Negative-type photosensitive composition

Abstract

Provided is a negative photosensitive composition that can form a pattern having a specific taper angle and can form a cured film having high transmittance. [Solution] A negative photosensitive composition comprising (I) a polysiloxane, (II) an acrylic polymer, (III) a compound containing two or more (meth)acryloyloxy groups, (IV) a polymerization initiator, and (V) a solvent, wherein the component (III) is a combination of two or more types, and the content of the component (III) is 10.0 to 25.0 mass % based on the total content of the components (I) and (II).

Description

[Technical Field]

[0001] This invention relates to a negative-type photosensitive composition. Furthermore, this invention relates to a method for manufacturing a pattern using the same, and a method for manufacturing a device using the same. [Background technology]

[0002] In display devices such as organic electroluminescent elements (OLEDs), quantum dot displays, and thin-film transistor arrays, partitions are formed to separate pixels. One known method for forming these partitions is photolithography using a photosensitive resin composition. When a partition wall pattern is formed using a photosensitive resin composition, the walls of the formed pattern are required to have a taper angle that meets certain needs. Methods for adjusting the taper angle through processes such as exposure amount, development time, and post-bake temperature are known (for example, Patent Document 1).

[0003] A proposal has been made to improve the apparent aperture ratio and thus the brightness by making the partition walls translucent, thus creating a demand for partition walls with high transmittance. Furthermore, UV curing of materials adjacent to the partition walls becomes possible, enabling improvements in the manufacturing process. [Prior art documents] [Patent Documents]

[0004] [Patent Document 1] Japanese Patent Publication No. 2016-167447 [Overview of the project] [Problems that the invention aims to solve]

[0005] The present invention has been made based on the circumstances described above, and aims to provide a negative-type photosensitive composition that has a specific taper angle and can form a pattern of a cured film with high transmittance.

Means for Solving the Problem

[0006] The negative photosensitive composition according to the present invention comprises (I) polysiloxane, (II) acrylic polymer, (III) a compound containing two or more (meth)acryloyloxy groups, (IV) a polymerization initiator, and (V) a solvent and is composed of The component (III) is a combination of two or more kinds, The content of the component (III) is 10.0 to 25.0% by mass based on the total content of the components (I) and (II).

[0007] The method for producing a pattern according to the present invention comprises applying the above negative photosensitive composition to a substrate, exposing it, and developing it.

[0008] The method for producing a device according to the present invention comprises the above method for producing a pattern.

Advantages of the Invention

[0009] The negative photosensitive composition according to the present invention can form a pattern having a specific taper angle by heating. The cured film formed using the negative photosensitive composition according to the present invention has a high transmittance. Further, the negative photosensitive composition according to the present invention can achieve thick film formation.

Brief Description of the Drawings

[0010] [Figure 1] Conceptual diagram for explaining the taper angle.

Embodiments for Carrying Out the Invention

[0011] Hereinafter, embodiments of the present invention will be described in detail. In this specification, unless otherwise particularly limited, symbols, units, abbreviations, and terms shall have the following meanings. In this specification, unless otherwise specified, the singular includes the plural, and "one" or "it" means "at least one." In this specification, unless otherwise specified, an element of a concept can be expressed by multiple types, and if a quantity (e.g., mass %) or mole %) is given, that quantity means the sum of those multiple types. "And / or" includes all combinations of elements, as well as their use individually.

[0012] In this specification, when numerical ranges are indicated using ~ or -, they include both endpoints and have the same units. For example, 5~25 mol% means between 5 mol% and 25 mol%.

[0013] In this specification, hydrocarbons mean those containing carbon and hydrogen, and optionally oxygen or nitrogen. A hydrocarbon group means a hydrocarbon that is monovalent or divalent or more. In this specification, aliphatic hydrocarbons mean linear, branched, or cyclic aliphatic hydrocarbons, and aliphatic hydrocarbon groups mean monovalent or divalent or more aliphatic hydrocarbons. Aromatic hydrocarbons mean hydrocarbons containing aromatic rings, which may optionally have aliphatic hydrocarbon groups as substituents or be condensed with alicyclic rings. Aromatic hydrocarbon groups mean monovalent or divalent or more aromatic hydrocarbons. Furthermore, an aromatic ring means a hydrocarbon having a conjugated unsaturated ring structure, and an alicyclic ring means a hydrocarbon having a ring structure but not a conjugated unsaturated ring structure.

[0014] In this specification, alkyl means a group obtained by removing one arbitrary hydrogen from a linear or branched saturated hydrocarbon, and includes linear and branched alkyl groups, while cycloalkyl means a group obtained by removing one hydrogen from a saturated hydrocarbon containing a cyclic structure, and optionally includes a linear or branched alkyl group as a side chain in the cyclic structure.

[0015] In this specification, "aryl" means a group obtained by removing one hydrogen atom from an aromatic hydrocarbon. "Alkylene" means a group obtained by removing two hydrogen atoms from a linear or branched saturated hydrocarbon. "Arylene" means a hydrocarbon group obtained by removing two hydrogen atoms from an aromatic hydrocarbon.

[0016] In this specification, "C x~y "C x ~C y " and "C x The notation, such as "...", refers to the number of carbon atoms in the molecule or substituent. For example, C 1~6 Alkyl refers to an alkyl group having 1 to 6 carbon atoms (such as methyl, ethyl, propyl, butyl, pentyl, and hexyl). Furthermore, as used herein, fluoroalkyl refers to an alkyl group in which one or more hydrogen atoms are replaced by fluorine, and fluoroaryl refers to an aryl group in which one or more hydrogen atoms are replaced by fluorine.

[0017] In this specification, when a polymer has multiple types of repeating units, these repeating units copolymerize. These copolymerizations are either alternating copolymerization, random copolymerization, block copolymerization, graft copolymerization, or a mixture thereof. In this specification, % represents mass percentage, and ratio represents mass ratio.

[0018] In this specification, the unit of temperature is Celsius. For example, 20 degrees means 20 degrees Celsius.

[0019] <Negative-type photosensitive composition> The negative-type photosensitive composition according to the present invention (hereinafter sometimes simply referred to as "the composition") comprises (I) a polysiloxane, (II) an acrylic polymer, (III) a compound containing two or more (meth)acryloyloxy groups, (IV) a polymerization initiator, and (V) a solvent, wherein component (III) consists of two or more types, and the content of component (III) is 10.0 to 25.0% by mass, based on the total content of components (I) and (II). Hereinafter, each component contained in the composition according to the present invention will be described in detail.

