TW200817838A - Photosensitive resin composition for interlayer insulation film and forming method of interlayer insulation film - Google Patents

Abstract

An objective of the invention is to provide a photosensitive resin composition for interlayer insulation films capable of forming a pattern having a higher resolution. The photosensitive resin composition for interlayer insulation films comprises an alkali-soluble resin component (A) and a photosensitizing agent (B), wherein the component (A) comprises a copolymer (A1) comprising a phenolic hydroxyl group-containing constitutional unit (a1) and a crosslinkable group-containing constitutional unit (a2), and the component (B) comprises a compound obtained by condensing a quinonediazide group-containing compound and a phenolic hydroxyl group-containing compound, in which R0 represents hydrogen or methyl, R1 represents single bond or C1 to C5 alkylene, R2 represents C1 to C5 alkyl, a represents an integer of 1 to 5, b represents 0 or an integer of 1 to 4, a+b is lower than 5, moreover, when there are more than two R2, the R2s can be the same or different. A resist pattern obtained from the photosensitive resin composition for interlayer insulation films has a resolution of ≤ 2 μm.

Description

[Technical Field] The present invention relates to a photosensitive resin composition for an interlayer insulating film and a method for forming an interlayer insulating film. [Prior Art] In the past, an interlayer insulating film was formed in an electronic component such as a liquid crystal display device, an integrated circuit device, or a solid-state imaging device. The interlayer insulating film is provided to insulate between wirings arranged in a layered manner. The interlayer insulating film is formed using a photosensitive resin composition (for example, refer to Patent Documents 1, 2, and 3). For example, a TFT (Thin Film Transistor) type liquid crystal display device can be generally manufactured in the following order. A polarizing plate was placed on the glass substrate, and a transparent conductive circuit layer and a TFT were formed, and then an interlayer insulating film was used to cover the back surface plate.

In the case of providing a polarizing plate on a glass substrate and forming a pattern of a black matrix and a color filter, a transparent conductive circuit layer and a layer film are formed in this order to manufacture a surface plate. Then, the back panel and the surface panel are opposed to each other with a spacer interposed therebetween, and liquid crystal is sealed between the two sheets to manufacture a tft type liquid crystal display device. The interlayer insulating film is usually %' and exposed, developed to form a pattern, and the interlayer insulating film is required to have good chemical properties and pattern contours, and 'in order to form the interlayer insulating film to form an interlayer insulating film, it is necessary to have an upper layer. It is formed by coating a photosensitive resin composition to thermally harden the pattern. It has various properties such as transparency, heat resistance, flatness, and resolution. The photosensitive resin composition, as escape characteristics and imaging properties, sensitivity, etc. 5 200817838 Intermediary, also various characteristics. x Requires that the above-mentioned photosensitive resin composition does not cause deterioration of σ σ quality (especially long-term stability of viscosity) even if it is stored for a long period of time, that is, it requires high storage stability of β [Patent Document 1 1 lack of i] Japanese Patent Laid-Open Publication No. Hei. No. Hei. No. Hei. No. 2000-62180.

In the case of the photosensitive resin composition described in the documents 1 to 3, the resin warfare contained in the photosensitive resin composition described in the documents 1 to 3 has the development, resolution, and sensitivity. Degree and other issues. 'The above-mentioned salty (five) t 4 precursor resin composition, because of the high temperature baking step during heat hardening, especially when such high temperature baking is performed, the transparency of the interlayer insulating M ^ deep film obtained may be low. The situation. In the photosensitive compositions of Patent Documents 1 to 3, it is difficult to form a pattern of a good pattern contour of the barrier (interlayer insulating film), and as time passes, a viscosity rises, etc., and the child's ambiguity is insufficient, and The chemical resistance or the resolution of the interlayer insulating film is also insufficient. Further, when the pattern is formed by using the photosensitive composition, it is difficult to suppress the film reduction of the formed pattern in the development step if the development liquid is not diluted, and there is a problem in the work efficiency direction. . Therefore, the concentration of the developing solution must be adjusted before the developing step. In view of the above-mentioned problems, the object of the present invention is to provide a photosensitive resin composition for an interlayer insulating film which can provide a higher resolution, and in particular to provide a photosensitive resin composition for an interlayer insulating film of 6 200817838, which can provide a high temperature even at a high temperature. The baking step does not cause thermal decomposition and has a high transparency of the interlayer insulating film; and provides a photosensitive resin composition for an interlayer insulating film capable of forming a pattern having a better contour and having high chemical resistance; A photosensitive resin composition for an interlayer insulating film having a higher storage stability; and a photosensitive resin composition for an interlayer insulating film which is excellent in developability using a general-purpose developing solution, and an interlayer insulating film [Formulation Method 0] [Means for Solving the Problem] The present inventors have found that a photosensitive resin composition for an interlayer insulating film which can solve the above problems can be provided by using a copolymer having a specific unit in an alkali-soluble resin component. The present invention has been completed. The first aspect of the present invention is a photosensitive resin composition for an interlayer insulating film, comprising a photosensitive resin composition for an interlayer insulating film of an alkali-soluble resin component (A) and a photosensitive agent (B), wherein the alkali solubility is The resin component (A) contains a copolymer (A1) containing a structural unit (al) represented by the following formula (a-Ι) and a structural unit U2) having a crosslinkable group, [ Chemical formula 1]

(R2)b (〇H)a (a-1) 200817838 [In the above formula, R0 represents a hydrogen atom or a methyl group, R1 represents a single bond or an alkylene group having a hindrance of 1 to 5, and R2 represents a hindrance An alkyl group having a number of 1 to 5, a represents an integer of 1 to 5, b represents an integer of 〇 or 1 to 4, a + b is 5 or less, and when there are two or more R 2 systems, the R 2 may mutually Different, can be the same]. Further, in the present invention, the "structural unit" means a monomer unit constituting a polymer. The second aspect of the present invention is a photosensitive resin composition for an interlayer insulating film, which is a photosensitive resin composition for an interlayer insulating film used in a method for forming an interlayer insulating film, and the method for forming the interlayer insulating film includes Step: a coating step of coating a photosensitive resin composition on a substrate, and an exposure step for selectively exposing the photosensitive resin composition after coating; & imaging using an alkali developing solution after exposure The photosensitive resin composition for an interlayer insulating film contains an alkali-soluble resin component (A) and a photosensitive agent (B), and the alkali-soluble resin component (A) contains a copolymer (A1), and the copolymer (A 1) a structural unit (a) containing a phenolic hydroxyl structural unit and a structural unit (a2) containing an epoxy structural unit, and the sensitizing agent (B) is a compound derived from a benzoquinonediazide-based compound, In the development step, when the image is developed by a 2.38 mass% aqueous solution of tetramethylammonium hydroxide, the dissolution rate of the unexposed portion is 10 nm/sec or less, and the dissolution rate of the exposed portion is 1 〇N/sec or more.The third aspect of the present invention is a photosensitive resin composition for an interlayer insulating film, which comprises a photosensitive resin composition for an interlayer insulating film of a soluble resin component (A) and a photosensitive agent (B), wherein the alkali solubility is Resin component 8 200817838 (A) contains a copolymer (Al) containing a right/3 structural unit (al) having a phenolic hydroxyl structural unit, and a crosslinkable ... The structure is earlier (a2), and the photosensitive resin composition for the interlayer insulating film is used for the photoresist layer, and the sidewall angle of the photoresist pattern is from 4 5 degrees to 90 degrees.

A fourth aspect of the present invention is a photosensitive resin composition for an interlayer insulating film, which comprises a photosensitive resin composition for an interlayer insulating film of a soluble resin component (A) and a photosensitive agent (B), wherein the precursor resin Soluble resin component (A) contains copolymer (A1) 'The copolymer (A1) contains a structural unit (al) having a phenolic hydroxyl structural unit, and a structural unit (a2) having a crosslinkable group, and the aforementioned photosensitive The agent (B) contains a compound obtained by condensing a benzoquinonediazide-based compound and a sulfhydryl group-containing compound, and the resolution of the photoresist pattern obtained by using the photosensitive resin composition for an interlayer insulating film is 2 microns or less. The fifth aspect of the present invention is a photosensitive resin composition for an interlayer insulating film, comprising a photosensitive resin composition for an interlayer insulating film of an alkali-soluble resin component (A) and a photosensitive agent (B), wherein the alkali solubility is The resin component (A) contains a copolymer (A1) containing only a phenolic hydroxyl structural unit represented by the general formula (ai) as a structural unit (al) containing an acidic structural unit, and contains The structural unit (a2) represented by the general formula (a-2) is used as another structural unit, [Chemical Formula 2] 9 200817838

(a-2)

