed of copper or surface treated copper;
  • any one of the first inorganic material layer and the second inorganic material layer is formed of stainless steel or surface treated stainless steel while the other is formed of alloy copper or surface treated alloy copper.
  • the type of the inorganic material is not particularly limited, and any inorganic material may be stacked on the insulating layer so far as the inorganic material meets the objective of the present invention.
  • the laminate according to the present invention may be produced by any method without particular limitation so far as the final layer construction of the laminate is the same.
  • Examples of production methods include: a method (cast method) wherein a solution of a material for the insulating layer is coated directly onto the surface of the inorganic material to form one or more stacked layers as the insulating layer, another inorganic material is optionally laminated, and the assembly is then thermocompression bonded; a method (film method) wherein an adhesive insulating layer is formed on a previously provided insulating film (core insulating layer), an inorganic material is stacked and thermocompression bonded onto the top surface and the back surface of the adhesive insulating layer; and a method wherein, after the formation of an adhesive insulating layer onto an insulating film as a core layer, an inorganic material layer is formed by vapor deposition, sputtering, plating or the like.
  • the lower limit of the mean roughness Rz of the inorganic material on its surface, which, together with the insulating layer, forms an interface, is preferably 0.2 ⁇ m from the viewpoint of developing adhesion.
  • the upper limit of Rz is preferably 15 ⁇ m because, when Rz exceeds 15 ⁇ m, the formation of a fine pattern is difficult.
  • An inorganic material having Rz in the range of 0.5 to 10 ⁇ m is easily available as a general-purpose commercially available metal foil and thus is particularly preferred from the practical point of view.
  • the insulating layer in the insulating film according to the present invention may take the form of a coating of a resin, or alternatively may take the form of a resin film.
  • the insulating film according to the present invention may be wet etched after lamination onto an inorganic material layer to form a laminate, or alternatively may be wet etched before the lamination. Specific embodiments of use of the insulating film according to the present invention are as follows.
  • the etching shape is not generally linear. In this case, the layer having a lower etching rate remains unetched. As shown in FIG. 9, in the laminate, when the etching rate of the adhesive insulating layer is excessively low, the etching shape is such that the upper adhesive insulating layer and the lower adhesive insulating layer are left in a projected form. On the other hand, when the etching rate of the adhesive insulating layer is excessively high, the etching shape is such that the adhesive insulating layer is etched at an earlier stage than the core insulating layer.
  • the etching shape is such that the center portion in the insulating layer is left in a projected form.
  • all the layers, i.e., the core insulating layer and the adhesive insulating layers, constituting the insulating layer have an identical etching rate. In this case, the realization of a sharp etching shape is expected. In etching by a wet process, however, in many cases, the etching rate of the adhesive insulating layer is significantly different from the etching rate of the core insulating layer.
  • an alkali-amine etching liquid as disclosed in Japanese Patent Laid-Open No. 97081/1998 may be mentioned as a suitable etching liquid.
  • the etching liquid is not particularly limited to this only.
  • the etching liquid is preferably an aqueous alkaline solution and is more preferably a basic chemical liquid having a pH value of not less than 9, still more preferably not less than 11.
  • the etching liquid may be an organic alkali or an inorganic alkali or a mixture of an organic alkali with an inorganic alkali.
  • the temperature, at which wet etching is carried out, is not particularly limited so far as the etchant can exhibit the desired function.
  • the etching temperature is preferably in the range of 0 to 110° C.
  • the etching rate is generally low.
  • the etching temperature is in the range of 30 to 90° C.
  • wet etching is carried out at a temperature in the range of 50 to 90° C. from the viewpoints of suppressing a change in composition of the etchant due to the evaporation of components or the like and, in addition, shortening the etching time.
  • An electronic circuit component can be generally produced by the following method.
  • a photosensitive resin layer is formed by coating or lamination onto the surface of the metal on its circuit formation side in the laminate according to the present invention.
  • a mask with a desired pattern image drawn thereon is brought into intimate contact with the surface of the photosensitive resin layer, and an electromagnetic radiation with a wavelength, to which the photosensitive resin is sensitive, is applied.
  • the exposed portion in the case of a positive-working photosensitive resin or the unexposed portion in the case of a negative-working photosensitive resin is eluted with a predetermined developing solution to form a desired circuit image on the metal.
