WO2013136722A1 - 金属張積層板、プリント配線基板、半導体パッケージ、および半導体装置 - Google Patents

金属張積層板、プリント配線基板、半導体パッケージ、および半導体装置 Download PDF

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Publication number
WO2013136722A1
WO2013136722A1 PCT/JP2013/001387 JP2013001387W WO2013136722A1 WO 2013136722 A1 WO2013136722 A1 WO 2013136722A1 JP 2013001387 W JP2013001387 W JP 2013001387W WO 2013136722 A1 WO2013136722 A1 WO 2013136722A1
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Prior art keywords
metal
resin
clad laminate
less
glass
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PCT/JP2013/001387
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English (en)
French (fr)
Japanese (ja)
Inventor
大東　範行
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住友ベークライト株式会社
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Priority to KR1020147023625A priority Critical patent/KR20140144177A/ko
Publication of WO2013136722A1 publication Critical patent/WO2013136722A1/ja

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    • 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
    • B32B17/00—Layered products essentially comprising sheet glass, or glass, slag, or like fibres
    • B32B17/02—Layered products essentially comprising sheet glass, or glass, slag, or like fibres in the form of fibres or filaments
    • B32B17/04—Layered products essentially comprising sheet glass, or glass, slag, or like fibres in the form of fibres or filaments bonded with or embedded in a plastic substance
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L23/00—Details of semiconductor or other solid state devices
    • H01L23/12—Mountings, e.g. non-detachable insulating substrates
    • H01L23/14—Mountings, e.g. non-detachable insulating substrates characterised by the material or its electrical properties
    • H01L23/145—Organic substrates, e.g. plastic
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L23/00—Details of semiconductor or other solid state devices
    • H01L23/28—Encapsulations, e.g. encapsulating layers, coatings, e.g. for protection
    • H01L23/31—Encapsulations, e.g. encapsulating layers, coatings, e.g. for protection characterised by the arrangement or shape
    • H01L23/3107—Encapsulations, e.g. encapsulating layers, coatings, e.g. for protection characterised by the arrangement or shape the device being completely enclosed
    • H01L23/3121—Encapsulations, e.g. encapsulating layers, coatings, e.g. for protection characterised by the arrangement or shape the device being completely enclosed a substrate forming part of the encapsulation
    • H01L23/3128—Encapsulations, e.g. encapsulating layers, coatings, e.g. for protection characterised by the arrangement or shape the device being completely enclosed a substrate forming part of the encapsulation the substrate having spherical bumps for external connection
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L23/00—Details of semiconductor or other solid state devices
    • H01L23/48—Arrangements for conducting electric current to or from the solid state body in operation, e.g. leads, terminal arrangements ; Selection of materials therefor
    • H01L23/488—Arrangements for conducting electric current to or from the solid state body in operation, e.g. leads, terminal arrangements ; Selection of materials therefor consisting of soldered or bonded constructions
    • H01L23/498—Leads, i.e. metallisations or lead-frames on insulating substrates, e.g. chip carriers
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L23/00—Details of semiconductor or other solid state devices
    • H01L23/48—Arrangements for conducting electric current to or from the solid state body in operation, e.g. leads, terminal arrangements ; Selection of materials therefor
    • H01L23/488—Arrangements for conducting electric current to or from the solid state body in operation, e.g. leads, terminal arrangements ; Selection of materials therefor consisting of soldered or bonded constructions
    • H01L23/498—Leads, i.e. metallisations or lead-frames on insulating substrates, e.g. chip carriers
    • H01L23/49866—Leads, i.e. metallisations or lead-frames on insulating substrates, e.g. chip carriers characterised by the materials
    • H01L23/49894—Materials of the insulating layers or coatings
    • 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
    • H05K1/0366—Organic insulating material consisting of two or more materials, e.g. two or more polymers, polymer + filler, + reinforcement reinforced, e.g. by fibres, fabrics
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L2224/00—Indexing scheme for arrangements for connecting or disconnecting semiconductor or solid-state bodies and methods related thereto as covered by H01L24/00
    • H01L2224/01—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
    • H01L2224/10—Bump connectors; Manufacturing methods related thereto
    • H01L2224/15—Structure, shape, material or disposition of the bump connectors after the connecting process
    • H01L2224/16—Structure, shape, material or disposition of the bump connectors after the connecting process of an individual bump connector
    • H01L2224/161—Disposition
    • H01L2224/16151—Disposition the bump connector connecting between a semiconductor or solid-state body and an item not being a semiconductor or solid-state body, e.g. chip-to-substrate, chip-to-passive
    • H01L2224/16221—Disposition the bump connector connecting between a semiconductor or solid-state body and an item not being a semiconductor or solid-state body, e.g. chip-to-substrate, chip-to-passive the body and the item being stacked
    • H01L2224/16225—Disposition the bump connector connecting between a semiconductor or solid-state body and an item not being a semiconductor or solid-state body, e.g. chip-to-substrate, chip-to-passive the body and the item being stacked the item being non-metallic, e.g. insulating substrate with or without metallisation
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L2924/00—Indexing scheme for arrangements or methods for connecting or disconnecting semiconductor or solid-state bodies as covered by H01L24/00
    • H01L2924/15—Details of package parts other than the semiconductor or other solid state devices to be connected
    • H01L2924/151—Die mounting substrate
    • H01L2924/153—Connection portion
    • H01L2924/1531—Connection portion the connection portion being formed only on the surface of the substrate opposite to the die mounting surface
    • H01L2924/15311—Connection portion the connection portion being formed only on the surface of the substrate opposite to the die mounting surface being a ball array, e.g. BGA
    • 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
    • H05K1/0373—Organic insulating material consisting of two or more materials, e.g. two or more polymers, polymer + filler, + reinforcement containing additives, e.g. fillers
    • 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
    • H05K2201/02—Fillers; Particles; Fibers; Reinforcement materials
    • H05K2201/0275—Fibers and reinforcement materials
    • H05K2201/029—Woven fibrous reinforcement or textile
    • 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
    • H05K2201/06—Thermal details
    • H05K2201/068—Thermal details wherein the coefficient of thermal expansion is important

Definitions

  • the present invention relates to a metal-clad laminate, a printed wiring board, a semiconductor package, and a semiconductor device.
  • printed circuit boards also called circuit boards
  • circuit boards tend to be made thinner and thinner with the demand for higher functionality and lighter and thinner electronic devices.
  • a general printed wiring board is mainly composed of a laminate using a prepreg provided with a fiber base layer and a resin layer.
  • the current laminated board is mainly used for FCBGA (Flip Chip Ball Grid Array) used in, for example, a CPU (Central Processing Unit) and has a thickness of about 0.8 mm.
  • FCBGA Flexible Chip Ball Grid Array
  • thinning of laminates has been promoted for reasons such as reduction in substrate cost due to demands for reduction in thickness, reduction in member cost, processing cost, and improvement in electrical characteristics.
  • a laminate having a thickness of about 0.4 mm, further 0.2 mm or less has been developed.
  • Patent Document 1 Japanese Patent Laid-Open No. 2007-50599 discloses that an adhesive layer containing a thermoplastic polyimide is formed during thermal lamination in a manufacturing process of a flexible metal-clad laminate. Further, it is described that the tension applied to the film-like joining member is regulated within the range of 0.1 to 1 N / m. By taking such a measure, it is said that a flexible metal-clad laminate having excellent dimensional stability can be obtained even if the thickness of the film-like joining member is as thin as 5 to 15 ⁇ m or less.
  • the present invention has been made in view of the above-described problems, and provides a metal-clad laminate in which warpage during mounting is reduced.
  • the present inventor has intensively investigated the mechanism of warping of the metal-clad laminate.
  • an insulating layer whose linear expansion coefficient satisfies a specific condition is used, it is possible to reduce the warpage of the metal-clad laminate during mounting. I found out.
  • thermomechanical analyzer (1) a temperature raising step from 25 ° C. to 300 ° C .; (2) Perform thermomechanical analysis measurement including a temperature lowering process from 300 ° C. to 25 ° C., In the surface direction of the insulating layer, The linear expansion coefficient calculated in the range from 25 ° C. to T g in the temperature raising step is ⁇ 1 , The linear expansion coefficient calculated in the range of 300 ° C.
  • T g represents the glass transition temperature by dynamic viscoelasticity measurement of the insulating layer (temperature increase rate 5 ° C./min, frequency 1 Hz).)
  • a printed wiring board obtained by subjecting the metal-clad laminate to circuit processing.
  • a semiconductor package in which a semiconductor element is mounted on the printed wiring board.
  • a semiconductor device including the semiconductor package is provided.
  • FIG. 1 is a cross-sectional view showing a configuration of a metal-clad laminate 100 in the present embodiment.
  • the metal-clad laminate 100 includes an insulating layer 101 including a thermosetting resin, a filler, and a fiber base material, and includes metal foils 103 on both surfaces of the insulating layer 101. Then, the metal-clad laminate 100 is obtained by removing the metal foils 103 on both sides by etching, and using a thermomechanical analyzer, (1) a temperature rising step from 25 ° C. to 300 ° C., and (2) 300 ° C. to 25 ° C.
  • the linear expansion coefficients ⁇ 1 , ⁇ 2, and ⁇ 3 in the surface direction of the insulating layer 101 calculated under the following conditions are ⁇ 3 > ⁇ 1 > It meets the ⁇ 2 of the conditions.
  • ⁇ 1 is a linear expansion coefficient calculated in the range from (1) 25 ° C. to T g in the temperature raising step
  • ⁇ 2 is a linear expansion coefficient calculated in the range from (1) T g in the temperature raising step to 300 ° C.
  • ⁇ 3 is a linear expansion coefficient calculated in the range of (2) 300 ° C. to 25 ° C. in the temperature lowering step.
  • T g represents the glass transition temperature by dynamic viscoelasticity measurement of the insulating layer 101 (heating rate 5 ° C. / min, frequency 1 Hz).
  • the linear expansion coefficient of this embodiment shows the average value in each said temperature range.
  • the metal-clad laminate 100 of the present embodiment that satisfies the above conditions can reduce warpage of the metal-clad laminate 100 during heat treatment such as reflow.
  • the reason why the warp can be reduced is not necessarily clear, but the following reason is presumed.
  • the metal-clad laminate 100 of this embodiment has a feature that the linear expansion coefficient of the insulating layer 101 decreases when the temperature of the metal-clad laminate 100 exceeds the glass transition temperature. This is considered to mean that the residual stress of the metal-clad laminate 100 is relaxed by receiving the thermal history.
  • the metal-clad laminate 100 of the present embodiment undergoes a heat treatment process such as reflow, so that the residual stress of the metal-clad laminate 100 is relieved, and as a result, warpage of the metal-clad laminate 100 is reduced. it is conceivable that. Therefore, the metal-clad laminate 100 of the present embodiment that satisfies the above conditions can reduce the warp of the metal-clad laminate 100 after heat treatment such as reflow. Further, as a result, warpage of the semiconductor package 200 and the semiconductor device 300 including the metal-clad laminate 100 can be reduced.
  • the reference length of the insulating layer 101 before the thermomechanical analysis measurement is set to L 0, and the insulating layer 101 at 25 ° C. in the above temperature lowering step.