[In the above formula, RG represents a hydrogen atom or a fluorenyl group, R1 represents an alkylene group having a single bond carbon number of 1 to 5, R2 represents an alkyl group having 1 to 5 carbon atoms, and R3 represents a hydrogen atom or a methyl group. a is an integer of 1 to 5, b is an integer of 0 or 1, and a + b is 5 or less. When two or more R2 systems are present, the R2 may be different from each other or may be the same. Moreover, the present invention also provides a method for forming an interlayer insulating film, which is a method for forming an interlayer insulating film comprising the steps of: applying a coating step of coating an insensitive resin composition on a substrate; and selecting a photosensitive resin composition after coating Exposure step of exposure to the ground; and development step of using alkali development imaging after exposure; wherein the photosensitive resin composition contains an alkali-soluble resin component (A), and the alkali-soluble resin component (A) contains copolymerization (A1) The copolymer (A1) contains a structural unit (al) represented by the following formula (a-Ι), and a structure (a2) having a crosslinkable group, and the developing solution of the above-mentioned developing step A tetraammonium hydroxide aqueous solution having a concentration of 1% by mass or more and 3% by mass or less is used. Or the light-soluble substance of the coating light group of ～4, etc. 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 2008 Further, it is preferable to obtain a photosensitive resin composition for an interlayer insulating film which can provide an interlayer insulating film having higher transparency than before. Further, according to the second aspect of the present invention, it is possible to provide a photosensitive resin composition for an interlayer insulating film, and it is possible to use a general-purpose developing liquid, and the film formed by the pattern after development is reduced in amount. Further, according to the third aspect of the present invention, it is possible to provide a photosensitive resin composition for an interlayer insulating film, and it is possible to form a pattern having a better rim. . Further, according to the fourth aspect of the present invention, it is possible to form an interlayer insulating film having high chemical resistance and a finer pattern. Moreover, according to the fifth aspect of the present invention, it is possible to provide a photosensitive resin composition for an interlayer insulating film having higher storage stability. Finally, according to the method for forming an interlayer insulating film of the present invention, it is possible to provide a method of forming an interlayer insulating film by using a general-purpose developing liquid to form an interlayer insulating film, and a photosensitive resin composition for an interlayer insulating film. [Embodiment] In the first aspect, the photosensitive resin composition for interlayer insulating film of the present invention contains a soluble resin component (hereinafter referred to as a "ruthenium" component) and a sensitizer (Β) ( Hereinafter also referred to as (Β) ingredients). In the second aspect, the interlayer insulating film of the present invention comprises a photosensitive resin composition 11 200817838, and may contain an alkali-soluble resin component (A) (hereinafter also referred to as component (A)) and a photosensitive agent (B) (below). Also referred to as component (B), the above-mentioned test mixture J > the crystalline resin component (A) contains a copolymer containing a structural unit (al) containing an acidic earth and a constituent unit, and The structural unit having a crosslinkable group, ^, and the sensitizer (B) contains a benzoquinonediazide-based compound. In this case, the photosensitive resin composition layer formed of the photosensitive resin composition for an interlayer insulating film has a dissolution rate of the exposed portion/not exposed.

The dissolution rate is 5 or more. Thereby, it is possible to visualize the contrast between the unexposed portion and the light-emitting portion, and it is possible to obtain a pattern of " Thereby, a good interlayer insulating film can be formed. Further, the unexposed portion has a speed of 10 nm/sec or less. 4, ... ~ ~ 丨 w w Qing group, because the dissolution rate in the imaging solution is too fast, so it is difficult to obtain the contrast between the exposed part and the unexposed part, must be 2.38% by mass The aqueous solution of tetraammonium hydroxide was diluted (example h 0.4% by mass) to perform development. but. When the photosensitive resin composition for an interlayer insulating film of the present invention is used, the dilution step can be omitted. Further, in the third aspect, the side wall angle of the photoresist pattern obtained by the photosensitive resin composition for an interlayer insulating film is preferably 45 or more and 9 or less. The side wall angle is obtained by using, in particular, i% by mass to 3% by mass of a nitrogen oxynitride > trough solution (TMA®) aqueous solution, particularly a commercially available 2 3 § mass % hydrazine aqueous solution as a developing solution. It is better. Further, in the fourth aspect, the photosensitive property of the interlayer insulating film of the present invention is used? = substance, may contain an alkali-soluble resin component (Α), and a sensitizer (Β), citing 3 alkali-soluble resin component (A) containing a specific structural unit of a total of 12 200817838 polymer (Al), and the aforementioned sensitizer ( B) is a compound containing a phenylhydrazine diazide-based compound and a phenol-containing hydroxy compound. Further, the resolution of the pattern formed by the photosensitive resin composition for the interlayer insulating film is 2 · 0 μm or less. [Alkali-soluble resin component (A)] The component (A) in the present invention contains a copolymer (A1) having a structural unit (al) and a structural unit having a crosslinkable group. (a2). The composition for an interlayer insulating film of the present invention can be used as the component (a) by containing a copolymer having a structural unit (a1) and a structural unit (a2), whereby the resolution and storage stability of the applied pattern can be improved. Further, development can be carried out by directly using an aqueous solution of tetraammonium hydroxide which is usually used in an amount of 2.8 % by mass. The dilution step can be omitted, but the previous interlayer insulating film composition must be diluted with a 2.38 mass% aqueous solution of tetramethylammonium hydroxide (e.g., 4% by mass) and then developed. Further, in the second aspect, the (Α) component in the present invention may further contain a copolymer (A1) containing a structural unit having an acidic group structural unit (having an acidic group) (al) And a structural unit having a crosslinkable group (a2). In this case, the component (A) of the photosensitive resin composition for an interlayer insulating film of the present invention contains the copolymer (A1), and the copolymer (A1) contains the above structural unit (al) and structural unit (a2). The solubility in the developing solution can be controlled, and development can be carried out by directly using the 3.8% by mass aqueous solution of tetramethyl sulphate which is usually used. Therefore, the dilution step can be omitted. Further, since the photosensitive resin composition for an interlayer insulating film of the present invention contains a copolymer having a structural unit of 13 200817838 (a 1 ), the developing solution and the storage stability can be improved. The acid-containing structural unit in the present invention may, for example, be a monocarboxylic acid such as acrylic acid, methacrylic acid or crotonic acid; maleic acid, fumaric acid, citraconic acid, mesaconic acid, and itaconium. A dicarboxylic acid such as an acid; a structural unit derived from an unsaturated carboxylic acid such as an anhydride of a dicarboxylic acid; and a structural unit represented by the following formula (a-1). Further, in the fourth aspect, the component (A) in the present invention contains the copolymer (A 1) 'the copolymer (A 1 ) contains a structural unit (al) having a phenolic hydroxyl structural unit, and has a cross The structural unit of the joint (a2). By including these structural units, resolution and preservation stability can be improved. In the fifth aspect, the component (A) in the present invention contains the copolymer (A1), and the copolymer (A1) contains only the phenolic hydroxy structure represented by the general formula

The unit is especially good. [Chemical Formula 3]

(〇H)a (a-1) 14 200817838 [In the above formula, RG represents a hydrogen atom or a methyl group, R1 represents an alkylene group having a single carbon number of 1 to 5, and R2 represents a carbon number of 1 to 5; An alkyl group, a is an integer of 1 to 5, b is an integer of 0 or 1 to 4, a + b is 5 or less, and when two or more R 2 are present, the R 2 may be different from each other, or may be The above formula (a-1), RG is a hydrogen atom or a fluorenyl group, and the fluorenyl group is further, and R1 represents a single bond or a linear or branched alkyl group having 1 to 5 carbon atoms. Methylene, ethyl, propyl, exo, n-butyl, isobutyl, tributenyl, pentenyl, iso-yl, neopentenyl, etc. When the ethyl group is a good bond, it is particularly preferable because it can improve the alkali solubility and can improve the heat resistance as a layer from time to time. Further, a represents an integer of 1 to 5, and the effect of the present invention is In the case of easy production, a is preferably 1. When the bonding position of the warp group in the benzene ring is based on the bond of the R1 (first position), it is preferable to bond to the fourth position. Further, R2 represents a linear chain having a carbon number of 1 to 5. The branched chain-like entertainment may specifically be a methyl group, an ethyl group, a propyl group, an isopropyl group, a n-butyl group, a group, a tributyl group, a pentyl group, an isopentyl group, a neopentyl group, etc. In terms of production, a mercapto group or an ethyl group is preferred. Further, b represents an integer of 0 or 1 to 4. Specific examples of the structural unit include the following structural formula (a- Ι-ία -1 - 2) The material shown is particularly good for the structural unit shown by ( a -1 -1). The bond or the expression is η ] ° is good. The isopropyl pentene is a single film, the carbon source: the base Iso easy 1) and 15 200817838 [Chemical Formula 4]

The structural unit (al) can be introduced into the copolymer (A1) by copolymerizing a polymerizable monomer represented by the following formula (a-1) / with another polymerizable monomer. [Chemical Formula 5] R0

[R0, R1, R2, a, b are the same as described above] 16 200817838 The structural unit (a2) in the present invention has a structural position of a crosslinkable group. The crosslinkable group is a material which is crosslinked by heat, and examples thereof include an organic group having an ethylenic double bond, an organic group having an epoxy group, and an organic group having an oxycyclobutane group. Among these structural units (a2), an organic group having an epoxy group is preferred from the viewpoint of easy copolymer formation. Further, when (a2) is an organic group having a bad emulsion group, the photosensitive resin composition for interlayer filming has a problem in terms of storage stability, and it is possible to combine the structural units shown in (a1) above. The copolymer is formed to enhance the preservation stability. In the structural unit (a2) having such a crosslinkable group, examples of the organic group containing an epoxy group include glycidyl acrylate, glycidyl acrylate, and acrylic-β-A. Glycidyl propyl ester, methacryl-β-methylglycidyl propyl ester, α·glycidyl ethacrylate, α-n-propyl acrylate propyl acrylate, α-n-butyl acrylate propylene Ester, acrylic acid-3 butyl butyl acrylate, 3,4-epoxybutyl methacrylate, -6,7-epoxy acrylate, -6,7-epoxyheptyl methacrylate, α-ethyl Glycosyl-6,7-cycloheptyl ester, o-vinylbenzylepoxypropyl ether, m-vinylbenzyl epoxidized propyl ether, p-vinylbenzylepoxypropyl ether, (3,4-ring A polymerizable monomer such as oxycyclohexyl)methyl hydrazine acrylate is derived by copolymerization. This structural unit (a 2) can be made singly or in combination. The structural unit (a2) which is particularly preferable, or the fifth aspect structural unit (a2) in the present invention, may be a structural unit represented by the following formula (a-2). It has a heterogeneous edge but has a citrate, a 4-heptyloxy group, etc. 17 200817838 [Chemical Formula 6]