[0020] (I) Polysiloxane In the present invention, the structure of the polysiloxane used is not particularly limited and can be arbitrarily selected according to the purpose. The skeletal structure of the polysiloxane can be classified into a silicone skeleton (the number of oxygen atoms bonded to a silicon atom is 2), a silsesquioxane skeleton (the number of oxygen atoms bonded to a silicon atom is 3), and a silica skeleton (the number of oxygen atoms bonded to a silicon atom is 4) according to the number of oxygen atoms bonded to the silicon atom. In the present invention, any of these may be used. The polysiloxane molecule may contain a plurality of combinations of these skeletal structures.

[0021] The polysiloxane used in the present invention preferably comprises a repeating unit represented by formula (Ia).

Chemical formula

[0022] In the repeating unit shown in equation (Ia), R Ia Examples include (i) alkyl groups such as methyl, ethyl, propyl, butyl, pentyl, hexyl, heptyl, octyl, and decyl; (ii) aryl groups such as phenyl, tolyl, and benzyl; (iii) fluoroalkyl groups such as trifluoromethyl, 2,2,2-trifluoroethyl, and 3,3,3-trifluoropropyl; (iv) fluoroaryl groups; (v) cycloalkyl groups such as cyclohexyl; (vi) nitrogen-containing groups having an amino or imide structure such as isocyanate and amino; and (vii) oxygen-containing groups having an epoxy structure such as glycidyl, or an acryloyl or methacryloyl structure. Preferably, methyl, ethyl, propyl, butyl, pentyl, hexyl, and phenyl. Ia When the compound is methyl, it is preferable because the raw materials are readily available, the film hardness after curing is high, and it has high chemical resistance. Also, R Ia When the compound is phenyl, it is preferable because it increases the solubility of the polysiloxane in the solvent, making the cured film less prone to cracking.

[0023] The polysiloxane used in the present invention may further contain repeating units represented by the following formula (Ib). [ka] During the ceremony, R Ib A group is a group obtained by removing multiple hydrogen atoms from a nitrogen and / or oxygen-containing cyclic aliphatic hydrocarbon compound, including amino, imino, and / or carbonyl groups.

[0024] In equation (Ib), R IbPreferably, these are groups obtained by removing multiple, preferably two or three, hydrogens from a nitrogen-containing aliphatic hydrocarbon ring, more preferably a five-membered or six-membered ring containing nitrogen as a component, including an imino and / or carbonyl. Examples include groups obtained by removing two or three hydrogens from piperidine, pyrrolidine, and isocyanurate. Ib This connects the Si atoms contained within multiple repeating units.

[0025] The polysiloxane used in the present invention may further contain repeating units represented by the following formula (Ic). [ka]

[0026] The repeating units represented by formulas (Ib) and (Ic) may, if their proportions are high, lead to a decrease in the sensitivity of the composition, a decrease in compatibility with solvents and additives, and an increase in film stress, making them more prone to cracking. Therefore, it is preferable that their proportions be 40 mol% or less, and more preferably 20 mol% or less, relative to the total number of repeating units of the polysiloxane.

[0027] The polysiloxane used in the present invention may further contain repeating units represented by the following formula (Id). [ka] During the ceremony, R Id These are, independently, hydrogen and C 1~30 (preferably C 1~10 ) represents a linear, branched, or cyclic, saturated or unsaturated, aliphatic hydrocarbon group or aromatic hydrocarbon group. The aliphatic hydrocarbon group and the aromatic hydrocarbon group are, respectively, unsubstituted or composed of fluorine, hydroxyl, or carbon. 1~8 Substituted with alkoxy, and In the aliphatic hydrocarbon group and the aromatic hydrocarbon group, methylene is either not replaced, or one or more methylene groups are replaced by oxy, imino, or carbonyl groups, provided that R Id It is not hydroxyl or alkoxy.

[0028] In the repeating unit shown by equation (Id), R Id Examples include (i) alkyl groups such as methyl, ethyl, propyl, butyl, pentyl, hexyl, heptyl, octyl, and decyl; (ii) aryl groups such as phenyl, tolyl, and benzyl; (iii) fluoroalkyl groups such as trifluoromethyl, 2,2,2-trifluoroethyl, and 3,3,3-trifluoropropyl; (iv) fluoroaryl groups; (v) cycloalkyl groups such as cyclohexyl; (vi) nitrogen-containing groups having an amino or imide structure such as isocyanate and amino; and (vii) oxygen-containing groups having an epoxy structure such as glycidyl, or an acryloyl or methacryloyl structure. Preferably, methyl, ethyl, propyl, butyl, pentyl, hexyl, and phenyl are preferred. Id When the compound is methyl, it is preferable because the raw materials are readily available, the film hardness after curing is high, and it has high chemical resistance. Also, R Id When the compound is phenyl, it is preferable because it increases the solubility of the polysiloxane in the solvent, making the cured film less prone to cracking.

[0029] By having the repeating units of formula (Id) above, the polysiloxane according to the present invention can be partially linear in structure. However, it is preferable that the linear structure portion be small because it reduces heat resistance. Specifically, the repeating units of formula (Id) are preferably 30 mol% or less, and more preferably 5 mol% or less, relative to the total number of repeating units of the polysiloxane. Having no repeating units of formula (Id) (0 mol%) is also one aspect of the present invention.

[0030] The polysiloxane used in the present invention may contain two or more repeating units. For example, R IaIt may also contain three types of repeating units, having a repeating unit represented by formula (Ia) and a repeating unit represented by formula (Ic), where methyl and phenyl are present.

[0031] In addition, the polysiloxane used in the present invention preferably has a silanol. Here, a silanol refers to a polysiloxane in which an OH group is directly bonded to the Si skeleton, and in a polysiloxane containing repeating units such as formulas (Ia) to (Id), a hydroxyl group is directly bonded to the silicon atom. That is, the -O in formulas (Ia) to (Id). 0.5 - vs. -O 0.5 Silanols are formed by the bonding of hydrogen atoms. The silanol content in polysiloxanes varies depending on the synthesis conditions of the polysiloxane, such as the monomer mixing ratio and the type of reaction catalyst.

[0032] The mass-average molecular weight of the polysiloxane used in this invention is not particularly limited. However, higher molecular weights tend to improve coating properties. On the other hand, lower molecular weights allow for fewer limitations on synthesis conditions and easier synthesis, while polysiloxanes with very high molecular weights are difficult to synthesize. For these reasons, the mass-average molecular weight of the polysiloxane is usually 500 to 25,000, and preferably 1,000 to 20,000 from the viewpoint of solubility in organic solvents. Here, the mass-average molecular weight is the polystyrene-equivalent mass-average molecular weight, which can be measured by gel permeation chromatography based on polystyrene.

