Transfer film, transfer film manufacturing method, hardening layer manufacturing method, and semiconductor package manufacturing method

Abstract

To provide a transfer film, a transfer film manufacturing method, a hardening layer manufacturing method, and a semiconductor package manufacturing method capable of forming a hardening layer with a small linear expansion coefficient in-plane direction, on the transferred material.SOLUTION: A transfer film of the present invention includes a temporary support body in which the laminate including a temporary support precursor and a curable composition layer precursor including a resin is stretched by uniaxial drawing or biaxial drawing, and includes a curable composition layer.SELECTED DRAWING: None

Description

[Technical Field]

[0001] The present invention relates to a transfer film, a method for manufacturing a transfer film, a method for manufacturing a cured layer, and a method for manufacturing a semiconductor package. [Background technology]

[0002] In display devices such as organic electroluminescence (EL) display devices and liquid crystal display devices, a method of providing a cover window on a panel to protect the panel is known. For example, Patent Document 1 discloses a method for manufacturing a cover window including a glass substrate and a resin layer, in which a dry film including a base material and a resin layer is bonded to the glass substrate so that the resin layer is in contact with the glass substrate, and then the base material of the dry film is peeled off and the resin layer is heated. Here, the dry film having a transferable resin layer as described in Patent Document 1 may also be used in the manufacture of an insulating film for insulating and protecting wiring in a semiconductor package. [Prior art documents] [Patent documents]

[0003] [Patent Document 1] Japanese Patent Publication No. 2022-053257 Summary of the Invention [Problem to be solved by the invention]

[0004] An example of a method for manufacturing a semiconductor package is a method in which the resin layer of a transfer film having a temporary support and a resin layer is brought into contact with an object to be transferred, the resin layer is laminated to the object to be transferred, the temporary support is peeled off, the resin layer placed on the object to be transferred is cured in a pattern to obtain a cured layer, and then a circuit pattern is formed on the obtained cured layer. The present inventors attempted to manufacture a semiconductor package using a dry film as described in Patent Document 1 and found that the in-plane linear expansion coefficient of the cured layer formed on the transfer target may be large. If the in-plane linear expansion coefficient of the cured layer is large, cracks may occur in the cured layer, which may result in a decrease in the performance of the semiconductor package.

[0005] Therefore, an object of the present invention is to provide a transfer film that can form a cured layer with a small linear expansion coefficient in the in-plane direction on a transfer target. Another object of the present invention is to provide a method for manufacturing a transfer film, a method for manufacturing a cured layer, and a method for manufacturing a semiconductor package. [Means for solving the problem]

[0006] As a result of extensive research into solving the above problems, the present inventors have found that the above problems can be solved by the following configuration, and have completed the present invention.

[0007] [1] A transfer film comprising a temporary support and a curable composition layer, which is obtained by uniaxially or biaxially stretching a laminate comprising a temporary support precursor and a curable composition layer precursor containing a resin. [2] the laminate has the temporary support precursor, the curable composition layer precursor, and the cover film precursor in this order, The transfer film according to [1], which has the temporary support, the curable composition layer, and a cover film in this order. [3] A transfer film comprising a temporary support and a curable composition layer containing a resin, The transfer film, wherein the resin contained in the curable composition layer is oriented in an in-plane direction. [4] the temporary support comprises a resin, The transfer film according to [3], wherein the resin contained in the temporary support is oriented in an in-plane direction. [5] The transfer film according to [3] or [4], wherein the resin contained in the curable composition layer includes at least one selected from the group consisting of an epoxy resin, a polyimide precursor, a polyimide resin, a polyamide resin, a maleimide resin, a polyphenylene ether resin, and a silicone resin. [6] The transfer film according to any one of [3] to [5], which has the temporary support, the curable composition layer, and a cover film in this order. [7] A method for producing a transfer film, comprising uniaxially or biaxially stretching a laminate including a temporary support precursor and a curable composition layer precursor containing a resin, to obtain a transfer film including the temporary support and the curable composition layer. [8] the laminate has the temporary support precursor, the curable composition layer precursor, and the cover film precursor in this order, The method for producing a transfer film according to [7], wherein the transfer film has the temporary support, the curable composition layer, and the cover film in this order. [9] a step of transferring the curable composition layer in the transfer film according to any one of [1] to [6] onto a transfer target; and curing the curable composition layer transferred onto the transfer-receiving object to form a cured layer.

[10] The method for producing a cured layer according to [9], wherein the step of forming the cured layer is a step of subjecting the curable composition layer to patterned exposure and then performing a development treatment to obtain a patterned cured layer.

[11] The method for producing a cured layer according to

[10] , wherein the patterned cured layer is obtained by performing a heat treatment after the development treatment.

[12] The method for producing a cured layer according to [9], comprising a step of performing laser processing on the cured layer to obtain a patterned cured layer.

[13] A method for manufacturing a semiconductor package, comprising the method for manufacturing a cured layer according to any one of [9] to

[12] . [Effects of the Invention]

[0008] According to the present invention, it is possible to provide a transfer film that can form a cured layer having a small linear expansion coefficient in the in-plane direction on an object to be transferred. The present invention also provides a method for producing a transfer film, a method for producing a cured layer, and a method for producing a semiconductor package. DETAILED DESCRIPTION OF THE INVENTION

[0009] The present invention will be described in detail below. The following description of the components may be based on a representative embodiment of the present invention, but the present invention is not limited to such an embodiment.

[0010] In this specification, a numerical range expressed using "to" means a range that includes the numerical values ​​before and after "to" as the lower and upper limits. In addition, in this specification, when two or more types of a certain component are present, the "content" of that component means the total content of those two or more components. In the present specification, in the numerical ranges described in stages, the upper or lower limit value described in a certain numerical range may be replaced with the upper or lower limit value of another numerical range described in stages. Furthermore, in the numerical ranges described in the present specification, the upper or lower limit value described in a certain numerical range may be replaced with a value shown in the examples. As used herein, a combination of two or more preferred embodiments is a more preferred embodiment.

[0011] The term "step" in this specification includes not only an independent step, but also a step that cannot be clearly distinguished from other steps, as long as the intended purpose of the step is achieved.

[0012] In this specification, unless otherwise specified, the temperature condition may be 25° C. For example, the temperature when performing each of the above steps may be 25° C. unless otherwise specified.

[0013] In this specification, the term "transparent" means that the average transmittance of visible light with a wavelength of 400 to 700 nm is 80% or more, and preferably 90% or more. The average transmittance of visible light is a value measured using a spectrophotometer, and can be measured using, for example, a spectrophotometer U-3310 manufactured by Hitachi, Ltd.

[0014] In this specification, unless otherwise specified, "exposure" includes not only exposure using far ultraviolet light, extreme ultraviolet light, X-rays, EUV light, etc., as typified by mercury lamps and excimer lasers, but also exposure using particle beams such as electron beams and ion beams.

[0015] In this specification, the "solid content" of a composition refers to the components that form a film formed using the composition. Typically, when the composition contains a solvent (e.g., an organic solvent and water), it refers to all components excluding the solvent. Furthermore, liquid components that form a film are also considered to be solid content.

[0016] In this specification, unless otherwise specified, the content ratio of each repeating unit in a resin is a molar ratio. In this specification, unless otherwise specified, when a molecular weight distribution exists, the molecular weight is the weight average molecular weight (Mw). In this specification, the weight average molecular weight (Mw) and number average molecular weight (Mn) are values ​​determined by gel permeation chromatography (GPC) in terms of polystyrene.

[0017] In this specification, "(meth)acrylic acid" is a concept that encompasses both acrylic acid and methacrylic acid, "(meth)acryloyl group" is a concept that encompasses both acryloyl group and methacryloyl group, "(meth)acrylate" is a concept that encompasses both acrylate and methacrylate, and "(meth)acrylamide group" is a concept that encompasses both acrylamide group and methacrylamide group.

[0018] In this specification, the bonding direction of a divalent group (e.g., -CO-O-) is not limited unless otherwise specified. For example, when Y is -CO-O- in a compound represented by the formula "XYZ," the compound may be "XO-CO-Z" or "X-CO-OZ." Unless otherwise specified, the compounds described herein may include isomers (compounds with the same number of atoms but different structures), optical isomers, and isotopes. Furthermore, only one type of isomer or isotope may be included, or multiple types may be included.

[0019] Unless otherwise specified, the layer thickness (film thickness) in this specification is the average thickness measured using a scanning electron microscope (SEM) for thicknesses of 0.5 μm or more, and the average thickness measured using a transmission electron microscope (TEM) for thicknesses of less than 0.5 μm. The average thickness is obtained by cutting a sample to be measured using an ultramicrotome, measuring the thickness at any five points, and calculating the arithmetic average of the thicknesses.

[0020] In this specification, unless otherwise specified, the boiling point means the boiling point under normal pressure (1 atmosphere, 760 mmHg). In this specification, unless otherwise specified, the refractive index is a value measured by an ellipsometer at a wavelength of 550 nm.

[0021] In this specification, the term "longitudinal direction" means the longitudinal direction of the film during production of the transfer film, and is synonymous with the terms "conveyance direction" and "machine direction." In this specification, the term "width direction" means a direction perpendicular to the longitudinal direction. In this specification, "orthogonal" is not limited to being strictly orthogonal, but also includes being approximately orthogonal. "Approximately orthogonal" means that the angles intersect within a range of 90°±5°, preferably within a range of 90°±3°, and more preferably within a range of 90°±1°.

[0022] [Transfer film] Hereinafter, the transfer film of the present invention will be described in detail for each embodiment.

[0023] [First embodiment] The transfer film in the first embodiment (hereinafter also referred to as the "first transfer film") comprises a temporary support and a curable composition layer, which are formed by uniaxially or biaxially stretching a laminate comprising a temporary support precursor and a curable composition layer precursor containing a resin. It is presumed that the resin contained in the curable composition layer precursor is oriented in the in-plane direction of the curable composition layer by uniaxially or biaxially stretching the laminate, and as a result, when a cured layer is formed on a transfer target using the first transfer film, the linear expansion coefficient of the resulting cured layer in the in-plane direction is reduced.

[0024] <Laminate> The laminate used for uniaxial stretching or biaxial stretching includes a temporary support precursor and a curable composition layer precursor containing a resin. The laminate may further include a cover film precursor. In this case, it is preferable that the temporary support precursor, the curable composition layer precursor, and the cover film precursor are laminated in this order. The laminate is preferably in the form of a film.

[0025] (Temporary support precursor) The temporary support precursor is a member that supports the curable composition layer precursor and becomes the temporary support described below by uniaxial or biaxial stretching. The temporary support precursor may be a uniaxially or biaxially stretched member. In the present invention, even if the temporary support precursor is a member that has already been uniaxially or biaxially stretched, the member corresponding to the temporary support precursor contained in the first transfer film obtained by uniaxially or biaxially stretching the temporary support precursor in the state of a laminate is referred to as the temporary support.

[0026] The temporary support precursor may have either a single-layer structure or a multi-layer structure, and is preferably a film. The temporary support precursor preferably contains a resin, specific examples of which include polyethylene terephthalate (PET), polymethyl methacrylate, cellulose triacetate, polystyrene, polyimide, and polycarbonate, with polyethylene terephthalate being preferred.

[0027] The thickness of the temporary support precursor is preferably 5 to 200 μm, and from the viewpoint of ease of handling and versatility, more preferably 5 to 150 μm, still more preferably 5 to 50 μm, and particularly preferably 5 to 35 μm. The thickness of the temporary support precursor is determined as the arithmetic mean value of any five points measured by cross-sectional observation using an SEM (scanning electron microscope).

[0028] In order to improve the adhesion between the temporary support precursor and the curable composition layer precursor, the surface of the temporary support precursor that comes into contact with the curable composition layer precursor may be surface-modified by UV irradiation, corona discharge, plasma, or the like. When the surface is modified by UV irradiation, the exposure dose of UV irradiation is 10 to 2000 mJ / cm 2 is preferred, and 50 to 1000 mJ / cm 2 is more preferred. Examples of light sources for UV irradiation include low-pressure mercury lamps, high-pressure mercury lamps, ultra-high-pressure mercury lamps, carbon arc lamps, metal halide lamps, xenon lamps, chemical lamps, electrodeless discharge lamps, and light-emitting diodes that emit light in the wavelength range of 150 to 450 nm. The lamp output and illuminance can be adjusted as appropriate.

[0029] Examples of the temporary support precursor include a biaxially oriented polyethylene terephthalate film having a thickness of 16 μm, a biaxially oriented polyethylene terephthalate film having a thickness of 12 μm, and a biaxially oriented polyethylene terephthalate film having a thickness of 9 μm. The temporary support precursor may be a recycled product. Examples of recycled products include those obtained by cleaning and chipping used films and then forming the resulting materials into films. Examples of commercially available recycled products include the Ecouse series (manufactured by Toray Industries, Inc.).

[0030] Examples of the temporary support precursor include the members described in paragraphs 0017 to 0018 of JP 2014-085643 A, paragraphs 0019 to 0026 of JP 2016-027363 A, paragraphs 0041 to 0057 of WO 2012 / 081680 A, and paragraphs 0029 to 0040 of WO 2018 / 179370 A, the contents of which are incorporated herein by reference.

[0031] The temporary support precursor may have a layer containing fine particles (lubricant layer) on one or both sides of the temporary support precursor for the purpose of imparting ease of handling. The diameter of the fine particles contained in the lubricant layer is preferably 0.05 to 0.8 μm. The thickness of the lubricant layer is preferably 0.05 to 1.0 μm. Commercially available temporary support precursors include, for example, Lumirror 16FB40, Lumirror 16KS40, Lumirror #38-U48, Lumirror #75-U34, and Lumirror #25T60 (all manufactured by Toray Industries, Inc.); and Cosmoshine A4100, Cosmoshine A4160, Cosmoshine A4300, Cosmoshine A4360, and Cosmoshine A8300 (all manufactured by Toyobo Co., Ltd.).

[0032] (Curable composition layer precursor) The curable composition layer precursor is a member that contains a resin and becomes a curable composition layer described below by uniaxial or biaxial stretching. The curable composition layer precursor is preferably a layer formed using the curable composition described below. The various components that can be contained in the curable composition layer precursor are the same as the various components that can be contained in the curable composition described below, and preferred embodiments are also the same. However, the preferred ranges of the contents of the various components in the curable composition layer precursor are the same as the preferred ranges obtained by replacing "the content (% by mass) of the various components relative to the total solid content of the curable composition" described below with "the content (% by mass) of the various components relative to the total mass of the curable composition layer precursor." Specifically, the statement "The resin content is preferably 1.0 to 99.0% by mass relative to the total solid content of the curable composition" should be replaced with "The resin content is preferably 1.0 to 99.0% by mass relative to the total mass of the curable composition layer precursor."

[0033] The average thickness of the curable composition layer precursor is preferably 0.5 μm or more, more preferably 1.0 μm or more, even more preferably 3.0 μm or more, and particularly preferably 5.0 μm or more, from the viewpoint of superior insulation reliability. The average thickness of the curable composition layer precursor is preferably 100 μm or less, more preferably 50 μm or less, even more preferably 30 μm or less, and particularly preferably 20 μm or less, from the viewpoint of superior pattern resolution.

[0034] (Cover film precursor) The cover film precursor is a member that will become the cover film described below by uniaxially or biaxially stretching the laminate.

[0035] Examples of cover film precursors include polyethylene terephthalate films, polypropylene films, polystyrene films, and polycarbonate films. Examples of the cover film precursor include the cover films described in paragraphs 0083 to 0087 and 0093 of JP-A No. 2006-259138.

[0036] Examples of cover film precursors include Alphan (registered trademark) FG-201 (manufactured by Oji F-Tex Co., Ltd.), Alphan (registered trademark) E-201F (manufactured by Oji F-Tex Co., Ltd.), Therapeel (registered trademark) 25WZ (manufactured by Toray Advanced Film Co., Ltd.), and Lumirror (registered trademark) 16QS62 (16KS40) (manufactured by Toray Industries, Inc.). The cover film precursor may be a recycled product. Examples of recycled products include those obtained by cleaning and chipping used films, and then forming the resulting material into a film. Examples of commercially available recycled products include the Ecouse series (manufactured by Toray Industries, Inc.).

[0037] The number of fish eyes with a diameter of 80 μm or more contained in the cover film precursor is 5 / m 2 The following are preferred: Fisheyes are foreign matter, unmelted matter, and / or oxidized and deteriorated matter of the material that is introduced into the film when the material is thermally melted and then kneaded, extruded, and / or biaxially stretched, cast, or other methods are used to produce the film.

[0038] The number of particles with a diameter of 3 μm or more contained in the cover film precursor is 30 / mm 2 Preferably less than 10 pieces / mm 2 Less than 5 pieces / mm is more preferable. 2 The following is more preferable: This can suppress defects caused by the transfer of irregularities due to particles contained in the cover film precursor to the curable composition layer precursor.

[0039] The arithmetic mean roughness Ra of the surface of the cover film precursor is preferably 0.01 μm or more, more preferably 0.02 μm or more, and even more preferably 0.03 μm or more. If Ra is within this range, for example, when the first transfer film obtained using the laminate is long, the first transfer film can be easily wound up. Furthermore, from the viewpoint of suppressing defects during transfer, Ra is preferably less than 0.50 μm, more preferably 0.40 μm or less, and even more preferably 0.30 μm or less.