  • L 1 / L 0 deformation rate C 1 calculated in is preferably at 50ppm or 5000ppm or less, more not less 100ppm or 2000ppm or less It is preferably 500 ppm or more and 1500 ppm or less.
  • the deformation rate C 1 in the longitudinal direction 105 of the metal-clad laminate 100 is C 1x and the deformation rate C 1 in the lateral direction 107 perpendicular to the longitudinal direction 105 is C 1y , (C 1x ⁇ C 1y )
  • the absolute value is preferably 0 ppm or more and 1000 ppm or less, more preferably 0 ppm or more and 500 ppm or less, and particularly preferably 0 ppm or more and 200 ppm or less.
  • the anisotropy of the stress relaxation is small when the heat treatment such as reflow mounting
  • the warp of the metal-clad laminate 100 at the time can be further reduced.
  • the vertical direction 105 refers to the conveyance direction (so-called MD) of the laminated plate 100
  • the horizontal direction 107 refers to a direction orthogonal to the conveyance direction of the laminated plate (so-called TD).
  • the metal-clad in order to obtain the effect of preventing warpage of the laminate 100 more effectively, the reference length of the thermomechanical analysis measurements prior to the insulating layer 101 and L 0, insulation above T g in the heating step when the deformation amount from the reference length L 0 of the layer 101, the difference between the deformation amount from the reference length L 0 of the insulating layer 101 in the above T g in the cooling step was L 2, with L 2 / L 0 deformation ratio C 2 is calculated, is preferably 50ppm or 2500ppm or less, more preferably 200ppm or more 1000ppm or less, and particularly preferably 300ppm or 600ppm or less.
  • the deformation rate C 2 in the longitudinal direction 105 of the metal-clad laminate 100 is C 2x and the deformation rate C 2 in the lateral direction 107 perpendicular to the longitudinal direction 105 is C 2y , (C 2x ⁇ C 2y )
  • the absolute value is preferably 0 ppm or more and 500 ppm or less, more preferably 0 ppm or more and 200 ppm or less, and particularly preferably 0 ppm or more and 100 ppm or less.
  • the anisotropy of the stress relaxation is small when the heat treatment such as reflow mounting
  • the warp of the metal-clad laminate 100 at the time can be further reduced.
  • the glass transition temperature at a frequency of 1 Hz by dynamic viscoelasticity measurement of the insulating layer 101 is preferably 200 ° C. It is above, More preferably, it is 220 degreeC or more. About an upper limit, 350 degrees C or less is preferable, for example.
  • the metal-clad laminate 100 increases the rigidity of the metal-clad laminate 100 and further warps the metal-clad laminate 100 during mounting. Can be reduced.
  • the storage elastic modulus E ′ at 250 ° C. of the metal-clad laminate 100 is preferably 5 GPa or more. More preferably, it is 10 GPa or more, and particularly preferably 15 GPa or more. Although it does not specifically limit about an upper limit, For example, it can be 50 GPa or less.
  • the metal-clad laminate 100 increases the rigidity of the metal-clad laminate 100 and can further reduce the warp of the metal-clad laminate 100 during mounting.
  • the thickness of the insulating layer 101 (the portion excluding the metal foil 103 from the metal-clad laminate 100) in the present embodiment is preferably 0.025 mm or more and 0.6 mm or less. More preferably, it is 0.04 mm or more and 0.4 mm or less, More preferably, it is 0.04 mm or more and 0.3 mm or less, More preferably, it is 0.05 mm or more and 0.2 mm or less.
  • the thickness of the insulating layer 101 is within the above range, the balance between mechanical strength and productivity is particularly excellent, and the metal-clad laminate 100 suitable for a thin printed wiring board can be obtained.
  • the linear expansion coefficient in the plane direction of the insulating layer 101 is preferably such that ⁇ 1 is ⁇ 12 ppm / ° C. to 10 ppm / ° C., ⁇ 2 is ⁇ 15 ppm / ° C. to 8 ppm / ° C., and ⁇ 3 Is from ⁇ 10 ppm / ° C. to 15 ppm / ° C. More preferably, ⁇ 1 is ⁇ 8 ppm / ° C. to 10 ppm / ° C., ⁇ 2 is ⁇ 12 ppm / ° C. to 6 ppm / ° C., and ⁇ 3 is ⁇ 8 ppm / ° C.
  • ⁇ 1 is ⁇ 6 ppm / ° C. to 6 ppm / ° C.
  • ⁇ 2 is ⁇ 8 ppm / ° C. to 5 ppm / ° C.
  • ⁇ 3 is ⁇ 6 ppm / ° C. to 10 ppm / ° C.
  • the metal-clad laminate 100 is obtained by, for example, heat curing a prepreg that includes a thermosetting resin, a filler, and a fiber base material.
  • the prepreg used here is a sheet-like material, which has excellent dielectric properties, various properties such as mechanical and electrical connection reliability under high temperature and high humidity, and is suitable for manufacturing a metal-clad laminate 100 for a printed wiring board. preferable.
  • the present inventor adjusts the tension of the fiber base material to a low pressure, whereby the linear expansion coefficient ⁇ 1 , ⁇ in the surface direction of the insulating layer 101 is adjusted. It was found that 2 and ⁇ 3 satisfy the condition of ⁇ 3 > ⁇ 1 > ⁇ 2 and a metal-clad laminate 100 having excellent stress relaxation ability is obtained.
  • the prepreg in the present embodiment is not particularly limited.
  • a fiber base material whose tension is adjusted to a low pressure is impregnated with a resin composition containing one or more thermosetting resins and a filler, and then half Obtained by curing.
  • the method for impregnating the fiber base material with the resin composition is not particularly limited as long as the tension applied to the fiber base material can be adjusted to a low pressure.
  • an insulating resin layer with a support base material The method of laminating to a material, (2) The method of melt
  • a method of laminating an insulating resin layer with a supporting base material on a fiber base material is particularly preferable.
  • the method of laminating the resin layer with a supporting substrate on the fiber substrate is easy to adjust the tension applied to the fiber substrate to a low pressure.
  • a method of laminating the insulating resin layer with a supporting substrate on the fiber substrate is preferable. According to this method, the amount of the resin composition impregnated into the fiber substrate can be freely adjusted, and the moldability of the prepreg can be further improved.
  • FIG. 2 is a cross-sectional view showing a method for producing a prepreg.
  • FIG. 3 is a schematic diagram showing an example of the width dimension of each of the support base 13, the insulating resin layers 15a and 15b, and the fiber base 11 used in the prepreg manufacturing method of the present embodiment. .
  • a method for producing a prepreg using a method of laminating an insulating resin layer with a supporting substrate is as follows.
  • Insulating resin layers 15a and 15b containing a thermosetting resin and a filler are formed on one surface of the supporting substrate 13.
  • the insulating resin layer sides of the carrier materials 5a and 5b are overlapped on both surfaces of the fiber substrate 11, respectively, under reduced pressure conditions Laminating them.
  • the step (A) will be described.
  • the first carrier material 5a and the second carrier material 5b in which the insulating resin layers 15a and 15b including the thermosetting resin and the filler are formed on one side of the support base 13 are manufactured.
  • the carrier materials 5 a and 5 b are obtained by forming insulating resin layers 15 a and 15 b in a thin layer on one side of the support base 13.
  • the insulating resin layers 15 a and 15 b can be formed on one side of the support base 13 with a predetermined thickness.
  • carrier material 5a, 5b Although it does not specifically limit as a manufacturing method of carrier material 5a, 5b,
  • the method of applying the resin composition to the support base material 13 using various coater apparatuses such as a comma coater, a knife coater, and a die coater, a spray nozzle, etc.
  • a method of applying the resin composition to the support substrate 13 using the various spray devices Among these, the method of applying the resin composition to the support substrate 13 using various coater apparatuses is preferable. Thereby, the insulating resin layers 15a and 15b excellent in thickness accuracy can be formed with a simple apparatus.
  • the resin composition After applying the resin composition to the support substrate 13, it can be dried at room temperature or under heating as necessary. Thereby, when an organic solvent or a dispersion medium is used when preparing the resin composition, these are substantially removed to eliminate the tackiness of the surface of the insulating resin layer, and the carrier material 5a having excellent handleability. 5b. Moreover, the hardening reaction of a thermosetting resin can be advanced to the middle, and the fluidity
  • the thickness of the insulating resin layers 15a and 15b can be appropriately set according to the thickness of the fiber base 11 used. For example, it can be 1 ⁇ m or more and 100 ⁇ m or less.
  • the insulating resin layers 15a and 15b may be formed by one or a plurality of times of application using the same thermosetting resin, or formed by a plurality of times of application using different thermosetting resins. It may be what was done.
  • a protective film is provided on the upper surface side where the insulating resin layers 15a and 15b are formed, that is, on the side opposite to the support base material 13 for protecting the insulating resin layer surface. You may superimpose.
  • the material of the support base 13 is not particularly limited.
  • a metal foil formed from a metal such as an alloy can be suitably used.
  • the thermoplastic resin for forming the thermoplastic resin film polyethylene terephthalate is preferable because it is excellent in heat resistance and inexpensive.
  • a metal which forms metal foil it is excellent in electroconductivity, the circuit formation by an etching is easy, and since it is cheap, copper or a copper alloy is preferable.
  • the surface on which the insulating resin layers 15a and 15b are formed is preferably subjected to a peelable treatment. Thereby, the insulating resin layers 15a and 15b and the support base material 13 can be easily separated at the time of manufacturing the prepreg or after manufacturing.
  • the thickness of the thermoplastic resin film for example, a film having a thickness of 15 ⁇ m or more and 75 ⁇ m or less can be used. In this case, the workability at the time of manufacturing the carrier materials 5a and 5b can be improved. When the thickness of the thermoplastic resin film is not less than the above lower limit value, sufficient mechanical strength can be ensured when the carrier materials 5a and 5b are manufactured. Moreover, productivity of carrier material 5a, 5b can be improved as thickness is below the said upper limit.
  • a surface on which the insulating resin layers 15a and 15b are formed may be subjected to a detachable process, or is such a process not performed?
  • a material subjected to a treatment for improving the adhesion to the insulating resin layers 15a and 15b can be used.
  • the same effect as that obtained when the thermoplastic resin film is used is exhibited. be able to.
  • As the thickness of this metal foil for example, a thickness of 1 ⁇ m or more and 70 ⁇ m or less can be used. Thereby, workability
  • the thickness of the metal foil is equal to or more than the above lower limit value, sufficient mechanical strength can be ensured when the carrier materials 5a and 5b are manufactured. Moreover, productivity of carrier material 5a, 5b can be improved as thickness is below the said upper limit.
  • thermoplastic resin film or the metal foil with which the process which can peel on the surface in which insulating resin layer 15a, 15b is formed is used as the support base material 13, insulating resin layer 15a, 15b is formed.
  • the unevenness on the surface of the support substrate 13 on the side is preferably as small as possible. Accordingly, when the metal-clad laminate 100 is manufactured, the surface smoothness of the insulating layer 101 can be improved. Therefore, when a new conductor layer is formed by metal plating or the like after the surface of the insulating layer 101 is roughened. In addition, a fine circuit can be processed and formed more easily.