[0033] The method for synthesizing the polysiloxane used in the present invention is not particularly limited, but for example, it can be synthesized by the method disclosed in Japanese Patent No. 6639724.

[0034] (I) The polysiloxane content is preferably 2.0 to 15.0% by mass, and more preferably 3.0 to 12.0% by mass, based on the total mass of the composition.

[0035] The mixing ratio of (I) polysiloxane and (II) acrylic polymer is not particularly limited, but a higher proportion of acrylic polymer is preferable when making a thick coating film, while a higher proportion of polysiloxane is preferable when applied to high-temperature processes and from the viewpoint of transparency and chemical resistance after curing. The content of (I) polysiloxane is preferably 8.0 to 35.0% by mass, and more preferably 10.0 to 30.0% by mass, based on the total content of (I) polysiloxane and (II) acrylic polymer.

[0036] (II) Acrylic polymer The acrylic polymer used in the present invention can be selected from commonly used acrylic polymers, such as polyacrylic acid, polymethacrylic acid, alkyl polyacrylate, and alkyl polymethacrylate. The acrylic polymer used in the present invention preferably contains repeating units containing acryloyl groups, and more preferably further contains repeating units containing carboxyl groups and / or repeating units containing alkoxysilyl groups.

[0037] The repeating unit containing a carboxyl group is not particularly limited as long as it contains a carboxyl group in its side chain, but repeating units derived from unsaturated carboxylic acids, unsaturated carboxylic acid anhydrides, or mixtures thereof are preferred.

[0038] The repeating unit containing an alkoxysilyl group can be any repeating unit containing an alkoxysilyl group in its side chain, but a repeating unit derived from the monomer represented by the following formula (B) is preferred. X B -(CH2) a -Si(OR B ) b (CH3) 3-b (B) In the formula, X B R is a vinyl group, a styryl group, or a (meth)acryloyloxy group, B is a methyl group or an ethyl group, a is an integer from 0 to 3, and b is an integer from 1 to 3.

[0039] Furthermore, it is preferable that the polymer contains repeating units containing hydroxyl groups, derived from a hydroxyl group-containing unsaturated monomer.

[0040] The mass-average molecular weight of the acrylic polymer used in the present invention is not particularly limited, but is preferably 1,000 to 40,000, and more preferably 2,000 to 30,000. Here, the mass-average molecular weight is the polystyrene-equivalent mass-average molecular weight determined by gel permeation chromatography.

[0041] (II) The acrylic polymer content is preferably 18.0 to 35.0% by mass, and more preferably 20.0 to 32.0% by mass, based on the total mass of the composition.

[0042] (II) The content of the acrylic polymer is preferably 65.0 to 92.0% by mass, and more preferably 70.0 to 90.0% by mass, based on the total content of (I) polysiloxane and (II) acrylic polymer.

[0043] (III) Compounds containing two or more (meth)acryloyloxy groups The composition according to the present invention comprises two or more compounds containing two or more (meth)acryloyloxy groups (hereinafter sometimes referred to as (meth)acryloyloxy group-containing compounds). Here, (meth)acryloyloxy group is a general term for acryloyloxy group and methacryloyloxy group. This compound is a compound that can react with (I) polysiloxane and (II) acrylic polymer to form a crosslinked structure. Here, a compound containing two or more reactive (meth)acryloyloxy groups is necessary to form a crosslinked structure. By including three or more (meth)acryloyloxy groups, a higher-order crosslinked structure can be formed.

[0044] As compounds containing two or more (meth)acryloyloxy groups, esters obtained by the reaction of (α) a polyol compound having two or more hydroxyl groups and (β) two or more (meth)acrylic acid are preferably used. Examples of this polyol compound (α) include compounds having saturated or unsaturated aliphatic hydrocarbons, aromatic hydrocarbons, heterocyclic hydrocarbons, primary, secondary, or tertiary amines, ethers, etc. as a basic skeleton and having two or more hydroxyl groups as substituents. This polyol compound may also contain other substituents, such as carboxyl groups, carbonyl groups, amino groups, ether bonds, thiol groups, thioether bonds, etc., to the extent that it does not impair the effects of the present invention.

[0045] Preferred polyol compounds include alkyl polyols, aryl polyols, polyalkanolamines, cyanuric acid, or dipentaerythritol. Here, if the polyol compound (α) has three or more hydroxyl groups, it is not necessary for all hydroxyl groups to have reacted with meth(acrylic acid); they may be partially esterified. That is, these esters may have unreacted hydroxyl groups. Examples of such esters include tris(2-acryloyloxyethyl) isocyanurate, bis(2-acryloyloxyethyl) isocyanurate, dipentaerythritol hexa(meth)acrylate, tripentaerythritol octa(meth)acrylate, pentaerythritol tetra(meth)acrylate, dipropylene glycol diacrylate, trippropylene glycol diacrylate, trimethylolpropane triacrylate, polytetramethylene glycol dimethacrylate, trimethylolpropane trimethacrylate, ditrimethylolpropane tetraacrylate, tricyclodecanedimethanol diacrylate, 1,9-nonanediol diacrylate, 1,6-hexanediol diacrylate, and 1,10-decanediol diacrylate.

[0046] The composition according to the present invention comprises a combination of two or more (meth)acryloyloxy group-containing compounds, preferably a combination of three or more (meth)acryloyloxy group-containing compounds. A composition according to the present invention comprising a combination of three (meth)acryloyloxy group-containing compounds is a preferred embodiment of the present invention. While we do not wish to be bound by any particular theory, we believe that by combining multiple (meth)acryloyloxy group-containing compounds with different glass transition temperatures, it may be possible to suppress rapid thermal reflow during the post-bake process and enable the formation of specific taper angles.

[0047] Preferably, of the two or more (meth)acryloyloxy group-containing compounds, at least one is a compound containing three or more (meth)acryloyloxy groups. More preferably, at least one is a compound containing three or more (preferably three) (meth)acryloyloxy groups, and at least one is a two-compound compound containing (meth)acryloyloxy groups. Even more preferably, in order to improve the smoothness of the pattern surface, component (III) is a combination of one compound containing three (meth)acryloyloxy groups and two compounds containing two (meth)acryloyloxy groups. In the composition according to the present invention, the content of the compound containing three or more (meth)acryloyloxy groups is preferably 20.0 to 50.0% by mass, and more preferably 30.0 to 40.0% by mass, based on the total content of component (III).