[0040] The average thickness of the cover film precursor is preferably 5 μm or more, more preferably 8 μm or more, and even more preferably 10 μm or more, from the viewpoint of better protection performance of the curable composition layer contained in the first transfer film, and is preferably 50 μm or less, more preferably 30 μm or less, and even more preferably 20 μm or less, from the viewpoint of better handleability of the laminate.

[0041] (Intermediate layer precursor and thermoplastic resin layer precursor) The laminate may further include an intermediate layer precursor and / or a thermoplastic resin layer precursor, which are components that become the intermediate layer and thermoplastic resin layer described below by uniaxially or biaxially stretching the laminate. When the laminate has an intermediate layer precursor and / or a thermoplastic resin layer precursor, it is preferable that the laminate has the intermediate layer precursor and / or the thermoplastic resin layer precursor between the temporary support precursor and the curable composition layer precursor. Examples of the intermediate layer precursor and the thermoplastic resin layer precursor include the intermediate layer and the thermoplastic resin layer described in paragraphs 0164 to 0204 of WO 2021 / 166719, the contents of which are incorporated herein by reference.

[0042] (High refractive index layer precursor) The laminate may further include a high refractive index layer precursor, which is a member that becomes the high refractive index layer precursor described below by uniaxially or biaxially stretching the laminate. Examples of high refractive index layers include those described in paragraphs 0168 to 0188 of WO 2021 / 187549, the contents of which are incorporated herein by reference.

[0043] (Method of manufacturing laminate) The laminate can be produced by a known production method. One preferred embodiment of the method for producing a laminate is a method of forming a curable composition layer precursor by applying a curable composition (described later) onto a temporary support precursor. Specifically, a method including the steps of applying a curable composition to the surface of the temporary support precursor to form a coating film and drying the coating film to form a curable composition layer precursor is preferred. Examples of methods for applying the curable composition include slit coating, spin coating, curtain coating, and inkjet coating.

[0044] The method for producing a laminate preferably further includes a step of pressing a cover film onto the obtained curable composition layer precursor.

[0045] When the laminate has an intermediate layer precursor and / or a thermoplastic resin layer precursor, the compositions used for producing the intermediate layer precursor and the thermoplastic resin layer precursor and the method for producing them can be, for example, those described in paragraphs 0133 to 0136 and 0143 to 0144 of International Publication No. 2021 / 033451, the contents of which are incorporated herein by reference.

[0046] When the laminate has a high refractive index layer precursor, the composition used to produce the high refractive index layer precursor and the method for producing the same can be the same as those described in WO 2021 / 187549 regarding the high refractive index layer, and these contents are incorporated herein.

[0047] The obtained laminate may be wound up and stored in a roll form. When the laminate is in a roll form and the first transfer film obtained using the laminate is in a roll form, it can be provided in that form as it is for the lamination step with the transfer target in a roll-to-roll system.

[0048] <First transfer film> The first transfer film includes a temporary support and a curable composition layer. The first transfer film may further have a cover film, and in this case, it is preferable that the temporary support, the curable composition layer, and the cover film are laminated in this order.

[0049] (Temporary support) The temporary support is a member contained in a first transfer film obtained by stretching a laminate including a temporary support precursor, that is, a member obtained by stretching the temporary support precursor. The various components contained in the temporary support are the same as the various components contained in the temporary support precursor, and the preferred embodiments are also the same. The average thickness of the temporary support is preferably the same as that of the temporary support precursor. When the temporary support contains a resin, the resin contained in the temporary support is preferably oriented in the in-plane direction of the temporary support by stretching. The orientation state of the resin contained in the temporary support can be confirmed by the same method as the orientation state of the resin contained in the curable composition layer, except that the measurement target is the resin contained in the temporary support.

[0050] (Curable composition layer) The curable composition layer is a layer contained in a first transfer film obtained by stretching a laminate containing a curable composition layer precursor, i.e., a layer obtained by stretching the curable composition layer precursor. The various components contained in the curable composition layer are the same as the various components contained in the curable composition layer precursor, and preferred embodiments are also the same. In addition, the average thickness of the curable composition layer is preferably the same as that of the curable composition layer precursor.

[0051] The resin contained in the curable composition layer is preferably oriented in the in-plane direction of the curable composition layer by stretching (specifically, in the direction intersecting the thickness direction of the curable composition layer in the cross section obtained when the first transfer film is cut along the thickness direction). The orientation state of the resin can be confirmed by the method described in the Examples section below. When the first transfer film is a film obtained by uniaxially stretching a laminate, the resin contained in the curable composition layer preferably has molecular orientation in a uniaxial direction in the plane. When the first transfer film is a film obtained by biaxially stretching a laminate, it is preferable that the resin contained in the curable composition layer is oriented in a direction intersecting the thickness direction of the curable composition layer (i.e., in-plane direction of the curable composition layer) in the cross section obtained when the first transfer film is cut along the thickness direction.In this case, the resin may be oriented in a specific direction or randomly in the plane of the curable composition layer.

[0052] (cover film) The cover film may be a member included in a first transfer film obtained by stretching a laminate including a cover film precursor, that is, a film obtained by stretching the cover film precursor. When the cover film included in the first transfer film is a film obtained by stretching a cover film precursor, the various components contained in the cover film are the same as the various components contained in the cover film precursor, and the preferred embodiments are also the same. In addition, the number of particles with a diameter of 3 μm or more contained in the cover film, the arithmetic mean roughness Ra of the surface of the cover film, and the average thickness of the cover film are preferably the same as those of the cover film precursor. When the cover film contains a resin, the resin contained in the cover film may be oriented in the in-plane direction of the cover film.

[0053] On the other hand, the first transfer film including the cover film may be obtained by stretching a laminate not including a cover film precursor, and then disposing the cover film on the stretched laminate. When a cover film is disposed on the stretched laminate, specific examples and preferred embodiments of the cover film to be used are the same as those of the cover film precursor described above. That is, when a cover film is disposed on the stretched laminate, the cover film precursor described above can be used as the cover film.

[0054] (Intermediate layer and thermoplastic resin layer) The first transfer film may further have an intermediate layer and / or a thermoplastic resin layer. The intermediate layer and / or the thermoplastic resin layer is a layer contained in the first transfer film obtained by stretching a laminate including the intermediate layer precursor and / or the thermoplastic resin layer precursor, i.e., a layer obtained by stretching the intermediate layer precursor and / or the thermoplastic resin layer precursor. When the first transfer film has an intermediate layer and / or a thermoplastic resin layer, the first transfer film preferably has the intermediate layer and / or the thermoplastic resin layer between the temporary support and the curable composition layer.

[0055] The various components contained in the intermediate layer and the thermoplastic resin layer are the same as the various components contained in the intermediate layer precursor and the thermoplastic resin layer precursor, and the preferred embodiments are also the same. When the intermediate layer contains a resin, the resin contained in the intermediate layer may be oriented in the in-plane direction of the intermediate layer. The orientation state of the resin contained in the intermediate layer can be confirmed by the same method as the orientation state of the resin contained in the curable composition layer, except that the measurement target is the resin contained in the intermediate layer. When the thermoplastic resin layer contains a resin, the resin contained in the thermoplastic resin layer may be oriented in the in-plane direction of the thermoplastic resin layer. The orientation state of the resin contained in the thermoplastic resin layer can be confirmed by the same method as the orientation state of the resin contained in the curable composition layer, except that the measurement target is the resin contained in the thermoplastic resin layer.

[0056] (high refractive index layer) The first transfer film may further include a high refractive index layer. The high refractive index layer is a layer included in the first transfer film obtained by stretching a laminate including a high refractive index layer precursor, i.e., a layer obtained by stretching the high refractive index layer precursor. The various components contained in the high refractive index layer are the same as the various components contained in the high refractive index layer precursor, and the preferred embodiments are also the same. When the high refractive index layer contains a resin, the resin contained in the high refractive index layer may be oriented in the in-plane direction of the high refractive index layer. The orientation state of the resin contained in the high refractive index layer can be confirmed by the same method as the orientation state of the resin contained in the curable composition layer, except that the measurement target is the resin contained in the high refractive index layer.

[0057] (Application) The first transfer film can be used in the manufacture of protective or insulating films for touch panel electrodes, protective or insulating films for printed wiring boards, protective or insulating films for TFT substrates, interlayer insulating films in build-up substrates for semiconductor packages, organic interposers, color filters, overcoat films for color filters, and etching resists for wiring formation. In particular, the first transfer film can be suitably used for forming an insulating film, and the insulating film is preferably used as an insulating film for a semiconductor package. That is, the first transfer film is preferably used for forming an insulating film for a semiconductor package.

[0058] <Method for manufacturing first transfer film> An example of a method for producing the first transfer film is a method in which the above-mentioned laminate is uniaxially or biaxially stretched to obtain the above-mentioned first transfer film. An example of a method for uniaxially stretching the laminate is a mode in which only one of a longitudinal stretching step and a transverse stretching step, which will be described later, is performed on the laminate. An example of a method for biaxially stretching a laminate is to subject the laminate to both a longitudinal stretching step and a transverse stretching step, which will be described later. The order of the steps when biaxially stretching is performed will be described later. In the method for producing the first transfer film, biaxial stretching is preferably performed in order to obtain better effects of the present invention. That is, the first transfer film is preferably a film obtained by biaxially stretching the above-mentioned laminate.

[0059] (longitudinal stretching process) The longitudinal stretching step is a step of longitudinally stretching the laminate in the machine direction. The longitudinal stretching step can be carried out using, for example, a known longitudinal stretching device equipped with nip rolls. One example of a method for longitudinal stretching is to use two or more pairs of nip rolls arranged in the transport direction while conveying a film-like laminate through a pair of nip rolls in the longitudinal direction. For example, if a pair of nip rolls A is provided on the upstream side of the laminate transport direction and a pair of nip rolls B is provided on the downstream side, the laminate is stretched in the transport direction (MD; Machine Direction) by making the rotation speed of the downstream nip roll B faster than the rotation speed of the upstream nip roll A during transport. Two or more pairs of nip rolls may be provided on the upstream side, and two or more pairs of nip rolls may be provided on the downstream side.

[0060] In the longitudinal stretching step, the area stretching ratio (product of each stretching ratio) of the laminate is preferably 1.2 times or more, more preferably 1.5 times or more, of the area of ​​the laminate before stretching, from the viewpoint of facilitating orientation of the resin contained in the curable composition layer precursor in the in-plane direction of the curable composition layer, and the upper limit is preferably 20 times or less, more preferably 15 times or less, from the viewpoint of preventing breakage of the laminate. The temperature during longitudinal stretching of the laminate (hereinafter also referred to as "longitudinal stretching temperature") is preferably 5 to 80°C, more preferably 10 to 60°C, and even more preferably 15 to 40°C, since the resin contained in the curable composition layer precursor is easily oriented in the in-plane direction of the curable composition layer.

[0061] When stretching is performed using rolls such as nip rolls, the laminate in contact with the rolls can be heated by providing a heater or a pipe through which a warm solvent can flow inside the roll. Even when rolls are not used, the laminate can be heated by blowing hot air onto the laminate, bringing it into contact with a heat source such as a heater, or passing it near a heat source.

[0062] (lateral stretching process) The transverse stretching step is a step of transversely stretching the laminate in the width direction perpendicular to the longitudinal direction. An example of a transverse stretching process is a method that includes a stretching section that applies tension to the laminate in at least the width direction perpendicular to the longitudinal direction to stretch it transversely, a heat relaxation section that heats the laminate to release the tension, and a cooling section that cools the laminate after heat relaxation.

[0063] In the transverse stretching step, the area stretching ratio (product of each stretching ratio) of the laminate is preferably 1.2 times or more, more preferably 1.5 times or more, of the area of ​​the laminate before stretching, from the viewpoint of facilitating orientation of the resin contained in the curable composition layer precursor in the in-plane direction of the curable composition layer. The upper limit is preferably 20 times or less, more preferably 15 times or less, from the viewpoint of preventing breakage of the laminate. The temperature during transverse stretching of the laminate (hereinafter also referred to as "transverse stretching temperature") is preferably 5 to 80°C, more preferably 10 to 60°C, and even more preferably 15 to 40°C, since the resin contained in the curable composition layer precursor is easily oriented in the in-plane direction of the curable composition layer.

[0064] The transverse stretching step may be carried out by any means as long as the laminate is at least transversely stretched, but is preferably carried out using a known transverse stretching device or biaxial stretching machine. In the transverse stretching step, it is preferable to further cool the laminate that has passed through the heat-relaxing section.

[0065] When biaxial stretching is performed in the method for producing the first transfer film, both the longitudinal stretching step and the transverse stretching step are carried out. In this case, for example, in addition to a longitudinal stretching step in which the laminate is stretched in the longitudinal direction (MD) of the laminate, a transverse stretching step in which the laminate is stretched in the width direction (TD; transverse direction) perpendicular to the longitudinal direction is carried out. This results in a biaxially stretched first transfer film. When performing biaxial stretching, it is sufficient to perform stretching in MD and TD at least once each.

[0066] The biaxial stretching method may be either a sequential biaxial stretching method in which longitudinal stretching and transverse stretching are carried out separately, or a simultaneous biaxial stretching method in which longitudinal stretching and transverse stretching are carried out simultaneously. The longitudinal stretching and transverse stretching may each be carried out two or more times, and the order of the longitudinal stretching and transverse stretching is not important. Among these, a mode in which the longitudinal stretching and transverse stretching are carried out in this order is preferred.

[0067] When biaxial stretching is performed, the area stretching ratio (product of each stretching ratio) of the laminate is preferably 1.2 times or more, more preferably 1.5 times or more, of the area of ​​the laminate before stretching, from the viewpoint of facilitating orientation of the resin contained in the curable composition layer precursor in the in-plane direction of the curable composition layer. The upper limit is preferably 20 times or less, more preferably 15 times or less, from the viewpoint of preventing breakage of the laminate.

[0068] <Curable composition> The curable composition layer precursor can be formed using, for example, a curable composition. The curable composition is preferably a composition that is cured by the action of heat or light (such as ultraviolet light), and more preferably a composition that is cured by the action of light (such as ultraviolet light).

[0069] The various components that the curable composition may contain are described in detail below.

[0070] (resin) The curable composition preferably contains a resin. The resin preferably contains at least one selected from the group consisting of a polyimide precursor, a silicone resin, an epoxy resin, a polyimide resin, a polyamide resin, a maleimide resin, and a polyphenylene ether resin, in order to further improve the curability of the curable composition. Among these, the resin preferably contains at least one selected from the group consisting of an epoxy resin, a polyimide precursor, and a silicone resin, more preferably contains at least one selected from the group consisting of a polyimide precursor and a silicone resin, further preferably contains a polyimide precursor, and particularly preferably is a polyimide precursor, in terms of further improving the curability of the curable composition. The precursors of various resins are resins that can be converted into various resins by heat treatment, light treatment, or chemical treatment.

[0071] The resin may have a reactive group. Examples of the reactive group include a polymerizable group and a functional group other than a polymerizable group. Examples of the polymerizable group include known polymerizable groups such as a radical polymerizable group, an epoxy group, an oxetanyl group, a methylol group, and an alkoxymethyl group, and the radical polymerizable group is preferred. The radical polymerizable group is preferably a group having an ethylenically unsaturated double bond. Examples of the group having an ethylenically unsaturated double bond include a (meth)acryloyl group, a (meth)acrylamide group, a vinyl group, a styryl group, an allyl group, and a vinyl ether group, with a (meth)acryloyl group being preferred. Examples of functional groups other than polymerizable groups include amino groups, hydroxyl groups, and thiol groups, with amino groups being preferred, and secondary amino groups (e.g., phenylamino groups, methylamino groups, and ethylamino groups) or primary amino groups (-NH2) being more preferred.Functional groups other than silanol groups (Si-OH) are also preferred.

[0072] The resin may have an acid-decomposable group. Examples of the acid-decomposable group include the acid-decomposable groups described in paragraphs 0024 to 0031 of WO 2019 / 187881.

[0073] Polyimide resins and polyimide precursors The polyimide resin is a resin having an imide structure. The polyimide resin is preferably a resin having a cyclic imide structure. The polyimide may have a substituent. The polyimide resin is preferably a resin synthesized from a polyimide precursor having a repeating unit represented by formula (1) (e.g., a resin obtained by a ring-closing reaction). The polyimide precursor preferably has a repeating unit represented by formula (1).

[0074] [ka]

[0075] In formula (1), A 1 and A 2 R each independently represents an oxygen atom or -NH-. 111 represents a divalent organic group. 113 and R 114 R each independently represents a hydrogen atom or a monovalent organic group. 115 represents a tetravalent organic group.

[0076] In formula (1), A 1 and A 2 each independently represents an oxygen atom or —NH—. A 1 and A 2 is preferably an oxygen atom.