  • the support base material 13 when a metal foil that has not been subjected to a detachable process or has been subjected to a process that improves adhesion with the insulating resin layer is used as the support base material 13, during the production of the metal-clad laminate 100, This metal foil can be used as it is as a conductor layer for forming a circuit (metal foil 103 in FIG. 1).
  • the unevenness of the surface of the support base on the side where the insulating resin layers 15a and 15b are formed is not particularly limited, but for example, Ra: 0.1 ⁇ m or more and 1.5 ⁇ m or less can be used.
  • a fine circuit can be easily processed and formed by performing an etching process or the like on the metal foil 103.
  • thickness of this metal foil 103 what is 1 micrometer or more and 35 micrometers or less can be used suitably, for example.
  • the thickness of the metal foil 103 is not less than the above lower limit value, sufficient mechanical strength can be secured when the carrier materials 5a and 5b are manufactured. Further, if the thickness is not more than the above upper limit value, a fine circuit may be more easily formed by processing.
  • This metal foil 103 can be used for manufacturing the prepreg by using it for at least one of the support base materials 13 of the carrier materials 5a and 5b used for manufacturing the prepreg.
  • a metal foil 103 formed from one layer can be used, or a metal foil 103 formed of two or more layers from which the metal foil 103 can be peeled off is used. It can also be used.
  • the first metal foil 103 on the side to be in close contact with the insulating layer and the second metal foil 103 that can support the first metal foil 103 on the side opposite to the side to be in close contact with the insulating layer can be peeled off.
  • a bonded metal foil having a two-layer structure can be used.
  • step (B) the insulating resin layer side of the carrier material 5a, 5b in which the insulating resin layer is formed on one side of the supporting base material is superposed on both sides of the fiber base material 11, and these are put under reduced pressure conditions.
  • FIG. 2 shows an example when the carrier materials 5a and 5b and the fiber base material 11 are overlapped.
  • the carrier material 5a in which the first resin composition is applied to the substrate in advance and the carrier material 5b in which the second resin composition is applied to the substrate are manufactured.
  • the carrier materials 5a and 5b are overlapped from both sides of the fiber base material 11 under reduced pressure, and bonded with a laminating roll 61 heated to a temperature at which the resin composition melts as necessary.
  • the fiber base material 11 is impregnated with the resin composition coated on the base material.
  • the insulating resin layers of the carrier materials 5a and 5b and the fiber base material 11 are joined by bonding under reduced pressure, the inside of the fiber base material 11 or the insulating resin layers of the carrier materials 5a and 5b.
  • the fiber base material 11 and the fiber base material 11 Even if there is an unfilled portion at the bonding site between the fiber base material 11 and the fiber base material 11, it can be a reduced-pressure void or a substantial vacuum void.
  • the decompression condition is preferably 7000 Pa or less. More preferably, it is 3000 Pa or less. Thereby, the said effect can be expressed highly.
  • a vacuum box device, a vacuum becquerel device, or the like can be used as another device for joining the fiber base material 11 and the carrier materials 5a and 5b under such a reduced pressure.
  • the fiber base material 11 can be continuously supplied and transported in the same direction as the transport direction of the carrier materials 5a and 5b, and has dimensions in the width direction.
  • the dimension in the width direction refers to the dimension of the fiber base material 11 in the direction orthogonal to the transport direction of the fiber base material 11.
  • the thing of a long sheet form can be used suitably, for example.
  • the carrier materials 5a and 5b and the fiber base material 11 When laminating the carrier materials 5a and 5b and the fiber base material 11, it is preferable to heat to a temperature at which the insulating resin layer can be melted. Thereby, carrier material 5a, 5b and the fiber base material 11 can be joined easily. Moreover, when at least a part of the insulating resin layer is melted and impregnated into the fiber base material 11, it becomes easy to obtain a prepreg with good impregnation properties.
  • a method to heat For example, the method of using the laminate roll heated to predetermined temperature at the time of joining etc. can be used suitably.
  • the temperature to be heated here (hereinafter also referred to as “laminate temperature”) is not particularly limited because it varies depending on the type and composition of the resin forming the insulating resin layer, but the softening point of the resin forming the insulating resin layer + 10 ° C. The above temperature is preferred, and the softening point + 30 ° C. or more is more preferred. Thereby, the fiber base material 11 and the insulating resin layer can be easily joined. Further, the productivity of the metal-clad laminate 100 can be further improved by increasing the lamination speed. For example, it can be carried out at 60 ° C. or higher and 150 ° C. or lower.
  • the softening point can be defined by a peak temperature of G ′ / G ′′ in a dynamic viscoelasticity test, for example.
  • the laminating speed at the time of laminating is preferably from 0.5 m / min to 10 m / min, and more preferably from 1.0 m / min to 10 m / min. If it is 0.5 m / min or more, sufficient lamination becomes possible, and if it is 1.0 m / min or more, productivity can be further improved.
  • the lamination pressure is not particularly limited, but is preferably in the range of 15 N / cm 2 or more and 250 N / cm 2 or less, and more preferably in the range of 20 N / cm 2 or more and 100 N / cm 2 or less. Within this range, productivity can be further improved.
  • the tension applied to the fiber base material 11 is as small as possible without causing problems in appearance such as wrinkles. Specifically, it is preferably in the range of 10 N / m to 350 N / m, more preferably in the range of 15 N / m to 250 N / m, and in the range of 18 N / m to 150 N / m. It is particularly preferred that By setting the tension within the above range, strain generated in the prepreg is relieved, and as a result, the metal-clad laminate 100 having further excellent stress relieving ability can be obtained.
  • tensile_strength concerning the fiber base material 11 is included before the process of laminating. Thereby, it is possible to eliminate defects in appearance such as wrinkles that occur when laminating at a low tension.
  • the tension cutting method is not particularly limited, and for example, a known tension cutting method such as a nip roll or an S-shaped nip roll can be used. Further, the tension cut can be achieved by introducing a tension cut device before the lamination. By performing the tension cut by the method as exemplified above, the tension can be reduced as much as possible without impairing the transportability of the fiber base material 11. Therefore, the occurrence of distortion that occurs during lamination and causes warping can be further suppressed.
  • the specific configuration of the means for carrying out the lamination is not particularly limited, but in order to improve the appearance of the resulting metal-clad laminate 100, the pressure surface and the support base 13 are A protective film may be disposed between them.
  • FIG. 3 is a schematic diagram showing an example of the width dimension of each of the support base material, the insulating resin layer, and the fiber base material used in the prepreg manufacturing method of the present embodiment.
  • the carrier material 5a, 5b has a support base 13 having a width dimension larger than that of the fiber base 11 and an insulation having a width dimension larger than that of the fiber base 11. What has the resin layer 15 is used.
  • FIG. 3 (1) shows the relationship among the width direction dimensions of the support base 13, the insulating resin layers 15a and 15b, and the fiber cloth.
  • the insulating resin layer 15a of the carrier material 5a and the fiber base are formed in the inner region of the width direction dimension of the fiber base material 11, that is, in the region where the fiber base material 11 exists in the width direction.
  • the material 11 and the insulating resin layer 15b of the carrier material 5b and the fiber base material 11 can be bonded to each other.
  • the surface of the insulating resin layer 15a of the carrier material 5b and the surface of the insulating resin layer 15b of the carrier material 5b Can be directly joined. This state is shown in FIG.
  • the support base material 13 whose width direction dimension is larger than the fiber base material 11 as carrier material 5a, 5b
  • one of the carrier materials 5a, 5b for example, as the carrier material 5a, rather than the fiber base material 11
  • a material having an insulating resin layer 15a having a large width direction dimension may be used, and a carrier material 5b having an insulating resin layer 15b having the same width direction dimension as the fiber substrate 11 may be used.
  • carrier materials 5a and 5b those having the insulating resin layers 15a and 15b having the same width direction dimensions as the fiber base 11 may be used.
  • a step (C) in which heat treatment is performed at a temperature equal to or higher than the melting temperature of the insulating resin using the hot air drying device 62 may be performed.
  • Other methods for the heat treatment are not particularly limited, but conventionally known methods that can be heated at a predetermined temperature such as an infrared heating device, a heating roll device, a flat platen hot plate press device, a heat circulation heating device, an induction heating device, etc. It can be carried out using a heating device. Among these, the method of carrying out without substantially applying pressure to the above-mentioned joined one is preferable.
  • a hot air drying device or an infrared heating device it can be carried out without substantially applying pressure to the joined one.
  • a prepreg having a desired insulating layer thickness and high uniformity in the insulating layer thickness can be manufactured more efficiently. Can do.
  • a heating roll apparatus and a flat hot disk press apparatus it can implement by making a predetermined pressure act on the said joined thing.
  • the stress acting on the fiber base material along with the flow of the resin component can be minimized, the internal strain can be extremely reduced.
  • the pressure is not substantially applied when the resin component is melted, it is possible to substantially eliminate the occurrence of a dent in this step.
  • the heating temperature is not particularly limited because it varies depending on the type and composition of the resin forming the resin layer, but the temperature range is such that the thermosetting resin used melts and the curing reaction of the thermosetting resin does not proceed rapidly. It is preferable to do.
  • the time for the heat treatment is not particularly limited because it varies depending on the type of the thermosetting resin to be used, but it can be carried out, for example, by treating for 1 to 10 minutes.
  • a step of continuously winding the prepreg obtained above may be included as necessary.
  • a prepreg can be made into a roll form and the handling workability
  • the prepreg manufacturing method in the present embodiment other than the above method includes (2) a method of preparing a resin varnish by dissolving the resin composition in a solvent, and applying the resin varnish to a fiber substrate.
  • the method is described in paragraphs 0022 to 0041 of Reference Document 1 (Japanese Patent Laid-Open No. 2010-275337).
  • Reference Document 1 Japanese Patent Laid-Open No. 2010-275337
  • the fiber base material 3 is conveyed so as to pass between the two die coaters to a coating machine provided with the first coating device 1a and the second coating device 1b, which are two die coaters, on both sides thereof.
  • the resin varnish 4 is applied on each side.
  • the first coating apparatus 1a and the second coating apparatus 1b may use the same die coater or different ones.
  • the 1st coating apparatus 1a and the 2nd coating apparatus 1b may use a roll coater.
  • the coating distance L and the tip overlap distance D preferably have a constant distance as shown in FIGS. 4 and 5, but may not have a constant distance as shown in FIG. .
  • the first coating device 1 a and the second coating device 1 b each have a coating tip 2, and each coating tip 2 is elongated in the width direction of the fiber base 3.
  • tip part 2a which is a coating front-end
  • tip part 2b protrudes toward the other surface of the fiber base material 3.
  • the discharge amount per unit time of the resin varnish 4 discharged from the first coating device 1a and the second coating device 1b may be the same or different.
  • the thickness of the resin varnish 4 to be applied can be individually controlled on one side and the other side of the fiber base 3, and the layer of the resin layer The thickness can be easily adjusted.
  • a prepreg is manufactured by heating at a predetermined temperature in a dryer to volatilize the solvent of the applied resin varnish 4 and to semi-cur the resin composition.
  • the solvent used in the resin varnish preferably exhibits good solubility in the resin component in the resin composition, but a poor solvent may be used as long as it does not have an adverse effect.