  • the assembly in this stage is dipped in a solution, which can dissolve a metal, such as an aqueous ferric chloride solution, or alternatively the solution is sprayed on the substrate, whereby the exposed metal is eluted. Thereafter, the photosensitive resin is separated with a predetermined separation solution to form a circuit.
  • a solution which can dissolve a metal, such as an aqueous ferric chloride solution, or alternatively the solution is sprayed on the substrate, whereby the exposed metal is eluted.
  • the photosensitive resin is separated with a predetermined separation solution to form a circuit.
  • a mask with a desired pattern image drawn thereon is brought into intimate contact with the circuit formed on the surface of the metal, and the insulating layer is patterned by a dry or wet process.
  • Electronic circuit components to which the laminate according to the present invention can be applied, include, for example, wiring boards such as flexible printed boards, semiconductor-related components such as CSP (chip scale package), and devices such as nozzles of toner jet printers, particularly suspensions for hard disk drives.
  • wiring boards such as flexible printed boards
  • semiconductor-related components such as CSP (chip scale package)
  • devices such as nozzles of toner jet printers, particularly suspensions for hard disk drives.
  • the reason why the inorganic nitride and/or the inorganic fluoride are detected on the metal surface is probably that, since the plasma etching gas has a high temperature of 200° C. or above, after the removal of the resin constituting the insulating layer, such as a polyimide, the surface of the stainless steel is exposed and the exposed surface of the stainless steel is reacted with plasma to form the inorganic nitride and/or the inorganic fluoride.
  • Diamino compounds i.e., 4,4′-diamino-2′-methoxybenzanilide (20.5 g) and 4,4′-diaminodiphenyl ether (10.6 g), were dissolved in 340 g of DMAc as a solvent with stirring in a 500-ml separable flask to prepare a solution.
  • the solution was cooled in an ice bath, and 28.8 g of pyromellitic anhydride as a tetracarboxylic acid dianhydride was added to the cooled solution under a nitrogen gas stream. Thereafter, the temperature of the solution was returned to room temperature, and stirring was continued for 3 hr to allow a polymerization reaction to proceed to prepare viscous polyimide precursor solution A.
  • This polyimide precursor solution A was coated onto a stainless steel foil SUS 304 manufactured by Nippon Steel Corp. by means of an applicator so that the thickness of the coating after curing was 15 ⁇ m.
  • the coating was dried at 110° C. for 5 min, and the dried coating was then heat treated stepwise, i.e., at 130° C. for 3 min, at 160° C. for 3 min, at 200° C. for 3 min, at 250° C. for 3 min, at 300° C. for 3 min, and then at 360° C. for 3 min, to form a polyimide layer on the stainless steel foil.
  • the polyimide layer with the stainless steel foil remaining unremoved was immersed in a polyimide etching solution (TPE-3000 (tradename), manufactured by Toray Engineering Co., Ltd.) of 80° C. As a result, the polyimide layer was etched at a rate of 15 ⁇ m/min.
  • Diamino compounds i.e., 1,3-bis(4-aminophenoxy)-2,2′-dimethylpropane (22.1 g) and 3,4′-diaminodiphenyl ether (6.6 g), were dissolved in 340 g of DMAc as a solvent with stirring in a 500-ml separable flask to prepare a solution.
  • DMAc dimethylpropane
  • 9.7 g of pyromellitic anhydride as a tetracarboxylic acid dianhydride and 21.5 g of 3,4,3′,4′-benzophenonetetracarboxylic acid dianhydride were added to the solution under a nitrogen gas stream. Thereafter, stirring was continued for 3 hr to allow a polymerization reaction to proceed to prepare viscous polyimide precursor solution B.
  • This polyimide precursor solution B was coated onto a stainless steel foil SUS 304 manufactured by Nippon Steel Corp. by means of an applicator so that the thickness of the coating after curing was 15 ⁇ m.
  • the coating was dried at 110° C. for 5 min, and the dried coating was then heat treated stepwise, i.e., at 130° C. for 3 min, at 160° C. for 3 min, at 200° C. for 3 min, at 250° C. for 3 min, at 300° C. for 3 min, and then at 360° C. for 3 min, to form a polyimide layer on the stainless steel foil.