[0048] In another embodiment of the present invention, component (III) preferably includes a compound having an isocyanurate structure for the reason of improving alkali solubility during development and improving the heat resistance of the cured film. Specific examples of such compounds include tris(2-acryloyloxyethyl) isocyanurate, bis(2-acryloyloxyethyl) isocyanurate, tris(3-acryloyloxypropyl) isocyanurate, bis(3-acryloyloxypropyl) isocyanurate, tris(4-acryloyloxybutyl) isocyanurate, and bis(4-acryloyloxybutyl) isocyanurate, with tris(2-acryloyloxyethyl) isocyanurate being preferred. In the composition according to the present invention, the content of the compound having an isocyanurate structure is preferably 10.0 to 50.0% by mass, and more preferably 10.0 to 40.0% by mass, based on the total content of component (III).

[0049] From the viewpoint of reactivity, the molecular weight of a compound containing two or more (meth)acryloyloxy groups is preferably 200 to 2,000, and more preferably 200 to 1,500.

[0050] The total content of component (III) is adjusted according to the type of polymer and (meth)acryloyloxy group-containing compound used, but from the viewpoint of compatibility with the polymer, it is 10.0 to 25.0% by mass, preferably 10.0 to 20.0% by mass, based on the total content of (I) polysiloxane and (II) acrylic polymer.

[0051] (IV) Polymerization initiator The composition according to the present invention comprises a polymerization initiator. This polymerization initiator includes a polymerization initiator that generates an acid, base, or radical upon radiation, and a polymerization initiator that generates an acid, base, or radical upon heat. In the present invention, the reaction starts immediately after irradiation, and the reheating step performed after irradiation but before the development step can be omitted. Therefore, the former is preferred in terms of process shortening and cost, and a photoradical generator is more preferred.

[0052] Photoradical generators can improve resolution by strengthening the pattern shape or increasing the contrast during development. The photoradical generator used in this invention is a photoradical generator that releases radicals when irradiated with radiation. Here, examples of radiation include visible light, ultraviolet light, infrared light, X-rays, electron beams, alpha rays, or gamma rays.

[0053] The optimal amount of photoradical generator varies depending on the type and amount of active substances generated by the decomposition of the photoradical generator, the required sensitivity, and the dissolution contrast between the exposed and unexposed areas. However, based on the total content of components (I) and (II), it is preferably 0.001 to 30% by mass, and more preferably 0.01 to 10% by mass. If the amount is less than 0.001% by mass, the dissolution contrast between the exposed and unexposed areas may be too low, resulting in no additive effect. On the other hand, if the amount of photoradical generator is greater than 30% by mass, cracks may occur in the formed film, or discoloration due to the decomposition of the photoradical generator may become significant, reducing the colorless transparency of the film. Furthermore, if the amount is too high, thermal decomposition may cause deterioration of the electrical insulation properties of the cured product and gas release, which can lead to problems in subsequent processes. In addition, the film's resistance to photoresist stripping solutions, such as those primarily composed of monoethanolamine, may decrease.

[0054] Examples of photoradical generators include azo, peroxide, acylphosphine oxide, alkylphenone, oxime ester, and titanocene initiators. Among these, alkylphenone, acylphosphine oxide, and oxime ester initiators are preferred, including 2,2-dimethoxy-1,2-diphenylethane-1-one, 1-hydroxycyclohexylphenyl ketone, 2-hydroxy-2-methyl-1-phenylpropane-1-one, 1-[4-(2-hydroxyethoxy)phenyl]-2-hydroxy-2-methyl-1-propane-1-one, 2-hydroxy-1-{4-[4-(2-hydroxy-2-methylpropionyl)benzyl]phenyl}-2-methylpropane-1-one, and 2-methyl-1-(4-methylthiophenyl)-2-morpholinopropane-1- Examples include 2-benzyl-2-dimethylamino-1-(4-morpholinophenyl)-1-butanone, 2-(dimethylamino)-2-[(4-methylphenyl)methyl]-1-[4-(4-morpholinyl)phenyl]-1-butanone, 2,4,6-trimethylbenzoyldiphenylphosphine oxide, bis(2,4,6-trimethylbenzoyl)phenylphosphine oxide, 1,2-octanedion-1-[4-(phenylthio)-2-(O-benzoyl oxime)], and 1-[9-ethyl-6-(2-methylbenzoyl)-9H-carbazole-3-yl]ethanone-1-(O-acetyloxime).

[0055] (V) Solvent The composition according to the present invention comprises a solvent. This solvent is not particularly limited as long as it uniformly dissolves or disperses each component. Examples of solvents that can be used in the present invention include ethylene glycol monoalkyl ethers such as ethylene glycol monomethyl ether, ethylene glycol monoethyl ether, ethylene glycol monopropyl ether, and ethylene glycol monobutyl ether; diethylene glycol dialkyl ethers such as diethylene glycol dimethyl ether, diethylene glycol diethyl ether, diethylene glycol dipropyl ether, and diethylene glycol dibutyl ether; ethylene glycol alkyl ether acetates such as methyl cellosolve acetate and ethyl cellosolve acetate; and propylene glycol monoethyl ethers such as propylene glycol monomethyl ether and propylene glycol monoethyl ether. Examples include propylene glycol alkyl ether acetates such as propyl ether acetate (PGMEA), propylene glycol monoethyl ether acetate, and propylene glycol monopropyl ether acetate; aromatic hydrocarbons such as benzene, toluene, and xylene; ketones such as methyl ethyl ketone, acetone, methyl amyl ketone, methyl isobutyl ketone, and cyclohexanone; alcohols such as ethanol, propanol, butanol, hexanol, cyclohexanol, ethylene glycol, and glycerin; esters such as ethyl lactate, ethyl 3-ethoxypropionate, and methyl 3-methoxypropionate; and cyclic esters such as γ-butyrolactone. Of these, propylene glycol alkyl ether acetates or esters are preferred from the viewpoint of availability, ease of handling, and polymer solubility.

[0056] The solvent content of the composition according to the present invention can be arbitrarily adjusted depending on the method of coating the composition. For example, when coating the composition by spray coating, the proportion of solvent in the composition can be 90% by mass or more. In slit coating, which is used for coating large substrates, it is usually 60% by mass or more, preferably 70% by mass or more. The properties of the composition according to the present invention do not change significantly with respect to the amount of solvent.