  • the solvent exhibiting good solubility include acetone, methyl ethyl ketone, methyl isobutyl ketone, cyclohexanone, tetrahydrofuran, dimethylformamide, dimethylacetamide, dimethyl sulfoxide, ethylene glycol, cellosolve and carbitol.
  • the solid content of the resin varnish is not particularly limited, but is preferably 40% by mass to 80% by mass, and particularly preferably 50% by mass to 70% by mass. Thereby, the impregnation property to the fiber base material of the resin varnish can further be improved.
  • a prepreg can be obtained by impregnating a fiber base material with a resin composition and drying at a predetermined temperature, for example, 80 ° C. or more and 200 ° C. or less.
  • the manufacturing method of the metal-clad laminated board 100 using a prepreg is not specifically limited, For example, it is as follows. After peeling the supporting base material from the obtained prepreg, the metal foil 103 is overlapped on the upper and lower sides or one side of the outer side of the prepreg, and these are joined under a high vacuum condition using a laminator device or a becquerel device, or the outside of the prepreg as it is The metal foil 103 is stacked on both upper and lower surfaces or one surface.
  • the metal foil laminated on the prepreg can be heated and pressurized with a vacuum press or heated with a dryer to obtain the metal-clad laminate 100.
  • the thickness of the metal foil 103 is, for example, not less than 1 ⁇ m and not more than 35 ⁇ m. When the thickness of the metal foil 103 is not less than the above lower limit value, sufficient mechanical strength can be secured when the carrier materials 5a and 5b are manufactured. Further, if the thickness is not more than the above upper limit value, it may be easy to process and form a fine circuit.
  • metal foil when metal foil is used as a support base material, it can be used as the metal-clad laminate 100 as it is, without peeling a support base material.
  • Examples of the metal constituting the metal foil 103 include copper and copper alloys, aluminum and aluminum alloys, silver and silver alloys, gold and gold alloys, zinc and zinc alloys, nickel and nickel alloys, tin and tin. Alloy, iron and iron alloy, Kovar (trade name), 42 alloy, Fe-Ni alloy such as Invar or Super Invar, W or Mo, and the like. Also, an electrolytic copper foil with a carrier can be used.
  • thermosetting resin Although it does not specifically limit as a thermosetting resin, It is preferable that it has a low linear expansion coefficient and a high elasticity modulus, and is excellent in the reliability of thermal shock property.
  • the glass transition temperature of the thermosetting resin is preferably 160 ° C. or higher and 350 ° C. or lower, more preferably 180 ° C. or higher and 300 ° C. or lower. By using a thermosetting resin having such a glass transition temperature, the effect of further improving the lead-free solder reflow heat resistance can be obtained.
  • thermosetting resins for example, novolac type phenol resins such as phenol novolak resin, cresol novolak resin, bisphenol A novolak resin, unmodified resole phenol resin, oil-modified resole modified with tung oil, linseed oil, walnut oil, etc.
  • Phenol resin such as phenolic resin, bisphenol A type epoxy resin, bisphenol F type epoxy resin, bisphenol S type epoxy resin, bisphenol E type epoxy resin, bisphenol M type epoxy resin, bisphenol P type epoxy resin, bisphenol Bisphenol type epoxy resin such as Z type epoxy resin, novolak type epoxy resin such as phenol novolac type epoxy resin, cresol novolac type epoxy resin, biffe Type epoxy resin, biphenyl aralkyl type epoxy resin, aryl alkylene type epoxy resin, naphthalene type epoxy resin, anthracene type epoxy resin, phenoxy type epoxy resin, dicyclopentadiene type epoxy resin, norbornene type epoxy resin, adamantane type epoxy resin, fluorene Type epoxy resin, epoxy resin, urea (urea) resin, resin having triazine ring such as melamine resin, unsaturated polyester resin, bismaleimide resin, polyurethane resin, diallyl phthalate resin, silicone resin, resin having benzoxazine ring, Examples
  • cyanate resins are particularly preferable.
  • the thermal expansion coefficient of the insulating layer 101 can be reduced.
  • the cyanate resin is excellent in electrical characteristics (low dielectric constant, low dielectric loss tangent), mechanical strength, and the like.
  • cyanate resin for example, those obtained by reacting a cyanogen halide compound with phenols, or those obtained by prepolymerization by a method such as heating as required can be used.
  • bisphenol cyanate resins such as novolac type cyanate resin, bisphenol A type cyanate resin, bisphenol E type cyanate resin, tetramethylbisphenol F type cyanate resin, naphthol aralkyl type polyvalent naphthols, cyanogen halide, Cyanate resin, dicyclopentadiene-type cyanate resin, biphenylalkyl-type cyanate resin, and the like obtained by the above reaction.
  • novolac type cyanate resin is preferable.
  • the novolac type cyanate resin the crosslink density is increased and the heat resistance is improved. Therefore, flame retardancy of the insulating layer 101 and the like can be improved.
  • the novolak cyanate resin forms a triazine ring after the curing reaction. Furthermore, it is considered that novolak-type cyanate resin has a high benzene ring ratio due to its structure and is easily carbonized. Furthermore, even when the thickness of the insulating resin layer is 0.6 mm or less, the metal-clad laminate 100 including the insulating layer 101 produced by curing the novolac cyanate resin has excellent rigidity. In particular, since such a metal-clad laminate 100 is excellent in rigidity during heating, it is also excellent in reliability when mounting a semiconductor element. As a novolak-type cyanate resin, what is shown by the following general formula (I) can be used, for example.
  • the average repeating unit n of the novolak cyanate resin represented by the general formula (I) is an arbitrary integer.
  • the lower limit of n is not particularly limited, but is preferably 1 or more, and particularly preferably 2 or more. When n is not less than the above lower limit, the heat resistance of the novolak-type cyanate resin is improved, and it is possible to suppress desorption and volatilization of the low monomer during heating.
  • the upper limit of n is not particularly limited, but is preferably 10 or less, particularly preferably 7 or less. It can suppress that a melt viscosity becomes it high that n is below the said upper limit, and can suppress that the moldability of an insulating resin layer falls.
  • a naphthol type cyanate resin represented by the following general formula (II) is also preferably used.
  • the naphthol type cyanate resin represented by the following general formula (II) includes naphthols such as ⁇ -naphthol or ⁇ -naphthol, p-xylylene glycol, ⁇ , ⁇ '-dimethoxy-p-xylene, 1,4-di ( It is obtained by condensing naphthol aralkyl resin obtained by reaction with 2-hydroxy-2-propyl) benzene and cyanic acid.
  • n is more preferably 10 or less.
  • n 10 or less
  • the resin viscosity does not increase, the impregnation property to the fiber base material is good, and the performance as the metal-clad laminate 100 does not tend to deteriorate.
  • intramolecular polymerization hardly occurs at the time of synthesis, the liquid separation property at the time of washing with water tends to be improved, and the decrease in yield tends to be prevented.
  • R represents a hydrogen atom or a methyl group, and n represents an integer of 1 or more.
  • a dicyclopentadiene type cyanate resin represented by the following general formula (III) is also preferably used.
  • n in the following general formula (III) is more preferably 0 or more and 8 or less.
  • n is 8 or less, the resin viscosity is not high, the impregnation property to the fiber base material is good, and the performance as the metal-clad laminate 100 can be prevented from being lowered.
  • a dicyclopentadiene type cyanate resin it is excellent in low hygroscopicity and chemical resistance.
  • N represents an integer of 0 or more and 8 or less.
  • Mw500 or more is preferable and especially Mw600 or more is preferable.
  • Mw is equal to or more than the above lower limit value, it is possible to suppress the occurrence of tackiness when the insulating resin layer is produced, and to suppress the adhesion of the insulating resin layers to each other or the transfer of the resin. be able to.
  • the upper limit of Mw is not particularly limited, but is preferably Mw 4,500 or less, and particularly preferably Mw 3,000 or less.
  • Mw is equal to or less than the above upper limit value, it is possible to suppress the reaction from being accelerated, and it is possible to suppress the occurrence of molding defects and the decrease in interlayer peel strength when the printed wiring board is used.
  • Mw such as cyanate resin can be measured by, for example, GPC (gel permeation chromatography, standard substance: converted to polystyrene).
  • cyanate resin may be used individually by 1 type, may use together 2 or more types which have different Mw, and uses 1 type or 2 types and those prepolymers together. May be.
  • the content of the thermosetting resin contained in the resin composition is not particularly limited as long as it is appropriately adjusted according to the purpose, but is preferably 5% by mass or more and 90% by mass or less based on the entire resin composition, Furthermore, 10 mass% or more and 80 mass% or less are preferable, and 20 mass% or more and 50 mass% or less are especially preferable.
  • the content of the thermosetting resin is not less than the above lower limit value, handling properties are improved, and it becomes easy to form an insulating resin layer.
  • the content of the thermosetting resin is not more than the above upper limit value, the strength and flame retardancy of the insulating resin layer are improved, the linear expansion coefficient of the insulating resin layer is reduced, and the warp of the metal-clad laminate 100 is reduced. May improve.
  • an epoxy resin substantially free of halogen atoms
  • the epoxy resin include bisphenol A type epoxy resin, bisphenol F type epoxy resin, bisphenol E type epoxy resin, bisphenol S type epoxy resin, bisphenol M type epoxy resin, bisphenol P type epoxy resin, bisphenol Z type epoxy resin and the like.
  • Type epoxy resin phenol novolac type epoxy resin, novolac type epoxy resin such as cresol novolac type epoxy resin, arylphenyl type epoxy resin such as biphenyl type epoxy resin, xylylene type epoxy resin, biphenyl aralkyl type epoxy resin, naphthol type epoxy resin, Naphthalenediol type epoxy resin, bifunctional or tetrafunctional epoxy type naphthalene resin, naphthylene ether type epoxy resin, binaphthyl type epoxy resin Naphthalene-type epoxy resins such as xylene resin, naphthalene-aralkyl-type epoxy resin, anthracene-type epoxy resin, phenoxy-type epoxy resin, dicyclopentadiene-type epoxy resin, norbornene-type epoxy resin, adamantane-type epoxy resin, fluorene-type epoxy resin, etc. .
  • epoxy resin one of these may be used alone, or two or more having different weight average molecular weights may be used in combination, or one or two or more and those prepolymers may be used in combination. May be.
  • aryl alkylene type epoxy resins are particularly preferable. Thereby, moisture-absorbing solder heat resistance and flame retardance can be further improved.
  • the arylalkylene type epoxy resin refers to an epoxy resin having one or more arylalkylene groups in a repeating unit.
  • a xylylene type epoxy resin, a biphenyl dimethylene type epoxy resin, etc. are mentioned.
  • a biphenyl dimethylene type epoxy resin is preferable.
  • mold epoxy resin can be shown, for example with the following general formula (IV).
  • the average repeating unit n of the biphenyl dimethylene type epoxy resin represented by the general formula (IV) is an arbitrary integer.
  • the lower limit of n is not particularly limited, but is preferably 1 or more, and particularly preferably 2 or more. When n is not less than the above lower limit, crystallization of the biphenyldimethylene type epoxy resin can be suppressed and the solubility in a general-purpose solvent is improved, so that handling becomes easy.
  • the upper limit of n is not particularly limited, but is preferably 10 or less, and particularly preferably 5 or less. When n is less than or equal to the above upper limit, the fluidity of the resin is improved and the occurrence of molding defects and the like can be suppressed.