[0077] In formula (1), R 111 represents a divalent organic group. Examples of the divalent organic group include a divalent aliphatic group, a divalent aromatic ring group, and a combination thereof. The divalent organic group is preferably a divalent aliphatic group having 2 to 20 carbon atoms, a divalent aromatic ring group having 6 to 20 carbon atoms, or a combination thereof, and more preferably a divalent aromatic ring group having 6 to 20 carbon atoms. The aliphatic group may be linear, branched, or cyclic. The aromatic ring group may be monocyclic or polycyclic. The aliphatic group and the aromatic ring group may contain a heteroatom. The heteroatom may be contained in the divalent organic group as, for example, -O-, -CO-, -S-, -SO2-, or -NHCO-. R 111 As the diamine, a divalent organic group derived from a diamine is also preferred. As the diamine, a diamine used in the production of a polyimide precursor is preferred, and an aliphatic diamine or an aromatic diamine is more preferred. The diamine is preferably a diamine having a linear aliphatic group having 2 to 20 carbon atoms, a branched aliphatic group having 3 to 20 carbon atoms, a cyclic aliphatic group having 3 to 20 carbon atoms, an aromatic ring group having 6 to 20 carbon atoms, or a group that combines these, and more preferably a diamine having an aromatic ring group having 6 to 20 carbon atoms (aromatic diamine). Examples of the aromatic ring group include groups having the following structure:

[0078] [ka]

[0079] In AR-8 to AR-10, A represents a divalent aliphatic hydrocarbon group having 1 to 10 carbon atoms which may have a fluorine atom, -O-, -CO-, -S-, -SO2-, -NHCO- or a combination thereof, or a single bond. A is preferably an alkylene group having 1 to 3 carbon atoms which may have a fluorine atom, -O-, -CO-, -S- or -SO2-, more preferably -CH2-, -O-, -S-, -SO2-, -C(CF3)2- or -C(CH3)2-, and still more preferably -O-.

[0080] R 111 As for *-Ar 0 -L 0 -Ar 0 -* is also preferred. Ar 0 L each independently represents a divalent aromatic hydrocarbon group. 0 represents a divalent aliphatic hydrocarbon group having 1 to 10 carbon atoms which may have a fluorine atom, -O-, -CO-, -S-, -SO2-, -NHCO- or a group formed by combining these, or a single bond. * represents the bonding position. Ar 0 They may be the same or different from each other.

[0081] Ar 0 The number of carbon atoms in the divalent aromatic hydrocarbon group represented by the following formula is preferably 6 to 22, more preferably 6 to 18, and even more preferably 6 to 10. As the aromatic hydrocarbon group, a phenylene group is preferred. L 0 has the same meaning as A described above, and the preferred embodiments are also the same.

[0082] Examples of diamines include 1,2-diaminoethane, 1,2-diaminopropane, 1,3-diaminopropane, 1,4-diaminobutane, 1,6-diaminohexane; 1,2- or 1,3-diaminocyclopentane, 1,2-, 1,3-, or 1,4-diaminocyclohexane, 1,2-, 1,3-, or 1,4-bis(aminomethyl)cyclohexane, bis-(4-aminocyclohexyl)methane, bis-(3-aminocyclohexyl)methane, 4,4'-diamino-3,3'-dimethylcyclohexylmethane, or isophoronediamine; meta- or para- Phenylenediamine, diaminotoluene, 4,4'- or 3,3'-diaminobiphenyl, 4,4'-diaminodiphenyl ether, 3,3-diaminodiphenyl ether, 4,4'- or 3,3'-diaminodiphenylmethane, 4,4'- or 3,3'-diaminodiphenyl sulfone, 4,4'- or 3,3'-diaminodiphenyl sulfide, 4,4'- or 3,3'-diaminobenzophenone, 3,3'-dimethyl-4,4'-diaminobiphenyl, 2,2'-dimethyl-4,4'-diaminobiphenyl (4,4'-diamino-2,2'-dimethyl Biphenyl), 3,3'-dimethoxy-4,4'-diaminobiphenyl, 2,2-bis(4-aminophenyl)propane, 2,2-bis(4-aminophenyl)hexafluoropropane, 2,2-bis(3-hydroxy-4-aminophenyl)propane, 2,2-bis(3-hydroxy-4-aminophenyl)hexafluoropropane, 2,2-bis(3-amino-4-hydroxyphenyl)propane, 2,2-bis(3-amino-4-hydroxyphenyl)hexafluoropropane, bis(3-amino-4-hydroxyphenyl)sulfone, bis(4 -amino-3-hydroxyphenyl)sulfone, 4,4'-diaminoparaterphenyl, 4,4'-bis(4-aminophenoxy)biphenyl, bis[4-(4-aminophenoxy)phenyl]sulfone, bis[4-(3-aminophenoxy)phenyl]sulfone, bis[4-(2-aminophenoxy)phenyl]sulfone, 1,4-bis(4-aminophenoxy)benzene, 9,10-bis(4-aminophenyl)anthracene, 3,3'-dimethyl-4,4'-diaminodiphenylsulfone, 1,3-bis(4-aminophenoxy)benzene, 1,3-Bis(3-aminophenoxy)benzene, 1,3-bis(4-aminophenyl)benzene, 3,3'-diethyl-4,4'-diaminodiphenylmethane, 3,3'-dimethyl-4,4'-diaminodiphenylmethane, 4,4'-diaminooctafluorobiphenyl, 2,2-bis[4-(4-aminophenoxy)phenyl]propane, 2,2-bis[4-(4-aminophenoxy)phenyl]hexafluoropropane, 9,9-bis(4-aminophenyl)-10-hydroanthracene, 3,3',4,4'-tetraafluorobenzoate 4,4'-dimethyl-3,3'-diaminodiphenyl sulfone, 3,3',5,5'-tetramethyl-4,4'-diaminodiphenylmethane, 2-(3',5'-diaminobenzoyloxy)ethyl methacrylate, 2,4- or 2,5-diaminocumene, 2,5- Dimethyl-paraphenylenediamine, acetoguanamine, 2,3,5,6-tetramethyl-paraphenylenediamine, 2,4,6-trimethyl-metaphenylenediamine, bis(3-aminopropyl)tetramethyldisiloxane, 2,7-diaminofluorene, 2,5-diaminopyridine, 1,2-bis(4-aminophenyl)ethane, diaminobenzanilide, esters of diaminobenzoic acid, 1,5-diaminonaphthalene, diaminobenzotrifluoride, 1,3-bis(4-aminophenyl)hexafluoropropane , 1,4-bis(4-aminophenyl)octafluorobutane, 1,5-bis(4-aminophenyl)decafluoropentane, 1,7-bis(4-aminophenyl)tetradecafluoroheptane, 2,2-bis[4-(3-aminophenoxy)phenyl]hexafluoropropane, 2,2-bis[4-(2-aminophenoxy)phenyl]hexafluoropropane, 2,2-bis[4-(4-aminophenoxy)-3,5-dimethylphenyl]hexafluoropropane, 2,2-bis[4-(4-aminophenoxy)-3,4,4'-bis(3-amino-5-trifluoromethylphenoxy)diphenyl sulfone, 2,2-bis[4-(4-amino-3-trifluoromethylphenoxy)phenyl]hexafluoropropane, 3,3',5,5'-tetramethyl-4,4'-diaminobiphenyl, 4,4'-diamino-2,2'-bis(trifluoromethyl)biphenyl, 2,2',5,5',6,6'-hexafluorotolidine, and 4,4'-diaminoquaterphenyl. , Further, examples of diamines include compounds represented by any one of formulas (DA-1) to (DA-18).

[0083] [ka]

[0084] [ka]

[0085] The diamine may also be one having two or more alkylene glycol units in the main chain, and the diamine having two or more alkylene glycol units in the main chain is preferably one having two or more ethylene glycol chains and / or propylene glycol chains in one molecule. Also preferred is a diamine that does not contain an aromatic ring. Examples of the diamine include the Jeffamine (registered trademark) series (KH-511, ED-600, ED-900, ED-2003, EDR-148, EDR-176, D-200, D-400, D-2000, and D-4000, manufactured by HUNTSMAN), 1-(2-(2-(2-aminopropoxy)ethoxy)propoxy)propan-2-amine, and 1-(1-(1-(2-aminopropoxy)propan-2-yl)oxy)propan-2-amine.

[0086] In formula (1), R 113 and R 114 each independently represents a hydrogen atom or a monovalent organic group. R 113 and R 114 Preferably, at least one of R represents a group having a reactive group, 113 and R 114 It is more preferable that both of the following groups represent a group having a reactive group. Examples of the reactive group include the groups exemplified above as the reactive group that the resin may have. The monovalent organic group may be a monovalent organic group X, which will be described later. R 113 and R 114 Examples of the reactive group include the reactive groups described above, and a group having an ethylenically unsaturated double bond is preferred, and a vinyl group, an allyl group, a (meth)acryloyl group, or a group represented by formula (III) is more preferred.

[0087] [ka]

[0088] In formula (III), R 200 represents a hydrogen atom or a methyl group. 201 represents an alkylene group having 2 to 12 carbon atoms, -CH2CH(OH)CH2-, or a (poly)oxyalkylene group having 4 to 30 carbon atoms. * represents the bonding position.

[0089] In formula (III), R 200 represents a hydrogen atom or a methyl group. R 200 As the alkyl group, a methyl group is preferred.

[0090] In formula (III), R 201 represents an alkylene group having 2 to 12 carbon atoms, -CH2CH(OH)CH2-, or a (poly)oxyalkylene group having 4 to 30 carbon atoms. The number of carbon atoms in the alkylene group constituting the (poly)oxyalkylene group is preferably 1 to 12, more preferably 1 to 6, and even more preferably 1 to 3. The number of repetitions of oxyalkylene in the (poly)oxyalkylene group is preferably 1 to 12, more preferably 1 to 6, and even more preferably 1 to 3. The (poly)oxyalkylene group is a concept that encompasses both an oxyalkylene group and a polyoxyalkylene group. R 201 Examples of the alkyl group include an ethylene group, a propylene group, a trimethylene group, a tetramethylene group, a 1,2-butanediyl group, a 1,3-butanediyl group, a pentamethylene group, a hexamethylene group, an octamethylene group, a dodecamethylene group, and -CHCH(OH)CH-. An ethylene group, a propylene group, a trimethylene group, or -CHCH(OH)CH- is preferred, and an ethylene group is more preferred.

[0091] R 113 or R 114 Examples of the monovalent organic group represented by the formula (I) include an aliphatic group, an aromatic ring group, and an arylalkyl group having 1 to 3 acid groups. Examples include an aromatic ring group having 6 to 20 carbon atoms and having an acid group, and an arylalkyl group having 7 to 25 carbon atoms and having an acid group. More specifically, examples include a phenyl group having an acid group and a benzyl group having an acid group. The acid group is preferably a hydroxyl group or a carboxy group. R 113 and R 114 Also preferred as is a hydrogen atom, a 2-hydroxybenzyl group, a 3-hydroxybenzyl group, or a 4-hydroxybenzyl group. R 113 or R 114The monovalent organic group represented by the formula (I) also includes a leaving group that is eliminated by the action of an acid.

[0092] In formula (1), R 115 represents a tetravalent organic group. The tetravalent organic group is preferably a tetravalent organic group having an aromatic ring, and more preferably a group represented by formula (5) or (6).

[0093] [ka]

[0094] In formula (5), R 112 represents a divalent aliphatic hydrocarbon group having 1 to 10 carbon atoms which may have a fluorine atom, -O-, -CO-, -S-, -SO2-, -NHCO- or a group formed by combining these, or a single bond. * represents the bonding position. In formula (6), * represents a bonding position.

[0095] In formula (5), R 112 has the same meaning as A described above, and the preferred embodiments are also the same.

[0096] The tetravalent organic group may be, for example, a tetracarboxylic acid residue remaining after removing the acid dianhydride group from a tetracarboxylic acid dianhydride. The tetracarboxylic acid dianhydride is preferably a compound represented by formula (7).

[0097] [ka]

[0098] In formula (7), R 115 represents a tetravalent organic group. R in equation (7) 115 is R in Eq. (1). 115 The same definition and preferred embodiments are also the same.

[0099] Examples of tetracarboxylic dianhydrides include pyromellitic acid, pyromellitic dianhydride (PMDA), 3,3',4,4'-biphenyltetracarboxylic dianhydride, 3,3',4,4'-diphenylsulfidetetracarboxylic dianhydride, 3,3',4,4'-diphenylsulfonetetracarboxylic dianhydride, 3,3',4,4'-benzophenonetetracarboxylic dianhydride, and 3,3',4,4'-diphenylmethanetetracarboxylic dianhydride. Water, 2,2',3,3'-diphenylmethanetetracarboxylic dianhydride, 2,3,3',4'-biphenyltetracarboxylic dianhydride, 2,3,3',4'-benzophenonetetracarboxylic dianhydride, 4,4'-oxydiphthalic dianhydride, 2,3,6,7-naphthalenetetracarboxylic dianhydride, 1,4,5,7-naphthalenetetracarboxylic dianhydride, 2,2-bis(3,4-dicarboxyphenyl)propane dianhydride, 2,2-bis (2,3-Dicarboxyphenyl)propane dianhydride, 2,2-bis(3,4-dicarboxyphenyl)hexafluoropropane dianhydride, 1,3-diphenylhexafluoropropane-3,3,4,4-tetracarboxylic dianhydride, 1,4,5,6-naphthalenetetracarboxylic dianhydride, 2,2',3,3'-diphenyltetracarboxylic dianhydride, 3,4,9,10-perylenetetracarboxylic dianhydride, 1,2,4,5-naphthalene Examples thereof include tetracarboxylic dianhydrides, 1,4,5,8-naphthalenetetracarboxylic dianhydride, 1,8,9,10-phenanthrenetetracarboxylic dianhydride, 1,1-bis(2,3-dicarboxyphenyl)ethane dianhydride, 1,1-bis(3,4-dicarboxyphenyl)ethane dianhydride, 1,2,3,4-benzenetetracarboxylic dianhydride, and alkyl derivatives having 1 to 6 carbon atoms and alkoxy derivatives having 1 to 6 carbon atoms.

[0100] Examples of the tetracarboxylic dianhydride include compounds represented by any one of formulas (DAA-1) to (DAA-5).

[0101] [ka]

[0102] The monovalent organic group X is preferably an alkyl group which may have a substituent or an aromatic ring group which may have a substituent, and more preferably an alkyl group which may have an aromatic ring group. The alkyl group may be linear, branched, or cyclic, and the cyclic group may be monocyclic or polycyclic. The linear or branched alkyl group preferably has 1 to 30 carbon atoms. The cyclic alkyl group (cycloalkyl group) preferably has 3 to 30 carbon atoms. Examples of the alkyl group include linear or branched alkyl groups such as methyl, ethyl, propyl, butyl, pentyl, hexyl, heptyl, octyl, nonyl, decyl, dodecyl, tetradecyl, octadecyl, isopropyl, isobutyl, sec-butyl, t-butyl, 1-ethylpentyl, and 2-ethylhexyl groups; monocyclic cycloalkyl groups such as cyclopropyl, cyclobutyl, cyclopentyl, cyclohexyl, cycloheptyl, and cyclooctyl groups; and polycyclic cycloalkyl groups such as adamantyl, norbornyl, bornyl, camphenyl, decahydronaphthyl, tricyclodecanyl, tetracyclodecanyl, campholoyl, dicyclohexyl, and pinenyl groups. The substituent that the alkyl group may have is preferably an aromatic ring group, which will be described later.

[0103] The aromatic ring group may be either an aromatic hydrocarbon ring group or an aromatic heterocyclic group, and may be either a monocyclic or polycyclic group. Examples of the ring constituting the aromatic ring group include aromatic hydrocarbon rings such as a benzene ring, a naphthalene ring, a biphenyl ring, a fluorene ring, a pentalene ring, an indene ring, an azulene ring, a heptalene ring, an indacene ring, a perylene ring, a pentacene ring, an acenaphthene ring, a phenanthrene ring, an anthracene ring, a naphthacene ring, a chrysene ring, and a triphenylene ring; a fluorene ring, a pyrrole ring, a furan ring, a thiophene ring, an imidazole ring, an oxazole ring, a thiazole ring, a pyridine ring, a pyrazine ring, and a pyrrole ring; aromatic heterocyclic groups such as an imidine ring, a pyridazine ring, an indolizine ring, an indole ring, a benzofuran ring, a benzothiophene ring, an isobenzofuran ring, a quinolizine ring, a quinoline ring, a phthalazine ring, a naphthyridine ring, a quinoxaline ring, a quinoxazoline ring, an isoquinoline ring, a carbazole ring, a phenanthridine ring, an acridine ring, a phenanthroline ring, a thianthrene ring, a chromene ring, a xanthene ring, a phenoxathiin ring, a phenothiazine ring, and a phenazine ring; The substituent that the aromatic ring group may have is preferably the alkyl group described above.

[0104] The repeating unit represented by formula (1) is preferably a repeating unit represented by formula (1-A) or a repeating unit represented by formula (1-B).

[0105] [ka]

[0106] In formula (1-A) and formula (1-B), A 11 and A 12 represents an oxygen atom or -NH-. 111 and R 112 R each independently represents a divalent organic group. 113 and R 114 each independently represents a hydrogen atom or a monovalent organic group.

[0107] In formula (1-A) and formula (1-B), A 11 , A 12 , R 111 , R 113 , and R 114are respectively expressed as A in equation (1). 1 , A 2 , R 111 , R 113 , and R 114 The same definition and preferred embodiments are also the same. In formula (1-A), R 112 In equation (5), R 112 The same definition and preferred embodiments are also the same.

[0108] In formula (1-A), the bonding positions of the carbonyl group to the benzene ring are preferably 4, 5, 3', and 4' in formula (1-A). In formula (1-B), the bonding positions of the carbonyl group to the benzene ring are preferably 1, 2, 4, and 5 in formula (1-B).

[0109] The polyimide precursor may contain other repeating units in addition to the repeating unit represented by formula (1).