(a-2) [R3 represents a hydrogen atom or a mercapto group] From the viewpoints of ease of production, cost advantage, and improvement of solvent resistance of the obtained film, the use of the formula (a-2) is good. . Further, by combining the structural units shown in the above (a-1), it is possible to particularly enhance the storage of the composition for an interlayer insulating film, and the copolymer (A1) may also contain a structural unit (al). (a3). The structural unit (a3) is not particularly limited as long as it is a structural unit derived from a compound having a compound B. Examples of such structural units (a3) include unsaturated carboxylic acid esters, methacrylates, acrylamides, methacryl allyl compounds, vinyl ethers, vinyl esters, and phenelzine. The structural unit. Examples of the unsaturated carboxylic acid include monocarboxylic acids such as acrylic acid and mercaptoacrylic acid; maleic acid, fumaric acid, citraconic acid, and interlayer insulating units are copolymerization stability. (a2) Derived from unsaturated carboxylic acids such as olefinic double bonds, decyl acrylates, and the like, crotonic acid, and dicarboxylic acids such as 18 200817838 and econic acid. Structural units, etc. Examples of the acrylates include decyl acrylate, ethyl acrylate, propyl acrylate, isopropyl acrylate, butyl acrylate, amyl acrylate, ethyl hexyl acrylate, octyl acrylate, and acrylic acid-third octyl ester. A linear or branched alkane ester of acrylic acid; cyclohexyl acrylate, dicyclopentanyl acrylate, 2-nonylcyclohexyl acrylate, dicyclopentanyl acrylate, dicyclopentyloxyethyl acrylate, isodecyl acrylate, etc. Acrylic cycloalkyl ester; chloroethyl acrylate, 2,2-dimethylhydroxypropyl acrylate, 2-hydroxyethyl acrylate, 5-hydroxypentyl acrylate, trishydroxypropyl propane monoacrylate, neopentyl Alcohol-acrylic acid vinegar, benzyl acrylate vinegar, propyl acetophenoxy benzyl sulfonate, acetoacetic acid vinegar, tetrahydrofurfuryl acrylate, aryl acrylate (such as phenyl acrylate) and the like. Specific examples of the mercapto acrylates include methyl methacrylate, ethyl methacrylate, propyl methacrylate, isopropyl methacrylate, n-butyl methacrylate, and dibutyl methacrylate. Linear or branched alkyl methacrylate such as tert-butyl methacrylate, amyl methacrylate, hexyl methacrylate, octyl methacrylate, etc.; cyclohexyl methacrylate, methacrylic acid a mercapto acrylate alicyclic vinegar such as cyclopentyl ester, 2-methylcyclohexyl methacrylate, dicyclopentyloxy methacrylate or isodecyl methacrylate; benzyl hydrazide acrylate Chlorobenzyl acrylate, 2-hydroxyethyl methacrylate, 4-hydroxybutyl methacrylate, 5-hydroxypentyl methacrylate, 2,2-dimercapto-3-hydroxypropyl methacrylate Ester, trihydroxypropane monomethacrylate, neopentyl alcohol monodecyl acrylate, decyl methacrylate, tetrahydrofurfuryl methacrylate, aryl methacrylate (eg decyl propyl 19 200817838 phenyl enoate) , decyl methacrylate, naphthyl methacrylate, etc.). Specific examples of the acrylamides include acrylamide and N-alkyl acrylamide (the number of carbon atoms of the alkyl group is preferably 1 to 10, and examples thereof include a methyl group, an ethyl group, a propyl group, and a butyl group. Tributyl, heptyl, octyl, cyclohexyl, hydroxyethyl, benzyl, etc.), N-aryl acrylamide (for example, phenyl, tolyl, nitrophenyl, naphthyl, Hydroxyphenyl or the like), N,N-dialkyl acrylamide (the alkyl group preferably has a carbon number of 1 to 10), N,N-aryl acrylamide (aryl group such as phenyl), N- Mercapto-N-phenyl acrylamide, N-hydroxyethyl-N-mercapto acrylamide, N-2-acetamide ethyl-N-ethenyl acrylamide. Specific examples of the methacrylamides include mercapto acrylamide and N-alkyl methacrylamide (the number of carbon atoms of the alkyl group is preferably 1 to 10, and examples thereof include a methyl group and an ethyl group. , a tributyl group, an ethylhexyl group, a hydroxyethyl group, a cyclohexyl group, etc.), an N-arylmercapto acrylamide (the aryl group may, for example, a phenyl group), and an N,N-dialkylmethyl group. Acrylamide (alkyl with ethyl, propyl, butyl, etc.), N,N-diarylmethacrylamide (aryl based, for example, phenyl), N-hydroxyethyl-N-methylhydrazine Acrylamide, N-methyl-N-phenylmethacrylamide, N-ethyl-N-phenylmethacrylamide. The allyl compound may, for example, be an allyl ester (for example, allyl acetate, sodium sulphate, octoate, lauric acid, propyl acrylate, stearic acid) Propyl ester, allyl benzoate, allyl acetate, lactic acid, etc., and women's propoxyethanol. Specific examples of the vinyl ethers include alkyl vinyl ethers (for example, hexyl vinyl ether, octyl vinyl ether, mercapto vinyl ether, ethylhexyl vinyl ether, decyloxyethyl ethyl ether, ethoxyethyl ethyl b). Dilute bond, gas ethyl ethoxylate, 1 - fluorenyl 20 200817838 -2,2-dimercaptopropyl vinyl ether, 2-ethyl butyl vinyl ether, hydroxyethyl vinyl ether, diethylene glycol vinyl ether, Di-aminoethyl vinyl ether, diethylaminoethyl vinyl ether, butylaminoethyl vinyl ether, benzyl vinyl ether, tetrahydrofurfuryl vinyl ether, etc.), vinyl aryl ether (such as vinyl benzene) Ethyl ether, vinyl phenyl phenyl ether, vinyl chlorophenyl ether, vinyl-2,4-dichlorophenyl ether, vinyl naphthyl ether, vinyl decyl ether, etc.).