[0057] The composition according to the present invention requires the above-mentioned (I) to (V), but further compounds can be combined as needed. These materials that can be combined are described below. The components other than (I) to (V) in the overall composition are preferably 30% by mass or less, and more preferably 20% by mass or less, based on the total mass of the composition.

[0058] The composition according to the present invention may optionally contain other additives. Examples of such additives include developer dissolving accelerators, scum removers, adhesion enhancers, polymerization inhibitors, defoamers, surfactants, and sensitizers.

[0059] Developer dissolution accelerators, or scum removers, adjust the solubility of the formed film in the developer and prevent scum from remaining on the substrate after development. Crown ethers can be used as such additives. The simplest crown ether has the general formula (-CH2-CH2-O-). nThese are represented by the formula shown. In the present invention, preferred are those in which n is 4 to 7. Crown ethers are sometimes called x-crown-y-ethers, where x is the total number of atoms constituting the ring and y is the number of oxygen atoms contained therein. In the present invention, preferred are those selected from the group consisting of crown ethers with x=12, 15, 18, or 21 and y=x / 3, as well as their benzo-condensates and cyclohexyl-condensates. More preferred specific examples of crown ethers are 21-crown-7 ether, 18-crown-6 ether, 15-crown-5 ether, 12-crown-4 ether, dibenzo-21-crown-7 ether, dibenzo-18-crown-6 ether, dibenzo-15-crown-5 ether, dibenzo-12-crown-4 ether, dicyclohexyl-21-crown-7 ether, dicyclohexyl-18-crown-6 ether, dicyclohexyl-15-crown-5 ether, and dicyclohexyl-12-crown-4 ether. In the present invention, of these, those selected from 18-crown-6 ether and 15-crown-5 ether are most preferred. The content is preferably 0.05 to 15% by mass, and more preferably 0.1 to 10% by mass, based on the total content of components (I) and (II).

[0060] The adhesion enhancer has the effect of preventing the pattern from peeling off due to stress applied after firing when a cured film is formed using the composition according to the present invention. Preferred adhesion enhancers include imidazoles and silane coupling agents. Among the imidazoles, 2-hydroxybenzimidazole, 2-hydroxyethylbenzimidazole, benzimidazole, 2-hydroxyimidazole, imidazole, 2-mercaptoimidazole, and 2-aminoimidazole are preferred, and 2-hydroxybenzimidazole, benzimidazole, 2-hydroxyimidazole, and imidazole are particularly preferred.

[0061] Polymerization inhibitors that can be added include nitrones, nitroxide radicals, hydroquinones, catechols, phenothiazines, phenoxazines, hindered amines and their derivatives, as well as UV absorbers. Among these, methylhydroquinone, catechol, 4-t-butylcatechol, 3-methoxycatechol, phenothiazines, chlorpromazines, phenoxazines, and hindered amines are preferred, as are TINUVIN 144, 292, and 5100 (BASF). As UV absorbers, TINUVIN 326, 328, 384-2, 400, and 477 (BASF). These can be used individually or in combination, and their content is preferably 0.01 to 20% by mass, based on the total content of components (I) and (II).

[0062] As an antifoaming agent, alcohol (C1~ 18 Examples include higher fatty acids such as oleic acid and stearic acid, higher fatty acid esters such as glycerin monolaurelate, polyethers such as polyethylene glycol (PEG) (Mn200~10,000) and polypropylene glycol (PPG) (Mn200~10,000), silicone compounds such as dimethyl silicone oil, alkyl-modified silicone oil, and fluorosilicone oil, and organosiloxane surfactants, which are detailed below. These can be used individually or in combination, and their content is preferably 0.1 to 3% by mass, based on the total content of components (I) and (II).

[0063] Surfactants are added to improve coating properties, developability, and other characteristics. Examples of surfactants that can be used in the present invention include nonionic surfactants, anionic surfactants, and amphoteric surfactants.

[0064] Examples of nonionic surfactants include polyoxyethylene alkyl ethers such as polyoxyethylene lauryl ether, polyoxyethylene oleyl ether, and polyoxyethylene cetyl ether; polyoxyethylene fatty acid diesters, polyoxyethylene fatty acid monoesters, polyoxyethylene polyoxypyropylene block polymers; acetylene alcohol, acetylene glycol, acetylene glycol derivatives such as polyethoxylate of acetylene alcohol and polyethoxylate of acetylene glycol; fluorine-containing surfactants such as Florard (trade name, Sumitomo 3M Co., Ltd.), Megafac (trade name, DIC Corporation), Sulfuron (trade name, Asahi Glass Co., Ltd.); or organosiloxane surfactants such as KP341 (trade name, Shin-Etsu Chemical Co., Ltd.). Examples of the aforementioned acetylene glycol include 3-methyl-1-butyne-3-ol, 3-methyl-1-pentin-3-ol, 3,6-dimethyl-4-octin-3,6-diol, 2,4,7,9-tetramethyl-5-decine-4,7-diol, 3,5-dimethyl-1-hexyn-3-ol, 2,5-dimethyl-3-hexyn-2,5-diol, and 2,5-dimethyl-2,5-hexanediol.

[0065] Examples of anionic surfactants include ammonium salts or organic amine salts of alkyldiphenyl ether disulfonic acid, ammonium salts or organic amine salts of alkyldiphenyl ether sulfonic acid, ammonium salts or organic amine salts of alkylbenzene sulfonic acid, ammonium salts or organic amine salts of polyoxyethylene alkyl ether sulfate, and ammonium salts or organic amine salts of alkyl sulfate.

[0066] Furthermore, amphoteric surfactants include 2-alkyl-N-carboxymethyl-N-hydroxyethylimidazolium betaine and lauryl amidopropyl hydroxysulfone betaine.

[0067] These surfactants can be used individually or in combination of two or more, and their content is preferably 0.005 to 1% by mass, more preferably 0.01 to 0.5% by mass, based on the total mass of the composition.

[0068] Examples of sensitizers include coumarin, ketocoumarin and their derivatives, thiopyrillium salts, and acetophenones. The addition of sensitizing dyes enables patterning using inexpensive light sources such as high-pressure mercury lamps (360-430 nm). The content of the sensitizer is preferably 0.05-15% by mass, and more preferably 0.1-10% by mass, based on the total content of components (I) and (II).

[0069] <How to manufacture patterns> The method for manufacturing a pattern according to the present invention comprises applying the composition according to the present invention to a substrate, exposing it to light, and developing it. The method for manufacturing a pattern is described in order of steps as follows.