[0110] The content of the repeating unit represented by formula (1) is preferably 50 mol % or more, more preferably 70 mol % or more, and even more preferably 90 mol % or more, based on all repeating units of the polyimide precursor, and the upper limit is preferably 100 mol % or less.

[0111] The polyimide precursor also preferably contains a fluorine atom. The content of fluorine atoms in the polyimide precursor is preferably 10% by mass or more, more preferably 20% by mass or more, based on the total mass of the polyimide precursor, and the upper limit is preferably 50% by mass or less.

[0112] The polyimide precursor may be obtained by copolymerizing the repeating unit represented by formula (1) with an aliphatic group having a siloxane structure, which can improve adhesion to the transfer target. Examples of the aliphatic group having a siloxane structure include bis(3-aminopropyl)tetramethyldisiloxane and bis(paraaminophenyl)octamethylpentasiloxane.

[0113] The weight average molecular weight (Mw) of the polyimide precursor is preferably from 2,000 to 500,000, more preferably from 5,000 to 100,000, and even more preferably from 10,000 to 50,000. The number average molecular weight (Mn) of the polyimide precursor is preferably 800 to 250,000, more preferably 2,000 to 50,000, and even more preferably 4,000 to 25,000. The polydispersity (Mw / Mn) of the polyimide precursor is preferably from 1.5 to 3.5, more preferably from 2.0 to 3.0.

[0114] Silicone resin Silicone resin is a polymer with a siloxane bond as the main skeleton, specifically, M units (RSiO 1 / 2 ), D units (RSiO 2 / 2 ), T units (RSiO 3 / 2 ), and Q units (SiO 4 / 2 ) wherein R represents a monovalent organic group. Examples of silicone resins include curable silicone resins, silicone graft resins, and modified silicone resins such as alkyl-modified silicone resins, with curable silicone resins being preferred. Examples of the curable silicone resin include an addition reaction type silicone resin, a condensation reaction type silicone resin, and an ultraviolet or electron beam curable silicone resin.

[0115] Examples of addition reaction type silicone resins include resins obtained by reacting and curing polydimethylsiloxane, which has vinyl groups introduced at the terminals or side chains, with hydrogen siloxane using a platinum catalyst. An example of a condensation reaction type silicone resin is a resin having a three-dimensional crosslinked structure formed by condensing polydimethylsiloxane having a hydroxyl group at its terminal with polydimethylsiloxane having a hydrogen atom at its terminal using an organotin catalyst. Examples of UV-curable silicone resins include those that utilize the same radical reaction as silicone rubber crosslinking, those that are photocured by introducing unsaturated groups, those that use UV or electron beams to decompose onium salts to generate strong acids, which then cleave epoxy groups to crosslink, and those that crosslink via an addition reaction of thiol to vinyl siloxane.Specific examples include acrylate-modified polydimethylsiloxane and glycidoxy-modified polydimethylsiloxane. Examples of silicone resins include a dimethylsiloxane-methylvinylsiloxane copolymer terminated at both molecular chain ends with trimethylsiloxy groups, a dimethylsiloxane-diphenylsiloxane-methylvinylsiloxane copolymer terminated at both molecular chain ends with trimethylsiloxy groups, and a dimethylsiloxane-diphenylsiloxane copolymer terminated at both molecular chain ends with dimethylvinylsiloxy groups.

[0116] The silicone resin preferably has an aromatic ring. The aromatic ring is preferably an aromatic hydrocarbon ring, more preferably an aromatic hydrocarbon ring having 6 to 12 carbon atoms, and even more preferably a benzene ring.

[0117] As the silicone resin, a modified silicone resin obtained by reacting an organosilicon compound with a hydrosilylation agent is also preferred. The organosilicon compound preferably further contains a polymerizable group, such as a polymerizable group contained in a resin. The organosilicon compound may be, for example, a compound having a silyl group, and 1,4-bis(dimethylsilyl)benzene or trivinylphenylsilane is preferred. Examples of hydrosilylation agents include platinum-based catalysts such as platinum metal-supported carbon powder, platinum black, platinic chloride, chloroplatinic acid, reaction products of chloroplatinic acid and monohydric alcohols, complexes of chloroplatinic acid and olefins, and platinum bisacetoacetate; and platinum group metal catalysts such as palladium-based catalysts and rhodium-based catalysts. The reaction temperature is preferably 100 to 200° C., and the reaction time is preferably 1 to 10 hours.

[0118] Examples of silicone resins include resins obtained from organosiloxanes and curable compositions described in JP 2020-026502 A.

[0119] One preferred embodiment of the silicone resin is polysilsesquioxane. Polysilsesquioxane is a general term for polymers whose constituent units are the above-mentioned T units. The skeleton structure of the polysilsesquioxane is not particularly limited, and may be any of a cage polysilsesquioxane, a ladder polysilsesquioxane, a double-decker polysilsesquioxane, and a random polysilsesquioxane, with a ladder polysilsesquioxane or a cage polysilsesquioxane being preferred. The cage polysilsesquioxane may be either a complete cage polysilsesquioxane or an incomplete cage polysilsesquioxane, but a complete cage polysilsesquioxane is preferred. The cage polysilsesquioxanes include T8 polysilsesquioxanes consisting of eight T3 structural units, which will be described later; T3 polysilsesquioxanes consisting of ten T3 structural units, which will be described later; 10 T consisting of polysilsesquioxane and 12 of the following structural units T3 12 The polysilsesquioxane may be any of the polysilsesquioxanes.

[0120] The polysilsesquioxane preferably has a polymerizable group, since the cured layer formed from the curable composition has a smaller linear expansion coefficient in the in-plane direction and is more excellent in thermocycling resistance. Examples of the polymerizable group include known polymerizable groups such as radical polymerizable groups, epoxy groups, oxetanyl groups, methylol groups, and alkoxymethyl groups, with radical polymerizable groups being preferred. The radical polymerizable group is preferably a group having an ethylenically unsaturated double bond. Examples of the group having an ethylenically unsaturated double bond include a vinyl group, a styryl group, a (meth)acryloyl group, a (meth)acrylamide group, an allyl group, and a vinyl ether group, and the vinyl group, the styryl group, or the (meth)acryloyl group is preferred, and the styryl group is more preferred.

[0121] It is also preferable that the polysilsesquioxane has a chain hydrocarbon group, since this allows the cured layer formed from the curable composition to have better conformability to unevenness and a film including such a cured layer to be suitably used as a transfer film. Examples of the chain hydrocarbon group include an alkyl group, an alkenyl group, and an alkynyl group, with an alkyl group being preferred. The chain hydrocarbon group may be either a straight chain or a branched chain, and is preferably a straight chain. The chain hydrocarbon group preferably has 1 to 20 carbon atoms, more preferably 2 to 15 carbon atoms, and even more preferably 4 to 12 carbon atoms.

[0122] The polysilsesquioxane preferably contains a structural unit selected from the structural unit T1 represented by formula (T1), the structural unit T2 represented by formula (T2), and the structural unit T3 represented by formula (T3), more preferably contains a structural unit selected from the structural unit T2 and the structural unit T3, and even more preferably contains the structural unit T3. The structural units T1 to T3 belong to so-called T units. Formula (T1):R 1 -Si(OX 1 )2O 1 / 2 Formula (T2):R 1 -Si(OX 1 )O 2 / 2 Formula (T3):R 1 -SiO 3 / 2 In formulas (T1) to (T3), R 1 Each of X independently represents a monovalent organic group. 1 each independently represents a hydrogen atom or an alkyl group. In polysilsesquioxane, multiple R 1 may be the same or different. In other words, the polysilsesquioxane may contain different R 1 The copolymer may be a copolymer containing a plurality of structural units having the following structure:

[0123] In formulas (T1) to (T3), R 1 each independently represents a monovalent organic group. Examples of the monovalent organic group include a hydrocarbon group and a heteroatom-containing group. The hydrocarbon group may be either an aliphatic hydrocarbon group or an aromatic hydrocarbon group. The aliphatic hydrocarbon group may be either chain or cyclic, preferably chain. The chain aliphatic hydrocarbon group may be either linear or branched, preferably linear. The aliphatic hydrocarbon group preferably has 1 to 20 carbon atoms, more preferably 1 to 15 carbon atoms, and even more preferably 3 to 12 carbon atoms. The aromatic hydrocarbon group preferably has 4 to 20 carbon atoms, more preferably 5 to 12 carbon atoms, and even more preferably 5 or 6 carbon atoms. Examples of the heteroatom-containing group include groups in which one or more carbon atoms of the hydrocarbon group are substituted with heteroatoms. The heteroatom is preferably an oxygen atom, a nitrogen atom, or a sulfur atom. The hydrocarbon group and heteroatom-containing group may have a substituent, such as a halogen atom, an alkyl group, an alkoxy group, an aryl group, or the polymerizable group described above.

[0124] In terms of achieving better effects of the present invention, the curable composition preferably contains at least one selected from ladder-type polysilsesquioxanes and cage-type polysilsesquioxanes, more preferably contains a cage-type polysilsesquioxane, and even more preferably contains a ladder-type polysilsesquioxane and a cage-type polysilsesquioxane. The skeletal structure of the polysilsesquioxane is determined by the molecular weight obtained by GPC (Gel Permeation Chromatography) and29 It can be identified from the structural units, etc., obtained from the peak positions in Si-NMR (Nuclear Magnetic Resonance) spectrum measurements. Specifically, for example, the cage polysilsesquioxane has a peak top molecular weight of T8 polysilsesquioxane, T 10 Polysilsesquioxane, or T 12 It is detected as a peak corresponding to the molecular weight of polysilsesquioxane. The molecular weight of each of the above cage polysilsesquioxanes is calculated appropriately depending on the substituents possessed by the cage polysilsesquioxane, and is often detected as a peak at a weight average molecular weight (Mw) of 300 to 4,000.

[0125] Epoxy resin The epoxy resin is a resin having an epoxy group. Examples of epoxy resins include bisphenol A type epoxy resins, bisphenol F type epoxy resins, bisphenol S type epoxy resins, bisphenol AF type epoxy resins, dicyclopentadiene type epoxy resins, trisphenol epoxy resins, naphthol novolac epoxy resins, phenol novolac type epoxy resins, tert-butyl-catechol type epoxy resins, naphthalene type epoxy resins, naphthol type epoxy resins, anthracene type epoxy resins, glycidylamine type epoxy resins, glycidyl ester type epoxy resins, cresol novolac type epoxy resins, biphenyl type epoxy resins, linear aliphatic epoxy resins, epoxy resins having a butadiene structure, alicyclic epoxy resins, heterocyclic epoxy resins, spiro ring-containing epoxy resins, cyclohexanedimethanol type epoxy resins, naphthylene ether type epoxy resins, and trimethylol type epoxy resins.

[0126] The epoxy resin preferably contains an epoxy resin that is liquid at a temperature of 20°C (hereinafter also referred to as "liquid epoxy resin") and an epoxy resin that is solid at a temperature of 20°C (hereinafter also referred to as "solid epoxy resin"), in terms of excellent flexibility and improved breaking strength of the resulting cured layer.

[0127] As the liquid epoxy resin, bisphenol A type epoxy resin, bisphenol F type epoxy resin, phenol novolac type epoxy resin or naphthalene type epoxy resin is preferred, and bisphenol A type epoxy resin, bisphenol F type epoxy resin or naphthalene type epoxy resin is more preferred. Examples of liquid epoxy resins include HP4032, HP4032D, EXA4032SS, and HP4032SS (naphthalene-type epoxy resins) manufactured by DIC Corporation; jER828EL (bisphenol A-type epoxy resin), jER807 (bisphenol F-type epoxy resin), and jER152 (phenol novolac-type epoxy resin) manufactured by Mitsubishi Chemical Corporation; and ZX1059 (a mixture of bisphenol A-type epoxy resin and bisphenol F-type epoxy resin) manufactured by Nippon Steel Chemical Co., Ltd. As the liquid epoxy resin, HP4032SS or ZX1059 is preferred.

[0128] As the solid epoxy resin, a tetrafunctional naphthalene type epoxy resin, a cresol novolac type epoxy resin, a dicyclopentadiene type epoxy resin, a trisphenol epoxy resin, a naphthol novolac epoxy resin, a biphenyl type epoxy resin, or a naphthylene ether type epoxy resin is preferred, a tetrafunctional naphthalene type epoxy resin, a biphenyl type epoxy resin, or a naphthylene ether type epoxy resin is more preferred, and a biphenyl type epoxy resin is even more preferred. Examples of solid epoxy resins include HP-4700, HP-4710 (tetrafunctional naphthalene type epoxy resins), N-690 (cresol novolac type epoxy resin), N-695 (cresol novolac type epoxy resin), HP7200, HP7200H, HP7200K-65I (dicyclopentadiene type epoxy resins), EXA7311, EXA7311-G3, and HP6000 (naphthylene ether type epoxy resins), and EPPN-502H (trisphenol A type epoxy resins) manufactured by DIC Corporation. Examples of epoxy resins include NC7000L (naphthol novolac epoxy resin), NC3000H, NC3000, NC3000L, and NC3100 (biphenyl-type epoxy resins), manufactured by Nippon Kayaku Co., Ltd.; ESN475 (naphthol novolac-type epoxy resin) and ESN485 (naphthol novolac-type epoxy resin), manufactured by Nippon Steel Chemical Co., Ltd.; and YX4000H, YL6121 (biphenyl-type epoxy resin), and YX4000HK (bixylenol-type epoxy resin), manufactured by Mitsubishi Chemical Corporation. As the solid epoxy resin, YX4000HK, NC3000L or HP7200H is preferred.

[0129] Polyamide resin The polyamide resin is a resin having an amide bond. Examples of polyamide resins include acrylamide resins, vinylamide resins, and allylamide resins.

[0130] Maleimide resin The maleimide resin is a resin having a maleimide group. The maleimide resin is preferably a bismaleimide resin, and more preferably at least one selected from the group consisting of a bismaleimide resin represented by the following formula (III) and a novolac-type maleimide resin represented by the following formula (IV).

[0131] [ka] In formula (III), R represents a divalent organic group containing an aromatic ring or a linear, branched, or cyclic aliphatic hydrocarbon group. R is preferably a divalent group consisting of a benzene group, a toluene group, a xylene group, a naphthalene group, a linear, branched, or cyclic saturated hydrocarbon group, or a combination thereof. R is preferably a divalent group represented by the following formula (v), (vi), or (vii):

[0132] [ka]

[0133] [ka]

[0134] In formula (IV), s represents an integer of 0 to 20.

[0135] The maleimide resin may be a compound described in paragraphs 0020 to 0023 of JP-A No. 2003-321608. Commercially available maleimide resins include BMI-1000, 2000, 3000, 4000, 5000, 5100, and 7000 (bismaleimide resins manufactured by Daiwa Chemical Industry Co., Ltd.), BANI-X (bismaleimide resins manufactured by Shin-Nakamura Chemical Co., Ltd.), and BANI-M (bismaleimide resins manufactured by Shin-Nakamura Chemical Co., Ltd.).

[0136] Polyphenylene ether resin The polyphenylene ether resin is a resin having a phenylene ether group. The polyphenylene ether resin may have either a linear structure or a branched structure, and preferably has a branched structure. In the polyphenylene ether resin having a branched structure, it is preferable that ether bonds are directly bonded to at least three positions, i.e., the ipso position, the ortho position, and the para position, of at least one benzene ring constituting the polyphenylene ether resin.

[0137] The polyphenylene ether resin having a branched structure can be obtained, for example, by polymerizing two or more kinds of phenol compounds. The phenol compound is preferably a phenol compound having hydrogen atoms at the ortho and para positions and having a reactive group, or a mixture of a phenol compound having hydrogen atoms at the ortho and para positions and no reactive group and a phenol compound having no hydrogen atom at the ortho position, a hydrogen atom at the para position and having a reactive group.

[0138] Examples of phenol compounds used in the synthesis of polyphenylene ether resins include o-vinylphenol, m-vinylphenol, o-allylphenol, m-allylphenol, 3-vinyl-6-methylphenol, 3-vinyl-6-ethylphenol, 3-vinyl-5-methylphenol, 3-vinyl-5-ethylphenol, 3-allyl-6-methylphenol, 3-allyl-6-ethylphenol, 3-allyl-5-methylphenol, 3-allyl-5-ethylphenol, phenol, o-cresol, m-cresol, o-ethylphenol, m-ethylphenol, 2,3-xylenol, 2,5-xylenol, 3,5-xylenol, o-tert-butylphenol, m-tert-butylphenol, o-phenylphenol, m-phenylphenol, and 2-dodecylphenol. , 2-allyl-6-methylphenol, 2-allyl-6-ethylphenol, 2-allyl-6-phenylphenol, 2-allyl-6-styrylphenol, 2,6-divinylphenol, 2,6-diallylphenol, 2,6-diisopropenylphenol, 2,6-dibutenylphenol, 2,6-diisobutenylphenol, 2,6-diisopentenylphenol, 2-methyl-6-styrylphenol, 2-vinyl-6-methylphenol, 2-vinyl-6-ethylphenol, 2,6-dimethylphenol, 2,3,6-trimethylphenol, 2-methyl-6-ethylphenol, 2-ethyl-6-n-propylphenol, 2-methyl-6-n-butylphenol, 2-methyl-6-phenylphenol, 2,6-diphenylphenol, and 2,6-ditolylphenol. Of these, the phenol compound is preferably 2,6-dimethylphenol or 2-allylphenol.