Specific examples of the vinyl esters include vinyl butyrate, vinyl isobutyrate, tridecyl acetate, diethyl acetate, vinyl valerate, vinyl hexanoate, vinyl chloroacetate, and ethylene dichloroacetate. Ester, methoxyvinyl acetate, butoxy vinyl acetate, vinyl acetate, ethyl acetate, vinyl propionate, ethylene-β-phenyl butyrate, vinyl benzoate, vinyl urate Ester, vinyl chlorobenzoate, vinyl tetrachlorotoluate, vinyl naphthalate, and the like. Specific examples of the styrene include styrene and alkyl styrene (for example, methyl styrene, dimethyl styrene, trimethyl styrene, ethyl styrene, diethyl styrene, isopropyl styrene). , butyl styrene, hexyl styrene, cyclohexyl styrene, mercapto styrene, benzyl styrene, chlorodecyl styrene, trifluoromethyl styrene, ethoxymethyl styrene, ethoxylated Methylstyrene, etc., alkoxystyrene (such as methoxystyrene, 4-decyloxy-3-mercaptostyrene, dimethoxy styrene, etc.), halogen styrene (such as chlorostyrene) , Dichlorostyrene, Trichlorostyrene, Tetrastyrene, Pentachlorostyrene, Bromostyrene, Dibromostyrene, Iodostyrene, Fluorostyrene, Trifluorostyrene, 2-Bromo-4-III Fluorinyl styrene, 4·fluoro-3-trifluorodecyl styrene, etc.). Further, acrylonitrile, mercaptoacrylonitrile or the like can also be mentioned. 21 200817838 These structural units (a 34 main ^ 疋 疋 疋 from the alicyclic group (especially the propylene carbonate fat-burning gfc 戸 _ _ 曰 or ^ % ^ methacrylate) It is better to reduce the dielectric constant of the interlayer insulating germanium by the JtL Jubie ymb λ u Μ ^ 4 > , into this special moon-ring ring group. (4) It is better to have a structural unit derived from unsaturated acid-lowering m. That is, it does not contain a structural unit with a rebel base. This can improve the imaging performance and preserve stability. The resin component (A) particularly contains a copolymer containing a structural unit (al) and an oxime unit (a2) having an epoxy group as a crosslinking group, and does not contain a derivative derived from an unsaturated carboxylic acid. The structural unit, that is, the alkali-soluble resin component (A), preferably does not contain a structural unit having a carboxyl group, thereby improving chemical resistance and developing properties, and in particular, improving storage stability (especially viscosity) Long-term stability). Previous composition of interlayer insulating film Because it has poor storage stability and cannot be stored at room temperature, it must be stored frozen, and can be stored at room temperature by the above configuration. The structural unit (al) in the above-mentioned soluble resin component (A) is ι〇h ' Moer % ~ Moer % (Mo Erbi, (al): (a2): 1: 9~9: 1) is better, to 20 mol% ~ 80 mol% (Mo Erbi, (al ) · · (a2) : 2 : 8~8 : " 2) For better, 20%%~7〇%% is the best. • By making the ratio of structural units (al) in the above range In addition, the photosensitive resin composition for an interlayer insulating film can be sufficiently soluble, and the development property can be improved. Further, the side wall angle formed by the photosensitive tree composition of the interlayer insulating film can be 45 degrees. Above 90 degrees, it is possible to form a pattern having a good profile and a higher contrast than before. 22 200817838 Further, the structural unit (a2) in the above alkali-soluble resin component (A) is 10 mol% to 90 mol. The ear % is better 'more than 2 〇 mol% ~ 8 〇 耳 % is better, with 30 mol % ~ 70 mol % is particularly good. ' One by The ratio of the structural unit (a2) is within the above range, and it is possible to impart sufficient thermosetting property to the photosensitive resin composition for an interlayer insulating film, and it is possible to obtain chemical resistance as an interlayer insulating film. In particular, an alkali-soluble resin component (A) The ratio of the structural unit in the film is preferably 55 mol% or more, whereby the sidewall angle of the pattern formed of the photosensitive resin composition for the interlayer insulating film can be 8 〇 or more. The structural unit (a3) in the resin component (A) is preferably 0 mol% to 60 mol%, preferably 〇 mol% to 3 mol%, preferably 〇 mol% to 10 mol. % is better and is not included as the best. The mass average molecular weight of the above copolymer (A1) (Mw: the measured value obtained by conversion of gel permeation chromatography (GPC) to benzophenone) is preferably 2 〇〇〇 to 5 ,, and 5000 to 3 0000 is better. By setting the molecular weight to 2,000 or more, a film shape can be easily formed. Further, by setting the molecular weight to 50,000 or less, appropriate alkali solubility can be obtained. The above copolymer (A1) can be produced by a well-known radical polymerization. In other words, the polymerizable monomer obtained by derivatizing the structural units (al), (a2), and (a3) and a known radical polymerization initiator can be dissolved in a polymerization solvent, and then heated and scrambled to be produced. . Further, the alkali-soluble resin component (A) may contain other copolymer (A2) in addition to the above copolymer (A1). The copolymer (A2) may, for example, be a copolymer composed of a structural unit (a3) (including a homopolymer), a copolymer composed of 23 200817838 structural unit (al) and a structural unit (a3), A copolymer composed of a structural unit (a2) and a structural unit (a3). The copolymer (A2) may be one type or a combination of two or more types. The copolymer (A2) is preferably 5% by mass to 50 parts by mass, more preferably 3% by mass, based on 100 parts by weight of the copolymer (A1). The mass average molecular weight (Mw: measured value obtained by conversion of styrene by gel permeation chromatography (GPC)) of the copolymer (A2) is preferably from 2 Å to 50,000, more preferably from 5,000 to 30,000. [Photosensitive agent (B)] The photosensitive agent (B) is not particularly limited as long as it can be used as a photosensitive component, and a compound derived from a benzoquinonediazide-based compound can be mentioned. The compound derived from the benzene-containing diazide compound may specifically be a fully esterified or partially esterified compound of an age-old compound (also referred to as a phenolic hydroxy compound) and a naphthoquinonediazide sulfonated ruthenium compound. In the second aspect, the phenolic hydroxy compound is a compound having a Gram absorption coefficient of 1 or less at a wavelength of 35 Å. By using a sulfhydryl group-containing compound having such a property, the transparency of the interlayer insulating film formed can be improved, and it is particularly suitable for use in the i-line near the wavelength of 350 nm. The age-containing thiol compound is more preferably a non-diphenyl ketone-based compound which does not contain a carbonyl group. Thereby, the stability of the photosensitive resin composition can be improved. Specific examples of the compound of the above-mentioned age include polyhydroxydiphenyl ketones such as 2,3,4-trihydroxydiphenyl 24 200817838 ketone and 2,3,4,4'-tetrahydroxydiphenyl ketone;参(4-Hydroxyphenyl)decane, bis(4-hydroxy-3-methylphenyl)-2-hydroxyphenylmethane, bis(4-hydroxy-2,3,5-trimethylphenyl) 2-hydroxyphenylmethane, bis(4-yl-3,5-dimethylphenyl)-4-3⁄4phenyl fluorene, bis(4-lightyl-3,5-dimethylphenyl) 3-hydroxyphenyl decane, bis(4-hydroxy-3,5-diamidinophenyl)-2-hydroxyphenyl decane, bis(4-hydroxy-2,5-dimethylphenyl) 4-hydroxyphenylmethane, bis(4-hydroxy-2,5-diamidinophenyl)-3-hydroxyphenylnonane, bis(4-hydroxy-2,5-dimethylphenyl)- 2-hydroxyphenyl decane, bis(4-hydroxy-3,5-dimercaptophenyl)-3,4-diphenylene, bis(4-fatho-2,5-dimethyl Phenyl)-3,4-dihydroxyphenyl decane, bis(4-hydroxy-2,5-dimercaptophenyl)-2,4-dihydroxyphenyl decane, bis(4-hydroxyphenyl) -3 -decyloxy-4-hydroxyphenyldecane, bis(5-cyclohexyl-4-hydroxy-2-indenylphenyl)-4-hydroxyphenylmethane, bis(5-cyclohexyl-4 -hydroxy-2-a Phenyl)-3.hydroxyphenylmethane, bis(5-cyclohexyl-4-hydroxy-2-methylphenyl)-2 - phenylmethyl, bis(5-cyclohexyl-4-3⁄4yl- a phenolic compound such as 2-nonylphenyl)-3,4-dihydroxyphenyl decane; 2,4-bis(3,5-dimethyl-4-hydroxybenzyl)-5-hydroxyphenol Linear 3 nucleoside phenolic compound such as 2,6-bis(2,5-dimethyl-4-hydroxybenzyl)-4-methylphenol; bis[3-(2-oxyl-5--) Alkyl group - 4 - mercapto - 5- 3⁄4 hexyl phenyl] isopropane, bis[2,5-dimercapto-3-(4-hydroxy-5-methylbenzyl)-4-hydroxyphenyl ] decane, bis[2,5-dimercapto-3-(4-hydroxybenzyl)-4-hydroxyphenyl]decane, bis[3-(3,5-dimethyl-4-hydroxybenzyl) 4-hydroxy-5-mercaptophenyl]decane, bis[3-(3,5-dimethyl-4-hydroxybenzyl)-4-hydroxyd-ethylphenyl]decane, Bis[3-(3,5-diethyl-4-hydroxybenzyl)-4-hydroxy-5-nonylphenyl]methane, double 25 200817838 [3-(3,5-diethyl-4- Hydroxybenzyl)-4-hydroxy-5-ethylphenyl]decane, bis[2-hydroxy-3-(3,5-dimethyl-4-hydroxybenzyl)-5-methylphenyl] Methane, bis[2-hydroxy-3-(2-hydroxy-5-fluorenylbenzyl)-5-nonylphenyl]methane, bis[4-hydroxyl -3-(2-hydroxy-5-mercaptobenzyl)-5-methylphenyl]methane, bis[2,5-dimethyl-3-(2-hydroxy-5-methylbenzyl)- Linear 4-nucleoside phenolic compound such as 4-hydroxyphenyl]methane; 2,4-bis[2-hydroxy-3-(4-hydroxybenzyl)-5-fluorenylbenzyl]-6-cyclohexylphenol , 2,4-bis[4-hydroxy-3-(4-hydroxybenzyl)-5-methylbenzyl]-6-cyclohexylphenol, 2,6-bis[2,5-dimethyl-3 a linear polyphenol compound such as a linear 5-nuclear phenol compound such as (2-hydroxy-5-fluorenylbenzyl)-4-hydroxybenzyl]-4-methylphenol; double [2, 3, · three Hydroxyphenyl]decane, bis[2,4-dihydroxyphenyl]decane, 2,3,4-trihydroxyphenyl-4'hydroxyphenyldecane, 2-(2,3,4-tri Hydroxyphenyl)-2-(2 ' ,3 ' ,4,-trihydroxyphenyl)propane, 2-(2,4-dihydroxyphenyl)-2-(2' ,4' -dihydroxyphenyl Propane, 2-(4-hydroxyphenyl)-2-(4'-hydroxyphenyl)propane, 2-(3-fluoro-4-hydroxyphenyl)-2-(3,-fluoro-4' - Hydroxyphenyl)propane, 2-(2,4-dihydroxyphenyl)-2-(4'-hydroxyphenyl)propane, 2-(2,3,4-trihydroxyphenyl)-2-(4) '-Hydroxyphenyl)propane, 2-(2,3,4-trihydroxyphenyl)-2-(4' hydroxyphenyl)propane, 2-(2,3,4-trihydroxyl a bi-antibiotic compound such as phenyl)-2-(4'-hydroxy-3',5'-didecylphenyl)propane; ^(^-4-hydroxyphenyl)isopropyl]-4- [l,l-bis(4-hydroxyphenyl)ethyl]benzene, 1-[1-(3.methyl-4-hydroxyphenyl)isopropyl]-4-[l,l-bis(3 a polynuclear branched compound such as mercapto-4hydroxyphenyl)ethyl]benzene; a condensed phenolic compound such as 1,1-bis(4-hydroxyphenyl)cyclohexane. 26 200817838 These can be used alone or in combination of two or more. Further, when the sensitizer (B) is a condensate containing a benzoquinonediazide compound and a phenolic hydroxy compound, the hydrazine-containing compound may be a compound having a heat-separating temperature of 300 °C or higher. By using a compound having such a degree of thermal decomposition, it is possible to prevent thermal decomposition at the time of prebaking or thermal curing at 200 °C or higher. Thereby, it is possible to impart higher transparency to the formed interlayer film. In this case, the component (B) may specifically be a fully esterified product or a partially acetated compound of the above-mentioned phenolic hydroxy compound-containing naphthoquinone-substituted acid compound. Preferred examples of the hydrazine-containing compound include the following formula. The basic solution of the warm step and the 27th 200817838 [Chemical Formula 7]