[0070] (1) Coating process First, the composition according to the present invention is applied to a substrate. In the present invention, "on a substrate" includes cases where the composition is applied directly to the substrate, and cases where the composition is applied to the substrate via one or more intermediate layers. The formation of the coating film of the composition according to the present invention can be carried out by any conventional method known as a method for applying a photosensitive composition. Specifically, it can be arbitrarily selected from dip coating, roll coating, bar coating, brush coating, spray coating, doctor coating, flow coating, spin coating, and slit coating. Furthermore, suitable substrates such as silicon substrates, glass substrates, and resin films can be used as the substrate to which the composition is applied. Various semiconductor elements may be formed on these substrates as needed. When the substrate is a film, gravure coating can also be used. A drying step can be separately provided after the coating film is applied if desired. In addition, the coating step can be repeated once or two or more times as needed to achieve the desired thickness of the formed coating film.

[0071] (2) Pre-baking process After applying the composition to form a coating film, it is preferable to pre-bake (heat treat) the coating film to dry it and reduce the amount of solvent remaining in the coating film. The pre-bake process can generally be carried out at a temperature of 50 to 150°C, preferably 90 to 120°C, for 10 to 300 seconds, preferably 30 to 120 seconds, using a hot plate, or for 1 to 30 minutes, using a clean oven.

[0072] (3) Exposure process After forming the coating film, the surface of the coating film is irradiated with light. Any light source conventionally used in pattern formation methods can be used for light irradiation. Examples of such light sources include high-pressure mercury lamps, low-pressure mercury lamps, metal halide lamps, xenon lamps, laser diodes, LEDs, etc. Ultraviolet light such as g-line, h-line, and i-line is usually used as the irradiation light. Except for ultrafine processing such as semiconductors, it is common to use 360-430 nm light (high-pressure mercury lamp) for patterning of several micrometers to tens of micrometers. In particular, 430 nm light is often used in the case of liquid crystal display devices. As mentioned above, it is advantageous to combine the composition according to the present invention with a sensitizing dye in such cases. The energy of the irradiation light depends on the light source and the thickness of the coating film, but is generally 5-2,000 mJ / cm². 2 Preferably 10 to 1,000 mJ / cm² 2 Let's assume the irradiation light energy is 5 mJ / cm². 2 If the level is lower than this, sufficient resolution may not be obtained, while conversely, 2,000 mJ / cm² may not be sufficient. 2 If the exposure level is higher than this, it can result in overexposure and cause halation.

[0073] A general-purpose photomask can be used to irradiate light in a patterned manner. Such a photomask can be arbitrarily selected from well-known ones. The irradiation environment is not particularly limited, but generally, ambient atmosphere (air) or a nitrogen atmosphere is acceptable. Furthermore, when forming a film over the entire surface of the substrate, the entire surface of the substrate should be irradiated with light. In this invention, the term "patterned film" also includes the case where a film is formed over the entire surface of the substrate.

[0074] (4) Post-exposure heating process After exposure, post-exposure baking can be performed as needed to promote the polymer-polymer reactions within the film using a polymerization initiator. Unlike the heating step (6) described later, this heating treatment is not performed to completely harden the coating film, but rather to leave only the desired pattern on the substrate after development, allowing the remaining parts to be removed by development. Therefore, it is not essential in the present invention.

[0075] When heating is performed after exposure, a hot plate, oven, or furnace can be used. The heating temperature should not be excessively high, as it is undesirable for acids, bases, or radicals generated in the exposed area by light irradiation to diffuse into the unexposed area. From this viewpoint, the range of the heating temperature after exposure is preferably 40°C to 150°C, and more preferably 60°C to 120°C. Stepwise heating can also be applied as needed to control the curing rate of the composition. The atmosphere during heating is not particularly limited, but can be selected from an inert gas such as nitrogen, under vacuum, under reduced pressure, or in oxygen gas, for the purpose of controlling the curing rate of the composition. Furthermore, the heating time is preferably above a certain level in order to maintain a higher level of uniformity in the temperature history within the wafer surface, and is preferably not excessively long in order to suppress the diffusion of generated acids, bases, or radicals. From this viewpoint, the heating time is preferably 20 seconds to 500 seconds, and more preferably 40 seconds to 300 seconds.

[0076] (5)Developing process After exposure, and if necessary, after post-exposure heating, the coating film is developed. Any developer conventionally used for developing photosensitive compositions can be used as the developer. Preferred developers include alkaline developers, which are aqueous solutions of alkaline compounds such as tetraalkylammonium hydroxide, choline, alkali metal hydroxides, alkali metal metasilicates (hydrates), alkali metal phosphates (hydrates), ammonia, alkylamines, alkanolamines, and heterocyclic amines. Particularly preferred alkaline developers are aqueous solutions of tetramethylammonium hydroxide (TMAH), potassium hydroxide, or sodium hydroxide. These alkaline developers may further contain water-soluble organic solvents such as methanol or ethanol, or surfactants, as needed. The development method can also be arbitrarily selected from conventionally known methods. Specifically, methods include immersion in the developer (dip), paddle, shower, slit, cap coat, and spray. A pattern can be obtained through this development. After development with the developer, it is preferable to rinse with water.

[0077] (6) Post-bake process After development, the resulting pattern film is cured by heating. The same heating device used for the post-exposure heating described above can be used for this heating process. The heating temperature in this heating process is not particularly limited as long as it is a temperature at which the coating film can be cured, and can be set arbitrarily. However, if silanol groups of polysiloxane remain, the chemical resistance of the cured film may become insufficient, or the dielectric constant of the cured film may become high. From this viewpoint, a relatively high heating temperature is generally selected. Generally, in order to maintain a high residual film rate after curing, the curing temperature is more preferably 350°C or lower, and particularly preferably 250°C or lower. On the other hand, in order to promote the curing reaction and obtain a sufficiently cured film, the curing temperature is preferably 70°C or higher, more preferably 80°C or higher, and particularly preferably 90°C or higher. The heating time is not particularly limited, and is generally 10 minutes to 24 hours, preferably 30 minutes to 3 hours. Note that this heating time is the time from when the temperature of the pattern film reaches the desired heating temperature. Normally, it takes several minutes to several hours for the pattern film to reach the desired temperature from the temperature before heating.