  • epoxy resin other than the above a novolac type epoxy resin having a condensed ring aromatic hydrocarbon structure is preferable. Thereby, heat resistance and low thermal expansibility can further be improved.
  • the novolak type epoxy resin having a condensed ring aromatic hydrocarbon structure is a novolak type epoxy resin having a naphthalene, anthracene, phenanthrene, tetracene, chrysene, pyrene, triphenylene, and tetraphen or other condensed ring aromatic hydrocarbon structure.
  • the novolac type epoxy resin having a condensed ring aromatic hydrocarbon structure is excellent in low thermal expansion because a plurality of aromatic rings can be regularly arranged. Moreover, since the glass transition temperature is also high, it is excellent in heat resistance.
  • the molecular weight of the repeating structure is large, it is superior in flame retardancy compared to conventional novolak type epoxies, and the weakness of cyanate resin can be improved by combining with cyanate resin. Therefore, when used in combination with a cyanate resin, the glass transition temperature is further increased, so that the lead-free compatible mounting reliability is excellent.
  • the novolak-type epoxy resin having a condensed ring aromatic hydrocarbon structure is obtained by epoxidizing a novolac-type phenol resin synthesized from a phenol compound, a formaldehyde compound, and a condensed ring aromatic hydrocarbon compound.
  • the phenol compound is not particularly limited, but examples thereof include cresols such as phenol, o-cresol, m-cresol, p-cresol, 2,3-xylenol, 2,4-xylenol, 2,5-xylenol, 2, 6-xylenol, 3,4-xylenol, xylenols such as 3,5-xylenol, trimethylphenols such as 2,3,5 trimethylphenol, ethyl such as o-ethylphenol, m-ethylphenol, p-ethylphenol Phenols, alkylphenols such as isopropylphenol, butylphenol, t-butylphenol, o-phenylphenol, m-phenylphenol, p-phenylphenol, catechol, 1,5-dihydroxynaphthalene, 1,6-dihydroxynaphtha And naphthalenediols such as 2,7-dihydroxy
  • the aldehyde compound is not particularly limited, and examples thereof include formaldehyde, paraformaldehyde, trioxane, acetaldehyde, propionaldehyde, polyoxymethylene, chloral, hexamethylenetetramine, furfural, glyoxal, n-butyraldehyde, caproaldehyde, allylaldehyde, Examples include benzaldehyde, crotonaldehyde, acrolein, tetraoxymethylene, phenylacetaldehyde, o-tolualdehyde, salicylaldehyde, dihydroxybenzaldehyde, trihydroxybenzaldehyde, 4-hydroxy-3-methoxyaldehyde paraformaldehyde and the like.
  • the fused ring aromatic hydrocarbon compound is not particularly limited, but for example, naphthalene derivatives such as methoxynaphthalene and butoxynaphthalene, anthracene derivatives such as methoxyanthracene, phenanthrene derivatives such as methoxyphenanthrene, other tetracene derivatives, chrysene derivatives, pyrene derivatives, Derivatives such as triphenylene and tetraphen derivatives are mentioned.
  • the novolak-type epoxy resin having a condensed ring aromatic hydrocarbon structure is not particularly limited, and examples thereof include methoxynaphthalene-modified orthocresol novolak epoxy, butoxynaphthalene-modified meta (para) cresol novolak epoxy, and methoxynaphthalene-modified novolak epoxy. It is done. Among these, a novolac type epoxy resin having a condensed ring aromatic hydrocarbon structure represented by the following formula (V) is preferable.
  • Ar is a condensed ring aromatic hydrocarbon group
  • R may be the same or different from each other, and is a hydrogen atom, a hydrocarbon group having 1 to 10 carbon atoms, a halogen element, a phenyl group, A group selected from an aryl group such as a benzyl group and an organic group containing glycidyl ether, n, p and q are integers of 1 or more, and the values of p and q may be the same or different for each repeating unit. May be.
  • (Ar in formula (V) is a structure represented by (Ar1) to (Ar4) in formula (VI), and R in formula (VI) may be the same or different from each other. It is often a group selected from a hydrogen atom, a hydrocarbon group having 1 to 10 carbon atoms or a halogen element, an aryl group such as a phenyl group and a benzyl group, and an organic group including glycidyl ether.)
  • naphthalene type epoxy resins such as naphthol type epoxy resin, naphthalene diol type epoxy resin, bifunctional or tetrafunctional epoxy type naphthalene resin, naphthylene ether type epoxy resin and the like are preferable.
  • heat resistance and low thermal expansibility can further be improved.
  • the naphthalene ring has a higher ⁇ - ⁇ stacking effect than the benzene ring, it is particularly excellent in low thermal expansion and low thermal shrinkage.
  • the polycyclic structure has a high rigidity effect and the glass transition temperature is particularly high, the change in heat shrinkage before and after reflow is small.
  • the naphthol type epoxy resin for example, the following general formula (VII-1); as the naphthalene diol type epoxy resin, the following formula (VII-2); as the bifunctional or tetrafunctional epoxy type naphthalene resin, the following formula (VII-3): Examples of (VII-4) (VII-5) and naphthylene ether type epoxy resin can be represented by the following general formula (VII-6).
  • N represents an average number of 1 to 6, and R represents a glycidyl group or a hydrocarbon group having 1 to 10 carbon atoms.
  • R 1 represents a hydrogen atom or a methyl group
  • R 2 each independently represents a hydrogen atom, an alkyl group having 1 to 4 carbon atoms, an aralkyl group, a naphthalene group, or a glycidyl ether group-containing naphthalene.
  • o and m are each an integer of 0 to 2, and either o or m is 1 or more.
  • the lower limit of the content of the epoxy resin is not particularly limited, but is preferably 1% by mass or more, and particularly preferably 2% by mass or more in the entire resin composition. When the content is not less than the above lower limit, the reactivity of the cyanate resin is improved, and the moisture resistance of the resulting product can be improved.
  • the upper limit of content of an epoxy resin is not specifically limited, 55 mass% or less is preferable and especially 40 mass% or less is preferable. Heat resistance can be improved more as content is below the said upper limit.
  • the lower limit of the weight average molecular weight (Mw) of the epoxy resin is not particularly limited, but is preferably 500 or more, more preferably 800 or more. It can suppress that tackiness arises in a resin layer as Mw is more than the said lower limit.
  • the upper limit of Mw is not particularly limited, but is preferably Mw 20,000 or less, and particularly preferably Mw 15,000 or less. When the Mw is not more than the above upper limit value, the impregnation property to the fiber base material is improved during the production of the insulating resin layer, and a more uniform product can be obtained.
  • the Mw of the epoxy resin can be measured by GPC, for example.
  • Cyanate resins (especially novolak-type cyanate resins, naphthol-type cyanate resins, dicyclopentadiene-type cyanate resins) and epoxy resins (arylalkylene-type epoxy resins, especially biphenyldimethylene-type epoxy resins, condensed ring aromatic hydrocarbons)
  • epoxy resins arylalkylene-type epoxy resins, especially biphenyldimethylene-type epoxy resins, condensed ring aromatic hydrocarbons
  • a phenol resin examples include novolac type phenol resins, resol type phenol resins, aryl alkylene type phenol resins, and the like.
  • phenol resin one of these may be used alone, two or more having different weight average molecular weights may be used in combination, and one or two or more thereof and a prepolymer thereof may be used in combination. May be.
  • aryl alkylene type phenol resins are particularly preferable. Thereby, moisture absorption solder heat resistance can be improved further.
  • aryl alkylene type phenol resin examples include xylylene type phenol resin and biphenyl dimethylene type phenol resin.
  • a biphenyl dimethylene type phenol resin can be shown by the following general formula (VIII), for example.
  • the repeating unit n of the biphenyldimethylene type phenol resin represented by the general formula (VIII) is an arbitrary integer.
  • the lower limit of n is not particularly limited, but is preferably 1 or more, and particularly preferably 2 or more. Heat resistance can be improved more as n is more than the said lower limit.
  • the upper limit of the repeating unit n is not particularly limited, but is preferably 12 or less, particularly preferably 8 or less. Moreover, compatibility with other resin improves that n is below the said upper limit, and workability
  • Cyanate resin especially novolac-type cyanate resin, naphthol-type cyanate resin, dicyclopentadiene-type cyanate resin
  • epoxy resin arylalkylene-type epoxy resin, especially biphenyldimethylene-type epoxy resin, condensed ring aromatic hydrocarbon structure
  • a combination of a novolac type epoxy resin or a naphthol type epoxy resin) and an arylalkylene type phenol resin can control the crosslinking density and easily control the reactivity.
  • the lower limit of the content of the phenol resin is not particularly limited, but is preferably 1% by mass or more, and particularly preferably 5% by mass or more in the entire resin composition. Heat resistance can be improved as content of a phenol resin is more than the said lower limit.
  • the upper limit of content of a phenol resin is not specifically limited, However, 55 mass% or less is preferable in the whole resin composition, and 40 mass% or less is especially preferable. When the content of the phenol resin is not more than the above upper limit value, the characteristics of low thermal expansion can be improved.
  • the lower limit of the weight average molecular weight (Mw) of the phenol resin is not particularly limited, but is preferably Mw 400 or more, particularly preferably Mw 500 or more. It can suppress that tackiness arises in a resin layer as Mw is more than the said minimum.
  • the upper limit of Mw of the phenol resin is not particularly limited, but Mw is preferably 18,000 or less, and particularly preferably Mw 15,000 or less. When the Mw is not more than the above upper limit, the impregnation property to the fiber base material is improved during the production of the resin layer, and a more uniform product can be obtained.
  • the Mw of the phenol resin can be measured by GPC, for example.
  • cyanate resins especially novolak-type cyanate resins, naphthol-type cyanate resins, dicyclopentadiene-type cyanate resins
  • phenol resins arylalkylene-type phenol resins, especially biphenyldimethylene-type phenol resins
  • epoxy resins arylalkylene-type epoxy resins
  • the resin composition further contains an inorganic filler.
  • filler examples include silicates such as talc, calcined clay, unfired clay, mica and glass, oxides such as titanium oxide, alumina, boehmite, silica and fused silica, calcium carbonate, magnesium carbonate, hydrotalcite and the like.
  • silicates such as talc, calcined clay, unfired clay, mica and glass
  • oxides such as titanium oxide, alumina, boehmite, silica and fused silica, calcium carbonate, magnesium carbonate, hydrotalcite and the like.
  • hydroxides such as aluminum hydroxide, magnesium hydroxide, calcium hydroxide, sulfates or sulfites
  • barium sulfate calcium sulfate, calcium sulfite, zinc borate, barium metaborate, aluminum borate, boron
  • borates such as calcium oxide and sodium borate
  • nitrides such as aluminum nitride, boron nitride, silicon nitride, and carbon nitride
  • titanates such as strontium titanate and barium titanate.
  • the filler one of these may be used alone, or two or more may be used in combination.
  • silica is particularly preferable, and fused silica (especially spherical fused silica) is preferable in terms of excellent low thermal expansion.
  • the fused silica has a crushed shape and a spherical shape.
  • a usage method suitable for the purpose such as using spherical silica to lower the melt viscosity of the resin composition.