[0139] The polyphenylene ether resin also preferably has a reactive group, preferably a group having an ethylenically unsaturated double bond, more preferably a vinylphenyl group or a (meth)acryloyl group. When the polyphenylene ether resin has a reactive group, the curable composition preferably contains a maleimide compound, which reacts with the polyphenylene ether resin to give a modified polyphenylene ether. Examples of modified polyphenylene ethers include resins obtained by curing the resin compositions described in WO 2022 / 102756.

[0140] Examples of polyphenylene ether resins include poly(2,6-diethyl-1,4-phenylene) ether, poly(2-ethyl-6-n-propyl-1,4-phenylene) ether, poly(2,6-di-n-propyl-1,4-phenylene) ether, poly(2-methyl-6-n-butyl-1,4-phenylene) ether, poly(2-ethyl-6-isopropyl-1,4-phenylene) ether, poly(2-methyl-6-chloroethyl-1,4-phenylene) ether, poly(2-methyl-6-hydroxyethyl-1,4-phenylene) ether, and poly(2-methyl-6-chloroethyl-1,4-phenylene) ether. Examples of polyphenylene ether resins include those described in JP-A-2022-157695.

[0141] Other resins The resin may contain other resins in addition to the various resins described above. Examples of other resins include phenol resin, benzocyclobutene resin, fluorene resin, liquid crystal polymer, polyethersulfone, polyarylate, polyetherimide, polyphenylsulfone, polycarbonate, acrylonitrile-butadiene-styrene resin, and polyphenylene sulfide.

[0142] As described above, the resin contained in the curable composition may be a precursor of each of the resins described above.

[0143] The weight average molecular weight (Mw) of the resin is preferably from 2,000 to 500,000, more preferably from 5,000 to 100,000, and even more preferably from 5,000 to 50,000. The number average molecular weight (Mn) of the resin is preferably from 800 to 250,000, more preferably from 2,000 to 50,000, and even more preferably from 4,000 to 25,000. The polydispersity (Mw / Mn) of the resin is preferably from 1.0 to 3.5, more preferably from 2.0 to 3.0.

[0144] The resins may be used alone or in combination of two or more. The content of the resin is preferably from 1.0 to 99.0 mass %, more preferably from 5.0 to 98.0 mass %, and even more preferably from 5.0 to 95.0 mass %, based on the total solid content of the curable composition.

[0145] (inorganic filler) The curable composition may also contain an inorganic filler. The inorganic filler is preferably an inorganic filler. Examples of inorganic fillers include silicon dioxide (silica); silicates such as kaolinite, kaolin clay, calcined clay, talc, and glass fillers such as chion-doped glass; alumina, barium sulfate, mica powder, aluminum hydroxide, magnesium hydroxide, calcium carbonate, magnesium carbonate, magnesium oxide, boron nitride, aluminum borate, barium titanate, strontium titanate, calcium titanate, magnesium titanate, bismuth titanate, titanium oxide, barium zirconate, calcium zirconate, zirconium phosphate, cordierite, zirconium tungstate, and manganese nitride. The inorganic filler preferably contains at least one selected from the group consisting of silicon dioxide (silica), boron nitride, barium sulfate, and silicates, and more preferably contains silicon dioxide (silica).

[0146] The shape of the inorganic filler may be either spherical or non-spherical (for example, crushed or fibrous), with spherical being preferred.

[0147] The average particle size of the inorganic filler is preferably 500 nm or less, more preferably 300 nm or less, and even more preferably 150 nm or less. The lower limit of the average particle size of the inorganic filler is preferably more than 0 nm, more preferably 5 nm or more, even more preferably 10 nm or more, and particularly preferably 50 nm or more. The average particle size of the inorganic filler is also preferably 5 to 300 nm, more preferably 10 to 150 nm, and even more preferably 50 to 150 nm. The average particle size of the inorganic filler is a value calculated by the following particle size measurement method. Particle size measurement method: A rectangular area of ​​3 μm × 10 μm in a cross section along the normal direction of the surface of a composition layer formed using a curable composition is observed with a scanning electron microscope, and the long diameters of all inorganic fillers observed within the area are measured at five different locations on the film. The average value of the long diameters of all inorganic fillers measured in each step is taken as the average particle size of the inorganic fillers.

[0148] The particle size measurement method will now be described in detail. The curable composition is applied to a substrate (preferably a glass substrate) to form a composition layer. The thickness of the composition layer is preferably 3 μm or more. In addition, to form the composition layer, after applying the curable composition, a drying treatment may be carried out as necessary. A cross section of the resulting composition layer was cut out along the normal direction of the surface (the surface opposite the substrate side), and a rectangular area of ​​3 μm × 10 μm on the cross section was observed using a scanning electron microscope. The major axis of all inorganic fillers observed within the area was measured. The scanning electron microscope used was a Hitachi High-Tech S-4800. The magnification during observation was 50,000 times. The above operation is carried out at five different locations in the composition layer, and the average value (arithmetic mean value) of the major axes of all the inorganic fillers measured in each operation is taken as the average particle size of the inorganic filler. The above-mentioned major axis refers to the length of the longest line segment among the line segments connecting any two points on the outline of the external shape of the inorganic filler in the observed image. Furthermore, when the inorganic filler aggregates to form aggregates in the observed image, the major axis of each inorganic filler constituting the aggregate is measured.

[0149] Examples of inorganic fillers include NSS-3N (manufactured by Tokuyama Corporation, silicon dioxide), NHM-5N (manufactured by Tokuyama Corporation, silicon dioxide, solid content concentration 100% by mass), NHM-3N (manufactured by Tokuyama Corporation, silicon dioxide, solid content concentration 100% by mass), Seahoster KE-S30 (manufactured by Nippon Shokubai Co., Ltd., silicon dioxide, solid content concentration 100% by mass), YA050C-MJE (manufactured by Admatechs Co., Ltd., silicon dioxide, solid content concentration 50% by mass MEK (methyl ethyl ketone) slurry), SFP-20M (manufactured by Denka Co., Ltd., silicon dioxide), and PMA-ST. (manufactured by Nissan Chemical Industries, Ltd., silicon dioxide), MEK-ST-L (manufactured by Nissan Chemical Industries, Ltd., silicon dioxide), MEK-AC-5140Z (manufactured by Nissan Chemical Industries, Ltd., silicon dioxide), MEK-EC-2430Z (manufactured by Nissan Chemical Industries, Ltd., solids concentration 30% by mass), barium sulfate (manufactured by Nippon Solvay K.K., solids concentration 100% by mass), Y50SP-AM1 (manufactured by Admatechs Co., Ltd., silicon dioxide, MEK slurry with a solids concentration of 50% by mass), and Y50SZ-AM1 (manufactured by Admatechs Co., Ltd., silicon dioxide, MEK slurry with a solids concentration of 50% by mass).

[0150] The inorganic filler may be surface-modified with a surface treatment agent. Examples of the surface modifier include a silane coupling agent, a titanate coupling agent, a disilazane compound, and a basic compound. The surface modifier may have a reactive group, for example, the reactive groups that the above-mentioned resins may have.

[0151] The inorganic fillers may be used alone or in combination of two or more. The content of the inorganic filler is preferably 20.0% by mass or more, more preferably 30.0% by mass or more, based on the total solid content of the curable composition, and is preferably 90.0% by mass or less, more preferably 80.0% by mass or less, and even more preferably 75.0% by mass or less, based on the total solid content of the curable composition.

[0152] (Compounds having reactive groups) The curable composition may contain a compound having a reactive group. The compound having a reactive group is a compound different from the above-mentioned resin, and is a compound having a reactive group. Furthermore, the compound having a reactive group is preferably a compound different from the surface modifier. Examples of the reactive group possessed by the compound having a reactive group include reactive groups that can be possessed by the above-mentioned resins, and a polymerizable group is preferred. That is, the curable composition preferably contains a compound having a polymerizable group (hereinafter also referred to as a "polymerizable compound") as the compound having a reactive group. The compound having a reactive group may have one or more reactive groups, or may have two or more reactive groups. The number of reactive groups that the compound having a reactive group has is preferably 1 or 2 or more, more preferably 2 to 10, and even more preferably 2 to 6.

[0153] When the curable composition contains a polymerizable compound (preferably a compound having a group with an ethylenically unsaturated double bond), the curable composition preferably further contains a photopolymerization initiator, which will be described later.

[0154] A polymerizable compound is a compound having one or more polymerizable groups in one molecule. As the polymerizable compound, a compound having a group with an ethylenically unsaturated double bond is preferred, a compound having a (meth)acryloyl group, a vinyl group or a styryl group is more preferred, and a compound having a (meth)acryloyl group is even more preferred.

[0155] The number of polymerizable groups that the polymerizable compound has is preferably 1 or 2 or more, more preferably 2 to 10, and even more preferably 2 to 6. Examples of the polymerizable compound include a polymerizable compound having one polymerizable group in one molecule (hereinafter also referred to as a "monofunctional polymerizable compound"), a polymerizable compound having two polymerizable groups in one molecule (hereinafter also referred to as a "bifunctional polymerizable compound"), and a polymerizable compound having three or more polymerizable groups in one molecule (hereinafter also referred to as a "trifunctional or higher functional polymerizable compound"). The polymerizable compound is preferably a bifunctional polymerizable compound or a trifunctional or higher functional polymerizable compound.

[0156] Examples of bifunctional polymerizable compounds include polyethylene glycol (meth)acrylate, tricyclodecane dimethanol di(meth)acrylate, tricyclodecane dimenanol di(meth)acrylate, 1,9-nonanediol di(meth)acrylate, and 1,6-hexanediol di(meth)acrylate. Commercially available bifunctional polymerizable compounds include, for example, diethylene glycol dimethacrylate (2G, manufactured by Shin-Nakamura Chemical Co., Ltd.), triethylene glycol dimethacrylate (3G, manufactured by Shin-Nakamura Chemical Co., Ltd.), polyethylene glycol #200 dimethacrylate (4G, manufactured by Shin-Nakamura Chemical Co., Ltd.), tricyclodecane dimethanol diacrylate (A-DCP, manufactured by Shin-Nakamura Chemical Co., Ltd.), tricyclodecane dimenanol dimethacrylate (DCP, manufactured by Shin-Nakamura Chemical Co., Ltd.), 1,9-nonanediol diacrylate (A-NOD-N, manufactured by Shin-Nakamura Chemical Co., Ltd.), 1,6-hexanediol diacrylate (A-HD-N, manufactured by Shin-Nakamura Chemical Co., Ltd.), SR205NS (manufactured by Sartomer Inc.), and SR209 (manufactured by Sartomer Inc.).

[0157] Examples of the tri- or higher functional polymerizable compound include dipentaerythritol (tri / tetra / penta / hexa)(meth)acrylate, pentaerythritol (tri / tetra)(meth)acrylate, trimethylolpropane tri(meth)acrylate, ditrimethylolpropane tetra(meth)acrylate, isocyanuric acid (meth)acrylate, and (meth)acrylate compounds having a glycerin tri(meth)acrylate skeleton. The term "(tri / tetra / penta / hexa)(meth)acrylate" is a concept that encompasses tri(meth)acrylate, tetra(meth)acrylate, penta(meth)acrylate, and hexa(meth)acrylate, and the term "(tri / tetra)(meth)acrylate" is a concept that encompasses tri(meth)acrylate and tetra(meth)acrylate.

[0158] Examples of the polymerizable compound include caprolactone-modified (meth)acrylate compounds (KAYARAD (registered trademark) DPCA-20, etc., manufactured by Nippon Kayaku Co., Ltd., and A-9300-1CL, etc., manufactured by Shin-Nakamura Chemical Co., Ltd.), alkylene oxide-modified (meth)acrylate compounds (KAYARAD RP-1040, etc., manufactured by Nippon Kayaku Co., Ltd., ATM-35E and A-9300, etc., manufactured by Shin-Nakamura Chemical Co., Ltd., and EBECRYL (registered trademark) 135, etc., manufactured by Daicel-Allnex Corporation), and ethoxylated glycerin triacrylate (A-GLY-9E, etc., manufactured by Shin-Nakamura Chemical Co., Ltd.).

[0159] Examples of the polymerizable compound include urethane (meth)acrylate (preferably tri- or higher functional urethane (meth)acrylate). The number of polymerizable groups in the urethane (meth)acrylate is preferably 6 or more, more preferably 8 or more. The upper limit is preferably 20 or less. Examples of trifunctional or higher urethane (meth)acrylates include 8UX-015A (manufactured by Taisei Fine Chemical Co., Ltd.); UA-32P, U-15HA, and UA-1100H (all manufactured by Shin-Nakamura Chemical Co., Ltd.); AH-600 (manufactured by Kyoeisha Chemical Co., Ltd.); and UA-306H, UA-306T, UA-306I, UA-510H, and UX-5000 (all manufactured by Nippon Kayaku Co., Ltd.).

[0160] The compound having a reactive group may have liquid crystal properties.

[0161] The compound having a reactive group is also preferably a low molecular weight compound. The molecular weight of the compound having a reactive group is preferably 2000 or less, more preferably 1500 or less, and even more preferably 1000 or less. The molecular weight of the compound having a reactive group is preferably 100 or more, more preferably 150 or more, and even more preferably 200 or more.

[0162] The compound having a reactive group may be used alone or in combination of two or more. The content of the compound having a reactive group is preferably from 1 to 950 mass %, more preferably from 3 to 30 mass %, and even more preferably from 5 to 10 mass %, based on the total solid content of the curable composition.

[0163] (Photopolymerization initiator) The curable composition may contain a photopolymerization initiator in order to allow the curable composition to exhibit photolithographic properties. The above-mentioned "exhibiting photolithographic properties" means the property of being able to form a pattern by a photolithography method. When the first transfer film is used in the production of the cured layer and semiconductor package described below, it is preferable that the curable composition exhibits photolithographic properties, since this allows for the formation of a pattern with high precision. The photopolymerization initiator is a compound different from the various components described above. Examples of the photopolymerization initiator include a photoradical polymerization initiator, a photocationic polymerization initiator, and a photoanionic polymerization initiator, and a photoradical polymerization initiator is preferred.

[0164] Examples of the photopolymerization initiator include oxime ester compounds (photopolymerization initiators having an oxime ester structure), aminoacetophenone compounds (photopolymerization initiators having an aminoacetophenone structure), hydroxyacetophenone compounds (photopolymerization initiators having a hydroxyacetophenone structure), acylphosphine oxide compounds (photopolymerization initiators having an acylphosphine oxide structure), and bistriphenylimidazole compounds (photopolymerization initiators having a bistriphenylimidazole structure). As the photopolymerization initiator, an oxime ester compound or an aminoacetophenone compound is preferred, and an oxime ester compound is more preferred.

[0165] Examples of the oxime ester compound include 1,2-octanedione, 1-[4-(phenylthio)phenyl-, 2-(O-benzoyloxime)] (trade name: IRGACURE OXE-01, manufactured by BASF), ethanone, 1-[9-ethyl-6-(2-methylbenzoyl)-9H-carbazol-3-yl]-, 1-(O-acetyloxime) (trade name: IRGACURE OXE-02, manufactured by BASF), [8-[5-(2,4,6-trimethylphenyl)-11-(2-ethylhexyl)-11H-benzo[a]carbazolyl][2-(2,2,3,3-tetrafluoropropoxy)phenyl]methanone-(O-acetyloxime) (trade name: IRGACURE OXE-03, manufactured by BASF), 1-[4-[4-(2-benzofuranylcarbonyl)phenyl]thio]phenyl]-4-methylpentanone-1-(O-acetyloxime) (trade name: IRGACURE OXE-04, manufactured by BASF and trade name: Lunar 6, manufactured by DKSH Japan), 1-[4-(phenylthio)phenyl]-3-cyclopentylpropane-1,2-dione-2-(O-benzoyloxime) (trade name: TR-PBG-305, manufactured by Changzhou Powerful Electronic New Materials Co., Ltd.), 1,2-propanedione,3-cyclohexyl-1-[9-ethyl-6-(2-furanylcarbonyl)-9H-carbazol-3-yl]-,2-(O-acetyloxime) (trade name: TR-PBG-326, manufactured by Changzhou Powerful Electronic New Materials Co., Ltd.), and 3-cyclohexyl-1-(6-(2-(benzoyloxyimino)hexanoyl)-9-ethyl-9H-carbazol-3-yl)-propane-1,2-dione-2-(O-benzoyloxime) (trade name: TR-PBG-391, manufactured by Changzhou Powerful Electronic New Materials Co., Ltd.).

[0166] Examples of aminoacetophenone compounds include 2-(dimethylamino)-2-[(4-methylphenyl)methyl]-1-[4-(4-morpholinyl)phenyl]-1-butanone (trade name: Omnirad 379EG, Omnirad series, manufactured by IGM Resins BV), 2-methyl-1-(4-methylthiophenyl)-2-morpholinopropan-1-one (trade name: Omnirad 907), and APi-307 (1-(biphenyl-4-yl)-2-methyl-2-morpholinopropan-1-one, manufactured by Shenzhen UV-ChemTech Ltd.).