[0078] Figure 1 is a conceptual diagram showing a pattern 2 formed on substrate 1. In this invention, the pattern formed after the development process is typically rectangular. The angle between the pattern sidewall and the substrate is called the taper angle 3. The cross-section of the pattern after development is typically rectangular (taper angle = 90°), as shown in Figure 1(a). When this pattern is heated, the coating film temporarily softens, and the cross-sectional shape of the pattern tends to change from rectangular to trapezoidal. As a result, heating tends to decrease the inclination angle of the pattern sidewall, i.e., the taper angle, and increase the width at the bottom of the cross-section of the pattern, i.e., the line width. Figure 1(b) shows a trapezoidal pattern shape, where the taper angle 4 is reduced compared to Figure 1(a). When using the composition of the present invention, the shape is close to rectangular after development, but heating can change it to a shape with a taper angle of 15 to 80°, preferably 40 to 80°. Even with further heating, the taper angle does not become any smaller, and the shape can be maintained. The taper angle is determined at the point where the substrate and the pattern meet, and can be measured by observing the vertical cross-sectional shape of the pattern with a scanning electron microscope (SEM).

[0079] The resulting cured film has high transmittance. Specifically, the transmittance for light at a wavelength of 400 nm when the film thickness is 2 μm is preferably 90% or higher, and more preferably 95% or higher.

[0080] The device manufacturing method according to the present invention includes a method for manufacturing the pattern described above. Patterns manufactured using the composition according to the present invention have high transmittance and a specific taper angle, and are suitably used as partitions for separating pixels in display devices. Since the pattern according to the present invention can be made into a thick film, it can be suitably used in micro-LEDs, quantum dot displays, and organic electronic luminescence devices where thicker partition materials are required.

[0081] The present invention will be described in more detail below with reference to examples and comparative examples, but the present invention is not limited in any way by these examples and comparative examples.

[0082] Gel permeation chromatography (GPC) is performed using the HLC-8220GPC high-speed GPC system (trade name, Tosoh Corporation) and two Super Multipore HZ-N type GPC columns (trade name, Tosoh Corporation). The measurement is performed using monodisperse polystyrene as the standard sample, tetrahydrofuran as the developing solvent, and analytical conditions of a flow rate of 0.6 ml / min and column temperature of 40°C.

[0083] <Synthesis Example 1: Polysiloxane A> In a 2 L flask equipped with a stirrer, thermometer, and condenser, 49.0 g of 25% TMAH aqueous solution, 600 ml of isopropyl alcohol (IPA), and 4.0 g of water were charged. Next, a mixed solution of 68.0 g of methyltrimethoxysilane, 79.2 g of phenyltrimethoxysilane, and 15.2 g of tetramethoxysilane was prepared in a dropping funnel. This mixed solution was added dropwise at 40°C and stirred at the same temperature for 2 hours, after which a 10% HCl aqueous solution was added to neutralize it. 400 ml of toluene and 600 ml of water were added to the neutralized solution, and the mixture was separated into two layers. The aqueous layer was removed. The mixture was then washed three times with 300 ml of water, and the resulting organic layer was concentrated under reduced pressure to remove the solvent. PGMEA was added to the concentrate to adjust the solid content to 35% by mass, thereby obtaining a polysiloxane A solution. The mass-average molecular weight (Mw) of the obtained polysiloxane A was 1,700.

[0084] <Synthesis Example 2: Acrylic Polymer A> In a 2L flask equipped with a stirrer, thermometer, condenser, and nitrogen gas inlet tube, n-butanol and PGMEA solvents are charged and heated to an appropriate temperature under a nitrogen gas atmosphere, referencing the 10-hour half-life temperature of the initiator. Separately, a mixture of acrylic acid, γ-methacryloxypropyltrimethoxysilane, 2-hydroxyethyl methacrylate, and methyl methacrylate in a ratio of 10:20:20:50, azobisisobutyronitrile, and PGMEA is prepared and added dropwise to the solvent over 4 hours. The mixture is then reacted for 3 hours to obtain acrylic polymer A. The resulting acrylic polymer A has a Mw of 8,700.

[0085] <Synthesis Example 3: Acrylic Polymer B> In a 1 L flask equipped with a stirrer, thermometer, condenser, and nitrogen gas inlet tube, 16.4 g of azobisisobutyronitrile and 120 g of butanol were charged, and the mixture was heated to an appropriate temperature under a nitrogen gas atmosphere, referencing the 10-hour half-life temperature of the initiator. Separately, a mixture of 5.16 g of methacrylic acid, 46.5 g of 3-methacryloxypropylmethyldimethoxysilane, 6.5 g of 2-hydroxyethyl methacrylate, and 70.08 g of methyl methacrylate was prepared, and this mixture was added dropwise to the solvent over 4 hours. The mixture was then reacted for 3 hours to obtain acrylic polymer B. The resulting acrylic polymer B had a mass of 7,350.

[0086] <Example 1> A solution containing 20 parts by mass of polysiloxane A obtained in Synthesis Example 1, 40 parts by mass of acrylic polymer A obtained in Synthesis Example 2, and 40 parts by mass of acrylic polymer B obtained in Synthesis Example 3 is prepared by adding polymerization initiator A ("Adeka Arcles") Add 3 parts by mass of "NCI-930" (ADEKA Corporation), 6 parts by mass of (meth)acryloyloxy group-containing compound A (1,10-decanediol diacrylate "A-DOD-N", Shin Nakamura Chemical Industry Co., Ltd.), 6 parts by mass of (meth)acryloyloxy group-containing compound B (tricyclodecanedimethanol diacrylate "A-DCP", Shin Nakamura Chemical Industry Co., Ltd.), 6 parts by mass of (meth)acryloyloxy group-containing compound C (tris-(2-acryloxyethyl) isocyanurate "A-9300", Shin Nakamura Chemical Industry Co., Ltd.), and 0.5 parts by mass of surfactant A ("KF-53", Shin-Etsu Chemical Co., Ltd.), and add PGMEA to prepare a solution with a solid content of 35% by mass to obtain the composition of Example 1.

[0087] <Examples 2-5, Comparative Examples 1-6> The compositions of Examples 2-5 and Comparative Examples 1-6 were prepared in the same manner as in Example 1, except that the composition was changed as shown in Table 1. The numerical values ​​for each component in the table represent parts by mass. [Table 1]

[0088] Each of the obtained compositions is applied to a silicon wafer by spin coating, and after application, it is heated on a hot plate at 100°C for 90 seconds (pre-baking) to form a film. An i-line lithography machine is used to refract the sample at 50 mJ / cm². 2 The sample is exposed to light through a mask, immersed in a 2.38% by mass TMAH aqueous solution for 60 seconds, then rinsed with pure water for 30 seconds and dried. As a result, a 50 μm contact hole (C / H) pattern is formed. At this time, the cross-section was observed using a scanning electron microscope (SEM), and the film thickness and taper angle were measured. The results are shown in Table 1.