  • the lower limit of the average particle diameter of the filler is not particularly limited, but is preferably 0.01 ⁇ m or more, particularly preferably 0.1 ⁇ m or more. It can suppress that the viscosity of a varnish becomes high as the particle size of a filler is the said lower limit or more, and the workability
  • the upper limit of the average particle size is not particularly limited, but is preferably 5.0 ⁇ m or less, and particularly preferably 2.0 ⁇ m or less. When the particle size of the filler is not more than the above upper limit, phenomena such as sedimentation of the filler in the varnish can be suppressed, and a more uniform resin layer can be obtained. In addition, when the L / S of the conductor circuit of the inner layer substrate is less than 20/20 ⁇ m, it is possible to suppress the influence on the insulation between the wirings.
  • the average particle size of the filler is measured, for example, by measuring the particle size distribution of the particles on a volume basis using a laser diffraction type particle size distribution measuring device (manufactured by HORIBA, LA-500), and the median diameter (d 50 ) is defined as the average particle size. To do.
  • the filler is not particularly limited, but a monodisperse filler having an average particle diameter may be used, or a polydisperse filler having an average particle diameter may be used. Furthermore, a monodispersed and / or polydispersed filler having an average particle size may be used alone or in combination of two or more.
  • the filler is preferably spherical silica (especially spherical fused silica) having an average particle size of 5.0 ⁇ m or less, and particularly preferably spherical fused silica having an average particle size of 0.01 ⁇ m or more and 2.0 ⁇ m or less. Thereby, the filling property of the filler can be further improved.
  • the resin composition of the present embodiment preferably includes a nanosilica median diameter d 50 of less 100 nm (particularly spherical nanosilica) a volume-based particle size distribution by a laser diffraction scattering particle size distribution measuring method. Since the said nano silica can exist in the clearance gap of a filler with a large particle size, or the strand of a fiber base material, the filling property of a filler can further be improved by containing nano silica.
  • the content of the filler is not particularly limited, but is preferably 20% by mass or more and 80% by mass or less, and particularly preferably 30% by mass or more and 75% by mass or less in the entire resin composition. When the content is within the above range, particularly low thermal expansion and low water absorption can be achieved.
  • the resin composition used in the present embodiment can also contain a rubber component, for example, rubber particles can be used.
  • rubber particles include core-shell type rubber particles, crosslinked acrylonitrile butadiene rubber particles, crosslinked styrene butadiene rubber particles, acrylic rubber particles, and silicone particles.
  • the core-shell type rubber particles are rubber particles having a core layer and a shell layer.
  • a two-layer structure in which an outer shell layer is formed of a glassy polymer and an inner core layer is formed of a rubbery polymer or Examples include a three-layer structure in which the outer shell layer is made of a glassy polymer, the intermediate layer is made of a rubbery polymer, and the core layer is made of a glassy polymer.
  • the glassy polymer layer is made of, for example, a polymer of methyl methacrylate, and the rubbery polymer layer is made of, for example, a butyl acrylate polymer (butyl rubber).
  • core-shell type rubber particles include Staphyloid AC3832, AC3816N (trade names, manufactured by Ganz Kasei Co., Ltd.), and Metabrene KW-4426 (trade names, manufactured by Mitsubishi Rayon Co., Ltd.).
  • NBR crosslinked acrylonitrile butadiene rubber
  • XER-91 average particle size 0.5 ⁇ m, manufactured by JSR.
  • SBR crosslinked styrene butadiene rubber
  • acrylic rubber particles include methabrene W300A (average particle size 0.1 ⁇ m), W450A (average particle size 0.2 ⁇ m) (manufactured by Mitsubishi Rayon Co., Ltd.), and the like.
  • the silicone particles are not particularly limited as long as they are rubber elastic fine particles formed of organopolysiloxane.
  • core-shell structure particles coated with silicone mainly composed of a three-dimensional crosslinking type examples of silicone rubber fine particles.
  • commercially available products such as KMP-605, KMP-600, KMP-597, KMP-594 (manufactured by Shin-Etsu Chemical), Trefil E-500, Trefil E-600 (manufactured by Toray Dow Corning) Can be used.
  • the content of the rubber particles is not particularly limited, but is preferably 20% by mass or more and 80% by mass or less, and particularly preferably 30% by mass or more and 75% by mass or less based on the entire resin composition, including the above inorganic filler. . When the content is within the range, particularly low water absorption can be achieved.
  • additives such as a coupling agent, a curing accelerator, a curing agent, a thermoplastic resin, and an organic filler can be appropriately blended in the resin composition as necessary.
  • the resin composition used in the present embodiment can be suitably used in a liquid form in which the above components are dissolved and / or dispersed with an organic solvent or the like.
  • the coupling agent By using the coupling agent, the wettability of the interface between the thermosetting resin and the filler is improved, and the resin composition can be uniformly fixed to the fiber substrate. Therefore, it is preferable to use a coupling agent, and heat resistance, particularly solder heat resistance after moisture absorption can be improved.
  • any of those usually used as a coupling agent can be used. Specifically, an epoxy silane coupling agent, a cationic silane coupling agent, an aminosilane coupling agent, a titanate coupling agent, and silicone. It is preferable to use one or more coupling agents selected from oil-type coupling agents. Thereby, the wettability with the interface of a filler can be made high, and thereby heat resistance can be improved more.
  • the lower limit of the addition amount of the coupling agent is not particularly limited because it depends on the specific surface area of the filler, but is preferably 0.05 parts by mass or more, particularly 0.1 parts by mass or more with respect to 100 parts by mass of the filler.
  • the upper limit of the amount added is not particularly limited, but is preferably 3 parts by mass or less, and particularly preferably 2 parts by mass or less. When the content is not more than the above upper limit value, it is possible to suppress the influence on the reaction, and it is possible to suppress a decrease in bending strength and the like.
  • organic metal salts such as zinc naphthenate, cobalt naphthenate, tin octylate, cobalt octylate, zinc octylate, bisacetylacetonate cobalt (II), trisacetylacetonate cobalt (III), triethylamine, tributylamine, Tertiary amines such as diazabicyclo [2,2,2] octane, 2-phenyl-4-methylimidazole, 2-ethyl-4-ethylimidazole, 2-phenyl-4-ethylimidazole, 2-phenyl-4-methyl Imidazoles such as -5-hydroxyimidazole and 2-phenyl-4,5-dihydroxyimidazole, phenolic compounds such as phenol, bisphenol A and nonylphenol, organic acids such as acetic acid, benzoic acid, salicylic acid,
  • Etc. um salt compound or a mixture thereof.
  • the curing accelerator one kind including these derivatives may be used alone, or two or more kinds including these derivatives may be used in combination.
  • the onium salt compound is not particularly limited, and for example, an onium salt compound represented by the following general formula (IX) can be used.
  • R 1 , R 2 , R 3 and R 4 each represents an organic group having a substituted or unsubstituted aromatic ring or heterocyclic ring, or a substituted or unsubstituted aliphatic group. May be the same as or different from each other, and A ⁇ represents an anion of an n (n ⁇ 1) -valent proton donor having at least one proton that can be released outside the molecule, or a complex anion thereof. Is shown.
  • the minimum of content of a hardening accelerator is not specifically limited, 0.005 mass% or more of the whole resin composition is preferable, and 0.008 mass% or more is especially preferable.
  • the upper limit of the content is not particularly limited, but is preferably 5% by mass or less, and particularly preferably 2% by mass or less, based on the entire resin composition. The preservability of a prepreg can be improved more as content is below the said upper limit.
  • Polystyrene thermoplastic elastomers such as coalescence, polyolefin thermoplastic elastomers, polyamide elastomers, thermoplastic elastomers such as polyester elastomers, and diene elastomers such as polybutadiene, epoxy-modified polybutadiene, acrylic-modified polybutadiene, and methacryl-modified polybutadiene are used in combination. May be.
  • phenoxy resin examples include a phenoxy resin having a bisphenol skeleton, a phenoxy resin having a naphthalene skeleton, a phenoxy resin having an anthracene skeleton, and a phenoxy resin having a biphenyl skeleton.
  • a phenoxy resin having a structure having a plurality of these skeletons can also be used.
  • a phenoxy resin having a biphenyl skeleton and a bisphenol S skeleton as the phenoxy resin.
  • the glass transition temperature of the phenoxy resin can be increased due to the rigidity of the biphenyl skeleton, and the adhesion between the phenoxy resin and the metal can be improved due to the presence of the bisphenol S skeleton.
  • the heat resistance of the laminated board can be improved, and the adhesion of the wiring layer to the laminated board can be improved when a printed wiring board is manufactured.
  • a phenoxy resin having a bisphenol A skeleton and a bisphenol F skeleton as the phenoxy resin.
  • a phenoxy resin having a bisphenolacetophenone structure represented by the following general formula (X).
  • R 1 may be the same or different from each other, and is a hydrogen atom, a hydrocarbon group having 1 to 10 carbon atoms or a group selected from halogen elements
  • R 2 is a hydrogen atom, carbon It is a group selected from a hydrocarbon group having a number of 1 or more and 10 or less, or a halogen element
  • R 3 is a hydrogen atom or a hydrocarbon group having a carbon number of 1 or more and 10 or less
  • m is an integer of 0 or more and 5 or less.
  • the phenoxy resin containing a bisphenol acetophenone structure has a bulky structure, it has excellent solvent solubility and compatibility with the thermosetting resin component to be blended. Moreover, since a uniform rough surface can be formed with low roughness, the fine wiring formability is excellent.
  • the phenoxy resin having a bisphenolacetophenone structure can be synthesized by a known method such as a method in which an epoxy resin and a phenol resin are polymerized with a catalyst.
  • the phenoxy resin having a bisphenol acetophenone structure may contain a structure other than the bisphenol acetophenone structure of the general formula (X), and the structure is not particularly limited, but bisphenol A type, bisphenol F type, bisphenol S type, biphenyl Type, phenol novolac type, cresol novolac type structure and the like. Among them, those containing a biphenyl structure are preferable because of their high glass transition temperature.
  • the content of the bisphenol acetophenone structure of the general formula (X) in the phenoxy resin containing a bisphenol acetophenone structure is not particularly limited, but is preferably 5 mol% to 95 mol%, more preferably 10 mol% to 85 mol%. More preferably, it is 15 mol% or more and 75 mol% or less.
  • the effect which improves heat resistance and moisture-proof reliability can fully be exhibited as content is more than the said lower limit.
  • solvent solubility can be improved as content is below the said upper limit.
  • the weight average molecular weight (Mw) of the phenoxy resin is not particularly limited, but is preferably from 5,000 to 100,000, more preferably from 10,000 to 70,000, and most preferably from 20,000 to 50,000.
  • Mw is not more than the above upper limit, compatibility with other resins and solubility in a solvent can be improved.
  • it is at least the above lower limit the film-forming property is improved, and it is possible to suppress the occurrence of problems when used for the production of a printed wiring board.
  • the content of the phenoxy resin is not particularly limited, but is preferably 0.5% by mass or more and 40% by mass or less, and particularly preferably 1% by mass or more and 20% by mass or less of the resin composition excluding the filler.
  • the content is equal to or higher than the lower limit, it is possible to suppress a decrease in mechanical strength of the insulating resin layer and a decrease in plating adhesion with the conductor circuit.