OH 28 200817838

200817838 These may be used alone or in combination of two or more. Further, examples of the naphthoquinonediazidesulfonic acid compound include naphthoquinone-1,2-diazide-5-sudan acid or naphthalene 3-kun-1,2-diazide-4-transester. Further, examples of the other benzoquinonediazide-containing compound include o-quinonediazide, o-naphthoquinonediazide, o-quinonediazide or o-naphthoquinonediazidesulfonate. Nuclear substituted derivatives. Furthermore, it is possible to use o-benzoquinonediazidesulfonium chloride and a compound having a hydroxyl group or an amine group (for example, phenol, p-methoxyphenol, dimethylphenol, hydroquinone, bisphenol A, naphthol, catechol, Gallic phenol, gallicol monomethyl ether, gallic phenol 1,3 - dimethyl ether, gallic acid, esterified or etherified gallic acid, aniline, p-aminodiphenylamine The reaction product of (etc.). These may be used alone or in combination of two or more. These benzoquinonediazide-containing compounds can be obtained, for example, by a phenolic hydroxy compound, with Qin S Kun-1,2-dinitro nitrogen-5-continued chlorine, or Qin 1 Kun-1,2-difeng Nitro-4-sulfonyl chloride is completely esterified or partially esterified by condensation in the presence of a base such as triethanolamine, an alkali metal carbonate or an alkali metal hydrogencarbonate in a suitable solvent such as dioxane. To manufacture. The benzene-containing diazide compound is preferably a naphthene-doped azide reductate. Further, as the component (B), a non-diphenylketone-based benzoquinonediazide-based compound is preferably used, and a multi-nuclear branched compound is preferably used. Further, it is preferred that the phenolic hydroxyl group-containing compound has a Gram absorption coefficient of 1 or less at a wavelength of 350 nm. Thereby, a photosensitive resin composition for an interlayer insulating film can provide high sensitivity, and when it is used as an interlayer insulating film, the transmittance (transparency) can be improved. Further, the decomposition temperature of the phenolic hydroxy group-containing compound is preferably 300 ° C or more. Thereby, the transparency of the interlayer insulating film can be ensured. These (B) components, in particular, benzoquinone II using 1-[1-(4-hydroxyphenyl)isopropyl]-4-[l,l-bis(4-hydroxyphenyl)ethyl]benzene Azidosulfonate is preferred. Further, the sensitizer is capable of improving stability over time (foreign time). The content of the component (B) is from 10% by mass to 40% by mass based on the total solid content, preferably from 20% by mass to 30% by mass. By setting the content of the component (B) to 10% by mass or more, the film reduction rate can be reduced, and the resolution can be improved. It is also possible to reduce the film reduction of the pattern after patterning. In addition, by setting the content of the component (B) to 40% by mass or less, appropriate sensitivity and transmittance can be imparted. [Organic solvent (C)] The photosensitive resin composition for an interlayer insulating film of the present invention may contain an organic solvent (C) (hereinafter also referred to as a component (C)) in order to change the coating property or to adjust the viscosity. (C) component), benzene, toluene, xylene, mercapto ethyl ketone, acetone, methyl isobutyl ketone, cyclohexanone, decyl alcohol, ethanol, propanol, butanol, hexanol, Cyclohexanol, ethylene glycol, diethylene glycol, glycerin, ethylene glycol monomethyl ether, ethylene glycol monoethyl ether, propylene glycol monodecyl ether, propylene glycol monoethyl ether, diethylene glycol monodecyl ether, Diethylene glycol monoethyl ether, diethylene glycol dimethyl ether, diethylene glycol diethyl ether, 3-methoxybutyl acetate (MA), 3-methoxybutanol 31 200817838 (Β Μ), 3-methyl-3-decyloxyacetic acid butyl ester, propylene glycol monomethyl ether acetate (PGMEA), propylene glycol monomethyl ether propionate, propylene glycol monoethyl ether propionate, methyl carbonate, carbonic acid Ester, propyl carbonate, butyl carbonate or a mixture of these. Among them, a mixed solvent of cerium, or cerium and lanthanum is preferred.

The amount of use of the organic solvent (C) is not particularly limited, and a concentration that can be applied to a substrate or the like can be used, and is appropriately set in accordance with the thickness of the coating film. Specifically, it is preferred that the solid content concentration of the photosensitive resin composition is in the range of 1% by mass to 50% by mass, preferably 15% by mass to 35% by mass. [Others (D)] Further, in order to improve the coating property, the photosensitive resin composition for an interlayer insulating film of the present invention may be added with a surfactant, a sensitizer, an antifoaming agent, a crosslinking agent or the like. The surfactant may be a conventionally known one, and examples thereof include compounds such as anionic, cationic, and nonionic. Specifically, Χ-70·090 (trade name, manufactured by Shin-Etsu Chemical Co., Ltd.) and the like can be mentioned. By adding an surfactant, coating properties and flatness can be improved. As the sensitizer, a conventionally known positive-type resist can be used, and examples thereof include a compound having a phenolic hydroxyl group having a molecular weight of 1,000 or less. The antifoaming agent may also be a well-known one, and examples thereof include a lanthanide compound and a fluorine-based compound. Further, the crosslinking agent may, for example, be a polymerizable compound having an ethylenically unsaturated bond. From the viewpoint of good polymerizability and the ability to increase the strength of the obtained pattern-like film, it is preferred to use a monofunctional, bifunctional or trifunctional or higher (fluorenyl) acrylate. Examples of the monofunctional (meth) acrylate include 2-hydroxyethyl (meth)acrylate, carbitol (meth) acrylate, isophorone (meth) acrylate, and 3-methoxy group. Butyl (meth)acrylate, 2-hydroxyphenyl 2-(methyl)propenyloxyethyl phthalate, and the like. Examples of the commercially available product include ARONIX M-101, the same M-111, the same M-114 (manufactured by East Asia Chemical Industry Co., Ltd.), KAYARAD TC-110S, and the same TC-120S (Nippon Chemical Co., Ltd.). ), BIS COAT 158, same as 2311 (Osaka Organic Chemical Industry Co., Ltd.). The above-mentioned bifunctional (fluorenyl) acetoacetate may, for example, be an ethyl alcohol (mercapto) acrylate, 1,6-hexanediol di(meth) acrylate or 1,9-nonanediol bis (a) Acrylate, polypropylene glycol bis(indenyl) acrylate, tetraethylene glycol di(methyl) propionate, bisphenoxyethanol oxime diacrylate, and the like. Commercially available products include, for example, ARONIX-210, M-240, M-6200 East Asia Chemical Industry Co., Ltd., KAYARAD HDDA, HX-220, and R-604 (Sakamoto Chemical Co., Ltd.) )), BISCOAT 260, 312, and 335HP (Osaka Organic Chemical Industry Co., Ltd.). Examples of the above-mentioned trifunctional or higher (fluorenyl) acrylate include, for example, trishydroxypropyl propyl di(methyl) propyl acetoacetate, neodymium tetrakis(3) thioglycolate, and tris(A). Base) propylene methoxyethyl) phosphate, neopentyl alcohol tetra(meth) acrylate, dipentaerythritol penta(indenyl) acrylate, dipentaerythritol hexa(meth) acrylate vinegar, etc. . The commercially available product may, for example, be ARONIXM-309, the same M-400, the same M-402, the same M-405, the same M-450, the same M-7100,

Same as M-8 03 0, same as M_8 060 (East Asia Chemical Industry Co., Ltd.), KAYARAD 33 200817838