[0167] Examples of photopolymerization initiators include 2-hydroxy-1-{4-[4-(2-hydroxy-2-methyl-propionyl)-benzyl]phenyl}-2-methyl-propan-1-one (trade name: Omnirad 127), 2-benzyl-2-dimethylamino-1-(4-morpholinophenyl)-butanone-1 (trade name: Omnirad 369), 2-hydroxy-2-methyl-1-phenyl-propan-1-one (trade name: Omnirad 1173), 1-hydroxy-cyclohexyl-phenyl-ketone (trade name: Omnirad 184), 2,2-dimethoxy-1,2-diphenylethan-1-one (trade name: Omnirad 651), 2,4,6-trimethylbenzoyl-diphenylphosphine oxide (trade name: Omnirad TPO H) and bis(2,4,6-trimethylbenzoyl)phenylphosphine oxide (trade name: Omnirad 819). Examples of the photopolymerization initiator include those described in paragraphs 0031 to 0042 of JP-A No. 2011-095716 and paragraphs 0064 to 0081 of JP-A No. 2015-014783.

[0168] The photopolymerization initiator may be used alone or in combination of two or more. The content of the photopolymerization initiator is preferably from 0.01 to 10.0 mass %, more preferably from 0.1 to 5.0 mass %, and even more preferably from 0.1 to 3.0 mass %, based on the total solid content of the curable composition.

[0169] (thermal polymerization initiator) The curable composition may include a thermal polymerization initiator. The thermal polymerization initiator can be selected depending on the type of polymerizable compound, but a thermal radical polymerization initiator is preferred. The thermal radical polymerization initiator is a compound that generates radicals by thermal energy and initiates or accelerates the polymerization reaction of a polymerizable compound. Furthermore, the above-mentioned photopolymerization initiators may also have the function of initiating polymerization by heat, and may be added as thermal polymerization initiators.

[0170] Examples of the thermal polymerization initiator include known azo compounds and known peroxide compounds. Examples of the azo compounds include azobis compounds. The azo compounds may be compounds having a cyano group or may be compounds not having a cyano group. Examples of the peroxide compounds include ketone peroxides, peroxyketals, hydroperoxides, dialkyl peroxides, diacyl peroxides, peroxydicarbonates, and peroxyesters. As the thermal polymerization initiator, commercially available products can be used, and examples thereof include V-40, V-601, and VF-096 manufactured by Fujifilm Wako Pure Chemical Industries, Ltd., and Perhexyl O, Perhexyl D, Perhexyl I, Perhexa 25O, Perhexa 25Z, Percumyl D, Percumyl D-40, Percumyl D-40MB, Percumyl H, Percumyl P, and Percumyl ND manufactured by NOF Corporation. Specific examples of the thermal radical polymerization initiator include compounds described in paragraphs 0074 to 0118 of JP-A No. 2008-063554, the contents of which are incorporated herein by reference.

[0171] The thermal polymerization initiators may be used alone or in combination of two or more. The content of the thermal polymerization initiator is preferably from 0.05 to 10 mass %, more preferably from 0.1 to 10 mass %, and even more preferably from 0.1 to 5 mass %, based on the total solid content of the curable composition.

[0172] (thermal base generator) The curable composition may include a thermal base generator. When the curable composition contains a resin precursor, the reaction of the resin precursor is promoted by including a thermal base generator in the curable composition.

[0173] The thermal base generator is preferably an acidic compound or an onium salt compound (a compound consisting of a cation and an anion) that generates a base upon heating. The onium salt compound is preferably an ammonium salt compound (a compound consisting of an ammonium cation and an anion), an iminium salt compound (a compound consisting of an iminium cation and an anion), a sulfonium salt compound (a compound consisting of a sulfonium cation and an anion), an iodonium salt compound (a compound consisting of an iodonium cation and an anion), or a phosphonium salt compound (a compound consisting of a phosphonium cation and an anion), and more preferably an ammonium salt compound or an iminium salt compound. The anion constituting the onium salt compound is preferably a carboxylate anion, a phenol anion, a phosphate anion or a sulfate anion, and more preferably a carboxylate anion. The anion constituting the ammonium salt compound preferably further has an aromatic ring. Examples of the aromatic ring include A in formula (A1) described below. a1 Examples of aromatic rings that constitute aromatic ring groups represented by the following formula are given.

[0174] The base generated by the thermal base generator is preferably a secondary amine or a tertiary amine, more preferably a tertiary amine. The base may be linear, branched, or cyclic, and is preferably cyclic.

[0175] Examples of the thermal base generator include those described in WO 2018 / 038002.

[0176] The temperature at which the thermal base generator generates a base is preferably the heating temperature in step 4 in the method for producing a laminate described below. The temperature at which the thermal base generator generates a base is, for example, preferably 50 to 400°C, and more preferably 100 to 250°C. The temperature at which the thermal base generator generates a base can be measured by a known measurement method or a literature value. For example, the base generation temperature can be determined by the peak temperature of the lowest exothermic peak when the compound to be measured is heated to 250°C at 5°C / min in a pressure-resistant capsule using differential scanning calorimetry.

[0177] The thermal base generator may be used alone or in combination of two or more. The content of the thermal base generator is preferably from 0.01 to 10.0 mass %, more preferably from 0.1 to 5.0 mass %, based on the total solid content of the curable composition. The mass ratio of the content of the thermal base generator to the content of the resin is preferably from 0.0005 to 1.0, more preferably from 0.001 to 0.1, and even more preferably from 0.001 to 0.05.

[0178] (plasticizer) The curable composition may also include a plasticizer. The plasticizer is a compound different from the various components described above, and preferably does not have a reactive group.

[0179] The molecular weight of the plasticizer is preferably 200-1,000, more preferably 250-800, and even more preferably 300-600. When the plasticizer has a molecular weight distribution, the above-mentioned molecular weight refers to the weight average molecular weight.

[0180] The boiling point of the plasticizer is preferably from 230 to 500°C, more preferably from 280 to 480°C, further preferably from 300 to 450°C, and particularly preferably from 350 to 450°C. The boiling point is the boiling point under normal pressure (760 mmHg). In this specification, the boiling point of a compound is a value determined by the following measurement method. When a compound is distilled under normal pressure (760 mmHg), the boiling point is the temperature of the evaporated gas at the point where condensation begins (measured from 23 to 300°C, temperature rise rate 1°C / min). The distillation of the compound was carried out using a Liebig condenser. If distillation did not begin at 300°C under normal pressure, distillation was carried out under reduced pressure. Similar distillation was carried out at pressures of 100 mmHg, 50 mmHg, and 5 mmHg, in that order (measurement from 23 to 300°C, temperature increase rate 1°C / min, distillation at the next pressure if distillation did not begin at 300°C). The boiling point at normal pressure was calculated using the nomograph described in Science of Petroleum, Vol. II, p. 1281 (1938) based on the temperature and pressure at which condensation of the evaporated gas began. If distillation did not begin at 300°C under 5 mmHg, the boiling point at normal pressure was deemed to be greater than 500°C. The method of using a nomograph is well known. Specifically, a straight line was drawn between the boiling point at reduced pressure (line A) and the degree of vacuum (line C). The value at the intersection of the line drawn in step 1 and line B was read (step 2). This was deemed to be the boiling point at normal pressure.

[0181] The viscosity of the plasticizer at 25° C. is preferably from 0.01 to 500 mPa·s, more preferably from 0.05 to 300 mPa·s, and even more preferably from 0.1 to 100 mPa·s. The viscosity can be measured using a Brookfield viscometer.

[0182] Examples of the plasticizer include polycarboxylic acid esters, phosphoric acid esters, polyether esters, alkylene glycol monoalkyl ethers, alkylene glycol dialkyl ethers, and benzyl benzoate, with polycarboxylic acid esters being preferred.

[0183] Examples of polycarboxylic acid esters include aliphatic dicarboxylic acid esters (e.g., adipic acid esters, azelaic acid esters, and sebacate esters); aromatic dicarboxylic acid esters (e.g., phthalic acid esters); trimellitic acid esters; and citrate esters (e.g., tributyl acetyl citrate). Examples of polycarboxylic acid esters include ethylphthalyl ethyl glycolate, dihexyl phthalate, tributyl o-acetylcitrate, 2-ethylhexyl benzyl phthalate, bis(2-ethylhexyl) isophthalate, tris(2-ethylhexyl) trimellitate, and bis(2-butoxyethyl) adipate.

[0184] Examples of phosphate esters include triamyl phosphate and tris(2-butoxyethyl) phosphate.

[0185] The polyether esters are preferably organic acid esters of polyalkylene glycol. Examples of organic acids include monocarboxylic acids (e.g., butanoic acid, isobutanoic acid, 2-ethylbutyric acid, 2-ethylhexyl acid, and decanoic acid). Specific examples of polyether esters include triethylene glycol bis-2-ethylhexanoate.

[0186] Examples of alkylene glycol monoalkyl ethers and alkylene glycol dialkyl ethers include hexaethylene glycol monomethyl ether (mPEG6-OH), pentaethylene glycol monomethyl ether, tetraethylene glycol monomethyl ether, heptaethylene glycol monomethyl ether, octaethylene glycol monomethyl ether, nonaethylene glycol monomethyl ether, pentaethylene glycol dimethyl ether, hexaethylene glycol dimethyl ether, heptaethylene glycol dimethyl ether, octaethylene glycol dimethyl ether, and nonaethylene glycol dimethyl ether.

[0187] The plasticizers may be used alone or in combination of two or more. The content of the plasticizer is preferably 5.0 to 50.0 mass %, more preferably 10.0 to 30.0 mass %, based on the total solid content of the curable composition.

[0188] (surfactant) The curable composition may also include a surfactant.

[0189] Examples of surfactants include fluorine-based surfactants, hydrocarbon-based surfactants, and silicone-based surfactants. Silicone-based surfactants are preferred as surfactants. From the viewpoint of improving environmental compatibility, it is also preferred that the surfactant does not contain fluorine atoms.

[0190] Examples of fluorosurfactants include acrylic compounds that have a molecular structure containing a functional group having a fluorine atom, and when heated, the functional group having the fluorine atom is cleaved and the fluorine atom is volatilized. Examples of such fluorosurfactants include the Megafac DS series (manufactured by DIC Corporation, Chemical Daily (February 22, 2016), Nikkei Business Daily (February 23, 2016), and Megafac DS-21, etc.). The fluorosurfactant may be a polymer of a fluorine atom-containing vinyl ether compound having a fluorinated alkyl group or a fluorinated alkylene ether group and a hydrophilic vinyl ether compound. The fluorosurfactant may be a block polymer. The fluorine-based surfactant may be a fluorine-containing polymer compound containing a repeating unit derived from a (meth)acrylate compound having a fluorine atom and a repeating unit derived from a (meth)acrylate compound having two or more (preferably five or more) alkyleneoxy groups (preferably ethyleneoxy groups or propyleneoxy groups). Further, examples of fluorine-based surfactants include fluorine-containing polymers having a group with an ethylenically unsaturated double bond in the side chain, such as Megafac RS-101, RS-102, RS-718K, and RS-72-K (all manufactured by DIC Corporation).

[0191] As the fluorine-based surfactant, surfactants derived from alternative materials to compounds having a linear perfluoroalkyl group having seven or more carbon atoms, such as perfluorooctanoic acid (PFOA) and perfluorooctanesulfonic acid (PFOS), are preferred in terms of improving environmental friendliness.

[0192] Commercially available fluorine-based surfactants include, for example, Megafac F-171, F-172, F-173, F-176, F-177, F-141, F-142, F-143, F-144, F-437, F-475, F-477, F-479, F-482, F-551-A, F-552, F-554, and F-555- A, F-556, F-557, F-558, F-559, F-560, F-561, F-565, F-563, F-568, F-575, and F-780 (all manufactured by DIC); EXP.MFS-324, EXP.MFS-330, EXP.MFS-578, EXP.MFS-578-2, EXP.MFS- 579, EXP.MFS-586, EXP.MFS-587, EXP.MFS-628, EXP.MFS-631, EXP.MFS-603, R-41, R-41-LM, R-01, R-40, R-40-LM, RS-43, TF-1956, RS-90, R-94, RS-72-K, and DS-21 (all manufactured by DIC Corporation); Fluorad FC430, FC431, and FC171 (all manufactured by Sumitomo 3M); Surflon S-382, SC-101, SC-103, SC-104, SC-105, SC-1068, SC-381, SC-383, S-393, and KH-40 (all manufactured by AGC Corporation); PolyFox Examples include PF636, PF656, PF6320, PF6520, and PF7002 (all manufactured by OMNOVA); Ftergent 710FL, 710FM, 610FM, 601AD, 601ADH2, 602A, 215M, 245F, 251, 212M, 250, 209F, 222F, 208G, 710LA, 710FS, 730LM, 650AC, 681, and 683 (all manufactured by NEOS); and U-120E (manufactured by Unichem).

[0193] Examples of hydrocarbon surfactants include glycerol, trimethylolpropane, trimethylolethane, and their ethoxylates and propoxylates (e.g., glycerol propoxylate and glycerol ethoxylate), polyoxyethylene lauryl ether, polyoxyethylene stearyl ether, polyoxyethylene oleyl ether, polyoxyethylene octylphenyl ether, polyoxyethylene nonylphenyl ether, polyethylene glycol dilaurate, polyethylene glycol distearate, and sorbitan fatty acid esters. Commercially available hydrocarbon surfactants include, for example, Pluronic (registered trademark) L10, L31, L61, L62, 10R5, 17R2, and 25R2, Tetronic 304, 701, 704, 901, 904, and 150R1, and HYDROPALAT WE 3323 (all manufactured by BASF); Solsperse 20000 (manufactured by Lubrizol Japan); NCW-101, NCW-1001, and NCW-1002 (manufactured by Fujifilm Wako Pure Chemical Industries, Ltd.); Paionin D-1105, D-6112, D-6112-W, and D-6315 (manufactured by Takemoto Oil & Fat Co., Ltd.); and Olfine E1010, Surfynol 104, 400, and 440 (manufactured by Nissin Chemical Industry Co., Ltd.).

[0194] Examples of silicone surfactants include linear polymers consisting of siloxane bonds, modified siloxane polymers with organic groups introduced into the side chains and / or terminals, and polymers having repeating units with hydrophilic groups in the side chains and repeating units with groups having siloxane bonds in the side chains. Preferred silicone surfactants are polymers having repeating units with hydrophilic groups in the side chains and repeating units with groups having siloxane bonds in the side chains. The polymers may be either random copolymers or block copolymers.

[0195] Commercially available silicone surfactants include, for example, EXP.S-309-2, EXP.S-315, EXP.S-503-2, EXP.S-505-2, and S-506 (all manufactured by DIC Corporation); DOWSIL 8032 ADDITIVE, Toray Silicone DC3PA, Toray Silicone SH7PA, Toray Silicone DC11PA, Toray Silicone SH21PA, Toray Silicone SH28PA, Toray Silicone SH29PA, Toray Silicone SH30PA, and Toray Silicone SH8400 (all manufactured by Dow Corning Toray Co., Ltd.); X-22-4952, X-22-4272, and X-22-6266. , KF-351A, K354L, KF-355A, KF-945, KF-640, KF-642, KF-643, X-22-6191, X-22-4515, KF-6004, KF-6001, K F-6002, KP-101KP-103, KP-104, KP-105, KP-106, KP-109, KP-109, KP-112, KP-120, KP-121, KP-124, KP-125 , KP-301, KP-306, KP-310, KP-322, KP-323, KP-327, KP-341, KP-368, KP-369, KP-611, KP-620, KP-621, KP-626, and KP-652 (all manufactured by Shin-Etsu Silicones Co., Ltd.); F-4440, TSF-4300, TSF-4445, TSF-4460, and TSF-4452 (all manufactured by Momentive Perform BYK Materials; BYK300, BYK306, BYK307, BYK310, BYK320, BYK323, BYK325, BYK330, BYK313, BYK315N, BYK331, BYK333, BYK345, BYK347, BYK348, BYK349, BYK370, BYK377, BYK378, and BYK323 (all manufactured by BYK-Chemie).

[0196] The surfactant may also be a nonionic surfactant other than those mentioned above. Examples of surfactants include those described in paragraph 0017 of Japanese Patent No. 04502784 and paragraphs 0060 to 0071 of JP-A No. 2009-237362.

[0197] The surfactants may be used alone or in combination of two or more. The content of the surfactant is preferably from 0.01 to 3.0 mass %, more preferably from 0.05 to 1.0 mass %, and even more preferably from 0.1 to 0.8 mass %, based on the total solid content of the curable composition.

[0198] (rust inhibitor) The curable composition may also include a rust inhibitor. Examples of the rust inhibitor include heterocyclic compounds, such as triazole compounds, benzotriazole compounds, tetrazole compounds, thiadiazole compounds, triazine compounds, rhodanine compounds, thiazole compounds, benzothiazole compounds, benzimidazole compounds, benzoxazole compounds, pyrimidine compounds, and pyridine compounds, and triazole compounds, benzotriazole compounds, and tetrazole compounds are preferred. Examples of heterocyclic compounds include compounds described in WO 2022 / 039027.

[0199] The rust inhibitors may be used alone or in combination of two or more. The content of the rust inhibitor is preferably from 0.01 to 3.0 mass %, more preferably from 0.05 to 1.0 mass %, and even more preferably from 0.1 to 0.8 mass %, based on the total solid content of the curable composition.

[0200] (Other additives) The curable composition may contain other additives in addition to those described above. Examples of other additives include silane coupling agents, photoacid generators, curing agents, aliphatic thiol compounds, thermal crosslinking compounds, polymerization inhibitors, hydrogen donor compounds, solvents, impurities, sensitizers, alkoxysilane compounds, maleimide compounds, hydrosilylation agents, and chain transfer agents.