  • it is not more than the above upper limit value, an increase in the thermal expansion coefficient of the insulating layer can be suppressed, and the heat resistance can be lowered.
  • the resin composition may contain additives other than the above components such as pigments, dyes, antifoaming agents, leveling agents, ultraviolet absorbers, foaming agents, antioxidants, flame retardants, and ion scavengers as necessary. It may be added.
  • pigments examples include kaolin, synthetic iron oxide red, cadmium yellow, nickel titanium yellow, strontium yellow, hydrous chromium oxide, chromium oxide, cobalt aluminate, synthetic ultramarine blue and other inorganic pigments, phthalocyanine polycyclic pigments, azo pigments, etc. Etc.
  • the dye examples include isoindolinone, isoindoline, quinophthalone, xanthene, diketopyrrolopyrrole, perylene, perinone, anthraquinone, indigoid, oxazine, quinacridone, benzimidazolone, violanthrone, phthalocyanine, and azomethine.
  • Fiber base Although it does not specifically limit as a fiber base material, Polyamide-type resin fiber base materials, such as glass fiber base materials, such as a glass cloth, polybenzoxazole resin fiber, a polyamide resin fiber, an aromatic polyamide resin fiber, a wholly aromatic polyamide resin fiber Polyester resin fiber base materials such as polyester resin fibers, aromatic polyester resin fibers, wholly aromatic polyester resin fibers, synthetic fiber base materials composed mainly of polyimide resin fibers, fluororesin fibers, kraft paper, cotton Examples thereof include organic fiber base materials such as linter paper and paper base materials mainly composed of linter paper and kraft pulp mixed paper. Among these, a glass fiber substrate is particularly preferable from the viewpoint of strength and water absorption. Moreover, the thermal expansion coefficient of the insulating layer 101 can be further reduced by using a glass fiber substrate.
  • Polyamide-type resin fiber base materials such as glass fiber base materials, such as a glass cloth, polybenzoxazole resin fiber, a polyamide resin fiber, an aromatic polyamide resin fiber, a who
  • the glass fiber substrate used in the present embodiment preferably has a basis weight (weight of the fiber substrate per 1 m 2 ) of 4 g / m 2 or more and 150 g / m 2 or less, and 8 g / m 2 or more and 110 g / m. 2 or less, more preferably 12 g / m 2 or more and 60 g / m 2 or less, further preferably 12 g / m 2 or more and 30 g / m 2 or less, and further preferably 12 g / m 2 or more and 24 g / m 2 or less. It is particularly preferable that m 2 or less.
  • the basis weight is not more than the above upper limit value, the impregnation property of the resin composition in the fiber base material is improved, and the occurrence of strand voids and a decrease in insulation reliability can be suppressed.
  • strength of a glass fiber base material or a prepreg can be improved as basic weight is more than the said lower limit. As a result, handling properties can be improved, prepreg can be easily produced, and reduction in the warpage reduction effect of the substrate can be suppressed.
  • a glass fiber base material having a linear expansion coefficient of 6 ppm / ° C. or lower is particularly preferable, and a glass fiber base material of 3.5 ppm / ° C. or lower is more preferable.
  • a glass fiber base material having such a linear expansion coefficient warpage of the metal-clad laminate 100 of this embodiment can be further suppressed.
  • the tensile modulus of the material constituting the glass fiber substrate used in the present embodiment is preferably 60 GPa or more and 100 GPa or less, more preferably 65 GPa or more and 95 GPa or less, and particularly preferably 85 GPa or more and 95 GPa or less. preferable.
  • a fiber base material having such a tensile elastic modulus for example, deformation of the wiring board due to reflow heat during semiconductor mounting can be effectively suppressed, so that the connection reliability of electronic components is further improved.
  • the fiber base material used in the present embodiment preferably has a dielectric constant at 1 MHz of 3.8 or more and 7.0 or less, more preferably 3.8 or more and 6.8 or less. It is especially preferable that it is above 5.5.
  • the dielectric constant of the metal-clad laminate 100 can be further reduced, which is suitable for a semiconductor package using a high-speed signal.
  • glass fiber base material having the above-described linear expansion coefficient, tensile elastic modulus, and dielectric constant
  • examples of the glass fiber base material having the above-described linear expansion coefficient, tensile elastic modulus, and dielectric constant include E glass, S glass, D glass, T glass, NE glass, UT glass, L glass, and quartz glass.
  • a glass fiber substrate is preferably used.
  • the thickness of the fiber substrate is not particularly limited, but is preferably 5 ⁇ m or more and 150 ⁇ m or less, more preferably 10 ⁇ m or more and 100 ⁇ m or less, and further preferably 12 ⁇ m or more and 60 ⁇ m or less.
  • the thickness of the fiber base material is not more than the above upper limit value, the impregnation property of the resin composition in the fiber base material is improved, and the occurrence of a decrease in strand voids and insulation reliability can be suppressed.
  • strength of a fiber base material or a prepreg can be improved as the thickness of a fiber base material is more than the said lower limit. As a result, handling properties can be improved, prepreg can be easily produced, and reduction in the warpage reduction effect of the substrate can be suppressed.
  • the number of fiber base materials used is not limited to one, and a plurality of thin fiber base materials can be used in a stacked manner.
  • the total thickness only needs to satisfy the above range.
  • the sum total of the fiber base material and filler contained in the insulating layer 101 in this embodiment is 55 mass% or more and 90 mass% or less, and it is more preferable that it is 70 mass% or more and 85 mass% or less. preferable.
  • the rigidity of the metal-clad laminate 100 is increased while balancing the resin impregnation property and moldability into the fiber base material, and the metal-clad laminate at the time of mounting. The warp of the plate 100 can be further reduced.
  • the metal-clad laminate 100 can be used in a semiconductor package 200 as shown in FIG.
  • a method for manufacturing the semiconductor package 200 is not particularly limited, and examples thereof include the following methods. Through-holes for interlayer connection are formed in the metal-clad laminate 100, and a wiring layer is produced by a subtractive method, a semi-additive method, or the like. Thereafter, build-up layers (not shown in FIG. 7) are stacked as necessary, and the steps of interlayer connection and circuit formation by the additive method are repeated. And if necessary, the solder resist layer 201 is laminated
  • a part or all of the buildup layer and the solder resist layer may or may not include a fiber base material.
  • solder resist layer 201 After a photoresist is applied to the entire surface of the solder resist layer 201, a part of the photoresist is removed to expose a part of the solder resist layer 201. Note that a resist having a photoresist function may be used for the solder resist layer 201. In this case, the step of applying a photoresist can be omitted. Next, the exposed solder resist layer is removed to form the opening 209.
  • the semiconductor element 203 is fixed to the connection terminal 205 which is a part of the wiring pattern via the solder bump 207. Thereafter, the semiconductor element 203, the solder bump 207, and the like are sealed with a sealing material 211, whereby the semiconductor package 200 as shown in FIG. 7 is obtained.
  • the semiconductor package 200 can be used in a semiconductor device 300 as shown in FIG.
  • a method for manufacturing the semiconductor device 300 is not particularly limited, and examples thereof include the following methods.
  • the solder bump 301 is formed by supplying a solder paste to the opening 209 of the solder resist layer 201 of the obtained semiconductor package 200 and performing a reflow process.
  • the solder bump 301 can also be formed by attaching a solder ball prepared in advance to the opening 209.
  • the semiconductor package 200 is mounted on the mounting substrate 303 by joining the connection terminals 305 and the solder bumps 301 of the mounting substrate 303, and the semiconductor device 300 shown in FIG. 8 is obtained.
  • the metal-clad laminate 100 with reduced warpage is provided.
  • the metal-clad laminate 100 is thin, the occurrence of warpage can be effectively suppressed.
  • the printed wiring board using the metal-clad laminated board 100 in this embodiment is excellent in mechanical characteristics, such as curvature and dimensional stability, and a moldability. Therefore, the metal-clad laminate 100 in the present embodiment can be suitably used for applications that require reliability, such as printed wiring boards that require higher density and higher multilayer.
  • the occurrence of warpage is reduced in the above-described circuit processing and the subsequent processes. Further, the semiconductor package 200 in the present embodiment is less likely to warp and crack, and can be thinned. Therefore, the semiconductor device 300 including the semiconductor package 200 can improve connection reliability.
  • each thickness is represented by the average film thickness.
  • Epoxy resin A Biphenyl aralkyl type novolak epoxy resin (Nippon Kayaku Co., Ltd., NC-3000)
  • Epoxy resin B biphenyl aralkyl type epoxy resin (manufactured by Nippon Kayaku Co., Ltd., NC-3000FH)
  • Epoxy resin C naphthalene diol diglycidyl ether (DIC Corporation, Epicron HP-4032D)
  • Epoxy resin D naphthylene ether type epoxy resin (manufactured by DIC, Epicron HP-6000)
  • Epoxy resin E Rubber-modified epoxy resin (manufactured by Daicel Chemical Industries, PB-3600)
  • Epoxy resin F biphenyl aralkyl type epoxy resin (Nippon Kayaku Co., Ltd., NC-3000H)
  • Cyanate resin A Novolac-type cyanate resin (Lonza Japan, Primaset PT-30)
  • Cyanate resin B p-xylene-modified naphthol aralkyl-type cyanate resin represented by the general formula (II) (reaction product of naphthol aralkyl-type phenol resin (manufactured by Toto Kasei Co., Ltd., “SN-485 derivative”) and cyanogen chloride)
  • Phenol resin A biphenyl dimethylene type phenol resin (manufactured by Nippon Kayaku Co., Ltd., GPH-103)
  • Amine compound 4,4′-diaminodiphenylmethane bismaleimide compound (KMI Kasei Kogyo BMI-70)
  • Phenoxy resin A Phenoxy resin containing bisphenolacetophenone structure (Mitsubishi Chemical Corporation, YX-6594BH30, solid content 30% by weight)
  • Filler A Spherical silica (manufactured by Admatechs, SO-25R, average particle size 0.5 ⁇ m)
  • Filler B Spherical silica (manufactured by Admatechs, SO-31R, average particle size 1.0 ⁇ m)
  • Filler C Nanosilica (manufactured by Admatechs, Admanano, KBM403E surface-treated product, average particle size 50 nm)
  • Filler D Boehmite (Navaltech AOH-30)
  • Filler E Silicone particles (manufactured by Shin-Etsu Chemical Co., Ltd., KMP-600, average particle size 5 ⁇ m)
  • Coupling agent A ⁇ -glycidoxypropyltrimethoxysilane (manufactured by Momentive Performance Materials, A-187)
  • Coupling agent B N-phenyl- ⁇ -aminopropyltrimethoxysilane (manufactured by Shin-Etsu Chemical Co., Ltd., KBM-573)
  • Curing accelerator A Phosphorus catalyst of an onium salt compound corresponding to the above general formula (IX) (C05-MB, manufactured by Sumitomo Bakelite Co., Ltd.)
  • Curing accelerator B Zinc octylate curing accelerator C: 2-ethyl-4-methylimidazole (manufactured by Shikoku Chemicals, 2E4MZ)
  • the metal-clad laminate in this embodiment was produced using the following procedure. First, production of a prepreg will be described.
  • the composition of the resin varnish used is shown in Table 1 (solid substance amount%), and the thickness of each layer of the obtained prepregs 1 to 8 is shown in Table 2.