  • the polyimide layer thus formed was subjected to an etching test in the same manner as in Synthesis Example 1. As a result, the etching rate of the polyimide layer was found to be 8 ⁇ m/min.
  • Diamino compounds i.e., 1,3-bis(3-aminophenoxy)benzene (22.6 g) and p-phenylenediamine (3.6 g) were dissolved in 340 g of DMAc as a solvent with stirring in a 500-ml separable flask to prepare a solution.
  • DMAc dimethyl methacrylate
  • pyromellitic anhydride as a tetracarboxylic acid dianhydride
  • 24.1 g of 3,4,3′,4′-diphenylsulfonetetracarboxylic acid dianhydride were added to the solution under a nitrogen gas stream. Thereafter, stirring was continued for 3 hr to allow a polymerization reaction to proceed to prepare viscous polyimide precursor solution C.
  • This polyimide precursor solution C was coated onto a stainless steel foil SUS 304 manufactured by Nippon Steel Corp. by means of an applicator so that the thickness of the coating after curing was 15 ⁇ m.
  • the coating was dried at 110° C. for 5 min, and the dried coating was then heat treated stepwise, i.e., at 130° C. for 3 min, at 160° C. for 3 min, at 200° C. for 3 min, at 250° C. for 3 min, at 300° C. for 3 min, and then at 360° C. for 3 min, to form a polyimide layer on the stainless steel foil.
  • the polyimide layer thus formed was subjected to an etching test in the same manner as in Synthesis Example 1. As a result, the etching rate of the polyimide layer was found to be 14 ⁇ m/min.
  • Thermoplastic polyimide precursor resin solution B prepared in Synthesis Example 2 was coated onto a stainless steel foil SUS 304 manufactured by Nippon Steel Corp. by means of an applicator so that the thickness of the coating after curing was 1 ⁇ m. The coating was dried at 110° C. for 5 min. Low-thermal expansion polyimide precursor resin solution A prepared in Synthesis Example 1 was then coated onto the dried coating so that the thickness of the coating after curing was 14 ⁇ m. The coating was dried at 110° C. for 5 min to prepare a film formed material. The above procedure was repeated to prepare another film formed material. Thus, two film formed materials were provided.
  • Thermoplastic polyimide precursor resin solution C prepared in Synthesis Example 3 was coated to a thickness of 1.5 ⁇ m onto one of the film formed materials and to a thickness of 3 ⁇ m onto the other film formed material. These materials were then dried at 110° C. for 5 min. Thereafter, the materials were heat treated stepwise, i.e., at 130° C. for 3 min, at 160° C. for 3 min, at 200° C. for 3 min, at 250° C. for 3 min, at 300° C. for 3 min, and then at 360° C. for 3 min.
  • thermoplastic polyimide layer B low-expansion polyimide layer A
  • nonthermoplastic polyimide layer C nonthermoplastic polyimide layer C
  • the two materials were different from each other in the thickness of the nonthermoplastic polyimide layer C.
  • a copper alloy (C 7025 copper alloy, manufactured by Olin Corp.), which had a roughened surface having a mean roughness Rz of 1.6 ⁇ m, was provided and was put on top of the materials so that the rough surface was brought into contact with the thermoplastic polyimide layer C on the stainless steel foil.
  • Contact bonding was then carried out by means of a vacuum press at 330° C. for 60 min.
  • two laminates were prepared.
  • thermoplastic polyimide layer C 1.5 ⁇ m for one of the laminates and 3 ⁇ m for the other laminate.
  • a mask was provided on the SUS side of the laminate, and the masked laminate was immersed in a ferric chloride solution to etch the copper foil.
  • a 50 ⁇ m-thick alkali development-type dry film resist was laminated by a hot laminator onto the exposed surface of the thermoplastic polyimide layer C at a speed of 6.5 m/min under conditions of roll surface temperature 150° C. and line pressure 2 to 4 kg/cm, and the laminate was then allowed to stand at room temperature for 15 min. Thereafter, exposure was carried out using a predetermined mask by means of an intimate contact exposure system at 100 mJ/cm 2 .