TMPTA with DPHA, with DPCA-20, with DPCA-30, with DPCA-6 0 'with DPCA_120 (Sakamoto Chemical Co., Ltd.), BISCOAT 295, with 300, with 36〇, with GPT, with 3PA, with 400 (Osaka Organic Chemical Industry Co., Ltd.) and so on. These crosslinking agents may be used alone or in combination of two or more. In addition, the above-mentioned soluble resin component (A) is contained in the photosensitive resin composition for interlayer insulating film of the present invention, and sufficient thermosetting property can be obtained without adding the above-mentioned crosslinking agent, and a good interlayer insulating film can be formed. . In the photosensitive resin composition for interlayer insulating film of the present invention, for example, a roll mill, a ball mill, or a sand mill can be used for the component (A), the component (B), the component (c), and the component (D). The mixer is mixed (dispersed and kneaded) and filtered as necessary with a filter such as a 5 micron membrane filter. In particular, in the fifth aspect of the present invention, the photosensitive resin composition for an interlayer insulating film prepared in accordance with the above order is at 23. (The viscosity change rate after one month of storage is ±1% or less. 'It is suitable for wiring of liquid crystal display parts to prevent liquid crystal electronic parts from being inferior. The photosensitive resin composition for interlayer insulating films of this invention is used for formation of interlayer insulation film. It is designed to insulate between electrons such as a plurality of layers, integrated circuit elements, solid-state imaging elements, etc. It is also suitable for forming a protective element, such as a display element, an integrated circuit element, or a solid-state imaging element. [Method of Forming Interlayer Insulating Film] Photosensitive Resin Group The following describes a method of forming an interlayer insulating film using the interlayer insulating film 34 200817838 of the present invention. The method of forming an interlayer insulating film includes a coating step, And a developing step of applying a photosensitive resin composition on the substrate; the exposing step selectively exposing the coated photosensitive resin composition; and the developing step is using a base The developing solution develops the photosensitive resin composition after exposure, and the preferred developing solution for the developing step is concentrated. i. mass% or more and 3% by mass or less of a tetramethylammonium hydroxide aqueous solution. Hereinafter, each step will be described. First, the coating step is a spin coater, a roll coater, a spray coater, a slit coater, or the like, and the present invention is used. The photosensitive resin composition for an interlayer insulating film is applied to a support such as a substrate, and is dried to form a photosensitive resin composition layer. The substrate includes, for example, a wiring including a transparent conductive circuit, and the like. A glass plate such as a black matrix, a filter, or a polarizing plate. The method of drying the substrate on which the photosensitive resin composition is applied with the interlayer insulating film may be, for example, (1) 8 〇 2 在 2 on a hot plate. The method of drying the temperature of the crucible for 60 seconds to 120 seconds; (2) placing the method at room temperature for several hours to several days, and (3) placing it in a temperature heater or an infrared heater for tens of minutes to several hours to remove In the method of the solvent, the film thickness of the photosensitive resin composition for the interlayer insulating film is not particularly limited, and is preferably about 1.0 μm to 5.0 μm. The light step is performed by a predetermined mask. The light system is irradiated with ultraviolet light, excimer laser light, etc. The light source of the active energy ray is, for example, a low-pressure mercury lamp, #35 200817838, Ultrahigh-pressure mercury lamp, chemical lamp, excimer laser generating device, etc. The amount of energy ray to be irradiated varies depending on the composition of the photosensitive resin composition for the interlayer insulating film, for example, about 30 mJ/cini2 to 2000 mJ/cni2. The developing step forms a pattern by using a developing liquid to develop an exposed photosensitive resin composition layer, and the developing solution may be an aqueous solution of an organic alkali such as an aqueous solution of tetraammonium hydroxide (TMAH) or sodium hydroxide. An aqueous solution of an inorganic alkali such as potassium hydroxide, sodium metasilicate or sodium phosphate, whereby a protective film or an interlayer insulating film can be provided in a required range. The developing solution is preferably an aqueous solution of tetramethylammonium hydroxide (hereinafter also referred to as TMAH) in an amount of 1% by mass to 3% by mass. The concentration of the TMAH aqueous solution is preferably from 2% by mass to 2.5% by mass, and the concentration of the general-purpose product is preferably 2.38% by mass. By setting the concentration of the developing liquid to 3% by mass or less, the film reduction rate of the formed pattern can be reduced. In the exposure step, the photosensitive resin composition layer formed of the photosensitive resin composition for an interlayer insulating film of the present invention has a dissolution rate of 1 〇 in a 2.38 mass% TMAH aqueous solution. Below nanosecond/second, the exposure speed of the exposed portion in a 2.38 mass% TMAH aqueous solution was 10 nm/sec or more. By making the dissolution rate in such a range,

It is sufficient to reduce the film reduction rate of the formed pattern. In particular, when 2.38 mass% TMAH water/liquid mixture is used, it is not necessary to dilute the commercial product, and the step of diluting the developing liquid can be omitted. After the second, the seven patterns are heat-hardened. This heat curing temperature is heat-treated, for example, under the conditions of 150 C to 250. Further, it is preferable to perform overall exposure on the formed pattern. 36 200817838 Here, the photosensitive tree material for the interlayer insulating film of the present invention can be used to make the sidewall angle of the pattern formed according to the method of Shangchenggu and the soil attack method 45 to 90 degrees or less, preferably the Taiwanese cymbal. b is enough to be 90 degrees or less below 80 degrees. In the case of using the copolymer having a structural group having no carboxyl group as the component (4), it is possible to provide a photosensitive resin composition for a film having a high resolution. '曰1 absolutely

U, by using a compound obtained by condensing a benzoquinonediazide-based compound and a phenolic hydroxy-containing compound as a (Β) component, and the above-mentioned phenol-containing thiol compound is dyed at a wavelength of 350 nm. The Lan's absorption coefficient is i or less & The temporal stability of the photosensitive resin composition for interlayer insulating film can be improved. Further, it is possible to provide an interlayer insulating film having higher transparency. Further, by using a compound having a thermal decomposition temperature of 300 ° C or higher as the phenolic hydroxy compound in the component (B), it is possible to provide a photosensitive resin composition for an interlayer insulating film having high transparency. The photosensitive resin composition for an interlayer insulating film of the present invention can be suitably used for forming an interlayer insulating film, and is disposed in a layered manner on a line of an electronic component such as a liquid crystal display element, an integrated circuit element, or a solid-state image sensor. Insulation. Further, it is also suitable for forming a protective film for preventing deterioration or damage of electronic components such as a liquid crystal display element, an integrated circuit element, and a solid-state image sensor. [Examples] [Example 1] A photosensitive resin composition (photosensitive resin composition for interlayer insulating medium 37 200817838) was prepared by mixing the following components. (A) component: structural unit of the following formula (a-1-l): structural unit (a-2-l) = 40: 6 〇 (mole ratio) of resin 1 (mass average molecular weight 9000) · · 75 parts by mass [Chemical Formula 9]