  • P1 to P8 refer to prepregs 1 to prepreg 8
  • Unitika described in Table 2 refers to Unitika Glass Fiber
  • Nittobo refers to Nittobo.
  • Prepreg 1 Preparation of Varnish 1 of Resin Composition 11.0 parts by mass of biphenylaralkyl type novolac epoxy resin (Nippon Kayaku Co., Ltd., NC-3000) as epoxy resin A, 3.5 parts by mass of 4,4′-diaminodiphenylmethane as amine compound
  • As a bismaleimide compound 20.0 parts by mass of bis- (3-ethyl-5-methyl-4-maleimidophenyl) methane (manufactured by KAI Kasei Kogyo Co., Ltd., BMI-70) was dissolved and dispersed in methyl ethyl ketone.
  • Resin varnish 1 is dried on a thin copper foil with carrier foil (Mitsui Metal Mining Co., Ltd., Micro Thin Ex, 1.5 ⁇ m) as a support substrate using a die coater device. The film was coated to a thickness of 30 ⁇ m and dried for 5 minutes with a dryer at 160 ° C. to obtain a resin sheet 1A with a copper foil (carrier material 1A) for the first resin layer.
  • carrier foil Mitsubishi Metal Mining Co., Ltd., Micro Thin Ex, 1.5 ⁇ m
  • the resin varnish 1 is applied in the same manner onto an ultrathin copper foil with carrier foil (Mitsui Metal Mining Co., Ltd., Microcin Ex, 1.5 ⁇ m), and the thickness of the resin layer after drying is 30 ⁇ m. And drying for 5 minutes with a dryer at 160 ° C. to obtain a resin sheet 1B with copper foil (carrier material 1B) for the second resin layer.
  • an ultrathin copper foil with carrier foil Mitsubishi Metal Mining Co., Ltd., Microcin Ex, 1.5 ⁇ m
  • prepreg 1 The carrier material 1A for the first resin layer and the carrier material 1B for the second resin layer are made of a glass fiber substrate (thickness 91 ⁇ m, E glass woven fabric manufactured by Unitika, E10T, IPC standard 2116, linear expansion coefficient: 5. 5 ppm / ° C.) on both sides of the resin layer so as to face the fiber substrate, and impregnated with the resin composition by the vacuum laminating apparatus and hot air drying apparatus shown in FIG. 2 to obtain a prepreg 1 on which the copper foil was laminated. .
  • a glass fiber substrate thickness 91 ⁇ m, E glass woven fabric manufactured by Unitika, E10T, IPC standard 2116, linear expansion coefficient: 5. 5 ppm / ° C.
  • the carrier material A and the carrier material B are overlapped on both surfaces of the glass fiber base so that they are positioned at the center in the width direction of the glass fiber base, respectively, and 9.999 ⁇ 10 4 Pa (from normal pressure) Under a condition where the pressure was reduced by about 750 Torr) or more, the laminating speed was set to 2 m / min, the tension applied to the glass fiber substrate was set to 140 N / m, and bonding was performed using a 100 ° C. laminating roll.
  • the resin layers of the carrier material 1A and the carrier material 1B are respectively bonded to both sides of the glass fiber base material, and the width direction dimension of the glass fiber base material In the outer region, the resin layers of the carrier material 1A and the carrier material 1B were joined together.
  • prepreg 1 (P1).
  • prepregs 2 to 4 were different from Tables 1 and 2 except that the types of resin varnishes, the thicknesses of the first and second resin layers, the glass fiber substrate used, the lamination speed, and the tension applied to the glass fiber substrate were changed as shown in Tables 1 and 2 Was produced in the same manner as prepreg 1.
  • the prepreg 5 uses a PET film (polyethylene terephthalate, Purex manufactured by Teijin DuPont Films, Inc., thickness 36 ⁇ m) as a supporting substrate, the type of resin varnish, the thickness of the first and second resin layers, and the glass fiber base used. It was produced in the same manner as prepreg 1 except that the material, the lamination speed, and the tension applied to the glass fiber substrate were changed as shown in Tables 1 and 2.
  • Prepreg 6 The prepreg 6 impregnates a resin varnish 4 into a glass fiber substrate (thickness: 91 ⁇ m, Nittobo T-glass woven fabric, WTX-116E, IPC standard 2116T, linear expansion coefficient: 2.8 ppm / ° C.) with a coating apparatus. And dried in a heating furnace at 180 ° C. for 2 minutes to produce a 100 ⁇ m prepreg.
  • rate and the tension concerning a glass fiber base material were performed on the conditions of Table 2.
  • Prepreg 7 The prepreg 7 impregnates the resin varnish 4 into a glass fiber base (thickness: 43 ⁇ m, Nittobo T-glass woven fabric, WTX-1078, IPC standard 1078T, linear expansion coefficient: 2.8 ppm / ° C.) with a coating device. And dried in a heating furnace at 180 ° C. for 2 minutes to produce a 50 ⁇ m prepreg.
  • rate and the tension concerning a glass fiber base material were performed on the conditions of Table 2.
  • Example 1 Manufacture of metal-clad laminate A metal-clad laminate was obtained by sandwiching a prepreg 1 laminated with a copper foil between smooth metal plates and heating and pressing at 220 ° C. and 1.5 MPa for 2 hours. The thickness of the core layer (part consisting of the laminate) of the obtained laminate with metal foil was 0.10 mm.
  • an electroless copper plating film is formed to a thickness of about 0.5 ⁇ m, a plating resist is formed, and the electroless copper plating film is used as a feeding layer to form a pattern electroplated copper of 20 ⁇ m.
  • L / S 25/25 ⁇ m fine circuit processing was performed.
  • the power feeding layer was removed by flash etching.
  • solder resist layer was laminated, and then exposed and developed so that the semiconductor element mounting pad and the like were exposed, and then opened.
  • the electroless nickel plating layer 3 ⁇ m, and further, the electroless gold plating layer 0.1 ⁇ m and then the solder plating layer 5 ⁇ m are formed,
  • substrate was cut
  • a semiconductor element (TEG chip, size 8 mm ⁇ 8 mm, thickness 100 ⁇ m) having solder bumps was mounted on a printed wiring board for a semiconductor package by thermocompression bonding using a flip chip bonder device.
  • a liquid sealing resin (CRP-X4800B, manufactured by Sumitomo Bakelite Co., Ltd.) was filled, and the liquid sealing resin was cured to obtain a semiconductor package.
  • the liquid sealing resin was cured at a temperature of 150 ° C. for 120 minutes.
  • the solder bump of the semiconductor element used what was formed with the lead free solder of Sn / Ag / Cu composition.
  • Examples 2 to 4, 6 and Comparative Example 1 A metal-clad laminate and a semiconductor package were produced in the same manner as in Example 1 except that the type of prepreg was changed.
  • Example 5 Ultra-thin copper foil (Mitsui Metal Mining Co., Ltd., Micro Thin Ex, 1.5 ⁇ m) is superimposed on both sides of the two prepregs 5 from which the PET film has been peeled off, and heated and pressed at 220 ° C. and 3.0 MPa for 2 hours. As a result, a metal-clad laminate was obtained. The thickness of the core layer (part consisting of the laminate) of the obtained laminate with metal foil was 0.10 mm.
  • a semiconductor package was manufactured in the same manner as in Example 1 except that the carrier material shown in Table 2 was used.
  • Example 7 By superposing ultrathin copper foil (Mitsui Metal Mining Co., Ltd., Microcin Ex, 1.5 ⁇ m) on both surfaces of two prepregs 7 and heating and pressing at 220 ° C. and 3.0 MPa for 2 hours, A laminate was obtained. The thickness of the core layer (part consisting of the laminate) of the obtained laminate with metal foil was 0.10 mm. A semiconductor package was manufactured in the same manner as in Example 1 except that the carrier material shown in Table 2 was used.
  • ultrathin copper foil Mitsubishi Metal Mining Co., Ltd., Microcin Ex, 1.5 ⁇ m
  • the glass transition temperature was measured by dynamic viscoelasticity measurement (DMA). A test piece of 8 mm ⁇ 40 mm was cut out from the obtained laminate, and measured using a TA instrument DMA2980 at a heating rate of 5 ° C./min and a frequency of 1 Hz. The glass transition temperature was a temperature at which tan ⁇ had a maximum value at a frequency of 1 Hz.
  • DMA dynamic viscoelasticity measurement
  • the linear expansion coefficient ⁇ 3 at 25 ° C. was calculated. Simultaneously with the measurement of the linear expansion coefficient, the deformation amounts in the longitudinal direction (x) and the lateral direction (y) of the insulating layer were measured, respectively, and the deformation rates C 1 and C 2 were calculated from the following equations (1) and (2). Each was calculated.
  • C 1 L 1 / L 0 (1)
  • C 2 L 2 / L 0 (2)
  • L 0 is the reference length of the insulating layer ((1) the length of the insulating layer at 25 ° C. in the temperature raising process from 25 ° C. to 300 ° C.), specifically the length of one side of the test piece. It shows.
  • L 1 is a deformation amount from the reference length of the insulating layer at 25 ° C. in cooling step to 25 ° C. from (2) 300 °C.
  • L 2 is (1) the amount of deformation from the reference length L 0 of the insulating layer at T g in the temperature raising step from 25 ° C. to 300 ° C., and (2) the above amount in the temperature lowering step from 300 ° C. to 25 ° C. which is the difference between the deformation amount from the reference length L 0 of the insulating layer in the T g.
  • Warpage amount of the semiconductor package is determined by placing the chip surface on a chamber that can be heated and cooled, and the substrate (size: 14 mm x 14 mm) from the BGA surface in an atmosphere of -50 ° C and 125 ° C. The change in the amount of warpage in the upper 13 mm ⁇ 13 mm portion was measured. The sample used was the semiconductor package manufactured in the above example. Each code is as follows. A: Change in warpage amount was less than 150 ⁇ m (good) ⁇ : Change in warpage was 150 ⁇ m or more and less than 350 ⁇ m (substantially no problem) X: Change in warpage amount was 350 ⁇ m or more
  • the measurement range is 48 mm x 48 mm, the measurement is performed by applying a laser to one side of the substrate, the distance from the laser head is the difference between the farthest point and the nearest point, and the warp amount of each piece.
  • the average of the amount of warpage was taken as the amount of substrate warpage.
  • X Change in warpage amount was 150 ⁇ m or more

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  • Engineering & Computer Science (AREA)
  • Microelectronics & Electronic Packaging (AREA)
  • Physics & Mathematics (AREA)
  • Condensed Matter Physics & Semiconductors (AREA)
  • General Physics & Mathematics (AREA)
  • Computer Hardware Design (AREA)
  • Power Engineering (AREA)
  • Laminated Bodies (AREA)
PCT/JP2013/001387 2012-03-14 2013-03-06 金属張積層板、プリント配線基板、半導体パッケージ、および半導体装置 WO2013136722A1 (ja)

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JP7320388B2 (ja) * 2019-06-26 2023-08-03 旭化成株式会社 ガラスクロス、プリプレグ、及びプリント配線板
TWI748505B (zh) * 2020-06-08 2021-12-01 日商旭化成股份有限公司 玻璃布、預浸體、及印刷佈線板
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