  • the dry film resist was developed with a 1 wt % aqueous Na 2 CO 3 solution under conditions of temperature 30° C., spray pressure 2 kg, and development time 40 sec. Thereafter, the laminate was dried and was then immersed in an etching liquid TPE-3000 (tradename, manufactured by Toray Engineering Co., Ltd.) which had been stirred at 70° C. with a magnetic stirrer to such an extent that a whirlpool had been formed.
  • TPE-3000 tradename, manufactured by Toray Engineering Co., Ltd.
  • the laminate was taken out of the etching liquid, and the dry film resist was separated with a 3 wt % aqueous NaOH solution at 50° C. at a spray pressure of 1 kg.
  • the insulating layer which has been brought to a desired shape, was observed under SEM to inspect the etching shape.
  • a scanning electron microphotograph of sample A at a magnification of 1,000 times is shown in FIG. 10.
  • a scanning electron microphotograph of sample B at a magnification of 1,000 times is shown in FIG. 11.
  • Each sample (four patterns) used in the evaluation of the pattern shape was placed in the beaker, and a given amount of the blank was poured into the beaker.
  • the beaker was then placed within an ultrasonic irradiation system, and ultrasonic wave was applied for one min (extraction). After the application of ultrasonic wave, the beaker was taken out of the system, and the sample was taken out with the tweezers. After taking the sample out of the beaker, a given amount of the extract was set in a measuring apparatus equipped with an automatic fine particle measuring device for a liquid manufactured by HIAC/ROYCO, a suction-type semi-automatic sampling device, and a laser diode light blocking-type sensor to measure the amount of particles.
  • sample B comprising a thermoplastic polyimide having a larger thickness had a lower level of dusting.
  • the laminate and the insulating film according to the present invention when the average height of irregularities of an insulating layer as a result of transfer of surface irregularities of an inorganic material onto the insulating layer in an insulating film is rendered smaller than the thickness of the outermost insulating unit layer in the insulating layer, the etching shape after wet etching of the laminate and the insulating film is good and a highly reliable electronic circuit component, particularly a suspension, which causes no significant dusting, can be prepared.
  • the area of the insulating layer to be removed by etching is large and, at the same time, a fine pattern is required. Therefore, the effect attained by the application of the wet etching is large.
  • the laminate and the insulating film according to the present invention have enhanced wet etching reliability and thus are suitable for suspensions for hard disk drives.

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  • Chemical Kinetics & Catalysis (AREA)
  • General Chemical & Material Sciences (AREA)
  • Manufacturing & Machinery (AREA)
  • Microelectronics & Electronic Packaging (AREA)
  • Laminated Bodies (AREA)
  • Adjustment Of The Magnetic Head Position Track Following On Tapes (AREA)
  • Insulated Metal Substrates For Printed Circuits (AREA)
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US20070026678A1 (en) * 2001-02-16 2007-02-01 Dai Nippon Printing Co., Ltd. Wet etchable laminated body, insulation film, and electronic circuit part using the laminated body and the film
US20090035541A1 (en) * 2005-04-18 2009-02-05 Mitsui Chemicals, Inc. Metal laminate, method for manufacturing same and use thereof

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JP2008217843A (ja) * 2007-02-28 2008-09-18 Mitsui Chemicals Inc ハードディスクサスペンション用基材
CN101518969B (zh) * 2008-04-15 2012-10-31 上海网讯新材料科技股份有限公司 亚光平滑型金属塑料复合带
JP5724232B2 (ja) * 2010-07-09 2015-05-27 大日本印刷株式会社 サスペンション用基板、サスペンション用基板の製造方法、サスペンション、素子付サスペンションおよびハードディスクドライブ
US20140101935A1 (en) * 2012-10-15 2014-04-17 Samsung Electro-Mechanics Co., Ltd. Method for manufacturing printed circuit board
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CN103151306B (zh) * 2013-03-08 2015-06-17 上海和辉光电有限公司 一种柔性电子器件的制备方法
JP6967962B2 (ja) * 2017-12-27 2021-11-17 ローム株式会社 半導体装置および半導体装置の製造方法
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JP2002240194A (ja) 2002-08-28
US8066891B2 (en) 2011-11-29
CN102145566A (zh) 2011-08-10
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