(a-2-1) (B) Component: 1-[1-(4-hydroxyphenyl)isopropyl]-4-[l,l-bis(4-hydroxyphenyl)ethyl]benzene-1 , 2-naphthoquinonediazide-5-sulfonate (esterification rate: 67%) · "25 parts by mass (C) Component: 3-methoxyacetic acid butyl ester··· 23 3 parts by mass (D) Ingredients: surfactant (trade name: X-70-093) · · · 0.1 parts by mass of the above 1-[1-(4-hydroxyphenyl)isopropyl]-4-[l,l-double The thermal decomposition temperature of (4-hydroxyphenyl)ethyl]benzene was 365 ° C, and the Gram absorption coefficient was 0.003 at a wavelength of 350 nm. (Pattern forming method) 38 200817838 The above-mentioned photosensitive resin composition was formed into a film using a spin coater on a glass substrate (manufactured by DOW CORN I NG: 0. 7 mm x 150 mm (thickness X diameter)). After coating with a thickness of 3 μm, it was dried on a hot plate at 11 ° C for 2 minutes to obtain a coated film. The coating film was passed through a positive-type resist pattern of a 5 μm line pattern/5 μm gap pattern, and exposed using a mirror projection alignment exposure apparatus (trade name: Μ PA-600 FA, manufactured by CAN CN Co., Ltd.). Subsequently, it was immersed in a tetraammonium hydroxide 2·38 mass% aqueous solution (developing liquid) for 1 minute to carry out development, and then washed with pure water to remove an unnecessary portion to obtain a pattern. [Example 2] A photosensitive resin composition (a photosensitive resin composition for an interlayer insulating film) was prepared by using ί :: the following components'. Yuhua, the structural unit of the following formula (a -1 -1): | f 5〇 (Morby) 榭p 哲 ”), · 口口前位(a-2-1) = 5 〇: part 9 (mass 1 average molecular weight 8700) · · 75 mass (B) Ingredients · [1-(4-hydroxyphenyl) isopropyl] benzene in the field] bis (4-hydroxyphenyl)乙不酉昆二丰氮sulfonic acid / (C) Ingredients: 3 take e (digestion rate 67 / 〇 > · · · 25 parts by mass of methoxy butyl acetate · · · 23 3 quality dan ^ (D Ingredients ・• 屄品贝里份八1面活性剂 (trade name: Χ-70 093, 份八/Ue〇93) · · · 0.1 mass of the above-mentioned photosensitive resin composition, apricot is applied to form a pattern. ", Example 1 is carried out in the same manner as in Example 1 2008. [Example 3] The following components were mixed to prepare a photosensitive resin composition (photosensitive resin composition for interlayer insulating film). (A) Component: Resin 2 · · 50 parts by mass of structural unit (a-1-l): structural unit (a-2-l) = 20: 80 (mole ratio) of resin 3 (mass average molecular weight 8700) ··· 25 parts by mass (B) Ingredients: 1-[1-(4-hydroxyphenyl)isopropyl]-4-[l,l-bis(4-hydroxyphenyl)ethyl]benzene-1,2· Bismuth azide-5-sulfonate (esterification rate 67%) · "25 parts by mass (C) Ingredients: 3-methoxyacetic acid butyl ester ··· 233 parts by mass (D) Component: surfactant (product name: Χ-70-093) · · · 0 parts by mass of the photosensitive resin composition was used in the same manner as in Example 1 to form a pattern. [Example 4] The same procedure as in Example 1 was carried out except that 2,3,4,4'-tetrahydroxydiphenyl ketone-1,2-naphthoquinonediazide-5-sulfonate (esterification ratio: 80%) was used. Here, the thermal decomposition temperature of the above 2,3,4,4'-tetrahydroxydiphenyl ketone is 268 ° C, and the Gram absorption coefficient at a wavelength of 3 50 nm is 6.22. 5] except that the component (B) is 2,6-bis[(4-hydroxy-3,6·didecylphenyl)methyl]-4-methylphenol-1,2·naphthoquinonediazide- 5-sulfonate (esterification rate: 67%) was carried out in the same manner as in Example 1 except for the passage of 40, 2008, 17,838. Here, the above 2,6-bis[(4-hydroxy-3,6-di) The thermal decomposition temperature of methylphenyl)methyl]-4-methylphenol was 285 ° C. [Comparative Example 1] The following components were mixed to modulate the feeling (A) Ingredients: Styrene: methacrylic acid = 20: : 80 (mole ratio) copolymer (mass average molecular weight 7000) · ·· 30 parts by mass of methacrylic acid: methacrylic acid (3 , 4-epoxycyclohexyl)ester = 2 0: 80 (mole ratio) copolymer (mass average molecular weight 7000) ··· 45 parts by mass (B) Component: 1-[1-(4-hydroxyphenyl) Isopropyl]-4-[l,l-bis(4-hydroxyphenyl)ethyl]benzene-1,2-naphthoquinonediazide-5-sulfonate (esterification rate 67%)·· ·25 parts by mass (C) Component: 3-methoxyacetic acid butyl ester ··· 23 3 parts by mass (D) Component: surfactant (trade name: Χ-70-093) · · · 0.1 mass part using the above The photosensitive resin composition was formed in the same manner as in Example 1 to form a pattern. [Comparative Example 2] Using the same photosensitive resin composition as in Comparative Example 1, the pattern forming method of Example 1 was changed to dry at 90 ° C for 2 minutes using a hot plate, and further, tetramethylammonium hydroxide 0.4 was used. A mass % aqueous solution was used as a developing solution to form a pattern. 41 200817838 [Comparative Example 3] The following components were mixed to prepare a photosensitive resin composition. (A) Component: structural unit (all) (Mw = 93 00) · · · 75 parts by weight (B) Component: 1-[1-(4-hydroxyphenyl)isopropyl]-4-[l,l - bis(4-hydroxyphenyl)ethyl]benzene-1,2-naphthoquinonediazide-5-sulfonate (esterification rate: 67%) · "25 parts by mass (C) Component: 3 - oxime Butyl acetate. *. 233 parts by mass (D) Component: surfactant (trade name: X-70-093) · · · 0.1 parts by mass The same procedure as in Example 1 was carried out using the above-mentioned photosensitive resin composition. [Comparative Example 4] The photosensitive resin composition (photosensitive resin composition for interlayer insulating film) similar to that of Comparative Example 1 was used, and the pattern forming method of Example 1 was changed to use a hot plate at 90. The film was dried at ° C for 2 minutes, and a 0.4% by mass aqueous solution of tetraammonium hydroxide was used as a developing solution to form a pattern. [Evaluation] The photosensitive resin compositions of the above Examples and Comparative Examples were evaluated. Sensitivity, resolution, viscosity increase rate (preservation stability), sidewall angle of the formed pattern, film reduction rate of the formed pattern, and transmittance of the formed film. The method is as follows: Sensitivity: Varying the exposure, the exposure required to form a 5 micron line-pattern/5 micron 42 200817838 gap-pattern is used as sensitivity. Resolution and pattern sidewall angle: using scanning type Leigong soil The electron microscope (SEM) was used to observe and measure the pattern formed. The resolution is the minimum line width that can be formed by measuring the minimum exposure measured by the above sensitivity. Membrane reduction rate·Measured after development The ratio of the film thickness to the film thickness measured before development. The dissolution rate of the unexposed portion: the film thickness of the unexposed portion dissolved in 2.38 mass% of the TMHA aqueous solution in the second time during the exposure of Example 1. The dissolution rate of the exposed portion: when exposed in Example ,, the exposed portion was dissolved in a film thickness of 2.38 mass% of TMHA aqueous solution in 1 second. Transmittance: The obtained coating film was obtained in the same manner as above. After using an ultra-high pressure mercury lamp to be fully exposed through a positive mask, it is thermally cured in a clean oven at 230 ° C for 30 minutes to obtain a substrate with a cured film. A spectrophotometer (trade name: UV-25) will be used. 00 PC, manufactured by Shimadzu Corporation) The lowest transmittance measured at a wavelength of 400 nm to 8 Å is used as the transmission U. Thus, the drug property is obtained in the same manner as described above. The substrate with the cured film obtained was immersed in a stripping solution (ST-1 06, manufactured by Tokyo Ohka Kogyo Co., Ltd.) at 70 ° C for 5 minutes, washed with pure water and air-dried, and the change in film thickness was measured. When the amount of change is 5% or less of the film thickness before the impregnation, it is evaluated as 〇, when 2% or less is Δ, and when 2% or more is X. Viscosity increase rate (preservation stability): The viscosity of the resin composition after the resin composition was measured at room temperature for a period of one month, and the viscosity of the resin was measured, and the obtained value was used. Foreign matter elapsed time: The particle size counter was counted and counted for 1 month (the number of foreign substances at room temperature in both the examples and the comparative examples. Sensitivity over time: indicating storage for 1 month (example and comparative warm storage) The sensitivity of the post-sensitivity to the composition of the photosensitive resin composition. These results are shown in Table 1. The room sensitivity is 44 after the tonality of the resin.

[Id sensitivity time-dependent (%) S 1—Η 〇τ-Η 〇τ—^ S ο rH ON rH tH 〇\ rH rH o rH 〇\ rH Γ 1 ^ Foreign matter elapsed time (pieces/ml) inch (Ν 〇(Ν (Ν 1424 m cn oo rn m viscosity increase rate (%) 00 〇〇〇〇〇〇oq c? inch CN inch (N tH , d inch CN chemical resistance 〇〇〇〇〇 <1 < 1 X <] Transmittance (%) 91.9 92.4 92.0 81.0 79.0 89.3 J 89.3 91.7 1 89.3 -S 2 ill ΓΠ c^· 3 VO o (N inch · 1 Undissolved part dissolution rate (nano / sec) 0.55 9.45 0.65 11.5 0.90 24.60 4.75 10.85 1 Membrane reduction (%) Τ-Η 18.9 ΓΟ cn CN 00 49.2 as 21.7 OS Sidewall angle (.) CN 〇〇VO (N 00 JO 1 jn to v〇JO Resolution (micron) 〇CN «η o <N 1 o cn o CN 〇cn sensitivity (mJ/cm2) 250 〇Τ-1 250 400 1 400 o rH 400 Example 1 Example 2 Example 3 Example 4 Example 5 Comparative Example 1 Comparative Example 2 Comparative Example 3 Comparative Example 4 200817838 According to the above, it was found that the photosensitive resin composition of the present invention has a high resolution pattern, is excellent in change over time, and is resistant to the cured film. It can provide a high-permeability and high-transparent interlayer insulating film, and is particularly suitable for use in a display having high transmittance, as a permanent film such as an interlayer insulating film; and, can be formed with a good profile and high sensitivity. In addition, compared with the photosensitive resin composition of the interlayer insulating film of the prior art, it exhibits a small increase in viscosity and high storage stability, and further, it is known from the examples that the foreign matter is sensitized by time. In addition, the photosensitive resin composition for interlayer insulating film of the present invention can be developed using the general-purpose developing liquid used previously, and the film can be reduced in a small amount and has a good pattern. 】 No [main component symbol description] If there is no good case for the device that forms goodness, then 4 is also formed.

Claims (1)