[0201] The curable composition may contain a solvent. The solvent is not particularly limited as long as it can dissolve or disperse various components other than the solvent that may be contained in the curable composition. Examples of the solvent include water, alkylene glycol ether solvents, alkylene glycol ether acetate solvents, alcohol solvents (e.g., methanol and ethanol), ketone solvents (e.g., acetone and methyl ethyl ketone), aromatic hydrocarbon solvents (e.g., toluene), aprotic polar solvents (e.g., N,N-dimethylformamide), cyclic ether solvents (e.g., tetrahydrofuran), ester solvents (e.g., n-propyl acetate), amide solvents, lactone solvents, and solvents containing two or more of these. The solvent may be used alone or in combination of two or more. The content of the solvent is preferably from 50 to 1900 parts by mass, more preferably from 100 to 1200 parts by mass, and even more preferably from 100 to 900 parts by mass, relative to 100 parts by mass of the total solid content of the curable composition.

[0202] Examples of the silane coupling agent include the components described in paragraphs 0299 ​​to 0300 of JP-A No. 2021-128183. Examples of the aliphatic thiol compound, the thermally crosslinkable compound, the polymerization inhibitor, and the hydrogen donor compound include various components described in WO 2022 / 039027. Examples of the sensitizer and alkoxysilane compound include the components described in paragraphs 0097 to 0119 of WO 2018 / 179640. Examples of maleimide compounds (compounds having a maleimide ring) include known maleimide compounds and the maleimide compounds described in WO 2022 / 102756. Examples of hydrosilylation agents include platinum catalysts such as platinum metal-supported carbon powder, platinum black, platinic chloride, chloroplatinic acid, reaction products of chloroplatinic acid and monohydric alcohols, complexes of chloroplatinic acid and olefins, and platinum group metal catalysts such as platinum bisacetoacetate; and palladium-based catalysts and rhodium-based catalysts. The hydrosilylation agent is preferably used as a curing agent when a silicone resin or a precursor thereof is used as the resin. As the chain transfer agent, known compounds can be used.

[0203] Second Embodiment <Second transfer film> The transfer film in the second embodiment (hereinafter also referred to as the "second transfer film") is a transfer film comprising a temporary support and a curable composition layer containing a resin, and the resin contained in the curable composition layer is oriented in the in-plane direction. It is believed that the resin contained in the curable composition layer is oriented in the in-plane direction, which reduces the linear expansion coefficient of the resulting cured layer in the in-plane direction when the second transfer film is used to form a cured layer on the substrate.

[0204] The second transfer film is similar to the first transfer film described above, except that it is not specified that the second transfer film is a film obtained by uniaxially or biaxially stretching the above-mentioned laminate, and it is specified that the resin contained in the curable composition layer is oriented in the in-plane direction, and the preferred embodiments are also similar. In the following description of the second transfer film, the main differences from the first transfer film will be described, and descriptions of parts that are the same as those of the first transfer film may be omitted.

[0205] The second transfer film may be a film obtained by uniaxially or biaxially stretching the above-mentioned laminate, similar to the first transfer film, but is not limited thereto.

[0206] (Temporary support) The temporary support in the second transfer film is a member that supports the cured layer. As the temporary support for the second transfer film, the temporary support precursor in the above-mentioned laminate itself may be used as the temporary support, or the temporary support in the above-mentioned first transfer film (i.e., a member obtained by stretching the above-mentioned temporary support precursor) may be used. When the temporary support contains a resin, the resin contained in the temporary support may be oriented in the in-plane direction of the temporary support.

[0207] (Curable composition layer) The curable composition layer in the second transfer film is not particularly limited as long as the resin contained therein is oriented in the in-plane direction of the curable composition layer, and examples thereof include a layer obtained by stretching the above-mentioned curable composition layer precursor. The various components contained in the curable composition layer of the second transfer film are the same as the various components contained in the curable composition layer precursor described above, and preferred embodiments are also the same. In addition, the average thickness of the curable composition layer of the second transfer film is preferably the same as that of the curable composition layer precursor.

[0208] The resin contained in the curable composition layer is oriented in the in-plane direction of the curable composition layer (specifically, in the direction intersecting the thickness direction of the curable composition layer in the cross section obtained when the second transfer film is cut along the thickness direction). The orientation state of the resin can be confirmed by the method described in the Examples section below. In the second transfer film, the resin contained in the curable composition layer may be oriented in the in-plane direction of the curable composition layer, and may have molecular orientation in a uniaxial direction in the plane of the curable composition layer, or may have random molecular orientation in the plane of the curable composition layer.

[0209] Here, as will be described later in the Examples section, whether or not the resin contained in the curable composition layer is oriented in the in-plane direction of the curable composition layer can be determined, for example, by using an orientation coefficient f xz In this case, the orientation coefficient f xzIf the ratio is 0.15 or more, it can be determined that the resin contained in the curable composition layer is oriented in the in-plane direction of the curable composition layer. Orientation coefficient f in the direction parallel to the in-plane direction of the curable composition layer xz The orientation coefficient f is preferably 0.30 or more, more preferably 0.50 or more, and particularly preferably 0.70 or more, in order to obtain better effects of the present invention. xz The upper limit of is 1. The orientation coefficient f xz The measurement method is as shown in the Examples section below.

[0210] (cover film) The second transfer film may further have a cover film, and in this case, it is preferable that the temporary support, the curable composition layer, and the cover film are laminated in this order. The cover film may be the above-mentioned cover film precursor itself, or a film obtained by stretching the above-mentioned cover film precursor may be used. The various components contained in the cover film of the second transfer film are the same as the various components contained in the cover film precursor, and the preferred embodiments are also the same. When the cover film contains a resin, the resin contained in the cover film may be oriented in the in-plane direction of the cover film.

[0211] (Intermediate layer and thermoplastic resin layer) The second transfer film may further have an intermediate layer and / or a thermoplastic resin layer. As the intermediate layer and / or thermoplastic resin layer in the second transfer film, the above-mentioned intermediate layer precursor and / or thermoplastic resin layer precursor may be used as the intermediate layer and / or thermoplastic resin layer, or a layer obtained by stretching the above-mentioned intermediate layer precursor and / or thermoplastic resin layer precursor may be used. When the second transfer film has an intermediate layer and / or a thermoplastic resin layer, the second transfer film preferably has the intermediate layer and / or the thermoplastic resin layer between the temporary support and the curable composition layer. The various components contained in the intermediate layer and thermoplastic resin layer in the second transfer film are the same as the various components contained in the intermediate layer precursor and thermoplastic resin layer precursor, and the preferred embodiments are also the same. When the intermediate layer in the second transfer film contains a resin, the resin contained in the intermediate layer may be oriented in the in-plane direction of the intermediate layer. When the thermoplastic resin layer in the second transfer film contains a resin, the resin contained in the thermoplastic resin layer may be oriented in the in-plane direction of the thermoplastic resin layer.

[0212] (high refractive index layer) The second transfer film may further have a high refractive index layer. As the high refractive index layer in the second transfer film, the above-mentioned high refractive index layer precursor itself may be used as the high refractive index layer, or a layer obtained by stretching the above-mentioned high refractive index layer precursor may be used. The various components contained in the high refractive index layer in the second transfer film are the same as the various components contained in the high refractive index layer precursor, and the preferred embodiments are also the same. When the high refractive index layer in the second transfer film contains a resin, the resin contained in the high refractive index layer may be oriented in the in-plane direction of the high refractive index layer.

[0213] (Application) The second transfer film is used in the same manner as the first transfer film.

[0214] <Method for manufacturing the second transfer film> The method for producing the second transfer film is not particularly limited, but may be, for example, the same method as the method for producing the first transfer film described above.

[0215] [Method of manufacturing hardened layer] The method for producing the cured layer of the present invention comprises: a step of transferring the curable composition layer in the first transfer film or the second transfer film onto a transfer target (hereinafter also referred to as step A); and a step of curing the transferred curable composition layer to form a cured layer (hereinafter also referred to as step B). Each step of the method for producing the hardened layer will be described in detail below.

[0216] [Process A] Step A is a step of transferring the curable composition layer in the first transfer film or the second transfer film onto an object to be transferred. In the following description, the first transfer film and the second transfer film are collectively referred to as transfer films. Step A is preferably a step of bringing the surface of the curable composition layer in the transfer film opposite to the temporary support side into contact with the transfer target, and laminating the transfer film and the transfer target. Examples of methods for laminating the transfer film include known transfer methods and methods using known laminators such as laminators, vacuum laminators, and auto-cut laminators, and methods involving pressure and heat application using rolls or the like are preferred. The lamination temperature is preferably 70 to 130°C. Furthermore, when the transfer film has a cover film, step A is preferably carried out after the cover film has been peeled off from the transfer film.

[0217] <Transcribed material> Examples of the substrate to which the transfer is to be performed include a glass substrate, a glass epoxy substrate, a silicon substrate, a resin substrate, and a substrate having a conductive layer, with a substrate having a conductive layer being preferred. The refractive index of the transfer target is preferably 1.50 to 1.52.

[0218] The transfer target may be a light-transmitting substrate such as a glass substrate, and may be, for example, tempered glass such as Gorilla Glass manufactured by Corning Inc. Examples of materials contained in the transfer target include materials described in JP-A-2010-086684, JP-A-2010-152809, and JP-A-2010-257492.

[0219] The resin substrate is preferably a resin film with small optical distortion and / or high transparency, such as polyester, polyethylene terephthalate (PET), polyethylene naphthalate, polycarbonate, triacetyl cellulose, cycloolefin polymer, and polyimide.

[0220] As the substrate having a conductive layer, a resin substrate having a conductive layer is preferred, and a resin film having a conductive layer is more preferred, in that it can be produced by a roll-to-roll method.

[0221] Examples of the conductive layer include known conductive layers used for circuit wiring or touch panel wiring. From the viewpoints of conductivity and fine line formability, the conductive layer is preferably one or more layers selected from the group consisting of a metal layer (e.g., metal foil), a conductive metal oxide layer, a graphene layer, a carbon nanotube layer, and a conductive polymer layer, more preferably a metal layer, and even more preferably a copper layer or a silver layer. The conductive layer may be one or more layers. The conductive layer may be used alone or in combination of two or more types. Examples of materials for the conductive layer include elemental metals and conductive metal oxides. Examples of elemental metals include Al, Zn, Cu, Fe, Ni, Cr, Mo, Ag, and Au. Examples of conductive metal oxides include ITO (Indium Tin Oxide), IZO (Indium Zinc Oxide), and SiO2. The conductivity is determined by the volume resistivity of 1×10 6 This means that the volume resistivity is less than 1×10 4 It is preferably less than Ωcm.

[0222] The conductive layer may be patterned. Examples of methods for producing a patterned conductive layer include etching methods (e.g., subtractive methods and additive methods). Examples of etching methods include wet etching methods described in paragraphs 0048 to 0054 of JP 2010-152155 A and known dry etching methods such as plasma etching. The etching method may also be a method using an etching resist.

[0223] [Process B] Step B is a step of curing the curable composition layer transferred to the transfer-receiving object to form a cured layer. The method for curing the curable composition layer is appropriately determined depending on the types of components contained in the curable composition, and examples thereof include a method of heating the curable composition layer and a method of exposing the curable composition layer when the curable composition layer contains a photosensitive component. Alternatively, both heating and exposure may be performed.

[0224] When the curable composition layer contains a photosensitive component, step B may be a step of subjecting the curable composition layer to patterned exposure and then performing a development treatment to obtain a patterned cured layer (hereinafter also referred to as step B-1). "Pattern exposure" refers to a form of patterned exposure, i.e., exposure in a form in which exposed areas and unexposed areas are present. The positional relationship between the exposed areas and unexposed areas in patterned exposure is not particularly limited and may be adjusted as appropriate. The patterned exposure may be performed from the side opposite the curable composition layer to the transfer target, or from the side of the curable composition layer to the transfer target.

[0225] The light source used for exposure may be any light source that irradiates light in a wavelength range (e.g., light in wavelength ranges of 254 nm, 313 nm, 365 nm, and 405 nm) to which various photosensitive components (e.g., photopolymerization initiator, photoacid generator, etc.) in the curable composition layer are sensitive. Specific examples of such light sources include ultra-high pressure mercury lamps, high pressure mercury lamps, metal halide lamps, and LEDs (light emitting diodes). The exposure dose is 5 to 2000 mJ / cm 2 is preferred, and 10 to 1000 mJ / cm 2 is more preferred.

[0226] In step B-1, pattern exposure may be performed after peeling off the temporary support from the curable composition layer, or pattern exposure may be performed through the temporary support before peeling off the temporary support, and then the temporary support may be peeled off. In order to prevent mask contamination due to contact between the curable composition layer and the mask and to avoid the influence of foreign matter attached to the mask on the exposure, it is preferable to perform pattern exposure without peeling off the temporary support. Note that the pattern exposure may be exposure through a mask or direct exposure using a laser or the like. Examples of the mask include a quartz mask, a soda lime glass mask, and a film mask. A quartz mask is preferred because of its excellent dimensional accuracy, and a film mask is preferred because it can be easily made into a large size. The material of the film mask is preferably a polyester film, more preferably a polyethylene terephthalate film, for example, XPR-7S SG (manufactured by Fujifilm Global Graphic Systems Co., Ltd.).

[0227] The development treatment in step B-1 is carried out using, for example, a developer. Examples of the developer include an alkaline developer and an organic solvent developer.

[0228] The alkaline developer is preferably an alkaline aqueous solution. The alkaline aqueous solution is preferably a solution containing a compound having a pKa of 7 to 13 at a concentration of 0.05 to 5 mol / L. The water content in the alkaline developer is preferably 50% by mass or more, more preferably 60% by mass or more, even more preferably 85% by mass or more, particularly preferably 90% by mass or more, and most preferably 95% by mass or more, based on the total mass of the alkaline developer. The upper limit is preferably less than 100% by mass, based on the total mass of the alkaline developer. Examples of alkaline developers include aqueous sodium carbonate solutions, aqueous potassium carbonate solutions, aqueous sodium hydroxide solutions, aqueous potassium hydroxide solutions, and aqueous tetramethylammonium hydroxide (TMAH) solutions. The concentrations of the alkaline components constituting the alkaline developers include, for example, 0.1% by mass aqueous solutions, 1.0% by mass aqueous solutions, and 2.38% by mass aqueous solutions. The alkaline developer may also contain a water-soluble organic solvent, a surfactant, etc. Examples of the alkaline developer include the developer described in paragraph 0194 of WO 2015 / 093271.

[0229] Examples of organic solvent developers include developers containing organic solvents such as ketone solvents, ester solvents, alcohol solvents, amide solvents, ether solvents, and hydrocarbon solvents. As the organic solvent developer, cyclopentanone or propylene glycol monomethyl ether acetate is preferred, and cyclopentanone is more preferred. In the organic solvent developer, a plurality of organic solvents may be mixed, or may be mixed with an organic solvent other than those mentioned above or water. The content of water in the organic solvent developer is preferably less than 10% by mass, more preferably substantially free of water, based on the total mass of the organic solvent developer. The content of organic solvent in the organic solvent developer is preferably 50% by mass or more, more preferably 60% by mass or more, even more preferably 85% by mass or more, particularly preferably 90% by mass or more, and most preferably 95% by mass or more, based on the total mass of the organic solvent developer. The upper limit is preferably 100% by mass or less, based on the total mass of the organic solvent developer.

[0230] Examples of development methods include puddle development, shower development, spin development, and dip development. In shower development, unnecessary portions can be removed by spraying a developer onto the composition layer after exposure. It is also preferable to spray a detergent or the like onto the layer after development and remove development residues by scrubbing with a brush or the like. The temperature of the developer is preferably 20 to 40°C.

[0231] In step B-1, a heat treatment may be carried out after the development treatment, which promotes the reaction of the resin precursor (for example, the ring-closing reaction of the polyimide precursor) to form a resin. The temperature and time of the heat treatment can be appropriately selected depending on the type of resin and its precursor. The temperature for the heat treatment is preferably 120 to 400°C, more preferably 150 to 400°C, and even more preferably 180 to 350°C. The heat treatment time is preferably 1 to 24 hours, more preferably 1 to 12 hours, and even more preferably 1 to 9 hours. The heat treatment may be carried out in either an air environment or a nitrogen-substituted environment. The atmospheric pressure in the heat treatment environment is preferably 8.1 kPa or more, more preferably 50.66 kPa or more, and the upper limit is preferably 121.6 kPa or less, more preferably 111.46 kPa or less, and even more preferably 101.3 kPa or less.

[0232] The patterned cured layer refers to a state in which a pattern is formed on the cured layer. Examples of the pattern include a pattern having vias and linear grooves for forming wiring. The pattern having vias may be either through holes or via holes. The shape of the vias in the pattern can be, for example, a square, trapezoid, or inverted trapezoid in cross-sectional shape; and a circle or square in front shape (the shape of the via when observed from the direction where the via bottom is visible). An inverted trapezoid is preferred as the cross-sectional shape because it improves the adhesion of plated copper to the via wall surface. The via size (diameter) is preferably 300 μm or less, more preferably 100 μm or less, even more preferably 50 μm or less, and particularly preferably 5 μm or less. The lower limit is preferably 0.01 μm or more. The number of vias may be one or two or more, and is preferably two or more.