[0089] The wafer with the pattern formed as described above is heated on a hot plate at 230°C for 30 minutes (post-bake) to cure the film. At this time, the cross-section is observed using a scanning electron microscope (SEM), and the film thickness and taper angle are measured. Furthermore, the pattern reflowability is evaluated according to the following criteria. The results are shown in Table 1. A: Reflow occurs after baking, and the taper angle is 15-80°. B: Reflow occurs during post-bake, causing the taper angle to exceed 80°. C: Reflow does not occur before or after post-bake. In other words, the shape does not change. D: Reflow occurred during post-bake, making taper angle measurement impossible. Furthermore, even when the cured films using the compositions of Examples 1 to 5 are further heated in air at 250°C for 10 minutes, no change in the shape of the taper angle occurs.

[0090] [Transmittance] Each of the obtained compositions was applied to alkali-free glass by spin coating and pre-baked on a hot plate at 100°C for 90 seconds. An i-line exposure system was used to test at 50 mJ / cm². 2The entire coated surface is exposed to light, immersed in a 2.38% by mass TMAH aqueous solution for 60 seconds, and then rinsed with pure water for 30 seconds. After that, it is heated at 200°C for 1 hour to cure. The resulting cured film is adjusted to a thickness of 2.0 μm. The obtained cured film is measured using a UV absorption meter (U-4000) and the transmittance at a wavelength of 400 nm is determined. The results are shown in Table 1.

[0091] [modulus of elasticity] The resulting hardened film was indented and its elastic modulus was measured using the "ENT-2100" hardness tester (Elionix Co., Ltd.). The results are shown in Table 1. Some embodiments of the present invention are described below. [Aspect 1] (I) Polysiloxane, (II) Acrylic polymer, (III) Compounds containing two or more (meth)acryloyloxy groups, (IV) polymerization initiators, and (V) Solvent A negative-type photosensitive composition comprising, (III) The components are a combination of two or more types, A composition in which the content of component (III) is 10.0 to 25.0% by mass, based on the total content of components (I) and (II). [Aspect 2] (I) The composition according to embodiment 1, wherein the polysiloxane comprises a repeating unit represented by formula (Ia). [ka] (Here, R Ia is hydrogen, C 1~30 It represents a linear, branched, or cyclic, saturated or unsaturated, aliphatic hydrocarbon group or aromatic hydrocarbon group. The aliphatic hydrocarbon group and the aromatic hydrocarbon group are, respectively, unsubstituted or composed of fluorine, hydroxyl, or carbon. 1~8 Substituted with alkoxy, and In the aliphatic hydrocarbon group and the aromatic hydrocarbon group, methylene (-CH 2 -) is not replaced, or one or more methylene groups are replaced by oxy, imino, or carbonyl groups, provided that R Ia (It is hydroxyl, not alkoxy) [Aspect 3] (I) The composition according to embodiment 2, wherein the polysiloxane further comprises repeating units represented by the following formula (Ic). [ka] [Aspect 4] The composition according to at least one of embodiments 1 to 3, wherein the content of (I) polysiloxane is 8.0 to 35.0% by mass, based on the total content of (I) polysiloxane and (II) acrylic polymer. [Aspect 5] (III) The composition according to at least one of embodiments 1 to 4, wherein component (III) is an ester compound obtained by reacting a polyol compound having two or more hydroxyl groups with two or more (meth)acrylic acids. [Aspect 6] (III) A composition according to at least one of embodiments 1 to 5, wherein the components are a combination of three or more types. [Aspect 7] A method for producing a pattern, comprising applying a composition according to any one of embodiments 1 to 6 to a substrate, exposing it to light, and developing it. [Aspect 8] The method according to embodiment 7, further comprising heating after development. [Aspect 9] The method according to embodiment 8, wherein the taper angle after heating is in the range of 15 to 80°. [Aspect 10] A method for manufacturing a device, comprising the method described in at least one of embodiments 7 to 9. [Explanation of Symbols]

[0092] 1. Circuit board 2. Pattern 3. Taper angle 4. Taper angle

Claims

1. (I) Polysiloxane, (II) Acrylic polymer, (III) Compounds containing two or more (meth)acryloyloxy groups, (IV) polymerization initiator, and (V) Solvent A negative-type photosensitive composition comprising, Component (III) is a combination of the compound containing three of one type of (meth)acryloyloxy groups and the compound containing two of two types of (meth)acryloyloxy groups. A composition in which the content of component (III) is 10.0 to 18% by mass, based on the total content of components (I) and (II).

2. (I) The composition according to claim 1, wherein the polysiloxane comprises a repeating unit represented by formula (Ia). 【Chemistry 1】 (Here, R Ｉａ is hydrogen, C １～３０ It represents a linear, branched, or cyclic, saturated or unsaturated, aliphatic hydrocarbon group or aromatic hydrocarbon group. The aliphatic hydrocarbon group and the aromatic hydrocarbon group are, respectively, unsubstituted or composed of fluorine, hydroxyl, or carbon. １～８ Substituted with alkoxy, and In the aliphatic hydrocarbon group and the aromatic hydrocarbon group, methylene (-CH ２ -) is not replaced, or one or more methylene groups are replaced by oxy, imino, or carbonyl groups, provided that R Ｉａ (It is hydroxyl, not alkoxy)

3. (I) The composition according to claim 2, wherein the polysiloxane further comprises repeating units represented by the following formula (Ic). 【Chemistry 2】

4. The composition according to at least one of claims 1 to 3, wherein the content of (I) polysiloxane is 8.0 to 35.0% by mass, based on the total content of (I) polysiloxane and (II) acrylic polymer.

5. The composition according to at least one of claims 1 to 4, wherein component (III) is an ester compound obtained by reacting a polyol compound having two or more hydroxyl groups with two or more (meth)acrylic acids.

6. A method for producing a pattern, comprising applying the composition according to any one of claims 1 to 5 to a substrate, exposing it to light, and developing it.

7. The method according to claim 6, further comprising heating after development.

8. The method according to claim 7, wherein the taper angle after heating is in the range of 15 to 80°.

9. A method for manufacturing a device, comprising the method described in at least one of claims 6 to 8.

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