200817838 X. Patent application scope: 1 . A photosensitive resin composition for an interlayer insulating film, comprising a photosensitive resin composition for an interlayer insulating film containing an alkali-soluble resin component (A) and a photosensitive agent (B), wherein the alkali The soluble resin component (A) contains a copolymer (A1) having a structural unit (al) represented by the following formula (a-Ι) and a structural unit having a crosslinkable group (a2) , [Chemical Formula 1] [In the above formula, RG represents an argon atom or a fluorenyl group, R1 represents a single bond or an alkylene group having 1 to 5 carbon atoms, R2 represents an alkyl group having 1 to 5 carbon atoms, and a represents 1 to 5; The integer 'b' represents an integer of 0 or 1 to 4, and a + b is 5 or less. When there are two or more R2 systems, the R2s may be different from each other or may be the same. 2. The photosensitive resin composition for interlayer insulating film according to claim 1, wherein the structural unit (a2) contains a structural unit represented by the following formula (a-2), 47 200817838 [Chemical Formula 2] [R3 represents a ruthenium atom or a ruthenium group]. The photosensitive resin composition for interlayer insulating film according to claim 1 or 2, wherein the structural unit (a J) in the copolymer (A 1) and the structural unit (a2) The ratio of molar ratios is 2: 8~8: 2. 4. The photosensitive resin composition for interlayer insulating film according to claim 1, wherein the sensitizer (B) is a compound derived from a benzoquinonediazide-based compound. 5. The photosensitive resin composition for interlayer insulating film according to claim 1, wherein the sensitizer (B) is obtained by condensing a benzoquinonediazide-containing compound with a ruthenium-containing compound. The compound, and the phenolic hydroxyl group-containing compound has a Gram absorption coefficient of 1 or less at a wavelength of 350 nm. 6. The photosensitive resin composition for interlayer insulating film according to the fifth aspect of the patent application, wherein the phenolic hydroxy compound is a compound which does not contain a carbonyl group. 48 200817838 7 as described in claim 5 or 6 The photosensitive resin composition for interlayer insulating film, wherein the phenolic hydroxy compound is selected from the group consisting of a double enzyme type compound, a phenol type compound, a linear type 3 nucleus phenol compound, a linear type 4 nucleus g class compound, and a line type 5 At least one of a group consisting of a nucleus compound and a condensed compound. The photosensitive resin composition for interlayer insulating film according to claim 1, wherein the sensitizer (B) is obtained by condensing a benzoquinonediazide-containing compound with a chelating compound-containing compound. The compound having a phenolic hydroxy compound has a thermal decomposition temperature of 300 ° C or higher. A photosensitive resin composition for interlayer insulation, which is a photosensitive resin composition for an interlayer insulating film used in a method for forming an interlayer insulating film, and a method for forming the interlayer insulating film, comprising the steps of: coating photosensitive on a substrate a coating step of the resin composition; an exposure step of selectively applying the photosensitive resin after coating; and an imaging step of developing an alkali developing solution after exposure; and sensitizing the interlayer insulating film The resin composition contains an alkali-soluble resin component (Α) and a sensitizer (Β); • the alkali-soluble resin component (Α) contains a copolymer (Α1), and the structural unit (al) and ring containing the copolymer The oxygen (A 1 ) contains a structural unit (a2) containing a phenolic hydroxy structural unit-based structural unit; a diazide-based compound-derived 5% by mass aqueous solution of tetramethylammonium hydroxide. The sensitizer (B) is derived from benzene In the development step, when the image is developed by 2.38] 49 200817838, the dissolution rate of the unexposed portion is 1 〇N/sec or less, and the dissolution rate of the exposure portion is 10 nm/sec. . The photosensitive resin composition for interlayer insulating film according to claim 9, wherein a film reduction rate of the exposed portion after the developing step is 30% or less. 1. The photosensitive resin composition for interlayer insulating film according to claim 9 or 10, wherein the structural unit (al) contains only the structural unit represented by the formula (a-1). And the structural unit (a 2) contains a structural unit represented by the general formula (a - 2), [Chemical Formula 3] (R2)b (〇H)a (a-2) (a-1) [In the above formula, RG represents a hydrogen atom or a fluorenyl group, and R1 represents a single bond or an alkylene group having a carbon number of 1 to 5, R2 represents an alkyl group having 1 to 5 carbon atoms, R3 represents a hydrogen atom or a methyl group, a represents an integer of 1 to 5, b represents an integer of 0 or 1 to 4, and a + b is 5 or less, and When there are two or more R2 systems, these R2s may be different from each other or may be the same]. 50 200817838 12. A photosensitive resin composition for an interlayer insulating film comprising a photosensitive resin composition for an interlayer insulating film of an alkali-soluble resin component (A) and a photosensitive agent (B), wherein the alkali-soluble resin component is read ( A) a copolymer (A1) containing a structural unit (al) having a phenolic hydroxyl structural unit and a structural unit (a2) having a crosslinkable group, and an inductive resin for the interlayer insulating film The side wall angle of the photoresist pattern obtained by the composition is 45 degrees or more and 90 or less. 1 3 - The photosensitive fat composition for interlayer insulating film according to Item 1 of the patent application, wherein the sensitizer (B) is obtained by condensing an aging-containing compound containing a phenylhydrazine diazide compound The compound, and the phenolic hydroxyl group-containing compound has a Gram absorption coefficient of 1 or less at a wavelength of 350 nm. A photosensitive fat composition for interlayer insulating film according to claim 13 wherein the phenolic hydroxy compound is selected from the group consisting of bisphenol compounds, age-related compounds, and linear 3-nuclear phenols. At least one of a group consisting of a compound, a linear 4-core compound, a linear 5-nuclear phenol compound, and a condensed phenol compound. 1 5 . A photosensitive resin composition for an interlayer insulating film, comprising a photosensitive tree composition for an interlayer insulating film of an alkali-based resin component (A) and a photosensitive agent (B), wherein the alkali-soluble resin component is contained (A) containing a copolymer (A1) containing a structural unit (al) having a phenolic hydroxyl structural unit and a structural unit (a2) having a crosslinkable group; The light-sensing compound is dissolved in a resin 51 (2008). The sensitizer (B) contains a compound obtained by condensing a benzoquinonediazide-based compound with a phenol-containing base compound; and a photosensitive resin composition for the interlayer insulating film. The resolution of the obtained photoresist pattern was 2 μm or less. 1. The photosensitive resin composition for interlayer insulating film according to claim 12, wherein the structural unit (al) is represented by the following formula (a-1). a structural unit, and the structural unit (a2) is a structural unit represented by the following general formula (a-2), [Chemical Formula 4] (a-2) [In the above formula, RG represents an argon atom or a fluorenyl group, R1 represents a single bond or an alkylene group having 1 to 5 carbon atoms, and R2 represents an alkyl group having 1 to 5 carbon atoms, and R3 is a In the case of a hydrogen atom or a fluorenyl group, a represents an integer of 1 to 5, b represents an integer of 0 or 1 to 4, a + b is 5 or less, and when two or more R 2 systems are present, the R 2 may be different from each other. , can be the same]. 52 200817838 17. A photosensitive resin composition for an interlayer insulating film, comprising a photosensitive resin composition for an interlayer insulating film of an alkali-soluble resin component (A) and a photosensitive agent (B), wherein the alkali-soluble resin component (A) a copolymer (A1) containing only a phenolic hydroxyl structural unit represented by the general formula (a-1) as a structural unit (al) containing an acidic structural unit, and containing The structural unit (a2) represented by the formula (a-2) is used as another structural unit, f, [Chemical Formula 5] (a-1) (a-2) [In the above formula, RG represents a hydrogen atom or a methyl group, R1 represents a single bond or an alkylene group having 1 to 5 carbon atoms, and R2 represents a carbon number of 1 to 5; An alkyl group, R3 represents a hydrogen atom or a fluorenyl group, a represents an integer of 1 to 5, b represents an integer of 0 or 1 to 4, a + b is 5 or less, and when two or more R 2 systems are present, R2 can be different from each other or the same]. 1. The photosensitive tree 53 200817838 lipid composition for interlayer insulating film according to claim 17, wherein the content of the structural unit (a 1) in the copolymer is 10 mol% to 80 Molar%, and the content of the structural unit (a2) is from 1% by mole to 90% by mole. A photosensitive resin composition for an interlayer insulating film according to the above-mentioned claim 1, wherein the photosensitive resin composition for the interlayer insulating film has a viscosity change after being stored at 23 ° C for one month. The rate is ±丨% or less. The method for forming an interlayer insulating film is a method of forming an interlayer insulating film comprising the steps of: coating a photosensitive resin composition on a substrate; and selectively applying the photosensitive resin composition after coating An exposure step of exposing; and an imaging step of developing an alkali developing solution after exposure; wherein the photosensitive resin composition contains an alkali-soluble resin component (A), and the alkali-soluble resin component (A) contains a copolymer (A1) The copolymer (A1) contains a structural unit (a 1 ) represented by the following formula (a-1) and a structural unit (a2) having a crosslinkable group; the alkali imaging solution of the developing step An aqueous solution of tetramethylammonium arsenide having a concentration of 1% by mass or more and 3% by mass or less is used; [Chemical Formula 6] 54 200817838 [In the above formula, RG represents a hydrogen atom or a fluorenyl group, R1 represents an alkylene group having 1 to 5 carbon atoms, R2 represents an alkyl group having 1 to 5 carbon atoms, an integer of a 1 to 5, and b represents An integer of 0 or 1 to 4, when a + b is 5 or less and 2 or more R 2 is present, the R 2 may be different from each other, or may be phase 2 1. The interlayer insulating film as described in claim 20 The method A, wherein the structural unit (a-2) contains a enthalpy, a bond or a table represented by the following formula (2), and is the same as the 0 constitutive structure 55 200817838 [Chemical Formula 7] (a-2) [R3 represents a hydrogen atom or a methyl group]. 2 2. The interlayer insulating film method according to claim 20, wherein the alkali developing solution of the developing step uses an aqueous solution of tetraammonium hydroxide having a concentration of 2.3 8 . A photosensitive resin composition for an interlayer insulating film according to any one of claims 20 to 22, which is characterized in that the interlayer insulating film for an interlayer insulating film is an alkali-soluble resin. The resin component (A) and the sensitizer (B), the alkali-soluble resin component (A) contains a copolymer (A1), and (A1) contains a structural unit (al) represented by the following formula (a-Ι), And the structural unit of the group (a2), the form of the copolymer of the form of the film is crosslinked 56 200817838 [Chemical Formula 8] (a-1) [In the above formula, RG represents a hydrogen atom or a fluorenyl group, R1 represents a single bond or an alkylene group having 1 to 5 carbon atoms, and R2 represents an alkyl group having 1 to 5 carbon atoms, a system An integer of 1 to 5 is indicated, b is an integer of 0 or 1 to 4, a + b is 5 or less, and when two or more R2 are present, the R2 may be different from each other or may be the same. The photosensitive resin composition for interlayer insulating film according to claim 23, wherein the structural unit (a2) contains a structural unit represented by the following formula (a-2), 57 200817838 [ Chemical formula 9] (a-2) [R3 represents a hydrogen atom or a fluorenyl group]. 58 200817838 VII. Designation of representative representatives: (1) The representative representative of the case is: None. (2) The representative symbol of the representative figure is a simple description: None 8. If there is a chemical formula in this case, please disclose the chemical formula that best shows the characteristics of the invention: None