[0233] The cross-sectional shape of the linear grooves (a cross section intersecting the extension direction of the grooves and along the height direction of the grooves) may be a quadrangle (including a trapezoid). The diameter (width) of the linear groove is preferably 50 μm or less, more preferably 20 μm or less, and even more preferably 5 μm or less. The lower limit is preferably 0.01 μm or more.

[0234] The cured layer (patterned cured layer) is preferably used as an insulating film for a semiconductor package.

[0235] [Process C] The method for producing a cured film of the present invention may include a step of subjecting the cured layer to laser processing to obtain a patterned cured layer after step B. Here, step C may be performed, for example, when a patterned cured layer is not formed in step B (for example, when step B-1 is not employed). The laser processing method is not particularly limited, and any known method can be used. The patterned cured layer obtained in step C is similar to the patterned cured layer described in step B above.

[0236] [Other processes] The method for producing the cured layer may include other steps in addition to those described above. Other steps include, for example, the following steps:

[0237] <Cover film peeling process> In the method for producing a cured layer, when the transfer film has a cover film, it is preferable to include a step of peeling off the cover film of the transfer film (cover film peeling step). As the method for peeling off the cover film, a known method can be applied. The cover film peeling step is preferably carried out before step A.

[0238] [Semiconductor package manufacturing method] The method for manufacturing a semiconductor package of the present invention includes the method for manufacturing the hardened layer described above, and preferably further includes a step of forming a circuit pattern on the hardened layer described above. In the step of forming a circuit pattern, the cured layer on which the circuit pattern is to be formed is preferably the above-described patterned cured layer. The method for forming the circuit pattern is not particularly limited, but a semi-additive process is preferred because it allows for the formation of fine wiring. For example, in the semi-additive process, a seed layer is first formed by electroless copper plating using a palladium catalyst or the like on the via bottoms, via wall surfaces, and the entire surface of a pattern having vias. The seed layer is for forming a power supply layer for electrolytic copper plating, and the thickness of the seed layer is preferably 0.1 to 2.0 μm. If the thickness of the seed layer is 0.1 μm or more, it tends to be possible to suppress a decrease in connection reliability during electrolytic copper plating, and if the thickness of the seed layer is 2.0 μm or less, it is not necessary to increase the etching amount when flash etching the seed layer between wirings, and it tends to be possible to suppress damage to the wiring during etching. Electroless copper plating is performed by reacting copper ions with a reducing agent to deposit metallic copper on the surface of a via-containing pattern. Examples of electroless plating methods and electrolytic plating methods include known plating methods. The catalyst for the electroless plating treatment is preferably a palladium-tin mixed catalyst. The average primary particle size of the mixed catalyst is preferably 10 nm or less. The plating solution for the electroless plating treatment preferably contains hypophosphorous acid (reducing agent). Examples of electroless copper plating solutions include "MSK-DK" manufactured by Atotech Japan and "ThruCup (registered trademark) PEA ver. 4" series manufactured by Uemura Kogyo Co., Ltd.

[0239] When the pattern formed on the cured layer has vias, the method for manufacturing a semiconductor package may include a roughening step of roughening the pattern having vias. The roughening step is preferably performed before the step of forming a circuit pattern. By carrying out the roughening step, the surface of the pattern can be roughened to improve adhesion to the circuit wiring, and smears can also be removed at the same time. The roughening step may be, for example, a known desmear treatment, and is preferably a treatment in which a roughening solution is brought into contact with the surface. Examples of the roughening solution include a roughening solution containing chromium and sulfuric acid, a roughening solution containing alkaline permanganate (for example, a sodium permanganate roughening solution), and a roughening solution containing sodium fluoride, chromium, and sulfuric acid.

[0240] It is preferable to carry out a heat treatment after forming the circuit pattern, in order to improve the electrical insulation reliability, hardening characteristics, and adhesive strength with plated copper. The heating temperature is preferably 150 to 240° C., and the heating time is preferably 15 to 500 minutes. [Example]

[0241] The present invention will be described in more detail below with reference to examples. The materials, amounts used, ratios, treatment details, and treatment procedures shown in the following examples can be changed as appropriate without departing from the spirit of the present invention. Therefore, the scope of the present invention should not be construed as being limited by the examples shown below.

[0242] [Preparation of Curable Composition 1] A mixture was prepared by mixing various components in the amounts shown below (amounts based on solid content). Next, the mixture was diluted with a mixed solvent containing 25% by mass of MEK (methyl ethyl ketone) and 75% by mass of NMP (N-methyl-2-pyrrolidone) to a solid content of 30% by mass. In this way, curable composition 1 was obtained. Note that curable composition 1 is a so-called photosensitive composition containing a photosensitive component. ---------------------------------------------------------------------------------- Composition of curable composition 1 ---------------------------------------------------------------------------------- Polyimide precursor A-1 (see formula below) 82.0 parts by mass SR205NS (Sartomer) 7.2 parts by weight TR-HABI 101 (Tronly, photopolymerization initiator) 6.3 parts by mass Compound D-1 (see formula below, chain transfer agent) 0.5 parts by mass MEHQ (4-methoxyphenol) 0.3 parts by mass EAB-F (4,4'-bis(diethylamino)benzophenone, sensitizer) 0.1 part by mass Compound G-1 (see formula below, thermal base generator) 1.7 parts by mass HAT (5-amino-1H-tetrazole, rust inhibitor) 0.3 parts by mass Compound J-1 (see formula below) 1.6 parts by mass ----------------------------------------------------------------------------------

[0243] Polyimide precursor A-1 [ka]

[0244] Compound D-1 [ka]

[0245] Compound G-1 [ka]

[0246] Compound J-1 [ka]

[0247] <Method for synthesizing polyimide precursor A-1> 4,4'-Oxydiphthalic anhydride (dried at 140°C for 12 hours, 20.0 g, 64.5 mmol), 2-hydroxyethyl methacrylate (16.8 g, 129 mmol), hydroquinone (0.05 g), pyridine (20.4 g, 258 mmol), and diethylene glycol dimethyl ether (100 g) were mixed and stirred at 60°C for 18 hours to obtain a reaction mixture (a diester of 4,4'-oxydiphthalic acid and 2-hydroxyethyl methacrylate). The resulting diester was then chlorinated using thionyl chloride (SOCl2), to obtain a reaction mixture. Next, a solution of 4,4'-diaminodiphenyl ether (11.08 g, 58.7 mmol) in N-methylpyrrolidone (100 mL) was added dropwise to the reaction mixture over 20 minutes at -5 to 0°C. After reacting the reaction mixture at 0°C for 1 hour, ethanol (70 g) was added and the mixture was stirred at room temperature for 1 day. The resulting reaction solution was added to water (5 L) and stirred at 5,000 rpm for 15 minutes to obtain a crude polymer precipitate. The precipitate collected by filtration from the mixture was stirred in water (3 L) for 30 minutes and collected by filtration again. The resulting precipitate was dried under reduced pressure at 45°C for 3 days to obtain polyimide precursor A-1. The weight average molecular weight (Mw) of the polyimide precursor A-1 was 18,000, and the acid value was 0 mgKOH / g.

[0248] The acid value of Polyimide Precursor A-1 was determined according to JIS K0070 by dissolving 0.1 g of the synthesized Polyimide Precursor A-1 in 20 ml of NMP and titrating with KOH using thymolphthalein as an indicator.

[0249] [Example 1] The prepared curable composition 1 was applied to a temporary support precursor (Oji F-Tex Co., Ltd., polypropylene film, FG-201, thickness 30 μm) and dried at 100° C. to form a curable composition layer precursor, thereby obtaining a laminate 1 in which the temporary support precursor and the curable composition layer precursor were laminated in this order. The curable composition 1 was applied so that the film thickness of the curable composition layer precursor would be 30 μm after drying. Thereafter, the four sides of the laminate 1 were fixed, and the laminate was stretched in the horizontal direction to 1.5 times its original length in a thermostatic chamber at 40°C, and then sequentially stretched in the vertical direction to 1.5 times its original length. Next, a cover film (Oji F-Tex Co., Ltd., polypropylene film, FG-201, thickness 30 μm) was attached to the side of the curable composition layer precursor opposite the temporary support precursor, thereby obtaining a transfer film of Example 1. The transfer film of Example 1 is a film in which a temporary support, a curable composition layer, and a cover film are laminated in this order.

[0250] [Comparative Example 1] A transfer film of Comparative Example 1 was obtained in the same manner as in Example 1, except that the laminate 1 was not stretched. The transfer film of Comparative Example 1 is a film in which a temporary support precursor, a curable composition layer precursor, and a cover film are laminated in this order.

[0251] [Check orientation] Using samples (sample size: 2 cm square) obtained by peeling off the cover film from the transfer film of each of the examples and comparative examples, the orientation direction of the polyimide precursor was confirmed by polarized ATR-IR spectroscopy as follows. The measurement was carried out using a Nicolet is50 manufactured by Thrmo Scientific under the following conditions. Prism: Germanium Pressure between prism and sample: 20cN m Incident angle: 45° Number of reflections: 1 Resolution: 4cm -1

[0252] Measurement was carried out after confirming that the sample was in sufficient contact with the entire surface of the prism. The FTIR-ATR spectrum was measured by irradiating perpendicular polarized light (s-polarized light; transverse electric wave, TE wave) and horizontal polarized light (p-polarized light; transverse magnetic wave, TM wave) onto the incident plane consisting of light incident on the sample surface (surface of the curable composition layer or the precursor of the curable composition layer) and light reflected from the surface using a wire grid polarizer. The absorption spectrum when perpendicular polarized light was incident was measured. TE , the absorption spectrum when horizontally polarized light is incident is S TM It was decided. The obtained spectrum was subjected to atmospheric correction so that the signal derived from water vapor was below the noise level.

[0253] <Calculation of absorbance (peak area)> S TE and S TM In each spectrum, 1480-1510 cm -1 The area A enclosed by the spectrum and the baseline for a peak with a maximum absorption point in the range TE , area A TM was calculated.

[0254] <orientation factor f xz Calculation of> Area A TE , area A TM Using the above, the absorption coefficient k is calculated based on the equations described in paragraphs 0039 to 0043 of JP-A-2004-126109. x and k z was calculated. Infrared dichroic ratio D xz =k x / k z is an orientation coefficient f in a direction parallel to a direction intersecting the thickness direction of the curable composition layer or the curable composition layer precursor in a cross section along the thickness direction of the sample (i.e., an in-plane direction of the curable composition layer or the curable composition layer precursor), xz was calculated using the following formula:

number

[0255] where:

number

[0256] <Evaluation criteria> 0.15≦f xz If the condition is satisfied, it is determined that the orientation is in-plane, and 0≦f xz When the value was <0.15, it was determined to be randomly oriented.

[0257] As a result of the measurement, it was confirmed that the polyimide precursor was randomly oriented in the sample of Comparative Example 1, whereas the polyimide precursor was oriented in the in-plane direction of the curable composition layer in the sample of Example 1.

[0258] [Evaluation of the thermal expansion coefficient of the cured film] The cover film was peeled off from the transfer film of Example 1 and the transfer film of Comparative Example 1. Next, a copper-clad polyimide film (Metalloyal, manufactured by Toray Industries, Inc.) was used as the transfer substrate, and the transfer film of Example 1 or the transfer film of Comparative Example 1 after the cover film had been peeled off was transferred and laminated onto the transfer substrate, thereby obtaining a laminate having a 30.0 μm thick curable composition layer (curable composition layer precursor when the transfer film of Comparative Example 1 was used) on the transfer substrate. Note that the laminate obtained using the transfer film of Example 1 has the transfer substrate / curable composition layer / temporary support laminated in this order. Also, the laminate obtained using the transfer film of Comparative Example 1 has the transfer substrate / curable composition layer precursor / temporary support precursor laminated in this order. The obtained laminate was exposed to light (high-pressure mercury lamp, cumulative illuminance of 300 mJ / cm measured with an illuminometer at a wavelength of 365 nm) from the side opposite to the side of the object to which the curable composition layer (curable composition layer precursor when the transfer film of Comparative Example 1 was used) was transferred. 2 ), the temporary support was peeled off, and the film was then heated in an oven (200°C, 100 minutes), immersed in 2 M hydrochloric acid for 8 hours for a peeling treatment, rinsed (in pure water at room temperature for 1 hour), and then peeled off from the substrate to obtain a free-standing film (cured film) derived from the curable composition layer (curable composition layer precursor when the transfer film of Comparative Example 1 was used). Note that if the free-standing film could not be peeled off by the above peeling treatment, it was further immersed in 2 M hydrochloric acid for about a week and peeled off. The obtained free-standing film was cut into strips to prepare measurement samples. The freestanding film was cut into strips (19 mm x 5 mm) and the in-plane linear expansion coefficient was measured using a TMA (thermomechanical analyzer, TA Instruments "TMA450EM"). The measurement conditions were a heating rate of 10°C / min, a chuck distance of 20 mm, and a load of 45 mN. The in-plane linear expansion coefficient was measured as a value (ppm / K) in the temperature range of 50 to 150°C during heating, and was calculated as the average of three measurements. The results are shown in Table 1.

[0259] [Table 1]

[0260] As shown in Table 1, when a transfer film made by stretching the laminate was used (Example 1), it was shown that a cured layer with a small linear expansion coefficient in the in-plane direction could be transferred onto the object to be transferred, compared to when a transfer film made by not stretching the laminate was used (Comparative Example 1). Furthermore, as shown in Table 1, when a transfer film in which the orientation direction of the resin in the curable composition layer is the in-plane direction of the curable composition layer was used (Example 1), it was shown that a cured layer with a small linear expansion coefficient in the in-plane direction could be transferred to the object to be transferred, compared to when a transfer film in which the orientation direction of the resin in the layer corresponding to the curable composition layer is random (Comparative Example 1).

[0261] [Confirmation of hardening] A copper-clad polyimide film (Metalloyal, manufactured by Toray Industries, Inc.) was used as the substrate, and the transfer film of Example 1 after peeling off the cover film was laminated onto the substrate to obtain a laminate having the substrate / curable composition layer / temporary support. The obtained laminate was exposed from the temporary support side through a mask having a pattern of L / S (line / space) = 100 / 100 (μm / μm) (high-pressure mercury lamp, cumulative illuminance 0 to 1000 mJ / cm measured with an illuminometer at a wavelength of 365 nm). 2 at 5mJ / cm 2 The temporary support was peeled off 30 minutes after the exposure, and the obtained sample was immersed in cyclopentanone at 23°C for 120 seconds, and then in PGMEA (propylene glycol monomethyl ether acetate) at 23°C for 30 seconds to remove the unexposed areas and form a pattern. The resulting L / S=100 / 100 μm pattern was observed using an optical microscope, and the exposure dose at which the line width of the pattern was closest to the line width of the mask (100 μm) was determined to be the optimum exposure dose.

[0262] Next, the laminate having the above-mentioned substrate / curable composition layer / temporary support was exposed (high-pressure mercury lamp, the above-mentioned optimal exposure amount) through a mask having an L / S=15 / 15 (μm / μm) pattern from the temporary support side. 30 minutes after the exposure, the temporary support was peeled off, and the obtained sample was immersed in cyclopentanone at 23°C for 120 seconds, and then in PGMEA at 23°C for 30 seconds to obtain a patterned sample with L / S=15 / 15 (μm / μm). From the above, it was confirmed that the curable composition layer of the transfer film of Example 1 was photocurable.

Claims

1. A transfer film comprising a temporary support and a curable composition layer, which is obtained by uniaxially or biaxially stretching a laminate comprising a temporary support precursor and a curable composition layer precursor containing a resin.

2. the laminate includes the temporary support precursor, the curable composition layer precursor, and the cover film precursor in this order; The transfer film according to claim 1 , comprising the temporary support, the curable composition layer, and a cover film in this order.

3. A transfer film comprising a temporary support and a curable composition layer containing a resin, A transfer film in which the resin contained in the curable composition layer is oriented in an in-plane direction.

4. the temporary support comprises a resin, The transfer film according to claim 3 , wherein the resin contained in the temporary support is oriented in an in-plane direction.

5. 4. The transfer film according to claim 3, wherein the resin contained in the curable composition layer comprises at least one selected from the group consisting of a polyimide precursor, a silicone resin, an epoxy resin, a polyimide resin, a polyamide resin, a maleimide resin, and a polyphenylene ether resin.

6. The transfer film according to claim 3 , comprising the temporary support, the curable composition layer, and a cover film in this order.

7. A method for producing a transfer film, comprising uniaxially or biaxially stretching a laminate including a temporary support precursor and a curable composition layer precursor containing a resin, to obtain a transfer film including the temporary support and the curable composition layer.

8. the laminate includes the temporary support precursor, the curable composition layer precursor, and the cover film precursor in this order; The method for producing a transfer film according to claim 7 , wherein the transfer film has the temporary support, the curable composition layer, and the cover film in this order.

9. a step of transferring the curable composition layer in the transfer film according to claim 1 or 3 onto a transfer target; and curing the curable composition layer transferred onto the transfer target to form a cured layer.

10. The method for producing a cured layer according to claim 9 , wherein the step of forming the cured layer is a step of subjecting the curable composition layer to patterned exposure and then performing a development treatment to obtain a patterned cured layer.

11. The method for producing a cured layer according to claim 10 , wherein the patterned cured layer is obtained by performing a heat treatment after the development treatment.

12. The method for producing a cured layer according to claim 9 , further comprising the step of performing laser processing on the cured layer to obtain a patterned cured layer.

13. A method for manufacturing a semiconductor package, comprising the method for manufacturing a hardened layer according to claim 9.

Images